European Coal Geology and Technology

Geological Society Special Publications

Series Editor A. J. FLEET
 GEOLOGICAL SOCIETY SPECIAL PUBLICATION NO. 125

European Coal Geology and Technology

EDITED BY

R. GAYER
Department of Earth Sciences,
University of Wales, Cardiff

AND

J. PESEK
Charles University, Prague, Czech Republic

1997
Published by
The Geological Society
London
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 Contents

Preface vii

Regional coal reserves, coal basin tectonics and stratigraphy

DORUSKA, J. The Czech Republic Energy Policy: conception and implementation in a 1
market economy
PEgEK, J. & DOPITA, M. Coal production and usage in the Czech Republic 3
KUMPERA, O. Controls on the evolution of the Namurian paralic basin, Bohemian Massif, 13
Czech Republic
KRS, M., PEgEK, J., PRUNER, P., SKO~EK, V. & SLZPI~KOVA, J. The origin of magnetic 29
remanence components of Westphalian C to Stephanian C sediments, West Bohemia: a
record of waning Variscan tectonism
DREESEN, R., BOSSIROY, D., SWENNEN, R., THOREZ, J., FADDA, A. OTTELLI, L. & 49
KEPPENS, E. A depositional and diagenetic model for the Eocene Sulcis coal basin of SW
Sardinia
INANER, H. & NAKOMAN, E. Turkish lignite deposits 77
KARAYIGIT, A. I. & WHATELEY, M. K. G The origin and properties of a coal seam 101
associated with continental thin micritic limestones, Selimoglu-Divrigi, Turkey
KARAYIGIT, m. I. & WHATELEY, M. K. G. Chemical characteristics, mineralogical 115
composition and rank of high sulphur coking coals of Middle Miocene age in the G6kler
coal field, Gediz, Turkey
TICLEANU, N. & DIACONITA, D. The main coal facies and lithotypes of the Pliocene coal 131
basin, Oltenia, Romania
SI~KOV, G. D. Bulgarian low rank coals: geology and petrology 141
STUKELOVA,I. E. Coal petrology and facies associations of the South Yakutian Coal Basin, 149
Siberia

Coal petrology and palaeontology

GAYER, R. A., FOWLER, R. & DAVIES, G. Coal rank variations with depth related to major 161
thrust detachments in the South Wales coalfield: implications for fluid flow and
mineralization
DvoIL~K, J., HON~K, J., PE~EK, J. & VALTEROVA, P. Deep borehole evidence for a 179
southward extension of the Early Namurian deposits near N6m~i6ky, S Moravia Czech
Republic: implication for rapid coalification
KOSTOVA, I., MARKOVA, K. & KUNTSCHEV, K. M6ssbauer spectroscopic investigation of 195
low rank coal lithotypes
PREMOVIC, P. I., NIKOLIC, N. D. & PREMOVIC, M. P. Comparison of solid state ~3C NMR 201
of algal coals/anthracite and charcoal-like fusinites: further evidence for graphitic domains
SYKOROVA, I., (~ERN~', J., PAVLIKOVA, H. & WEISHAURTOV~,, Z. Composition and 207
properties of North Bohemian coals
STEFANOVA, M. & MAGNIER, C. Aliphatic biological markers in Miocene Maritza-Iztok 219
lignite, Bulgaria
SYBRYAJ,S. Floristic characters of the upper coal-bearing formation in the Transcarpathians 229
vi CONTENTS

Mineral matter in coal and the environment

BAQR1, S. R. H. The distribution of sulphur in the Palaeocene coals of the Sindh province of 237
Pakistan
CAVENDER,P. F. & SPEARS,D. A. Sulphur distribution in a multi-bed seam 245
BOUSKA, V., PESEK, J. & ZAK, K. Values of ~34S in iron disulphides of the North Bohemian 261
lignite basin, Czech Republic
JANKES, G., CVETKOVIC, O. & GLUMICIC, T. Determination of different forms of sulphur in 269
Yugoslav soft brown coals
PREMOVI(~, P. I., NIKOLIC, N. D., PAVLOVIC, M. S., JOVANOVIC, LJ. S. & PREMOVIC, M.P. 273
Origin of vanadium in coals: parts of the western Kentucky (USA) No. 9 coal rich in vanadium
SPEARS, D. A. Environmental impact of minerals in UK coals 287

Mining geophysics
GREGOR, V. & TI~2KY, A. A well logging method for the determination of the sulphur 297
contents in coal seams by means of deep gammaspectrometry
MACH, K. A logging correlation scheme for the main coal seam of the North Bohemian 309
brown coal basin, and the implications for the palaeogeographical development of the basin
HOLU~, K. Seismic monitoring for rock burst prevention in the Ostrava-Karvinfi coalfield, 321
Czech Republic
KALA~, Z. An analysis of mining induced seismicity and its relationship to fault zones 329
OPLU~TIL, S., PE~EK, J. & SKOPEC, J. Comparison of structures derived from mine workings 337
and those interpreted in seismic profiles: an example from the Ka~ice deposit, Kladno Mine,
Bohemia

Coal technology and coalbed methane

BARRAZA, J., CLOKE, M. & BELGHAZI, A. Improvements in direct coal liquefaction using 349
beneficiated coal fractions
ALEKSI(~, B. R., ERCEGOVAC, M. D., CVETKOVlC, O. G., MARKOVlC, B. Z., GLUMI(~IC, T. 357
L., ALEKSIC, B. D. & VITOROVIC, D. K. Conversion of low rank coal into liquid fuels by
direct hydrogenation
ASMATULU, R., ACARKAN, N., ONAL, G. & CELIK, M. S. Desulphurization of low-rank 365
coals by low-temperature carbonization
WHATELEY, M. K. G., GENCER, Z. & TUNCALI, E. Amelioration of high organic sulphur 371
coal for combustion in domestic stoves
STANOJEVI(~,P., JANKES,G., KUBROVIC,M., STANOJEVI(~,M. & BLAGOJEVI(~,P. The use of 379
pulverized lignite/natural gas mixed fuels in the high-temperature process of a cement rotary
kiln
DOUCHANOV, D. & MINKOVA, V. The possibility of underground gasification of Bulgarian 385
Dobrudja's coal
BOARDMAN, E. L. & RIPPON, J. H. Coalbed methane migration in and around fault zones 391
HOLUB, V., ELIAg, M., HRAZD[RA, P. & FRANCU, J. Geological research into gas sorbed in 409
the coal seams of the Carboniferous in the Mgeno-Roudnice basin, Czech Republic
GRZYBEK, I., GAWLIK, L., SUWALA, W. & KUZAK, R. Estimation method for methane 425
emission from Polish coal mining
TAKLA, G. & VAVRUS~.K, Z. Methane emissions and its utilization from Ostrava-Karvinfi 435
collieries in the Upper Silesian coal basin, Czech Republic

Index 441
 Preface

Despite the major reduction in the coal mining industry that has taken place in
Europe over the last decade, most European countries remain strongly dependent on
utilizing coal for both power production and in the steel industry. There is an
increasing tendency to import cheaper coal from sources outside Europe and this
trend is likely to continue and even expand. However, the need to use indigenous coal
is essential and by improving knowledge of coal geology and technology, more
efficient and competitive use of existing proven and indicated reserves will be possible.
This volume contains some 40 papers describing new research into coal geology
and coal technology. These have been grouped into five sections dealing with
separate aspects of the subject, so that related papers are placed together in the
volume. However, some important coal basins have been researched by several
different techniques, and papers on these topics have been included in the
appropriate different sections. For example, the Upper Silesian basin, one of the
most important Upper Palaeozoic coal basins in Europe, is covered by six papers in
four of the sections of the volume. Similarly, the North Bohemian lignite basin is
described in four papers placed in four different sections.
Coal deposits from twelve countries are covered in the volume, with the majority of
papers (34) covering deposits in Central and Eastern Europe. Nevertheless, the
geology and technology described, despite having a geographical bias, is of general
applicability. The deposits together with the associated concepts and methods may not
be well known in the west so that the papers and included references should provide an
invaluable data source. Thus the volume can be seen as a companion volume to
European Coal Geology (Whateley & Spears 1995) which concentrated on coal
deposits in western Europe. The present volume also describes new and important
research in western Europe, updating the coal geology provided in the earlier volume.
Section One includes 11 papers describing regional coal reserves, coal basin tectonics
and stratigraphy. The regions covered include Bulgaria, the Czech Republic, Romania,
Sardinia, Siberia, and Turkey. Amongst these interesting accounts are a paper by the
late Professor Otto Kumpera, which relates the coal accumulation in the Upper Silesian
basin to processes related to foreland basin tectonics, and a paper by Krs et ai. docu-
ments the waning effects of the Variscan orogeny in the Bohemian Massif by a detailed
study of palaeomagnetism. Dreesen et al. describe an unusual coal basin in Sardinia in
which coal forming environments are closely associated with carbonates and
evaporites. The section also contains an important paper by Pesek & Dopita discussing
the present and future energy requirements and associated environmental issues of the
Czech republic, as an example of one of the developing eastern European countries.
Section Two covers various aspects of coal petrology and palaeontology in seven
papers. These include papers describing unusual variations of coal rank with depth
in Moravia (Dvorak et al.) where coals remain at relatively low rank despite being
buried beneath the Carpathian thrust sheets, and in South Wales (Gayer et al.),
where high levels of heat flow and reversals in rank increase with depth are attributed
to fluid flow within the basin. Other authors describe the results of various analytical
approaches to the study of coal petrology, including solid state 13C NMR studies of
fusinites (Premovic et al.), M6ssbauer spectroscopy of low rank coal lithotypes
(Kostova et al.), and biochemical analysis of lignite (Stefanova & Magnier).
Section Three deals with mineral matter in coal and the environment. The six papers
include the sulphur contents of Pakistan coals (Baqri), of Yugoslavian lignites
viii PREFACE

(Jankes et ai.) and of a multi bed coal in the UK (Cavender & Spears). Bouska et aL
discuss the sulphur isotopic composition of North Bohemian lignites and Premovic
et aL present the results of vanadium analysis in Kentucky coals.
Section Four contains five papers concerned with mining geophysics. These include
well logging techniques applied to the North Bohemian lignite basin (Mach) and the
use of a deep gamma spectrometer (Gregor & Tezky). Seismic monitoring for rock
bursts (Holub) and mining induced seismicity (Kalab) are two aspects of seismic
investigation covered in the section.
The final Section Five includes papers describing coal technology and coalbed
methane. Liquefaction is discussed in two papers; one by Aleksic et aL using direct
hydrogenation of low rank coals and the other describing experiments on
beneficiated coal fractions (Barraza et aL). Desulfurization is also covered in two
papers; one by Asmatulu et al. and the other by Whateley et aL, both dealing with
unusual techniques to treat high sulphur Turkish coals. Gassification and coalbed
methane generation from mines is covered by Douchanov & Minkova, Gryzbek et aL
and Holub et aL, whilst Boardman & Rippon present an analysis of the influence of
faults in coalbed methane production.
The editors would like to thank all the authors for submitting the papers which
represent a selection of those originally presented at the Second European Coal
Conference in 1995 in Prague. We would also like to thank the many geologists who
reviewed the papers:

Mesdames & Messieurs Austin, Bouska, Brabham, Bright, Bryant, Cloke, Cole,
Cornford, Davidson, Davies, Dopita, Drozdzewski, Ellison, Frodsham, Gayer,
Gillespie, Glover, Goulty, Guion, Harris, Hathaway, Hemsley, Holub, Honek,
Jelinek, Jones, Juch, Karayigit, Konecny, Kostova, Kropacek, Kumpera, McLean,
Malan, Martinec, Miliorizos, Moore, Oplustil, Patrick, Pesek, Premovic, Querol,
Rhodes, Rippon, Rosa, Simunek, Skocek, Spears, Spiker, Thomas, Turner, Wagner,
Wakefield, Whateley.

Many of the papers were written by authors whose first language is not English and
this represented a problem not only for the authors but also for the reviewers. Both
worked very hard to produce the present results. We have been continually amazed at
the language skills of European geologists and hope that any slight errors remaining
in the texts do not detract from the value of the volume. Sadly, one of the authors,
Professor Kumpera, died before completing the final version of his major work on the
geology of the Upper Silesian basin. Although his widow, Anna Kumperova,
continued with the drafting of the diagrams, the conclusions have been added by the
editors who accept responsibility for any errors inadvertently produced. We would
also like to thank David Ogden, the staff editor at the Geological Society Publishing
House for his continuing support and editing of this volume.

Dr Rod Gayer, Cardiff

Professor Jiri Pesek, Prague

Reference
WHATELEY, M. K. G. & SPEARS, D. A. (eds) 1995. European Coal Geology. Geological Society, London,
Special Publication, 82.
 Preface

Despite the major reduction in the coal mining industry that has taken place in
Europe over the last decade, most European countries remain strongly dependent on
utilizing coal for both power production and in the steel industry. There is an
increasing tendency to import cheaper coal from sources outside Europe and this
trend is likely to continue and even expand. However, the need to use indigenous coal
is essential and by improving knowledge of coal geology and technology, more
efficient and competitive use of existing proven and indicated reserves will be possible.
This volume contains some 40 papers describing new research into coal geology
and coal technology. These have been grouped into five sections dealing with
separate aspects of the subject, so that related papers are placed together in the
volume. However, some important coal basins have been researched by several
different techniques, and papers on these topics have been included in the
appropriate different sections. For example, the Upper Silesian basin, one of the
most important Upper Palaeozoic coal basins in Europe, is covered by six papers in
four of the sections of the volume. Similarly, the North Bohemian lignite basin is
described in four papers placed in four different sections.
Coal deposits from twelve countries are covered in the volume, with the majority of
papers (34) covering deposits in Central and Eastern Europe. Nevertheless, the
geology and technology described, despite having a geographical bias, is of general
applicability. The deposits together with the associated concepts and methods may not
be well known in the west so that the papers and included references should provide an
invaluable data source. Thus the volume can be seen as a companion volume to
European Coal Geology (Whateley & Spears 1995) which concentrated on coal
deposits in western Europe. The present volume also describes new and important
research in western Europe, updating the coal geology provided in the earlier volume.
Section One includes 11 papers describing regional coal reserves, coal basin tectonics
and stratigraphy. The regions covered include Bulgaria, the Czech Republic, Romania,
Sardinia, Siberia, and Turkey. Amongst these interesting accounts are a paper by the
late Professor Otto Kumpera, which relates the coal accumulation in the Upper Silesian
basin to processes related to foreland basin tectonics, and a paper by Krs et ai. docu-
ments the waning effects of the Variscan orogeny in the Bohemian Massif by a detailed
study of palaeomagnetism. Dreesen et al. describe an unusual coal basin in Sardinia in
which coal forming environments are closely associated with carbonates and
evaporites. The section also contains an important paper by Pesek & Dopita discussing
the present and future energy requirements and associated environmental issues of the
Czech republic, as an example of one of the developing eastern European countries.
Section Two covers various aspects of coal petrology and palaeontology in seven
papers. These include papers describing unusual variations of coal rank with depth
in Moravia (Dvorak et al.) where coals remain at relatively low rank despite being
buried beneath the Carpathian thrust sheets, and in South Wales (Gayer et al.),
where high levels of heat flow and reversals in rank increase with depth are attributed
to fluid flow within the basin. Other authors describe the results of various analytical
approaches to the study of coal petrology, including solid state 13C NMR studies of
fusinites (Premovic et al.), M6ssbauer spectroscopy of low rank coal lithotypes
(Kostova et al.), and biochemical analysis of lignite (Stefanova & Magnier).
Section Three deals with mineral matter in coal and the environment. The six papers
include the sulphur contents of Pakistan coals (Baqri), of Yugoslavian lignites
viii PREFACE

(Jankes et ai.) and of a multi bed coal in the UK (Cavender & Spears). Bouska et aL
discuss the sulphur isotopic composition of North Bohemian lignites and Premovic
et aL present the results of vanadium analysis in Kentucky coals.
Section Four contains five papers concerned with mining geophysics. These include
well logging techniques applied to the North Bohemian lignite basin (Mach) and the
use of a deep gamma spectrometer (Gregor & Tezky). Seismic monitoring for rock
bursts (Holub) and mining induced seismicity (Kalab) are two aspects of seismic
investigation covered in the section.
The final Section Five includes papers describing coal technology and coalbed
methane. Liquefaction is discussed in two papers; one by Aleksic et aL using direct
hydrogenation of low rank coals and the other describing experiments on
beneficiated coal fractions (Barraza et aL). Desulfurization is also covered in two
papers; one by Asmatulu et al. and the other by Whateley et aL, both dealing with
unusual techniques to treat high sulphur Turkish coals. Gassification and coalbed
methane generation from mines is covered by Douchanov & Minkova, Gryzbek et aL
and Holub et aL, whilst Boardman & Rippon present an analysis of the influence of
faults in coalbed methane production.
The editors would like to thank all the authors for submitting the papers which
represent a selection of those originally presented at the Second European Coal
Conference in 1995 in Prague. We would also like to thank the many geologists who
reviewed the papers:

Mesdames & Messieurs Austin, Bouska, Brabham, Bright, Bryant, Cloke, Cole,
Cornford, Davidson, Davies, Dopita, Drozdzewski, Ellison, Frodsham, Gayer,
Gillespie, Glover, Goulty, Guion, Harris, Hathaway, Hemsley, Holub, Honek,
Jelinek, Jones, Juch, Karayigit, Konecny, Kostova, Kropacek, Kumpera, McLean,
Malan, Martinec, Miliorizos, Moore, Oplustil, Patrick, Pesek, Premovic, Querol,
Rhodes, Rippon, Rosa, Simunek, Skocek, Spears, Spiker, Thomas, Turner, Wagner,
Wakefield, Whateley.

Many of the papers were written by authors whose first language is not English and
this represented a problem not only for the authors but also for the reviewers. Both
worked very hard to produce the present results. We have been continually amazed at
the language skills of European geologists and hope that any slight errors remaining
in the texts do not detract from the value of the volume. Sadly, one of the authors,
Professor Kumpera, died before completing the final version of his major work on the
geology of the Upper Silesian basin. Although his widow, Anna Kumperova,
continued with the drafting of the diagrams, the conclusions have been added by the
editors who accept responsibility for any errors inadvertently produced. We would
also like to thank David Ogden, the staff editor at the Geological Society Publishing
House for his continuing support and editing of this volume.

Dr Rod Gayer, Cardiff

Professor Jiri Pesek, Prague

Reference
WHATELEY, M. K. G. & SPEARS, D. A. (eds) 1995. European Coal Geology. Geological Society, London,
Special Publication, 82.
The Czech Republic energy policy: conception and implementation in a
market economy
JOSEF DORUSKA

Ministry of Industry and Trade of the Czech Republic, 11015 Prague 1, Czech Republic

Abstract: In 1992 the government of the Czech Republic approved the 'Energy Policy of the
Czech Republic'. It was directed to the legislative and ecological respects which are
compatible with European Union countries.

In the period since February 1992, when the With respect to the above-mentioned principles,
energy policy was approved by the Government a programme of desulphurization of power
of the Czech Republic there have been many plants has been accepted. By 1998 the following
changes. For example, in July 1992 the Govern- power plants will be equipped with machinery
ment approved its programme; the former Czech for flue gas desulphurization:
and Slovak Federal Republic was divided into
the Czech and Slovak Republics; a major part of
the energy companies was privatized; price Tugimice II output 800 MW
adjustment of a considerable part of the energy Prun6~ov output 1490 MW
commodities was abrogated and the Ingoldstadt Po6erady output 1000 MW
oil pipeline construction was started. The Tisovfi output 110 MW
Government has considered many other aspects Chvaletice output 600 MW
M~lnik II output 220 MW
which have a substantial influence on the energy M61nik III output 500 MW
sector including documents on: Governmental D6tmarovice output 800 MW
policy concerning the environment of the Czech
Republic, of principles of the governmental
mineral policy; European agreement on incor- The realization of this programme will sig-
poration of the Czech Republic into the nificantly contribute to improvement of the
European Union; European Energy Charter; environment. The government of the Czech
results of the Uruguay round of GATT; Con- Republic realizes the importance of:
vention on climatic change; and others. Because
of the changes and new agreements there is a 9 ensuring the energy for the national economy
need to update the energy policy of the Czech 9 sustaining ecological limits resulting from the
Republic.
impacts on the environment
The updated energy policy that is being 9 ensuring the permanently sustainable devel-
elaborated by the Ministry of Industry and opment of the national economy
Trade, is created in such a way that the transition 9 fulfilling obligations of the Czech Republic
of the power industry would lead t o - i n resulting from the Energy Charter.
technical, legislative and ecological respects - a
compatibility with the power industries of the The government is ready to react to changing
advanced countries of the European Union. conditions in energy supplies. The government
The basic long-term objectives of the updated realizes that with respect to: (1) the level of
energy policy are:
national reserves of fossil energy sources, and
(2) the negative impacts of utilization of fossil
9 to ensure sufficient energy supplies for the energy sources on the environment; it is necessary
economy at acceptable prices; to develop ways that will respect both the Energy
9 to minimize negative impacts of energy Charter and conditions of permanently sustain-
production, distribution and consumption able development of the national economy.
on the environment in order to reach a The Czech Republic is one of a group of
common level in the countries of the countries of Central and Eastern Europe where
European Union; the transition process is taking place. In
9 to prepare the power economy of the Czech historical times the territory of the Czech
Republic for entry into the European Union Republic was part of the Roman Empire,
in legislative and technical respects. whereas in the Middle Ages borders were

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 1-2.
2 J. DORUSKA

difficult to define between dozens of kingdoms References

and principalities. At the beginning of the 21st
century we are on the threshold of transnational Resolution of the Government of the Czech Republic
integration of the energy sector. on the Power Policy of the CR, Prague, February
The basis of the economic prosperity of the 1992.
Updated Energy Policy of the CR, Ministry of
European Union countries was in steel and coal,
Industry and Trade of the Czech Republic,
but the development of human knowledge has Prague, June 1994.
extended this to include information and com- The Basic Principles of the Governmental Mineral
munication areas. In these areas the Czech Policy of the CR (work version), Ministry of
Republic is ready to play its full role. Economy of the Czech Republic, Prague, 1994.
 Coal production and usage in the Czech Republic
J. P E S E K 1 & M . D O P I T A ~

1Faculty of Science, Charles University, 128 43 Praha 2, Albertov 6, Czech Republic

2 Vysok{l s~kola bgt~skgt, 708 O00strava-Poruba, ti.17, listopadu, Czech Republic

Abstract: Coal mining in the industrialized countries of Europe including the Czech
Republic is witnessing a prolonged recession in the production of bituminous coal and
lignite in particular due to reduced demands. Recession in numerous fields of industry has
resulted apparently in lower production of metallurgical coke as well as in power generation.
In addition, some countries have substituted the burning of solid fossil fuels with petroleum
or natural gas or with other energy sources such as nuclear power, hydroenergy or
geothermal energy. The Czech Republic is facing similar problems.

Judging from various scenarios presented by noted that the Czech Republic always has been
different institutions, it is becoming apparent and will continue be more dependent on the
that the production of bituminous coal in the output of coal in power generation in the year
Czech Republic even after the year 2000 will not 2000 than any neighbouring country.
drop dramatically below the level of production
during 1993 and 1994. It is expected that about
14-16 x 106 metric tons of bituminous coal will Electric power generation vs coal production
be extracted in the year 2000 while the produc- and coal reserves
tion in 1994 was about 17 x 106metric tons.
Limited coal reserves in the workable levels of The whole spectrum of problems related to coal
coal mines which will still be in operation in mining can be divided basically in two groups.
2000 and whose prospects are promising, will The first involves issues related to mining and
require the development of new mine levels necessary protection of coal reserves, whereas
(e.g. Darkov and CSM mines in the Upper the second group involves issues related to
Silesian basin) and, around the year 2010, even improvement of the environment badly affected
the sinking of some new shafts in the Beskydy by mining operations.
piedmont part of the Upper Silesian basin. The policy to develop heavy industry following
Financial and time demands will play an the communist coup d'gtat in February 1948,
important role when establishing such a sce- resulted in considerable increase in pig iron, steel
nario. The cost of developing a new mine level, and other energy demanding products. This
taking into account the extent of the mining resulted in a rather high consumption of elec-
space required, the depth and the mining tricity by the former Czechoslovakia (Fig. 1).
method, may be from 1.5 to 3 x 109 K6 at the As more than 90% of Czechoslovakia electricity
current prices. Costs in developing a new mine was generated from lignite in the early 1960s,
can be as much as 20 x 109 K~ (see the Frengtfit lignite production in the years 1946 through
mine) but the anticipated output from such a 1984 increased from 19.5 x 106metric tonnes to
mine can only be achieved 10 to 15 years after more than 101 x l06., and generation of elec-
commencing its construction. Some extra time is tricity increased from 5.6 x 109 kWh in 1946 to
also required for conceptual issues, designing 89 x 109kWh in 1989. Nuclear power stations
and for negotiations with legal entities operating at Jaslovsk6 Bohunice and Dukovany came
in the region. These delaying factors argue for an into operation in the 1970s. The gradual intro-
intensification of studies to produce a long-term duction of nuclear power supplied only a part of
plan for solid and other fuel consumption in the the increase in energy demands of the former
Czech Republic in order to provide alternatives Czechoslovakia. However, in the 1980s, the
in the time span of 25 to 30 years. We consider
the role of government to be paramount in this
issue which is supported by numerous docu- * Similar considerable increase in production of lignite
after World War II was recorded in former Yugosla-
ments from industrialized European countries as
via, and in production of bituminous coal in former
well as from the USA. Our view, similar to that USSR, Poland and Australia. By contrast, a com-
of Formfinek (1994) is that the role and impor- pletely opposite trend in mining for coal in the same
tance of coal in the structure of primary energy period of time was recorded for instance in the USA,
sources has been underestimated. It is to be Great Britain, France and Spain.

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 3-12.
4 J. PESEK & M. DOPITA

100-
1
2 .........
8Q-

..~ 60-
QO0e

t,..O
40-

20-

O.
1935 4'0 4's ~'0 5'~ 6~ 6'~ 7~ 7~ ~0 ~s ~0 ~9'95
Fig. 1. Electrical power generation in the period 1937-1994 (1) in Czechoslovakia; (2) in the Czech Republic.
Note: Czech Republic constituted about two thirds of the territory of former Czechoslovakia.

patterns of production of electricity and coal important sector of the mineral raw materials
(particularly lignite) began to differ considerably mining industry. Coal has a prominent position
(see Figs 1-3). Whereas production of lignite among fossil fuels because natural hydrocarbon
reached its peak in 1985, the power generation resources in the Czech Republic are negligible.
culminated later in 1989. The relatively great Extraction of coal and its utilization has had a
difference between the decreasing coal produc- continuingly harmful influence on the environ-
tion but continuing increase in power generation ment, not only in coal mining districts (Ostrava
up to 1989 can be attributed to the electricity region, Kru~n6 hory piedmont basin) but also in
supply from nuclear power stations. areas where its consumption has been concen-
Apart from the major decrease in demand for trated such as around large coal-burning power
solid fuels in the former Czechoslovakia which is stations and in large cities (e.g. North Bohemian
also evident in the Czech Republic, the coal basin, the M6lnik region, Prague agglomeration
mining industry remains the largest and most and other large cities).

120

2 .........
100

80
"~
~176
".~
~- 6o-

20

0
4935 4'0 4~, 5'0 5'5 r~ 6's 7b 75 e:o ~ 9'0 19'95
Fig. 2. Production of lignite (in metric tonnes) in the period 1937-1994 (1) in Czechoslovakia; (2) in the
Czech Republic.
 COAL PRODUCTION IN THE CZECH REPUBLIC 5

25

~Z Is

10-

0 -----r
193s 4'0 45 s'0 & 60 & 7'0 7's 8b 8's ag'gs
Fig. 3. Production of bituminous coal both in former Czechoslovakia and in the Czech Republic (in metric
tonnes) in the period 1937-1994.

It is obvious that the high coal consumption respectively, whereas in the former Czechoslo-
in former Czechoslovakia has resulted in a vakia the equivalent requirement was 1.6kg!
significant depletion of coal reserves with These figures perhaps do not need any comment.
associated adverse impacts. Economic reform
introduced after 1989 accelerated further reduc-
tion in demand for bituminous coal and lignite
(Figs 2 & 3). This trend led to a decrease in coal Durability of workable coal reserves in
production to economically and technically mined levels of the Ostrava-Karvinfi coal
feasible levels and also to an abandonment of district and of other bituminous coal basins
selected (and by that time) inefficient mines. The
intentions of the Czech Government and pres- The Czech coal mining industry has reacted to
sure by local authorities are oriented towards a reduced demand for bituminous coal and lignite
reduction of the negative impacts of both coal in the same way as any other country's mining
mining and its combustion on the environment industry. Several underground mines have
(cf. Formfinek 1994, Reichmann 1994, Spousta already been abandoned with the result that in
1995). These factors are reflected in the present the Rosice-Oslavany, Plzefi and Intra Sudetic
position of the coal mining industry and in its basins, mining activities have ceased completely.
search for the most suitable methods for a rapid Lignite production in the single underground
inprovement of its situation. The solution lies mine in the Sokolov region as well as extraction of
not only in economical, technical and technolo- bituminous coal in the Ostrava part of the Upper
gical parameters, but also in averting potentially Silesian basin has also terminated. Reduction of
grave social and thus political consequences. coal mining in the Peffvald part of the Upper
The decrease in production of fossil fuels in Silesian basin is scheduled to commence during
the Czech Republic has resulted not only from 1995. Various volumes of workable reserves were
the above factors but also from the restructuring left behind in all the above-mentioned mines
of the economy which has led to a gradual (Table 1). If these volumes are included in an
reduction of metallurgical production and a overall diminution of workable coal reserves in
concentration on the manufacturing of energe- the Czech Republic and when taking into
tically less demanding products. However, it consideration minimum profit achieved by the
should be noted that the decline in industrial coal mining companies, it is necessary to discuss
production in the Czech Republic and in the again the fate of workable reserves which our
former Czechoslovakia in the years 1990-1993 country has currently at its disposal. Ostravsk6
has not been matched as yet by a similar doly a.s., our largest bituminous coal mining
decrease in the power demands. To manufacture company which together with the Dill CSM mine
products worth 1 USD, Austria and France produce more than 90% of the annual output in
needed in 1990, 0.18 and 0.2 kg of oil equivalent the Czech Republic showed a profit of only
 J. PESEK & M. DOPITA

Table 1. Workable reserves in 10 6 t o n n e s left in abandoned bituminous coal mines due to closure
programmes in the years 1990 through 1995

Sverma mine (OKR) 32.002 by January l, 1994

Hehnanice mine 26.863 by January l, 1994
Ostrava mine 30.496 by January 1, 1994
Odra mine 25.284 by January 1, 1994
J. Fu6ik mine 13.727 an estimate by the date of expected shut-down in 95
Krimich mine 2.5 an estimate by the date of expected shut-down in 95
Dobr6 ~t6sti mine 0.5 by January 1, 1991
Jind~ich mine 7.2 by January 1, 1994
Z. Nejedl2~ mine 121.14 by January 1, 1994
J. Sverma mine (VUD) 8.12 by January 1, 1992
Kate~ina mine 46.5 by January 1, 1994

147 x 106K6 (approximately 5.5 x 106USD) in Karvinfi coal district. Table 2 shows that the coal
1992, and 31.4 x 106K6 (approx. 1.2 x 106USD) reserves in currently operating mines will last
in 1993. The company applied selective but not without any large investment on average until
always well-advised mining measures to improve 2010 or 2016, depending on the percentage lost
mining methods. Nevertheless, it is necessary to during recovery, unless some unexpected event in
separate strictly workable reserves which occur in the mining industry occurs in the Ostrava region
the operating levels of existing mines from those e.g. abandonment of more mines, isolation of
whose development and extraction would require currently workable reserves due to regional or
huge investment, particularly in the Czech part of ecological limitations (see intensions of local
the Upper Silesian basin (Table 2). However, authorities to outline a safety pillar under the
individual mines of the Ostrava-Karvinfi coal city of Karvinfi and/or under the spa of Darkov).
district (OKR) have not at present sufficient Introduction of these or other measures would
financial resources for the required investment. It reduce the lifespan of workable coal reserves in
should be noted that one more underground the Czech Republic (Pe~ek & Pe~kovfi 1993; Pe~ek
bituminous coal mine in the Kladno region is still et al. 1993). It is to be hoped that these alarming
in operation. Its coal reserves, however, consti- figures should provoke the relevant authorities
tute less than 10% of workable reserves occurring into appropriate action. Almost 130 x 106 metric
in mined and developed levels of the Ostrava- tonnes of workable reserves have been left in

Table 2. Workable reserves of bituminous coal in I06 tonnes in operating mines in the Czech Republic registered by
December 31, 1994, and their duration in operating and developing levels

Upper Silesian basin

total workable reserves 586.6
of which confined to:
operating levels 149
developing levels 164
designed levels 164
total 454
Kladno basin
workable reserves in the Kladno mine 19
Total workable reserves confined to operating and developing levels 332
Anticipated output in the Czech Republic in 1995 (sine 1992) 16.4-16.7 i.e. average about 16.5
anticipated recovery factor
60% 100%

Decline in reserves of operating mines in 1995 -23.1 -16.5

Anticipated production in CR in 2000 (sine 1992) 14.5 14.5
Decline in reserves of operating mines in 1996 through 2000 -101.5 -76.5
Anticipated volume of reserves by January 1, 2001 201.8 239.0
Life of mineable reserves in operating mines in operating and
developing levels at the yearly anticipated output of 14.5 x 10 6 9.9 years 16.4 years
i.e. till the year 2010 2016
 COAL PRODUCTION IN THE CZECH REPUBLIC 7

prematurely closed mines of the O K R which highly questionable from the viewpoint of a
represents 6 to 8 years of coal production in long-term mineral policy. It may have been more
the Czech Republic. Further reserves appear to realistic to compare the costs involved in closing
be irretrievably lost in the Rosice-Oslavany selected mines with those related to subsiding
basin (RUD mines) and particularly in mines operating mines. There can be no doubt that if
of the Intra Sudettic basin (VUD). underground mining for bituminous coal had
been subsidized at a comparable rate to that
applied in countries of the European Economic
Community (see above) the so-called unprofita-
Issues related to profitability of underground ble Czech mines could have continued to
coal mining with particular reference to operate. It is obvious that outlay of capital
bituminous coal related to the development of new levels and/or a
new mine would be higher than any mining
Termination of bituminous coal production in company could afford. The question is whether it
the Rosice-Oslavany basin, then in NE Bohe- is more rewarding to extract the easily accessible
mia, and abandonment of coal mines in the coal reserves in mines scheduled to be shut down,
Ostrava region and in western Bohemia (see but in which some investment has already been
above) was motivated either by reduced con- made and operation costs incurred, in order to
sumption or by unprofitability of underground develop some part of the mining space. The
mining. To date it has been questionable relatively small volume of workable reserves of
whether discussion of profitability (i.e. not bituminous coal should provoke the country's
subsidized) of coal production is meaningful planner to reconsider the future of coal mining
under regulated (until recently) prices of coal and to assess if, within the next ten to fifteen
and the still regulated prices of energy. This is years, there will be any coal left to be extracted.
the major issue from which the majority of There is no doubt that in the long term some
partial problems are derived. revitalization of coal demand will occur. Coal
According to an EC commission report, the should be considered not only as a traditional
average expenditure related to extraction of fuel for energy generation and production of
1 metric ton of bituminous coal in EC coun- coke but also and in particular as an irreplace-
tries in 1990 was equal to 200DM (3460K6, able raw material for the chemical industry.
i.e. 102ECU). Expenditure in Germany was There is a requirement for the thoughtful manip-
260DM (132ECU). In 1994, their figures ulation of the coal reserves because present
were 289 DM (147 ECU) in the Ruhr basin and mining methods do not allow the remaining coal
265DM (135ECU) in the Saar basin but the to be extracted from prematurely abandoned
price of 1 metric tonne of an equivalent of mines. Consequently, coal reserves of aban-
bituminous coal imported into Germany was doned basins (coal districts) are lost forever
70 DM (36 ECU) in 1994. Expenditure in Great including elimination of mining skills in the
Britain as only 150DM (76ECU) in 1994. region. Reference to abandonment of numerous
Consequently, prices in Germany were subsi- mines in industrialized western countries
dized by 54.5 ECU per metric tonne, i.e. about appears to be irrelevant when considering our
1853 K6 (1 E C U = 3 4 K 6 ) . In Spain the equiva- specific situation. The fundamental difference
lent subsidy was 26.4 ECU per tonne. However, between the Czech Republic and for instance
in 1993 the subsidy in Germany increased Great Britain, Germany and/or other countries
to 69.5 ECU per tonne, and in 1994 to 215 DM is in the fact that some of these countries includ-
(109ECU) per tonne in the Ruhr basin and ing USA and Canada have considerably larger
210DM (107ECU) in the Saar basin which is yet untouched coal reserves which can be
K6 3720 and 3633 respectively. In contrast, exploited in the event of revitalized demands
expenditure related to the extraction of 1 tonne for bituminous coal.
of bituminous coal in Spain were reduced to
ECU 19.8 per tonne in 1993, when numerous
unprofitable mines were shut down. Where to obtain energy after exhaustion of
Comparing geological and mining conditions, coal reserves?
the Ruhr basin appears to be unambiguously
very similar to the OKR. Thus the intention to A considerable reduction in coal mining
make underground mining bituminous coal in (e.g. France) or even its complete liquidation
the Czech Republic profitable, seems to be highly (e.g. Belgium) has taken place in several west
problematic. It may be too late to reverse, but European countries. The generation of electri-
closing so-called non-profitable mines remains city from classical sources is either substantially
8 J. PESEK & M. DOPITA

(France) or partially (.numerous west European its obligations and shuts down the Chernobyl
countries) replaced by nuclear energy, indigen- nuclear power station by the year 2000. It is
ous or imported noble fuels or the partial anticipated that this nuclear capacity will be
substitution of indigenous coal by imported replaced by the construction of new coal burning
cheaper coal. The absence of large deposits power stations.
of crude oil and gas in the Czech Republic, the
slow and expensive construction of the Temelin
nuclear power plant which, together with the
high level waste repository, is opposed by both Is coal a strategic raw material for the
the Czech and foreign public, suggest that the Czech Republic?
Czech Republic could in the future be dependent
We believe that this question deserves an
on importing a large volume of coal for the
unambiguous positive answer. Provided that
generation of electricity, once the domestic fossil
more than 30-35% electricity requirement is
fuels have been exhausted. Consequently, prior
generated by combusting mostly lignite from
to the complete exhaustion of the Czech coal
opencast mines (in the year 2000 still about
reserves, the republic should either plan the
construction of further nuclear power stations or 48%), then there can be no other answer. We
recall the economic break-down resulting from
make advance arrangements with potential coal
the sudden extreme drop in temperature which
exporting countries (such as Poland) for the
occurred between December 31, 1978 and
supply of the necessary volume of coal. These
January 1, 1979. If we look at coal from another
negotiations should involve not only contracts
angle, the Czech administration should at least
containing long-term financial guarantees but
create the conditions and apply appropriate
also specifications and data on basic technolo-
measures to secure enough coal reserves for
gical parameters of the imported coal including
operating power and heating plants at large
limits on harmful substances, etc. Published data
agglomerations. This is required to prevent a
suggest that coal from the Polish part of the
reduction in power and heat generation leading
Upper Silesian basin has for instance a higher
to a complete breakdown of the whole economy
content of sulphur. It is also necessary to deter-
because of, for instance, extreme climatic
mine the volume of coal that can be imported via
changes or other reasons such as long-lasting
the international transport network, particularly
strikes of miners or railroad workers.
through the present railroad system, and also to
consider boat transport, etc. However, if the
coal is imported from other than neigbouring
countries, then its import will be limited by the Regional and enviromental limitations
transport capacity of the transit countries and stimulated by the Czech administration
would also incur transit charges which show
an increasing trend. Another issue involves The Government of the Czech Republic has
payments for imported electricity or fuels. The since 1991 passed several decrees constraining
administration would need to consider the finan- the limits of mining within the current coal
cial sources required to pay for them. Such mining areas particularly in the Kru~n~ hory
considerations are not premature for longterm piedmont coal basins (see e.g. S~korova et al.
planning. The future price of imported electricity this volume, Bou~ka et al. this volume). The
or fuels should also be considered. The repub- mining areas are delimited, according to law
lic's present trade balance is static and the No. 44/1988 Coll. of the Czech National Council
import of large volume of coal could seriously and in the wording of decree No. 172/92 from
destabilize the situation. Despite the short-term 16 March 1992 of the Czech Board of Mines, by
fluctuations of prices we consider that the risk of the district Boards of Mines. The new mining
a significant rise in price of coal and/or other law under preparation will attempt to reflect this
fossil fuels should not be underestimated. situation. In our view, the situation is paradox-
This reasoning is especially pertinent in the ical, as the Government of the Czech Republic
event of further reductions or a complete shut in order to reduce the negative impacts of coal
down of coal mining in central and western mining on the population and environment, has
Europe, bearing in mind that the present low developed its own decrees on the regional and
wage manpower in South African Republic, ecological limits before making laws. There is no
Ukraine and other countries will not last much doubt that the destruction of tens of commu-
longer. In the case of Ukraine the present nities after 1948, including the ancient town
problems in coal mining may lead to a reduction of Most in northern Bohemia, resulted from
of exported coal, particularly if Ukraine meets originally useful objectives, i.e. making coal
 COAL PRODUCTION IN THE CZECH REPUBLIC 9

reserves available for mining (as we now know, basin in Germany, where more than ten com-
wanton coal mining), but it also essentially munities had to give way to coal mining is not
affected the destiny of thousands of families that different from the CSA mine. Unlike the
had to abandon their homes and native land. common practice introduced in former Czecho-
The current protection of other communities slovakia after 1948, the stoped out workings are
against liquidation unfortunately leads to other immediately restored after abandonment, com-
paradoxes. On the one hand, everyone, particu- pletely new villages are built and the inhabitants
larly the citizens in the North Bohemian basin, of the abandoned communities are offered
are right in calling for improvement of the adequate housing.
environment in the basin area, but on the other
hand, mining for coal with the lowest sulphur
content in the North Bohemian basin at The problem of improvement of
Chaba~ovice has been rather prematurely the environment
reduced. The same aspect applies to the activity
of the 'rescuers' of the Libkovice village, con- Emissions of sulphur and nitrogen oxides that
sidering that it is the underground mines in the often exceed the limits from time to time give
North Bohemian basin which usually extract rise to air conditions approaching smog. This is
essentially better-quality coal than do the open particularly frequent in many of the densely
cast mines (the coals from the former show populated towns where it has caused a reduction
usually lower sulphur and ash contents). in life expectancy and calls for a radical solution
The most controversial decision in this respect that has been the subject of a number of crucial
is the decree No. 441 from 1991 of the Govern- government decrees. It is a very serious problem
ment of the Czech Republic which constrains with political overtones. The measures aimed at
the development of the CSA open cast mine mitigating the negative influences on the envir-
in the North Bohemian basin. This decree onment should take place at two parallel levels.
confines the extraction in this mine to the Whereas some solutions can be put into practice
limits of the so-called first phase of its develop- almost 'from day to day', the second group of
ment. This reduces its reserves to such an extent problems can be solved only within a longer
that extraction will come to an end in 2007. The time interval and at considerably higher costs.
original mining scheme suggested that it would
operate until about 2050, which was projected The medium- to long-term solutions
for the second phase of its development. The
scheme would, nevertheless, entail the destruc- Desulphurization of thermal power plants. Accor-
tion of the villages of Ji~etin and t~ernice. The ding to the agreement on the atmosphere, all
problem of a shorter or longer life for this mine, power plants in the Czech Republic will have to
however, requires that its solution cannot be comply with emission limits that correspond
postponed until the first years of the next to European standards by 1998. Until then, the
century, when a qualified decision could be Czech Energy Company must shut down in
taken based on actual needs. Extraction tech- the thermal power plants obsolete units with a
nology (turning of a face) requires the problem capacity totalling 2280 MW. Until now, 11 units
to be solved before the end of 1996. If the with an output of 1225MW have been shut
Government of the Czech Republic changes its down. In five smaller power plants efficient fluid
earlier decision, not to allow the second phase, bed boilers will be installed, whereas the
after this date the second phase would only be remaining 31, with a total output of 5730 MW,
possible (if at all?) with huge financial losses and will be desulphurized by 1998 (Otava 1994).
with considerable losses in coal recovery. The Installations of desulphurization systems in
fact that the sterilization of these reserves will Czech thermal power stations will require
not only reduce the life of the mine by more than extraction, preparation and transportation of a
40 years, but will also markedly influence that relatively large quantity of limestone (wet lime-
of the whole Basin should also be taken into stone washing), for the treatment. This will have
consideration. a harmful influence on both the environment
We are of the opinion that the problems elsewhere, and also the limestone reserves. It will
associated with destroying the communities were also be necessary to establish a market for the
unnecessarily politicized. None of the large-scale gypsum bi-product generated by the treatment,
open cast mining in densely populated Europe whose annual production will be 5 x 10 6 metric
could have taken place without destroying those tonnes (M. Ku~vart pets. comm.), which is
communities that were in the path of the mine around five times the country's current con-
developments. For instance, the Lower Rhine sumption of gypsum.
10 J. PESEK & M. DOPITA

Fluid combustion of medium- to high-ash coals or N-oxide pollution that causes smog. Never-
high-sulphur coals. Fluid combustion (particu- theless, the problem could be solved by suitable
larly under circulation or under pressure) would legislative measures. The creation of suitable
result in higher efficiency, and the use of reserves reserves of low-sulphur coal at the thermal
of coal with a heating value equal to or greater power stations and urban heating plants would
then 6 MJ kg -1 . These coals have not been con- preclude unforeseen shutdowns of these facilities
sidered for suitable mining due to their low (see above). Alternatively, it might be possible to
quality. This could markedly extend the length substitute high-sulphur lignite by the lower-
of life not only of some of the mines, but of sulphur bituminous coal. This would, however,
whole districts (basins) where these reserves are be possible only after the costly upgrading of
currently not extracted. There would also be an furnaces in the heating plants and power
associated negative impact on the environment stations. This would, nevertheless, bring some
elsewhere resulting from the extraction and trans- benefits. Owing to the higher heating value and
portation of limestone which needs to be mixed lower ash content of the bituminous coal, the
with the high-sulphur coal prior to burning. volume of the combusted bituminous coal would
be lower as would be the volume of ash and/or
clinker. Neither would it be necessary to carry
Use of natural gas in major towns and power out a costly desulphurization of the emissions
stations. A substantial or complete substitu- from medium-size consumers (50 to 300 MW),
tion of coal combustion by gas in the thermal since the sulphur contents in the coals used in
power plants, heating plants and in the domestic power plants usually does not exceed 0.6%
heating in major towns in the Czech Republic
provides a real possibility of reducing harmful
emission in the most exposed regions. This
concept has been both approved and initiated
within an environmental program supported by
Conclusions
6.1 • 109K~ of government finance. It is, how- Public opinion in the Czech Republic, as in most
ever, necessary to bear in mind the long-term developed countries is more and more concerned
dependence on natural gas from Russia with to see a rapid improvement in the environment.
37% of the world gas reserves. The construction This should provide a driving force for change.
of a new gas pipeline through Byelorus and It is clear that many of the current ecological
Poland to western Europe, planned to transport problems are linked with coal mining and the
2-3 • 109m 3 gas to Frankfurt an der Oder by burning of solid fuel. Therefore many countries
1996, confirms a necessary diversification of gas are interested in developing new technologies for
sources as a safeguard against possible changing coal use covered under the heading of clean coal
attitudes in the transit states. It will be necessary technology. Its principal goal is to make the use
to explore the possibility of linking into this gas of coal more environmentally friendly and at the
pipeline, whose capacity, however, is not same time to increase the efficiency of its
planned to increase until long after the year combustion. Several technologies have been
2000. We are not the only ones who take the industrially established, others are being tested.
view that, in the longer term, the prices of In the USA, which has the largest viable
natural gas on the world markets will increase. bituminous coal reserves in the world, a great
If gas subsidies in the Czech Republic are deal of attention is paid to the problems of
completely removed by 1998, it may put a bituminous coal liquefaction and to the produc-
considerable financial strain on consumers. tion of coal bed methane. It has been estimated
Should the prices of gas be higher for small- that about 20 to 25% of coal reserves in the
scale consumers than for large-scale consumers, USA are high sulphur coals (1.5% and more).
as is suggested in some reports, we would In our opinion, coal liquefaction is not an option
consider this approach to be unjustfied. in the Czech Republic in the foreseeable future.
This paper therefore, has concentrated on
several solutions which should be adopted in a
Relatively short-term solutions systematic way. Some of these would lead to
an improvement in the environment and to an
Obligatory preferential supplies to large-scale increase of reserves of a material that might
consumers in major towns and in the North already be exhausted by 2020. As reserves dwindle
Bohemian basin with low-sulphur fuel. In the coal will no longer be the principal source of
immediate future, we will only be able to mon- environmental pollution, but will remain an
itor but not solve the major problem of S- and important raw material for the chemical industry.
 COAL P R O D U C T I O N IN THE CZECH REPUBLIC 11

Everyone of us should bear in m i n d that this will PEgEK,J. & PESKOV~,,J. 1993. Prospects of mining and
be the time of our children's generation. We do decline in coal reserves of the Czech Republic.
not want them to deplore the imprudence of their (In Czech). Uhli-Rudy, 41, 136-138.
parents! But we must not be unrealistic in - - & 1995. Coal production and coal reserves
of the Czech Republic and former Czechoslova-
thinking that whatever our e c o n o m y will need,
kia. In: WHATELEY, M. K. G. & SPEARS, D. A.
can be easily bought or imported. This raw (eds) European Coal Geology. Geological Society,
material (as well as others) will be hard to pay London, Special Publication, 82, 189-194.
for and it will be necessary to create (and finance) - - , DOPITA, M., OPLUSTIL,S., PEgKOV.A,,J., KOULA,J.
the conditions enabling to realize this idea. & ZELENKA,O. 1993. Real volume of coal reserves
to be extracted in operating mines of the Czech
Republic. Part I. Bituminous coal. (In Czech).
References Uhli-Rudy, 41, 307-316.
REICHMANN,F. 1994. Ecology and mining for mineral
FORMANEK,V. 1994. The need for well-advised energy raw materials. (In Czech). Uhli-Rudy-Geologick)
policy in the Czech Republic. (In Czech). Uhli- prdzkum, 1, 414-416.
Rudy-Geologickf~ prdzkum, 1, 405-408. SPOUSTA, Z. 1995. A commentary to the document:
OTAVA, B. 1994. Clear clouds of Po6erady made by "The role of coal industry in energy policy and
CEZ (Czech Energy Company). (In Czech). the role of state in mining". (In Czech). Uhli-
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 Controls on the evolution of the Namurian paralic basin,
Bohemian Massif, Czech Republic
O. K U M P E R A

VSB-Technical University of Ostrava, Institute of Geological Engineering, Ostrava-Poruba,

tK17.listopadu, 708 33, Czech Republic

Abstract. The Namurian A paralic molasse deposits of the Upper Silesian Coal Basin form
erosion remnants of an extensive foreland basin located in the eastern part of the Bohemian
Massif. This basin represents the latest stage of development of the Moravian-Silesian
Paleozoic Basin (Devonian-Westphalian). The paralic molasse stage of the foreland basin
evolved from foreland basins with flysch and with marine molasse. The deposition of the
thick paralic molasse (Ostrava Formation) started in the Namurian A. In comparison with
other coal-bearing foreland basins situated along the Variscan margin in Europe, this is
characterized not only by earlier deposition, but also by a different tectonic setting. It is
located in the Moravian-Silesian branch of the Variscan orocline striking NNE-SSW, i.e.
perpendicularly to the strikes of more western European foreland basins. In the Vis6an and
Namurian, the foreland basin developed rapidly under the influence of the western thrust-
fold belt in the collision zone. The deposition was influenced by contrasting subsidence
activities of the youngest and most external trough - Variscan foredeep - and the platform.
The Upper Silesian Basin shows therefore a distinct W-E lithological and structural polarity
and zonation.

The Upper Silesian Coal Basin (Fig. 1) repre- surroundings of N~m6i6ky in Southern Moravia
sents one of the most important European (Purkyfiovfi 1978). In these boreholes, the coal-
paralic and limnic hard coal basins. The bearing Carboniferous formations were shown
boundaries of the basin are not completely to be below mineable depths with the top of the
known as its coal-bearing sediments are mostly formations being at 2711 m and the base greater
covered with younger sediments and can be seen than 4787m. These data suggest that before
only in small outcrops. The rocks are mainly denudation, the Czech part of the Upper Silesian
known either from deep exploration and/or Basin covered a great area in the south and
structural boreholes or from mines. The total southeast, which was not limited by the Czech
known area of the basin is approximately boundary, and that the erosional remnants of
6500km 2, of which more than two thirds are the coal-bearing Carboniferous formations are
situated in Poland. The Czech part of the basin, preserved in half-grabens south of the zone
the Ostrava-Karvinfi coalfield (Dopita & Kum- of the Sulov faults, buried beneath the nappes of
pera 1993a), is located in the southern parts of the Outer Carpathians.
the basin with a known area of around
2000km 2. However, the actual extent of the
Czech part of the basin is far greater as shown
by prognostic studies (Zeman 1977) and paleo- The paralic molasse (Ostrava Formation -
geographic analyses (Turnau 1962, 1970; Dopita Namurian A) in the framework of the
& Kumpera 1993b). Moravian-Silesian Paleozoie Basin
Coal-beating sediments in the south of the
district were found at mineable depths in deep The molasse formations of the Upper Silesian
boreholes only in the area shown in Fig. 4. Paleozoic Basin form part of the thick Devonian-
According to geophysical data, further south Carboniferous accretionary wedge, which is pre-
they plunge steeply south under the nappes of served as erosional remnants of a large basin
the Outer Carpathians in the zone of the E - W at the eastern margin of the Bohemian Massif
striking Sulov faults, where they have been (Fig. 1).
found in the Jablfinka 1 borehole at a depth of The basin formed as a result of a continental
2985-3870m under the nappes northwest of plate collision at the eastern border of the
Vsetin (Polick~, & Hon6k 1984). The extent of Bohemian Massif from Devonian through
the Upper Carboniferous coal-bearing sediments Westphalian times (Kumpera & Foldyna 1992).
beneath the Carpathians nappes must be even In the collision zone several units of the Czech
greater as proved by deep boreholes in the Massif meet. These units are defined in the

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geologyand Technology,
Geological Society Special Publication No. 125, pp. 13-27.
14 O. KUMPERA

Fig. 1. Schematic geological map of the Moravian-Silesian Paleozoic Basin (compiled after J. Dvo~fik, A. Kotas,
M. Dopita, O. Kumpera, J. Foldyna) 1, Devonian; 2, Permian; 3, plutonic complex of Brunovistulian basement;
4, crystalline complex of Brunovistulian basement; 5, Namurian A-predominantly coal-bearing paralic molasse;
6, Namurian B-Westphalian-predominantely coal-bearing continental molasse; 7, Lower Carboniferous;
8, remnant basin relic; 9, borehole Krfisnfi; 10, locality of Fig. 3.

Report of the Working Group for Regional wedge with a complex composition and struc-
Geological Classification of the Bohemian ture. The preserved filling of the basin represents
Massif at the former Czechoslovak Stratigraphic a rather small erosional remnant of a far larger
Commission (Chulpa6 & Vrfina 1994). In the basinal structure.
west, internal orogenic zones of the Bohemian The Moravian-Silesian Paleozoic Basin under-
Massif are interpreted as the hangingwall to this went a complicated evolution in the course of the
collision zone (Fritz et al. 1993). The eastern collision covering several types of basins (Klein
Cadomian block of the Brunovistulian basement 1987). These are described by Kumpera (1983),
formed the footwall which gradually disinte- Hladil (1988), Dopita & Kumpera (1993a), and
grated and subsided (Kumpera 1988) during an Kumpera & Martinec (1995). Carboniferous
oblique collision (Grygar 1992). The deeply foreland basins with molasse represent develop-
eroded roots of the collision suture are located ment during the latest stage of oblique collision.
in the Silesian and Lugian units in the north and
in the Moravian and Moldanubian units in the
south. The collision of the two plates of a Partial troughs within the
contrasting crustal character resulted in a rapid Moravian-Silesian Paleozoic Basin
uplift in the central parts of the Bohemian
Massif and the formation and evolution of The basin depocentre migrated from the colli-
subsiding and migrating foreland basins, the sion zone towards the foreland (Kumpera 1971;
final basin being located on Brunovistulian Dvo~fik 1973). The sedimentary wedge mainly
basement (Fig. 2). This consequently led to the consists of siliciclastic flysch and molasse sedi-
development of a thick sedimentary accretionary ments (a smaller part belongs to platform
 NAMURIAN PARALIC MOLASSE IN BOHEMIAN MASSIF 15

Fig. 2. Schematic conception of the partial flysch troughs and molasse fordeep and of the surrounding source
areas in the Moravian-Silesian Paleozoic Basin during the Late Vis6an and Namurian A stages of development.
Two of the troughs and depressions are in Fig. 3.

carbonates and rift d e p o s i t s - K u m p e r a & and forebulges of different ages are well
Martinec 1995). The total thickness of the documented in the eastern part of the Paleozoic
Carboniferous sedimentary wedge (after com- basin (Fig. 3). In the western trough (eastern
paction) is more than 12km, although, due to flysch basin in Fig. 3), the thickness of Upper
the prograding wedge, this is never developed in Vis6an flysch is reduced from 2500m in the
one location. The average rate of sedimentation western part to 100m, or less, in the eastern
is therefore about 270 m Ma -1 . The accretionary part. In the eastern elevation, stratigraphic gaps
wedge has its greatest thicknesses in the west, in at different Vis6an levels have been even
the vicinity of a broad collision zone, and above observed. The eastern trough is filled with
all in the northwest. The preserved maximum thick uppermost Vis6an and Upper Carbonifer-
thickness is about 6 km, whereas the total thick- ous molasse deposits.
ness decreases gradually to 200 m in the extreme
eastern parts of the basin. The decrease is not
continuous, but the thickness distribution varies The Variscan foredeep and platform in
within narrow partial troughs and forebulges the development of the Upper Silesian
(Figs 2 & 3) which developed during the Coal Basin
Carboniferous (Kumpera 1983). Some of these
troughs and elevations have been proved con- The initial ideas of uniform geotectonic develop-
elusively by isopach studies. Two partial basins ment of the Upper Silesian Basin have been

w E
FORELAND BASIN PLATFORM
1 EASTERNFLYSCH FOREDEEP FOREBULGE I "
BASIN Orlov~
Budi~ov Odry-Hranice Vala~sk~ Mezi~I~f s t r u c t u r e Fren~t~t p. Radh.
0 .... .'. ..... ; ...... , ._.; .. ; i , ]

I " i - . 9~ am
" ur A
9. . . . . . , . ~-.~--

9 ,..~r ~ ~

I 2 3 4 5

Fig. 3. Palinspastic cross section showing the thickness of stratigraphic units at the transition from the foreland
basin with flysch to the foreland basin with molasse in the Moravian-Silesian Paleozoic Basin during Late Visban
(Goa-~) and Namurian A. l, carbonates; 2, predominantly shaly deposits; 3, predominantly graywackes;
4, conglomerates; 5, coal-bearing paralic molasse.
16 O. KUMPERA

modified in terms of a polytype basin (Havlena contrasting subsidence rates of the foredeep and
1982) as a result of deep exploration boreholes. the platform (Fig. 4). Thus the foredeep is
The first boreholes sunk in the southern and characterized by a full subsidence compensation
southeastern parts of the basin within the coal- and the platform by a retarded subsidence.
bearing Carboniferous showed considerable
differences between the area of active mining
in the north and areas under exploration in The main lateral changes in the iithological
the south. With continual exploration, it has
development of the Namurian paralic
been determined that thicknesses of parts of
the Carboniferous sequence diminish towards the molasse (Ostrava Formation)
east and southeast. In addition, their coal See Table 1 of Dvo~ik et al. this volume, for the
capacity and the thickness and number of seams stratigraphic classification of the mollasse-filled
also decrease.
foreland basin.
Extensive borehole exploration throughout
the area of the basin together with new data
from the deeper levels of the mines has proved
that in the course of the Carboniferous devel- Thickness of the Ostrava Formation
opment, the coal basin was divided into two First of all, the foredeep and the platform differ
parts with distinct developments and structures in the thickness of the paralic molasse. In the
(Fig. 3): foredeep, the thickness of the Ostrava Forma-
9 The younger Variscan foredeep, represented tion reaches up to 3200 m and decreases to about
by a narrow mobile zone along the western 100m or less in the platform forebulge (in the
margin of the basin. vicinity of the Kop~ivnice-T~inec anticlinorium).
9 The Upper Silesian stable block, an extensive These changes are well illustrated on isopach
platform in the eastern part of the basin. maps of the total thicknesses of individual litho-
stratigraphic units of the Ostrava Formation,
This division is only apparent in the Upper namely the Pet~kovice and Jaklovec Members
Vis~an and Upper Carboniferous levels of the (Figs 5 & 6). All members show maximum thick-
basin. During the Devonian and the earliest nesses in the foredeep (especially in the north), but
Carboniferous, the whole preserved part of the thicknesses decrease to the east, particularly the
basin was a platform. Thus, the Devonian and southeast, in the area of the forebulge. This
Lower Carboniferous carbonates have a similar contrast in thickness gradually diminishes in
thickness throughout the basin (up to 700 m in successively younger stratigraphic units, from
the south and up to 1100m in the northern parts the oldest (Peffkovice Member) to the youngest
of the basin in Poland). By Early Vis~an time, fully preserved unit (Jaklovec Member). The
Variscan deformation had reached the eastern youngest unit of the Ostrava F o r m a t i o n -
boundary of the basin. It is only the Upper Poruba Member - has not been studied because
Vis6an formations that are largely of a clastic the upper part of the member is nowhere
character. Their thickness reaches 1000-1500 m preserved.
in the foredeep but eastwards, towards the Estimates of sediment accumulation rates
platform, decreases to 100m (in the Krfisn~, 1 across the whole basin vary from 250-
borehole- Roth 1979). Correlated stratigraphi- 350 m Ma -1 in the Late Vis6an flysch depression,
cal units of the molasse vary considerably in through a surprisingly high 9 0 0 m M a -1 in the
thickness across the basin. The foredeep is filled foredeep during Namurian A, to zero in the
with marine and paralic molasse sediments, platform forebulge.
whose compacted thickness is up to 4500m
(before compaction, the thickness may have
reached more than 6000m) in the depocentre, Lateral changes in coal accumulation
whereas it decreases to 200m or less over the
easternmost platform forebulge. The foredeep and the platform differ not only in
In addition to variations in thickness, the the thickness of the paralic molasse, but also
foredeep and platform differ markedly, espe- in the number and thickness of coal seams
cially in the development of the paralic molasse developed. Coal accumulation decreases mark-
(Ostrava Formation - lower Namurian - Ez edly towards the platform (Dopita & Kumpera
zone). The main feature of the coal-bearing 1993b). The Ostrava Formation contains more
paralic molasse deposition was that subsidence than 170 coal seams with an average thickness
was compensated by clastic supply. Neverthe- of 73 cm in the foredeep, whereas the number of
less, the sedimentation was influenced by the coal seams in the same stratigraphic interval
 N A M U R I A N PARALIC MOLASSE IN BOHEMIAN MASSIF 17

OL4N b

" " -lZ N

/ \
,~,j-,-,.,--~.,~ I, - - . . .
| ~J ,"
.9 ZN ..."~
1
"-. ..... o-'*

7n j" ~ FB
a b c
"- .'7'.

L. "1."
~ 5 .....
!--- ~ .No. / ~,

o,, ". :.'| - ,. 9

:'".. '.. / - .L!.."| , > 10
i,!
-
7 "
>
>" 11

| 12
13
-@ \~,--~ os- 14
i C~F'~,-r I~ 0 50km
L ~

Fig. 4. Outline of the early Namurian palaeogeography in the Czech part of the Upper Silesian Coal Basin.
1, paralic molasse in known regions (with compensated subsidence); 2, postulated pre-erosional extent of paralic
molasse; 3, paralic molasse in regions with retarded subsidence; 4, source areas (a-lowlands, b-hills, c-mountains),
ZN-prograding thrust zones; 5, present erosional limits of the known basinal regions; 6, postulated original limits
of the basin; 7, depocentre axis; 8, postulated forebulges; 9, directions of marine trangressions; 10, directions of
clastic transport; 11, rivers and deltas; 12, humid climate; 13, postulated volcanic centres; 14, state boundaries,
FB-postulated forebulge.

decreases to 40, or even 20, in the platform, platform diminishes towards the younger strati-
where some parts of the Ostrava Formation are graphic units, particularly in the southern areas,
even non-productive. This is illustrated in the where an extensive platform forebulge was
maps of total coal accumulation of the Pettko- gradually uplifted in the vicinity of the present
vice Member (Fig. 7) and the Jaklovec Member Koptivnice-Ttinec anticlinorium.
(Fig. 8) with maximum values in the foredeep
and minimum values in the vicinity of the
platform forebulge. These maps show the
division of the basin into sub-areas, where Lateral changes in the distribution of
subsidence was more or less compensated by other lithotypes
sedimentation. Spatial variations in coal accu-
mulation in the sub-areas are thought to have Simultaneous changes in the number, thickness
been controlled by the interplay between tec- and character of various correlatable strati-
tonics and clastic supply. The isopach maps graphic units can be observed between the
suggest a slight shift of the maximum coal foredeep and platform. Up to 80 marine and
accumulation eastwards with the younger units, brackish bands, representing marine transgres-
probably due to an eastward migration of the sions, have been recorded altogether in the
depocentre. As with total sediment thickness, northern part of the foredeep (Reho~ &
the contrast between the foredeep and the l~eho~ov~ 1972) These show progressively less
18 O. K U M P E R A

2F-
, !

0I, 1(2 20
,,I
km

Fig. 5. Isopach map of the Pet~kovice Member (lower part of the Ostrava Formation, Czech part of the Upper
Silesian Coal Basin). 1, present limits of the basin; 2, limit of the Frengt~tt relic of the Karvinfi Formation; 3,
isopach in metres.

marine influence or disappear towards the plat- conditions transgressed from north to south
form so that only the four most important, thick and west to east through the foredeep and, from
bands are present in the eastern part of the time to time, even reached the area of the Upper
platform. The thickness of those bands with the Silesian platform block. The foredeep, in which
most stable areal distribution is up to 180 m in each marine transgression resulted in at least
the foredeep but is markedly reduced towards 22m of accumulated clastic sediments, repre-
the platform. The faunal content changes sents an area regularly flooded by the sea,
significantly also from north to south in the whereas the platform was an area only some-
area of the foredeep. Towards the south, times flooded (Havlena 1982). In addition,
elements of a brackish fauna, or even a fresh- volcanoclastic rocks present in the f o r e d e e p -
water fauna, occur more often at the expense of altered tuffites in terrigenous siliclastic sedi-
elements of a marine fauna in a considerable ments, kaolinite tonsteins in coal seams (up to
number of marine bands (l~eho~ & l~eho~ovfi 16 beds in the f o r e d e e p - Dopita & Krfilik
1972). These changes are even more marked in a 1977), and kaolinized tuffites redeposited as
W - E direction. This indicates that marine 'whetstone' rocks (30 beds in the western part)
 NAMURIAN PARALIC MOLASSE IN BOHEMIAN MASSIF 19

Q -,
10
i
20 km

Fig. 6. Isopach map of the Jaklovec Member (Upper part of the Ostrava Formation, Czech part of the Upper
Silesian Coal Basin). For 1-3, see Fig. 5.

disappear towards the platform. This can be local variations in the thickness of the Main
seen in the isopach map (Fig. 9) of the s.c. Main Whetstone that probably represent a combina-
Ostrava Whetstone, which forms an important tion of subsidence and fluvial control. Volcanic
marker bed in the lower part of the Ostrava For- material was largely redeposited into the fore-
mation over large areas of the basin. Figure 9 deep from the platform by complex sedimentary
shows a decrease in its thickness from 12m in processes. A map of composite thickness of all
the west to 0 m in the east. It also shows marked the volcanogenic beds in the Ostrava Formation
20 O. KUMPERA

?'g'l

-/
/

0 z9

Fig. 7. Total coal accumulation map of the Pet~kovice Member (lower part of the Ostrava Formation, Czech part
of the Upper Silesian Coal Basin). For 1-3 see Fig. 5.

(not shown), shows a similar pattern. It must be A similar pattern of the main trends in the
stressed that some of these beds have an areal development of the basin is given by the
extent ranging from 102-103 km 2. The thickness distribution of coalification intensity (Adamu-
of individual cyclothems, the grain size and the sovfi et al. 1992). The more modern methods of
number of sandstone and conglomerate layers coal quality determination have not been suffi-
increase towards the southeastern part of the ciently and equally applied to the whole area of
platform indicating a source area in the vicinity the Czech part of the Upper Silesian Coal Basin
of the Kop~ivnice-T~inec anticlinorium - Fig. 10 so that the degree of coalification has been
(Jansa 1967). characterized by volatile matter V aaf. The map
 N A M U R I A N PARALIC MOLASSE IN BOHEMIAN MASSIF 21

2#";71
F"-t
I
//

/ I ,o
,o i 1

0 10 20kin

Fig. 8. Total coal accumulation map of Jaklovec Member (Upper part of the Ostrava Formation, Czech part of
the Upper Silesian Coal Basin). For 1-3 see Fig. 5.

of coalification of the upper surface of the lowest V daf values in the area of the Upper
Ostrava Formation again illustrates the basic Silesian platform are only 20% and the maxi-
difference between the area of the Variscan mum is more than 35% V daf in the youngest part
foredeep and the Upper Silesian platform. In the of the paralic molasse sequence.
area of the Variscan foredeep on its west margin, Generally, the degree of coalification is con-
the V daf values fall to less than 10~ whereas the trolled by stratigraphy; the coalification is lower
22 O. KUMPERA

,t _l

0.I__
10
i.,
2,0kin
Fig. 9. Isopach map of the Main Ostrava whetstone horizon (lower part of the Ostrava Formation, Czech part of
the Upper Silesian Coal Basin),For 1-3 see Fig. 5.

in the younger members of the formation. of coalification occurs in the Namurian A in

However, at the same time, the intensity of South Moravia (up to 40.9% Vaaf). Doubtless,
coalification depends on the thickness of the this is connected with a generally low subsidence
basin fill in any region. At comparable strati- rate in the southern areas of the Moravian-
graphic levels, the degree of coalification in Silesian Paleozoic Basin.
the Upper Silesian platform is lower than that By contrast, the highest degree of coalification
in the Variscan foredeep. The lowermost degree in the western part of the foredeep is probably
 NAMURIAN PARALIC MOLASSE IN BOHEMIAN MASSIF 23

4r,-

I--3 1
2 P _z, l

-,

L..._./

0 10 20 km
I I ,.J

Fig. 10. Isolines of sandstone index in the Jaklovec Member (Upper part of the Ostrava Formation, Czech part of
the Upper Silesian Coal Basin).l, limits of the basin; 2, limits of the Fren~tfit relic of the Karvinfi Formation;
3, sandstone index (%).

partly a result of the deepest burial of coal- Structural zonation

bearing strata during the coalification processes,
and partly due to the greatest heat flow at the The Upper Silesian Basin is stratigraphically
Variscan front in the west of the basin. This is and paleogeographically (e.g. Havlena 1982) as
in good agreement with the results from well as geotectonically and structurally (Kum-
the whole Moravian-Silesian Paleozoic Basin pera 1971, 1980; Kotas 1985) asymmetric. The
(Sko6ek 1976). main manifestation of tectonic asymmetry in a
24 O. KUMPERA

W - E direction is the greater intensity of folding thickness of a member with the maximum
and the development of more complex structures number of marine occurrences documented by
in the western part of the basin. In the eastern bands in that member with a marine or brackish
part of the basin within the area of the Upper fauna, the frequency of marine influence can be
Silesian platform, the prevailing structures quantified. The greatest effects occur in the
are taphrogenic. Structural asymmetry parallel Peffkovice Member (1 transgression per 22m
to the Variscan orogenic trend is expressed thickness of sediments). Lesser effects are
in somewhat more complicated tectonic styles in recorded in the Hru~ov and Poruba Members
northern areas. Thus, the regional tectonic (1 transgression per 94 m and 49 m of sediments,
scheme, like the other features described above, respectively). These data indicate that although
prove a generally greater mobility of the basin in considerable variations in subsidence rate
the west and in the north. occurred (as shown by the thick nonproductive
A detailed analysis of basinal tectonic struc- sequences with a prevailing marine influence
tures indicates the presence of structural zonality upon the megacycle boundaries), the rate of
within the foredeep area. Here, parallel to the subsidence gradually decreased.
axis of the foredeeep, narrow zones trending in a
NNE-SSW direction and characterized by
unusual fold-fault structures are present. Thus, Periodical variation between marine molasse
it is possible to delineate a zone containing a and paralic molasse
holomorphic style of folding along the western
margins of the basin. To the east, this zone is Thick and laterally extensive marine units occur,
fringed by the zone of western brachystructures. widely separated by 300 to 500 m thick sequences
After that, the area of idiomorphic (ejective) of paralic molasse containing great coal accu-
folds follows, within which the parallel narrow mulations. The most important are the marine
zones of the Mich~ilkovice-Rybnik and Orlovfi- bands associated with the seams Naneta, Fran-
Bohugovice anticlinal fold-fault structures are ti~ka, Enna, Barbora, Roemer and Gaebler.
developed. Between these two anticline-fault These marine bands have a rather constant
structures, the zone of eastern brachystructures faunal content over the whole Czech part of the
is located. The tectonic zones are characterized basin and have a considerable thickness up to
by specific fold-fault structures (Foldyna & 180 m. Periods of extensive marine flooding are
Kumpera 1991). associated with considerable falls in coal accu-
mulation or even in the development of barren
measures (Dopita & Havlena 1980). Closely
associated with the most stable faunal bands in
The main vertical changes in the development the Ostrava Formation are nonproductive or
of the paralic molasse (Ostrava Formation) only weakly coal-bearing sequences, whose thick-
ness varies between 100-240m. They divide the
Vertical changes in some lithological parameters
richly coal-bearing sequences of the Ostrava
point to important processes in the development
Formation. The lithological nature and mainly
of the basin as well as to the changing basinal
a marine origin of nonproductive parts of
regime.
the sequence indicate periods, when subsidence
remained uncompensated over almost the whole
of the Czech part of the basin.
The abundance of marine facies Thus the Ostrava Formation can be classified
Marine conditions greatly influenced the sedi- as a polyfacial sequence, in which the prevailing
mentation of the lower part of the Ostrava paralic molasse was several times interrupted by
Formation but became less significant upwards. the development of marine molasse. The marine
This can be demonstrated by the number of molasse was formed, in contrast to the paralic
marine units in successive members of the molasse, during periods of uncompensated sub-
Ostrava Formation. In the Pet~kovice Member, sidence. This suggest changes in subsidence rates
up to 32 bands with marine or brackish faunas and tectonic activity both within the basin and in
are known, in the Hrugov Member 26 and in the the source area.
Jaklovec Member, marine or Lingula-bearing
bands are represented only by the Susta marine Changes in volcanic activity
band and the Barbora group of 4 bands. Marine
influence increased again in the Poruba Member, The layers of volcanogenic sediments reflect
where up to 20 bands (Reho~ & l~eho~ov~ 1972) intensive volcanic activity in volcanic centres,
have been found. By comparing the maximum which have yet to be identified in detail, although
 NAMURIAN PARALIC MOLASSE IN BOHEMIAN MASSIF 25

they are probably in the western source area. The glacio-eustatic changes of the sea level as well as
most important is the Ostrava Whetstone, whose to climatic oscillations during the Late Carboni-
thickness is up to 12 m, and which is developed ferous. They can be correlated with the meso-
over almost the whole area of the Czech part of thems described by Ramsbottom (1979) from
the basin with the exception of the easternmost northwestern Europe (Sko6ek 1991). A shortage
areas. Another important unit is the strati- of radiometric age data makes it difficult to
graphically lower whetstone of the Leonard interpret the influence of climatic changes on
seam. The early Namurian A was the most sedimentation in the Carboniferous of the
volcanically active period in the near source area, Upper Silesian Basin. However, it would
producing frequent and thick layers of whetstone expected that these changes could contribute to
in the paralic basin. Later, the volcanic activity lithological changes in cyclothems, or they could
waned and mostly only produced layers of be reflected in marine transgressions which
tonstein in the swamps and peat moors which might result in a complex interplay with
were quiet sedimentary environments protected tectonics.
from resedimentation. Thin pyroclastic layers
falling into a high energy environment would
have been kaolinized and dispersed amongst Some paleogeographic features of the basin
clastic materials. Nevertheless, in the lower
Namurian A sequence up to 46 units of As with the earlier stages of the development of
volcanogenic sediments have been preserved at the Moravian-Silesian Basin, the Namurian A
various stratigraphic levels. Their maximum total paralic molasse basin developed on continental
thickness is 16 m indicating that the Namurian A crust in the foreland under a compressional
represents a period of strong and frequent regime. Therefore, the basin was filled by
volcanic activity in the Variscides of Central erosion of rocks of the overthrust lithospheric
Europe. The diminution in the total thickness of plate both in the inner parts of the Bohemian
volcanogenic sediments to the east suggests their Massif and in the foreland thrust zone. This
redeposition from the platform to the foredeep. latter consisted of the waning collision zone and
also the western areas of the Paleozoic rocks in
the Moravian-Silesian Basin, which were, pro-
Changes in the petrographic and gressively, included into the thrust-fold zone.
geochemical composition Also sedimentation in the paralic molasse took
place partly at the expense of synsedimentary
Changes can also be observed in the petro- uplift within the platform foreland. Active tec-
graphic composition of psammites through the tonic development both in the source area and in
stratigraphic sequence. Among them, graywacke the area of the basin itself, resulted in a
sandstones prevail. In the upper part of the significant resedimentation of elastics connected
paralic molasse, the number of graywacke with the processes of basinal cannibalism (Kum-
layers, arkosic sandstones and arkoses increase pera & Martinec 1994).
(Fialovfi et al. 1978). This relates to important The Czech part of the Upper Silesian Basin
changes in the source area. Whereas in the lower that is preserved today, represents an erosional
part of the Ostrava Formation, the major source remnant of the former basinal structure that was
lay in the western orogenic area together with originally substantially larger than today. The
resedimentation of older Carboniferous clastics; western part of the basin-fill had been already
in the upper part, the influence of the eastern eroded by the end of the development of the
source area of the stable Upper Silesian block Variscan fold-thrust structure and the uplifts of
(e.g. from the area of the forebulge) gradually the Rheno-Hercynian and Sub-Variscan zones.
manifested itself. This is also indicated by the The axis of the maximum compensated sub-
geochemistry of some claystones suggesting an sidence is thought to be situated to the west of
increasing supply from morphologically flatter the existing erosional western boundary of the
source areas which were exposed to long-term basin. This axis plunged to the north. Towards
chemical weathering. the western margin of the basin, all indications
of mobility become more marked: thicknesses of
stratigraphic units (Figs 5 & 6), coal accumu-
The influence of eustatic movements lation (Figs 6 & 7), degree of coalification,
upon sedimentation thickness and number of faunal bands, etc. Along
its western boundary, the basin is amputated by
Some major changes in the lithology of the tectonics and erosion. It can be assumed that
Namurian paralic sequence can be related to within the early Namurian, the basin extended
26 O. KUMPERA

along the whole eastern margin of the Bohemian onto the forebulge; (b) the development of
Massif (Fig. 4). The original southern margin of marine bands and the degree of marine influence
the basin is not known, but on the evidence from diminish, indicating marine transgression
deep boreholes located at Nrm~i~ky (Dvo~fik towards the south and east; (c) the thickness of
et al. 1997) as well as an analysis of the tectonic volcanogenic coal tonsteins and whetstones-
position, it is probable that the basin extended both show a decrease in thickness towards the
originally as far as the Austrian border, where its forebulge; (d) the development of individual
remnants are still preserved. Likewise, it is cyclothems, showing a general increase in both
possible that the coal-bearing deposits covered grainsize and number of sandstone and con-
a considerable area to the southeast and east glomerate beds towards the forebulge indicating
beneath rocks of the Styrian (Carpathian) a source area in the southeast; (e) degree of
nappes (Dopita & Kumpera 1993b). coalification, which decreases at any one strati-
As described above various source areas can graphic level from west to east and southeast,
be postulated for the basin fill. The western attributable to a combination of shallower
source area comprised both the areas formed by burial and lower heatflow in the stable area of
the crystalline complex and cover sediments. The the forebulge; and (f) intensity of fold/fault
geological composition of the denuded surface structure with a generally asymmetric pattern
changed in the course of sedimentation during developed, verging to the east.
the Namurian A. A great amount of arkosic 4. Vertical changes in the sediment fill of the
sandstones and arkoses in psammites in the foreland basin reflect a diminishing tectonic
upper part of the Ostrava Formation and a source from the Variscan hinterland in the
considerable content of K feldspars indicate that west. These are documented as: (a) diminution
the level of erosion had cut down into the larger in the number of marine occurrences upwards,
granitoid bodies. During the later Namurian A indicating a decreasing subsidence rate with
eastern source areas joined those in the west. time; (b) common interruptions of marine
In contrast to the orogenic western source, these conditions by coal-rich parallic molasse suggest-
less extensive source areas were intraplatform ing intermittently changing subsidence rates and
elevations in the foreland. Their intermittent tectonic activity in the source areas; (c) decrease
influence was first seen in the sedimentation of in total thickness of volcanogenic ash, suggest-
the Hru~ov Member by the Kopfivnice-Tfinec ing a waning volcanic activity in the mountain
uplift. In the later Namurian A low elevations belt from Namurian A times; and (d) changing
within the platform areas sourced short streams geochemistry of claystones, indicating a gradual
that fed the more eastern part of the basin. lowering of relief in the source area.
The relief of source areas became gradually
less and less flat and produced more chemically Professor Kumpera died before corrections to the
mature solid products of weathering (Kumpera manuscript had been completed. Final corrections
& Martinec 1993). were made by the editors

Conclusions References
1. The Visran Upper Carboniferous coal- ADAMUSOVA, M., DOPITA, M., FOLDYNA, J., KALEN-
bearing molasse of the Upper Silesian Coal Basin DOVA, J., KUMPERA, O. (~ STRAKOS, Z. 1992.
represents the latest and most eastward devel- The isopachous and coalification maps of
coal-bearing molasses in the Czechoslovak part of
opment of a Variscan foreland basin, formed the Upper Silesian black coal basin. Sbor. Vdd.
as a result of oblique continental collision in Praci Vys. Sk. Bdfi, Ostrava, 28, 1~. HG. (1),
the west. 27-38.
2. The molasse-filled foreland basin is divided CrtLUPA~, I. & VRANA, S. (eds) 1994. Regional
into a western foredeep with up to 4.5km of Geological Subdivision of the Bohemian Massif
sediment and an eastern platform (forebulge) on the Territory of the Czech Republic. Journal of
with less than 200m of sediment. Decreasing the Czech Geological Society, 39, 127-144.
thickness from foredeep to forebulge is recorded DOPITA, M. & HAVLENA, V. 1980. Geology and mining
for each of the stratigraphic units but younger in the Ostrava-Karvin6 Coalfield. OKD, Ostrava.
-- & KRALiK, J. 1977. Coal tonsteins in Ostrava-
units show less marked thickness changes.
Karvin6 Coal Basin. OKD, Ostrava, 1-213.
3. Contrasts between foredeep and forebulge - - & KUMPERA,O. 1993a. Geology of the Ostrava-
are documented in: (a) coal accumulation- Karvinfi coalfield, Upper Silesian Basin, Czech
both the number of coal seams and the total coal Republic, and its influence on mining. Interna-
thickness diminish towards the east and south tional Journal of Coal Geology, 23, 291-321.
 N A M U R I A N P A R A L I C MOLASSE IN B O H E M I A N MASSIF 27

& - - 1 9 9 3 b . Contribution to the Paleogeo- --, 1988. Brunovistulicum in Variscan development

graphy of Namurian A in the Bohemian Massif (in Czech). Acta Univ. Carolinae, Geol. Praha,
(Czech). Sbor. v6d. Praci Vys. Sk. bfin, Ostrava, 401-410.
39, R. HG, 1104, 41-51. - - & FOLDYNA,J. 1992. Development of Moravian-
Dvo0akK, J. 1973. Synsedimentary tectonics of the Silesian Paleozoic Basin. Sbor. Vdd. pracl, Vys.
Palaeozoic of the Drahany Upland (Sudeticum, Sk. b6~. Ostrava, I~. HG, 38.
Moravia, Czechoslovakia). Tectonophysics, 17, -- & MARTINEC, P. 1993. V~voj sedimentfi kar-
359-391. bonsk6ho akre6niho klinu moravskoslezsk6
--, HONEK, J., PESEK, J. & VALTEROVA, P. 1997. pfinve. Sbor. 1. desko-polskO konf. o sedimentol.
Deep borehole evidence for a southward exten- karbonu, UG Ak. Vfid CR, Ostrava, 125-166.
sion of the Early Namurian deposits near & 1994. The development of the Carbonifer-
Nemcicky, S. Moravia, Czech Republic: implica- ous accretionary wedge in the Moravian-Silesian
tion for rapid coalifaction. This volume. Paleozoic Basin. Journal of the Czech Geological
FIALOVA, V., POLICK~(, J. & HONI~K, J. 1978. Society, 39, 1, 63-64.
Petrography and lithology of the Jaklovec POLICK~/, J. & HONI~K,P. 1984. Produktivni karbon ve
Member (in Czech.). Ostrava, Sbor. GPO, 16, vrtu Jablfinka 1. Gas. Mineral. Geol., Praha, 29, 4,
5-38. 445.
FOLDYNA, J. & KUMPERA, O. 1991. Tectonic zones PURKYlqOVA, M. 1978. Fl6ra svrchniho karbonu
and areas in Subvariscan Zone of the Bohemian (namuru A) v paleozoiku JV svahfi Cesk6ho
Massif (Upper Silesian Basin). Acta Univers. masivu u N6m6i6ek na ji~ni Morav~. Gas. Slez.
Carol. Kettner, Praha, 3-4, 165-281. Muzea, Opava, A 27.
FRITZ, H., DALLMEYER, R. D., NEUBAUER, F. & RAMSHOTTOM, W. H. C. 1979. Rates of transgression
URBAN, M. 1993. Thick-skinned versus thin- and regression in the Carboniferous of NW
skinned thrusting: Mechanism for the formation Europe. Journal of the Geological Society,
of inverted metamorphic section in the SE London, 136, 147-153.
Bohemian Massif. Journal of the Czech Geological ROTH, Z. 1979. The Krfisn~i 1 borehole in the central
Society 38, 33-34. part of the Moravskoslezske6 Beskydy Moun-
GRYGAR, R. 1992. Kinematics of Lugosilesian orocline tains. Vdst. (Jstf . (lst. geol. Praha, 55, 2, 75-83.
accretion wedge in relation to the Brunovistulian ]~EHOI~, F. & I~EHOI~VA, M. 1972. Makrofauna
foreland. Sbor. Vdd. Praci Vys. Sk. bdd, Ostrava, uhlonosn~ho karbonu deskoslovenskd (6sti horno-
I~. HG, 38, 1, 49-72. slezsk~ phnve, Ostrava, Profil.
HAVLENA, V. 1982. The Namurian deposits of the SKO~EK, V. 1975. Regional and geological interpreta-
Upper Silesian Coal Basin. Rozpr. Cs. Akad. tion of organic matter coalification in the late
V(d., R. mat. p(ir. vdd, 92, 7, 1-79. Palaeozoic sediments of the Bohemian Massif.
HLADIL, J. 1988. Zonality in the Devonian carbonate Vdst. (Jst(. Ust. geol. Praha, 51, l, 13-25.
sediments in Moravia (CSFR). Proc. 1st Int. 1991. Indications of the Late Carboniferous
Conf. Bohemian Massif, Praha, 121-126. eustatic and climatic oscillations in the Upper
JANSA, L. F. 1967. Sedimentological evolution of Silesian Basin. Vdst. (lst(. tQst. geol. Praha, 66, 2,
Carboniferous strata in southern part of Upper 85-96.
Silesian Coal Basin. PhD Thesis, Charles Uni- TURNAU, E. 1962. The Age of Coal Fragments from the
versity, Praha, MS, (in Czech). Cretaceous Deposits in the Outer Carpathians,
KLEIN, G. DE V. 1987. Current aspects of basin Determined on Microspores. Bull. Acad. Polonaise
analysis. Sedimentary Geology, 50, 95-118. Sci. Krak6w, gOol.-g~ogr., 10, 2, 85-89.
KOTAS, A. 1985. Structural Evolution of the Upper 1970. Mikroflora i paleogeografia karbonu pro-
Silesian Coal Basin (Poland). C. R. 10. Congr. Int. duktywnego v polskiej czesci Karpat. Biul. Ins.
Strat. Geol. Carb., Madrid, 3, 459-469. geol., Warszawa, 235, 13, 163-229.
KUMPERA, O. 1983. Lower Carboniferous geology of ZEMAN, J. 1977. Progn6za roz~i~eni uhlonosnOho
Jesenlky Block (in Czech). Knih Ust[. Ust. geol. karbonu pod vn6jgim flygem Z/tpadnich Karpat.
59, Praha. Geol. Prdzk., Praha, 19, 12, 353-357.
 The origin of magnetic remanence components of Westphalian C
to Stephanian C sediments, West Bohemia:
a record of waning Variscan tectonism
M I R O S L A V K R S ~, JIt~I P E S E K 2, P E T R P R U N E R ~, V L A D I M [ R SKO(~EK 2
& JANA SLEPICKOVA 2

1 Geological Institute, Academy of Sciences of the Czech Republic, Rozvojov6 135,

165 O0 Prague 6, Czech Republic
2 Faculty o f Sciences, Charles University, Albertov 6, 128 43 Prague 2, Czech Republic

Abstract. Petromagnetic and magnetomineralogical investigations of Westphalian C to

Stephanian C rocks from the Central and Western Bohemian Late Palaeozoic Basins were
undertaken to determine the origin of magnetic remanence components and of ferrimagnetic
minerals - carriers of respective remanence components in a variety of rock types including
tufts, tuffites, siltstones, sandstones, grey and red claystones. Multi-component analysis
allowed the separation of remanence components and a selection of petromagnetic and/or
magnetomineralogical methods were used to determine the ferrimagnetic minerals.
Magnetite was found to be the principal carrier of Variscan remanence components in
most non-red-coloured rocks and haematite in red claystones originated during diagenesis in
the Carboniferous period. In several samples, haematite, goethite and other Fe-oxides were
found to result from recent weathering. In some samples, the Variscan remanence
components were separated at relatively low temperatures, from about 150 ~ onwards.
Variscan virtual pole positions have been derived from relatively small sets of samples.
Nevertheless, they show that the rocks of the Westphalian C and D ages were more
intensively deformed than those of the Stephanian, agreeing with an overall decrease in
intensity of deformation in the final stages of the Variscan orogeny.

This paper aims to establish a geological- components. Distinguishing epigenetic rema-

historical succession for the generation of the nence components from those of a syngenetic
remanence components in Carboniferous rocks origin on the basis of a multi-component analysis
of the Late Palaeozoic Basins in Central is possible only where these components mutually
and Western Bohemia and to determine the differ in direction. A Variscan overprint took
minerals - carriers of their respective remanence place in the Bohemian Massif in the Latest

Table 1. Units of Central and Western Bohemian Late Paleozoic Basins

Age Formation Member

C Lin6

Otruby

B Slan~, Malesice

Stephanian Jelenice
Carboniferous , ,

A? T~nec

Cantabrian
o 9 e e . ~ 9 o t 9 9 . e n 9 o e 9 9 ,, . 9 9 9 o : N2;'~any
D Kladno
Westphalian
C Radnice

(1) Double line indicates gap in sedimentation

From Gayer, R. & Pegek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 29-47.
30 M. K R S E T AL.

k~

0 < <

k~

0or
-H -H -H -H-H
c--I
rm

oo c~
Cq
-H~ -H -H -H-H
O ~ ~'h r C',l
r r r c'-I r
0

I-~ ko

oo o o~ o~ o~ o~

r162

,.el . o.
o
-8

.,..~ 0 O0 0 0 0

o
 MAGNETIC REMANENCE COMPONENTS 31

r~

op o
~.~ -

~
.-
~.~ b E

< <
0p.

~ t"-I

-H -H -H -H
t~
m m ~
t~
t~

C'-I

~r t"r

O0
n~
0

<< <<
~ O 0

n9 E .o .o
9 ~

~ , ~-~ co~

~,.tn
o~

,~ ~ o~ o
o~

o o~

oo o~
32 M. KRS E T AL.

~"'~ ' , , f ~ . ~,,, __

L.
CZECH
REPUBLC
I /
\ J
~. ,.,.?' ~v

RB~ /r
TLUSTICE

~HoR
. M
RIOAO~
LeR
MR
i
I N

~777<-qB~ ~Skm

Fig. 1. A sketch map of the Western Bohemian Carboniferous and selected Carboniferous Relics in the broader
region of the Western Bohemian and Central Bohemian Basins, incl. localities of collected oriented samples.
1, Lin6 Formation; 2, Slan~, Fm; 3, T~,nec Fm; 4, TS,nec and Kladno Fms (undifferentiated); 5, Kladno Fm
(N~any and Radnice Members); 6, Late Proterozoic and Early Palaeozoic rocks (crystalline rocks and
sediments); 7, fructure line; 8, uncertain boundary between lithostratigraphic units. Basins: MB, Man6tin;
ZB, Zihle; PB, Plzefi; RB, Radnice. Carboniferous Relics: LeR, Letkov; MiR, Mirogov; HoR, Ho~ovice;
ZeR, Zebr~k.

Carboniferous to the Earliest Permian, which ing or deposition of the rocks; all other
caused directions of the overprint components to components generated later (chemoremanent,
be close or even identical with the palaeomagnetic viscous magnetization) are epigenetic. The
directions of the analyzed Carboniferous rocks. processes of syngenesis and epigenesis in red-
Study of the origin of the remanence components beds is not precisely dated, since these rocks,
therefore required the use of other methods. besides the detrital (syngenetic) magnetization,
A combination ofpalaeomagnetic, petromagnetic show a larger proportion of the chemorema-
and magnetomineralogical methods appeared to nent magnetization which most probably is due
be the most suitable one. The different values to a gradual dehydration of unstable Fe-oxides
of unblocking temperatures and the varying into the final stable haematite phase (Krs &
spectra of micro-coercive forces reflect the Pruner 1995). Even haematite is frequently re-
variable mineral composition and grain size of magnetized, most probably because of the
the ferrimagnetics. circulation of water with dissociated oxygen,
Thermoremanent magnetization in volcanic or it may be generated by an intensive weath-
rocks and the detrital magnetization carried ering of magnetite or of some Fe-sulphides
by finely disseminated magnetite grains in (Krs 1967).
sandstones, claystones and siltstones are Biostratigraphically well dated rocks of West-
mostly syngenetic. Under the term of syngen- phalian C D and Stephanian A B and C ages were
esis we include magnetization related to cool- chosen for our study. The previously derived and
 MAGNETIC REMANENCE COMPONENTS 33

Mt/Mn -3
No. 7199A3 1] ~.+.+~_~,,
~---~-Jn = 112 x l 0 Aim

~ 0.16 x 103AIm
"t
[ , , , , , ,~-
200 N....~400 500~
O...XZ f _ ~ , , , , , "-4~t
I e...XY o NSI 3 0 0 . / - ~,60
-2- 100 C'----TR-
._: .oo oom , /
Iooooo
9 }o~ -,,~ ,~o~
w4,,,,,,-/_+--,,,,
\ ~oo~-: /
///- ~oo~ ~oX : /12o
W
Up 9 ' -4 Down 210 ~ 150
1unit=79.Tx10 Aim S

No.7199A1 No.7201A2

"/ ~Mts/~t \
0,1,
200 400 500~ 200 400 600~
~'t/~n ~t ~ t
~t ~n--729x165ts,l 21 /
I I I I | I

200 400 500~ 200 400 500~

"-t" t ----t

Fig. 2. Bil~ Hora near Plzefi. Westphalian C, tuffite. The upper half of the figure: results of thermal
demagnetization of the natural sample. The uppermost plot shows normalized values of Mt/Mn in relation to
temperature t~ Mt is the remanent magnetic moment of the sample demagnetized at temperature t~ Mn is the
remanent magnetic moment of the sample in natural state. Beneath the plot of Mt/M, in relation to t~
Zijderveld's diagram and stereographic projection of remanent magnetization vectors are given for the sample in
natural state (NS) and after progressive thermal demagnetization at temperature t~ The lower half of the figure
presents results of thermal demagnetization of the samples subjected to saturation magnetization (prior to
thermal treatment). The plots show normalized values of Mt,s/Ms and ~t/Jt~ in relation to temperature t~ Mt,s
is the remanent magnetic moment of the sample in saturated state and thermally demagnetized at temperature
t~ Ms is the remanent magnetic mament with saturated magnetization Js under the room temperature; ~ t is the
volume magnetic susceptibility of the sample demagnetized at temperature t~ ~n is the volume magnetic
susceptibility of the sample at room temperature.

statistically averaged palaeomagnetic directions Outline of geology of the areas investigated

within the Westphalian-Stephanian range (Krs
1968) were thus verified by refined techniques. The Late Palaeozoic Basins of the Central and
Another objective was to verify and to date more Western Bohemia consist of terrigenous
accurately the genesis of the palaeotectonic ('limnic') deposits. These form an almost
rotations that had already been identified in the uninterrupted area of about 3500km 2. The
Bohemian Massif early in the palaeomagnetic Central and Western Bohemian Basins are
research of the region (Birkenmajer, Krs & parts of the Bohemian Massif megahorst.
Nairn 1968). Their origin was connected with tectonic
34 M. KRS E T AL.

Mt I'Mnj~Jn =253 x 1(] 6 Aim

0 5-] ~-h~ 11.9 x I0-6A Im

o...XZ "[ ~"+-+'+~';

' o;oo
.h ~ _ --q-, --,,-)
9~ I ~ ), ) I
oo./
l
:- \
~'o---540oC Down [ - \
"~,.,...500 oc I - I

-
t/" ,ooo
200 oc 0J--~-24 50 120

\ 150~ 2 1 0 ~ 150
1unit=31.Sx1()6A/m 250~ S

No. 7 1 9 0 A 2 No. 7 1 9 6 A 3
MtslMs Mr,siMs

0.4 '~

200 400 600~ 200 400 600~

Mt/Mn "-'~t ~ft/;Fn "-" t
2" I / ~ n = 12 x10-6 [SI] 24 ~fn=7.5x 1C~6[ SI ]

I I I ! I I I I 1 I l I
200 400 600 ~ 200 400 600 ~
"--"t --" t

Fig. 3, Tlustice near Zebrfik. Westphalian C, tuff, tuffite. See caption to Fig. 2.

activity during the Variscan orogeny, reflected dominantly of fluviatile deposits, while the
in a progressive but uneven subsidence of the others are chiefly lacustrine. Mudstones and
Variscan intramontane area in which most of claystones of the Kladno and Slan~r Formations
the limnic basins of Western and Central are mostly grey, with a few significant coal
Europe were formed. seams, whereas those of the two remaining
Initial sedimentation in the Central and formations are mostly red.
Western Bohemian Basins began in the West- The Carboniferous deposits in general dip
phalian C and with some breaks in deposition, primarily at only a few degrees. However, the
probably reflecting the Variscan orogeny, along dip may have been steepened by uneven
with several diastems, sediment accumulation subsidenced blocks. The strata of some basins
continued at least up to the Stephanian C or, show definite, although general, dips. Large
more likely, Autunian time. However, Autu- outcrops in the Plzefi Basin consist of deposits
nian clastics have nowhere been found pre- dipping mainly to the E to SE, whereas in the
served in the Central and Western Bohemian southern part of the Central Bohemian Basin the
Basins. deposits dip generally to the N.
The stratigraphic sequence is divided into Reconstruction of the faults and fault
four formations, some of which are subdivided systems in the Central and Western Bohemian
into members and horizons (Table 1). The first Basins poses serious problems. Here, with the
two, Kladno and T~,nec Formations, consist exception of the northern parts of the Central
 MAGNETIC REMANENCE COMPONENTS 35

1.43 1.29.
Mt/Mn/1.52 1.31 5.81]

45ooq N,/ s -{ jn=498• \

400% ~ / 6 k-*
| 1o3 x 16 Aim ----'
Up NS--~) n ~ ......
2 0, 0....j . _,~,
J ~ 0 ,0 ," 600~
,

e...XY .~.~.M~' . 3

400oC ",>Q~--._.100o C~r "

; o
1 unit=239x1(55Alm S 210 ~ S 150

No. 7 2 5 0 A 3 No. 7 2 5 6 A 4

200 400 500oc 200 400 600o(2

--~t ~ o ~ -',-t

..... , ,~n.70• 5 s r]
200 400 5OO~ 200 400 600%
~t --"- t

Fig. 4. Bilfi Hora near Plzefi. Westphalian C, laminated sandstone, reddish claystone. See caption to Fig. 2.

Bohemian Basins, subsidence faults predomi- the order of l0 -~ to 102m. Fault planes are
nate and generally strike N W - S E to N N E - estimated to dip on average 65 ~ to 70 ~, but
SSW and E-W. In the Ohe River district the very low angle faults dipping about 10~ to
Carboniferous is cut by NE to SW trending 25 ~ are also present together with steep to
faults parallel to the Litom6f'ice Deep Fault. vertical faults. Faults often virgate and vicariate,
Furrow-like depressions owe their origin to the isolated fractures becoming Y-shaped. A
recurrent movements that took place along number of faults were active in both syn-
N N E - S S W trending basement faults. All sedimentary and postsedimentary conditions,
basins exhibit, besides disjunctive tectonic while others formed after the termination of
structures, conjuctive phenomena. A close re- deposition.
lationship exists between these two types of
tectonic factors. Some faults were produced by
displacement along one plane, while others Laboratory procedures
form zones up to several hundred metres wide.
The faults trend in a curved pattern; the throw Laboratory procedures were combined in a
and dip vary. The fault throw ranges from way that enabled the derivation of both the
several cm to several hundreds of metres. Most palaeomagnetic directions and the determina-
frequently movements along the faults are of tion of the m i n e r a l s - carriers of the respective
36 M. KRS E T AL.

Mtl~..~J n=7719x 165Aim

No.7244A2 ' 1-"~H"N--~-
| 4, , ~
0.5t 56.5x 166Aim

N o...xz '260' ~ 60o 8oooc

e...XY ~ "-"" t
I 200oc ~NS / _
.T 3oooc..~c~ 3o~ : "k.~o
/ 7oooc / / L~s-52ooc/
//o~ w-I'"" ' " : + ! ' " " " ~E
U/5zooc E \ -I /
W___~F_! ; : I I I '. : \ -4 /
Up ~ B50~ Down 2 4 0 ~ 4 ~ 68/0~
">-~\ ',LZ...-'C
l~ j680~
S lunit=Tg6xl()6AIm 210 ~ " - 150

No. 7240 A1 No. 7244A1

M t . l ~ _ j s = 1091x,(]4Aim Nt'ls]~-~
" Js=17432x ,(]4Alrn

i 1 i 1 i --I-
200
400 600~ 200 400 600~
~r _ ~m.m~o --4. t ~'t I~,n --4- t

2 t ~ 2 gtn=8X1()6 [ S,]
I (~6[SI l ltt~m-11"~4~~
I I I I I 1 i i 1 I I 1

200 400 600 oC 200 400 600 ~

---'-- t --" t

Fig. 5. Mirogov, 'Lomy na JanovE. Westphalian D, grey siltstone. See caption to Fig. 2.

remanence components. This method provides ment (P[ihoda et al. 1989) securing generation of
data to be used for the reconstruction of the a high magnetic vacuum in a medium of
history of the origin of the magnetization thermally demagnetized specimens. The rema-
components. The following approach was nent magnetization of specimens in their natural
adopted: state is identified by the symbol Jn, the
Hand samples were collected in the field from corresponding remanent magnetic moment by
the localities mentioned in Table 2 and at the symbol Mn. The remanent magnetic moment
locations shown in Fig. 1. Laboratory speci- of the rock specimen demagnetized at tempera-
mens in the form of small cubes were prepared ture t~ is denoted by Mt. Graphs of normalized
from the hand samples to be measured on values of M t / M n = ~ ( t ) were constructed for
spinner magnetometers JR-4 and JR-5 (Jelinek each analyzed specimen and they provided
1966). The hand samples are designated by both primary information on the unblocking tem-
numbers and by the letter A, e.g. 7190A. peratures of the minerals - carriers of remanent
Laboratory specimens are designated by indexes magnetization.
1, 2, 3, etc., for example 7190A1, 7190A2, The directions of Jn and those of the remanent
7190A3, etc. magnetization of the thermally demagnetized
Laboratory rock specimens in their natural specimens in the course of a progressive thermal
state were subjected to progressive thermal demagnetization are shown in stereographic
demagnetization by using the MAVACS equip- projection. The orthogonal projection of the
 MAGNETIC REMANENCE COMPONENTS 37

100[ % ] ~ o,-' * ' ~ * ~

9ao
~ Roudn6 near Plze6 0/o" 271100[pT1

No. 7217A3

l l I ' [ | I -' I "nil tIu|'l ' I II Ill'l n

1 2 4 6 810 20 4060 100 200 4(33 1000[rnT]
80 600 800
fi___.
lOO-%]
90"
Pit between Ledce end Zitov ~'13413[nT]
80-
I 70" /
60-
~" SO" No.7335A5
~IRM/t~H
-~ 4o-
30"
20"
10-
, , ~ ,, I
I I ' ' I ''I 'I'I I ' I 'I 'l'l'
1 2 4 6 810 20 40 60 100 200 4.00 lO00[mT]
80 600 800

Fig. 6. Isothermal remanent magnetization (IRM) in dependence on direct magnetic field (H). No. 7217A3: a
sample of grey claystone from the Roudn/t locality near Plzefi; No. 7335A5: a sample of red claystone from a pit
between Ledce and Zilov.

remanent magnetization vectors is shown by with appropriate accuracy, pilot samples were
the Zijderveld's diagram, where a full circle selected for the respective localities. They were
indicates projection onto a horizontal plane subjected to isothermal progressive magnetiza-
(XY) and a blank circle indicates projection tion by a direct magnetic field up to the
onto a north-south vertical plane (XZ). The saturation state with the use of a direct field
natural state of the specimens is designated by with a maximum intensity of 1000mT
NS. Phase or mineralogical changes of magne- (10 000 Oe). Dependence of the isothermal
tically active (mostly ferrimagnetic) minerals remanent magnetization (IRM) on the direct
frequently occur during the laboratory thermal magnetic field (H) was tested for 28 specimens.
tests. These changes can be clearly derived from Again, owing to the large amount of data these
the graphs of the normalized values of graphs are not shown here. However, this
~,/~t =f(t), where Jg, designates the volume information will be used for data interpreta-
magnetic susceptibility of specimens in the tion, see below. The specimens with the
natural state and ~ t the susceptibility of samples saturated remanent magnetization Js and with
demagnetized at temperature t~ The 9 and the corresponding remanent saturation moment
~ , values were measured on a kappabridge Ms, were subjected to a progressive thermal
KLY-2 (Jelinek 1973). Because of an excessive demagnetization by using the MAVACS equip-
number of data, these graphs are not shown in ment. The plots of the normalized values Mr,s~
the present paper, only typical examples of pilot Ms in relation to the temperature t~ of the
specimens are presented. demagnetization for the pilot specimens are
In order to determine the unblocking tem- shown in Figs 2 to 5 and in Figs 7 to 12. The
peratures of minerals in low magnetic rocks symbol Mt,s indicates the moment of a speci-
(with a low content of ferrimagnetic minerals) men that had a remanent magnetic saturation
38 M. KRS ET AL.

H ~
Mr/ ?n+~---~k J n :555 x 10 5A/m
No. 7222 A3 ,\

W N E / ~5.5x10 Aim
I I I I

540oC 'Oo n L , ,
;'--s 200 N 400 600~
-----300oC

V S
Q,..XY

1unit = 79.6 xlOSA/m--

210 ~
S
150

Mt,s/MsNO. 7217A3_L ~,,t,s/MsNO.7219 A1-4

/-- / \
o

2 0 0 ~ 400 500~ 200 400 600%

~t/~n t --~'t ~t/~n ----~ t

1 x16 s [,Sll 1 :.~

i i i i i i i i i

200 400 600~ 200 400 600~

-'~t --~t

Fig. 7. Roudnfi near Plzefi. Westphalian D, grey claystone. See caption to Fig. 2.

moment of Ms in the initial state and was magnetic properties, with varied geological
subsequently demagnetized at temperature t~ history, origin of the remanence components,
Separation of the remanent magnetization and with variable magnetically active minerals.
components was carried out by using the This paper describes typical examples of the
multi-component analysis of Kirschvink (1980). measurement results.
The statistics of Fisher (1953) were used for both
the derivation of mean palaeomagnetic direc-
tions from the data of progressive thermal Bil5 Hora near Plzefi, 7198A-7201A, tuffite,
demagnetization for selected sets of rocks with Westphalian C
suitable physical properties and for calculation
of mean directions of the pertinent remanence Various Fe-oxides with markedly unstable prop-
components derived by the multi-component erties were identified. Specimen No. 7199A3
analysis. shows a single-component remanence with hae-
matite generated by recent weathering as its
carrier. This specimen with recently generated
Results of laboratory measurements haematite shows a narrow spectrum of micro-
coercive forces, the saturation state was reached
The heterogeneous petrographic rock types in a high field of 900 mT in intensity. Another
selected for laboratory treatment represent a investigated specimen No. 7201A2 with various
natural material with a wide spectrum of Fe-oxides shows a wide spectrum of micro-
 MAGNETIC REMANENCE COMPONENTS 39

Mt/Mn .+"+~. .
1-.~-+/ ~'+-+._
NO. 7 2 0 6 A1 I \ Jn=84 * I(]4Alm~.
0.54
I I I
12"8x1()4A/m~--~
! ! I |
o...xz 200 N 400 600~
N
t e...XY 200~
-- 300~ \,., o

".1~ 450~ S
,, 585oC ~ -~-,,.-,
660~ -o'--- \ 100~
/ft / "~-%oooc
, ooc
: 71 : : :_: : : : : Ej J
Up lunit=Zg6xl(~4Ai m Down 210 " ' - - ' r " ' - 150
S
MLslM s No. 7 2 0 2 A 2 MI,slMs N o . 7 2 0 6 A 2

I I J I I C 215-~ ~ ~ I -

2 ~/~n 200/ 400 "-~'t

600~ 200 400.,, 600~
it/~r /L~" --~'t

1 ! _ /
200 400 500~ 200 400 600~
"-~'t "-~'t

Fig. 8. Rad6ice near Plzefi. The Westphalian D/Earliest Stephanian, grey claystone. See caption to Fig. 2.

coercive forces, the saturation state was reached IRM on a magnetizing field H was investigated
at 200mT. Samples of this group did not and in three samples a saturation state was
preserve their Variscan magnetic directions reached in a direct magnetic field of 700mT,
owing to intensive weathering. Some samples which is characteristic of magnetically hard
also revealed a conspicuous instability during samples. Unblocking temperatures for goethite
their thermal treatment (Fig. 2). _<100~ and for magnetite below 580~ can be
derived from the graphs of Mt, s/Ms plotted
against temperature (Fig. 3).
Tlustice near Zebrdk, 7190A-7197A,
tuff- tuffite, Westphalian C Bild Hora near Plze~, 7247A-7259A,
Two-component magnetization predominates. laminated sandstone, reddish claystone,
Goethite is the carrier of the remanent magne- Westphalian C
tization with the direction of the recent geomag-
netic field (influence of weathering). The carrier Samples show physically unstable properties. The
of the characteristic magnetization is a minor carriers of the magnetization are the Fe-oxides
magnetite proportion. The Variscan remanence with unblocking temperatures mostly below
component is well separable at an interval of 500~ generated by weathering. Only two speci-
250~176 In four samples the increase in mens (No. 7250A1- laminated sandstone and
40 M. KRS ET AL.

MilMn
No. 7215AI I l~/"\+'-,~_.
o...xz ~.. " ] J.=684x16 A/m.w.+..~ /
i...XY
/ / . . . . . \ ,J,
T *-^o^ 200 N 400 600~
9 + ~4u u E ~..~.-J--.~-.30 -'~t

up Oo n 3 0 0 / : .60

-/--/ "~' /-WT.'__~_'_'.]~I,~';"'''' ' 't E

/ / f%. ~ 24o1\ I'!__3oo~ /~2o

,</,- { - ,oooo
, ' -
1 unit =7g.6x lOBA/m 200oC S

No.7211A1 No.7215A3
11,~
Mt,slMs
Js=2651xl0-4AIm

| i , ! ! |---

200 400 SO0~ 200 400 B00~

"gt I~n --D t ~ftlafn ~t
2 t 0tn=lggxlOB[ Sll
I t -i: - -- - - -~. ---'~,i -'i 1
l
~ ' , | | i i i i

200 4 0 B00~ 200 400 B00~

"-~t ---"t

Fig. 9. Rad6ice near Plzefi. Stephanian A, green siltstone. See caption to Fig. 2.

No. 7256A2 - red claystone) yielded palaeomag- In specimen No. 7244A2, a Variscan direction of
netic directions. Phase changes, derivable from remanence at high demagnetization tempera-
the graphs of Mt, s/Ms plotted against tempera- tures of 650~ and 680~ is visible (Fig. 5).
ture, point to a low reliability of derivation of the
palaeomagnetic directions (Fig. 4).
Roudn6 near Plzefi, 7217A-7223A, grey
claystone, Westphalian D
MiroEov, 'Lomy na Janovd' quarries,
7236A-7246A, grey siltstone, Westphalian D Minerals with a wide spectrum of unblocking
temperatures mostly below 400~ and of micro-
The samples were mostly unsuitable for palaeo- coercive forces are the carriers of the magne-
magnetic analysis, only in three of them were tization. Figure 6 examplifies development of
Variscan palaeomagnetic directions within tem- isothermal remanent magnetization in depen-
perature interval of 100~176 (300~ dence on direct magnetic field for samples from
obtained. A low proportion of magnetite has the Roudnfi locality near Plzefi (No. 7217A3)
been proved, e.g. in specimen No. 7240A1. The and from a red claystone pit between Ledce
intensively weathered samples showed haema- and Zilov (No. 7335A5). A broad spectrum of
tite, with the direction of remanent magnetiza- micro-coercive forces for the sample from
tion close to the present-day geomagnetic field. Roudnfi is evident. Haematite has not been
 MAGNETIC REMANENCE COMPONENTS 41

M t l M n / J n = 8 6 0 x l(~6AIm
No. 72 24 A3 1]+'--+'+\4..~

0"5t \ 33.4x 1(~6A/m

o...XZ N / ~4---:-lJ
Q XY t , , ,,, '
"'" t 200 '~ 400
~ ~ ~ . 3 u
^~' _ 600~
~
'

:[.45ooc E /'I - "% "

w ,: ,,:%~,, t:: : : 300/ - \6o
up / ~ 3oo~ 0ow. s- / : \
W illlil i I E

50oC S

IV I_a..---~176 ~,~>%._Z_.--~,=~
S 150oC =,u /
200~ ~S ,-,~
1unit =7g.6 x 106Aim
Mr,sIMs No.7227A2 Mt.s/M s No.7228A2
1 ] ~ J s :4171x164Alrn I~ Js :4768x1154A/rn

200 400 600~ 200 400 600~

~'t/~n ---"t ~t/a'n -'-'- t
2t ~'n=151x166 Is1] 2t ~n=18xld6[sl]

I I i / i I i i '1 I i !
200 400 600~ 200 400 600~
" " t "-'-t

Fig. 10. Dolni Vtk~. Stephanian B, siltstone. See caption to Fig. 2.

proved, the proportion of magnetite is low. Variscan remanence component, being separ-
Ferrimagnetic minerals are represented by able within a temperature range 250~176
Fe-oxides, by goethite and probably by one Samples containing exclusively haematite, gen-
of the "r-Fe203 or rl-Fe203. The Variscan erated by recent weathering, show a narrower
remanence component is separable at a rela- spectrum of microcoercive forces and they
tively low temperature, within the interval of reach the saturation state in high intensity
(100) 150~176 (Fig. 7). magnetic fields (Fig. 8).

Rad~ice near Plzeti, 7208A-7216A, green

Raddice near PlzetL 7202A-7207A,
siltstone, Stephanian A
grey claystone, Westphalian D/the
Earliest Stephanian No haematite was detected in this sample group.
Otherwise, magnetic properties similar to
Multi-component remanence is caused by samples from the previous locality have been
syngenetic magnetite and by secondary Fe- proved. Magnetite is, again, the carrier of the
oxides, ranging from goethite to haematite, Variscan remanence component, which is separ-
formed by recent weathering (specimen No able in the temperature interval 250~
7206A1). Magnetite is the carrier of the (Fig. 9).
42 M. K R S E T AL.

Dolni Vlkf~Y, 7224A-7231A, siltstone, haematite with unblocking temperature below

680~ Three sites were sampled at this locality.
Stephanian B
The group of samples 7263A-7272A shows
Mostly minerals with a low unblocking tem- palaeomagnetic directions that correspond well
perature below 300~ are the remanence car- to those from the clay pit between the villages of
riers. The saturation state was reached at a field Ledce and Zilov (samples No. 7232A-7235A),
intensity of 350 mT; these are therefore medium- see below. The high stability of palaeomagnetic
magnetic-hardness minerals. Graphs of Mt,s/Ms remanence is also well documented by the results
plotted against temperature show a higher of progressive thermal demagnetization of the
proportion of minerals with a lower unblocking specimens (Table 3). The structure of Zijder-
temperature, but even a lower content of veld's diagrams, graphs of Mt/Mn and Mt,s/Ms
magnetite has been proved with unblocking plotted against temperature, and the extraordin-
temperature below 580~ The Variscan rema- ary stability of magnetic susceptibility vs. the
nence component is already separable at rela- thermal fields from the Zihle locality (Fig. 11)
tively low temperatures, within an interval of entirely correspond to the values established for
150~ to 300~ (Fig. 10). the clay pit locality between the villages of Ledce
and Zilov (cf. Fig. 12).

Zihle, a red claystone pit, 7260A-7272A, red

A red claystone pit between the villages
claystone, Stephanian C
of Ledce and Zilov, 7232A-7235A,
The remanence consists of two components, a red claystone, Stephanian C
smaller proportion represented by viscous mag-
netization. The carrier of the principal rema- The two-component remanence is due to a
nence component is an extraordinarily stable small proportion of viscous (recent) component

Table 3. Results of progressive thermal demagnetization using the MAVACS

apparatus. A red claystone pit, locality Zihle. Stephanian C, red claystone, Nos of
samples 7263A-7267A
Temperature Mean direction of a9s (~ k
(~ remanent magnetization

D(~ I(~

20 215.5 19.9 11.8 43.2 5

100 206.5 11.1 10.6 52.8 5
150 206.4 9.8 10.4 54.6 5
200 206.5 9.0 10.6 52.9 5
250 206.1 9.2 10.7 51.7 5
300 206.2 8.7 10.6 53.5 5
350 205.6 8.6 9.8 61.7 5
400 205.5 8.2 9.9 60.6 5
450 205.3 8.9 9.6 64.2 5
500 204.5 8.7 10.1 58.8 5
540 204.7 8.4 10.9 50.5 5
580 204.6 8.2 10.7 52.1 5
620 203.4 8.3 10.2 57.7 5
650 208.6 8.0 12.9 35.9 5
680 176.9 - 1.2 12.5 38.2 5
700 . . . . 5

D, I, declination, inclination of the remanent magnetization after dip correction;

a9s, semi-vertical angle of the cone of confidence calculated according to Fisher
(1953) at the 950 probability level; k, precision parameter; n, number of the samples
analyzed.
 MAGNETIC REMANENCE COMPONENTS 43

Mt/~In 0.5x 164Aim

W I

Up 700oC~
I : :
1' 'o'
680~ /

650~ ~
58~c4 / \
500~

NS ~,, c
-~-~_ 400~
[- 300~
b'~200oC 21U~_----q'50
100~ 1 unit =15.9xl(~4A/m S
/M NO.7263A2 MtdM s NO. 7 2 7 0 A 2

200 400 600~ 200 400 600%

aft/~'n n =221x10-6[SI] --"t ~ft~.n.~_~n=249x166 [sI] --"- t

! | ! i ! ! ' ! ! i i i i

200 400 600~ 200 400 600~

--"t "----t

Fig. 11. Zihle, a red claystone pit. Stephanian C, red claystone. See caption to Fig. 2.

and to a prevailing Variscan component directions, but to determine on several repre-

brought about by syngenetic haematite. The sentative rock samples, the genetic history of
haematite is characterized by a narrow spec- the remanence components or the overprint
trum of micro-coercive forces and by high components. This approach has, nevertheless,
magnetic hardness (the lower part of Fig. 6). partially verified the results of previous palaeo-
The stability of palaeomagnetic directions is magnetic measurements (Krs 1968) by using a
extraordinarily high. Table 4 shows the mean refined methodology, particularly by introdu-
remanence directions using Fisher's (1953) cing the multi-component analysis of rema-
statistics of four samples submitted to progres- nence and by using the thermal demagnetizaion
sive thermal demagnetization. The Variscan in a high magnetic vacuum. Table 5 sum-
remanence directions are derivable within an marizes the derived palaeomagnetic directions
interval of 150~176 and optimum clean- and the corresponding virtual pole positions.
ing was achieved at a temperature of 620~ Higher values of palaeomagnetic declination
(Fig. 12). have been proved at several localities (Rad6ice
near Plzefi- grey claystone, Bil~ Hora near
Plzefi and also at the red claystone localities
Palaeomagnetic directions and virtual between the villages of Ledce and Zilov, Zihle).
pole positions Similar higher values of palaeomagnetic decli-
nation in western Bohemia were reported
The objective of our work was not merely to earlier (Birkenmajer et al. 1968). The data
increase the data base of palaeomagnetic presented here indicate that the higher values
44 M. KRS E T AL.

MtlMn
NO. 7232AI 11~"+'~,
I\
-4
'N-,,.~.~.0.8x10 Aim

w " /
u# : " =~f' "~0o~o/ . . . .
200
.,
~
,/'g~
600 800~
7 ~ 6sooc ~ .
o...xz f :
o...XY / ~ , T 585o C uu/ - "k,,~u

/ hoooc,l \ / : /

150~C S 210 ~ 150

1unit = 23.9 x 1()4A/rn S

No.7235A5
Mr,s/Ms
1 1 ~ ~ 1 ~ 4 0 2 3 x 1(}4A/m

200 400 600~

~tlMn ~ t

! i ! i I !

200 400 600~

--~.f

Fig. 12. Between villages Ledce and 7,ilov, a red claystone pit. Stephanian C, red claystone. See caption to Fig. 2.

for palaeomagnetic declination in the Carboni- qap = 37.46 ~N; Ap--163.76 ~ E; 0 { 9 5 = 6.7~ k =
ferous are not constant across the studied area, 132.7; N - 5 . The difference in magnitude of
but differ from one locality to another. On the the precision parameter k is significant. The
other hand, the palaeomagnetic directions for mean pole positions calculated in this paper
Early Permian rocks are homogeneous in the correspond well to those derived on a larger
territory of the Bohemian Massif, indicating an data set for the whole Bohemian Massif, on
extraordinary tectonic stability (consolidation rocks dated biostratigraphically (Krs & Pruner
of blocks of the newly forming supercontinent 1995).
Pangea, Krs & Pruner 1995).
Figure 13 shows the virtual pole positions for
the studied Westphalian and Stephanian rocks. Conclusions
Although the pole positions have been calcu-
lated from a small number of samples, the Palaeomagnetic, petromagnetic, magnetominer-
Westphalian rocks exhibit a higher scatter of alogic analyses and the multi-component ana-
palaeomagnetic data than do those of the lyses of remanence of rocks of Westphalian C to
Stephanian. For rocks of the Westphalian the Stephanian C ages in the Central and Western
~,p = 36.25 ~N; Ap : 164.87 ~ E; Q{95: 15.4~ Bohemian Late Palaeozoic Basins have provided
k=36.4; N = 4 ; for rocks of the Stephanian the following information:
 MAGNETIC REMANENCE COMPONENTS 45

Table 4. Results of progressive thermal demagnetization using the MAVACS

apparatus. A red claystone pit, between villages Ledce and Zilov. Stephanian C, red
claystone, Nos of samples 7232A-7235A

Temperature Mean direction of o~95 (~ k

(~ remanent magnetization

D(~ I(~

20 208.8 -9.9 14.0 44.3 4

100 206.8 -12.9 14.4 41.6 4
150 206.3 - 14.4 14.5 40.9 4
200 206.1 - 14.4 14.3 42.1 4
250 205.7 - 13.9 14.2 42.7 4
300 205.8 - 14.1 14.3 42.4 4
350 205.5 -12.5 14.4 41.7 4
400 205.4 - 11.8 14.4 41.9 4
450 204.6 - 10.0 14.0 44.2 4
500 204.9 -10.1 13.6 46.4 4
540 204.9 -8.3 13.9 44.8 4
580 205.0 -7.1 13.3 48.8 4
620 204.3 -5.2 12.8 52.3 4
650 204.9 - 5.3 13.2 49.2 4
680 177.4 -2.9 5.2 307.8 4
700 38.2 -35.5 49.4 4.4 4

D, I, declination, inclination of the remanent magnetization after dip correction;

a95, semi-vertical angle of the cone of confidence calculated according to Fisher
(1953) at the 95% probability level; k, precision parameter; n, number of the samples
analyzed.

Table 5. Virtual pole positions, mean palaeomagnetic directions. Plzet[ Basin, Westphalian C to Stephanian C,
cf Table 2

Site Locality Mean a95 (~ k n Virtual Ovals

palaeomagrnetic pole of
directions positions confidence

Dp (o) /p (~ ~p(~ Ap(~ dm (~ dp (~

1 Bilfi Hora near unstable sample 3

Plzefi
2 Tlustice near Zebrfik 201.4 18.6 10.5 34.2 7 27.69 169.89 10.93 5.68
3 Bil~i Hora near Plzefi 218.5 -12.8 19.7 162.3 2 36.04 143.52 20.07 10.23
4 Miro~ov 'Lomy na 200.8 2.8 10.5 131.8 3 36.27 167.51 10.50 5.25
Janov6'
5 Roudnfi near Plzefi 190.7 -5.7 6.5 87.1 7 42.22 178.90 6.52 3.27
6 Rad6ice near Plzefi 212.2 -10.8 3.6 653.8 4 38.07 150.98 3.65 1.85
7 Rad6ice near Plzefi 196.5 3.0 14.4 15.7 8 36.81 172.56 14.41 7.21
8 Dolni V l k ~ 197.4 -0.6 6.8 79.1 7 38.32 170.88 6.80 3.40
9 Zihle, a red 205.0 2.3 7.2 45.6 10 34.40 162.57 7.20 3.60
claystone pit in
operation
10 A red claystone 204.3 -5.2 12.8 52.3 4 38.47 161.66 12.84 6.44
pit, between
Ledce and Zilov

Dp, Ip, mean palaeomagnetic declination, inclination; a95, semi-vertical angle of the cone of confidence calculated
at the 95% probability level; k, precision parameter; n, number of the samples analyzed; ~p, Ap, palaeolatitude,
palaeolongitude of the virtual pole position; dm, dp, ovals of confidence calculated at the 95% probability level.
46 M. KRS E T AL.

Westphalian Step hanian

Fig. 13. Stereographic projection of virtual pole positions. Virtual pole positions are denoted by small full circles.
The mean pole position calculated from virtual pole positions is denoted by a crossed small full circle, it is
circumscribed by a circle of confidence calculated according to Fisher (1953) at the 95% probability level.
Westphalian: 2, Tlustice near Zebr~k, Westph. C; 3, Bil~ Hora near Plzefi, Westph. C; 4, Miro~ov, 'Lomy na
Janov6', Westph. D; 5, Roudnfi near Plzefi, Westph. D. Stephanian: 6, Rad6ice near Plzefi, the Westph. D/Earl.
Steph.; 7, Rad6ice near Plzefi, Steph. A; 8, Dolni Vlk~,~, Steph. B; 9, Zihle, a red claystone pit, Steph. C;
10, Between villages Ledce and Zilov, a red claystone pit, Steph. C.

(1) Magnetite is the principal carrier of the its direction of remanent magnetization corre-
Variscan remanence component in most non- sponds to that of the field of a recent (theoretical,
red-coloured rocks. In tufts and tuffites the co-axial, geocentric) magnetic dipole.
magnetization is of thermoremanent and detrital (4) Except for the Bilfi Hora locality near
origin, and it is also of detrital origin in grey, Plzefi (highly weathered tuffite), all rocks of the
green claystones and siltstones. In these cases, localities studied (Tables 2 and 5) show a multi-
magnetite is syngenetic with the rock, i.e. the component remanence and some of them also a
direction of its Variscan palaeomagnetic rema- Variscan remanence component.
nence component corresponds to the time of (5) In some rocks, the Variscan remanence
deposition and compaction of the rock. component was already separable at low
(2) In the red-coloured rocks, haematite is the temperatures, e.g. in the grey claystone from
carrier of palaeomagnetization which clearly Roudnfi near Plzefi from (100) 150~ upwards,
originated during the diagenesis of the rock and in a claystone from Dolni V l k ~ from
(red claystone). Haematite of this type is 150~ In red claystones from the localities of
physically stable; it has been proved to contain 2;ihle and from the clay pit between the
a slightly viscous component and its spectrum of villages of Ledce and Zilov, the Variscan
unblocking temperatures is wide. component was separable from (100) 150~
(3) In some rocks other than red, e.g. in the upwards. These data indicate that these local-
grey siltstone from the Miro~ov locality, in the ities were not significantly reworked chemi-
'Lomy na Janov6' quarries and in the grey cally, thermally or by other processes in post-
claystone from the Rad6ice near Plzefi locality, Variscan times. It was the recent rock weath-
haematite has been found to be a product of ering that caused either a partial or a complete
weathering. Haematite of this type shows a obliteration of the Variscan remanence com-
narrow spectrum of unblocking temperatures; ponent in some of the rocks.
 MAGNETIC REMANENCE COMPONENTS 47

(6) Virtual pole positions have been derived FISHER, R. 1953. Dispersion on a sphere. Proceedings
from relatively small sets of data. Nevertheless, of the Royal Society, A217, 295-305.
the Westphalian rocks seem to have undergone JELiNEK, V. 1966. A high sensitivity spinner magnet-
ometer. Studia geophysica et geodaetica, Praha,
palaeotectonic deformation more intensively
10, 58-78.
than those of the Stephanian. This is in - - 1 9 7 3 . Precision A.C. bridge set for measuring
accordance with an overall decrease in palaeo- magnetic susceptibility and its anisotropy. Studia
tectonic deformation in the final phase of the geophysica et geodaetica, Praha, 17, 36-48,
Variscan orogeny, which finally terminated by KIRSCHVINK, J. L. 1980. The least-squares line and
Early Permian times (Krs & Pruner 1995). plane and the analysis of palaeomagnetic data.
Geophysical Journal of the Royal Astronomical
The authors wish to thank Professor R. Gayer and Society, 62, 69%718.
Dr. V. Kropfirek for reviewing the paper and sug- KRS, M. 1967. Research Note: On the palaeomagnetic
gestions. They are also grateful to Professor R. Gayer stability of Red sediments. Geophysical Journal of
for improvement of the English. The authors would the Royal Astronomical Society, 12, 313-317.
like to thank Mrs. Marta Krsov/t and RNDr. Daniela 1968. Rheological aspects of palaeomagnetism?
Venhodovfi for their help in laboratory works. They International Geological Congress Prague,
also acknowledge the financial support through the XXXIII Session, 19-28 August 1968, Proceed-
Grant No. 113/94 of the Charles University in Prague. ings, Section 5, 87-96.
& PRUNER, P. 1995. Palaeomagnetism and
palaeogeography of the Variscan formations of
the Bohemian Massif, comparison with other
References European regions. Journal of the Czech Geological
Society, Praha, 40/1-2, 3-46.
BIRKENMAJER,K., KRS, M. & NAIRN,A. E. M. 1968. PI~iHODA, K., KRS, M., PESINA,B. & BLAHA,J. 1989.
A palaeomagnetic study of Upper Carboniferous MAVACS- a new system creating a non-mag-
rocks from the Inner Sudetic Basin and the netic environment for palaeomagnetic studies.
Bohemian Massif. Bulletin of the American Special Issue Cuadernos de Geologia Ibdrica,
Geological Society, 79,589-608. Madrid, 12, 223-250.
A depositional and diagenetic model for the Eocene Sulcis coal basin of
SW Sardinia
ROLAND DREESEN'*, DOMINIQUE B O S S I R O Y ~, R U D Y S W E N N E N ~,
JACQUES T H O R E Z 3, A U R E L I O F A D D A 4,
LUCIANO OTTELLI 5 & EDDY KEPPENS 5

l Institut Scientifique de Service Public, 200 Rue du Chdra, B-4000 Li@e, Belgium
2 Katholieke Universiteit Leuven, Afdeling Fysico-chemische Geologie,
Celestijnenlaan 200 C, B-3001 Leuven, Belgium
3 Universit~ de Lidge, Service de G~ologie GOnOrale, GOologie des Argiles et Sddimentologie
des Silicoclastiques, AllOe du 6 Aofft, B18, B-4000 Sart Tilman par Lidge 1 Belgium
4 Carbosulcis, Miniera Monte Sinni, 1-09010 Cortoghiana (Ca), Sardinia, Italy
5 Vrije Universiteit Brussel, Eenheid Geochronologie, Laboratorium voor Stabiele Isotopen
Geochemie, Pleinlaan 2, B-1050 Brussels, Belgium
* Current address." VITO, Boeretang 200, 2400 Mol, Belgium

Abstract: Detailed sedimentological, mineralogical and petrographical analysis of closely

spaced cored boreholes has enabled the development of a revised depositional model for the
early Eocene coal-bearing Produttivo Formation of the Sulcis Basin. The deposition of
autochthonous-hypautochthonous palustrine-lacustrine coals and associated carbonates
was interrupted episodically by sedimentation of allochthonous lithocalcirudites and
lithocalcarenites. The latter clastics display characteristic upward shoaling tidal flat
sequences related to marine incursions. This interpretation is in contrast to the previously
accepted fluvial origin of the detrital episodes. The coarse basal transgressive lag deposits
consist of various carbonate intraclasts, dolosparite, grains consisting of calcite cement and
euhedral-subhedral evaporite-bearing quartz grains. Combined stable isotope and
cathodoluminiscence analysis has revealed a complex diagenetic history for the clastic
deposits. The potential extrabasinal or intrabasinal provenance of the clasts, in particular
the origin of the evaporite relicts, is discussed. The subtropical-tropical coastal marshes of
the Florida Everglades (USA) are proposed as a possible modern analogue for the sub-
bituminous Sulcis coals.

The Sulcis coal basin in southwest Sardinia carbonates, which are closely associated with the
(Fig. 1) represents the only subbituminous coal coals. The latter concentrated on the search for
deposit in Italy. Between 1979 and 1992 over local lithological and palaeontological marker
two hundred exploration boreholes were drilled beds. Most of these data are unpublished and
from the surface and from underground galleries were made available to us by courtesy of the
by Carbosulcis S.p.A. Recently, a number of Board of Directors of Carbosulcis.
these cored drillholes have been reinvestigated as The coal-bearing sequence (the so-called
part of an international research project funded 'Produttivo') displays complex interfingering of
by the European Commission (ECSC). The marine-influenced and non-marine sediments,
main objective of this work is to enhance the including coals, carbonaceous mudstones, marls,
resolution or reliability of intrabasinal litho- brackish to fresh-water limestones, and carbo-
stratigraphical correlations of coal seams nate-rich detrital rocks. The latter 'hybrid'
through an integrated sedimentological and clastic rock types (quartz-rich lithocalcirudites,
sequence stratigraphical approach. lithocalcarenites) represent minor or major clastic
Previous sedimentological analyses include intercalations, which can be used for subdividing
scientific case studies conducted under the super- the coal-bearing sequence into successive litho-
vision of Italian universities (Siena, Cagliari) and logical intervals. This paper will focus on the
consultancy studies completed by national or origin and the role of the latter 'detrital'
international experts. The former dealt with intervals in the context of a revised depositional
micropaleontological, palaeoecological or micro- model for the coal-bearing deposits of the
facies characteristics of the marine and lacustrine Sulcis Basin.

From Gayer, R. & Pegek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 49-75.
50 R. DREESEN E T AL.

Fig. 1. Location map of Sulcis mining project area (dark shaded area) in SW Sardinia.

Regional geological setting, average thickness is 40-50 m at depths between

palaeogeography and stratigraphy 200 and 400m. The estimated coal reserves
exceed some 250 million tons.
The coal-bearing Sulcis Basin formed during The Sulcis coal can be classified as a low
early Tertiary times as a result of extensional rank non-caking coal with very high volatile
tectonic events which affected the south-eastern matter, low reflectance and calorific values
edge of the Iberian Plate (Assorgia et al. 1992). (sub-bituminous A-B coal; Glanzbraunkohle).
After an initial sea level rise at the base of The heterolithic coal-bearing Caenozoic sedi-
the Palaeogene, a sea level fall was induced in the ments of the Sulcis Basin have been affected
early Eocene by the Pyrenean orogeny in the west- by E-W and N N W - S S E oriented block faults
ern Mediterranean area. Subsequently, the (Fig. 2), which can be related to the anti-
synsedimentary graben-like Sulcis Basin was clockwise rotation of the Corso-Sardinian
formed and reached equilibrium between sub- microplate (Orsini et al. 1980) during successive
sidence and infill (Fadda et al. 1994). The Sulcis tectonic phases of the Alpine orogeny. Eocene
Basin was infilled by various sedimentary normal growth (listric) faults created half-
and volcano-sedimentary deposits: Palaeogene graben structures and were responsible for
marine, brackish and continental (coal-bearing) thickness variations of the coeval sedimentary
deposits, Oligo-Miocene calc-alkaline volcanics deposits (Assorgia et al. 1992). The coal seams
(ignimbrites); and Neogene fluviatile and fluvio- and the associated 'barren rocks' (mostly lime-
lacustrine deposits. stones and marls) are often affected by small-
The aeral extent of the Sulcis Basin is scale folds. The latter occur in narrow belts and
estimated at about 200 km 2. It is bordered to they originated as a result of differential lateral
the east by Palaeozoic basement outcrop and to movements (gravitational sliding or slumping;
the west by the sea (Fig. 2). The Eocene coal- Bandelow & Gangel 1993) related to rollover
bearing formation ('Formazione produttiva a phenomena (Cocozza et al. 1989; Fadda et al.
lignite' or 'Produttivo') has a known subsurface 1994). According to Plaziat's (1981) palinspastic
areal extent of more than 100 km 2. It dips to the palaeogeographic reconstruction of the peri-
SSW with an average dip of 8-10 ~. The Pyrenean region, the Sulcis area represented a
thickness of the Produttivo and the number coastal embayment during early Eocene times.
and thickness of the coal seams gradually This area was bordered by a shallow sea in the SE
increase to the SSW. The Produttivo Formation and was intermittently affected by terrigenous
reaches a maximium thickness of 70 m. In the influxes derived from a continental source,
mining project area of Monte Sinni (Fig. 1) its supposedly located in the NW. The latter
 EOCENE SULCIS COAL BASIN 51

Fig. 2. Simplified geological map of the Sulcis Basin, SW Sardinia (modified after Fadda et al. 1994). Heavy lines
correspond to major faults.

Fig. 3. Palaeogeographical map of the peri-Pyrenean region during Ilerdian (Ypresian; early Eocene) times
(modified after Plaziat 1981).

source area would correspond to the Pyreneo- and the Pyrenean foreland (Languedoc area)
Provengal mountain chain (Fig. 3). Tambareau which corroborate the continental continuity
et al. (1989) have stressed the analogies between between the Pyrenean area and Sardinia.
the continental microfaunas and palynofloras The Palaeogene deposits of the Sulcis Basin
of the Ilerdian (Ypresian) deposits of Sardinia reach a maximum thickness of 140m and
52 R. DREESEN E T A L .

DEPOSITIONAL ENVIRONMENT

STAGES FORMATIONS MAJOR LITHOLOGIES COCOZZA et al. 1989

CONSULTANCY THIS PAPER
ASSORGIA et al. 1991 STUDIES
FADDA et al. 1994

volcanics
tu
u ...... ~ ...... pyroclastlcs '
interbedded
O Volcano - not studied
z sedimentary ............. rhyolitic Ignlmbrttas within
complex continental
0 ............. andesitic basaits
terdgenous
successiona not studied

0
Z
0
~
~_) . . . ~ .

Cixerri Fm.
I
450 m ,~, b . . , h . . ,, ,,., ,~

polygenic
cong,o.~
sandstones
alluvial fans
alluvial fans
LU alltatones braided plains
claystones lacustrine
~ t o ~ o ~
palustrine
0 ., .......... "-" siltat. ~ r . ~ L cgl. fluvial channels fluvial channels episodically
i Produttivo freshwater Iimest. ~ custdne supralittoral
paludal -
interrupted by
channellized
Fm. marls parallc lagoonal tidal clastic
i ~ '1r 7~ rr. ~ - ,- claystones lagoonal littoral deposits reworking
pseudomorphosed
~ evaporites
Miliolitic ~ b i o - calcarenites hypersaline &
Limestone mesohallne sublittoral

P-,-~_':-CF.~

PALAEOZOIC~
Fm.
30- 40 m
B~S~L CONGLO.U.., --

PERMO- " ~ J f / J
- ~ ~-=- .
marls

. .

folded
. . . . . . . .
lagoons
w ...... lag

' notstudied
\
\
restricted
marine with
fluctuating
salinities to
ah\...allowmarine
~
BASEMENT \ TRIAS.~C ~ v j / / / metasedl.,mentary
\
Fig. 4. Stratigraphic scheme, major lithologies and depositional settings of the Palaeogene deposits in the
Sulcis area.

display a characteristic transgressive-regressive and palynomorphs suggesting a Cuisian (late

megasequence with marine carbonates above a Ypresian) age (Pittau 1977; Salvadori 1979). The
polymict conglomerate at the base; paralic- Produttivo Formation is unconformably over-
continental heterolithic sediments in the lain by the Cixerri Formation, the basal part of
middle; and continental facies at the top of which has been assigned to the earliest Lutetian
the sequence (Fig. 4). A marked reduction in (Middle Eocene) on the basis of palynomorph
diversity of the microfaunas and an inferred and charophyte content (Pittau Demelia 1979).
salinity anomaly about 35m above the base of
the marine carbonates marks the onset of a
regression, which reached its acme with the Previous work
deposition of continental coal-bearing sedi-
ments. The resulting heterolithic paralic forma- The first detailed sedimentological-palaeoecolo-
tion, the so-called 'Produttivo' is sandwiched gical work on the coal-bearing Tertiary Sulcis
between shallow marine limestones ('Calcare a Basin was an unpublished study conducted by
Miliolidi') at the base and coarse detrital fluvial the University of Siena (Cocozza et al. 1989).
deposits at the top ('Cixerri Formation') In this study, four major lithostratigraphical
(Fig. 4). Most of the boreholes drilled by units were recognized within the 'Eocene series'.
Carbosulcis reached the top of the Miliolitic The basal unit corresponds to the shallowing-
Limestones Formation only. Good biostrati- upward coastal-lagoonal carbonates of the
graphic markers are restricted to the marine Miliolitic Limestone Formation (Fig. 4). The
carbonates. The basal part of the Miliolitic second and third units roughly correspond to
Limestones contains large foraminifera (Alveo- the coal-bearing ('Produttivo') sequence. The
linids and Orbitolitids) which suggest an Ilerdian second unit was interpreted as a gradual tran-
age (early Ypresian, Early Eocene; Cherchi sition from coastal-lagoonal carbonates through
1983). The age of the coal-bearing formation is brackish-lagoonal and heterolithic coal-bearing
more difficult to determine due to obvious lacustrine-palustrine facies. The latter unit
palaeoecological constraints. However, the is interrupted by an important fining-upward
lowest coal-bearing strata yield charophytes clastic deposit, which has been interpreted as
 EOCENE SULCIS COAL BASIN 53

fluvial in origin. The third unit is lithologically studies has been the subdivision of the coal-
similar to the second, but the coals tend to be bearing sequence into informal lithostratigraphic
thicker. Its upper limit is marked by a second units, and the regrouping of the numerous tiny
clastic episode. The fourth and final unit coal layers into 10-12 multi-seam coal horizons.
corresponds to the Cixerri Formation (partita) This lithostratigraphic scheme was based on
and is characterized by the lack of coal and by lithological predominance criteria and on the
the dominance of coarse clastics. The latter have presence of local marker beds. However, bed-by-
been interpreted as braided fluvial channel bed correlation is not generally possible, except in
deposits. the case of closely spaced boreholes. Even then,
The carbonates of the basal unit comprise a correlation of individual coal seams is proble-
variety of microfacies types, indicating low- matic because of marked seam irregularities. The
energy, shallow lagoonal environments of a wedge-shaped sandstones which erode under-
tropical to subtropical arid coastal zone lying coals, were interpreted as fluvial channels.
(Cocozza et al. 1989). The benthic foraminiferal The coarser clastics of the overlying Cixerri
faunas indicate dominant hypersaline lagoonal Formation were attributed to alluvial fan depos-
conditions, with intermittent freshwater influxes its. A stratigraphical study recently conducted by
(temporary hyposaline conditions; Cocozza Montan Consulting GmbH (Bandelow & Gangel
etal. 1989). Foraminiferal wacke/packstones with 1993) lead to similar conclusions. Although
ostracodes, molluscs, green algae and echino- potential marker beds were identified (including
derms are the dominant microfacies type. Cross- questionable bentonite layers) and the correla-
bedded grainstones with peloids, low-energy tion of coal seams over larger distances between
fibro-radiated ooids, intraclasts and cyanobac- closely spaced boreholes was possible, a bed-
terial oncoids are less frequent. The latter by-bed correlation of the coal seams remained
grainstones enclose corroded larger foraminifera uncertain, due to the combined effect of
with open-marine affinities (Alveolina, Orbito- synsedimentary tectonics (difference in thickness
lites), the presence of which can been related to of coeval strata) and sedimentological events
storm-induced transport. All microfacies types (e.g. wash-out phenomena).
show more or less important bioturbation.
Near-emergence is indicated by plant rootlets,
incipient pedogenesis, and mottling whereas Facies spectrum and distribution
micro-karst phenomena suggest temporary sub-
aerial exposure. The carbonates in the second The 40-70 m thick heterolithic sequence of the
and third unit comprise freshwater-influenced Produttivo Formation is subdivided into four
restricted-marine ('paralic') and lacustrine lime- informal lithostratigraphic units, based on a
stones (Cocozza et al. 1989). The paralic mud/ detailed study of 50 closely spaced cored bore-
wacke/packstones contain abundant smooth- holes in the area of Monte Sinni (Fig. 1). Each
shelled ostracodes, brackish foraminifera (e.g. unit contains one or more parasequences,
Ammonia), freshwater molluscs, charophytes bounded by unconformities which correspond
and dwarf miliolinids. Rare gastropod-bivalve to the erosional bases of the 'detrital episodes'
coquinas (Cyrena, Potamides) occur in their (Fig. 5).
basal part. The lacustrine limestones consist of The boundary between the Miliolid Lime-
mudstones, wackestones and (pseudo) pack- stones and the Produttivo is not clear-cut, but
stones with variable amounts of skeletal grains consists of a gradual transition from restricted
such as those of freshwater gastropods, fresh- marine to lacustrine-palustrine limestone facies.
water bivalves and charophytes. Plant root This boundary represents not an unconformity
pedoturbation and other pedogenetic features but rather a palaeoecological/palaeoenviron-
are common. mental change within the coastal lagoon setting.
The clastic or detrital facies consist of fining- The sudden occurrence of 'paralic' microfaunas
upward sequences of rudites, arenites and silt- (mixohaline or hyposaline conditions) and the
stones. These strata have been related to braided first occurrence of (autochthonous) coal seams,
fiver deposits in a distal alluvial plain setting can be used as criteria for defining the base of
(Cocozza et al. 1989). the Produttivo Formation. This event is char-
Other unpublished reports (e.g. by RIMIN acterized by the mass occurrence of (pyritized)
1990-1991) contain less sedimentological infor- smooth-shelled ostracodes and by an important
mation. These studies focussed on the stratigra- decrease or even disappearance of miliolinids
phical framework of the Produttivo. The clastic (dwarf forms). The Cixerri Formation which
episodes have been again interpreted as channe- unconformably overlies the Produttivo consists
lized fluvial deposits. A major result of these of conglomerates, coarse sandstones and var-
54 R. DREESEN E T A L .

the stacking of analogous parasequences. In

contrast with the unpublished reports referred to
earlier, we consider the detrital episodes not
as fluvial deposits but rather as marine sedi-
ments. They are interpreted as shallow marine
tidal deposits, displaying characteristic subtidal-
intertidal-supratidal upward-shoaling sequences
(Fig. 6). The 'detrital' sediments represent the
lowermost part of each parasequence. The upper
part consists of 'continental' supratidal deposits,
which grade vertically (and laterally) into lacus-
trine and palustrine coal-bearing facies.
The tidal character of the clastics is indicated
by a vertical suite of characteristic sedimentary
structures, whereas tidal subenvironments may
be distinguished on the basis of lithologies and
associations of structures (Terwindt 1988).
Marine fossils are apparently lacking in the
studied shallow marine tidal deposits, despite
indirect evidence for in-situ organic activity such
as intense bioturbation and the presence of
escape structures. Reworked cyanobacterial
mats or oncoids (stromatolites) and fragmented
thick-shelled (mixohaline?) molluscs occur in the
basal part of each parasequence. We suggest that
this apparent lack of in situ organisms must be
related to the extreme harsh environmental
conditions (abnormal salinities) during deposi-
tion of the subtidal and intertidal sediments.
Analogous observations have been made in tidal
sequences from the Late Devonian Psammites
du Condroz Group of the Ardennes in Belgium
(Thorez et al. 1988).
The subtidal facies is represented by relatively
thin (5-20cm) coarse-grained lag deposits
('microconglomerates') overlaying erosional
Fig. 5. Ideal parasequence within the Produttivo unconformities. The lags are composed of grey
Formation, with evolution of relative water depth and
relative sea level (MFS: marine flooding surface; TST: quartz-rich (litho-)calci-dolorudites and (litho-)
transgressive system tract; HST: highstand system calci-doloarenites displaying some grading and
tract; LST: lowstand system tract; EV: evaporite; oblique or cross stratification. The subangular,
PAL/LAC: palustrine / lacustrine; TF: tidal flats. strongly packed pebbles or granules include
Not to scale. various intraclasts such as grains consisting of
calcite and dolomite cement, lacustrine mud/
wackestones, pedogenic carbonates, black peb-
iegated mudstones. The lack of coals and lime- bles, oncoids, stromatolitic crusts, chert, coal
stones is used here as a criterion to distinguish it and mollusc fragments. Euhedral quartz grains
from the Produttivo, although a gradual transi- are common and locally abundant. This subtidal
tion cannot be excluded. facies is interpreted as a thin transgressive
The ideal parasequence or depositional unit unit. It coincides with a transgressive lag, which
within the Produttivo Formation is an upward- resulted from the reworking of underlying
shoaling unit, several metres to about 10 metres or lateral deposits, i.e. the winnowing of fine-
thick. It is bounded by marine flooding surfaces, grained sediments and the accumulation of
coinciding with an erosional unconformity coarse-grained sediments on the ravinement
(Fig. 5) and marking the base of a 'detrital' surface, during shoreface erosion (Swift 1975).
episode. This depositional unit corresponds to a The ravinement surface corresponds here to the
parasequence, in the sense of Van Wagoner et al. flooding surface (MFS; Fig. 5). Because of the
(1988, 1990), and the Produttivo Formation reduced sediment influx (as the shelf area
is composed of a parasequence-set formed by expands the volume of sediment being supplied
 EOCENE SULCIS COAL BASIN 55

Fig. 6. Borehole 67-91: Lithologies, sedimentary structures and inferred tidal subenvironments within clastic
deposits of the Produttivo Formation. Logs a and b refer to basal parts of lithostratigraphic intervals D and C
respectively (see Fig. 7).

per unit area decreases) one of the principal 'sandstones', 'siltstones' and 'mudstones', which
sources of coarse material for transgressive correspond to intensly bioturbated, alternating
deposition is cannibalization of previously calcarenites and carbonaceous calcilutites. Indi-
deposited sediments (Arnott 1995). vidual beds are between ten and several tens of
The intertidal facies consist of a sequence, a cm in thickness, not exceeding 1 m. The latter
few to several metres in thickness, of grey calcarenites and calcilutites vertically grade into
56 R. DREESEN E T AL.

dolarenites and dololutites: stained acetate peels ostracodes) as well as pyritized charophyte
(Friedman 1959; Katz & Friedman 1965; Dick- gyrogonites.
son 1966) and X-ray diffraction indicate non- Individual coal seams never exceed lm in
ferroan and ferroan dolomite (the latter as a thickness, but coal-limestone associations build
cement) increasing from bottom to top (Fig. 7). up sequences several metres thick. The coals are
Kaolinite is omnipresent. Lenticular, flaser and composed of leaf cuticles, spores, pollen and
ripple bedding are most common, whereas sub-ordinate algae. Petrographic analysis of
pervasive pedoturbation (due to plant roots?) several hundreds of samples gives an average
frequently induces destratification. Lower and of 73.3% vitrinite, 11% liptinite, and 5% inert-
upper intertidal subenvironments can be distin- inite (Fadda et al. 1994). The liptinites fre-
guished on the basis of sedimentary structures quently contain alginite, whereas fusinite and
(Fig. 6). Vertically recurrent microconglomeratic semifusinite are common in the inertinites of the
or litharenitic levels suggest stacking of the tidal lower coal seams. Other physico-chemical para-
sand bodies. meters include: volatile matter content of 42%,
The supratidal facies consist of a sequence, vitrinite reflectance values of 0.45 to 0.5%,
several meters in thickness, of grey dololutites fixed carbon of 48 to 52%, average ash content
displaying a rather massive aspect due to intense of 10% and average S content of 6% (Fadda
bio- and pedoturbation. Palaeosols are present et al. 1994). The ash analysis shows a low silica
as proved by the occurrence of mottling and ratio with high iron (24%) and sulphate (17%)
illuviation-oxidation phenomena along rootlets content.
and by the presence of caliche nodules. The The general lack of well-developed seatearths
change from marine to continental supratidal or rooted horizons and stump or stem horizons
conditions is marked by a change in colour (grey (Fadda et al. 1994) suggests that some of the
versus tan/beige) and by pedogenetic features: Produttivo coals are allochthonous: they result
incipient calcretes, rootlets or seatearths related from the reworking of plant remains from
to overlying coals. swampy-marshy zones into subaqueous, near-
The overlying palustrine-lacustrine facies are shore lacustrine areas. Moreover, the presence of
characterized by irregularly alternating coals, alginite in most of the coal seams would indicate
carbonaceous mudstones, freshwater limestones a partial algal origin. The palynomorph content
and marls. The beige to characteristically hazel- of the coal-bearing strata is rather poor and
nut-brown coloured ('nocciola') limestones have badly preserved. The associations are dominated
been deposited in shallow, nearshore lacustrine by herbaceous plant pollen typical of both warm
environments (littoral carbonates). They consist palustrine-savanna and moderate steppe-prairie
of bioclastic and phytoclastic material: plant type environments (Cocozza et al. 1989). The
remains and skeletal debris of fresh-water mol- good preservation of fresh-water mollusc shells
luscs (including limnic gastropods e.g. Planorbis, and charophyte gyrogonites in the coals and the
Paludina, Melanopsis; Cocozza et al. 1989), close association with carbonates suggest that
smooth-shelled ostracodes and charophyte gyro- water acidity was very low. Decimetric coquinas
gonites. Lignite laminae are common and all are sometimes interbedded with the coal-lime-
intermediate lithologies exist between relatively stone sequence in the lowermost part of the
pure, non-carbonaceous limestones and impure Produttivo. These coarse mollusc packstones
coals. Staining shows that the limestones consist locally display erosional bases and contain coal
exclusively of non-ferroan calcite. Strongly clasts. They are almost exclusively composed of
packed monospecific mollusc shell debris may gastropod (Potamides) and bivalve (Cyrena)
account for the characteristic pseudopackstone packstones, suggesting mixohaline environments
texture. Although deep water facies have not (Cocozza et al. 1989). The scoured bases,
been recorded, some limestones are poor in orientation of the shells and indistinct grading
skeletal debris and display a varvoid texture. of the coquinas point to a possible storm-
Dissolution residues reveal only a subordinate induced origin.
amount or even a lack of siliciclastic material For four selected lithostratigraphical intervals
(Fig. 7). The limestones contain numerous roots (A through D), cumulative thicknesses of
and there is evidence for subaerial exposure, such lithology classes have been processed into
as the presence of rhizoliths, Microcodium, isopach maps, using simple kriging contour
desiccation cracks, micro-karst phenomena and routines. The contour maps (Fig. 8) cover an
nodular fragmentation or 'micro-brecciation'. area of about 16 km 2, which approximately
Marls are interbedded with the limestones. They corresponds to the mining project area (Fig. 1).
are generally dark-coloured, carbonaceous, The following lithologies have been selected and
rooted and contain occasional shells (mollusc, grouped for processing: coals (including all dirty
Fig. 7. Borehole 67-91: Lithological-sedimentological log showing mineralogy, clay minerals (right) and
interpreted depositional environment (left). A-D: lithostratigraphical intervals; S.M.: shallow-marine,
R.M.: restricted marine; SB: subtidal; SB/IT: subtidal/intertidal, IT: intertidal, SP (m): (marine) supratidal,
PL/LC: palustrine/lacustrine, PS: palaeosol; Ca: Calcite; Do: Dolomite; Qtz: Quartz; Cl: Clays; KF: K-Feldspar;
K: Kaolinite; I: Illite; C: Chlorite; Sm: Smectite; (10-14C) and (10-14Sm): irregular mixed layers. Shaded lines
represent allochtonous coals. Arrows correspond to upward shoaling trends. Left-hand side of log corresponds to
carbonates, right-hand side of log to clastics and coals.
58 R. D R E E S E N E T AL.

,,.._.,,

e.-.

ff
..=

8~
EOCENE SULCIS COAL BASIN 59
60 R. DREESEN E T AL.

coals and carbonaceous mudstones), lacustrine thickness and lateral extent (Fig. 9): the small
limestones (including all marly limestones), and and thin lenticular sand bodies are interpreted as
the clastics (including 'siltstones', 'sandstones' shallow marine channel or gully fills whereas the
and 'conglomerates'). larger sand bodies correspond to stacked sand
The regressive trend of the Produttivo is sheets. The latter have a lateral extent up to 1
evidenced by a progradation, in time, of coal km and a maximum thickness of 5 m.
from the SW to the NE. Furthermore, a com-
parison of the coal and the limestone isopach
maps reveals a good correlation between both Petrography and geochemistry
lithologies, except for the earliest interval A.
This suggests that the limestones are genetically Methods
related to the coals (corroborating the inferred
lacustrine-palustrine environment). However, More than 100 thin-sections have been studied
the limestones of interval A are not true lacu- with conventional and cathodoluminescence
strine but rather paralic in origin: i.e. they were (C.L.) petrography. C.L. petrography was
deposited under hyposaline, restricted marine carried out with Technosyn Cold Cathodo
conditions indicated by their microfacies and Luminescence Model 8200 Mark II. Operating
microfaunal content. Their maximum thickness conditions were 16-20 kV gun potential, 420 #A
shows a N N W - S S E to N N E - S S W orientation, beam current, 0.05 Torr vacuum and 5 m m beam
which parallels or corresponds to the former width. After careful petrographic characteriza-
coastline. The coals and the clastics are mutually tion of individual authigenic minerals, a micro-
exclusive, as shown by the location and orienta- scope mounted micro-drill assembly (with a
tion of their zones of maximum thickness. The drill-bit of 0 . 5 - 1 m m ) was used to obtain
area of maximum development of the clastics carbonate powders of 1-10mg for isotopic
roughly corresponds to that of the paralic belt, analysis. However, complete separation of indi-
which would corroborate their relation with the vidual phases was not always possible. Isotopic
marine environment. The stacking of zones of analysis of carbon and oxygen was performed
maximum thickness of clastic rocks in the NW on a Finnigan Mat delta E stable isotope ratio
corner of the studied area (compare the succes- mass spectrometer. Carbonate powders were
sive siltstone/sandstone/conglomerate isopach dissolved in >100% orthophosphoric acid at
maps in Fig. 8) might indicate the existence of 25~ All data have been corrected following
a narrow depression or a preferential pathway, procedures modified from Craig (1957). The
such as a channel or a 'slough', for the clastics in isotopic compositions are expressed as 0 values
this area. The clastic bodies have a variable in per mil (%0) difference from the PDB

Fig. 10. (1) Photomicrograph of non-stained calci-dolomite. Dolomite and monocrystalline quartz rock. Locally
a chert particle (ch) as well as some spherical chalcedony bioclasts (s) occur. Scale = 160 #m; PPL; (borehole 4/B
76~tr-47.50 m). (2) Photomicrograph of an euhedral quartz particle with carbonate (c) and lath shaped anhydrite
(A) inclusions, surrounded mainly by monocrystalline quartz and algal micrites (M) particles. Notice that the
latter are severely affected by compaction. Scale = 80 #m; PPL; (borehole 4/B 76~tr-38.30 m).
(3) Photomicrograph of quartz particles consisting of different phases which locally possess a euhedral outline.
A lath shaped internal arrangement is accentuated by the presence of elongated calcite inclusions. Locally some
minute lath shaped anhydrite inclusions (A) occur. This particle is surrounded by micritic algal clasts.
Scale = 80 #m; PPL; (borehole 43/90-433.25 m). (4) Photomicrograph of quartz particles with ghosts of
pseudomorphosed lath shaped crystals displaying a felted texture. This particle is dominantly surrounded by
dolomite as well as quartz particles. Notice that some of the latter possess a euhedral to subhedral outline.
Furthermore some micrite algal particles (M) are present. Scale = 80 #m; NPL; (borehole 43/90-447.70 m).
(5) Photomicrograph of different types of particles, namely a length slow chalcedony particle (CH) with dolomite
inclusions (D), a laminated micritic algal particle (M) and a micrite particle with relict sponge spines (S).
Scale = 80#m; PPL; (borehole 43/90-433.25 m). (6) Photomicrograph of well-rounded polycrystalline quartz
particle surrounded by dolomite. Typical is the undulose extinction as well as the trails of minute inclusions
within the quartz phases. In the lower left corner part of a monocrystalline quartz grain with sometimes lath
shaped calcite inclusions occurs. Scale = 20 #m; PPL; (borehole 47/90-477.60 m). (7) Photomicrograph of
intensely compacted micritic algal clasts next to dolomite and quartz particles. Notice the microsparitic nature
(MS) of the algal clast on the left side of the picture. Scale = 85 #m NPL; (borehole 67/91-377.30 m).
(8) Cathodoluminescence photomicrograph of Fig. 10.7. The fine tubular texture within the algal clast as well as
recrystallisation textures become more apparent. Notice the presence of a zoned calcite particle with truncated
edges between the algal clasts. Furthermore dull red dolomite particles are easily distinguishable from the non- to
darkbrown luminescing quartz particles. Around some of the dolomite particles a dull luminescing cement (D1) is
present. It precedes a deep red phase (D2). Scale = 85#m; CL; (borehole 67/91-377.30 m).
EOCENE SULCIS COAL BASIN 61
62 R. DREESEN ET AL.

international standard. Reproducibility, deter- (1980) and Swennen & Viaene (1986). According
mined by replicate analysis of samples NBS 19 to these authors such evaporite replacement
and NBS 20, is better than 0.1%o for oxygen and silica diagenesis preferentially develops within
0.05%o for carbon. No correction for dolomite or schizohaline settings.
siderite dissolution by phosphoric acid has been A similar origin can also be proposed for
applied. some of the microflamboyant, concentric and
spherulitic chalcedony particles (Fig. 10.5) con-
taining anhydrite inclusions or their pseudomor-
Petrography of sedimentary particles phosed outlines. However, not all chalcedony
particles can be shown to have an evaporite
A detailed study of the (litho-)calci-dolorudites related origin. The overall proportion of 'chert'
and (litho-)calci-doloarenites of the Produttivo particles is less than 3%. Within some poly-
Formation revealed that the detrital grains crystalline quartz grains anhydrite-related relicts
mainly consist of quartz and carbonate (dolomite have also been observed. However, most of the
and calcite) particles (Fig. 10.1). Well rounded polycrystalline quartz particles consist of a
chert as well as feldspar particles (K-feldspar and mosaic of intricate or well defined quartz
subordinate plagioclase) are present in low crystals. Sometimes, these crystals display a
concentrations (<5%). Cements are in general parallel alignment and an undulose or gradual
scarce and dominantly consist of dolomite, phase extinction (Fig. 10.6). The grains are often
ferroan dolomite and locally some calcite. well rounded and are most likely of meta-
Authigenic kaolinite and pyrite content locally morphic origin.
can grade up to 5%. Intracrystalline porosity Under cathodoluminescence the majority of
between dolomite phases as well as secondary these quartz particles possess a dull to dull
porosity locally can be in the order of 15%. brown luminescence (Fig. 10.8; Fig. 11.5-6).
Monocrystalline quartz particles exceed 95% Carbonate grains, which locally make up to 80%
of the total quartz population. Two dominant of the detrital content (Fig. 10.1) dominantly
types can be differentiated. Firstly, rounded to consist of dolosparite. Dolomicrite, micrite and
subrounded quartz grains with minute (< 1 #m) sparite grains are also present. Most dolosparite
inclusions which often are arranged along particles have a grain size which is similar to that
intraparticle planes. Most of these grains possess of neighbouring quartz grains. In transmitted
a uniform extinction and their origin is not light a cloudy core can often be differentiated
determinable. Secondly, euhedral to subhedral from a transparent rim. They are both in optical
quartz phases which are characterized by lath- continuity. Under C.L. this corresponds to a
shaped inclusions (Fig. 10.2-3). Few rounded reddish brown to brown central part and a dull
examples also exist. The inclusions, which can be brown rim (Fig. 11.6). The centre is often broken
30 by 5 #m in size, either are aligned parallel to in different pieces and rehealed by the dull
each other, or are scattered within their host. A brown or deep reddish dolomite phase. This,
zonal arrangement is less common. Petrographic together with the fact that the rim is missing
characteristics as well as SEM-EDX data, where adjacent grains touch each other, points
indicate that these lath-shaped inclusions consist towards a post-compactional origin for the rim.
of anhydrite or calcite. Other inclusions are Most of the larger carbonate grains, which
framboidal pyrite and rhomb-shaped dolomite. often are severely affected by compaction,
In some cases, lath-shaped inclusions have been consist of micrite or microsparite (Fig. 10.7).
completely replaced by mega-quartz, their out- Within most of these pyrite- and organic matter-
line is often still visible (Fig. 10.4). In many cases enriched micrite grains faint radial and con-
a typical felted texture is present. Important here centric microtextures are recognizable. Under
is the fact that in none of the cases has a dust rim C.L. these textures become more distinct
been identified in the inclusion-bearing part of (Fig. 10.8). Bright yellow tubes within a dull
the quartz grains. Thus the euhedral to subhe- brown matrix testify that these micrite particles
dral outline does not relate to post-depositional correspond to disrupted and transported poro-
authigenic quartz overgrowth. Furthermore, stromate algae. Within these clasts lozenge-
some grains clearly show transportation fea- shaped calcite pseudomorphs after gypsum are
tures. Broken edges crosscut both quartz and the locally present (Fig. 11.1). C.L. characteristics of
lath-shaped inclusions. These curious quartz the microsparite particles clearly indicate that
phases correspond to transported early diage- these correspond to cemented and/or partly
netic replaced evaporites. These textures are recrystallized porostromate algae (Fig. 10.8).
similar to the megaquartz phases described by Some of the cements within these porostromate
Folk & Pittman (1971), Milliken (1979), Arbey algae reflect a complex cementation history. In
 EOCENE SULCIS COAL BASIN 63

addition to these algal fragments micrite clasts the nearly time equivalent Planu Sartu Member
with sponge spicules have also been identified (Bechst~idt & Boni 1989). The complex zonation
(Fig. 10.5). Within lithostratigraphic unit D pattern recorded in the calcite cement particles
some micrite clasts with pedogenetic textures, would then reflect the complex diagenetic
such as circumgranular cracks and glaebules are history recorded within these source area
present (Fig. 11.2). rocks. Evaporite moulds and some gypsum
The sparite grains are most easily recognizable platelets have been described from the 'Dolomia
after staining (Fig. 11.3) or under C.L. In the Rigata' (Schledding 1985). However, their
latter case they display a number of bright occurrences are minor and they are not silicified.
luminescing textures typical for cements such as Whether quartz pseudomorphs after evaporites
different types of zonation patterns, sector zona- occur in the nearby hinterland is not clear. In
tion, variation in cement-type succession (e.g. this scenario one would expect also to find many
acicular followed by blocky, etc.) (Fig. 11.5-6). more Cambrian allochems (e.g. oolites, intra-
The truncated particle terminations indicate that clasts) and reworked Cambrian fossil debris (e.g.
cementation did not occurred in situ but that echinoids, Archaeocyathids, trilobites) which
these are sparite clasts which have been eroded occur in time-equivalent strata, which is not
and transported. Partly broken and compacted the case. Euhedral quartzes could also have been
cement particles (Fig. 11.6) also support this derived from nearby Triassic outcrops in SW
interpretation. Many of the intensively zoned Sardinia (but no longer exposed because of
cement grains reflect a broad spectrum of varia- extensive erosion) or from the Triassic in
tions in cementation conditions, most of which southern France (given the palaeogeographic
are compatible with shallow meteoric diagenesis position of Sardinia, close to the Pyrenees;
in their source area. Also textures which may Fig. 3). Quartz bipyramids with anhydrite inclu-
correspond to marine diagenesis (acicular sions are quite common in the Keuper of the
non-luminescent crystal crusts), as well as Corbi6res area (Debelmas 1974; Jalfrezo 1977).
speleothem-like textures have been identified. These Triassic evaporite-bearing sediments were
Large blocky uniformly dull or bright yellow unroofed by the uppermost Cretaceous, and
particles may represent reworked shallow burial certainly by the Palaeocene, and were thus
cements formed either in reducing or suboxic providing clasts.
conditions or burial cements. A broad spectrum Another scenario would be that these particles
of cemented lithologies was evidently being are quasi synsedimentary in origin. This would
eroded during Eocene times and their excellent imply that during Eocene times (time equivalent
preservation state suggest a nearby source area. with the deposition of Miliolitic Limestone
Other unusual particles observed include: Formation or Produttivo Formation) a carbo-
mono-axial chalcedony sponge spicules, up to nate-evaporite succession was deposited which
20#m in diameter (Fig. 11.3) which are also underwent complex diagenesis. This diagenesis
incorporated in larger chert particles; oolites, would be characterised by differentiated calcite
which commonly enclose a quartz nucleus; in cementation, dolomitisation and selective silici-
some cases lath shaped anhydrite crystals or fication of evaporites. This scenario is supported
their calcitized pseudomorphs occur within the by the existence of algal clasts displaying a
quartz grain; bioclasts such as gastropods, complex calcite cement zonation pattern and the
ostracodes, charophytes, bivalves, which occur presence of gypsum pseudomorphs (Fig. 11.1).
within discrete layers. Development of such a hypersaline setting with
Some of these particles, such as poly- and evaporite ponds would fit into the general
monocrystalline quartz, are extrabasinal in palaeo-environmental context, but whether suf-
origin and most likely are derived from the ficient time would be available for such diage-
Palaeozoic sedimentary and intrusive igneous netic overprinting can be questioned. The
hinterland. However, for the dolomite particles, alkaline depositional conditions, however, are
the calcite cement grains ('sparites') and the favourable for silicification (Arbey 1980).
evaporite-bearing quartz grains, an extrabasinal Within such a setting dolomitization could also
origin is less obvious. An extrabasinal origin can be one of the dominant diagenetic processes: in
be argued since the immediate (actual) sur- fact concomittant dolomitization and silicifica-
roundings of the Eocene Sulcis basin consist tion of evaporites has often been reported in
mainly of Cambro-Silurian formations including literature (e.g. Swett 1965; Tucker 1976 and
Cambrian carbonates. The dolomite particles others). In order to generate clasts, these strata
could be derived from the Lower Cambrian would subsequently have to be eroded, which
Dolomia Rigata or the overlying Grey Dolomite could be explained by block-faulting which has
Formation and Black Limestones Formation or been reported during Eocene time in the Sulcis
64 R. D R E E S E N E T AL.
 EOCENE SULCIS COAL BASIN 65

basin. This mechanism may thus have given rise Early diagenetic products
to a nearby emergent source area for the
considered particle types. This block-faulted In the lower part of the Produttivo Formation
barrier could perhaps also explain the develop- but much more common in the Miliolitic
ment of a lacustrine-palustrine basin. Within Formation, biomold development followed by
this scenario the major difference in shape circumgranular intraparticle calcite cementa-
between the euhedral to subhedral evaporite- tion is common in the bioclastic horizons.
bearing quartz grains and the well to sub- Also recrystallization phenomena can be
rounded mono- and polycrystalline quartz observed and most likely relate to the stabili-
particles could be easily explained. However, in zation of aragonite and high Mg-calcite
the extra-basinal scenario this difference might components and/or neomorphism of fine crys-
simply relate to the degree of reworking of talline shell textures. Within these layers as
quartz particles from older sandstones. well as higher in units B and C (Fig. 9),
framboidal pyrite may locally exceed 5%. Its
Diagenesis origin is here tentatively related to the activity
of sulphate reducing bacteria which implies a
Unravelling the diagenetic history of the regular supply and infiltration of marine water
'Produttivo' strata is complicated not only by the to provide the sulphate ions. Higher upwards
existence of diagenetic particles such as dolomite in the sequence (unit D) pyrite is less common.
and 'sparite' grains (Fig. 11.5-6) but also by the Here, siderite cement and siderite nodules are
severe compaction of most lithologies (Fig. 10.7; more common and occur close to the devel-
Fig. 11.2). Furthermore, cements are not very opment of pedogenetic textures (glaebules,
common. In general a distinction between very circumgranular cracks, desiccation features,
localised early diagenetic products and post- etc.). The fact that siderite instead of pyrite
compactional phases can be made. In Fig. 12 a preferentially formed suggest a shift towards
generalized paragenetic succession is given. methanogenic related processes. Around some

Fig. 11. (1) Photomicrograph of a micritic algal clast with calcite pseudomorphs after lozenge-shaped gypsum
crystals. Scale = 80 #m; NPL; (borehole 54/90-332.65 m). (2) Photomicrograph of glaebule particle with
circumgranular cracks cemented by several generations of calcite. Small disortic textures (Do) are locally
discernible. This particle is surrounded by quartz and micritic algal particles. Scale = 80 #m; NPL; (borehole
58/90-503.85 m). (3) Photomicrograph of calci-dolorudite where the four most common particles are visible
namely: a) quartz (Qz), b) dolomite (D: brownish hue, not stained), c) calcite (C: red stained), d) micritic algal
particles (M) which became very dark due to staining. One circular section of a chalcedony bioclast (S; sponge
spicule) is also discernible. Notice the presence of a blue ferroan dolomite phase which is affecting especially the
dolomite particles. This ferroan dolomite phase also occurs in compactional cracks. Scale--85 #m; NPL;
(borehole 67/91-377.60 m). (4) Cathodoluminescence photomicrograph with non- to darkbrown luminescing
quartz (Qz) and dull red dolomite particles (D). In the central part some dolomite rhombs (DR) occur. The bright
yellow (B) and orange yellow (O) particles corresponds to calcite particles. The following cements are present:
a) dull luminescing dolomite (D 1) which only develops around some dolomite particles, b) red luminescing
dolomite cement (D2), c) brown yellow to yellow calcite cement (C) characterized by sector zonation, d) purple
luminescing kaolinite (Ka). Notice that between D2 and the calcite a corrosive contact exists (see arrows).
Scale = 85 #m CL; (borehole 67/91-377.30 m). (5) Cathodoluminescence photomicrograph of calci-dolorudite
with in the central part nicely zoned calcite cement particle. Here the truncated texture of the cement is clearly
visible. Apart from non- to darkbrown luminescing quartz (Qz) and dull red dolomite (D) particles a bright blue
luminescing K feldspar (Ka) is present as well as many micritic algal clasts (M) and other bright luminescing
sparite (B) particles. Kaolinite (Ka) is the only easily recognizable cement. Scale = 85 #m; CL; (borehole 67/91-
377.30 m). (6) Cathodoluminescence photomicrograph of calci-dolorudite with similar composition as plate 3.5.
Here the central calcite cement particle displays compactional cracks which are cemented by brown yellow calcite
(C). Post-compactional dull luminescing dolomite (D 1) and red luminescing dolomite (D2) cement is also present.
Between these dolomite cements and the calcite cement a corrosive contact exists (see arrows). Scale = 85 #m; CL;
(borehole 67/91-377.30m). (7) Cathodoluminescence photomicrograph of contact between a quartz (Qz) calci-
dolorudite in the upper part consisting of dolomite (D) particle and a lower part composed of rhombic dolomite
crystals which most likely developed within a sheltered pore. The position of the bioclast is now taken over by the
bright yellow luminescent calcite (C). Between the dolomite rhombs as well as within the calcite cement some
purple luminescent kaolinite (Ka) occurs. Notice that the kaolinite booklets in the calcite clearly are floating and
are corroded (see arrows). Scale = 85 #m; CL; (borehole 67/91-377.60 m). (8) Cathodoluminescence
photomicrograph with the classical particles of a calci-dolorudite (see plate 1.5 for abbreviations). In the central
part a calcite cement particle (CC) is present. Scale = 85 #m; CL; (borehole 67/91-363.16 m).
66 R. DREESEN ET AL.

DIAGENESIS

EARLY .- BURIAL

SEDIMENTATION

PEDOGENESlS (L)

SIDERITISATION (L)

FRAMBOIDAL PYRITISATION (L)

CALCITE I PRECIPITATION (L)

BIOMOLD DEVELOPMENT
& RECRYSTALISATION (L)

AUTHIGENIC QUARTZ DEVELOPMENT

COMPACTION 1 STYLOIJTISATION
& COALIFICATION

NON-FERROAN DOLOMITE (NFDI)

FRACTURING EPISODE I

FERROAN DOLOMITE (FDI)

NON-FERROAN DOLOMITE (NFDII)

SECONDARY POROSITY DEVELOPMENT

KAOLINITE FORMATION

FRACTURING EPISODE II

BLOCKY BRIGHT YELLOW TO

BROWN CALCITE II

L ) = only locally developed

Fig. 12. Generalized paragenetic succession of diagenetic events in the Produttivo Formation.

of the monocrystalline quartz particles a thin phase possesses a dull lunminescence (Fig. 11.6).
authigenic rim is present, however it is not It is only present within pores which survived
determinable whether it formed before or after compaction and is absent at grain to grain
compaction. contacts. This cement is often covered by
ferroan dolomite which luminesces deep red
(Fig. 11.6; FDI). The irregular to wispy contact
Compaction between both cement phases as well as the fact
that ferroan dolomite spots also occur within
Interpenetrating to sutural grain to grain con- the dolomite grains and along cleavage planes
tacts in addition to the existence of sutured and (Fig. 11.5) indicate that most of the dolomite
non-sutured seam solutions testify to an impor- phases were partly to entirely recrystallized by
tant episode of compaction. Low amplitude ferroan dolomitizing solutions. The ferroan
stylolites are present locally. The micrite/micro- dolomite also occurs as rehealing phases in the
sparite particles are affected, while dolomite and compactional cracks of broken dolomite grains.
'sparite' particles show similar textures to the The many thin fractures which are cemented by
quartz grains (Fig. 10.8). The period during ferroan dolomite testify to an important phase
which burial gave rise to the compaction features of fracturing preceeding ingress of these solu-
most likely corresponds with the major period of tions. In the central part of some of these
coalification. fractures a non-ferroan blocky dolomite cement
(NFDII) occurs which has not been recognized
outside the fractures. Whether this was linked to
Late diagenetic products a fracturating episode is not obvious.
A relatively important late diagenetic episode
Syntaxial non-ferroan dolomite (NFDI) over- was the development of secondary porosity
growths affecting only dolomite particles is often which is most likely related to feldspar dissolu-
present. This nearly inclusion free transparent tion. This is supported by the fact that the
 EOCENE SULCIS COAL BASIN 67

feldspar content in the siderite nodules is an can serve as a standard value against which the
order of magnitude higher than in the surround- diagenetic products can be evaluated. Reported
ing lithologies. Early diagenetic siderite cemen- estimates for Lower Eocene marine carbonates
tation and nodule formation are believed to vary around +0.5 + 5%o Ox80 and +2.3 •
have sealed these parts of the rock so that they 0130 (bulk sediment data reported by Shackle-
were unaffected by late diagenetic processes. ton 1986). The coquina debris and its marine
A relationship exists between lithologies with limestone matrix (Miliolitic Formation) which
high secondary porosity and abundant kaolinite possess values of 0i80 of -5.0 + 0.3%0 and 013C
matrix, as recorded by Giles & Marshall (1986). of -1.30+0.05%o are clearly depleted with
Kaolinite booklets occur within primary inter- respect to Lower Eocene marine values. This
crystalline pores as well as in secondary pores also accounts for stable oxygen and carbon data
(Fig. 11.2-3). A genetic link between feldspar from the Miliolitic Limestone of the Sulcis Basin
dissolution and kaolinite precipitation seems reported by Perna et al. (1994) ( 0 1 8 0 : - 5 . 7 to
likely, especially within a setting where coalifica- -9%o and 013C: -0.6 to -3.3%o). Recrystalliza-
tion occurred. According to Giles & Marshall tion by meteoric and/or warm fluids with
(1986) organic acids liberated during the involvement of depleted CO2, most likely
maturation of organic matter, especially coal, derived either from soil-gas CO2 or from decar-
are efficient agents of feldspar dissolution. In the boxylation reactions within the coal layers of the
case of a closed to semi-closed diagenetic system Produttivo Formation are possible explanations.
ions, liberated during dissolution can give rise to This seems also to account for most isotopic
the precipitation of kaolinite and other authi- signatures of the calcarenites and other detrital
genic minerals such as illite and authi- calcite/dolomite dominated lithologies sampled
genic quartz. The latter, however, have not been in this study. These strata cluster within an area
recognised in the studied strata. defined by 013C of -4.5 • and 0180 of
Finally, after a renewed fracturing episode, -7.2 +0.8%o. Sample 400.00m however is more
fluid channeled along these fractures caused depleted in 0180 (-9.82%0). This may relate to
calcite fracture fill and limited cementation. the presence of minute calcite II veinlets and
A corrosive contact between this bright yellow possibly to recrystallization due to interaction
to brown luminescent calcite and other carbo- with calcite II bearing solutions. One of the
nate phases, especially the ferroan dolomite larger calcite II veins analysed was collected
cement (FDI; Fig. 11.4), testifies to the aggres- from this sample. 013C and 0180 values of the
sive nature of these fluids or to the circulation of glaebules respectively plot around -9.2%o and
undersaturated fluids preceeding cementation. -5.4%o (Table 1 and Fig. 13). The influence of
Within some larger cavities corroded kaolinite soil-gas CO2 in the soil formation is clearly
booklets appear to float in this late diagenetic reflected in the depleted 013C of these pedogenic
calcite (Fig. 11.7), indicating that this calcite carbonates (Salomons et al. 1978; Cerling 1991).
cementation postdates kaolinite precipitation. The oxygen isotope signature is in agreement
A remarkable feature of this calcite cement with a meteoric water dominated system.
is that it only occurs in fractures or large The few sampled siderites are characterized by
(>300 #m) pores. a 013C varying between -0.5 to +2.8%0 and
0180 varying between -4.9 to -8.0%0. The
carbon signature could be interpreted to reflect
Stable isotopes siderite formation in equilibrium with atmo-
spheric CO2. However, based on the bacterial
Table 1 is split in two parts, and gives the 013C micro-textures observed under high magnifica-
and 0180 of the analysed samples. Part A groups tion as well as on literature data (e.g. Curtis
all the samples which consisted of rather pure et al. 1986; Moore et al. 1992), this signature
sedimentary or diagenetic phases, or where based most likely reflects a mixture of different CO2
on microscopic examination, the relative propor- sources of which atmospheric CO2 could be one
tions of different contributing phases can be source. A depleted sulphate reduction CO2 type
estimated. It was not possible to sample calcite I is less likely to be involved since these siderites
and the non-ferroan dolomite I seperately. In occur in unit D where marine incursions less
part B samples are grouped where such an frequently occurred. This is also deduced from
estimation could not be carried out due to the the virtual absence of framboidal pyrite. CO2
presence of too many different components. derived from bacterial fermentation could be
An essential first step in diagenetic studies is involved, however this is not the only CO2
the estimation of the original isotopic composi- source since the carbon isotopic composition is
tion of marine water. This starting composition less enriched in comparison to the + 15%o which
68 R. D R E E S E N E T AL.

Table 1. Oxygen and carbon isotope data of diagenetic and sedimentary components of the
Eocene Sulcis Basin (FD: ferroan dolomite; NFD: non-ferroan dolomite)

PART A 013C 0180

Glaebules in claymatrix -9.25 -5.57
374.00 Glaebules (pure) -9.29 -5.35
Siderite (nodule centre) +2.78 -7.98
359.9 Siderite (nodule edge) +2.38 -6.38
358.90 Siderite nodule -0.47 -4.97
400.00 Calcite vein -4.51 -10.46
403.35 Calcite vein (with pyrite) -4.05 - 11.16

403.35 Ferroan limestone matrix -6.05 -7.78

400.00 Limestone matrix -2.30 -9.82
394.80 Bivalve shells + limestone (70% + 30%) -1.35 -4.68
394.80 Limestone around bioclasts -1.25 -5.29
390.40 Limestone matrix -3.88 -8.06
383.20 Limestone matrix -2.67 -7.13
377.60 Limestone components -5.89 -6.42
363.38 Limestone matrix -4.45 -7.10
355.70 Limestone matrix + < F D -4.43 -6.55
355.40 Limestone matrix, slightly ferroan -3.59 -6.42
Ferroan dolomite matrix +0.11 -4.14
360.30 Ferroan dolomite matrix -8.34 -7.95
359.89 Ferroan dolomite matrix +0.68 -7.42
357.70 Ferroan dolomite matrix (>80% FD) -8.82 -7.62
355.40 Ferroan matrix between FD vein -1.58 -6.97
355.00 Ferroan dolomite matrix (>90% FD) -1.81 -7.44
355.00 Ferroan dolomite vein + 20% matrix -0.87 -6.04
355.00 Ferroan dolomite vein (pure) +0.11 -5.62
355.00 Ferroan dolomite vein (pure) -0.86 -7.55
354.00 (Ferroan) dolomite vein -0.70 -8.56
362.70 Non ferroan + ferroan dolomite vein -9.04 -8.13
359.89 Non ferroan § ferroan dolomite vein -10.96 -8.33

PART B

Limestone/dolomite matrix + FD -3.63 -6.13

377.30 Dominantly FD+limestone/dolomite matrix -4.16 -5.33
377.30 Limestone/dolomite + FD + NFD? -6.11 -6.44
377.30 Dominantly FD + limestone/dolomite -4.40 -6.40
377.10 Dominantly FD + matrix -2.34 -4.21
377.10 FD + limestone § NFD? -3.67 -5.26
375.29 Limestone matrix with FD vein -4.54 -7.62
365.90 Dominantly limestone/dolomite matrix + FD -3.44 -8.04
363.16 Dominantly limestone/dolomite matrix -5.43 -7.01
362.70 Dominantly FD -5.78 -7.07
361.75 Dominantly FD + dolomite matrix 6.69 -8.34
358.90"Dominantly FD + limestone/dolomite matrix -7.54 -7.29
358.25 Dominantly FD in organic rich mud -3.05 -7.57
354.00 Dominantly FD + limestone/dolomite matrix -4.60 -6.50
ML-1 Miliolitic limestone (Perna et al. 1994) -3.30 -7.01
ML-2 Miliolitic limestone (Perna et al. 1994) -0.66 -8.97
ML-3 Miliolitic limestone (Perna et al. 1994) -1.87 -5.10
ML-4 Miliolitic limestone (Perna et al. 1994) -2.07 -6.88
 EOCENE SULCIS COAL BASIN 69

a13C

SIDERITE
FERROAN DOLOMITE
/ T+2
(GROUP 1)
_[+,
a180

-11 -10 -4 -3 -2 -1

MILIOLITIC 11" 11=

LIMESTONE

% . A, 4, 9
CALCARENITE
(CALCITE& DOLOMITEGRAINS)
CALCITEVEINS

FERROAN+ NON FERROAN

DOLOMITE
(GROUP2)
~ .~...- GI.AEBULES

9-10

9 GLAEBULES
~= SIDERITES
9 CALCITEVEINS
A CALCARENITE
~k FERROANDOLOMITE
9 NON-FERROANDOLOMITE
X MILIOLITICLIMESTONE
1~ MILIOLITICLIMESTONESULClS BORENOLES
9 MIXEDSAMPLES

Fig. 13. Plot of carbon and oxygen stable isotope data from the Produttivo Formation.

is typical for the anaerobic (bacterial) carbonate linked is not yet clear. It is therefore proposed
reduction and fermentation processes (Irwin that at least two post-compactional dolomitiza-
et al. 1977; Irwin 1980 and others). tion stages should be differentiated. Both could
Ferroan dolomite veins as well as intensively be related to circulation of meteoric water,
ferroan dolomitized strata have been sampled at however their ferroan post-compactional and
different stratigraphic levels within the Produt- dolomitizing nature point to circulation of
tivo Formation. Their 013C-0180 plot into two evolved fluids. According to their 013C signature
distinct areas. Group I clusters around a 013C of depleted CO2 was not or only slightly involved
- 1 +2%o and 9180 o f - 6 4 - 2 % 0 . The second in the group I ferroan dolomites, whilst in the
group is characterized by depleted 013C values group II ferroan + non ferroan dolomites, CO2
varying around -8.5 4- 0.5%o and 9180 values of derived from decarboxylation reactions should
-7.8 + 0.3%o. In fact this group clusters close to be taken into consideration.
the values of the sampled non-ferroan dolomites The calcite II cements and veins are char-
II with even more depleted 013C values down to acterized by moderately depleted 013C values
-10.96%o and with rather similar olSO-values. (-4.254-0.30%o) and highly depleted 9180
Whether both dolomite types are genetically values (-10.80 + 0.40%o). Such depleted oxygen
70 R. DREESEN E T AL.

values are characteristic of high temperature lithology-type is dominated by the pure palus-
fluids. However, fluid inclusion data are needed trine/lacustrine carbonates. Most of the coal
to correctly evaluate the significance of their layers do not occur in situ but limited trans-
isotopic signature. port is indicated (hypautochthonous coals). The
absence of in situ evaporites, the limited devel-
opment of microkarst and desiccation cracks
Depositonal setting and the fact that the successions are capped with
coal horizons point towards sub-humid climatic
The Sulcis coals most probably originated as a conditions (Platt & Wright 1992). Root devel-
response to rising sea level. They represent in fact opment within the autochthonous carbonates
the upper end member of a highstand system is extensive. The limited pedogenetic features,
tract (Fig. 5). The coarse lag at the base of each such as glaebules and 'micro-nodular' structures
clastic episode corresponds to a transgressive indicate occasional emergence but they become
system tract followed by the intertidal-supratidal more frequent in the upper part of the Produt-
lower member of the highstand system tract. The tivo Formation. Well developed calcretes,
lag is composed of reworked material, including terrestrial gastropods and desiccation breccias
various limestone intraclasts, silicified evaporites which reflect prolonged exposure are absent.
and dolomites. The latter possibly represent the All these features point towards a complex
only relicts of a lowstand system tract, which has environment of marginal marine, brackish and
been completely eroded and winnowed by fresh-water settings. The Florida Everglades
hurricanes (?) before the next marine flooding provides a potentially useful modern analogue.
event. A working model illustrating the succes- This area is characterized by intensely vegetated
sive stages in the development of the ideal fresh-water marshland, swamp and fresh-water
parasequence of the Produttivo Formation is to brackish lagoons. The coastal mangrove
depicted in Fig. 14. It is interesting to note that region may provide an analogue for the Sulcis
the successive flooding events ('detrital episodes') coal swamp. The Everglades has a very low
within the Produttivo Formation apparently topographic gradient and minimal relief (<5m)
coincide with the main transgressive cycles where large areas show dense fresh-water wet-
(3th order cycles 2.3 to 2.6) of Haq et al. (1988) land vegetation (marsh, prairie and swamp
for the Lower Eocene (Ilerdian/Cuisian). Alter- forest) (Olmsted & Loope 1984). Areally the
natively, the silicified evaporites have been saw grass marsh is the most important environ-
eroded and reworked from emerged Palaezoic ment and also the most important peat-forming
rocks (Cambro-Silurian basement) or Triassic environment in southern Florida. The filtering
rocks in the near hinterland and episodically effect of this vegetation possibly explains the
swept into the fresh-water marsh. pure nature of the autochthonous carbonates.
Within the Produttivo Formation two lithol- Lakes, forming areas of algal carbonate sedi-
ogy types can be differentiated. Within the mentation also occur, however, they only make
first type the allochthonous calci/doloarenites up a small proportion of the total area. Wide
dominate. Here, particles clearly have been marshy zones occur in the lower lying areas
transported, however, most of them only over forming ponds and broad, low-gradient vege-
limited distances. The second autochthonous tated or open channels termed 'sloughs'. Water

Fig. 14. Idealized block diagram (not to scale) and successive stages in the development of an ideal parasequence
in the Produttivo Formation (Sulcis Basin, Early Tertiary). 1: LST (lowstand system tract): during a fall of the
relative sea level, several small areas became emerged. Marginal marine facies (with oncoids and stromatolite
mats) as well as evaporitic ponds developed during periods of extreme desiccation (dolomite, anhydrite, gypsum),
whereas the evaporite sediments were affected by early diagenetic silicification. The latter ponds might have been
fed by intermittent water supply (either ephemeral streams or marine incursions). Palustrine facies extended
offshore producing an intermittent marshy vegetation (rooting). 2: TST (transgressive system tract): a rise of the
sea level (vertical arrow) induced a reworking of all the inshore sediments, and triggered their transport (large
horizontal arrow) and accumulation in a more landward position. The reworked sediments cover (displaying a
fining upward trend) consists of residual dolomite (partial dissolution), calcite and limestone clasts, silicified
evaporites, oncoids, fragmented stromatolitic crusts and peat clasts. 3: HST-TF (highstand system tract - tidal
flats): subsequent tidal conditions resulted in the temporary development of subtidal, intertidal and supratidal
subenvironments. The (channelized) tidal sands prograded somewhat farther seaward (large horizontal arrow)
thanks to the available accomodation space. 4: HST (highstand system tract): extensive supratidal conditions, a
relatively high water table in the area and a lack of detrital input lead to the development of extensive lacustrine-
palustrine facies with hypautochtonous peat formation and fresh water carbonates.
EOCENE SULCIS COAL BASIN 71
72 R. DREESEN E T A L .

drainage occurs mainly along these sloughs, but Cambrian in origin as the Cambrian limestones
water flow is sluggish. A similar type of'sloughs' were generally too strongly recrystallized and
may have existed in Eocene time in the Sulcis homogenized (showing twinned and bent crys-
area. These depressions then could have been tals; Maria Boni, personal communication). The
filled by allochthonous sediments. Consequently hypothesis of silicified evaporites reworked from
these sandbodies may not correspond to channel remote Triassic outcrops is not plausible because
fills of braided rivers as previously described of the freshness and the size of the quartz
(Cocozza et al. 1989; Assorgia et al. 1992; Fadda bipyramids, excluding transport over larger
et al. 1994). distances. A nearby Triassic source area is also
Thin (millimetre thick) evaporite layers unlikely: if quartz bipyramids were supplied as
actively precipitate within the surficial desiccated clasts to the Sulcis basin, why are they totally
algal crusts in the central areas of the mud banks lacking in the Miliolitic Limestone Formation?
in Florida Bay. Precipitation of thin evaporites The idea of a synsedimentary origin for the
and peat formation thus occur simultaneously in allochems is supported by the presence of
the Florida setting today, but they form in gypsum pseudomorphs within the porostromate
different sedimentary environments. However, oncoids. Also the complex cement characteris-
the evaporites are not silicified and they would tics within these algal mats could, after rework-
most likely be destroyed if they were trans- ing, generate the 'sparite' particles. Finally, the
ported. If the evaporites were silicified it is nearly non-abraded aspect of the euhedral to
possible that they could be ripped up by tropical subhedral quartz grains replacing evaporites
storms and hurricanes and transported and also supports a very limited transport. Periods
deposited along the coastal levee in the coastal of extreme desiccation, leading to the establish-
swamp and in the sloughs. This may explain the ment of hypersaline conditions within the
irregular distribution of the sandbodies shown in lacustrine ponds (evaporitic carbonate flats)
Fig. 9. may have led to evaporite precipitation, asso-
The marl layers or lenses found below the saw ciated with diagenetic silicification and dolomi-
grass peat in the open marshes of the Florida tization. Subsequently, bypramidal evaporite-
Everglades may represent a modern analogue bearing quartz and dolomite grains could have
for the fresh water carbonates of the Eocene easily been reworked by episodic high-energy
Sulcis coals. The calcium contained in the events and redistributed as clasts. Diagenetic
surficial waters was precipitated, either by lime silicification of coeval evaporitic lacustrine
secreting algae (algal mats) or by the combined carbonate facies might have taken place by
effect of all herbaceous plants present on the leaching of biogenic siliceous mineral matter
carbon dioxide content of the flowing surface from the peats, a phenomenon already reported
water (Spackman et al. 1964). The precipitation from the Okefenokee Swamp and the Everglades
of marl as opposed to peat reflects a rather (Cohen et al. 1987; Andrejko et al. 1983; Cohen
delicate balance between the rate of subsidence 1995). The biogenic silica commonly consists of
(or differential peat compaction or ground water sponge spicules and plant phytoliths. Siliceous
table rise) and the rate of peat accumulation. If sponge spicules have frequently been observed
the rate of subsidence (or water table rise) is too in the calci-dolorudites and -arenites of the
fast, the saw grass peat surface will soon be Produttivo Formation. Silicophytoliths (opaline
covered by an algal mat producing a layer of silica) are commonly produced by sedges and
marl. A few centimetres of difference in water grasses (Andrejko et al. 1983; Cohen 1995): the
depth is all that appears to separate the two latter represented a dominant plant community
environments but the size of the areas involved is in the Eocene Sulcis peats. Biological degrada-
often to be measured in terms of square tion processes play a significant role in silica
kilometres (Spackman et al. 1964). This devel- dissolution and mobility in a peat-forming
opment will continue until the area has been environment. The apparent lack of observed
built up to a level that would permit repopula- spicules and the occurrence of chert lenses
tion by saw grasses. in Tertiary lignites deposited under similar
Although the hypothesis of reworked Cam- conditions to the Ekofenokee peats might be
brian allochems from the hinterland is not a function of such bioerosional activities
entirely dismissed, and euhedral quartzes might (Andrejko et al. 1983). The high SIO2/A1203
well have been derived from unroofed silicified (%) ratios (average 1.95) of the Sulcis coal ashes,
Triassic evaporites, we still favour the idea of suggest an excess in silica possibly related to
coeval evaporitic lacustrine and palustrine car- authigenic biogenic silica (the dominant clay
bonate facies in the Eocene Sulcis Basin. The mineral being kaolinite with a Si/A1 ratio of
reworked calcite allochems are probably not about 1; Szymanski et al. 1990).
 EOCENE SULCIS COAL BASIN 73

Facies assemblages characteristic of fluctuat- grains and that of dolomite cement clasts in the
ing, evaporitic and non-evaporitic lacustrine latter deposits suggests reworking of evaporitic
episodes have been recorded in the Tertiary facies. Petrographic evidence favours the idea
Narbonne Basin from the northern Pyrenean of a synsedimentary origin for these particles,
foreland in southeastern France (Szulc et al. although reworking of silicified evaporite-bear-
1991). Silicified evaporite horizons have been ing Cambrian or Triassic rocks from the nearby
recorded in the basal Cretaceous palustrine hinterland cannot be totally rejected. This
deposits of the Rupelo Formation in North working model implies periods of extreme
Spain (Platt 1989). Minor lenticular gypsum and desiccation during the Eocene, leading to the
nodular anhydrite have been described from the establishment of evaporitic conditions within
carbonate dominated coal-bearing lacustrine the lacustrine ponds of the Sulcis Basin
facies of the Oligocene Calaf and Mequinenza marshes. Palustrine carbonate marshes and
sequences in the Ebro Basin, NE Spain (Cabrera evaporite carbonate flats have been described
& Saez 1987). Here, paludal carbonate marshes from elsewhere in the stratigraphic record, and
or swamps and evaporitic carbonate flats devel- simultaneous evaporite precipitation, fresh
oped in the outer lacustrine fringes at times of water carbonate deposition and peat formation
lowered water level. Similarly, evaporites have can actually be observed in the Florida Ever-
been recorded from shallow carbonate lacustrine glades, which is believed to be the most
facies in the Permian of the Aragon-Bearn Basin appropriate modern analogue.
(Pyrenees) (Garc6s & Aguilar 1992): pseudo-
morphs after gypsum and evaporite replacement This study has been conducted with the financial
textures formed in restricted or littoral palus- support of the European Commission (Convention
trine areas during low stand lake levels. E.C.S.C. n~ 7220-AF/214). We thank It. Marco Slavik
and Ir. Gianfranco Manconi (Carbosulcis S.p.A.,
Cortoghiana) for access to data. We are most indebted
to MM. Giorgio Sardu and Giancarlo Contini
Conclusion (Carbosulcis S.p.A.) for help with sampling and
description of the cores, and to MM. Marc Bauwens,
Detailed sedimentological-petrographical analy- William Vaesen and Pierre Blavier (I.S.Se.P., Li6ge)
sis of cores from autochthonous and allochtho- for assistance with thin section preparation, figures
nous lithology types of the Produttivo For- and photographs. Dr. Romeo Flores (USGS, Denver,
mation, results in a revised depositional model Colorado) is thanked for the stimulating discussions
for the Eocene coal-bearing strata of the Sulcis on the origin of the clastic sand bodies. A special note
of thanks goes to Paul Guion (Oxford), Michael Dusar
Basin in Southwest Sardinia. The Florida
(Brussels) and Stanislav Oplustil (Prague) for their
Everglades are considered as a modern analo- careful reading, constructive criticism and helpful
gue of the Produttivo Formation: a tropical- suggestions, improving the content of the original
subtropical coastal marsh, adjacent to restricted manuscript. Finally, we thank Maria Boni (Naples)
lagoons with low tidal fluctuations. Mangroves for the information on the Cambrian carbonates of
lining the muddy coastlines allowed grass SW-Sardinia.
marshes to expand behind them and formed
an efficient trap for sediments carried by the
flood tide. After initially prevailing restricted
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correlazione relative al 'Produttivo' dei sondaggi & MURRU, M. 1989. Caract&isation de l'Ilerdien
a carotaggio continuo della miniera di M.Sini. continental dans le domaine ouest-mrditrrranren.
Relazione conclusiva sui lavori svolti. Internal Comptes Rendus de l'Aeaddmie des Sciences, Paris,
report Carbosulcis S.p.A. 308, Srrie II, 689-695.
SALOMONS, W~ GOUDIE, A. & MOOK, W. G. 1978. TERWINDT, J. H. J. 1988. Palaeo-tidal reconstructions
Isotopic composition of calcrete deposits from of inshore tidal depositional environments. In: DE
Europe, Africa and India. Earth Surficial Process, BOER, P. L., VAN GELDER, A. & NIO, S. D. (eds)
3, 43-57. Tide-influenced Sedimentary Environments and
SALVADORI, A. 1979. II Bacino Paleogenico del Sulcis. Facies. Sedimentary and Petroleum Geology,
Ricerca di correlazioni biostratigrafiche. PhD Dordrecht, Reidel, 233-264.
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Cagliari, Sardinia. Late Precambrium of Finmark, Arctic Norway.
SCHLEDDING, T. 1985. Fazies, Geochemie und Palgio- Sedimentary Geology, 16, 193-204.
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Sedimentary Geology, 14, 1-43.
 Turkish lignite deposits
H. I N A N E R & E. N A K O M A N

Faculty of Engoleering, Department of Geology, Bornova, Izmir, Turkey

Abstract: The distribution of lignite deposits in Turkey is such that in general the Eocene
lignites are in northern Turkey, Oligocene lignites are in northwestern Turkey, Miocene
lignites are in western Turkey, and Pliocene-Pleistocene lignites are in eastern Turkey. Only
the Oligocene lignites are paralic deposits, the rest being formed in a limnic environment.
Turkey has about 8.4 Gt of lignite reserves of which 3.9 Gt are the exploitable reserves. Most
of the known lignite deposits in Turkey are of low calorific value and have high contents of
ash, moisture and total sulphur. Almost 80% of the total reserves have calorific values below
2500 kcalkg-1. The lignites having low calorific values are generally consumed in power
plants. The lignites having relatively high calorific values are exploited for domestic and
industrial use in the country. The majority of Turkish lignite deposits are worked in open-pit
mines, but there are also some underground operations.

In this article general information will be given determined in the whole of Turkey. Some
about the stratigraphies, reserves, qualities and 115 000 km 2 have been explored, 40 000 km 2
mining methods for the major lignites deposits have been investigated in detail, and more than
of Turkey. These deposits have been explored 1.1 Mm have been drilled during evaluation.
and evaluated by the General Directorate of
Mineral Research and Exploration (MTA),
and exploited using various mining methods by
the Turkish Coal Enterprises (TK|). Coal General information about lignite deposits
exploration is ongoing with geological mapping of Turkey
and drillings in the several lignite fields. Gen-
erally, large deposits are mined by T K i and low The distribution of lignite deposits in Turkey is
reserve (small) deposits are mined by private such that generally the Eocene lignites are in
enterprises. northern Turkey, Oligocene lignites are in north-
According to recent studies (MTA 1993), western Turkey, Miocene lignites are in western
there are 181 well explored lignite deposits and Turkey, and Pliocene-Pleistocene lignites are in
98 lignite deposits which require further inves- eastern Turkey (Fig. 1). Only the Oligocene
tigation. There is very little information about lignites were formed in a paralic environment.
many of the privately small lignite deposits. Up The rest of the Turkish lignite deposits were
to now, 8.4Gt of lignite reserves have been deposited in a limnic environment.

_._-, k ,, ) ._./.~.
/~Demirhanh ~ ) -
~)~,6...*..v)'e e L A c K ~ ~_ A s E A /'~ "~"a

> . / M a _ _ i l a m ~ ~ V A ~ir "Ollu ~. ,_,

Homs~an ~.~
BURSA 13uk AI 9 ERZURUM j
9 9 De ikorK~l 9K o 9 Refahffe o .... t~" "
l~lrpllar 9 YOZG,AT5o(" url ~l~lll
~2 )
_V~AN~oVAN (-~

. . . . . . ;..; % Tufonbeyfi ADIyAMAN 9"'-'1 t .

<~ ~ S,~keeAYOiN L~. . . . ~ V ~ oKONYA KAHRAMANMARA~ ~ O /.~-'~..-J ./"
I v~-~'I v ~ \ ki o C~l~si /'-.. "v"
in ~ahinali i ~ B~ROUR ]/JBeysehir I r
. . .~. .' ~ 9 Vataw i Hale ~ HARAMAN ~ /I l'~"

Er--~ek ~-.-v" II E o c e n e L i g n i t e s
o 9 Oligocene Lignites

ITERRANE 'P Pliocene Lignites

Fig. 1. Distribution of lignite deposits in Turkey.

From Gayer, R. & Pe~ek, J. (eds), 1997, European CoalGeologyand Technology,

Geological Society Special Publication No. 125, pp. 77-99.
 -'~ 0

.~ o

v, ~o5~ ~ OZ Z~

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~ +

e~

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C',.1 r ~tNI "~" .,.,~

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80 H. iNANER & E. NAKOMAN

Eocene lignites the locations suitable for coal deposition. These

are the deposits of: Mengen, Merke~ler, G6yniik,
Eocene lignites are located in very limited areas Sorgun, (Teltek and Tosya (Fig. 1).
in Turkey, because marine conditions prevailed Eocene lignites were deposited in closed basins
until the end of the Oligocene over much of the with a basement generally made up of the
country. Coal formation occurred in only small Palaeozoic or Mesozoic rocks. Coal seams are
islands in the Mesogene Sea. Eocene lignites developed usually between marls. These coals
occur in northern Turkey parallel to the bound- are laterally restricted and usually not thick.
aries facing Anotalia within the Pontide system There are one or two coal seams 0.90-6.00m
which was unaffected by tectonic movements, at thick. Lignites are bright, brittle and have good

j . / Oemirhanh "~" 2
,,.....,~'__ O. _ OKIRKLAREli \
9 ",~ EDIRNE V~e k
BLACK SEA
\ ~ 0 Saray
f "J ~ Edir k~ ~ $ a f ~ , i a r ~ " ZON GULOAK

J Hask~y TEKIRDAr ~ n
) 9 5TANBUL 0 Mengen
9 f" ,,AlOMalkara~ ~"~
\j" Ahmctpasa ~ _ _ _
OMerke~ler
,T J MARMARA SEA
|

BO. A
E) AQ 0 Beypazam
Sa~,rlar _murmu B9 9Altda rnar
0 Devecikona#l ~ - i v i l i
~ lrpl l ar Or Kele$
BA LIKESiR Hamzaok 9 Harmanalan O
O "~_ 9 Davutlar 9Oomaniq B a h crek ~y
TLi'kpiyal, Cak.r~oursunbey O TUncbilek .
Tav.~nh 0 Seyit6mer
9 ~Kozlui~ren
Cinge t'-~- neni~ I |

'~
,,,
~d
=rhala
""t~ ~-.--Beni~. 11
ua'ar - - e _ ~ e . ~

Ey~ez Merkez
Evci,er
I.~ktar Soma
0
KUTAHYA

Gediz

0 MANiSA 0 Hararnikby
:::C:;bIZMiR 9KurucjOI

I/gin

z BcyTechir G. KONYA
AYDIN ~'~ E)
O DENiZLi ~ Avdanclk
,O'keO O~ahinali Q J ~ 9
Beysehir
~ Eskihi asa~_ p'~Jrcjut ~Ka'- Karadik'n 9 kq alar
l,~ M itas,__._.-'~_, o vataOa,, ....
.. v, _. v ~ S y . ~~ Bayw
Karacannsar. ~ M ' '~=' -

~ ~4ralan~~"~ Eki zkOy

~" ~ ,) '-1 0 D e p o s i t
~ " L f~ ~ !e S e c t o r
o Zsk
~__-~/~ ...........
~~/~---' ....
. ', I~1 STUDY
~:1 AREA M E 0 I T E R R A N E A N
I
I
"

Fig. 2. Lignite deposits and sectors of Western Turkey.

 TURKISH LIGNITE DEPOSITS 81

quality. Some of deposits have a high total Extensional tectonics started in the Middle
sulphur content (between 1.25% and 9.60%). Miocene and still continues in this area. The
Reserves are small (Table 1). age of lignites is overwhelmingly the Middle
Miocene (Akgtin & Akyol 1992). Intensive flora
cover which grew in the tropical-subtropical
climatic conditions resulted in the accumulation
Oligocene lignites of thick peat deposits in structually active limnic
basins. The flora cover became poorer with the
The Oligocene paralic lignites are generally found
cooler climatic conditions from the Late Mio-
in northwest Turkey. Among these deposits are:
cene up to the end of Pliocene (Akgfin & Akyol
Saray, Malkara, Demirhanh, Harmanh, ile, and
1992). Because of this, there are very few Late
Vize. There are some other small lignite deposits
Miocene lignites in western Turkey.
at Kale in southwest Turkey and Sereflikoqhisar
Some of the most important Miocene lignites
central Turkey which probably formed on islands
are: Muf~la region (Yata~an-Milas) deposits,
(Fig. 1). Eustatic sea level changes took place
Soma, Beypazan, Seyit6mer, Tunqbilek, Orha-
during the Oligocene, resulting in the formation
nell, Keles, Devecikona~l, ~an, ~lrpdar, Sahi-
of these paralic lignite deposits. Coal seams are
nali, S6ke, Gediz, Dursunbey, Alpagut, Oltu,
numerous but thin in these deposits. Reserves
A~kale, Bahqek6y, Kemaliye, and Ermenek
are higher than the Eocene lignites, but the
(Table 3).
quality is poorer (Table 2).
Miocene lignites have very high reserve
capacities. These lignite-bearing formations lie
unconformably on basement rocks of the
Miocene lignites Palaeozoic and Mesozoic. Lignite seams are
underlain by a fining-upward sequence of con-
The Miocene lignites are generally located in glomerates, sandstones, and siltstones, and are
fault bounded basins in western Turkey (Fig. 1). overlain by marls, limestones, tuffites and also

~..~_....~._j~s,,oP ~
KASI"AMONU ~ ~ ~ B&lkaya K.-. ~
o ~ "- ,
/sp,r
otP~ e
..
9 5utkans
o ~r .~
Tosya Alpagut Cettek O ,
0 0 ~...,..~..~,\
Orta Ayvak~r | o HOrasan
0 | Q Askale
0
CANKIRI CORUM Refahiye O i "\.,,
O ERZURUM ~.~'
ANKARA 5orgun SiVAS O ",~
| | O Q ERZ~NCAN Karhova Erci~ L
Baheeh~y
o ~ZGAT Kemaliye o
Kangal 0
Hamal ~ Etyemez t.- 3
Kalbur'~aym | AN .~
~ et eflikochi~r BiNGOL !
| ~-.. -!
KAu Afsin- Elbistan
~.~ 0
0
Tufanbeyll Go'lba~ ,.. .~. "~ 9
KONYA /'~" .v-.~..,.j ~ . / r \
o p ADIYAMAN
O |
KAHRA'NANM ARA,~
KARAMAN /
| ' " ADANA .-'"
o Province
o Deposit
enek Tp t ! 9 Sector
0 25 krn,
Z
I ~ STUDY AREA

Fig, 3. Lignite deposits and sectors of Eastern Turkey.

 ,,..a

o= , ~ o

b
~ ..~Z
~05~ 0 ~0~ ~0 D~O ~ 0 ~ 0 ~ 0 0 ~Z 0 Z

.0

o goo ~o o ~ g o o g o o o o o g o o go o
+

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~C

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~ ~o ~ o ~ ~ ~ ~ ~ ~ ~ ~ - ~

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 ,-1

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s ZZ 0 ~ 0 0 0 ~ZZZ 9 0 ~Z

~gg googoo o~ oo~176go~ o~ Io~ o~ o~ g I

~ O~ O~

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.~ . m ~ . ~ . mo o o o . o o ~ ~ m~
<,~

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.~ o
 ~ 0 ~

~a

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gggg gggogoo o o~176 ,

~ D 0
O~ . . . . .

<,._.

,x 8~
 TURKISH LIGNITE DEPOSITS 85

recent alluvium. Although there is a great recrystallized limestones. The Paleocene is repre-
variation in the lignitic quality of the region, sented by marls and limestones. The Eocene is
(between 1335 kcal kg- 1 and 4500 kcal kg- 1) the divided into two, with the ipresian made up of
Miocene aged lignites are generally good in sandy and marine limestones, and sandstones
quality. Lignite seams are few, usually one or two and the Lutecian, comprising seven units (Kaya
and rarely three, and their mineable thickness & Dizer 1984). The Lutecian starts with fossili-
is 1.00-25.00metres. The majority of these ferous limestones at the base, followed by Marls
deposits are worked as open pit mines, although and limestones. Stratigraphically the lignite
there are also underground mines in the region. bearing bituminous shale layers are found near
The lignite reserves of western Turkey.make up the base. The upper levels are made up of smelly
33% of the total Turkish reserves (Inaner & limestones, highly fossiliferous marl-limestones
Nakoman 1993). and platy marls, whereas the Upper Eocene is
represented by agglomerates, conglomerates and
sandstones. These rocks have a Quaternary cover
of slope debris (Fig. 4). There are two coal seams,
Pliocene lignites an upper and lower, with an average thickness of
5.00 m. The percentage of average moisture, ash,
The Pliocene lignites are generally located in and total sulphur in the original coal are 9.70%
eastern Turkey (Fig. 1), where subtropical 20.98% and 9.25% respectively and a calorific
microclimatics enabled some peat to accumulate value of 4755 kcalkg -1. The proven, probable,
in limnic basins. The Pliocene lignite deposits possible, and total reserves are; 23539760;
are: Af~in-Elbistan, Bey~ehir, Ilgan, Kangal, 39736697; 14690000; and 78016350 tonnes
Orta, G61ba~l, Karhova, Tufanbeyli, Erci~, respectively (Table 1). It is worked by longwall
Ispir, Horasan, and Refahiye. mining.
These are limnic deposits. The basement is
generally Palaeozic or Mesozoic limestones,
ophiolotic rocks, recrystallized limestones, meta-
morphic schists and serpentinites. Coal seams Malkara deposit
are very few, usually one or two. Mineable seams
are thick (between 1.00 m and 39.58 m) but there The Oligocene Malkara coal deposits are located
are sterile partings within the seams. Most of in the northwest of Tekirda~ Province in
these lignites have high moisture and ash European Turkey (Fig. 1). The sectors are
contents (25.31-53.42% and 11.38-36.37%), Ahmetpa~a and Hask6y (Fig. 2). Thirteen coal
and low calorific values (1083-2239 kcal kg-1). seams are developed in a sandstone-marl series,
The average calorific values are about but only three seams are mineable (Fig. 5). The
1000kcalkg -1. However, these lignites have coal has an average quality (Table 2), with
usually large reserves (Table 4). These lignites contents of moisture, ash, and total sulphur in
are generally consumed in power plants. Depos- the original coal of 25.30% 33.29% and 1.29%
its such as Ispir, Erci~ and Refahiye which have respectively, and calorific value varying between
low reserves are used for regional domestic 2014 to 2317kcalkg -~. The total reserves are
heating. 11.595357 • 10 6 tonnes. The coals are worked
by both open-pit and underground mining.
There is currently no production in the area.

Descriptions of selected Turkish

lignite deposits Mu~la region (Yata~an-Milas) deposits
The following descriptions include examples
Lignite-bearing Neogene sediments cover large
with higher reserves from the Eocene, Oligocene,
areas in the districts of Yata~an and Milas
Miocene, and Pliocene.
situated in the province of Mu~la in southwest
Turkey (Fig. 1). These deposits are Turgut,
Eskihisar, Bayar, Ba~yaka, Tlnaz, Karacahisar,
Mengen deposit Sekk6y, Ekizk6y, (~aklralan, Htisamlar and
Alatepe (Fig. 2). Stratigraphically these 11
This Eocene deposit is situated in the northeast deposits are very similar and can be summarized
of Bolu Province in northwest Turkey. The together:
basement is made up of Palaeozoic metamorphic The Kerme Formation lies unconformably on
and igneous rocks, and Mesozoic sandstones and a basement of Palaeozoic gneisses and schists,
 o
~'~ ~ ,,
~o

~ o
N ~z
~o5~ 0 Z OZ 9 0 Z Z ZZZ Z~ Z 9

,.o

0 0 O 0 ~ 0 0 0 0 0 0 0 O 0 0 O 0
0 0 O 0 ~ 0 0 0 0 0 0 0 ~ 0 0 O 0
0 0 O 0 ~ 0 0 0 0 0 0 0 ~ 0 0 O 0

~ ~.+ ~

0 O 0
0 0 0 0 0 ~ 0 0 0 0 0 0 o 0 ~ 0 0 O 0

o~ ~-~

~9 ~_,~
i ~~
~'~
~ ~ I ~ O o l l l l l ~ l

o~ ~ ~o ~

8~ . ~ ~ Inl

= = ~ ~ = o . = ~
 TURKISH LIGNITE DEPOSITS 87

AGE LI THOLOGY EXPLANATIONS

QUATERNARY Slope debris

. . . . . . . .
, . . . . . . . . . , Sandstone
i . . . . . . ....
UPPER EOCENE. . . . . . . . . Conglomerate
o ooooo ooo o
o ~, o o o oc Agglomerate
_Tl.lT I-L-i
T2
-- T - i- - t --~ Fossiliferous limestone
-iT)T1 T IT
I 9 I I I ~ Smelly limestone
I I I I - Marl

~ Coat s e a m ( t o p )

EOCENE ~ Coal seam( bottom )

Bituminous mar[

J I I I ~ Marine limestone
I I I I
I. I. I, I SQodstone ~
I I I I-~
I l l l
PALAEOCENE J I 1 I Limestone

Recrystollized limestone
CRETACEOUS
. . . . . . S a n d s t o n e

PALAEOZ01C
~--~=~-~ Metomor~ic and
"--'1 Igneous rocks

F i g . 4. Schematic stratJgraphic section of the Mengen Deposit.

and Mesozoic marbles. This formation contains Soma deposit

occasionally 1.50-2.00 m thick lignite seams, the
majority of which are not economically exploi- This Miocene deposit is in the district of Soma
table, and are not developed across the whole which is in the north of Manisa Province in
region. The overlying Turgut Formation is made western Turkey (Fig. 1). The sectors of this
up of conglomerates, claystones, siltstones, deposit are; Eynez, Merkez, I~klar, Tarhala,
sandstones and gravelstones. A 20m thick ~inge, Dualar, Evciler, Deni~ I Deni~ II, Kozlu6-
lignite seam occurs between the Turgut Forma- ren and Tfirkpiyale (Fig. 2). Stratigraphically
tion and the overlying Sekk6y Formation. This these deposits in the Soma lignite region show
in turn is succeeded by the Yataf~an Formation similar characteristics (Fig. 7). The basement
consisting of gravelstones, claystones, sand- is made up of Palaeozoic metamorphic schists
stones, tufts, marls and limestones, and by the and greywackes, and Mesozoic crystalline lime-
Miler limestones which are only locally devel- stones. The lignite-bearing Miocene sediments,
oped. Alluvium overlies the Neogene sediments consisting of units of gravelstones-sandstones-
(Fig. 6). clay, marl and limestones, lie unconformably on
Only one seam of 3.30-17.50m mineable the basement. There are two coal units; the main
thickness. This seam has the following average seam at the base of the marl and the middle
quality: moisture 19.38-39.19%; ash 18.54- seam in the middle-top parts of the limestone.
50.14%; and total sulphur 2.35-5.00% all The Pliocene sediments, lying unconformably on
in the original coal, and a calorific value the Miocene sediments, are made up of coloured
varying from 1434-2671kcalkg -1. There are clayey sandstone, tuff-marl-agglomerate, gravel-
706.159 x 10 6 tonnes total proven reserves and stone varved clay and silicified limestone-tuffite
60000 X 10 6 tonnes probable reserves. Total (Nakoman 1971). The upper coal seam unit is
reserves are 766.159x 10 6 tonnes (Table 3). present in the coloured clay-sandstone units.
There are open-pit mining operations in some Unconformably overlying the Pliocene sedi-
of these sectors, using either dragline, or ments are Holocene units which are made up
excavator and truck methods. of terrace gravels, alluvium and slope debris.
88 H. INANER & E. NAKOMAN

AGE LITHOLOGY EXPLANATIONS

QUATERNARY Alluvium

T T T T T]"
Sandstone, ctaystone,
marl, tuff
PLIOCENE
A A A A AA
A A A Basalt
A A A A
A A A A

m Coal seam( top )

Sandstone, marl

OLIGOCENE
Coo[ s e a m ( m i d d l e )

Mctrt

Coal seam ( bottom )

Sandstone

Conglomerate

PALAEOZOIC Gneiss

Fig. 5. Schematic stratigraphic section of the Malkara Deposit.

Andesites and basalts cover very large areas in Beypazarl deposit

the south and north of the Soma Region.
The three coal seams in the Soma region, Beypazari is 100 km northwest of Ankara and
described above, vary in mineable thickness from contains Miocene lignite deposits (Fig.l). The
deposit to deposit. The bottom, main seam, sectors of this deposit are; A B, and Altdamar
makes up the major part of mineable deposits in (Fig. 2). Pre-Neogene rocks in the region are
the region, except in the Deni~ I and Deni~ II represented by Palaeozoic metamorphic schists
sectors, where only the upper seam is mined. The and Palaeocene-Eocene Klzdbaylr Formation.
coal properties are given below for the Soma coal The coal-bearing t~oraklar Formation is made
region. Average coal thickness is 2.00-25.00m. up of cyclic sequences of sandstones, agglomer-
On an original coal basis the average moisture ates and tuffites. Four formations containing
is 12.24-30.28%, the ash 30.00-46.54%, the volcano-sedimentary rock units above the
total sulphur 0.93-3.52% and the calorific t~oraklar Formation are the Hlrka Formation,
value 1486-3428 kcal kg -1. The total reserves with bituminous shales and natural soda, the
for these sectors are 601.255725 x 106 tonnes Karadoruk Formation of solely limestones, the
proven, 54.571977 x 106 tonnes probable and Pliocene Softa-1 Formation of sandstones and
22.764500 x 106 tonnes possible reserves, giving claystones, and the Softa-2 Formation of chalks
a total reserve of 678.592202 x 106 tonnes. Both and clayey limestones. Pleistocene unconsoli-
open-pit (truck and shovel) and underground dated gravels and Holocene terrace gravels,
mining operations (longwall mining with sub- slope debris and alluvium overlie the Neo-
level caving) are employed in the area. gene volcano-sedimentary rocks (MTA 1993).
 TURKISH LIGNITE DEPOSITS 89

AGE LITHOLOGY EXPLANATIONS

i,

QUATERNARY Alluvium ( 20 m.)

Limestone ( 50 m.)

~ " _ ~ " 7 --"TL";'.o--. . . . .

r T T, Grovelstone, claystone,
.'7.2-............
. ~ o o T ;-'." 7 . - sandstone, conglomerate
~ marl (150m.)
MIOCENE
Coal seam
...................
.L'.'--" : - ' . " ' . ' - - "':- Conglomerat e, sandstone,
:.-7._.-7 ....~_7_" -7-.~: claystone ( 200 m.)
..................
.......... . .........
o~,ooo=,,- 0 %,'o-eo
o-o-o-,, * o--- 9
'{ i "ii i i ! )':'.:.: :':']ii:. Sandst0ne, marl ( 200 m.)
...................
.............
Coal seams
Marine limestone
i .............

MESOZOIC ILi[~ Mot ble

--r

PALAEOZOIC
Gneisses

Fig. 6. Schematic stratigraphic section of the Mu~la Region (Yata~an-Milas) Deposit.

Neogene volcanics erupted from the begining (Fig. 1). The Domani~ region, which also has
of the Neogene intercalate with all formations coal, is to the north of this region. The oldest
(Fig. 8). rocks in the Tun~bilek area, which form the
Two coal seams are present, varying in basement are Palaeozoic metamorphic schists
thickness between 2.64 and 6.00 metres. The and crystallized limestones, and Cretaceous
percentages of average moisture, a s h , and total ultrabasic rocks. The basement is unconform-
sulphur in the original coal are 14.83-26.44%, ably overlain by the Miocene and Pliocene units.
25.36-48.70% 2.79-4.04% respectively, and the The Miocene units start with compact clastic
calorific value is 1989-2839 kcalkg -1. The total formations and continue with a clay-marl
proven and workable reserves are 390.3175 • sequence. The Tungbilek coal seam occurs in
106 tonnes and 236 • 106 tonnes respectively. the lower parts of clay-marl sequence. Fresh
The coal is worked by underground mining, water limestone and silicic limestone layers are
using a fully-mechanized longwall method. present at higher levels (Nakoman 1988).
The Pliocene is 300m thick and starts with
clastic sediments which are transitional upwards
to agglomerates and tuftites (Fig. 9). The fresh
Tunfbilek deposit water limestones divide this series into two parts;
andesitic volcanic rocks overlying tufts, tuffites
The Miocene Tungbilek coal region covers large and agglomerates which in turn are overlain by
areas in the west and the north of the Tav~anll basaltic lavas. The Quaternary is made up of
district belonging to the Kiitahya Province slope debris. There is a single Miocene coal seam,
90 H. INANER & E. NAKOMAN

AGE L[ THOLOGY EXPLANATIONS

QUATERNARY Alluvium,
slope debris

VV V VvVvVvVvV V Volcanic r o c k
PLEISTOCENE Tuff, tuffite, l i m e s t o n e
T T T T Claystone, s a n d s t o n e
,'~": 2 '~-:" : : .~':'- ' "-~":'~
Q o o o o o
T T T T A g g l o m e r a t e , tuff, tuffi te
TT TTT T T
PLIOCENE Marl
Coal s e a m ( t o p )
Sandstone, c laystone

Coal s e a m ( m i d d l e )

I Limestone
1 1
I I 1
I I I
MIOCENE
Mar[

Coal seam ( bottom )

-o - o _o_o_o Claystone, sandstone

MESOZOIC Limestone

PALAEOZOIC Metamorphic schists

Fig. 7. Schematic stratigraphic section ofthe Soma Deposit.

which is 0.90-14.75m thickness and contains conglomerates and sandstones followed by blue
several laterally impersistent layers and lenses. green coloured basal clays and by the main seam
The percentages of water, ash and total sulphur (bottom seam). The main seam is covered by
in the original coal are 10.65-14.35%, 38.08- clays with diatoms and marls with bituminous
48.85% and 1.46-2.25% respectively and the marls. The top seam overlies these claystone and
calorific value is 2021-2657kcalkg -1. The marls. The Pliocene concordantly overlies the
proved and probable reserves are 270.850 x 106 top seam seam, and starts with marl, tuffite and
tonnes and 46.882x 106 tonnes respectively limestone (Nakoman 1988). The youngest unit is
making the total reserves of 317.732x 106 alluvium in the region. The top seam is too thin
tonnes for the region. It is worked both by to be mineable. The bottom seam averages
open-pit and underground mining operations. 16.00m mineable thickness. The percentages of
The opencast mining uses dragline, and excava- water, ash and total sulphur in the original coal
tor and truck systems. Underground mining is are 32.98%, 31.18% and 1.21% respectively,
mainly by longwall with sublevel caving. and the calorific value is 1900kcalkg -1. The
proved reserves are 198.666 x 106 tonnes in the
Seyit6mer region. The seam is worked by open-
pit mining methods with a dragline, excavator
Seyit6mer deposit and truck system.

This area of Miocene coal is near Seyit6mer city

in the west of Turkey (Fig. 1). The basement of
the Seyit6mer region is generally made up of Can deposit
serpentinized ultrabasic rocks (gabbro, amphi-
bolite, diorite, etc.), radiolarites and crystalline These Miocene coals are found in and around
limestones (Fig.10). The Miocene which discon- (~an within the county of (~anakkale in northwest
cordantly overlies the basement, starts with basal Turkey (Fig. 1). The basement is made up of
 TURKISH LIGNITE DEPOSITS 91

AGE LITHOLOGY EXPLANATIONS

,,

HOLOCENE Terrace gravel

0 0 0 0 0
O 0 o 0
PLEISTOCENE o o b o Unconsotidated gravel
o o o o
"'~ 0 0 o

C h a l k , c l a y e y limestone
PLIOCENE =I- I - I - l- (Softa-2 Forrootion)
9 . ._L,&__.:=,=.. S a n d s t o n e ~ c l a y s t o n e
Sof t a - 1 F o r m a t i o n )

T T T T T
Ctaystone, marl, tuff

T T T
_ I l i l

L",'
Limestone

MIOCENE Is Ist I 9
I s l 1"~1) ( Karadoruk Formation)
,,,

Bituminous shale, natural soda

-- ( Hirka Formation )

Coat seam

..a_s.~..:_L..
r~" -, . T . .T_. S a n d s t o n e , a g g l o m e r a t e , t u f f i t e

o o o o o ~ o ~0 _% ( (~ o r a k l ~ " F o r m o t i o n )

C l a y s t o n e , s a n d s t o n e , gravelstor~
PALAEOCENE-EOCENE
. . . . . ( Kizilbaytr Formation)
= = o o = ,,

PALAEOZOIC Metamorphic schists

......

Fig. 8. Schematic stratigraphic section of the Beypazan Deposit.

Palaeozoic phyllites, Mesozoic arkoses, lime- mining methods and is currently mined by
stones, spilite and diapsidic diabases (MTA truck and shovel methods in an open pit mine
1993). The Miocene is represented by lignitic at Can.
clays and tuffite layers reaching up to 400 m in
thickness above the basement. The Pliocene
consists of agglomerates about 300 m in thick-
ness. The Plio-Pleistocene comprises a young Orhaneli deposit
andesitic volcanic suite (Fig. 11). The Quaternary
takes the form of gravel terraces and alluvium. The sectors of Burmu, ~ivili and Sa~lrlar show
There is only one seam with an average mineable similar stratigraphic sequences at the northwest
thickness of 16 m. The percentages of water, ash of Orhaneli in the Province of Bursa (Fig. 12).
and total sulphur in the original coal are 18.21%, The pre-Neogene rocks are made up of schist,
27.90% and 4.20% respectively with a calo- marbles and ophiolites and the Neogene forma-
rific value of 2994 kcal kg- 1. The proven reserves tions of detrital rocks with conglomerates, coaly
which can be exploited by both open-pit and marl and tuffites at the base, and volcanic tufts
underground mines, are 85.387 x 106 tonnes and and lava flows at the top. The post-Neogene
1.5 x 106 tonnes making a total of 86.887 x 106 sediments are Pleistocene gravels and valley fill
tonnes, of which only 73.7 x 106 tonnes are alluvium (Fig. 12). The only coal seam is
workable (Table 3). The deposit has been Miocene in age and hard and differs in quality
worked by both open-pit and underground from sector to sector.
92 H. INANER & E. NAKOMAN

AGE LITHOLOGY EXPLANATIONS

i

QUATERNARY Slope debris

i

A AA AA A A A Basaltic [avos
T T T T T T T Tuff
V V V Andesite
V V V V
PLIOCENE
Fresh water limestone

T T T T T T T ~ Tuffite, agglomerate
9 , .

oo o o o o o ..
1 s l s [ '_J.' Silicic timestone
sl- I , J,
Claystone, marl
MIOCENE
Coal seam ( 2-14.75m, )

s 5 s ;
CRETACEOUS UItrabasic rock
sSs 55 S's; s
~ ' Metamorphic schist
~'-"-"--x..
PALAEOZOIC ~ , Crystallized hmestone

Fig. 9. Schematic stratigraphic section of the Tun~bilek Deposit.

A C~ LITHOL O G Y EXPLANATION
S

QUATERNARY Alluvium

I 1 L imestone
l l 1
T T
PLIOCENE
T T Tuffite

Marl

Cacti seam ( top )

Diotomic claystone

Bituminous mar[

MIOCENE
Coat s e a m ( b o t t o m )

Blue green coloured,

basal claystone

Basal conglomerate
Crystallized limestone
PALAEOZOI C R adiolari t e. serpantinize(
uitmbasic rock

Fig. 10. Schematic stratigraphic section of the Seyit6mer Deposit.

This deposit has been worked by both open-pit calorific value is 2134-2850 kcal kg -1 . The proven
and underground mining methods. In the sectors and workable reserves are 32.340 • 106 tonnes
which are mined by open-pit, the percentages of and 29.100 • 106 tonnes respectively. In the
water and ash in the original coal are 21.29- sectors which have underground mining, the
24.45% and 22.47-42.96% respectively, and the percentages of water and ash in the original
 TURKISH LIGNITE DEPOSITS 93

AGE LITHOLOGY EXPLANATIONS

' o"9 . .o, . -,0 -,'o'
QUATERNARY "O. O*- " 0 Alluvium
"'0' " .0 '*.

V V V V
V V V
PLIO-PLEISTOCENE V V V V
Andesite

PLIOCENE Agglomerate

--T -- T --
T -- T _ T Tuff, Lignltic CIoystone
-T T --
yu
UPPER --T--T--T -- C(aystone, tuff
MIOCENE
Cool seam ( bottom )
T T T T T
T T T T T Andesitic Tuff
r T T T T
T T T ConglomeraCe

M ESOZOIC Arkose, spil/t e ond

diopsitic di abase
PALAEOZOIC Phyl lit e

Fig. 11. Schematic stratigraphic section of the (~an Deposit.

coal vary are 21.37-25.29% and 14.46- percentages of water, ash and total sulphur in the
37.88% respectively and the calorific value is original coal are 50.00%, 20.00% and 1.46%,
2294-3412kcal kg -1. The proven and workable respectively, and the calorific value averages
reserves are 13.712 x 10 6 tonnes and 9.6 x 10 6 1050 kcal kg -1. There are 3 357.340 x 10 6 tonnes
tonnes respectively. The total proven and work- of proved and 2.115 x l 0 6 tonnes of workable
able reserves are 46.052 x 10 6 tons and reserves (Table 4). It is being worked by open pit
38.70 x 10 6 tonnes respectively (Table 3). The mining. The Af~in-Elbistan Lignite Establish-
mining is by dragline. ment was formed to feed the largest coal power
station with a capacity of 20 mtpy in Turkey. As
the largest open cast mining project in the
country, six bucket wheel excavators, five sprea-
Af~in-Elbistan deposit ders, five reclaimers and a belt conveyor system
of approximately 55 km in a total length are
The Pliocene Af~in-Elbistan lignite deposit is utilised.
located in southeastern Turkey (Fig. 1). This
deposit is the biggest in Turkey and covers
120 km 2. The Pre-Neogene basement consists of
Permo-Carboniferous limestones, Eocene lime- Bey~ehir deposit
stones and ophiolites (MTA 1993). Neogene
sediments are limnic in character and the This Pliocene lignite deposit is in the west of
sediments below the coal are made up of Konya Province in southcentral Turkey (Fig. 1).
claystone, marls, and gravelstone. Freshwater The sectors of this deposit are: Karadiken,
limestones and Post-Neogene formations, about AvdancN, Ak~alar (Fig. 2). Stratigraphically
80m thick, consist of gravels and sandstones these sectors show smiliar characteristics. The
overlying the coal bearing formations (Fig. 13). basement is made up of Palaezoic metamorphic
The coal has a minumum thickness of 4.00 m, schists and Mesozoic crystalline limestones.
and a maximum of 58.00 m, averaging 39.58 m. Pliocene sediments lie unconformably on the
The coal lies between 10.00 and 150m beneath basement. These are made up of the generally
the surface, with an average depth of 50 m. The loose and occasionally uncemented gravels,
94 H. INANER & E. NAKOMAN

AGE LITHOLOGY EXPLANATION

9 .o . . . .

~ : ai" o..'o. POST

PLEISTOCENE " ' ' o' " " . AUuvium, gravel
, o" 9
,. o .' :o NEOGENE
- o ' . . . , 9

Andesite
./ I .. \. /\/ i
Basalt
T T T T
T T T
T T T T
PLIOCENE T T T
T T T T
T T T
T T T T Tuff
T T T .u_
T T T T
T T T ~
u
T T T T ~ u~
T T T z
T T T T 0
T T T

T g
T T
Tuffite
T
T T ~
UPPER ~ w
(..9
T ~ o
MIOCENE ~- m
Coo[ seom
._ Marl
~l-Iol-l-Iol-I- I~
l--I--I--l-- I--l-l'l
I Ii1--1~1 I-I-
Bosal congtomerate

UPPER A A A A
A A A Ophio[ite
CRETACEOUS ~ A_~ ~
m

Vg~ Marble
PALAEOZOIC ~ ~ / ~ ~(y:)n
rr
Metamorphi c schists

Fig. 12. Schematic stratigraphic section of the Orhaneli Deposit.

sands and clays (MTA 1993). Lignitic beds, Kangal deposit

limestones and marls lie concordantly over these
units. The top levels of the Pliocene are made up This Pliocene deposit which has three sectors,
of limestones. The youngest units are alluviums namely Kalburqaym, Etyemez, and Hamal, is
in the region (Fig. 14). situated 25km south of Kangal city in east
The seam thickness varies between 3.20 to central Turkey (Figs 1 & 3). Stratigraphically
8.14m. The average moisture, ash, and total these sector are very similar. The basement is
sulphur contents in the original coal are: 45.35- made up of the Mesozoic low grade meta-
53.42%, 16.55-27.00%, and 1.09-1.10%, morphic limestones and ophiolites. Neogene
respectively and the calorific value is 1083- sediments lie unconformably on the basement.
1430kcalkg -1. There are 10.276 • 106 tonnes of These are divided into two formations: The
proven reserves which can be worked by under- Kalburqayln and Bicir Formations. The Kalbur-
ground mining method in Ak~alar sector. The qaym Formation begins with gravels at the base,
total proved and workable reserves which could and is overlain by coaly units. The coal and coaly
be worked by open-pit mining, are 218.590 • 106 clays contain gastropod fossils. The Bicir For-
tonnes and 160.326x 106 tonnes respectively mation lies conformably on the Kalburqaym
(Table 4). There is no production in the area. Formation. The Bicir Formation can be easily
 TURKISH LIGNITE DEPOSITS 95

AGE LITHOLOGY EXPLANATIONS

-o 9 ~,.. o .
POSTNEOGENE m . o Gravel, s a n d s t o n e
( 8 0 m thick)
o o o 9 o

1 I ~ ~
I I ] Fresh w a t e r limestones
l I I
1 [ 1
I ] I I
I [ I i
NEOGENE
Coot seom
( 4 - 5 8 m. thick)

Cloystone, marl, grovelstone

oo_Oo o.go_o go_

EOCENE I I I Limestone, o p h i o l i t e
I I l

Limestone
P ERMOCARBONIFEROUS

Fig. 13. Schematic stratigraphic section of the Af~in-Elbistan Deposit.

AGE LIT HOLOGY EXPLANATIONS

OUATERNARY Alluvium

Mort

I I I l
1 1 I Limestone
1 I i I
PLIOCENE 1 I I
Cool seom
-- o ~ o . ~ o - o . . o
- o - . o - .o 9 e. o -
- . o - - o - - - - 0 - o 9 o. Uncemented grovels, sonds
o - - . - ~ . o . - ; o o_.-
o .--.o
- - o
- - o.~.--=.__o
- -
and days
Oo ~ 1 7~6o ----.o'. o .

MESOZOIC Crystallized limestone

PALAEOZOI C Metamorphic schists

Fig. 14. Schematic stratigraphic section of the Bey~ehir Deposit.

distinguishable by its yellowish white coloured upper seam is 1.90 to 12.00m. The percentages
limestones, clayey limestones and marls. Post of average moisture, ash, and total sulphur in
Neogene rocks are volcanics and the Quaternary the original coal are 49.83-52.09%, 19.04-
is made up of terrace gravels and slope debris 21.00%, and 2.02-3.57% respectively, and the
(Fig. 15). calorific value is 1207-1494kcal kg -1. The total
There are two coal seams, the bottom and proven reserves are 202.607 x 106 tonnes. It is
upper. The average thickness of the bottom seam being worked by open-pit (truck and shovel) and
is 8.00 to 15.00 m and the average thickness of underground methods (Table 4).
96 H. iNANER & E. NAKOMAN

AGE LITHOLOGY EXPLANATIONS

QUATERNARY Terrace gravel

A A A
A A A A Basalt
POSTNEOGENE
T T T T T
Tuff
T T T T

Yellowish white coloured

timestone, c l a y e y limestone.
marls
,'T~ ITli!TL,
-l-
- I - l--l-l-l-l-
- J
1 I I I I I
I i i I I I ( Bicir F o r m a t i o n )
I I I I I I I
I J I I I I

NEOGENE
Clayey mar[

Coal seam ( top )

Marl

Coal seam ( b o t t o m )

o . 9 a
L'.~ ~ ~ 9 Gravelstone
o D o o o o ( Kalbur~ay=r= Formation )

Semi- metamorphic limestone

MESOZOIC
Ophiolite

Fig. 15. Schematic stratigraphic section of the Kangal Deposit.

Orta deposit could be worked only by open-pit mining which

is not yet operational (Table 4).
This Pliocene deposit is near (~ankm in north
central Turkey (Fig. 1). The basement consists of
Lower Creteceous crystalline limestone. Volcan-
ism, which continued from the Eocene to the end Karhova deposit
of the Miocene, produced a volcanic cover over
large areas of the region and form the base of This Pliocene deposit is located in the northeast
coal beds. The coal bearing formation lies of Bing61 Province (Fig. 1). The basement is
disconcordantly over the basement volcanics made up of the andesites and the basalts which
and is assumed to be Pliocene in age (MTA are Upper Miocene in age. Above these ande-
1993). It is made up of sandy claystones and sites and basalts, cyclic sequences, consisting
conglomerates, containing thick but low calorific of 10-15m of Pliocene tufts and tuffites and
value lignites. The youngest sediments are 20-25m of siltstone, sandstone, gravelstone,
modern alluvial deposits (Fig. 16). conglomerates and clays, were deposited. The
Two coal seams are developed with an average boundary between this series and the coaly series
thickness of 20 m. The percentages of moisture is made up a band of 2.5 m thick agglomerates-
and ash are; 48.47%, and 28.59%, respectively, tufts. The coaly series follows concordantly
and the calorific value is 868 kcal kg -1 . The total above basement rocks. The thickness of this
proven reserves are 123.165 • 106 tonnes, which series which is made up of clays, clayey tuffites,
 T U R K I S H LIGNITE DEPOSITS 97

AGE LITHOLOGY EXPLANATIONS

QUATERNARY Alluvial deposits

~.- . . . . .

O O O o o o

Coal seam ( t o p )
PLIOCENE Sandy claystone

Coal seam ( bottom )

," -

~ ~ 0 ~ O O O
Conglomerot e
V V V V
V V
V V V V V
EOCENE V V V V V Volcanic rocks
V V V V V
V V V V V
V V V v V

LOWER CRETACEOUS Cryst at[ized |imestone

-1-
Fig. 16. Schematic stratigraphic section of the Orta Deposit.

[ AGE LITHOLOGY EXPLANATIONS

QUATERNARY Alluvium, grovel, travertines

v V V V v
V V V V v V Andesite, basalt
T TTT T TT T Tuff, agglomerate

ii Coat seam ( top )

o " o " "o',' " o.: ,o..

PLIOCENE Sandstone, gravelstone

Coal seam(bottom)

Tuff. tuffite

V V V V
V V
V V V V V
V V V V V
UPPER MIOCENE Andesite, basalt
V V V V V
V V V V V
V V V V V

CRETACEOUS Basement rock

Fig. 17. Schematic stratigraphic section of the Karhova Deposit.

sands and gravels is about 350-400m and The average thickness of the bottom seam is
contains two coal seams. A younger volcanic 8.50m. The percentages of moisture ash and
unit of agglomerates, tufts, andesites and basalts total sulphur in the original coal in the under-
overlies them. The quaternary is represented by ground mining area, are; 43.00%, 24.63%
gravels with travertines and alluvium (Fig. 17). and 0.57% respectively, with a calorific value
98 H. INANER & E. NAKOMAN

of 1663kcalkg -1. The proven reserves are in the range 2500-3000 kcal k g -1, while only 7%
53.884 x 10 6 tonnes. The percentages of moist- are over 3000 kcal kg -1. The calorific value for
ure ash and total sulphur in the original coal of industrial and household use must be greater
the open-pit mining area, are; 46.56%, 24.08%, than 3000 kcal kg -1 (Table 5). Thus 93% of total
and 0.47%, respectively, with a calorific value of reserves are unsuitable for industrial and house-
1458 kcal kg -1. The proven reserves are 30 x 10 6 hold purposes. These low calorific value lignites
tonnes. The coal can be worked by both open-pit can only be used in for power plants. Electrical
and underground mining methods. There is no energy in Turkey is produced in both thermal
current production (Table 4). and hydro power plants, with a total installed
capacity of 20125 MW. Thermal power plants
represent about 52% (10443 MW) of the total
General economic evaluation and results installed capacity, the rest being hydro-electrical
plants. The installed capacity of lignite fired
Estimates of the total lignite reserves in Turkey power plants is 5450MW. These are Af~in-
from studies to date are about 8.4Gt, out of Elbistan, (~aylrhan, Kangal, Kemerk6y, Orha-
which 3.9 Gt are the exploitable reserves. Turk- neli, Seyit6mer, Soma, Tunqbilek, Yata~an and
ish lignite reserves represent around 2% of the Yenik6y.
world total (K6ktiirk 1994). TKI owns 6 Gt of The total saleable lignite production of
these lignite reserves which amount to 72% of Turkey is 45.4Mt, 38.7Mt of which are pro-
the total reserves of the country. 3.2 Gt of the duced by TKi and the rest by private enterprise
TKi reserves are in the Pliocene Af~in-Elbistan (K6kti.irk 1994).
coal basin. Almost 90% of Turkish lignite deposits are
There have been no serious investigations worked as open-pit mines, the remainder being
during the past decade into the development of underground mines. In terms of the technology
the lignite reserves in Turkey. Additional employed in mining lignites, TKI is well
exploration must be carried out to find new equipped for open-pit mining compared with
deposits. A range of information is required underground mining. Underground mining is
before the coal reserves could be utilized in the being carried out either by fully mechanized or
power plants. semi mechanized systems depending on the
Most of the known lignite deposits in Turkey formation and coal seam conditions. Coal
are of low calorific value and have high contents mining in the Beypazan underground mine is
of ash, moisture and total sulphur. 6 Gt of lignite performed by a fully mechanized system and
reserves (72%) are concentrated within 70 impor- similar systems are envisaged for other under-
tant deposits. The lignite reserves, both worked ground operations. Depending on the geological
and unworked, owned by TKI, are classified and mining conditions different mining systems
according to the calorific values as shown in such as dragline-excavator-truck, excavator-
Table 5. truck or bucket wheel excavator-belt conveyor
Almost 80% of the total reserves have systems are used in the opencast mines for
calorific values below 2500kcalkg -1, 13% are coal production and overburden removel. The

Table 5. According to the lower calorific values, the proved and total lignite
reserves in Turkey

Lower calorific Proved reserves (%) Total reserves (%)

value (kcalkg-1) (tonnes • 10 6) (tonnes • 10 6)

>1000 123.2 1.6 265.7 3.2

1001-1500 4367.1 59.5 4519.1 54.0
1501-2000 870.3 11.9 972.2 11.6
2001-2500 674.0 9.2 932.2 11.1
2501-3000 927.0 12.6 1105.3 13.2
3001-3500 324.4 4.4 401.0 4.8
3501-4000 4.3 0.1 28.5 0.3
4001-4500 11.8 0.2 31.8 0.4
>4501 36.9 0.5 118.6 1.4
Total 7339.0 100.0 8374.4 100.0
 TURKISH LIGNITE DEPOSITS 99

Table 6. Areas of utilization for the Turkish/ignites References

Consumption % AKGUN,F. & AKYOL,E. 1992. Palynostratigraphy of the

coal-bearing Neogene deposits in Bfiyfik Menderes
Thermal power stations 67.4 Graben, Western Anatolia. 1st. International sym-
Domestic heating 16.5 posium on Eastern Mediterranean Geology, Pro-
Industrial factories 15.7 ceedings and Abstracts, Adana, Turkey.
Internal consumption 0.4 ALTAr, M., (~ELEBI, E. & FIKRET, H. 1994. Develop-
ment of energy sector of Turkey and projections of
supply and demand (1970-2010), 6th National
Energy Congress. izmir, Turkey (in Turkish).
INANER, H. 8r NAKOMAN,E. 1993. Lignite deposits of
machinery and equipment used in open cast the western T~irkiye, Bulletin of the Geological
operations mostly reflects the latest technolo- Society of Greece, 28]2, 493-505.
gies. Draglines of various capacities are utilized KAYA, O. & DiZER, A. 1984. Stratigraphy of Mengen
in major open cast operations. Coal Basin, MTA Publication, No. 97/98 Ankara,
Lignite is used mainly to generate electricity in Turkey (in Turkish).
thermal power station (67.4%), for domestic KOKTORK, A. 1994. Lignite Sources and Utilization in
heating (16.5%), industrial factories (15.7%), Turkey, Turkish Energy Day, 6th National Energy
Congress, Izmir, Turkey (unpublished, in Turkish).
and internal consumption (0.4%) (Alta~ et al,
MTA, 1993. Turkish Coal Inventory, Ankara (in
1994). The lignites with low calorific values are Turkish).
generally consumed in power plants under state NAKOMAN E. 1971. Coal, MTA Educational Series
ownership. Private lignite companies usually No. 8, Ankara (in Turkish).
supply lignite for domestic and industrial uses - - 1 9 8 8 . Coal Deposits of Turkey, Postgraduate
(Table 6). Lecture Notes, Izmir (unpublished, in Turkish).
 The origin and properties of a coal seam associated with continental
thin micritic limestones, Selimoglu-Divrigi, Turkey
A. I. K A R A Y I G I T 1 & M. K. G. W H A T E L E Y 2

1Department of Geological Engineering, Hacettepe University, Beytepe-Ankara, Turkey

2Department of Geology, University of Leicester, University Road, Leicester LE1 7RH, UK

Abstract: The Selimoglu coalfield is situated at the southeastern part of Divrigi, which is
geographically distinct from the major coalfields of Turkey. A number of thin and lenticular
coal seams and sedimentary rocks occur in the Selimoglu unit of the Ogulbey Formation of
Upper Miocene age. Only one seam, which is produced by an underground method, is
associated with continental thin micritic limestones that have a total thickness of about
150 cm. It has a macroscopically bright appearance and a working thickness of 50-90 cm
(70 cm average). A total of 32 channel samples were collected from the mined seam for
proximate, mineralogical and petrographic analyses. The results of proximate analyses on
an air-dried basis show that the coal is characterized by low moisture content (1.68%
average), high ash yield (24.04% average), high total sulphur content (up to 8.92%) and
high calorific value (5606kcalkg-1 average). The coals average 65.5% vitrinite, 4.5%
liptinite, 2.5% inertinite and 27.4% mineral matter. Desmocollinite is the dominant maceral
in the vitrinite group and calcites in the whole-coal minerals. Carbonate minerals with
irregular shapes are in general early-diagenetic, and occur in desmocollinites in all the
samples. The micritic texture of the limestone shows both diagenetic and authigenic origin in
subaquatic conditions with high pH, but organic debris is allochthonous in origin. The
reflectance values of telocollinite (0.77% Rr) show a high volatile bituminous coal rank. The
random reflectance of telocollinite and spectral maxima (625-661 nm) of sporinites, and
proximate analyses reveal that the thermal history may have been affected by volcanic
activity that occurred in the coal field.

Most Miocene coals in Turkey are of lignite or (1965). The basic geological characteristics of
subbituminous coal rank and are generally the Divrigi region, including the northern
associated with claystone, marl and rarely small part of the study area have been investi-
sandstone. However, there is a lack of informa- gated by Tunc et al. (1991). This present paper
tion about this type of formation in Turkey. The represents an extension of a preliminary study
coal seam, which is produced in an underground by Karayigit (1993).
mine, forms a useful example to assess the
formation of coal associated with continental
micritic limestones in the Selimoglu coal
field. This paper summarizes the geological Methods of study
setting and stratigraphy of the coal field, and
presents proximate analyses, the mineralogic- Representative rock, coal and coaly bituminous
petrographic composition, spectral properties shale samples were collected; from which thin
of some liptinite macerals and the rank of the sections of rock samples were prepared to
coal seam. determine the petrographic composition. X-ray
The Selimoglu coal field is geographically powder diffraction (XRD) analyses were per-
remote from the major coalfields of Turkey, and formed to determine the mineralogical composi-
is situated 20 km southeast from Divrigi (Fig. 1). tion of limestones. In addition, for age deter-
About 30-50 t/day of coal is produced in Coal mination, limestones, marls and claystones were
Mine II (for location see Fig. lb and lc). The sieved for ostracoda, and palynological investi-
region containing the coal field was first investi- gations were made on coals and coaly bitumi-
gated by Wedding (1965), who studied the nous shale. A total of 32 (31 samples from Coal
stratigraphy of the region. This was followed Mine II and 1 sample from Coal Mine I for
with studies by Keskin et al. (1984), who revised locations see Fig. lc) fresh, channel coal samples
the geological map and determined a similar that represent the full thickness, including dirt
stratigraphy for the coal field as that of Wedding bands ( < l c m thick) within the seam, were

From Gayer, R. & Pe~ek, J. (eds), 1997, EuropeanCoalGeologyand Technology,

Geological Society Special Publication No. 125, pp. 101-114.
102 A. I. K A R A Y I G I T & M. K. G. W H A T E L E Y

Fig. 1. (a) The stratigraphical sequence of the Selimoglu coal field, (b) simplified geological map around the coal
mines, (e) some macroscopical seam sections, lateral extend of the mining seam and the underground map on a
more detailed geological map (modified after Karayigit 1993).
 CONTINENTAL MICRITIC LIMESTONES, TURKEY 103

collected from the coal seam for proximate, Geological setting and stratigraphy
mineralogical and petrographic analyses.
Proximate analyses (moisture, ash, volatile The location map of the study area, the
matter) as well as total sulphur analyses and stratigraphical sequence of the coal field and
calorific values of all samples were performed simplified geological map around the coal mines
and the reported results expressed as weight are shown in Fig. 1. The Giines ophiolite forms
percentages, except calorific values, and made in the basement in the coal field (Fig. la). It is of
accordance with the ASTM (1991) procedure. Upper Cretaceous age and contains generally
The whole-coal minerals of all coal samples were serpentinized rocks (Tunc et al. 1991). The
identified by X-ray powder diffraction (XRD). Ogulbey Formation rests unconformably on
After identifying all peaks on the every X R D the basement. It has an extensive areal distribu-
diagram, the net area under each diagnostic tion and is subdivided into three informal units;
peak was determined and converted to a per- from base upward, Hantepe unit, coal-bearing
centage for each mineral. In order to determine Selimoglu unit and Hanioglu unit (Fig. 1a). The
the chemical composition of carbonates and Hantepe unit, which has an average thickness of
some silicate minerals, two coal briquettes were 90m, contains mainly thin bedded lacustrine
selected and examined on a JEOL 8250 electron micritic limestones (Fig. la) that are composed
microprobe. of calcites.
Maceral analyses were determined using a The Selimoglu unit only hosts coal seams
reflected light microscope (Leitz MPV II) with a throughout the coal field and the thickness can
32x objective and oil immersion (noil :1.518) on reach up to a maximum of 295 m. In the lower
polished briquettes. Ordinary white light from a part of the unit, reddish mudstones and minor
tungsten lamp and blue light, K510 barrier filter sandy limestones and thin sandstones (<20cm
for determination of liptinite macerals were used thick) are more common. In the middle and
for illumination. The analyses are based on upper part, the unit consists of laterally dis-
counting 500 points on each sample and the continuous rocks ranging in grain size from
reported results are expressed as volume per- conglomeratic sandstone to claystone, and also
centages of the various macerals and minerals. coal seams and limestones. At the top, a laterally
Petrographic constituents of the coals were extensive coaly bituminous shale (about 100cm
determined using the information given by thick), which can be used as a marker in the coal
ICCP (1963; 1971) and Stach et al. (1982). field, is present. The conglomeratic sandstone
Random reflectances of vitrinite (telocollinite occurs as a cross-stratified channel fill sequence.
and desmocollinite) were measured with a Most of the thick-bedded sandstones contain
minimum of 50 points on every briquette using pebbly channel lags. Both the conglomeratic
the same microscope with a 50• oil immer- and thick-bedded sandstones display erosional
sion objective, sapphire (0.551%R) and glass bases, and they are interpreted as fluvial
(1.23% R) standards for calibration. deposits. Thinner sandstones, with large
During spectral fuorescence emission mea- amounts of calcitic cement, show no sedimen-
surements of liptinite mecerals, a Leitz MPV- tary structures.
SP microscope fitted with a high-pressure Only one coal seam, which is exposed around
100WHg light source, a BG38 and a BG1 Selimoglu village (Fig. 1b and c), is produced by
filter, and a K460 barrier filter was used. underground mining. This seam is associated
Spectral intensities in the range of 460-700 nm with continental thin micritic limestone lenses
were measured and corrected spectral intensi- and bands (Fig. lc), that have a total thickness
ties were automatically produced using a of about 150 cm. The seam has a macroscopi-
connected computer. Some numerical para- cally bright appearance and a working thickness
meters, such as relative intensities, wavelength of 50-90 cm (70 cm average). Its thickness within
of maximum intensity ()~max) and the logarith- the limestones decreases from Coal Mine III to
mic ratio (Q) of the relative intensity of red Coal Mine I (Fig. lc), which presumably relates
(650nm) and green (500nm), were then gener- to subsidence, carbonate precipitation and
ated from them. The principles, basic calibra- organic matter supply in the peat environment.
tion techniques and some applications of The limestones are well cemented and composed
measuring fluorescence in geological samples of calcite. The micritic texture of the limestones
are documented in the work of Jacob (1964; shows both diagenetic and authigenic origin
1973), Pflug (1966), Ottenjann et al. (1975), (Gierlowski-Kordesh et al. 1991), but organic
Teichmtiller & Ottenjann (1977), Teichmiiller & debris is probably allochthonous in origin. Up
Wolf (1977), Robert (1981), Crelling (1983), to 7 other different coal seams (<50 cm thick) in
and Teerman et al. (1987). the unit have no economic significance.
104 A. I. KARAYIGIT & M. K. G. WHATELEY

The lower part of the Selimoglu unit was dried basis. The moisture contents are low and
interpreted to have been accumulated in a average 1.68% (Table 1). In addition, it was
lacustrine environment, but its middle and determined that the moisture contents of the
upper parts are in general thought to represent coals on an as-received basis are less than 5%
an alluvial-fluvial environment in a prograding according to unpublished reports of the coal
lacustrine deltaic system. The mined seam was mining company. This means that the coals are
probably formed in a small, shallow lake or characterized by low moisture contents.
pond on an alluvial plain, whereas the other The coals are also characterized by high
seams occurred in small swamps between fluvial values of ash yields, volatile matter contents
channels. and calorific values (Table 1). The average value
The Hanioglu unit, which has an average of the volatile matter contents on a dry, ash-free
thickness of 500m, contains alternations of basis are calculated as 52.82% from the results
limestone-marl, and claystone-limestone-marl on an air-dried basis. This value shows a
of lacustrine origin. The limestones have a subbituminous coal rank (Unsworth et al.
similar petrographic composition to those of 1991). Whereas the coals, during the volatile
the Hantepe unit. matter determination, produced an agglomerate
An Upper Miocene to Pliocene (?) age, based button showing swelling. This character, as
on ostracod studies, was given to the Ogulbey known, suggests at least a bituminous coal
Formation. In addition, charas and gastropods rank in the ASTM (1991) classification. It
were also found in some samples. All the fossils appears that the volatile matter contents was
appear to be of non-marine origin. The mined increased from the micritic limestones that
seam in the Selimoglu unit does not contain formed in the coals.
sufficient diagnostic palynomorphs to determine The coals are characterized by high values of
its age. However, in some samples collected from total sulphur contents (Table 1). High sulphur
the other coal seams and the coaly bituminous contents in coals are commonly explained by the
shale, some spores and pollens were determined proximity of the original peat to marine waters
as Miocene in age. It was concluded that the during deposition, as the sulphate ions in
Ogulbey Formation was of Upper Miocene age. seawater provide an abundant source of sulphur
The Dejdekar volcanics of Upper Miocene (Casagrande et al. 1977; Cohen et al. 1984;
(or Lower Pliocene?) age are usually massive Given & Miller 1985). Whereas, as mentioned
with rarely columnar jointing, and were intruded earlier, there are no marine overburden deposits
into the Ogulbey Formation. These rocks are
petrographically identified as andesite, trachyan-
desite and dacite. The Yamadag lava flows
are of Lower Pliocene age (Tunc et al. 1991) Table 1. Range and average values of the proximate
and they were petrographically determined as analyses and minerals identified by X-ray diffraction
olivine-basalt. Over these units, Quaternary studies of all the coal samples on an air-dried basis
deposits contain alluvium, landslides and rock-
Analyses Range Average
falls (Fig. la and b).
During field studies, it was determined that Proximate analysis
the nearly horizontalyl bedded Ogulbey Forma- Moisture (%) 1.20-4.00 1.68
tion in the area close to the Dejdekar volcanic Ash (%) 17.86-32.46 24.04
intrusion was tilted up to 70 ~. Even though the Volatile matter (%) 36,08-47.10 39.12
rocks of the Ogulbey Formation above the Total sulphur (%) 4.14-8.92 5.64
intrusion have been mainly eroded, the forma- Calorific value (kcal kg-1) 4284-6312 5606
tion has a circular outcrop (representing a dome Calorific value (MJ kg-1 ) 17.94-26.43 23.47
fold) produced by the Dejdekar volcanic intru- XRD analysis of the whole coal (%)
sion. A number of normal faults in the Ogulbey Clay minerals (30)* 0-8 2
Formation were formed by the volcanic intru- Gypsum (8) 0-8 1
sion (Fig. lb). Quartz (32) 1-16 9
Feldspar (27) 0-28 7
Calcite (32) 33-96 70
Dolomite (27) 0-7 2
Results and discussion Pyrite (32) 1-19 10
Marcasite (3) 0-2 0
P r o x i m a t e analysis
* Figures in brackets are the number of samples
Table 1 summarizes the results of the proximate determined on X-ray powder diffraction (XRD)
and X R D analyses of the coal samples on an air- diagram.
 CONTINENTAL MICRITIC LIMESTONES, TURKEY 105

in the coal field. The high sulphur contents of The dominant mineral in the coals is calcite
the coals can be related to possibly high water (Table 1 and Fig. 2). Pyrite is by far the
table, high pH and low Eh in the calcium-rich dominant sulphide present in the samples;
peat-forming environment (Stach et al. 1982; marcasite is extremely rare. Quartz, feldspar
Roberts 1988). These conditions will be dis- including plagioclase (Fig. 3a) and K-feldspar,
cussed below in the light of the results of the clay minerals, dolomite and gypsum make up
other analyses. the other constituents (Table 1). Plagioclase
and most of the quartz (Fig. 3c) may be of
detritial origin, eroded and transported from
the granitic and dacitic basement rocks that
Mineralogy are exposed in the Divrigi region. Gypsum
was probably of secondary origin; the cir-
The major mineral phases found in the coals on culation of more recent oxidizing meteoric
an air-dried basis were determined by XRD waters may have caused the oxidation of the
analysis. The minerals, their range and average pyrites and the resulting sulphate is precipi-
values are given in Table 1. Two examples of tated as gypsum as secondary minerals in the
XRD traces are presented in Fig. 2. coal seams.

Cm: Clay m i n e r a l s
F: Feldspar
Q: Quartz
C: Calcite
D: Dolomite
Py: Pyrite

Q
Q C PY
A;
C I C
~ i ; ~C : .Co.

9- Z L , . L ~ . . ~'

c ~
Q ~
Cm ~ . CC~ c qC ~

Q o%

][ ' II . . . . I . . . . I .... 1 .... I .... I .... I .... [ .... I .... I .... I .... I 20
5 10 15 20 25 30 35 40 45 50 55 60 65

(CuKot)

Fig. 2. Two examples of X-ray powder diffraction (XRD) traces from the mining seam in the Selimoglucoal field.
Fig. 3. (a) Plagioclases (P) showing some alterations with white zonal structures (A) determined by a scanning
electron microscope image, (b) early-diagenetic corbanate minerals (C), pyrite (Py) within desmocollinite (Dc),
(e) early-diagenetic corbanate minerals (C), quartz (Q) and inertinite (I) within desmocollinite (Dc).
 CONTINENTAL MICRITIC LIMESTONES, TURKEY 107

Table 2. The detection limits of electron microprobe for been derived from the serpentinized Gfines
carbonate analysis, range and average values of the ophiolite.
chemical compositions of early diagenetic carbonate The chemical composition of plagioclase,
minerals analysed on two coal briquettes selected from K-feldspar and quartz and the relevant detection
the coal samples
limits on the electron microprobe are shown in
Carbonate Detection Range Average Table 3. The analysis results of the plagioclase
analysis limits indicate an andesine-labradorite composition.
(%) (n ----43) In addition, some alterations showing white
zonal structures were determined within plagio-
CaO 0.02 22.46-49.21 39.17 clases in a scanning electron microscope image
MgO 0.02 0.27-4.61 1.43 (Fig. 3a). The alteration zone within the large
FeO 0.05 0.01-0.36 0.08 plagioclase grain shown in Fig. 3a was analysed
MnO 0.05 0-0.08 0.03
SrO 0.08 0.02-0.68 0.13 at four points and the total oxide composition
BaO 0.15 0.01-0.22 0.11 was found to be less than 61.87%, in which
CO2 (by difference) 49.00-76.44 59.04 43.39-51.49 SIO2% 0.01-0.05 TiO2, 4.26-5.36
A1203%, 0.01-0.04 CrO3%, 0.04-0.08 FeO%,
n: The number of measurements 0.02-0.03 M n O % 0-0.01 M g O % , 1.58-2.89
C a O % , 2.16-2.39 N a 2 0 % , 0.08-0.19 K 2 0 %
and 0.01-0.03 N i O % were determined. It is
possible that the alteration zone was formed by
The detection limits of the electron micro- chemical weathering of plagioclase in the peat
probe, and the range and average values of the environment, and was later infilled with mainly
elements in the early diagenetic carbonate quartz and small amounts of clay minerals that
minerals in the coals, are presented in Table 2. occurred in peat environment.
The dominant constituent is CaO which has a The chemical composition of the quartz
range of 22.46-49.21% (39.17% average). It is minerals indicates that some quartz minerals are
thought that the lower C a O % values are from almost pure SiO2 (Table 3) and it is possible that
organic materials and/or clay minerals mixed in these quartz minerals may be of detrital origin.
the calcium carbonate. MgO is less than 5% in
the calcium carbonates. FeO, MnO, SrO and
BaO are mainly below detection limits. Minor Petrographic composition and
amounts of dolomite were identified by X R D depositional environment
analyses in the coal samples (Table 1). It is
possible that Mg required for dolomite and The range and average values of the results
found in some calcium carbonates may have obtained from the petrographic analyses are

Table 3. The detection limits of electron microprobe for silicate analysis, range and average values of the chemical
compositions of plagioclase, K-feldspar and quartz on two coal briquettes elected from the coal samples

Silicate Detection Plagioclase (n = 16) K-Feldspar Quartz (n = 7)

analysis (%) limits (n = 1)
Range Average Range Average

SiO2 0.02 53.54-57.91 56.23 63.99 81.66-101.01 89.51

TiO2 0.04 0-0.04 0.02 0.00 0-0.62 0.11
A1203 0.02 25.52-29.10 26.70 17.72 0-0.72 0.13
Cr203 0.04 0-0.04 0.03 0.04 0.01-0.04 0.02
FeO 0.05 0.22-0.47 0.29 0.10 0.02-1.61 0.30
MnO 0.05 0.01-0.03 0.03 0.04 0.01-0.03 0.02
MgO 0.02 0-0.05 0.02 0.00 0-0.22 0.05
CaO 0.02 8.47-12.51 9.59 0.01 0.01-0.32 0.17
Na20 0.02 4.67-6.54 5.87 0.82 0-0.56 0.15
K20 0.02 0.17-0.37 0.28 15.63 0-0.09 0.03
NiO 0.04 0-0.04 0.02 0.02 0-0.04 0.02
Total 97.67-100.52 99.05 98.37 82.68-101.11 90.51

n: number of measurements
108 A. I. KARAYIGIT & M. K. G. WHATELEY

Vitrinite cence colour. Exsudatinite is generally observed

as yellow, yellowish orange, orange and brown.
Alginite shows very strong green fluorescence
colour. Bituminite shows yellow-yellowish
orange, and occurs as a groundmass to alginite
and the other macerals, and is mainly found in a
finely dispersed form mixed with mineral matter.
"7 \* Liptodetrinite is composed of small masses of
liptinite group macerals which are too small to
*i o \* identify as a particular maceral; in many cases in
the coals such masses may be small decomposi-
"7 \* tion products of alginite.
The presence of alginite in coal has an impor-
tant paleoenvironment significance in recon-
~-/ . . . . . . . . . '~ structing the ancient coal swamps. In general,
o 4 8 12 16 20 z4 28 32 3~ 40
alginite and its decomposition products indicate
Liptinite Inertinite
wet conditions in intermontane and platform
Fig. 4. Locations o f petrographic constituents in basins rather than in foredeep basins, and
the form o f a ternary diagram on a mineral-matter alginite-bearing coals can be interpreted as
free basis. subaquatic (Hagemann & Wolf 1989).
More aerobic conditions and oxidative bio-
degradation produce maceral precursors of
the inertinite group from mainly macerals in the
vitrinite group (Stach et al. 1982). However,
given in Table 4, and the constituents are also the amount of inertinite macerals in the coals is
presented in the form of a triangular diagram on negligible, and inertodetrinite is slightly more
a mineral-matter free basis (Fig. 4). The average abundant than the other inertinite macerals
maceral content of all the samples on a mineral- (Table 4). This result indicates that aeorobic
matter free basis is 90.5% vitrinite, 6.0% microorganisms and fires were not significant
liptinite, 3.5% inertinite (Table 4). As shown factors in the peat environment.
by Fig. 4 the petrographic compositions of all In the coals, some minerals show similar
but one sample (which was from Coal Mine I, amounts by both XRD analyses and coal
for location see Fig. lc) are similar to each other. microscopy (Table 1 and 4). During petro-
The dominant vitrinite group maceral is graphic analyses, carbonate minerals, which are
desmocollinite (Fig. 3b and c; Table 4). Desmo- mainly calcite and minor amounts of dolomite
collinite is the dominant vitrinite type of reed determined by XRD analyses (Table 1), were
peats, which accumulated in reed swamps with evaluated in two groups, as early diagenetic
grasses, sedges and ferns and in general require a (syngenetic) and late diagenetic (epigenetic). The
higher water table than do forest swamps (Stach early diagenetic carbonate minerals are generally
et al. 1982). The vitrinite group macerals derive brownish-gray in reflected light and have weak
from organic precursors formed at relatively low yellowish fluorescence colour and irregular
redox potentials (Eh). This suggests that the shape in a clearly microlayered desmocollinite
coals studied were developed in a low Eh. in all the samples (Fig. 3b and c). The weak
Total liptinite varies from 1.7 to 18.8 % on a fluorescence colour probably indicates organic
mineral matter-free basis with the most impor- materials within them. Whereas, the late diage-
tant maceral of this group being liptodetrinite netic carbonate minerals were formed in coal
(Table 4). In addition to the liptinite macerals cleats, and they are black-gray with common
presented in Table 4 a minor amount of alginite polysynthetic twinning in reflected light and no
(or telalginite) was found. Sporinites have fluorescence colour. They were not included in
generally weak yellowish orange and brown the petrographic analysis. Thus, the carbonate
fluorescence. Cutinites are very thin in the minerals given in Table 4 are only early
samples and show very weak orange brown- diagenetic.
reddish brown fluorescence. Resinites have Clay minerals and quartz were black in
yellow-orange brown fluorescence and in general reflected light. Some quartz grains are rounded
occur together with corpocollinite and fluorinite and subrounded, have a 20-40#m diameter
surrounded by cutinites. Fluorinite, which prob- and are of detrital origin. Framboidal pyrite
ably forms from plant oils (Teichmfiller 1974), mostly form circular shaped framboids between
shows strong greenish yellow-yellow fluores- 10-20 #m in diameter. Crystalline pyrite consists
 CONTINENTAL MICRITIC LIMESTONES, TURKEY 109

Table 4. The petrographic constituents of the coals, range and average values of
their volume percentages, and also random reflectances of telocollinite and
desmocollinite

Macceral analysis and Range Average

%Rr measurement

Telocollinite 1.8 (2.4)*-14.1 (15.6) 5.7 (7.9)

Desmocollinite 29.6 (52.9)-64.6 (81.6) 49.1 (67.8)
Corpocollnite 3.6 (5.9)-15.2 (18.8) 8.0 (10.9)
Vitrodetrinite 0.7(0.8)-5.6 (9.2) 2.7 (4.0)
Vitrinite 43.6 (74.5)-85.0 (95.3) 65.5 (90.5)
Sporinite 0.0-1.0 (1.4) 0.3 (0.4)
Cutinite 0.0-2.9 (3.4) 0.6 (0.7)
Resinite 0.0-1.5 (1.9) 0.2 (0.2)
Fluorininte 0.0-1.7 (2.0) 0.1 (0.1)
Exsudatinite 0.0-1.8 (2.3) 0.3 (0.4)
Bituminite 0.0-1.0 (1.1) 0.1 (0.1)
Liptodetrinite 0.9 (1.3)-9.8 (11.2) 3.1 (4.1)
Liptinite 0.9 (1.7)-16.4 (18.8) 4.5 (6.0)
Fusinite 0.0-2.2 (2.7) 0.6 (0.8)
Semifusinite 0.0-0.4 (0.6) 0.0
Micrinite 0.0-1.5 (1.8) 0.5 (0.7)
Macrinite 0.0-1.4 (2.4) 0.4 (0.6)
Sclerotinite 0.0-0.5 (0.7) 0.1 (0.1)
Inertodetrinite 0.0-2.5 (2.8) 0.8 (1.2)
Inertinite 0.9 (1.1)-5.9 (6.7) 2.5 (3.5)
Carbonate mineralst 2.4-44.8 17.2
Clay minerals + quartz 1.3-16.9 5.1
Framboidal pyrite 0.7-7.8 3.2
Crystal pyrite 0.5-3.8 1.6
Massive pyrite 0.0-4.1 0.4
Mineral matter 7.9-53.7 27.4
Random reflectance measurement ( % Rr )
%Rr in telocollinite 0.68-0.79 0.77
%Rr in desmocollinite 0.50~.65 0.61

* Figures in brackets are the values in a mineral matter-free basis.

t Carbonate minerals include mainly calcite and minor amounts of dolomite.
%Rr: Mean random reflectance of vitrinite for every coal sample

of individual euhedral shaped pyrite 1-5 #m in subaqueous throughout the coal and carbonate
diameter. Massive pyrite was observed mainly sedimentation in the peat swamp. It is possible
in fracture surfaces of the macerals. Pyrite that the Upper Carboniferous-Lower Cretac-
is mainly found as framboidal and crystal eous(?) Munzur limestones, and limestone-marl
pyrite with relatively lower amounts of mas- alternations of the Kozluca Formation of
sive pyrite (Table 4). The formation of the Ypresian-Lutetian age (Tunc et al. 1991),
massive pyrite and late diagenetic carbonate which are located around the study area, may
minerals can be related to the late diagenetic have played an important role as source rocks
cleat mineralization, which was probably in the formation of the limestone-bearing
formed by deep burial during the deposition of sequence in the coal field. The influx of
the Hanioglu unit and later modified by volcanic calcium-rich waters into the swamp reduced
activity in the coal field. the acidity of the peat to a much greater degree
Finally, the abundant desmocollinites in the than would have sea water. Bacterial activity is
vitrinite group, minor amounts of the inertinite accelerated, resulting in increased degradation
group macerals and the presence of alginite of plant remains. Most calcium-rich coals
(telalginite) and bituminite (or lamalginite) in almost always show the characteristics of sub-
the coals indicate that the conditions remained aquatic genesis and are remarkably high in
110 A. I. KARAYIGIT & M. K. G. WHATELEY

organic sulphur and syngenetic pyrite, probably maxima (/~max) values of sporinites are less
due to severe bacterial activity and abundant than 580nm in lignites and subbituminous
supply of protein-rich substances (Stach et al. coals, whereas for bituminous coals this value
1982). In the light of this, the Selimoglu swamp is higher (Robert 1981). In this study, the
environment may have had high pH and low Eh spectral maxima of 17 different sporinites are
conditions, and an accelerated bacterial activity between 625-661 nm, their fluorescence inten-
resulting in HzS reacting with Fe z+ and organic sities at spectral maxima are medium or weak
peat components to form pyrite and organic (0.029-0.248 when calibrated to unity), and
sulphur compounds. In addition, it is also their Q (red/green ratio) values show a
possible that the HzS formation could have relatively broad range (1.35-2.69) (Table 5).
been accelerated by ground water carrying Based on the coal classification given by
sulphate derived from the thick gypsum-bearing Robert (1981), the range values of the "~max
rocks around the Divrigi region. An additional of sporinites indicate a high volatile bitumi-
study on sulphur isotopic ratios for evaporites nous coal stage. This rank, as explained below,
and pyrite in the coals would be needed to solve is similar to the coal stage determined by %Rr
the problem in detail. of telocollinite.

Fluorescence spectroscopy Reflectance measurement and rank

The fluorescence spectra of sporinite, cutinite, The random reflectance of telocollinite and
resinite, fluorinite, exsudatinite and alginite were desmocollinite, which are submacerals of the
measured, and Table 5 summarizes the range of vitrinite group, were measured mainly at a
values of /~max and red/green ratio (Q). The minimum 50 points on each coal sample and
lowest values of the '~max and red/green ratios the mean values for every coal sample were
were measured in alginite (Table 4), because of calculated (Table 4).
its very strong green fluorescence. Typical The range and average values of the random
examples of fluorescence spectral curves of reflectance of desmocollinite are lower than
some liptinite macerals are presented in Fig. 5. for telocollinite. The relatively weak reflectance
Similar curve trends are seen only between of desmocollinite is probably due to decomposi-
cutinite and resinite; the other curves are tion products of cellulose, and cellulose-rich
generally different for each liptinite maceral huminites/vitrinites showing particularly weak
(Fig. 5). It appears that it is possible to identify reflectances (Stach et al. 1982). The average
some liptinite macerals in Turkish coals using value of all the measurements for desmocollinite
these given typical spectral curves. and telocollinite is 0.61%Rr and 0.77%Rr,
The fluorescence of sporinite varies steadily respectively (Table 4). The 0.77% Rr value of
with rank from green to yellow, then to brown telocollinite shows a high volatile bituminous
red; the fluorescence measurement constitutes a coal rank in the ASTM classification given by
coal rank parameter, for example, the spectral Stach et al. (1982).

Table 5. The range values of the wavelength of the maximum intensity

in nm (Amax)and red/green ratio (Q) of some liptinite macerals

Maceral n /~max Red/Green Ratio, Q

Range Range
Sporinite 17 625-661 1.35 (3.00)-2.69 (16.00)
Cutinite 4 645-676 1.54 (4.00)-1.96 (8.50)
Resinite 8 592-657 1.31 (2.58)-2.20(10.20)
Fluorinite 14 593-632 1.09 (1.43)-1.42 (3.79)
Exsudatinite 12 598-651 1.25 (2.23)-2.31 (13.50
Alginite 2 475-553 0.81 (0.41)-0.89 (0.60)

n: number of measurements.
Amax:The wavelength of the maximum intensity in nm.
Figures in brackets are the arithmetic values.
 CONTINENTAL MICRITIC LIMESTONES, TURKEY 111

100
Spodnite 1~ / Cutinite
8O
.~_~70
~00
_=
~50
.~ 40
-~aO
or
20
10t-
0 , , 9 ~
0 i
450 500 550 6O0 650 7O0
450 500 550 600 650 700
Wavelength (nm! Wavelength (nrn)

100 100
Resinite 90-
~80 o~80
70 70-
~00-
~50 ~-
>=4o-
-~30-
rr 20 n~ 2 0 -

10-
0 0
450 5O0 550 6O0 650 7OO 450 500 550 600 650 7OO
Wavelength (nm) Wavelength (nm)

100 100
90 90-
8O
70 70 -
~00-
_~50 _50-
>=4o
~r 3 0 N30. _,
of 20 20-
10-
0 I P P ,, ' ~" , 0 I i ; ;
450 500 550 600 650 700 450 500 550 600 650 7~
Wavelength (nm) Wavelength(nm)

Fig. 5. Typical examples of fluorescence spectral curves of some liptinite macerals from the mining seam in the
Selimoglu coal field.

Most Miocene coals in Turkey are of lignite have been affected by the volcanic activity that
or subbituminous coal rank, whereas the occurred in the coal field.
investigated coals have a high volatile bitumi-
nous rank. The results obtained from %Rr of
telocollinite and spectral maxima (625-661 nm) Conclusions
of sporinites, the low moisture content (1.68%
average), high calorific values (5606kcalkg -1 In the Selimoglu coal field, only one coal seam,
average) and agglomerating characters of the which is associated with thin continental micritic
coals suggest that the thermal history may limestones, is exploited by underground mining.
112 A. I. KARAYIGIT & M. K. G. WHATELEY

It has a macroscopically bright appearance and (eds) Peat and CoaL" Origin, Facies, and Deposi-
a working thickness of 50-90cm (70 cm aver- tional Models. International Journal of Coal
age), and it was probably accumulated in a Geology, 12, 511-522.
small, shallow lake or pond on an alluvial plain. ICCP, 1963; 1971. Internationales Lexikon Ffir Koh-
lenpetrologie. Centre National de la Recherche
The coal seam is characterized by low moisture
Scientifique 15, Quai-Anatole-France, Paris.
content (1.68% average), high ash yield (24.04% JACOB H. 1964. Neue Erkenntnisse auf dem Gebiet der
average), high total sulphur content (up to Lumineszenmikroskopie fossiler Brennstoffe.-
8.92%) and high calorific value (5606kcal kg -1 Fortschr. Geol. Rheinld. u. Westf. 12, 569-588,
average). The maceral and mineral matter Krefeld.
contents on a mineral-matter free basis average 1973. Kombination yon Fluoreszenz-und Reflex-
90.5% vitrinite, 6.0% liptinite and 3.5% inerti- ions-Mikroskopphotometrie der organischen Stoffe
nite. It is thought that peat formation may have yon Sedimenten und Boden.-Leitz-Mitt. Wiss. u.
been developed in subaquatic conditions with Techn. VI, 1 21-27, Frankfurt.
KARAYIGIT, A. I. 1993. Geological and sedimentologi-
high pH and low Eh and an accelerated bacterial
cal investigation of the Selimoglu (Divrigi-Sivas)
activity. Most Miocene coals in Turkey are of basin, and chemical-petrographic properties of the
lignite or subbituminous coal rank, whereas the coals. Project no: TBAG 948/YBAG 15, TUBI-
investigated coals are of a high volatile bitumi- TAK, Earth Sciences Research Grant Committee
nous rank. It is possible that the thermal history [in Turkish].
may have been affected by volcanic activity that KESKIN, E., GI3RSOY, N. & GI2RSOY, B. 1984. Geology
occurred in the coal field. of the Sivas-Divrigi (Selimoglu-Mursal) area.
MTA Report No: 7616. [In Turkish]
We acknowledge the Turkish Scientific and Research OTTENJANN, K., TEICHMOLLER,M. & WOLF, M. 1975.
Council (TUBITAK) for supported first writer's Spectral fluorescence measurements of sporinites
research project (TBAG/YBAG-948), the British in reflected light and their applicability for
Council of Turkey who supported Karayigit's expenses coalification studies. In: ALPERN, B. (ed.) P~tro-
in UK and for the help given by S. Toprak with the graphie de la MatiOre Organique des Sediments,
microscope for spectral analyses and C. Tunoglu with Relation avec la Paleotemperature et le Potentiel
osctracod studies. Our thanks also to R. Wilson for the Petrolier, Paris, 67-95.
help with the electron microprobe studies. PFLUG, H. D. 1966. Fluoreszenzmessungen an Gesteinen
und Fossilien.-Leitz-Mitt. Wiss. u. Techn. II, 6
Frankfurt, 183-188.
ROBERT, P. 1981. Classification of organic matter
References by means of fluorescence; application to hydro-
carbon source rocks. #International Journal of Coal
ASTM 1991. Annual Book of A S T M Standards, Geology, l, 101-137.
Gaseous Fuels; Coal and Coke. 1916 Race Street, ROBERTS, D. L. 1988. The relationship between
Philadelphia, PA 19103, 05.05. macerals and sulphur content of some South
CASAGRANDE, D., SIEFERT, L., BERSCHINSKI, C. & African Permian coals. International Journal of
SUTTON, N. 1977. Sulfur in peat forming systems Coal Geology, 10, 399-410.
of Okefenokee Swamp and Florida Everglades: STACH, E., MACKOWSKY,M.-TH., TEICHMULLER,M.,
Origins of sulfur in coals. Geochimica et Cosmo- TAYLOR, G. H., CHANDRA,D. & TEICHMf3LLER,R.
chimica Acta, 41, 161-167. 1982. Stach's Textbook of Coal Petrology. Geb-
COHEN, A. O., SPACKMAN, W. & DOLSEN, P. 1984. ruder Borntraeger, Berlin.
Occurrence and distribution of sulfur in peat- TEERMAN, S. C., CRELLING,J. C. & GLASS, G. B. 1987.
forming environments of southern Florida. Inter- Fluorescence spectral analysis of resinite macerals
national Journal of Coal Geology, 4, 73-96. from coals of the Hanna Formation. Wyoming,
CRELLING, J. C. 1983. Current uses of fluorescence USA. International Journal of Coal Geology, 7,
microscopy in coal petrology. Journal of Micro- 315-334.
scopy, 132, 132-147. TEICHM(]LLER, M. 1974. Uber neue Macerale der
GIERLOWSKI-KORDESH, E., GOMEZ FERNANDEZ,J. C. Liptinit-Gruppe und die Entstehung des Micrites.-
& MELI~NDEZ, N. 1991. Carbonate and coal Fortschr. Geol. Rheinld. u. Westf 24, 37-64.
deposition in an alluvial-lacustrine setting: OTTENJANN, K. 1977. Liptinite und lipoide
Lower Cretaceous (Weald) in the Iberian Range Stoffe in einem ErdO'lmuttergestein.-ErdG1 u.
(east-central Spain). International Association of Kohle, 30, 387-398.
Sedimentology, Special Publication, 13, 109-125. -- ~ WOLF, M. 1977. Application of fluorescence
GIVEN, P. H. & MILLER, R. N. 1985. Distribution of microscopy in coal petrology and oil exploration.
forms of sulfur in peat from saline environments Journal of Microscopy, 109, 49-73, London.
in the Florida Everglades. International Journal of TUNG, M., OZCELIK, O., TUTKUN, Z. & GOKCE, A.
Coal Geology, 5, 397-409. 1991. Basic geological characteristics of the
HAGEMANN, H. W. & WOLF, M. 1989. Paleoenviron- Divrigi-Yakuplu-Ilic-Hamo (Sivas) area. Doga
ments of lacustrine coals- the occurrence of algae Turkish Journal of Engineering and Environmental
in humic coals. In: LYONS, P. C. & ALPERN, B. Sciences, 15:2, 225-245. [In Turkish]
 C O N T I N E N T A L MICRITIC LIMESTONES, T U R K E Y 113

UNSWORTH, J. F., BARRATT, D. J. & ROBERTS, P. T. WEDDING, E., 1965. A report on the Divrigi (Sivas)
1991. Coal quality and combustion performance. lignite basin. Directorate of Mineral Research and
An International Perspective. Coal Science and Exploration, Report No: 3774, [in Turkish
Technology, 19, Elsevier, Amsterdam. translation].
Chemical characteristics, mineralogical composition and rank of high
sulphur coking coals of Middle Miocene age in the G6kler coal field,
Gediz, Turkey
A. I. K A R A Y I G I T l & M. K. G. W H A T E L E Y 2

1Department of Geological Engineering, Hacettepe University, Beytepe-Ankara, Turkey

2 Department of Geology, University of Leicester, University Road, Leicester LE1 7RH, UK

Abstract: Most Miocene coals in Turkey are of subbituminous to lignite rank. The G6kler
coal field in the western part of Turkey contains mainly high sulphur coals of bituminous
rank. The chemical characteristics, mineralogical composition and rank of high sulphur
coking coals of Middle Miocene age in the coal field are investigated for the first time. A
total of 46 channel and core samples were collected from underground mine workings and
from boreholes drilled in the coal field.
The results of the proximate analyses as well as total sulphur analyses and calorific values
on an air-dried basis show on average 1.2% moisture, 22.9% ash, 34.6% volatile matter,
6.9% total sulphur contents and 5850kcalkg -1 calorific value. X-ray powder diffraction
studies of the coal samples on an air-dried basis show quartz, pyrite and calcite to be the
dominant minerals; kaolinite, hydromuscovite, dolomite, gypsum, iron sulphate hydrate and
rarely illite/smectite and feldspar constitute the remainder. Secondary calcite in random
fractures surfaces of the coals is especially abundant in samples obtained from an area
adjacent to the fault zones. The mean random reflectance values (%Rr) of telocollinite vary
between 0.50 and 0.95%. These values show that the rank can be determined as a high
volatile bituminous stage. In addition, these coals can form isotropic coke. Fluorescence
intensities of sporinite are weak to very weak. The mean random vitrinite reflectance values
within the coal field generally increase towards southern parts of the coal field. It is thought
that this increase can be related to the recent hydrothermal antimony mineralization in the
southeastern parts of the coal field.

The coal field is located east of Gediz in the rocks of the Muratdagi region were investigated
northwestern part of the Muratdagi region by Bing61 (1977) in detail, and also, for the first
(Fig. 1). In Turkey, the coal and coal-bearing time, Bing61 determined the age of the G6kler
strata have been studied extensively by the coals as Middle Miocene age using palynological
General Directorate of Mineral Resource and studies. G6kce (1987) investigated the geology of
Exploration (MTA) and Turkish Coal Enter- the antimony mineralization found in the
prise. Most Miocene coals of Turkey, for Muratdagi region. He proposed that the anti-
example Krtahya-Seyit6mer and Tuncbilek, mony mineralization formed from the hydro-
Canakkale-Can, Manisa-Soma, Mugla-Yata- thermal solutions which are still precipitating
gan and Ankara-Beypazari are of subbitumi- antimony at the present time. Aral (1989)
nous to lignite coal rank depending on their indicated that all host rocks were first strongly
chemical properties with calorific values which silicified and open spaces were lined with
range from 1900 to 3500kcalkg -1. The investi- crystalline quartz prior to mineralization.
gated G6kler coals have a calorific value greater Mineralization is of two types: antimonite with
than 5200kcalkg-aand sulphur contents of pyrite and marcasite as in the G6yntik mine, and
more than 5% according to unpublished reports antimonite with no other sulphides as in the
prepared by MTA. Derek@ mine including the Sakarciburnu and
The Gediz region contains important mineral Karciolukpinari mineralizations (Fig. 1). Mer-
deposits like borax and antimony, as well as coal cury minerals are absent. Trace amounts of
deposits. Some studies on the regional geology, arsenopyrite and sphalerite are present at the
coal geology and antimony mineralization have G6ynfik mine. Gangue minerals observed in
been made by Atabek (1939), Kalafatcioglu both mineralization stages are quartz, chalced-
(1961), Akkus (1962), Lebktichner (I965), ony, opal, calcite, clay minerals, and fuchsite.
G6kmen (1970), Grin (1975), Bing61 (1977), Major secondary antimony minerals are anti-
K6ksoy & Ileri (1977), G6kce (1987), K6ksoy mony oxides such as valentinite, cervantinite,
et al. (1987) and Aral (1989). The stratigraphy, kermesite, and metaantimonite (Aral 1989). The
petrological properties and geochronology of detailed geology and economic potential of the

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 115-130.
116 A. I. K A R A Y I G I T & M. K. G. W H A T E L E Y

. w

9~., ~ co

~ ~o o

.~= Eo~ 121 v ~

{~ .

~ | ._
~.~,
~o ~ o~ ~- i ~o ~.
0
E
".~_ oo
0
Jaddt~) (~.ssl~JnF) ~ E 0 l--
o

N N~ 0

F~
"6

oo

I N_e :0
0

.=.

~ m m m m ~ m

mmmmmm
immm m m ~ m m E
o
o o
o,-~l
0.0 : o

. ,...~ ,,~
~N

%o
.~ g
 HIGH SULPHUR COKING COALS, TURKEY 117

northeastern part of the coal field was studied by factories. The overall objective of this study was
K6ksoy et al. (1987), and they proposed the to determine the chemical properties, mineralo-
generalized stratigraphical sequence of the coal gical composition and rank of the high sulphur
field (Fig. 2). G6kler coals, and explain why this coal, which
In the coal field, total coal production is about has high calorific values and swelling indices
1 Mt per year, which is sold mainly to cement between 5 and 8.5, is used for industrial purposes.

z 03
0 u)
uJ
LU
o ; o .o,ooY EXPLANATION
o "1-
LL I---

Alluvium
7i+ r Gray-white sandstone with cross-bedding
and sericites
0 " ~ . ~ UNCONFORMITY

Gray-white conglomerate interbedded with

sandstone, claystone and limestone
I~ ~ - . ' - ' . - ." -,'~

UNCONFORMITY

Fossiliferous, yellow-white, lacustrine limestone

, !
Gray sandstone-claystone with gypsum (Gyp)

..
;--I~ I-- 12
iii z
Z 0 L;~+...~-., ~-_-_,+..*+..-_
l,i,l Light brown, thin bedding sandstone
0 ~; E', ...................

ILl " : ~, Greenish claystone

J n; it) --
0 ,,,
E3
_ . '~,

~ . . . .
Claystone-marl with common seficites

B(~yOk seam
Claystone
Clayey dolomitic limestone with ostracode
KBcLik seam
Gray-light brown sandstone-claystone
with sericites
Reddish poligenic conglomerate
UNCONFORMITY
Kmk-1 :Mafic and ultramafic rocks
Kmk-2: Metedetrital rocks
Kmk-3: Limestone and marble
o t.<s, s i
Fig. 2. The generalized stratigraphical sequence of the G6kler coal field (modified after K6ksoy et al. 1987).
118 A. I. KARAYIGIT & M. K. G. WHATELEY

Geological setting and marble of the Muratdagi Melange crop out.

The bedding dips of the G6kler Formation are
Rocks which range in age from Jurassic to 30-50 ~ at the boundary of basement rocks,
Quaternary crop out in the Muratdagi region. In and 10-15 ~ below the Karsakatepe deposits. All
this region (Fig. 1), the Asagibelova Formation the basement rocks and the coal-bearing G6kler
of Jurassic age, Muratdagi Melange of Cretac- Formation were cut by a number of normal
eous age, Paleocene Baklan Granite, Miocene faults which strike NW-SE, and by less frequent
Karacahisar volcanics (mainly rhyolite) and strike-slip faults cutting the normal faults
coal-bearing G6kler Formation, Pliocene Kar- (Fig. 1) (G6kce 1987). In the northeastern part
sakatepe deposits and Quaternary G6cfiktepe of the coal field a small syncline and anticline
sediments and alluvium were identified by were determined from underground maps and
G6kce (1987). The Karacahisar volcanics were shown on iso-reflectance map (see Fig. 8).
also considered as Middle Miocene age and were Tectonically the area is still active as evidenced
deposited contemporaneously with the coal- by the occurrence of strong earthquakes in the
bearing sediments in the Muratdagi region region; the last one occurred on March 28, 1970.
(G6kce 1987). However, our field studies have The coal seams are located at the base of the
failed to locate the volcanics in the coal field. In G6kler Formation (Fig. 2), and examples of
the basement immediately below the coal field, their macroscopic seam sections are shown in
serpentinized mafic and ultramafic rocks, meta- Fig. 3. There are two coal seams, the upper
detrital rocks, that consist mainly of quartz and Bfiyfik and the lower Kticfik seams. They are
muscovite, and different types of limestone separated by about 3 m of black claystone and

(roof)

Coal
Brecciated coal
Clayey dolomitic limestone
[~ Claystone
Claystone with coal
Borehole missing

5O

0 1 (floor)

BOyi3k seam Ki.icCik seam Unnamed

seam

Fig. 3. Examples of macroscopical seam sections of the Biiyfik, Kiiciak and unnamed seams.
 HIGH SULPHUR COKING COALS, TURKEY 119

brown to dark brown clayey dolomitic limestone MPV-SP microscope equipped with a high-
with ostracode that is laterally extensive and pressure 100WHg light source, a BG38 and a
50-100 cm thick (Fig. 2). The presence of clayey UG 1 filter, and a K460 barrier filter was used.
dolomitic limestone as an intra-seam unit is This microscope system was computerised
some indication of limited acid conditions so that spectral intensities in the range of
during peat accumulation. Towards the coal 460-700nm could be measured and corrected
field margins this parting interval gradually spectral intensities automatically produced.
decreases and the coal seams amalgamate into Some numerical parameters, such as relative
a single coal seam. In this study, this single intensities, wavelength of maximum intensity
seam, coal seams in some boreholes and some (Amax) and the logarithmic ratio (Q) of the
undefined coal seams in the underground mines relative intensity of red (650nm) and green
which cannot clearly be differentiated are (500 nm), were then generated from them. The
referred to as the unnamed seam (Fig. 3). principles, basic calibration techniques and some
The B~iyiik seam appears to be dull because of applications of measuring fluorescence in geolo-
black claystone partings in the seam (Fig. 3). gical samples are given by Jacob (1964; 1973),
The Kticfik seam is bright and contains less Ottenjann et al. (1975), Teichmtiller & Ottenjann
mineral partings than the Btiytik seam (Fig. 3). (1977), Teichmtiller & Wolf (1977), Crelling
The Biiytik and Kfictik seams average 170 cm (1983) and Teerman et al. (1987).
and 120 cm thick, respectively. The floor rock of All coal samples on an air-dried basis, except
the Ktictik seam is green claystone that includes two samples with insufficient coal, were analysed
rare sericites. The roof rock of the Bfiyiik seam by X-ray powder diffraction (XRD) methods.
is claystone-marl with common sericite. After identification of the whole-coal minerals
on each XRD diagram, the nett area under each
diagnostic peak for every mineral was deter-
Methods mined and then the nett area value was converted
to a percentage. In order to determine the
A total of 46 channel and core coal samples were chemical composition of some silicate minerals,
collected from the Grkler coal field (for sample two coal polished briquettes were selected, one
locations, see Fig. 8). Thirty seven samples were from the Btiyfik (sample no: GM-10) and
collected from the underground mine workings one from the Kticfik (sample no: C-94) seams,
and 9 from core samples from the 6 boreholes. which were examined on JEOL8250 electron
All samples were mechanically crushed to 1 mm microprobe. The mineralogic composition (by
size and split into two subsamples (ASTM weight percentage) determined on the electron
1991). One sample was used for petrographic microprobe was grouped according to our inter-
briquette preparation and embedded in cold pretation of the minerals. The information given
setting epofix resin, and then polished. The other by Newman & Brown (1987) was used for
was further reduced to 60 mesh (250#m) for interpretation of the clay minerals by their
proximate analysis (moisture, ash and volatile chemical composition.
matter) as well as total sulphur analysis and
calorific value of all samples on an air-dried
basis. In addition, for some evaluations, volatile
Results and discussion
matter and calorific values on a dry, ash-free
basis were calculated from the results on an air- Chemical character&tics
dried basis. Sulphur forms and Free Swelling
Index (FSI) tests were determined on only six Table 1 summarizes the results of the chemical
samples selected from the samples. The analyses characteristics and XRD analyses on an air-
were made according to the ASTM (1991) dried basis and random reflectance measure-
procedure and presented as weight percentages, ments of all coal samples. In addition, the
except calorific values. histograms of some analytical results are
Random reflectances of the maceral vitrinite shown in Fig. 4.
group telocollinite were measured at a minimum The moisture contents of the coals on an air-
of 50 points on every coal polished briquette dried basis are low and average 1.2% (Table 1).
(ICCP 1963; 1971; Stach et al. 1982). A Leitz In addition, it was determined that the moisture
MPV II microscope with a 50x oil immersion content of the coals on an as-received basis is
(n:1.518) objective, sapphire (0.551%R) and less than 5% according to unpublished reports
glass (1.23%R) standards for reflectance cali- of the coal mining companies. The ash yields
bration were used. During spectral fluorescence show a broad variation ranging from 10.9-
measurements of some liptinite macerals, a Leitz 51.2% but they are generally less than 40%. The
120 A. I. KARAYIGIT & M. K. G. WHATELEY

Table 1. The chemical characteristics, mineralogical composition and vitrinite reflectance measurements of the
Bfiyfik, Kficfik and unnamed seams in the G6kler coalfield
ii iiiii
?

BiJy~Jkseam KOcOkseam Unnamedseam Average

Analyses 19 sample 16 sam lep~__~ 11 sample ~ for~e ,
m L
Range Range ~
Range coal field

Jloisture % ~ 0.7-2.6~ 0 . 5 - ~ 1.2

~sh % ~ 10.9-35.3 ~ 1 2 . 7 ~

tolatile matter % ~. 23,1-41,2 (33.7) 33.6-41,7~ 28.1-43.8 (32.7) 34.6

Total sulphur % ~ 0.7-8.7 ~ 6.1-10.1 (8.0) 6,9

~ u r * % 2.2-3.5 1.14.1 2.1-2.9 2.7

~ h u r * % ~' 0.5-0,8 0.2-1.1 0.3-0.7 0.6

Or anic sul hut* % 2.2-2.5 3.8-4.0 tI 3,1-3.7 3.2

Calorific value, kcal k -1 3591-6887 5668 ~ 2977-7169 (5392) 585O

Calorific value, MJ 15.03-28.83 (23.73) 22.80-30.40 (26.7._~ 12.46-30.02(22.58) 24.49

~ index* + 1.0-5.0 7.0-7.5 t 8.0-8.5

<aolinite ~ 0-6 (3 0-9 2)

Ilite/smectite 90-..__3.3 (0.~_) 3___.~.~____~

0- 0 0

~" ~dromuscovite 90-..._.._~7 (4) ~ 0-7 ( 2 ) a_2_

~, E ~yn~um o-6~ ~ 0-6 1

) ~uartz 9 12-86(59) 20-75 ~ 3-84 ( 5 0 ~ _

Felds ar 0 ~ 0 0

~ Calcite 0-82 (10) ~ 0-94 (16) 15

~ )oiomite 0-20 (2) ~ 0-31 ~6) 3

e._.yrite ~ ~ 2-~..~~ 1_L.6

~ d r a t e + 0-16 (4) 0-13 ~ 0-17 (5) 5

; n ~ ~ 50-60 5a

=~ ~ %Rr ~ ~ 0.50-~ 0.7__~2

o~ ;~ Standard deviation I 0.02-0.05 (0.03) 0.02-0,05(0.04) . 0.03-0.05,(0.04) 0.04

r 9

*: Analysis of only six samples; Hydromuscovite here describes illite, muscovite and illite
Figures in brackets are the average values
n: Number of the random reflectance measurements measured on every coal sample
%Rr: Mean random reflectance of telocoUinite for every coal sample

Kticiik seam has a relatively lower average ash lated volatile matter contents on a dry, ash-free
yield than the others (Table 1 and Fig. 4a). basis for the Biiytik, Ktictik and unnamed seams
The volatile matter contents of the coal range 37.6-62.9% (average 46.4%), 40.8-57.1%
samples, like their ash yields, show a broad (average 45.6%) and 36.8-71.1% (average
range of 23.1-43.8% (average 34.6%), but most 46.2%), respectively. These values in general
of them are 27.5-42.5% (Fig. 4c). The calcu- vary between 35-55% (Fig. 4d), and the range of
 HIGH SULPHUR COKING COALS, TURKEY 121

50 50-
IB BQy(Jk s e a m Total sulphur %,
45 Ash %, (adb) 45 .
(~Ib)
I-I KQcLik s e a m
9 Unn, a m e d s e a m
35 1 35.
~ 30 30.

20 ~ 20'
15 15 -
10 10 9

,
o , IH ', il o.
15 20 25 30 35 40 45 50 55 1 2 3 4 5 6 7 8 9 10 11
(a) Class (b) Class

60-
45 Volatile matter %, Volatile matter %,
4O
(adb) 50- (daf)

35
~ 4 0 -

25
u_ 20
~20.
15
10
10-
5

22.5 25 27.5 30 32.5 35 37.5 40 42.5 45 35 40 45 50 55 60 65 70 75

(c) Class Class
(d)

60-
45 Calorific v a l u e 55- Calorific value
kcal kg ' , (adb) 50- kcal kg-1, (dad)
40
45-
35
40-
~'35.
~25 ~L. -
"20 25"
15 ~20.
15-
10
10-
5 5-
0 O-

(e) cl=,,~ (f) c=~

'adb): A i r - d r i e d basis; (daf): Dry, a s h - f r e e basis

Fig. 4. Histograms of (a) ash yields, (b) total sulphur contents, (c) and (d) volatile matter contents, (e) and (f)
calorific values.

values suggests a subbituminous to bituminous (Fig. 4b). Relatively higher-total sulphur con-
coal rank according to the classification given by tents were found in the samples collected from
Unsworth et al. (1991). On the other hand the area around the syncline. This indicates that
during the volatile matter determination, the the conditions for formation of sulphur in the
coals produced an agglomerate button showing swamp environment probably changed laterally.
swelling. The sulphur forms show that the sulphate
The total sulphur contents reach up to 10.1% sulphur content is only 9% (average 0.6%) of
(Table 1), and most of them are 5-10% the total sulphur content while the pyritic
122 A. I. KARAYIGIT & M. K. G. WHATELEY

sulphur (average 2.7%) and organic sulphur eastern part of the coal field. This coke is very
(average 3.2%) make up respectively 42% and strong with good pore structure. A polished
49% (Table 1). There are many possible origins briquette of this coke was prepared for petro-
of sulphur in the precursor peat, such as marine graphic investigation. It was observed that this
roof rocks (Horne et al. 1978), marine influences coke shows isotropic coke structure. Its prox-
during deposition (Casagrande et al. 1977), imate analysis on an air-dried basis is:
accelerated microbial degradation as the result
of increased swamp water (pH > 6) (Renton &
Bird 1991). The coal field is situated in an Moisture % 4.4
intermontane basin and there are no marine Ash %: 21.1
rocks in both the coal-bearing G6kler Forma- Volatile matter %: 12.1
tion and the Karsakatepe deposits. It is possible Fixed carbon %: 62.4
that the origin of the original sulphate of the Total sulphur %: 7.6
G6kler swamp environment related to the Combustible sulphur %: 5.8
volcanic rocks that formed contemporaneously Sulpur in ash %: 1.8
in the Muratdagi region and/or accelerated Calorific value (kcal kg-1) 5541
microbial degradation in increased swamp
water (>pH 6). These conditions would also be
ideal for the precipitation of the iron disulphide This coke, naturally, has a lower volatile
minerals (Renton & Bird 1991). This problem matter than the coals on an air-dried basis, but
and lateral suphur variation in the coal field are total sulphur and moisture contents are slightly
the subject of on-going investigations. higher. The higher moisture content is presum-
The calorific values, like ash yield and volatile ably from pore waters. The combustible sulphur
matter content, show a broad range of 2977- content is still high. These results indicate that
7260kcalkg -1 (average 5850kcalkg-1), and these coals are suitable for industrial purposes
most calorific values are 5000-7500kcalkg -1 and not for coking coal in iron and steel
(Fig. 4e). The Kficfik seam, because of relatively manufacture, because the total sulphur content
lower ash yields, has a higher average calorific of a metallurgical coke is usually preferred to be
value than the other seams (Table 1). Most of less than 1%.
the calorific values on a dry, ash-free basis are In the literature, some similar high volatile,
7000-8500kcalkg -1 (Fig. 4f) and the values high-fluidity Indian caking coals of Permian and
suggest a bituminous coal rank. Tertiary age have been referred to as 'abnormal
FSI or crucible swelling number is a small- coal' by Chandra et al. (1984). Some character-
scale test for obtaining information about the istics of these abnormal coals (Chaudhuri &
free-swelling properties of a coal; the results may Ghose 1990) are compared with the G6kler coals
be used as an indication of the caking character- (Table 2). The moisture and volatile matter
istics of the coal when burned as a fuel (ASTM contents of the Indian and G6kler coals are
1991). The method is one of the most commonly quite similar. Although the G6kler coals have
used tests in the coking industry to determine much higher ash yields than the Indian coals,
whether a coal will coke. Coals are generally they show higher FSI values.
considered to have coking properties if their FSI
is over four, whereas a FSI of seven or more
indicates a high quality coking coal. The test is Mineral matter
significantly affected by factors such as particle
size distribution, heating rate, oxidation, weath- X R D studies of the whole-coal samples show
ering, petrographic composition, and mineral quartz, pyrite, and calcite in some samples to be
(or ash) content (Carpenter 1988). All the the dominant minerals; kaolinite, hydromusco-
investigated coals, except one low FSI value vite, dolomite, gypsum, iron sulphate hydrate,
that was found in a sample with a high ash yield and rarely illite/smectite and feldspar constitute
(51.2%) on an air-dried basis, display FSI values the remainder (Table 1). The chemical composi-
between 5 and 8.5 (Table 1). The FSI results tion of silica, kaolinite and hydromuscovite and
indicate that the investigated coals have both the relevant detection limits on the electron
caking and quality coke-forming properties, microprobe are shown in Table 3. The hydro-
which is unusual in Turkish coals of this age. muscovites interpreted from the microprobe
Further evidences of coking properties of the results include illite, muscovite or sericite.
G6kler coals are seen where spontaneous The chemical compositions of the individual
combustion has resulted in coke formation silica particles vary across a broad range
locally in the underground mine in the north- (Table 3), but some have a very high SiO2 content.
 HIGH SULPHUR COKING COALS, TURKEY 123

In this study it is thought that the particles that with small amounts of clay minerals which
have a high SiO2 content are quartz grains in contain a maximum of 7.49% A1203 and 5.19%
detrital origin. They are believed to have been FeO content and minor amounts of CaO, Na20
transported from the metadetrital basement and K20. They may have been derived from an
rocks that have the very high quartz and alteration of detrital feldspar and/or muscovite,
muscovite contents. The remaining silica particles which are common in basement clastic rocks,
with low SiO2 contents are intimately intergrown and/or plant-derived silica in the mire environ-

Table 2. Comparison of some characteristics of the abnormal Indian coals with the G6kler coals

Moisture Ash Voiatile Free

% % Matter % Swelling %Rr
(adb) ,, (adb) (dmmf) Index
G6kler coals (Middle Miocene)
B(lyUk seam 3.4 51.2 44.1 1.0 0.67
BOyfJk seam 1.7 38.8 46.3 5.0 0.74
K0c0k seam ,| 9
1.1 14.7 41.3 7.0 0.74
Ktlctlk s e a m 2.6 15.2 40.5 ,.
7.5 0.83
unnamed seam 1.1 30.1 46.2 8.0 0.70,,

unnamed seam., ,
1.6
,i
28.0 36.0 8.5 0.95
Indian coals B

Tikak coal-Tertiary
,.
2.0 3.1 43.9 4.0 0.59
Bhatdih coal-Permian ..
1.3 23.0 37.6 5.5 0.86
Ranipur coal-Permian 1.5 16.8 37.5 4.5 0.82
|111 i i

(adb): Air-dried basis; (dmmf): Dry, mineral matter-free basis

%Rr: Mean random reflectance of telocollinite for every coal sample

Table 3. The detection limits of electron microprobe for silicate analysis and results of the chemical analyses of
silica, kaolinite and hydromuscovite
== ..

Silicate Detection Silica (n:22) Kaolinite (n:3) Hydromuscovite (n:5)

Analysis, % Limit Range 1 2 3 1 2 3 4 6
SiO2 0.02 45.76-99.67 (81.15) 43.25 46.24 46.46 38.56 42.45 45.43 52.69 54.48
TiO2 0.04 0.00-0.04 (0.02) 0.54 0.31 0.01 0.13 0.20 0.17 0.36 0.17
AI203 0.02 0.00-7.49 (1.36) 30.38 33.05 36.76 27.91 25.57 31.74 24.78 26.03
Cr20 ~ 0.04 0.00-0.05 (0.02) 0.03 0.02 0.01 0.04 0.02 0.02 0.03 0.04
FeO 0.05 0.03-5.19 (0.43) 1.86 0.39 0.18 1.62 2.06 2.09 1.46 0.89
MnO 0.05 0.00-0.04 (0.02) 0.04 0.03 0.02 0.02 0.04 0.00 0.01 0.03
MgO 0.02 0.00-0.21 (0.03) 0.48 0.04 ....
0.08 0.83 1.31 1.06 0.80 1.06
CaO 0.02 0.00-0.40 (0.09) 0.52 0.23 0.04 0.41 0.51 0.29 0.19 0.52
Na20 0.02 0.00-0.32 (0.10) 0.06 0.21 0.04 0.04 0.09 0.08 0.08 0.11
K20 0.02 ,.
0.00-0.43 (0.07) 0.62 0.01 0.56 2.70 4.32 3.00 2.36 2.53
NiO ,.,
0.04 0.00-0.07 (0.02) 0.05 0.02 0.00 0.01 0.01 0.07 0.06 0.02
Total 54.13-99.84 (83.31) 77.83 80.55 84.16 72.27 76.58 83.95 82.82 85.88
n: Number of measurements; Fiqures in brackets are the average values
124 A. I. KARAYIGIT & M. K. G. WHATELEY

ment. However, very few feldspars have still been average) and the coals can be classified as 'High
identified in the coal samples (Table 1). Volatile Bituminous C-A' and the average value
The calcite contents determined in 25 samples as 'High Volatile Bituminous B' according to the
range from 2-94% and the higher values (>58%) ASTM classification presented by Stach et al.
were only obtained from seven samples (C-56, (1982).
57, 106, 108; 86-1, 86-3/2, 86-10, for sample The average value (0.72%Rr) is compared
location see Fig. 8) located in an area adjacent to with the some other coals in Turkey studied by
the fault zones. Petrographically, these calcites Dogru (1978), Karayigit (1983), Yagmurlu &
are epigenetic forming in random fracture Karayigit (1984), Demirel (1989), Karayigit &
surfaces of the coals, and so they are termed Cicioglu (1994), Karayigit & Eris (1994), Wha-
breccioid coals (Fig. 3). Dolomite was deter- teley & Tuncali (1995). The distribution and
mined in only 11 samples ranging from 2 to 31%, average random reflectance values of huminite/
and only 4 samples contain both more calcite and vitrinite of the compared coals in Turkey are
low dolomite, whereas, 7 samples include only presented in Fig. 5a and b respectively. The
dolomite. Petrographically, these dolomites and/ G6kler coals have a higher average reflectance
or calcites (>24%) occur within coal macerals value than some very important Turkish lignites,
and associated with clay minerals. It appears that such as Seyit6mer, Tuncbilek and Beypazari.
these are early diagenetic (syngenetic) minerals. Only the Askale coals of Miocene age have a
The coals contain large amounts of pyrite similar %Rr to the G6kler coals. The Askale
(Table 1). In addition, gypsum and iron sulphate coal field is in a very complex tectonic system
hydrate have also been determined in a few and located near the Northern Anatolian Fault
samples. The sulphate minerals are not normally Zone, which is a major, plate bounding strike-
found in fresh coals, but are commonly seen on slip fault in Turkey. Dogru (1978) indicated that
mine faces that have been exposed for some time the Askale coals have been affected by this fault,
(Ward 1978). This means that the circulation of producing high reflectance values. The high
more recent oxidizing meteoric waters may have %Rr values of the G6kler coals are discussed
caused the oxidation of the pyrite and the below.
resulting sulphate is precipitated as iron sulphate
hydrate as secondary minerals in the coal seams.
In addition, sulphuric acid produced during the Fluorescence spectroscopy
process may react with any carbonate minerals
present to form gysum. Within this study, the fluorescence spectra of
Kaolinite is the most abundant of the sporinites were measured in order to obtain
clay minerals determined in the coal samples some additional information on the rank of the
(Table 1). Kaolinite minerals interpreted from G6kler coals. During petrographic examination
the results of the electron microprobe analysis with blue light and an orange barrier filter, it
have slightly lower A1203 contents than ideal was found that sporinites fluoresce a weak
kaolinites. The kaolinite is thought to have yellowish orange and reddish brown. In addi-
formed by weathering of feldspars in the acid tion, some samples having unusually high
waters of the coal swamp. The chemical reflectance values contain exsudatinite maceral
composition of the hydromuscovites (Table 3) showing orange, reddish orange and reddish
contains lower K20 contents than ideal mica or brown fluorescence. In the samples, exsudatinite
illite. It is thought that these hydromuscovites is a secondary maceral and it is difficult to
are detritial in origin and they were transported identify by reflected light with an oil immersion
from the metadetrital rocks. Sericites are also lens because of its dark colour. Exsudatinites
common in the overburden deposits of the coal appear to fill voids and cracks in vitrinite.
seams (Fig. 2). Occasionally, they fill edges of pyrite, especially
massive pyrite.
The spectral maxima of 17 different sporinites
Reflectance measurements, classification and taken from six samples with reflectance values of
compar&on with some Turk&h coals 0.50-0.76%Rr are between 605-670nm and
their fluorescence intensities at spectral maxima
Random reflectance of telocollinite was mea- are weak to very weak (0.01-0.07 when cali-
sured at a minimum 50 points on each coal brated to unity), and their Q ratios show a broad
sample and the mean value and its standard range (1.12-4.28). With increasing rank
deviation were calculated (Table 1). The mean (>0.76% Rr) the sporinites in the samples do
random reflectance (%Rr) of telocollinite for all not fluoresce. On some samples, some sporinites
coal samples ranges from 0.50 to 0.95 % (0.72% have variable fluorescence, for example, the
 HIGH SULPHUR COKING COALS, TURKEY 125

BLACK SEA N

(!1) MEDITERRANEAN
SEA

RANK
%Rr
DIN ASTM
1.0
0.9-
v,. 0.11 -

- /
o.7 -~
I
0.6 ~
0.5 ' U
(Glanz-) - ~ Sub- B
Dull ~ ~; Bit. C 0.4 ""

Soft ~ Lignite 0.3

0.2

Peat Peat
(To~ I I r I I l r I I I I I I I f I I

(b)
,!|
Fig. 5. (a) The distribution of the compared coals in Turkey, (b) locations of the average %Rr values of
huminite/vitrinite for every coal fields in the DIN and ASTM classifications.

spectral maxima and Q values of five sporinites Examples of the selected spectral curves of
on a single sample (sample no: 86-6) show sporinites and exsudatinites are shown in Fig. 6.
a range of values between 641-670nm and Sporinite shows many sharp peaks (Fig. 6a). The
1.12-2.64, respectively. This fresh coal sample coal sample with lowest vitrinite reflectance
was taken from the core of the unnamed seam value (0.50% Rr) has a higher wavelength of
and has the lowest vitrinite reflectance value maximum intensity (666nm) than the sample
(0.50% Rr) which has not been influenced by (621 nm) with a higher vitrinite reflectance value
weathering. Weathering of sporinites has been (0.76% Rr). This means that there is not a good
shown to produce different fluorescence values. relationship between the wavelengths of max-
It is believed that the high fluorescence spectral imum intensity of sporinites and %Rr, which
values may be related to a relatively irregular are used as coal rank parameters. This may be
increase in rank of the sporinite macerals in the related to the hydrothermal alteration of the
same sample at the begining of the bituminous coal samples under post-depositional conditions
coal rank, which was described as the first in the coal field.
coalification jump of liptinites (Stach et al. The spectral maxima of exsudatinite measured
1982). It may also be due to different botanical at 7 points on four different coal samples, which
origins or syn-or post-depositional conditions. have 0.56-0.84%Rr, are between 602 and
126 A. I. KARAYIGIT & M. K. G. WHATELEY

100
90+
80 +
spomize ~i
...... un (0.76%Rr) .',~
' '= i
70 §
1l
60 + un (0.50%Rr) , '~i!
50 t-
40 §
30 t-
20 +
10+ "r
0 , I

450 500 550 600 650 700

(a) Wavelength (nm)

100

Exsudatinite ,; ', ~, ,' ";

80
70 ...... un (0.84%Rr) ;II'\ j' 'V
60
50
40
30
20

0 , ,
450 500 550 600 650 700
(b) Wavelength (nm)

Fig. 6. Examples of two spectral curves of sporinite (a) and exsudatinite (b).

654nm. Their fluorescence intensities at the is no clear relationship between calcite and
spectral maxima are higher (0.112-0.343) than dolomite, and volatile matter contents because
sporinites. Compared to the sporinites, exsuda- of analytical errors and X R D analyses. On the
tinites form fewer sharp peaks (Fig. 6a and b). other hand, the second group consists of higher
The dashed line spectrum in Fig. 6b shows a volatile matter contents because of epigenetic
typical spectral curve for exsudatinite. It appears calcites. Figure 7c shows a weak relationship
that it is possible to identify exsudatinite in between volatile matter content on an a dry, ash-
Turkish coals using this typical spectral curve. free basis and % R r of telocollinite.
Finally, volatile matter content and calorific
value, which are used as coal rank parameters, in
Relations among coal rank parameters and some samples are mainly affected by the high ash
coal rank variation in the coalfield yield and carbonate minerals in the coals. The
)k.... values and intensities of the spectral
Graphical comparison of some chemical and maxima in sporinites are high, and weak-very
X R D analyses, and % R r results are given in weak, respectively and their Q ratios show a
Fig. 7. There is no clear relationship between broad range. With increasing coal rank the
volatile matter and calorific value on a dry, ash- sporinites in the samples do not fluoresce. The
free basis (Fig. 7a). A plot of calcite and % R r values in this field are more useful
dolomite versus volatile matter content on a indicators of lateral variations in rank than the
dry, ash-free basis (Fig. 7b) shows two different fluorescence measurements of sporinites and the
groups. The first group includes lower calcite chemical analyses of the coal samples.
and dolomite contents, whereas the second The Bfiyfik and Kficfik seams obtained from
group has higher. The early diagenetic carbonate the same borehole have very similar reflectance
minerals are situated in the first group, but there values (for example 0.76-0.77%Rr at 86-2;
 H I G H SULPHUR COKING COALS, T U R K E Y 127

9000 n
i 9 I
"I
8000

- 7000

8 6000 9 L
i +
>-
I
O 5O0O

|I
4000 ~ i
30 35 40 45 50 55 60 65 70 75 80

(a) Volatile matter %, (daf)

80

" " 65
75
7o t IoB0y0ksea
1 / 9 Kuc0k seam /
~a Unnamed seam~
Group IIo ~

~ 6o
Group I
N 55
~ so
N 45
"~ 40
>
35
30 I I I I
0 10 20 30 40 50 60 70 80 90 100
(b) Calcite + Dolomite %
1.00
n ! o Buyuk seam l
3
o
0.90 9Kucuk seam
0.80
a ~
Co

~ o 9
I n Unnamed seam J
,_ 0.70
rr o o 9
0.60 # ~
O O n
9 o
0.50 []

0.40

0,30 I I I I I I I : :
(c) 30 35 40 45 55 50 60 65 70 75 BO
Volatile matter %, (daf)

(adb):Air-dried basis; (daf): Dry, ash-free basis; CV: Calorific value

%Rr: Mean random reflectance of telocollinite for every coal sample

Fig. 7. Graphical comparisons of the chemical analyses, X-ray powder diffraction (XRD) analyses, and %Rr
measurements of telocollinite. (a) relationship between volatile matter contents versus calorific values,
(b) calcite + dolomite contents determined by XRD versus volatile matter contents, (c) volatile matter contents
versus %Rr.

0.76-0.74% Rr at 86-3; for location see Fig. 8). which are determined from a number of under-
This shows that the parting sediments (3 m thick) ground mine maps, and antimony mineralization
between the two coal seams do not clearly in the Deliktas and Karacatepe areas also
influence the reflectance values. Figure 8 shows illustrated on the map. The iso-reflectance
the iso-reflectance map of the coal field. Sample values for the seams over the whole coal field in
locations, reflectance values, faults and folds, general increase toward southern parts of the
128 A. I. K A R A Y I G I T & M. K. G. W H A T E L E Y

/' ~, +* 8 6

! 9 C:'-- + " --~ ..~ = Z:..v: ~ = Q-

t

/ "" c- ~+ \ d~_ -~ := :~ '- 3:', 3 ~" ,=, 6

/ 0 :; ,!-:
./.. ~ ~. ~ : /I T ~
\ et"
:; m
,0 o 9 [] < --
<; ~.
~o ~
o -~
........ ~- ~..,o.. i o'/. \ ~ ~ ~ --~
~ . . .;l \ ~,. ~ ~ " _ N | ="I
o . :j--'~ \ ._=~ ~ ~ ~, .; ._~ 1 ~ ~I
9 -// ~ \ ~ ~ o ~ ~ ~ ~ ~ o- ~ t

9 - i,- ~ ul

~ ~.., ,, . o~..- : ,',A .v ~ :1~.+ ~ .

..-,. 9 9" ..- . ~~ ~ ~i-

7 -
-~ _~''. ~,.'~L=,_ ~/ :. ~ _ ~ ~" II "..". \ ~\ + - ~,
.- ,. "
"~ ,- .~ ~
~ ~ _ ~ " 0. . ,~,

\ ~. .... .- ~ .- .~,~..i~~o i ,- ~-- ,.~ + \ _ ~ .~

~-i~ ..~- ..;'..

"'~Z~ /.i + ~
"~ ~ " . ~,<~ . 0 , I 0

~,
o,il._o. ". ...... ~ . . ~ . .
_.. , ,,
,, \ ,,, \ ~ .~.. /".. .,~-0~:
}\ ~ \ ,o o . . . / .."/ -/
6
 HIGH SULPHUR COKING COALS, TURKEY 129

coal field (Fig. 8). In addition, the reflectance the coal field. The %Rr values within the coal
values seem to increase toward the Karakaya field generally increase towards the southern
fault zone (Fig. 8), and also in the same fault parts of the coal field. It is thought that this
zone the values increase from 0.74-0.76% Rr increase can be related to the recent hydro-
(borehole 86-3) to 0.93% Rr (GM-11) near the thermal antimony mineralization. The asso-
silicifed zone of antimony mineralization. This ciated high heat flow has also resulted in a
indicates that this fault zone probably was weak devolatilization of the coals (Fig. 8c), and
affected by the antimony mineralization or high an increase in the wavelengths of the spectral
heat flow. On the other hand, the brecciated maxima of sporinites, to an optimum degree
coals including higher calcite and dolomite producing the coking properties in these coals.
contents have relatively low %Rr values (for
example: C-106/0.58; C-108/0.57; C-56/0.65; We acknowledge the British Council of Turkey who
C-57/0.65 and 86-10/0.59; Fig. 8). These results supported Karayigit's expenses in UK and the
imply that the normal faults and the brecciated Research Foundation of Hacettepe University,
coals were probably formed prior to antimony Ankara, Turkey for supporting the reseach project,
the help given by S. Toprak for spectral analyses of
mineralization. liptinite maceral groups and R. Wilson for evaluation
During field studies antimony mineralization of the microprobe results. We also thank O. Mal~n and
and associated silicification were seen along the M. Miliorizos who critically reviewed the manuscript.
strike-slip fault zone, which is identified by
G6kce (1987) and around Karacatepe antimony
mineralization in the limestone-marble of the References
Muratdagi Melange (Fig. 8). In addition, a
number of calcareous cones were formed prob- AKKUS, F. M. 1962. Geology of the area between
ably by hot-springs in the Muratdagi region. Kiitahya and Gediz. MTA Bulletin, 58, 21-30
K6ksoy & Ileri (1977) determined that some [in Turkish with English abstract].
cones of recent hot-springs in the Ilica, about ARAL, H. 1989. Antimony mineralization in the
Northern Muratdagi (western Turkey). Economic
40 km west of study area, contain high antimony
Geology, 84, 780-787.
values. G6kce (1987) proposed that the miner- ASTM, 1991. Annual Book of ASTM Standards,
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 The main coal facies and lithotypes of the Pliocene coal basin,
Oltenia, Romania
NICOLAE TICLEANU & DORINA DIACONITA

Geological Institute o f R o m a n i a , 1 Caransebe,~ Street, 78344 Bucure~ti - 32, R o m a n i a

Abstract: This paper presents the results of palaeobotanical studies correlated with coal
petrography research carried out by the authors in the western part of the Dacic Basin
(Oltenia) coal deposits. Of the seven coal facies that have been distinguished so far in the
lignites of Oltenia, the present paper deals with the five main facies generated by: swamp
deciduous forest, Carex ssp. grassy marsh, swamp with Glyptostrobus, reed swamp and
aquatic macrophyte prairie. The palaeoecological and palaeophytocoenoical studies have
led to the reconstruction of the factors that characterize the major coal facies.

General geological setting Previous research

The Pliocene coal basin of Oltenia contains the According to Teichmfiller (in Stach et al. 1982)
most important coal deposits in Romania and it 'the term "coal facies" refers to the primary
is situated south of the South Carpathians, genetic types of coal, which are dependent on the
between the Danube and the Olt Valley. milieux under which the peat originates.' At
The coal precursor, peat accumulated in the the same time, the coal facies also includes the
western area of the Dacic Basin. Structurally, petrographical composition and the physical-
the coal basin overlies the Carpathians Foredeep chemical properties of coal.
and the Moesian Platform (Fig. 1). Using these factors, Ticleanu & Bi~oianu
According to Ticleanu et al. (1988) and (1989) have described seven facies in the
Ticleanu & Andreescu (1988) the tectonic- Pliocene coal of Oltenia. The petrographical
structural units have played a very important coal structure (Bi[oianu & Ilie 1967, Ilie &
role in the distribution of the coal deposits. Thus Bi!~oianu 1967), the connections between the
the greatest thickness of most of the 22 coal petrography and the physical-chemical charac-
layers is situated on the internal side of the fore teristics of coal) Ticleanu et al. 1989, 1992) and
deep. On the external side of the foredeep both the identification of coal-generating vegetation
the number and the thickness of the coal layers and environmental conditions (Ticleanu 1986,
decrease so that in the Neogene cover on the 1992a, b) have also been studied.
Platform there are only 1-2 beds with thickness
exceeding 2 m, and they occur as local pockets.
According to Andreescu et al. (1985) the Methodology
sequence of the Pliocene coal deposits consists
This study is designed to improve the knowledge
of three lithostratigraphic units (Fig. 2):
of the characteristic flora of the main coal facies
9 the Berbe~ti Formation (Uppermost Pontian- by reconstructing the environments in which the
Lower Dacian, according to Andreescu (oral parental material accumulated in the Pliocene.
communication) is mainly psammitic and in For a better understanding of plant commu-
the upper half contains clayey intercalation nities we have identified the flora using the
and six coal layers (A, B and I-IV) that methodology and the terminology presented
constitute the Valea Vi~enilor coal complex; by Ticleanu (1992a, b, 1995a, b), and we have
9 the Jiu-Motru Formation (Upper Dacian- combined this with the results of taphonomical,
Middle Romanian) is mainly pelitic-psammi- palaeophytocoenotical, palaeocarpological and
tic with eight coal layers (V-XIII) that cuticulary analyses carried out over the last few
constitute the Motru coal complex, the years. The fossil plant material that we studied
most important coal complex in the basin; for the palaeoecological and palaeophytocoeno-
9 the Cfinde~ti Formation (Middle Romanian- tical interpretations, came from over 12 500 m of
Pleistocene) is mostly psammitic-psephitic cores from 85 boreholes and from the working
that includes clayey intercalation and five faces of 22 coal open-pit mines. The results of
coal layers (XIV-XVIII). These constitute this research identified over 800 accumulations of
the B~lce~ti coal complex, developed only in fossil vegetable remains (AFVR), of which 585
the central area of the basin. are autochthonous, 153 are hypautochthonous,
28 are allochthonous and 24 are of mixed origins.

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 131-139.
132 N. TICLEANU & D. DIACONITA

9 , ,' ' ' 9 " , ' . k " " " "

9 'i . .IINT.FRN, AL}.'~ "-~,' .... ' ' '.'."

,(EXTER'NAL)'

CRAIovA\
MOES[AN PLAZrFORM
t
t
/
l

LEGEND
............... 1 - The Oltenia coal basin boundary

....... . . . . L_J_ 2 - Pericarpathian fault

, 3 - Flexure

Fig. 1. Sketch map of the delimitation of the Oltenia coal basin and its structural framework.

Besides these, 68 AFVRs of fossil fruits and The authors have carried out many petrogra-
fructifications and over 560 AFVRs of fossil phical analyses with a view to establishing
wood accumulations (xylite), were identified. connections between coal facies and coal litho-
This wide range of AFVRs indicates the auto- types generated by these.
chthony of the coals in Oltenia and enables the
reconstruction of the plant communities to the
level of palaeophytocoenoses. Brief palaeogeographical, palaeoclimatical
The knowledge about coal-generating plant and palaeophitocoenotical description
communities and environment has been extended
on the basis of correlation of taphonomical Palaeogeographically speaking, the coal deposits
investigations, ecological demands and coenoti- in Oltenia accumulated on the western side of
cal characteristics of modern plant equivalents of the Dacic Basin (Fig. 1), which, most of the time,
fossil plants and fossil plants associations. The in the Pliocene was a large alluvial-lacustrine
use of the principle of uniformitarianism has plain. Because of vertical tectonic movements,
been facilitated by the relatively young age of the morphological aspect of this accumulation
coal deposits (2.5-4.5 Ma) and by the fact that plain changed cyclically (Ticleanu 1992a), each
most of the fossil plants (41) and palaeophyto- cycle having four stages: fluviatile, fluvio-lacus-
coenoses (18) of the Pliocene swamps in Oltenia trine, telmatical and lacustrine.
are also to be found today, or still have The cyclical variations of the subsidence rates
direct modern equivalents in today's swamps in have determined the cyclical distribution of
Romania. stages, each of them being characterized by a
 PLIOCENE COAL FACIES AND LITHOTYPES IN ROMANIA 133

The above climatic premises have encouraged

the development of a hygro-hydrophyte vegeta-
tion relatively poor in species but very rich in
Bk, LCE.STI specimens. Ticleanu (1992a) has identified more
I than 70 species. The most frequent species are
COALY COMPLEX
Byttneriphyllum tiliaefolium, Phragmites oenin-
gensis, Glyptostrobus europaeus, Salix ssp.,
Stratiotes dacicus, Carex ssp. Typha latissima,
Trapa ssp., Acer tricuspidatum, Nelumbo proto-
speciosa and Osmunda regalis, the other species
being found in less than 5 AFVR each.
The first six taxa constituted plant commu-
nities (palaeophytocoenoses) alone but they also
HOTRU generated associations with other taxons. The
COALY COMPLEX most frequent palaeophytocoenoses were identi-
fied in autochthonous AFVRs. These are
(ordered by their frequency): Byttneriphyllum
tiliaefolium (122), Glyptostrobus europaeus
(108), Phragmites oeningensis (84), Salix ssp.
(43), Byttneriphyllurn tiliaefolium & Glyptostro-
VALEA VISENILOR bus europaeus (19), Phragmites oeningensis &
COALY COMPLEX Typha latissima (19), Stratiotes dacicus (18),
Trapa ssp. (18), Byttneriophyllum tiliaefolium &
Coals
Salix ssp. (12) and Carex ssp. (12).
f----'~cioy~
Sillic r162
Using modern swamps in Romania as analo-
~ R$~mml~'Q gues, the Pliocene swamp plant communities are
P~.ephile believed to be distributed first of all by their
Fig. 2. Synthetic lithostratigraphic column of the demands for water. From this point of view,
Pliocene coal deposits from Oltenia. using a similar method to Teichmtiller's (1958)
several areas (palaeobiotope) can be distin-
guished (Fig. 3): marginal; seasonally fooded;
prevailing lithofacies: mainly sandy in the almost permanently flooded; permanently cov-
fluviatile stages, sandy-silty-clayey in the fluvio- ered by water, between 0 and 2 metres deep,
lacustrine stages, with peats in the telmatical permanently covered by water, between 0 (2)
stages and mainly clayey in the lacustrine ones. and 3 metres deep, depending on the stage of
During the telmatical stages the basin sub- vegetation's evolution and open water area.
sidence was low and equalled plant accumulation Each of the above areas (palaeobiotope)
rates, allowing most of the accumulation plane includes one or more vegetal associations
to be covered by eutrophical low moors, with (phytocoenoses). These associations constitute
thicknesses ranging between 0 and few metres. ecological series from the centre to the margins
Climate type that allows large swamp genera- of the swamp.
tion is characterized by a positive hydrological In this way, in the modern swamps in the
regime, where precipitation exceeds evapotran- Danube Delta, Rudescu et al. (1965) shows the
spiration. According to Ticleanu (1995c), during presence of one ecological series that contains
the Pliocene peatmoor generation the mean the following vegetal associations (from the
annual temperature fluctuated between 14 and open water to the marginal area): Characetum,
15.5~ and the precipitation quantity exceeded Nupharetum, Phragmitetum, Typhaetum, Scirpe-
1200 mm per year, almost uniformly distributed tum, Carecetum, Juncetum, Salicetum.
with only a slight summer peak. In these con- Except the Juncetum association, not yet
ditions, the temperature of the peat was found, all the others have corresponding palaeo-
probably 16-22~ with a maximum in Upper phytocoenoses in the Pliocene swamps.
Dacian. Modern analogues suggest that the flooded
The presence inside the coal layers of some areas of vegetation in the Pliocene are domi-
centimetre-scale argillaceous intercalations with nated by grass associations, especially Carex
some fossil vegetable remains (FVR) concentra- (prevailing herbaceous stage). Later these grass
tions, some with much pollen and others with dominated associations were replaced by palus-
many fossil leaves, shows the existence of spring tral forest associations (prevailing forest stage).
and autumn floods. Unlike the modern swamps, where the flooded
134 N. TICLEANU & D. DIACONITA

Zts
~ -

0~.

~q

r..)

,
II II II II
t

r
i i
,,

g
Z;>- ~ ~.

II II II II tl

>-
1 ,,1 M

~.~~e ~ "~
-~1 1-, ~..~1
m

-~--'--
- >
~- ~ ~ ~-i

II II II II II II ".~

m
t~. = e

9 t
-~, . - ~ ~d ~
m 5 ~ o o ~ ~ ~ ~" '~

,
 PLIOCENE COAL FACIES AND LITHOTYPES IN ROMANIA 135

forest areas are dominated by Salix, Populus, Table 1. The main physical and chemical characteristics
Alnus and Betula, the Pliocene swamps forest of the lithotypes of the Olternia.
palaeophytocoenoses were dominated by Lithotype Aanh (%) Vd (%) Qd (kcal/kg)
Byttneriophyllum tiliaefolium, Salix ssp., Glyp-
tostrobus europaeus, as well as other tree species. Xylite 1.26-3.35 47.7-68.4 5042-6034
Because rainfall distribution controls various Xylitic coal 8.58-17.82 39.0-52.2 4340-5378
factors (such as swamp bottom morphology, Weak xylitic 16.79-28.0 36.2-46.9 3874-4871
annual rainfall quantity, evapotranspiration coal
etc.), the areas occur as more or less parallel Detrital coal 22.11-48.45 27.8-38.8 2503-4012
bands. The general aspect of the vegetation was
Aanh, Anhydrous ash; V~ Volatile matter (air-dried
that of a huge mosaic such as that presented by
basis); Qa Upper calorific value.
McCaffrey & Hamilton (in Cohen et al. 1984),
for the Okefenokee swamp map of the southeast
United States. In the first stages of the evoluion of the Carex
swamp's vegetal cover, there were only small
clumps of bushes of Salix cinerea and Salix
The main coal facies and the lithotypes pliocenica distant from the open water but they
developed into bigger and bigger clusters, as they
According to Ticleanu & Biloianu (1989) the grew nearer to the central open water area of the
Pliocene coals in Oltenia contain the following swamp where they occurred beside Byttneriphyl-
facies: Sequoia abietina forest, swamp deciduous lum tiliaefolium, Nyssa, Glyptostrobus, etc.
forest, Carex spp. grassy marsh, swamps with Palaeobiotope: floodable areas, but only in the
Glyptostrobus, reed swamps, floating vegetal first stages of vegetation evolution.
formation and aquatic vegetation. Type of deposition: mainly autochthonous,
Considering the fact that the first facies played partially hypautochthonous by vegetable
an insignificant role in the coal-generating remains brought by floods and less allochtho-
phytomass constitution and the sixth one led nous (pollen, leaves fragments and fruits
only to coaly clays, in this study we shall refer brought by wind).
only to the remaining facies which constitute Depositional milieux: telmatic.
those of real significance, together with an Environmental characteristics: the peat is gener-
addititional facies - aquatic macrophyte prarie. ated especially by roots and less by aerial
To describe the primary characteristics of coal remains of plants, deposited under aerobic-
layers in each coal facies we have used Teich- anaerobic conditions with a moderate to weakly
mfiller's method (in Stach et al. 1982). acid pH(5.0-6.8), rarely from weak acid to
neutral (6.0-7.2), and extremely rarely in an
alkaline environment.
The coal faciesmgrassy marsh Carex ssp. Lithotype: detrital coal, i.e. a groundmass with a
fine detritic texture, more or less layered, more
Plant communities: palaeophytocoenoses with than 50mm thick, frequently with more than
Carex ssp. (Carex flagellata, Carex cf nigra etc.) 30% ash content (Table 1). According to Pop
Associated dements: Scirpus rnaeotica, Cladium (1960) the actual Carex peat contains more than
mariscus, Cladium palaeomariscus, Sparganium 10% ash, and where flooded, this percentage
neglectum, Najas pliocenica, Butomus umbelatus, increases because of the mineral material sus-
Oenanthe aquatica, Trichosanthes fragilis, Pedi- pended in water. We consider that transforma-
cularis sp., Lythraceae ( ?Lythrum salicaria), etc. tion of peat into lignite can lead to a relative
Most of these taxa are still living today and enrichment of the ash content up to 30%.
examples are found in actual Carex ssp. swamps The petrographical composition of the detrital
in Romania (Pop 1960). In the palustrian coal lithotype shows its high humodetrinite
vegetation in the Danube Delta, Popescu et al. content (Table 2).
(1981) have identified the association with
Claudietum mirisci.
The presence of taxa that generate actual The coal facies---deciduous forest
phytocoenoses ( Carecetum, Scirpetum and Clau-
dictum) and the relatively high density of their Plant communities: Palaeophytocoenoses with
seeds in the clays and the clayey silts that Byttneriophyllum tiliaefolium, Byttneriophyllium
accompany the coal layers prove the develop- tiliaefolium-Glyptostrobus europaeus, Salix ssp.-
ment on large areas of coal facies of swamps Glyptostrobus europaeus, Salix ssp. (Salix abla,
with sedge (Carex ssp.). Salix fragilis, Salix grandifolia, etc.).
136 N. TICLEANU & D. DIACONITA,

Table 2. Petrographical composition of the Pliocene coals between the Danube and the Amaradia Valley after
Bitoianu (in Ticleanu et al. 1989, 1992)..
Group of macerals Huminite % Liptinite (%) Inertnite (%)

Ubgroup of Humotelinite Humodetrinite Humocollinite

erals
Lithotype
xylite 68.2-87.0 8.0-12.7 0.1-0.13 0.15-0.20 0.31-1.2
xylitic coal 49.0-49.6 25.8-32 0.6-0.7 1.30-3.0 2.40-3.2
weak xylitical coal 22.0-27.8 51.8-54 0.3-1.3 1.80-3.5 2.70-4.4
detrital coal 8.0-18.5 59.0-61.7 0.2-3.7 1.10-1.5 2.07-4.2

Associated elements: Acer tricuspidatum, Populus areas occasional Stratiotes dacicus were found.
populina, Nyssa disseminata, Liquidambar euro- This explains the relatively high frequency of
paeum and Carya cf. aquatica. seeds of this species in the xylitic coal. Surround-
Palaeophytocoenoses with Byttneriophyllum ing Glyptostrobus europaeus trunks, and between
tiliaefolium, Glyptostrobus europaeus and Nyssa these trunks and pneumatophores fern bushes
were located in the central areas of the swamp, (Osmunda regalis) were growing similar to
and Salix ssp. in the marginal ones. Osmunda lignitum (Petrescu & Givulescu 1986),
Palaeobiotope: seasonally flooded areas. in Chattian swamps in the Petro~ani Basin.
Type of deposition: frequently autochthonous, The role of Glyptostrobus europaeus species in
rarely hypautochthonous, and extremely rarely the genesis of coals, has been treated in many
allochthonous (pollen, flying fruits). papers. The most recent is the paper by Boulter
Depositional milieux: telmatic. et al. (1993).
Environmental characteristics: acid pH (3.5-5), Palaeobiotope: almost permanently flooded areas,
deposited in aerobic-anaerobic conditions, to where water withdraws for only one or two
explain the rapid loss of most of the cellulose. months in a year.
Lithotypes: detrital coal, weak xylitical coal and Type of deposition: mainly autochthonous.
rarely xylite coal. The weak xylitic coal Depositional milieux: telmatic to subaquatic
was probably generated in the internal part of (limnic).
the seasonally flooded area, to the limit Environmental characteristics: in closed horizon-
of the almost permanently flooded area, tally structured palaeophytocoenoses (pure
from palaeophytocoenoses with Byttneriophyl- Glyptostrobus forest) the pH was probably low
lum tiliaefolium-Glyptostrobus europaeus and (3.5-5) and in open structured ones the pH was
Salix ssp.-Glyptostrobus europaeus. In the same higher but still weakly acidic (5.6--6.6) and less
areas a very small part of the lithotype xylite also probably neutral (6.8-7.2), as in modern swamps
accumulated, included in detrital coal, resem- with Stratiotes aloides, the modern equivalent of
bling rare xylite lenses and bands with more than Stratiotes dacicus species.
50 mm thick. Considering that the palaeophytocoenoses
Generally, the ash content is relatively low, with Glyptostrobus europaeus were covered by
because of the protection granted by the sur- water between ten and eleven months in a year,
rounding palaeophytocoenoses against water the plant material accumulated under mostly
with suspended clay content. anaerobic conditions.
Lithotypes: xylitic coal, xylite and weak xylitical
coal.
The coal facies--forest swamp The xylitic coal lithotype is composed of
with Glyptostrobus alternating bands of fine coal mass, weakly
banded, and bands and lenses of fossil wood
Plant communities: palaeophytocoenoses with (xylite) both less than 50 mm thick. The xylitic
Glyptostrobus europaeus. coal is second in importance (30% of the entire
Associated elements: very rare Taxodium dubium reserves) after detrital coal in the soft brown
and Nyssa disseminata representing Miocene coals in Oltenia. Many coal layers consist only
relicts. In open horizontal structured palaeo- of this lithotype.
phytocoenoses, trees were scarce, and between Pieces of charcoal (inertinite) with a variety of
them were areas covered by water, even when different sizes occur relatively frequently, in the
the water level was at its lowest. In these prairie detrital of xylitic coal. In our opinion, these
 PLIOCENE COAL FACIES AND LITHOTYPES IN ROMANIA 137

show the presence of frequent natural fires in the because this facies contains frequent seeds of
forest swamp. These fires have played the same Stratiotes dacicus. The quantity of this coal
role in the Pliocene swamps as they do in shows the importance of palaeophytocoenoses
modern swamps for the vegetation in Okefeno- with Phragmites in coal generating phytomass
kee, as shown by Izlar (in Cohen et al. 1984). constitution.
The ash content of the xylitic coal lithotype is
relatively low, because the clayey material is
kept out by the surrounding palaeophytocoe-
noses. The ash content of the xylitic coal Aquatic macrophyte prairie
lithotype is also proportional to the amount of
xylite. The ash content xylite is very low (Aanh: Plant communities: palaeophytocoenoses domi-
1.26-3.35%) and is of primary origin (Table 1). nated by one of the main taxa: Stratiotes
Another important lithotype generated in the dacicus, Trapa urceolata, Trapa expectata, Myr-
same facies is xylite that represents between 5 iophyllum nagavicum, Hydrocharis morsus-renae,
and 20% of entire coal volume, and is repre- Potamogeton corniculatus, Ceratophyllum demer-
sented by lenses and bands that can reach up to sum, Ceratophyllum submersum, Nymphaea alba,
a few meters long and 50-350 mm thick, some- Nuphar pliocenicum and Nelumbo protospeciosa.
times even more. More than 80% of the xylite The relative high number (68) of AFVR of
represents branches, trunks and roots of Glyp- aquatic plants, and their palaeocarpological
tostroboxylon tenerum, identified by Petrescu content has helped us to identify 15 palaeophy-
(oral communication). tocoenoses in the Pliocene swamps. From the
The xylite lithotype is characterized by the 27 aquatic plant associations found by Popescu
highest humotelinite content (Table 2). et al. (1981) in the Danube Delta, at least
eight also existed as such in the Pliocene
(Hydrocharitetum morsus-ranae, Stratiotetum,
Cerato_phylletum demersi, Myriophyllo-Pota-
The coal facies--reed swamp metum, Najadetum, Myriophyllo-Nupharetum,
Trapo-Nymphoidetum and Trapetum).
Plant communities: palaeophytocoenoses with Associated elements: Salvinia sp., Spirematosper-
Phragmites oeningensis and with Typha latis- mum wetzleri, Brasenia tanaitica, Myriophyllum
sima. spinosum, Trapa givulescui, Trapa victoriae,
Associated elements: Sparganium noduliferum, Trapa horrida, which could also generate mono-
Stratiotes dacicus, Butomus umbelatus, Najas coenoses. The aquatic macrophyte prairies are
lanceolata, Equisetum sp., Carex ssp. the first in an ecological succession (Fig. 3).
Palaeobiotope: permanently covered by water Vertically, in the genetical series, the aquatic
with a depth of less than 2 m, at maximum. In macrophyte prairies are replaced by swamps
deeper water the plants are drowned. with Phragmites, and these by forest swamps.
Type of deposition: autochthonous, partially Such successions can be foune in many of the
hypautochthonous up to the limit with the coal open-pit mines in Oltenia.
aquatic macrophyte prairie, because of the Palaeobiotope: permanently flooded areas, with
action of streams and storm waves. a depth of more than 2 m (in the initial stage of
Depositional milieux: subaquatic (limnic). the vegetation evolution the depth can be
Environmental characteristics: similar to modern between 0 and 3 m).
swamps with Phragmites australis, where the pH Type of deposition: autochthonous, but in many
is mainly neutral to alkaline. The plant material ways hypautochthonous because of water cur-
accumulates in anaerobic conditions. rents and storm waves than move the plant
Modern peats with Phragmites contain from material from low deep swamps.
15 to 20% ash content. By residual enrichment, Depositional milieux: subaquatic (limnic).
the resulting coals could reach between 30-50% Environmental characteristics: Similar to swamp
ash content. lakes in the Danube Delta and the Romanian
Ph. australis, is growing today in the Danube Plain where the water is introduced into the
Delta on a surface of more than 20000 ha, in lake via rivers, but almost double the rainfall
which a surface of more than 100000ha is and with a pH from neutral to alkaline. The
covered by 'plaur', a floating vegetal mass, plant remains accumulated in an anaerobic
mainly generated by the rhyzome of this species. environment.
Lithotype: detrital coal. Distinguished from the Lithotypes: frequently, in this environment coaly
detrital coal from swamps with sedge (Carex clays and clayey coals were generated. Never-
ssp.) and from hygrophite deciduous forest, theless, the frequency of Nelumbo leaves, strictly
138 N. T I C L E A N U & D. DIACONIT-~

autochthonous on the X layer level in Pinoasa References

and Plo~tina open-pit mines, lead us to the
conclusion that this species has played an ANDREESCU, I., TICLEANU, N., PANA, I., PAULIUC, S.,
important role in the phytomass constitution. PELIN, M. & BARUS, T. 1985. Stratigraphie des
d6p6ts pliocenes a charbons. Zone est d'Oltenie
In the same way that in the Okefenokee swamp (Secteur Olt-Jiu). Analele Universitdlii Bucure~ti,
(Cohen et al. 1984) Nymphaea peat together with Geologie, 34, 87-96.
Taxodium peat constitutes more than 80% of BITOIANU, C. & ILIE, S. 1967. Contribu~ii la studiul
this peat. petrografic al c~trbunilor de la Valea Motrului
Palaeophytocoenoses with Stratiotes and with (Oltenia). Studii tehnice #i economice, 7, A,
Trapa could generate such peats and also detrital 165-173.
coals. BOULTER, M. C., HUBBARD, N. L. B. R. & KVACEK,Z.
1993. A comparison of intuitive and objective
interpretations of Miocene plant assemblages
from north Bohemia. Palaeogeography, Palaeo-
climatology, Palaeoecology, 101, 81-96.
Conclusions COHEN, A. D., CASAGRANDE,D. J., ANREJKO, M. J. &
BEST, G. R. 1984. The Okefenokee Swamp: its
The Pliocene coals in Oltenia were generated in natural history, geology and geochemistry. Wet-
five distinct coal facies (grassy marsh Carex ssp., land Surveys, 709.
swamp deciduous forest, swamp with Glypto- ILIE, S. & BITOIANU, C. 1967. Studiul petrografic al
strobus, reed swamps and aquatic macrophyte c~rbunilor de la Rovinari. Studii tehnice #i
prairie) with a time and spatial distribution economice, 7, A, 177-185.
controlled, first of all, by the hydrological level, PETRESCU, I. tYr GIVULESCU, R. 1986. Flore et vegeta-
which has generated palaeobiotopes with differ- tion de la Valea du Jiu (Basin Petro~ani). Revue de
ent environmental factors (pH, Eh, etc.). Palaeobiologie continentale XIV, 2, 385-395.
Each facies has a characteristic plant commu- PoP, E. 1960. Mla~tinile de turb~ din R. P. Romgm~t.
Editura Academiei, 511.
nity, composed of one or more palaeophytocoe- POPESCU, A., SANDA, V. & NEDELCU, G. A. 1981.
noses generated by plants belonging to major Allgemeine Ubersicht fiber die Vegetation des
taxonomic groups (angiosperm, mono and Donaudeltas. Horti Bucurestiensis, Acta Botanica,
dicotyledon and gymnosperm) distinguished by 175-191.
the content in the main coal-generating sub- RUDESCU, L., NICULESCU, C. & CHIVU, I. P. 1965.
stance (cellulose, pentosane, lignin, etc.). Monorafia stufului din Delta Dun~rii. Editura
In the primary peat swamps different environ- Academiei Romdne Bucure~ti.
mental conditions from one palaeobiotope to STACH, E., MACKOWSKY, M. Th., TAYLOR, G. H.,
another and important quantities of vegetal CHANDRA, D., TEICHMULLER, M. t~r TEICHMUL-
LER, M. & TEICHMI~ILLER,R. 1975. Coal Petrol-
phytomass with different chemical composition ogy, Berlin.
accumulated. This determined the development TEICHMIJLLER, M. 1958. Rekonstruktionen verschid-
of distinct lithotypes, characterised by physical- ener Moor typen Hauptfl6zes der Niederrhei-
chemical properties (Table 1) and certain petro- nischen Braunkohlen. Fortschritte in der Geologie
graphical characteristics (Table 2), that enabled yon Rheinland und Westfalen, 2, 599-612.
differentiation of the main lithotypes detrital TICLEANU, N. 1986. Date preliminare privind studiul
coal, xylite and xylitic coal. palaeobotanic al unor foraje de referin~t, 70-71/
Phytogeographical considerations indicate 3, Palaeontologie, 235-248.
that the coal-generating flora are distinguished 1992a. Studiul genetic al principalelor zficfiminte
de cfirbuni neogeni din Romfinia pe baza palaeo-
by a strong Pliocene characteristic feature deter- fitocenozelor caracteristice, privire speciafft la
mined by: Oltenia. Tezd de doctorat, 339. Universitatea
Bucureqti, Romfinia.
the fact that corresponding modern plant - - 1 9 9 2 b . Main coal-generating palaeophytocoe-
assemblages are prevalent in the eutrophical noses in the Pliocene of Oltenia. Romanian
low moors in Romania, Journal of Palaeontology, 75, 75-80.
the important role of species Glyptostrobus 1995a. An Attempt to Reconstitute the Evolution
europaeus and Byttneriophyllum tiliaefolium; of the Mean Annual Temperature in the Neogene
the sporadic presence (relict) of the species: of Romania. Romanian Journal of Palaeontology,
Taxodium dubium, Nyssa disseminata, Acer 76/3, 137-144.
- - - 1 9 9 5 b . Taphonomic Researches on the Fossil
tricuspidatum, Carya cf aquatica and Liqui- Plants from the Pliocene Coal Deposits in Oltenia.
dambar europaeum, all of them characteristic Romanian Journal of Palaeontology, 75/3, 153-160.
of the Miocene flora in Europe, and with - - 1 9 9 5 c . Utilisation of the Palaeobotanical Data in
modern correspondents in the south-east of the Study of the Coal Deposits. Romanian Journal
North America. of Palaeontology, 76/3, 145-152.
 PLIOCENE COAL FACIES A N D LITHOTYPES IN R O M A N I A 139

- - & ANDREESCU, [. 1988. Considerations on the the Olt-Jiu sector and the structural-genetic
development of Pliocene coaly complexes in the factors. Ddri de seamd, Institutul de Geologie ~i
Jiu-Motru Sector (Oltenia). Ddri de searnd, Geofizicd, 72-73/2. Z&'dminte, 215-226.
Institutul de Geologie l'i Geofizicd, 72-73/2. - - - , BITOIANU,C., MUNTIU, O. & NAGAT, F1. 1989.
Zdcdminte, 227-244. Palaeofitocenozele carbogeneratoare, petrografia
- - & BITOIANU,C. 1989. Coal Facies, Characteristic ~i chimismul litotipilor din c~rbunii plioceni
Palaeophytocoenoses and Lithotypes of Pliocene dintre Valea Jiulu ~i Valea Amaradiei. Ddri de
from Oltenia. Studia Universitatis Babeq - Bolyai, seamd. Institutul de Geologie ~i Geofizicd, 74/2,
34, 2, 89-93. Zdcdrninte-Geochimie, 115-129.
- - , ANDREESCU, l., BITOIANU, C., PAULIUC, S., TICLEANU, N., BITOANU,C., NICOLAE, Gh., POPESCU,
NICOLAE, Gh., NI[COLAE,V., POPESCU,A., BARUS, A., TICLEANU,M., MUNTIU, O. & PROD,~,NESCU,I.
T., PASLARU,T., GRIGORESCU, Gh. & TICLEANU, 1992. P~trographie et propri6t6s physico-chimiques
M. 1988. Remarks on the relationship between des charbons pliocenes du secteur Jiu-Danube.
the spatial distribution of the coal complexes in Romanian Journal Mineral Deposits, 75, 107-115.
 Bulgarian low rank coals: geology and petrology

GEORGE D. SISKOV

Sofia University 'St. Kliment Ohridski', 15 Tsar Osvoboditel Blvd, 1504 Sofia, Bulgaria

Abstract: The largest coal-forming maximum in Bulgaria took place during the Neogene.
Fifteen coal deposits are located in four coal-bearing provinces. The coal deposits south of
the Balkan Mountains were formed in small grabens and depressions filled with molasse.
Only the coals in Northern Bulgaria were formed in a small palaeodelta. The coal measures
are of varying thickness and contain a few coal seams, with compact to complex structure
and a range of thickness. Three groups are defined on the basis of maceral composition,
allowing a reconstruction of the coal-forming ecosystems and the genesis of the genotypes
during biochemical coalification. According to Alpern's classification the coals have middle
to high ash content (ashy to coaly facies). They are of huminite type with low liptinite and
inertinite content, and of low rank - lignite and mat brown coals.

Bulgaria contains more than 50 coal deposits but the beginning of the Late Oligocene (Si~kov
most of them are of no industrial value due to et al. 1986). In that period typical marine sedi-
the complex conditions affecting their exploita- mentation was gradually replaced by limnic
tion, the nonprospective character of the sedimentation caused by progressive regression
resource and the low quality of the coals (high (Panov 1982). The coal formation occurred in
ash and sulphur content). Their formation highly peneplaned coastal areas covered with
coincides with the world coal-forming maxima eutrophic swamps.
during Carboniferous, Early Jurassic, Late
Cretaceous, Paleogene and Neogene.
The geological potential of Bulgarian coal 24~ 26~
resources is about 8 x 109 tonnes, of which 85 %
are low rank, 15 % middle rank, and < 1% high
rank coals. According to the Bulgarian Stan-
dard they are divided into four g r o u p s -
lignites, brown coals (mat and bright), hard coals,
and anthracites (Si~kov & Valceva 1983). Lignites
are concentrated in the Neogene sediments and
!
zt
.
__U 2
are one of the main energy resources in Bulgaria.

) V 4 ",-s - ~ .,*'* \ l

Geology of the Neogene coal deposits

On the basis of topographical, morphotectonic, mmm
mm mmmmmm mmmm
lithologic and genetic characteristics the Neo-
gene coal deposits are located in four coal-
bearing provinces, three of them being south of 5OO

the Balkan Mountains (Fig. 1, Table 1). Om-

The coal formation process started in Middle 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16
Miocene and ended in Pliocene. It took place
within the period of the Pyrenian and Styrian Fig. 1. Location of the coal-bearing provinces,
phases of the Late Alpine orogeny and was geolgical age and structure of the coal-bearing strata of
concentrated in local depressions and grabens the Neogene coal deposits in Bulgaria. A, Dacian coal,
filled with molasse (Ivanov 1983). Features bearing province: (1) Lom; (2) Kozloduj;
representing continuous coal formation during B, Thracian coal-bearing province: (3) Elhovo;
(4) Mariza East; (5) Mariza West; C, Sofia coal-bearing
the Paleogene maximum have been established province: (6) Sofia; (7) Beli Brjag; (8) Aldomirovzy;
in the region of the Thracian Valley. Here, after (9) Stanjanzy; (10) Kovachevzy; (11) Karlovo;
the Savic phase, a post-tectonic depression was (12) Chukurovo; D, Strimon-Mesta coal-bearing
formed (Ivanov 1983) in which there were province: (13) Kjustendil; (14) Oranovo; (15) Razlog;
favourable conditions for coal formation from (16) Goze Delchev.

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 141-148.
142 G . D . SISKOV

Table 1. Neogene coal deposits in Bulgaria

Coal-forming Coal-bearing Coal deposits Number of Geological age

maximum provinces coal seams
Neogene Dacian Lom 3 Pliocene
Kozloduj 2 Pliocene
Thracian Elhovo 3 Pliocene
Mariza East 3 Early-Middle Miocene
Mariza West 4 Early-Middle Miocene
Sofia Sofia 3 Pliocene-Late Miocene
Beli Brjag 1-5 Pliocene-Late Miocene
Aldomirovzy 1-3 Pliocene-Late Miocene
Stanjanzy 1 Pliocene-Late Miocene
Kovacevzy 1 Pliocene-Late Miocene
Karlovo 3 Pliocene-Late Miocene
Chukurovo 16 Middle Miocene
Strimon-Mesta Kjustendil 1 Pliocene-Late Miocene
Oranovo 4 Pliocene-Late Miocene
Razlog 8 Pliocene-Late Miocene
Goze Delchev 14 Pliocene-Late Miocene

Thracian coal-bearing province under the silicified 'Stone Forest' has been
found. Geological and petrological studies have
This province is situated in the area of the shown that the coal formation occurred in a
Thracian depression and is filled with sediments swamp situated in the crater of an extinct
of the lower (Paleogene) and the upper coal- volcano which was destroyed by a storm
bearing molasse (Neogene). during which marine water influx produced a
The coal formation started in the Late rapid change of geochemical conditions. The
Oligocene and continued through the Miocene coal layer is covered with pyritized wood tissue
and into the Pliocene. Gradual younging of the with upright silicified Taxodium stumps mostly
coal-bearing sediments occurred from west covered by recent sands (Si~kov et al. 1988).
(Mariza West) to east (Elhovo). According to
Kojumdgieva (1983) this is due to the gradual
progression of the regression in this direction as Sofia coal-bearing province
well as to the formation of the Black Sea. Under
these circumstances the plain had been raised This province covers the area of Western
relatively following the marine regression. The Bulgaria between the Balkan and the Sredna
period of relatively compensated sedimentation Gora Mountains. The coal-bearing sediments fill
led to the formation of thick peat deposits. The subequatorial grabens and small depressions in
Second coal seam of the Mariza East deposit which coal formation started in the Middle
(maximum thickness of 25 m) is a good illustra- Miocene (Chukurovo) and lasted till the begin-
tion of the long duration of the peat formation ning of the Pliocene (Stanjanzy).
process. In this highly active tectonic zone continental
The coal-bearing strata consist of terrigenous lakes were formed, later to be rapidly filled
sediments varying in thickness from 45 m (mini- with terrigenous sediments. Gradually these
mum at Mariza East) to 390m (maximum at lakes were transformed into eutrophic swamps
Elhovo) where 3-4 coal seams form coal-bearing with a high degree of mineralization and highly
measures of varying thickness (up to a maximum dynamic ground waters. The coal-bearing strata
of 25 m). consist of clastic sediments - conglomerates,
Paleogeographical reconstruction shows that sands, clays. Their thickness varies from 25 to
the water table in the eutrophic swamps was 100 m while in the outlying parts of the deposit it
generally high, falling very low only during reaches 900 m (Sofia). The number of coal seams
seasonal desiccations. varies from 1 to 5, except at Chukurovo where 16
An interesting phenomenon is the small coal coal seams are present in the coal-bearing
deposit in the area of the Gulf of Sozopol, where sequence. The thickness of the coal seams
a thin coal layer with preserved root systems varies up to a maximum of 15-20 m.
 BULGARIAN LOW RANK COALS 143

Strimon-Mesta coal-bearing province some small coal deposits which are older
(Kojumdgieva & Popov 1988).
This province is located in the southwestern part In various parts of the Lom deposit the deltaic
of Bulgaria. Several small coal deposits are sedimentary complex differs in structure and
situated along the valleys of the Strimon and thickness as illustrated by the irregular alterna-
Mesta rivers in almost meridional orientation. tion of the lithological bodies, represented by
The coal deposits were formed in restricted and coarser to finer clastic sediments. These sedi-
small grabens filled with coarse clastic terrige- ments contain unevenly developed benches and
nous sediments. The thickness of the coal- lenses which vary in number; a typical feature of
bearing strata varies reaching a maximum of a subaeral delta. The finer pelitic sediments of
800m (Goze Delchev). In the highly active the Lom area are typical of the lower-upper
tectonic zone favourable conditions for the delta plain (Si~kov & Angelov 1984).
formation of mezotrophic to oligotrophic In the Lom depression extensive but uneven
swamps occurred resulting in a variable number peat accumulation occurred associated with a
of coal s e a m s - 1 (Kjustendil) to 14 (Goze vast lower-upper delta plain in which lateral facies
Delchev). Laterally their thickness changes very migration was developed by a northward shift of
rapidly. The coal seams very often wedge out the deltaic front and contained fluvial channels.
and split into benches and lenses of coaly clay The coal formation in the zone of the
and clay. Kozloduj deposit developed in a coastal plain
environment. The swamp was large. In contrast
to the Lom deposit the coals were found in
Dacian coal-bearing province interdeltaic environments with a high water
table and associated with fine-grained clastic
This province is located mostly in the northern
sediments. The coal seams are up to 4 m thick
areas of the Moesian Platform including the
and cover an area of about 1 km 2 (Si~kov &
Lom and the Kozloduj deposits, the latter
representing the southern fragments of the Angelov, unpublished data).
Oltenia basin in Romania.
The coal formation is connected with the Petrology of the Neogene coals
desiccation of the Pontian Basin during a
prolonged regression in the Pliocene (Kojumd- Over 6200 coal samples were collected from
gieva 1983). The coal sediments are of Pliocene opencast and underground mines, exploratory
age - Dacian-Romanian, with the exception of boreholes and outcrops.

Table 2. Maceral composition of the Bulgarian low rank coals

No. Coal deposits Ash Maceral composition (%)

A d (%)
Total Org. matter

H L I M H L I

1. Lom 42.6 53 3 1 43 92 5 3
2. Kozloduj 20.1 71 7 1 21 90 8 2
3. Elhovo 38.3 60 2 2 36 96 2 2
4. Mariza East (briqueting) 20.2 74 1 2 23 96 1 3
5. Mariza East (energetic) 39.7 61 2 1 36 95 3 2
6. Mariza West 23.8 63 8 4 25 82 12 6
7. Sofia 16.6 77 7 2 14 89 9 2
8. Beli Brjag 15.0 66 7 8 19 87 9 4
9. Aldomirovzy 25.4 64 8 6 22 88 11 1
10. Stanjanzy 21.9 74 8 5 13 85 8 7
11. Karlovo 17.7 70 8 5 17 83 10 7
12. Kovachevzy 33.2 68 4 6 22 89 5 6
13. Chukurovo 22.3 75 14 1 10 84 15 1
14. Kjustendil 23.1 36 3 15 46 67 5 28
15. Oranovo 20.1 63 7 3 27 88 10 2
16. Razlog 20.8 75 6 1 18 92 7 1
17. Goze Delchev 17.6 80 11 3 6 85 11 4
144 G . D . SISKOV

Petrological data show that the homogeneous H

genotypes gelide, peptide, liptide and fiside form
the coal matter in various proportions, though
gelide and peptide predominate. The heteroge-
neous genotypes gelofuside, fusoliptide, etc. are
also represent.
The wide genotype differentiation is caused
by: (1) the different chemical, anatomical,
species and plant ecosystem compositions of RANK
the coal-forming plants and their behaviour
during peat formation; (2) the physico-chemical
parameters (Eh, pH) of the ground water
80% 80%
environment; (3) the type and rate of the
chemical reactions and petrological processes A~-/.
depending on the oxygen supply; (4) the activa-
SHALES
tion energy involved in the phytogenic matter
transformation during microbial metabolic pro- 75
cesses (Si~kov 1988). W SHALEY
m
In the lithotype balance humoclarite is pre- o 50
,< 1
valent (up to 85%). A higher quantity of xylain u. 35

and liptain(the latter is a specific lithotype ~A~ ,~,1I

formed by impregnated coniferous fragments
with resins - Si~kov 1976) fragments of various
size are found mainly in the coal deposits from
ASHY
PURE
4 1(
,I I,'i5i 'r
IIII
the Thracian and the Sofia coal-bearing pro-
Rr %
vinces. They are distributed chaotically. Semi-
BRIGHT
fusain and fusain are found in small amounts, 16
and occasionally mark bedding in the coal seams 17
15
of some deposits from the Thracian (Elhovo, MAT

Mariza East) and Strimon-Mesta provinces Z 0.3

(Kjustendil, Goze Delchev). <
n"
All mono-, bi- and trimacerites are represented 10,S 862 -Tg

in the microlithotype composition. Humoclarite 0.2 LIGNITE 4 1~3[ 11 |

prevails and, along with carbargilite represents

partially to completely disintegrated plants,
consisting of variously fragmented atrinite, and ~Io I
fILIal1
100% H 80% L
more rarely, of densinite. TYPE

The average compositions of the maceral Fig. 2. Triangular diagram and petrological position
analyses are given in Table 2. The macerals of by type, facies and rank of the Neogene coals in
the three groups are in different proportions, Bulgaria according to Alpern's classification: 1, Lom;
with the huminite macerals predominating. They 2, Kozloduj; 3, Elhovo; 4, 5, Mariza East; 6, Mariza
form the groundmass in which other fragmen- West; 7, Sofia; 8, Beli Brjag; 9, Aldomirovzy;
10, Stanjanzy; 11, Karlovo; 12, Kovachevzy;
tary macerals of the huminite, liptinite and 13, Chukurovo; 15, Oranovo; 16, Razlog; 17, Goze
inertinite groups are chaotically dispersed. Atri- Delchev.
nite and densinite are present in differing
amounts. Liptinite macerals are represented
mainly as resinite and more rarely as cutinite, that the Neogene coals in Bulgaria are of
sporinite and suberinite. huminite type with a minimum content of
The mineral components are represented by liptinite and inertinite.
widely varying amounts of clays and pyrite. The The principal components are determined on
clay minerals consist of kaolinite, illite and the basis of a correlation matrix using the
montmorilonite. algorithm reported by Wehlstedt & Davis
The maceral amount recalculated per organic (1968). The Q-dendrograph was plotted by the
matter shows that the Neogene coals are method of McCammon&Wenninnger (1970)
relatively homogeneous in composition contain- (Si~kov & Andreev 1987).
ing more than 80% of huminite, with the The cluster analyses indicate that the Neogene
exception of the Kjustendil coals (Table 2, coals are very distinctly differentiated into three
Fig. 2). The average petrological data show groups (Fig. 3, Table 3).
 BULGARIAN LOW RANK COALS 145

tectonic position of the coal deposits, the

I I physico-chemical environment in the peat bogs
0.06 I B
I and the hydrodynamics of the groundwater
[ J ] I
0.04
i A2 I
table.
B2 B~
Coals in which the coal-forming communities
are equally divided between forest and herbac-
0.02
eous populations are referred to Group A.
The petrological investigations show that the
2 7 16 8 17 15 9 13 6 11 10 12 1 4 5 3 14
forest vegetation consists of angiosperm and
40 50 60 HII coniferous species. The coniferous species in
1PC = 0.74 H - 0.08 L - 0.66 I (79%) /
1Q
\
~3 combination with herbaceous vegetation form
2PC = - 0.34 H - 0.81L - 0.48 I (21%) ./ A \ Subgroup A~ where the amount of densinite
-20
groundmass considerably predominates. The
amount of well preserved wood tissue producing
textinite and textoulminite filled with resinite
also increases.
- 30
Coals from three deposits form Subgroup A2
(Table 3) in which herbaceous vegetation pre-
dominates while the number of angiosperm and
Fig. 3. Q-dendrograph and grouping of the Neogene coniferous species is equivalent. The amount of
coal deposits by their maceral composition: 1, Lore; densinite is prevalent and the content of eu-
2, Kozloduj; 3, Elhovo; 4, 5, Mariza East; 6, Mariza ulminite and gelinite increases. The coals from
West; 7, Sofia; 8, Bell Brjag; 9, Aldomirovzy; the Chukurovo deposit are distinct. They con-
10, Stanjanzy; 11, Karlovo; 12, Kovachevzy; tain mainly species, Taxodiaceae being particu-
13, Chukurovo; 14, Kjustendil; 15, Oranovo; larly typical. Due to the prevalence of coniferous
16, Razlog; 17, Goze Delchev.
vegetation the amount of resinite also increases
markedly.
Coals predominantly formed by herbaceous
Groups A and B are each subdivided into two vegetation in peat-producing ecosystems with a
subgroups. Coals, having huminite 82-92%, are lower participation of forest species are assigned
referred to Group A. Coals, containing huminite to Group B. In this case huminite macerals are
above 92%, are assigned to Group B. A highly gelified and the groundmass consists of
significant difference is observed in the Kjusten- atrinite. Their division into two subgroups is
dil deposit due to the higher content of inertinite based on the amount of inertinite.
(Group C). Another important petrological factor, related
The grouping of the coals in accordance with to the genesis of coal macerals is the nature of
the ratios (H/I) and (L/I, H) is illustrated in the peat swamps and their hydrodynamics.
Fig. 3, where the H/I ratio has an average value Where major tectonic activity and enhanced
of 79%. hydrodynamics and aeration of ground water
The statistical analysis of the maceral content occurs, possible seasonal desiccation would
provides a means of reconstructing the peat- result in oxidation leading to a deviation from
forming ecosystems in combination with the the general maceral balance. This is the reason

Table 3. Petrological groups of the Neogene coal deposits in Bulgaria

Group Subgroup Maceral composition (%) Coal deposits

H L I

A A1 85-92 7-11 1-4 Kozloduj (2), Sofia (7), Beli Brjag (8),
Aldomirovzy (9), Oranovo (15),
Razlog (16), Goze Delchev (17)
A2 82-85 8-12 6-7 Mariza West (6), Stanjanzy (10),
Karlovo (11), Chukurovo (13)
B B1 > 92 1-5 2-3 Lom (1), Elhovo (3), Mariza East (4, 5)
B2 89 5 6 Kovachevzy (12)
C 67 15 28 Kjustendil (14)
 Table 4. Rank parameters of the Neogene coals in Bulgaria

Coal deposits Relectance Bed moisture Carbon Volatile matter Calorific value
Rr (%) W r (%) C daf (%) VM daf (%) Osdaf (kJ/kg)

Lom 0.13 50.0 64.7 67.7 22.52

Kozloduj 0.22 51.8 65.1 64.1 22.68
Elhovo 0.18 63.6 63.8 53.0 22.76
Mariza East 0.20 64.4 65.0 55.8 22.31
Mariza West 0.21 43.1 62.3 58.8 22.87
Sofia 0.22 50.0 64.6 52.0 23.51
Beli Brjag 0.22 47.5 63.8 53.4 23.27
Aldomirovzy 0.21 51.6 64.1 52.6 22.92
Stanjanzy 0.21 52.5 61.6 61.0 19.42
Kovachevzy 0.22 48.6 63.9 67.3 22.78
Karlovo 0.19 44.0 64.8 58.8 23.77
Chukurovo 0.20 33.0 64.3 57.0 23.38
Kjustendil 0.33 26.6 66.9 51.0 23.98
Oranovo 0.34 30.4 66.0 48.3 23.85
Razlog 0.39 32.5 64.8 55.4 22.92
Goze Delchev 0.41 43.5 67.9 49.1 23.02

LOW RANK I TRANSITIONzoNE ] MEDIUMRANK

.x
I Xx [ ~ . ~ ~

-24 MJ/Ro .-- , ~ -

21.

Q = 21.569+ 6.316Rr - 3.183Rr2

r = 0.653, n = 27

19 . .
0.4 0.6 0.8 1~0 %RF
l~ls~3~tl L , ,, , l,,
Stand.
ASH LIGNITE SUB. ~ B I T ' ~ - ~ HIGHVOL BITUMINOUS

r
xx
W = 76.602 - 159.664Rr + 101.913Rr 2
xx x ~ ~ x r = 0.862, n=27

6al o~
0.2 0.4 0.6 0.8 1.0

x x VM = 69.187
x ~ ~ r = 0.836, n-26~7"15Rr + 26"885Rr2

x x x x

_x
o2
0.2 0.4 0.6 0.8 1.0

75 ~ 2 x x x x xx
70
x ,,~mll-"~ )(~' x r = 0.924, n=27

0.2 0.4 0.6 O.8 1.0 %Rr

Fig. 4. Rank classification of the Cenozoic coals in Bulgaria and the position of the Neogene coals according to
Alpern's classification, Bulgarian Standard and ASTM as well as relationship of reflectance (Rr, %), bed moisture
(W r, %), volatile matter (VM daf, %), carbon content (C daf, %) and calorific value (Qdaf, MJ/kg).
 BULGARIAN LOW RANK COALS 147

for the difference in the coals from the Kjus- The author would like to thank Dr A. Andreev
tendil and Kovachevzy deposits. (Geological Institute of the Bulgarian Academy of
The results of the maceral analysis of our Sciences) for computation of the maceral data. The
study appear to be in agreement with the author is also indebted to Dr I. Todorov (Bulgarian
Research & Services Group Ltd) for the preparation of
published indices (Diessel 1986; Calder et al.
the figures.
1991).
The coal facies determined on the basis of the
ash content and maceral composition are illu-
strated in Fig. 2, where the position of macerals References
is projected on the abscissa. ALPERN, B. 1981. Pour une classification syntetique
The content of ash is between 17.6 wt % universelle des combustibles. In: La geologie des
(Goze Delchev) and 42.6 wt % (Lore). Most of charbons, des schistes bitumineux et des kerogenes,
the coals belong to the ashy humic facies. Only 271-290.
coals from the Lom and Elhovo deposits as well CALDER, J. H., GIBBING,M. R. • MUKHOPADHYAY,P.
as a part of the Mariza East deposit are coally K. 1991. Peat formation in a Westphalian B
humic facies. piendment setting, Cumberland Basin, Nova
Scotia: implications for the maceral-based inter-
The average classification parameters - humi-
preparation of rheotrophic and raised paleomires.
nite (gelinite) reflectance (Rr, %), calorific value Bulletin de la Societe geologique de France, 162, 2,
(Qsdaf, MJ/kg), bed moisture (W r, %), yield of 283-298.
volatile matter ( V M ~ %) and carbon content DIESSEL, C. F. K. 1986. On the correlation between
(C dav, %), are given in Table 4. coal facies and depositional environments. In.
The position of the Neogene coals is plotted in Advances in the Study of the Sydney Basin.
Fig. 4. There are good correlations between the Proceedings of 20th Newcastle Symposium~
huminite reflectance and the other classification 19-22.
parameters. |VANOV, Z. 1983. Apercu general sur l'evolution geo-
logique et structurale des Balkanides. In: Guide de
l'exeursion. University Press of Sofia, 3-26.
KOJUMDGIEVA,E. 1983. Paleogeographic environment
during the desiccation of the Black Sea. Palaeo-
Conclusion geography, Palaeoclimatology, Palaeoecology, 43,
195-204.
The Neogene coals in Bulgaria belong to the low - - & PoPov, N. 1988 . Lithostratigraphy of the
rank coals of Alpern's classification. On the Neogene sediments in Bulgaria. Palaeontology,
ASTM scheme they are determined as lignites. Stratigraphy, Lithology, 25, 3-26.
According to the Bulgarian Standard the MCCAMMON, R. I. t~ WENNINNGER, G. 1970. The
dendrograph. Kansas Geological Survey Computer
coals are divided into lignites (Class O1) and
Control, 48.
mat brown coals (Class O2), with the exception PANOV, G. 1982. Tertiary coal sedimentation in the
of the coals from the Goze Delchev deposit Upperthracian depression. PhD thesis.
which are referred to the bright brown coals SlgI~OV, G. 1976. Liptain- properties and genesis.
(Class 03). Annuaire de l'Universite de Sofia, Faculte de
The low coalification of the coals from the Geoloque et Geographie, 67, 1, 151-169.
Thracian, Sofia and Dacian coal-bearing pro- 1988. Theoretical fundamentals of biochemical
vinces is a consequence of the relatively small eoalification. Kliment Ohridski University Press,
thickness of the overburden sediments and the Sofia.
- - & ANDREEV,A. 1987. A way to reconstruct coal-
short geological time for the development of the
forming peleoplant communities based on the
coalification process. The coalification degree of micropetrographic composition of Bulgarian
the coals from the Strimon-Mesta province is Neogene coals. Comptes rendus de l'Academie
higher and depends on: (1) the thickness of the bulgar des sciences, 40, 4, 77-80.
overburden sediments (to 500m) which has & ANGELOV, A. 1984. Delta-plain model of
caused the reorientation of the coal genotypes sedimentation of the Lom lignite basin. Comptes
(lithotypes, microlithotypes, macerals) and the rendus de l'Academie bulgar des sciences, 37, 11,
appearance of macro- and microbedding; and 1531-1533.
(2) an anomalous geothermal gradient. Veli- - - & VALCEVA,S. 1983. Petrological nomenclature
of lignites and brown coals. Comptes rendus de
nov&Bojadgieva (1981) have stated that the
l'Academie bulgar des sciences, 36, 6, 799-801.
temperature measured in the boreholes at 300 m SISKOV, G., STEFANOVA, U. t~ ZLATEV, I. 1986.
depth is 37-38~ and at 500m depth, 66~ Petrological characteristics of the coals from the
(3) the tectonic mobility - rapid tectonic move- Brod member in the West Mariza basin. Annuaire
ments occurring along faults, typical of the zone de l'Universite de Sofia, Faculte de Geologie et
of the Kraishte lineament. Geographie, 76, l, 40-53.
148 G.D. SISKOV

SISKOV, G., VALCEVA, S. & PIMPIREV, H. 1988. VELINOV, T. & BOJADGIEVA, K. 1981. Geothermal
Preconditions for the formation of the 'Stone investigations in Bulgaria. Technika, Sofia.
forest' and coal deposits in the Gulf of Sozopol. WEHLSTEDT, W. C. & DAVIS, J. C. 1968. Fortran IV
Annuaire de l'Universite de Sofia, Faculte de program for computation and display of principal
Geologie et geographie, 77, 1, 190--200. components. Kansas Geological Survey Computer
Control, 21.
 Coal petrology and facies associations of the South Yakutian
Coal Basin, Siberia
I. E. S T U K A L O V A

Geological Institute of Russian Academy of Sciences, Pyzhevsky per., 7,

Moscow, 109017, Russia

Abstract: The South Yakutian Coal Basin consists of isolated depressions in the south of
the Yakutian region of Eastern Siberia in Russia, which are filled with Jurassic and
Cretaceous coal-bearing sediments. The basin contains considerable resources of high-
quality bituminous coals, with a caking index (y) of 6-21 mm. The coal-bearing formation
contains coal seams of various thickness, from 0.5-2.5m up to 15.0m and above. Some of
them are near the surface and can be mined by opencut methods. Genetic types and facies of
the Mesozoic coal-bearing strata have been recognised as proluvial, alluvial, delta,
lacustrine-swamp and peat bogs sediments. The petrographic composition of the
sandstones identified four terrigenous-mineral associations, which are represented by true
arkoses, greywacke arkoses, feldspar-quartz and quartz-feldspar greywackes. Humic coals
consists of vitrinite (70-90%), inertinite (10-20%) and liptinite (0-10%) maceral groups. In
the vitrinite maceral group there is a high percentage of telinite macerals, up to 60-65%. The
basin is characterized by a high alteration of Mesozoic sediments and organic matter. Coals
are of middle and high rank (0.65-2.15% R0). There are high concentrations of bitumen in
chloroform extracts of organic matter from the coals, from 0.0938% to 3.6466%. The
mineral matter of terrigenous rocks is altered to the catagenetic stage and the metagenetic
stage. The South Yakutian coals are of high quality because of their rank and composition.

The South Yakutian Coal Basin is located in the are situated in the region. It is a very important
south of the Yakutian region of Eastern Siberia coal basin in Russia, and contains considerable
in Russia, between 56~ ~ North and 120~ ~ resources of high-quality bituminous coals. The
East (Fig. 1). The basin extends from the coal-bearing formation contains coal seams
Oliokma river in the west to the Uchur fiver in varying in thickness from 0.5-2.5m to greater
the east and covers an area of 25 100 square km. than 15.0 m. Some of the seams are near the
The towns of Aldan, Nerjungri and Chulman surface and can be mined by opencut methods.
The South Yakutian Coal Basin includes three
main coal-bearing regions, namely: Usmun,
A l d a n o - C h u l m a n and Tokin regions (Fig. 1).
- ;OON The Nerjungri coalfield in the A l d a n o - C h u l m a n
region contains caking coals which are now
opencut mined, producing about 9 Mt per year.
The Nerjungri coalfield is situated near the rail
station at Chulman town and the coals are
exported to the Far East region of Russia and to
Japan. The Elga coalfield in the Tokin region
also contains caking coals, but the coalfield is
situated far from the rail system and it will be
opencut mined in the future.
The stratigraphy and coal-bearing potential of
120 0 126~ 132.* E the sediments in the South Yakutian Coal Basin
have been investigated by many authors (Pros-
Q 75 150Km
i * . I viryakova 1961; Mokrinsky 1961; Waltz 1961;
Fatkulin et al. 1970; Bredihin 1973; Prilutsky
1979; Zhelinsky 1980; Markovich 1981; Vlasov
1981; Nazarov & Stukalova 1991) and are now
Fig. 1. Sketch map of the South Yakutian Coal well known; but many problems have yet to be
Basin (revised after Bredihin 1973). 1, Mesozoic solved. At present there is no information about
coal-bearing deposits; 2, Coal-bearing regions: reasons for the high degree of metamorphism of
(1) Usmun, (2) Aldano-Chulman, (3) Tokin. the South Yakutian coals.

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geologyand Technology,
Geological Society Special Publication No. 125, pp. 149-160.
150 I. E. STUKALOVA

There is no concensus about the tectonic rocks also occur. Mesozoic rocks are more
position of the South Yakutian Coal Basin. than 3500m thick and are represented by
Some investigators consider that the basin various members of terrigenous strata, ranging
formed in intermontain depressions (Bredihin from Early Jurassic to Early Cretaceous in age.
1973; Terentyev 1979; Vlasov 1981); others that Lower Cretaceous terrigenous sediments with-
the depressions are paleorifts (Nazarov & out coals of the Nagornaya Member are
Stukalova 1991). developed in the south of the region as are
Cretaceous volcanic sediments of the Karaulov
Member. Jurassic-Cretaceous alkaline intrusive
Geological setting and stratigraphy rocks also occur (Fig. 2).
Coal-bearing strata are developed in the
The South Yakutian Coal Basin consists of Usmun and Aldano-Chulman regions, where
isolated depressions in the south of the Siberian Early Jurassic deposits of the Juhta Member
platform, which are filled with Jurassic and consist of conglomerates and coarse and
Cretaceous coal-bearing sediments (Fig. 2). The medium sandstones of proluvial origin (Fig. 3).
Mesozoic aulacogens are related to major region Middle Jurassic sediments of the Duraji Member
faults. The Mesozoic sediments are deposited on are represented by coarse, medium and fine
Archean-Proterozoic igneous and high-grade ground alluvial sandstones with many coal
metamorphic basement. Precambrian granites seams between 0.5-2.0m thickness. Upper
and gneisses are widespread in the region and Jurassic sediments comprise three Members:
metamorphosed. Lower Cambrian carbonate Kabakta, Berkakit and Nerjungra. The Kabakta

Fig. 2. Geological map of the South Yakutian Coal Basin, Siberia (revised after Zhelinsky, 1980). 1-4, Mesozoic
coal-bearing deposits: (1) Lower Jurassic, Juhta Member (J1); (2) Middle Jurassic, Duraji Member (J2); (3) Upper
Jurassic, Kabakta, Berkakit and Nerjungra Members 03); (4) Lower Cretaceous, Holodnican Member (Crl);
(5) Lower Cretaceous terrigenous sediments of Nagornaya Member; (6) Cretaceous volcanic sediments
of Karaulov Member; (7) Jurassic-Cretaceous alkaline intrusive rocks; (8) Lower Cambrian carbonate
metamorphic rocks; (9) Precambrian igneous and metamorphic rocks; (10) faults; (11) Coal-bearing regions:
1, Usmun, 2, Aldano-Chulman, 3, Tokin; (12) profiles with boreholes in regions: (AB) Usmun region,
(CD) Aldano-Chulman region, (EF) Tokin region.
 SOUTH YAKUTIAN COAL BASIN 151

/./sare/t ,4,~#erzo- @~i~

re eian Clqu[azo'/t
/'e.Cte/t r e j i ~#

~9":'. ~K. , , ~~:%

.."~ ~. ~ m ~

~9 . .... '7

o~

- ~.. ~ .~--~

Fig. 3. Stratigraphy, lithology and coal rank in coal-bearing strata in three regions of the South Yakutian
Coal Basin.

and Berkakit Members consist of nearshore Holodnican Member contain, in the Tokin
medium and fine grained sandstones and coarse region, alluvial conglomerates, coarse, medium
and fine grained siltstones and mudstones with and fine-grained santstones and coarse and fine-
paralic coal seams 1.0-2.5 m in thickness. The grained siltstones with thick coal seams
Nerjungra Member is formed of alluvial and (5.0-10.0 m). In the Aldano-Chulman region
deltaic coarse, medium and fine-grained sand- the Early Cretaceous sediments consist of
stones and coarse and fine-grained siltstones alluvial conglomerates and sandstones without
with coal seams of great thickness up to 25.0- coals, and in the Usmun region Early Cretac-
30.0m in the Aldano-Chulman region. The eous sediments are absent (Fig. 3).
high-quality caking coals of the Nerjungry The strata are cyclic and contain a complex
coalfield in the Aldano-Chulman region are of floral fragments and palinology (Mokrinsky
mined by opencut methods. In the Usmun 1961; Bredihin 1973). The age of coal-bearing
region the Nerjungry Member is missing. In strata has been determined by the flora and
the Tokin region the Nerjungra Member is other fossils. The Jurassic sequence is character-
represented by proluvial and alluvial coarse ized by the flora Annulariopsis microphylla
and medium grained sandstones with thin coal Vassil., Neocalamites sp., Phlebopteris cf. poly-
seams. Early Cretaceous sediments of the podiodes Brougn., Czekanowskia Setacea Heer,
152 I. E. S T U K A L O V A
 SOUTH YAKUTIAN COAL BASIN 153

Raphaelia diamensis Sew, Cladophlebis serrulata

Sam and others (Prosviryakova 1961; Bredihin
1973; Markovich 1981). too"/.
The cretaceous rocks contain the flora Equi-
setites asiaticus Pryn., Ctenis yokoyamai Kr. et
Pryn., cf. burejensis Pryn., Coniopteris nym-
phrum Heer, Czekanowskia rigida Heer, Pityo-
phyllum nordenskioldii (Heer) Nath., and others
(Prosviryakova 1961; Markovich 1981).
The palaeoenvironment and facies of the
Mesozoic coal-bearing strata have been deter-
mined as proluvial, alluvial, delta, lacustrine-
swamp and peat bogs (Nazarov & Stukalova
1991).
s F
too% 1s

Petrographic composition of coals

One of the aims of the study of the South Fig. 5. Terrigenous-mineral associations of sandstones
Yakutian coals was to explain the high caking in the coal-bearing strata of the South Yakutian Coal
characteristics of the coals. We investigated Basin (revised after Nazarov & Stukalova, 1991).
coals in the Usmun, A l d a n o - C h u l m a n and Diagram by Shutov 1972. Explanation: Q, quartz;
Tokin regions of the South Yakutian Coal F, feldspar; R, rock fragments; (1) true arkoses and
Basin. The method was to define the maceral feldspar~luartz sandstones with a low content of
composition, and the technological and chemi- quartzite, granite and gneiss fragments; typical of the
cal properties of the very thick coals, such as Lower Jurassic association in the Aldano~hulman
and the Usmun regions; (2) feldspar~luartz
the Upper Jurassic coal seams in the A l d a n o -
greywackes and greywacke arkoses with a high content
Chulman region and the Lower Cretaceous coal of quartzite, granite and gneiss fragments; typical of
seams in the Tokin region. The coals were the Middle and Upper Jurassic association in the three
analyzed microscopically, and by chemical and regions; (3)'greywacke arkoses, feldspar-quartz
organic geochemical methods. We investigated greywackes and quartz-feldspar greywackes with high
the maceral composition of the coals using content of quartz porphyry, felsitic porphyry, andesite,
transmitted light with thin sections and incident granite and trachyte fragments; typical of the Upper
light with polished sections with magnifications Jurassic and Lower Cretaceous association in the
of 20-600x. Humic coals consist of vitrinite Aldano-Chulman region; (4) greywacke arkoses and
quartz-feldspar greywackes with a high content of
(70-90%), inertinite (10-20%) and liptinite
rhyolite, felsitic porphyry, trachyte and their tuff
(0-10%) maceral groups. The vitrinite maceral fragments; typical of the Lower Cretaceous association
group contains a high percentage of telinite in the Tokin region.
macerals, up to 60-65% (Fig. 4). For example,
bituminous coals with high volatile matter con- components (L) represented by cutinite and
tent in the Elga coalfield of the Tokin region, resinite (sample 225.0/131 and sample 325.0/
using an oil immersion objective, was shown to 131, Fig. 4, photo 5,6).
contain: inertinite components (I) representing
transformed wood fragments (sample 375.0/128
and sample 410.0/128, Fig. 4, photo 1,2); a high Proximate analyses and vitrinite
percentage, up to 70-80%, of vitrinite compo- reflectance values
nents (Vt) represented by telinite (Vtl) and
collinite (Vt2) (sample 505.0/128 and sample Chemical analyses of the South Yakutian coals
320.0/131, Fig. 4, photo 3,4); and liptinite gave moisture contents (W daf) from 0.20% to

Fig. 4. Petrographic composition of bituninous coals with high volatile matter in the Tokin region (Elga coalfield)
of the South Yakutian Coal Basin, Lower Cretaceous, Holodnikan Member, incident light, oil immersion,
magnification x300. Indices: Vtl, telinite; Vt2, collinite; I, inertinite; L, liptinite. Photo 1. Sample 375.0/128.
Inertinite components, borehole 128, depth 375.0 m. Photo 2. Sample 410.0/128. Inertinite components, borehole
128, depth 410.0 m. Photo 3. Sample 505.0/128. Vitrinite components (collinite), borehole 128, depth 505.0 m.
Photo 4. Sample 320.0/131. Vitrinite components (telinite), borehole 131, depth 320.0m. Photo 5. Sample
225.10/131. Liptinite components (cutinite and resinite), borehole 131, depth 225.0 m. Photo 6. Sample 325.0/131.
Liptinite components (cutinite) and vitrinite components (telinite), borehole 131, depth 325.0 m.
154 I. E. STUKALOVA

J-W A/-E
, A B

2z

i 177

50 53 51]

::: x
,~.~, ~'~ 21
. ~ 9~ ~ [ ~ [7~]~.
7

0,5~ o

[r/ s Fzz:I, IX.xls -B]e

Fig. 6. Lithology and terrigenous-mineral associations of the coal-bearing strata in the Aldano Chulman region
of the South Yakutian Coal Basin, Siberia. Expiation for figures 6-8: 1, conglomerates; 2, sandstones; 3, siltstones
and mudstones; 4, coal seams; 5, true arkoses and feldspar-quartz sandstones with a low content of quartzite,
granite and gneiss fragments; typical of the Lower Jurassic association in the Aldano Chulman and the Usmun
regions; 6, feldspar-quartz greywackes and greywacke arkoses with a high content of quartzite, granite and gneiss
fragments; typical of the Middle and Upper Jurassic association in the three regions; 7, greywacke arkoses,
feldspar-quartz greywackes and quartz-feldspar greywackes with a high content of quartz porphyry, felsitic
porphyry, andesite, granite and trachyte fragments; typical of the Upper Jurassic and Lower Cretaceous
association in the Aldano-Chulman region; 8, greywacke arkoses and quartz-feldspar greywackes with a high
content of rhyolite, felsitic porphyry, trachyte and their tuff fragments; typical of the Lower Cretaceous
association in the Tokin region; 9, isoreflectance lines; 10, boreholes.

2.80%, volatile matter contents (V daf) ranging of 0.65-2.15%. In all the boreholes investigated
from 17.0% to 40.0%, ash content (A daf) vary- (more than 50 boreholes with more than 500
ing from 1.57% to 25.92%, caking index (y) of samples) the vitrinite reflectance values increase
6-21 ram. with depth. In the Usmun region the vitrinite
Vitrinite reflectance was measured according reflectance (Ro) of organic matter varies from
to ICCP standards (Stach 1982) on polished 0.55% to 1.00%. On the profile A - B of the
sections of the coals using a microscope-photo- Usmun region (Fig. 6) the isoreflectance lines of
meter 'MRE-Leitz', with a magnification of 0.55% R0 and 0.85% R0 are indicated. These are
600x. Jurassic and Cretaceous coals in the high volatile bituminous coals (Fig. 3). In the
South Yakutian Coal Basin have middle and A l d a n o - C h u l m a n region the vitrinite reflectance
high rank, with vitrinite reflectance values (R0) varies from 1.15% to 2.15%. The profile C - D of
 SOUTH YAKUTIAN COAL BASIN 155

I G 1868
2531

' 253~ \ LL2811m

44 O 2, 4 X~
%,~ _ ' I

2785

' -- . . . . . -~i Z 7 8 4 277S

-~~i ~2777

,.'.N
~
..-~, "
:-~X' ',-2. "-I,55R ~
2.
,,-%

~" A ~
, ~

4)
,0 'x'~r~ ii:l~
11
'-2"
9 o,

t-I -Ro

Fig. 7. Lithology and terrigenous-mineral associations of the coal-bearing strata in the Aldano-Chulman region
of the South Yakutian Coal Basin, Siberia.

the Aldano-Chulman region (Fig. 7) shows 1990; Puttmann et al. 1985) bitumen analyses
isoreflectance lines of 1.55% R0 and 2.00% Ro. and column chromatography were carried out.
These are low volatile bituminous coals (Fig. 3). Samples from different coalfields in the South
In the Tokin region of the South Yakutian Coal Yakutian Basin were investigated. In the Usmun
Basin vitrinite reflectance ranges from 0.65% to region we investigated high volatile coals from
1.15%. On the profile E-F of the Tokin region three boreholes, No 50, 165 and 203 in the
(Fig. 8) isoreflectance lines of 0.75%Ro, Syllach coalfield. The vitrinite reflectance (R0) is
0.85% R0 and 1.00% R0 are shown. These are 0.75%, the volatile matter is about 33-40% and
high volatile bituminous coals (Fig. 3). the caking index is 6-21 ram. In the Tokin
region high volatile coals were investigated with
a vitrinite reflectance of about 1.0%, volatile
Bitumen analyses matter of about 27-40% and a caking index is
6-21 mm. The coals are from boreholes No 13,
In order to better understand the effects of 108, 110, 146, 158 and 160 in the Elga coalfield.
metamorphism on the technological and chemi- In the Aldano-Chulman region low volatile
cal properties of the coals (Teichmuller 1974, coals were investigated with 1.5%R0 and
156 I. E. STUKALOVA

N-s
E F
128
l,~176

".[~
0
~ ,
77
.', 131 0 1 2Kin
p 9
9 .~- ltIO)~ I I I
.=. ,~!v
12 15

I~1
~ ' ~176 8
/ /
0 85 " -" g,o
z_z]
!::I 9
'

,'-; ~ ~ 1B
,~/ X "" ~ ~

I
*~,o-
i 9 i /
:.:~<
//~ ~; .,'
.r .
-'-'
9 ~ . "'"
~1 1,0 Ro

Fig. 8. Lithology and terrigenous-mineral associations of the coal-bearing strata in the Tokin region of the South
Yakutian Coal Basin, Siberia.

17-22% volatile matter. The caking index is up in the basin yielded high levels of bitumen.
to 6-21 mm. The samples were from borehole Concentrations of chloroformic bitumen vary
No 3455 in Nerungri coalfield. from 0.0938% to 3.6466%, of alcohol-benzolic
According bitumen analyses, the fifteen inves- bitumen (A) from 0.0345% to 3.7266% and of
tigated samples contain water (H20) from alcohol-benzolic bitumen (C) from 0.0322% to
0.08% to 2.71%. The contents of ash varies 1.886%. Concentrations of total bitumen range
from 9.20% to 40.75% and CO2 from 0.80% to from 0.1635% to 7.9838%.
10.00%. Insoluble organic matter varies between Chloroform extracts were separated into dif-
77.88%-95.05%. No humic acids were detected ferent fractions by column chromatography. The
due to the high alteration of sediments. Extracts concentrations of methano-naphthene oils are
of organic matter in chloroform from the coals from 6.25% to 26.21%, and of polyaromatic

Fig. 9. Petrographic composition of sandstones in coal-bearing strata in the Aldano-Chulman region of the
South Yakutian Coal Basin, transmitted light, crossed polars, magnification • Indices: Q, quartz;
P1, plagioclases; F, feldspars; R, rock fragments. Photo 1. Sample 27.5/1868. Lower Cretaceous, Holodnican
Member, borehole 1868, depth 27.5 m. Greywacke sandstone with high content of quartz and felsitic porphyry,
quartzites and granites, sericitization of feldspar. Photo 2. Sample 74.5/1868. Lower Cretaceous, Holodnican
Member, borehole 1868, depth 74.5 m. Greywacke sandstone with high content of quartz and felsitic porphyry,
quartzites and granites, chloritic and laumontite cement, sericitization of feldspar. Photo 3. Sample 560.1/2777.
Middle Jurassic, Duraji Member, borehole 2777, depth 560.1 m. Quartz-feldspar greywacke with high content of
felsitic and quartz porphyry, granites, gneisses and rare trachytes, hydromica and laumontite cement. Photo 4.
Sample 590.4/2777. Middle Jurassic, Duraji Member, borehole 2777, depth 590.4 m. Feldspar-quartz greywacke
with high content of granites and gneisses, hydromica and quartz cement. Photo 5. Sample 837.9/2777. Lower
Jurassic, Juhta Member, borehole 2777, depth 837.9 m. Feldspar-quartz sandstone with few quartzite, granite and
rarely dolomite fragments, hydromica and laumontite cement. Photo 6. Sample 847.9/2777. Lower Jurassic, Juhta
Member, borehole 2777, depth 847.9 m. Feldspar-quartz sandstone with few quartzite and granite fragments.
SOUTH YAKUTIAN COAL BASIN 157
158 I. E. STUKALOVA

oils from 4.92% to 15.95%. The total content of Quartz-feldspar greywacke of sample 560.1/
methano-naphthene, aromatic and polyaromatic 2777 from 560.1m in borehole 2777 contains
oils is from 12.50% to 34.13%, with a maximum 20% of quartz (Q), 40% of feldspar (F)
of 43.51%, representing a high concentration of and 40% of rock fragments (R), represented
hydrocarbons. The extracts contain 7.38-21.90% by felsitic and quartz porphyries, granites,
of benzolic resins 0.41% to 1.88% of alcohol gneisses and trachytes. These sandstones contain
resins and 0.49-1.15% of alcohol-benzolic resins a hydromica and laumontite pore cement
present in three samples. The concentration of (Fig. 9, photo 3). Another example, sample
high molecular weight resins and combinations 590.4/2777, is represented by feldspar-quartz
are from 4.92% to 21.39%. The contents of all greywacke from 590.4m in borehole 2777. It
resins varies from 13.30% to 49.90%. The contains 30% of quartz (Q), 35% of feldspar (F)
extracts also contain asphaltenes ranging from and 35% of rock fragments (R), represented
20.34% to 69.95%. by granites and gneisses. These sandstones
The high concentration of bitumen in the contain a hydromica and quartz pore cement
chloroform extracts of organic matter of the (Fig. 9, photo 4).
South Yakutian coals, is probably responsible The third association of true arkoses, grey-
for the high caking properties of the coals. wackes with high content of quartz and felsitic
porphyries, quartzites and granites (Fig. 4), is
typical of the Upper Jurassic and Lower Cretac-
Petrographic composition of sandstones eous deposits in the Aldano-Chulman region
(Fig. 7). For example, the greywacke medium
The petrographic composition of the sandstones sandstone of sample 27.5/1868 from 27.5m in
in coal-bearing strata of the South Yakutian borehole 1868 contains 20% of quartz (Q), 30%
Coal Basin identified four terrigenous-mineral of feldspar (F) and 50% of rock fragments (R),
associations, according to the scheme proposed represented by quartz and felsitic porphyries,
by Shutov (1972). The first is represented by quartzites and granites. The sericitization of
true arkoses and feldspar-quartz sandstones feldspar is widespread (Fig. 9, photo 1). Another
with a low content of quartzite, granite and example, sample 74.5/1868 is represented by
gneiss fragments (Fig. 5). It is a typical Lower greywacke medium sandstone from 74.5m in
Jurassic association in the Usmun and Aldano- borehole 1868 in the Aldano-Chulman region
Chulman regions (Figs 6 & 7). For example, from the Lower Cretaceous, Holodnican
sample 837.9/2777 from a depth of 837.9m Member. It contains 25% of quartz (Q), 25%
in borehole 2777 in the Aldano-Chulman of feldspar (F) and 50% of rock fragments (R),
region, is a feldspar-quartz coarse sandstone represented with high content of quartz and
containing 60% of quartz (Q), 20% of feldspar felsitic porhpyries, quartzites and granites. These
(F) and 20% of rock fragments (R), represented sandstones contain a chloritic and laumontite
by quartzite, granite and dolomite fragments. pore cement. The sericitization of feldspar is
These sandstones contain a hydromica and widespread (Fig. 9, photo 2).
laumontite pore cement (Fig. 9, photo 5). The fourth association of feldpathic grey-
Another example, sample 847.9/2777 from a wackes and greywacke with a high content of
depth of 847.9m in the same borehole 2777, is rhyolites, felsitic porphyries, trachites and their
a feldspar-quartz medium sandstone containing tufts (Fig. 4), is mostly encountered in the Lower
55% of quartz (Q), 20% of feldspar (F) Cretaceous deposits of the Tokin region (Fig. 8).
and 25% of rock fragments (R), represented
by quartzite and granite fragments. Feldspar
is represented by plagioclases (P1). These Mineral alteration
sandstones contain a hydromica pore cement
(Fig. 9, photo 6). Mineral alterations were investigated both by
The second association features greywacke light microscopy and by X-ray diffraction
arkoses, feldspar-quartz and quartz-feldspar analyses of clay minerals. The mineral matter
greywackes with a high content of felsitic within the terrigenous rocks of the South
and quartz porphyries, granites, gneisses and Yakutian Coal Basin has been altered within
rare trachytes (Fig. 5). It is characteristic of the catagenetic and metagenetic stages. The
the greater part of the Middle and Upper terminology of the stages and periods of litho-
Jurassic coal-bearing strata in three regions genesis are those proposed by Vassoevich (1962).
(Figs 6, 7, 8). For example, the Duraji Member The metagenetic stage is seen in highly altered
in the Aldano-Chulman region is represented by Lower Jurassic deposits in the basin (Figs 5 & 7).
feldspar-quartz greywackes (Fig. 9, photo 3,4). In this stage of lithogenesis the blastic structures
 SOUTH YAKUTIAN COAL BASIN 159

and welded joints are widely spaced. X-ray The South Yakutian coals are of high quality
diffraction analyses of clay minerals show that because of their rank and composition. The
kaolinite, dickite, and mica of the 1 Md polytype secondary bitumen macerals are probably
are present. responsible for the high caking index of the
The catagenetic stage affects Middle and coals and their coking properties, as compared
Upper Jurassic and Lower Cretaceous deposits with coals of the same rank from others
in the basin. This stage of lithogenesis is coalfields and basins.
characterized by alteration of allogenic minerals Sandstones in the coal-bearing formation are
and formation of new structures. The catagenetic represented by true arkoses, greywacke arkoses,
stage includes two subzones: the smectite-mica feldspar-quartz and quartz-feldspar greywackes.
subzone and the laumontite subzone. X-ray The mineral matter of terrigenous rocks are
diffraction analyses of clay minerals show that altered to the catagenetic stage and the metage-
the rocks from the smectite-mica subzone contain netic stage. Vitrinite reflectance and mineralogi-
up to 5-15% mixed-layer phase smectite-mica cal parameters were used to evaluate the stages of
and chlorite. X-ray diffraction analyses of the alteration of sediments.
clay nminerals show that in the laumontite
subzone laumontite, chlorite and mixed-layer
phase smectite-mica with packages up to
10-15% are present. Laumontite forms mainly References
in the central parts of pores or substitutes for BREDIHIN, I. S. 1973. South Yakutian (Aldan) Coal
other minerals such as plagioclase, hornblende, Basin. Geology of coalfields and shales of
biotite and pyroxene (Fig. 9). Other authigenic the USSR., Vol. 9, Nedra Publishing, Moscow,
minerals typical of the laumontite subzone are 5-117 (in Russian).
epidote, sphene and quartz. FATKULIN, I. Ya., GEBLER, I. I. & RESHETKO,A. N.
The characteristics of the three regions of the 1970. Statistic correlation between vitribite reflec-
South Yakutian Coal Basin were compared. tance and quality of the coals in the Aldano-
Chulman region. Chemistry of fuels, Vol. 3,
Different parts of the basin demonstrate differ- 141-143 (in Russian).
ent alteration of organic and mineral matter. MARKOVICH, E. M. 1981. Palaeobotanic considerations
Lower Jurassic deposits in the basin are in the of stratigraphy and correlation. South Yakutian
metagenetic stage. In the Usmun region high coal-bearing formation, Leningrad, Nauka Pub-
volatile bituminous coals occur and in the lishing, 33-43 (in Russian).
Aldano-Chulman region there are low volatile MOKR1NSKY,V. V. 1961. Metamorphism of coals in the
bituminous coals. South Yakutia. South Yakutian Coal Basin,
The middle-Upper Jurassic and Lower Creta- Leningrad, Publishing of Academy of Sciences
ceous deposits of the basin are in the catagenetic of the USSR, 382-420 (in Russian).
NAZAROV,V. I. & STUKALOVA,I. E. 1991. Catagenetic
stage. The coals in the A l d a n o - C h u l m a n region
alterations of the Jurassic and Lower Cretaceous
are low volatile bituminous rank and in the deposits in South Yakutia. Geology of the coal-
Tokin region they are high volatile bituminous fields, Ekaterinburg, 100-112 (in Russian).
coals. PRILUTSKY, A. M. 1979. Petrographic composition and
quality of coals in the South Yakutian Coal Basin.
Stratigraphy, paleoenvironment and lithology of
the South Yakutian Coal Basin. Transections,
VSEGEI, Vol. 306, Leningrad, Nauka Publishing,
Conclusions 78 82 (in Russian).
PROSVIRYAKOVA,Z. P. 1961. Palaeobotanic character-
Investigation of the coals in the Usmun,
istics of the coal deposits in the South Yakutia.
Aldano-Chulman and Tokin regions of the South Yakutian coal-bearing formation, Publish-
South Yakutian Coal Basin demonstrate that ing of USSR Academy of Sciences, Vol. XI,
humic coals consist of vitrinite (70-90%), pp. 122 175 (in Russian).
inertinite (10-20%) and liptinite (0-10%) mac- PUTTMANN, W., WOLF, M. & WOLFF-FISCHER, E.
eral groups. There is a high percentage of telinite 1985. Chemical characteristics of liptinite macerals
macerals, up to 60-65%, in the vitrinite maceral in humic and sapropelic coals'. Advances in
group. According to chemical analyses the coals Organic Geochemistry, Vol. 10, 625-632.
contain moisture (W daf) from 0.20% to 2.80%, STACH, E., MACKOWSKY,M. Th., TEICHMULLER,M.,
TAYLOR, G. H., CHANDRA, D. & TEICHMULLER,
volatile matter (V daf) ranging from 17.0% to
R. 1982. Stach's Textbook of Coal Petrology'.
40.0%, ash content (A daf) between 1.57% 3rd edn. Gebruder Borntraeger, Berlin.
to 25.92%, caking index (y) is 6-21 ram. Coals SHUTOV, V. D. 1972. Classification of the terrigenous
are of middle to high rank, with vitrinite rocks and greywackes. Greywackes, Nauka
reflactance values (R0) of 0.65-2.15%. Publishing, Moscow, 9-29 (in Russian).
160 I. E. S T U K A L O V A

TEICHMULLER, M. T. 1974. Generation of petroleum VLASSOV, V. M. 1981. Usmun, Tokin and Gonam
like substances in coal seams as seen under the reg(ons in the South Yakutian Coal Basin. South
microscope. In: TISSOT, B. & BIENNER, F. (eds) Yakutian Coal Formation, Leningrad, Nedra
Advances in Organic Geochemistry, Paris, 321-348. Publishing, 24-32 (in Russian).
- - 1 9 9 0 . The genesis of coal from the viewpoint of WALTZ, I. I. 1961. Petrographic composition and
coal geology. International Journal of Coal Geol- structure of coal seams in South Yakutia. South
ogy, 16, 121-124. Yakutian Coal Basin, Leningrad, Publishing of
TERENTYEV, E. V. 1978. Tectonics of the coalfields of Academy of Sciences of the USSR, 176-277
the USSR. Geology of coalfields and shales of the (in Russian).
USSR, 12, Nedra Publishing, Moscow, 94-162 ZHELINSKY, V. M. 1980. Mesozoic coal-bearing forma-
(in Russian). tion of South Yakutia. Novosibirsk, Nauka Pub-
VASSEOVICH, N. B. 1962. About terminology for the lishing (in Russian).
stages and periods of lithogenesis. Transactions,
VNIGRI, 190, Leningrad, 220-230 (in Russian).
Coal rank variations with depth related to major thrust detachments in
the South Wales coalfield: implications for fluid flow and mineralization
ROD GAYER, RICHARD FOWLER & GARETH DAVIES

Department of Earth Sciences, University of Wales Cardiff, PO Box 914,

Cardiff, CF1 3YE, UK

Abstract: Coal maturity data in the form of volatile matter (daf and dmmf) and random
vitrinite reflectance have been analysed for the South Wales coalfield. They show that in
general coals increase in rank with depth, obeying Hilt's law, and increase in rank laterally
from high volatile bituminous coals in the south and east of the coalfield to anthracite in the
northwest of the coalfield. The lateral increase in rank does not coincide with the basin
depocentre which was located to the southwest of the coal basin during Westphalian times.
The rank pattern with depth in the Westphalian A-Lower Westphalian C Coal Measures of
the eastern half of the coalfield suggests a palaeogeothermal gradient of approx.
310~ -1, equivalent to a basal heatflow of 295mWm -2. Investigation of vitrinite
reflectance in a coal sequence repeated by intense Variscan thrusting indicates that coal rank
was acquired both pre- and syn-thrusting. Detailed analysis of the volatile matter data
reveals the presence of excursions from Hilt's law present in one or more coal seams close to
the boundary between Westphalian A & B. Of the 154 data sets analysed from the coalfield,
94 (61%) show one or more excursion. It is shown that the excursions correlate with thrust
detachments within the coal seams, and it is argued that the excursions represent an increase
in maturity temperature caused by fluids carrying heat into the coal seam along the
seismically active thrusts. The fluids may also have been responsible for the carbonate, oxide
and sulphide mineralization of the coalfield. Preliminary comparisons with the Ruhr coal
basin in Germany suggest that future studies involving computer generated thermal models
are required to understand the thermal evolution of both basins.

The South Wales coalfield represents a major maturity with depth in the coalfield. By con-
Late Carboniferous coal basin developed on the verting maturity indices to temperature, using
Variscan foreland. Mining in the coalfield has the formula devised by Barker & Goldstein
long recognised the presence of coals ranging in (1990), values of palaeo-geothermal gradients
rank from high volatile bituminous coals in the both for specific stratigraphic intervals within
south and east of the coalfield, through inter- the Coal Measures succession and for different
mediate ranks, into anthracite in the northwest localities within the coalfield are derived. It is
of the coalfield. Attempts to explain this rapid argued that the magnitudes and variations of
rank variation, laterally over c. 50km, have these geothermal gradients are difficult to
ranged from those invoking differences in the reconcile with a burial model alone and that
original coal-forming plant communities or the presence of excursions in maturity values
depositional environments (Strahan & Pollard coincident with thrust detachments in the coals
1915; MacKenzie-Taylor 1926; Fuchs 1946), suggests a causal link, possibly associated with
through those resulting from differential burial the flow of hot mineralizing fluids guided by
(Jones 1949; Wellman 1950; White 1991) to thrusts.
those associated with differing heat flows
brought about by magmatic heating (Firth
1971), frictional heating along thrusts (Trotter Regional geology of the
1948, 1950, 1954), differing basement regimes
South Wales coalfield
(Gill et al. 1979), and effects of hot fluids (Davies
& Bloxam 1974; Gayer et al. 1991; Austin & Stratigraphy
Burnett 1994). Most of these have been dis-
cussed in detail by White (1991) and by Austin & The sediments of the South Wales coal basin are
Burnett (1994), but no convincing proof of the preserved in a structurally complex E - W trend-
process producing the rank variation has been ing Variscan synclinorium extending from SW
forthcoming. Dyfed to the western flank of the Usk antiform
This paper presents some additional data on (Fig. 1). The coal basin overlies a southward
the age of rank development relative to Variscan thickening (0-1 km) Lower Carboniferous plat-
thrusting and the presence of variations in form carbonate sequence (Wilson et al. 1987)

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 161-178.
162 R. GAYER ET AL.

+ lI

./71
!

+ / +

/ // +

S
/

§ +\ ,\*
0 km 10
,.;'-CCA v +
\+ + +

Upper Pennant Measures

I 1 LowerPennant Measures ~ Faults

Lower & Middle Coal Measures " ~... Antitorm

i q Pre- and Post-Coal Measures "-4- Synform

Fig. 1. Map of South Wales coalfield, showing major structures and generalized stratigraphy. BTS,
Betws-Tonyrefail Synform; CCA, Cardiff-Cowbridge Antiform; CCD, Careg-Cennen Disturbance; GS, Gelligaer
Synform; LCS, Llantwit-Caerphilly Synform; LLD, Llanon Disturbance; MA, Maesteg Antiform; MGF, Moel
Gilau Fault; ND, Neath Disturbance; PA, Pontypridd Antiform; SVD, Swansea Valley Disturbance; TD,
Trimsaran Disturbance; UA, Usk Antiform; 1, Ffos Las OCCS; 2, Treforgan No. 2 borehole; 3, Treforgan No. 3
borehole; 4, Park Slip OCCS; 5, Ffaldau Colliery; 6, Park Colliery; 7, Ffyndaff OCCS; 8, Maerdy Colliery;
9, Llanharan Colliery; 10, Coedely Colliery; 11, Lewis Merthyr Colliery; 12, Cwm No. 4 shaft; 13, Lady Windsor
Colliery; 14, Merthyr Vale Colliery; 15, Windsor Colliery; 16, Nantgarw Colliery; 17, Penalta Colliery,
18, Brittania Colliery; 19, Bedwas Colliery; 20, Oakdale Colliery; 21, Nine Mile Point Colliery; 22, Celynen North
Colliery; 23, Celynen South Colliery; 24, Blaenserchan No. 2 shaft and Underground Borehole.

that passes conformably downwards into a thick response to a Variscan tectonic load to the south
(3 km) Old Red Sandstone unit and a shallow in SW England. The basin was filled by sediment
marine Lower Palaeozoic succession. Crystalline derived both from the north but mainly from
basement underlies the coal basin at depths the erosion of the tectonic load to the south
ranging from 3.5km in the northwest of the (Kelling 1988, Jones 1989a, Hartley & Warr
main coalfield to over 6 km in the east (Hillier 1990). Throughout Silesian sedimentation the
1989). The Coal Measures sequence is up to basin depocentre was oriented approximately
3.5 km thick in the centre of the basin and ranges E-W (varying from NE-SW to NW-SE) and
in age from basal Namurian to early Stephanian, centred on the Swansea-Gower area (Fig. 2).
covering a time span of some 21 Ma (according Stratigraphical thicknesses decrease markedly
the timescale of Lippolt et al. (1984)). The basin away from the depocentre, particularly to the
was initiated during the early Namurian, follow- east but more gradually to the north and
ing a regional compressional event that resulted west (Hartley 1993). The basin-fill sequence
in the breakup of the Dinantian carbonate coarsens and shallows upwards from marine
platform, relocation of the basin depocentre mudstones and sandstones (Namurian A-lower
and the influx of clastic detritus (Hartley & Warr Westphalian A), through coastal plain coal-
1990). The basin has been interpreted as a Late bearing mudstones and sandstones (upper West-
Carboniferous foreland basin at the northern phalian A-lower Westphalian C) to coarse
margin of the Variscan orogenic belt (Kelling grained sandstones and conglomerates deposited
1988; Gayer & Jones 1989) thought to have in an alluvial braidplain (upper Westphalian C-
been formed by lithospheric downflexure as a Stephanian) (Fig. 3, Jones 1989b, Hartley 1993).
 COALIFICATION EXCURSIONS AND T H R U S T - G U I D E D FLUIDS 163

2,5

a. Shale Gp., Namurian R2-G1

75

b. Upper Westphalian A ~ _ ~ ~ ~

-- _ ..~.~ 10

dlf
120 11 ~ :30

c. Lower Westphalian B ~ ~ _ ~,,,f~-

=1oo

d. Brithdir Beds, Upper Westphalian C

Fig. 2. Isopach maps for four time slices to show depocentrc in south of the coalfield. Contours in metres.
164 R. GAYER E T AL.

< NN Mynyddis lyn 114

Z
< ~.-_-.-_-.-.-.-,
-r Swansea Three F e e t

U.I m

m
Hughes
if? ----.-~
~ -.-.-.-.-.,
Z Brithdir 98
< Captain
i
._1
<
-r
a.

1.1.1
N No2

Upper
Rhondda

Cwmgorse
91

M.B.
....
i
Abergorky 65

Cefn Coed M.B. SCALE (km)

.....
Z Pentre 60 3
<
m n Two Feet Nine 42 Stephanian
n,' Four F e e t 4 0
i S i x F e e t 37 2.5
C a e r a u 36
N i n e F e e t 31
< Bute 30 westphalian
Amman Rider D 2
Z
~-~ M.B.
Yard
i
Z < ~" Seven F e e t 2 6
< m
Five Feet 13 1.5

< Garw I0 wes tphalian

Z
< -r
~_ o
(3 ......~ C 1

Z ~o
ua
~ " Gastrioceras
s u b c r e n a t u m M.B.
Westphalian i
A & B i
sandstone 0.5 [
NaRurian
............ marine band
dominantly mudstone ]
i coal

Fig. 3. Generalized stratigraphical column (not to scale) of the South Wales Coalfield, showing the main
sandstone units in the lower part of the Lower Coal Measures and in the Upper (Pennant) Coal measures, and the
principal coal seams with their seam numbers, as used in the text. The seam numbers follow an unpublished
report by Mr Robin Thewlis, formerly of British Coal Opencast. The inset (lower right) shows the stratigraphical
column to scale.

The majority of the 125 coal seams present in the Structure

coalfield occur in the productive Coal Measures
of late Westphalian A-Westphalian B age. The basin-fill has been affected by Variscan
Although no younger solid formations overlie deformation, the principal elements of which
the Upper Carboniferous Coal Measures, to the are: (i) approx. E - W trending basin-scale north-
south of the coal basin, in the Vale of verging folds; (ii) strike-parallel thrusts (and
Glamorgan, a relatively thin (<300 m) Mesozoic associated lag faults), with southward directed
sequence (Upper Triassic-Lower Jurassic) rests transport along the southern margin of the
unconformably on Variscan deformed Dinan- coalfield, but northwards in the centre and
tian-Namurian rocks. Vitrinite reflectance north of the coalfield; (iii) E N E - W S W trending
values of 0.51%Rm in the Lower Jurassic rocks zones of fold and thrust disturbance, thought to
(Cornford 1986) suggest a possible younger represent reactivated basement Caledonoid
Mesozoic cover subsequently eroded. structures as Variscan thrust ramps (Jones
 COALIFICATION EXCURSIONS AND THRUST-GUIDED FLUIDS 165

1991; Brooks et al. 1994); and (iv) NNW-SSE along coal seams with imbricate thrusts branch-
striking cross faults, commonly showing evi- ing upwards into the hangingwall sequence, or
dence of early strike-slip movement and later as isolated thrust ramps which in some cases are
normal dip-slip movement (Fig. 1, Cole et al. linked downwards to the thrust detachments in
1991). All of these structures have been inter- coal seams (Jones 1991; Hathaway & Gayer
preted as the effects of a northwards propaga- 1994). Thrust detachments commonly occur
tion of Variscan fold and thrust deformation within the coals of the lower part of the
into the coal-bearing foreland basin (Gayer et al. productive Coal Measures, so that at Park Slip
1991). Jones (1989a, b) showed that sedimenta- opencast coal site (OCCS) (Fig. 1), on the
tion throughout the Westphalian was affected by southern margin of the coalfield and at Ffyndaff
incipient development of the main E - W folds in OCCS (Fig. 1), on the northern margin, detach-
the coalfield, demonstrating the close timing ments occur in the Nine Feet group (seams
between basin subsidence and compressive 30-34) and Six Feet group (seams 36-39) of
deformation. seams (Cole et al. 1991; Jones 1991 and Fig. 4).
Of particular relevance to this paper are the At Ffos Las OCCS (Fig. 1) detachments occur in
thrusts, which have been analysed in some the Big (Four Feet seam 40) Kings (Two Feet
detail within the working opencast coal mines Nine seam 42) and Green (Upper Two Feet Nine
(e.g. Gayer et al. 1995). This analysis has shown seam 43) (Frodsham et al. 1993). Where thrust-
that thrusts occur either as major detachments ing has been intense, e.g. at Ffos Las OCCS

(a)

S N
Thrust 1 Bute Seam
Driver Seam ----.-"-- \
Thrust 2 _ ~ Thrust 4
~ # Red S e a m h i ,
Upper 6' Seam f ~ Thrust 3 - - i ~ J 1 ~ __~~---___~"

" Red S e a m " ~ ,~,,v//____~,.

Antithetic
0 100m

(b)

N S
I

/
/
/.

0 m 100
i

Fig. 4. Cross sections through the productive Coal Measures to show the style of thrust structure in the South
Wales coalfield. (a) Section drawn parallel to the thrust transport direction through Ffyndaff OCCS, based on coal
extraction sections. Note the thrust detachments through the Nine feet seam (seam 31) and Red seam
(seam 36). Modified from Gayer et al. (1994). (b) Section drawn from British Coal borehole data through Park Slip
West OCCS, showing thrust detachments at the level of the Six Feet seam (seam 37). See Fig. 1 for site locations.
166 R. GAYER E T AL.

in the northwest of the coalfield, with thrust during thrusting, as the coal seams matured by
shortening estimated at 70% (Cole et al. 1991), it compaction and dewatering (Gayer et al. 1991;
has been demonstrated that detachments within Gayer 1993).
several coal seams have moved simultaneously
producing a style of deformation that appears to
be unique to coal-bearing sequences. This has Metamorph&m
been termed Progressive Easy Slip Thrusting
(PEST) by Frodsham et al. (1993), and The sediments of the coalfield have been affected
explained in terms of fluid overpressuring by very low grade metamorphism within the

~ ~ . , ~ ~ ~ 23 27

a. No.2 RhonddaSeam ~ ' ~ ~ C__~

7 1 1

31

b. Fou

i ~ . , ~ ~ 19 ,,~ 23
27

1 11 15

31

Fig. 5. Maps of coal rank (%Vm) for the South Wales coalfield, after White (1991). (a) Five feet seam (Lower
Coal Measures); (b) Four Feet seam (Middle Coal Measures); (c) Rhondda No 2 seam (Upper Coal Measures).
Note the location of the anthracite area (less than 9% Vm) in the northwest of the coalfield and compare with the
Coal Measure isopach maps (Fig. 2).
 COALIFICATION EXCURSIONS AND THRUST-GUIDED FLUIDS 167

diagenetic grades of metamorphism, based on coalfield structure; in particular she showed that
illite crystallinity characteristics (White 1991). the coal isovols were folded by the coalfield
The metamorphism ranges into the lower synform and also by the Pontypridd antiform.
anchizone facies in the extreme northwest of The isovols do not however parallel stratigra-
the coalfield, based on the presence of pyro- phical boundaries precisely, cutting gently down
phyllite (Bevins et al. 1996). Coal rank, based on stratigraphy to the southeast. This may reflect
volatile matter contents (%Vm dmmf) and the thinner stratigraphy in this direction causing
vitrinite reflectance (%Rm) , increases from high a particular horizon to be less deeply buried and
volatile bituminous coal in the south and east of therefore of lower rank in the thinner succession
the coalfield to anthracite in the northwest of the in the southeast. It might also reflect a syn-
coalfield (Fig. 5, White 1991), coinciding with deformational age for rank development with
the illite crystallinity metamorphic pattern. the rocks on the southern flank of the coalfield
White (1991) demonstrated that the coal isovols being uptilted before the imposition of rank. To
(lines of equal volatile matter) are parallel to test the possibility of syn-deformational rank
stratigraphical boundaries around major fold development and specifically to determine the
structures in the coalfield, suggesting a pre- timing of rank formation relative to thrusting, a
Variscan folding origin for the coal rank study of the vitrinite reflectance of coals
development. The rapid lateral increase in coal repeated by several thrusts in the Ffos Las
rank has been discussed in detail by White OCCS has been undertaken.
(1991) and by Austin & Burnett (1994), who The structural geology in the Ffos Las OCCS
suggested that burial beneath a now eroded has recently been described by Frodsham et al.
sedimentary load (White 1992) or inflow of hot (1993). The site lies across the Llanon and
fluids either from the Variscan mountain belt to Trimsaron disturbances which are represented
the south (Gayer et al. 1991) or along deeply by four major north directed thrusts each with
penetrating faults in the underlying basement displacements greater than 100m, and many
(Austin & Burnett 1994) are the mechanisms in meso- and minor-scale thrusts (Fig. 6). The
most agreement with the observations. combined throw of the thrust-related structure is
1175 m and thrust shortening has been estimated
as 70%. Coal samples were collected from the
Local coal rank development and its Big (seam 40), Kings (seam 42), Green (seam 43)
relationship to thrusting and Graigog (seam 44) coal seams in the
different thrust sheets exposed by the opencast
White (1991), working on a coalfield scale, workings at the time of the study. The results of
showed that the coal rank in the coalfield was the vitrinite reflectance analyses are shown in
developed before the formation of the major Fig. 7 where Rm has been plotted against the

N Llannon Trimsaran S
Disturbance Disurbance

.... 7- _ _ : : " ) .

"~-~ ~ ~..-~ ~ . "--.. - - . . -~

Key: "" ~
100 metre
Graigog Rider, Graigog, Green and Kings seams
Big Seam
......... Other clastic rocks
Superficial deposits
Thrusts

Fig. 6. Cross-section of structure at Ffos Las OCCS based on borehole data (after Frodsham et al. 1993).
168 R. GAYER E T AL.

9, ~ .w.,+
,,.-,

I i I F ~,..:u
" ++ ' I -+| ~++
+I + ' I
, ++_ . _ ~
,,r:::::J o.,
rj I-,

, ~N, ~~ ~_-~ IW
..--.. 0

t-+

m..
ol
j ....-- ..---""--+ ' ' - I(
k+
#....~----

+ +~ooo++++o+o++++
-
++++++++++ " "+++++++
++++- +++++++---.
"
+.m ++++++++ ++-"++ o> 2'= o
+::I

<I,ll
q::I

..,_+

= l ,+... o

.~ u,,.B

+~L.+ "m--; <,.,

Ak

uO
r ~ ._...._ ~ ,_..-~ " - ' ~
\
i I
f J J
'.'- '" +~ mm ' " < :~ ''' ''' ''' ''' ''' '" b r', c~ o 0 (O b C) 0 ~ C)
m+ -+u(..+u++++++++
. . . . . . _.+_+++ +++ ~ + + (..+
m 0 (.b (.b (.b 0 0 9 s~ sz
0
9+ ~ c.)
 COALIFICATION EXCURSIONS AND THRUST-GUIDED FLUIDS 169

coal seams arranged (a) stratigraphically and The palaeogeotherm of 310 ~ km-1 is
(b) tectonically, in ascending thrust sheets. There approximately four times that of 50-
is no clear decrease in Rm with increased 75~ -l determined by Alderton & Bevins
stratigraphical height, suggesting that the rank (1996) from fluid inclusions within quartz
was not developed pre-thrusting, but there is no crystals grown in an ironstone nodule within
clear decrease in R m with higher tectonic the Middle Coal Measures in the central eastern
position suggesting that the rank was not part of the coalfield. Alderton & Bevins (1996)
developed post-thrusting (Fig. 7). There is a assumed a constant geothermal gradient
general decline in Rm upwards with stratigraphy between the sample position and the palaeo-
in each thrust sheet but with anomalous values surface. However, our plots of temperature
in the vicinity of thrusts. The R m pattern at against depth suggest that the geothermal
Ffos Las OCCS is therefore complex and can gradient was much higher within the mud and
only be explained if the vitrinite reflectance was coal dominated succession of the Middle Coal
developed both before and during thrusting. Measures and became appreciably less within
the sand dominated Upper Coal Measures.
Although there are insufficient vitrinite reflec-
Variations in coal rank with depth tance data from the northwest of the coalfield to
produce similar plots against depth, the higher
Establishment of the local temperatures required for the generation of
palaeogeothermal gradient anthracite with Rm values of up to 4% (327~
within an only marginally thicker Middle Coal
White (1991) demonstrated that the volatile Measures sequence suggest even higher geother-
matter (Vm dmmf) decreases constantly with mal gradients may have operated during the
depth across the coalfield, and therefore sug- rank development in this part of the coalfield.
gested that a constant geothermal gradient
operated during coalification, without specifying
a value for this gradient.
Barker & Goldstein (1990) have developed an Excursions from Hilt's law in the
empirical equation relating R m to temperature:
South Wales Coal Measures
T(~ = [(In Rm) + 1.26]/0.0081.
The detailed variation of rank (and therefore
This relationship can be used to reconstruct the temperature) with depth can be studied using the
local palaeogeothermal gradient in the South coal rank determinations from collieries, shafts
Wales coalfield. Values of vitrinite reflectance and boreholes throughout the coalfield. The vast
(Rm) from 12 collieries in the east of the coalfield majority of recorded coal maturity data for the
(Fig. 1) have been plotted against the local depth coalfield is in the form of volatile matter (dmmf
below seam 91, as recorded in the Btaenserchan or daf). This was the standard proximate
borehole (Fig. 8a). Figure 8b shows Vm (dmmf) analysis carried out by the former British Coal
from the same collieries and the same seams Corporation and, their predecessors, the
plotted against local depths beneath seam 91. National Coal Board. Within the last ten years
The two plots show very similar, but reversed vitrinite reflectance measurements were also
linear trends which suggests a linear increase in occasionally recorded, but these represent only
rank with depth. a small fraction of the total data set. Since
Using Barker & Goldstein's (1990) relation- almost all the mines are now closed and
ship, the variation in temperature with depth relatively few coal samples are available, it is
below seam 91 is plotted in Fig. 8c which gives a not possible to carry out new vitrinite reflectance
reconstructed palaeogeothermal gradient for analyses. Thus volatile matter content rather
the eastern part of the coalfield of approx. than vitrinite reflectance has been used for the
310~ -1. However, these plots are based on analyses. The plots of Fig. 8a & b suggest a close
the assumption that seam 91, close to the inverse relationship between Vm (dmmf) and
top of the Coal Measures, was isothermal, Rm, which has been extensively analysed by
(i.e. reached the same maximum temperature, McCartney & Teichmialler (1972), Bartenstein &
and thus the same values of R m and Vm) across Teichmiiller (1974), and Teichmfiller & Teich-
the relevant area of the coalfield. In fact Vm for mfiller (1982). Using the Barker & Goldstein
seam 91 varies from 28% to 33%, an estimated (1990) equation, it has been possible to relate
temperature difference of 18~ which is a likely both to temperature (Fig. 8c).
explanation for the scatter of data points in The data used were collated from British Coal
the plots. archives (White 1992) and from the Coal Survey
 >

9r
9 ///r
/-"
9 /
/-
/
/
/
J e~
/
/
>
./
/

o ./

g ~ g

(w) '16 m ~ ~o|oqqldoG

04,

>

@ 9

~m

(tu) 'I 6 ure~ ~OlOq 41d~G

~o

(m) 'I6 u*~s ,~opq 41d~(l

 COALIFICATION EXCURSIONS AND THRUST-GUIDED FLUIDS 171

Seam Records of the National Coal Board. Data structure (Woodland & Evans 1964). Thrust
sets were collected from 154 collieries, shafts and detachments commonly occur in seams 30-43,
boreholes in which Vm values from five or more with the greatest incidence in the Nine Feet
seams were available. For these localities Vm group (seams 30-34) and the Six Feet group
values were plotted against depth. In general a (seams 36-39) in the east of the coalfield and in
regular decrease in Vm occurs with increasing seam 40 in the west of the coalfield. At
depth, indicating an increase in rank with depth Llanharan colliery, in the hangingwall of the
and that Hilt's law is obeyed. However, 94 data major Llanharan thrust (Woodland & Evans
sets show an excursion from Hilt's law. Figure 9 1964), two excursions from Hilt's law are
shows 12 plots of variations of Vm (dmmf) with recorded in the Vm (daf) data at the level of
depth (after White 1992), representing the range seams 37 and 27. These are both associated with
of data available from locations across the coal- in-seam thrust detachments revealed by rash-
field. Three main types of pattern can be seen: ings, which also occur within or adjacent to
(i) Vm decreases regularly with depth through- coals 40, 36, 32, 30 and 13 (Fig. lla). In the New
out, with no excursion (e.g. Treforgan No. ! Shaft at Park colliery, rashings occur associated
borehole & Lady Windsor colliery); (ii) a single with coals between seams 31 and 36 with a Vm
excursion occurs to lower Vm content, shown by (dmmf) excursion present at seam 36. The
one or more seams (e.g. Cwm colliery); and Cockshot Rock, a persistent fluvial sandstone,
(iii) two or more excursions to lower Vm content lies 45m beneath the excursion at seam 36
occur (e.g. Coedely colliery). The excursion in (Fig. 11b) In this latter case, the absence of Vm
Vm is mirrored by similar excursions in the values for the seams between 31 & 36, in which
volatile elements Sulphur and Phosphorous the rashings are present and immediately
(Fig. 10). Where an excursion occurs the regular beneath which the permeable Cockshot rock
pattern of decreasing Vm with depth is per- occurs, means that the precise location and
turbed, with an increase in Vm occurring with extent of the excursion cannot be determined
depth above the excursion (e.g. Nantgarw col- precisely.
liery). The geothermal gradient, calculated by
converting %Vm to %Rm, using the graphs
in Stach et al. (1982), and thence to tempera- Discussion
ture, using the Barker & Goldstein (1990)
equation, is also highly variable with values Palaeogeothermal gradients and heat flow in
ranging from 8-15~ -~ at Nantgarw col- the South Wales coalfield
liery to 133-193~ k m -1 at nearby Cwm colliery
(Fig. 9). One of the outstanding problems of the South
The excursions from Hilt's law most com- Wales coal basin is the explanation for the major
monly occur centred on seam 37 (48% of lateral rank variation, with seams at the base of
excursions) but ranges from seam 80 (< 1%) to the Coal Measures varying from a Rm of 1.0%
seam 13 (2%). The excursion is thus not seam in the southeast of the coalfield to 4.0% in the
specific and hence is unlikely to be related to the northwest of the coalfield (White 1991). This
original coal composition. There does, however, represents a variation of maximum maturity
appear to be a strong correlation between the temperature from approx. 150~ in the south-
stratigraphical level of the excursion and the east to 325~ in the northwest. It is difficult to
presence of thrusting within the seam. Although explain this variation by burial depths alone,
it is difficult to obtain information on the since the depocentre for the preserved Coal
presence of in-seam thrusting from the aban- Measures succession lies to the south of the area
doned mine records, they can be directly of highest rank (compare Figs 2 & 5). It would
observed in the working opencast coal mines. require a considerable thickness of younger
Here thrust detachments in coal seams com- sediments deposited before the onset of Variscan
monly produce a pervasive, oblique, sigmoidally deformation to develop the required burial
shaped fabric that has been described as a temperatures (e.g. White 1992). Any such
cleavage duplex (Frodsham et al. 1993; Gayer sediments have since been completely eroded.
!993). The detachments also develop true Calculation of the required burial depth to
duplexes with roof thrusts immediately above produce the maximum maturity temperatures in
the seam roof and floor thrusts in the seat earth the northwest of the coalfield is not simple as it
below the seam. The duplexes interleave seat depends on a number of undefined variables that
earth and carbonaceous roof rock into the seam include the magnitude of the palaeo-heat flow
and can be recognised in boreholes and shafts as during the Late Carboniferous, and the thermal
'rashings', a miners' term for this type of conductivity of the now-eroded sedimentary
(a)
-250 Nhte MilePeat
Manly 4237~40 -150
,,~ -200 ~ 91
36 ~ 3 1
~-~ -300 ~ "250
t 4 ~ _ - 3 0 0 31 "-e-A"2
-350 1- --13#r26
-351) f I I -400 ! I I I I I
9 10 11 12 28 28.5 29 29.5 30 30.5
Volatile% dmmf Volatile% dmmf

-450 Lady WhMsor Ffaidaa

-100
-5oo[ -150
~ -550
-600
~
13.1/~/ 26 --
40

~ -200
-250 26~,,,,,/30
37

-650 -300 13~ ,

12 13 14 15 16 17 19 21 23
Volatile% dmmf Volatile% dmmf
Merthyr Vale Lewis Merthyr
-400
-420t 37~ -300 40----"-'-'-~"~31
~ 3 0
-350 t 306 ~
-460
-480 26 13
-500 I -450 I I I t I
12 12.5 13 13.5 16 16.5 17 17.5 18 18.5 19
Volatile% dmmf Volatile% dmmf

(b)

Treforl~m2 Treforf,~ 1
-200
-250
-230 t 3 6 ~
"~ -270
40
"~-25o ~ 3 / _ _ ~ 6 37
-310 ~-300 ~ 31
-330
-350 9 t t t t - -350 ~ I t I
4 4.5 5 5.5 6 6.5 7 5.7 5.8 5.9 6 6.1 6.2 6.3
Volatile% dmmf Volatile% dmmf
][~dwm Cwm 4
-550

~ -600"550
I 91~4
-650
-650
-700
-750 13 26
37
2
31
~ -700 37 36

400 C- t ]" i t i -850 t t P

26 26.5 27 27.5 28 28.5 29 23 25 27 29
Volatile% dmmf Volatile% dmmf
Naatgarw Coedely
-250

65
-300i

-700 42 -511t) 3 3 7 ~ 31
37 , -

D 30 W"
..-..----"~31
t t -650 t I
-800
28 29 30 31 32 20 25 30
Volatile% dmmf Volatile% dmmf
 COALIFICATION EXCURSIONS AND THRUST-GUIDED FLUIDS 173

cover. Whatever values might finally be reached produce higher than normal values immediately
for these variables and the thickness of the along and above the conduit, and higher than
cover, it would be necessary for the palaeo- normal thermal gradients in the overlying
geothermal gradient imposed by the model to sequence. Below the conduit temperatures
match the palaeogeothermal gradients mea- would have reverted to values associated with
sured in the various preserved stratigraphical the normal heat flow in a normal thermal
successions. gradient. Conodont CAI values for the Dinan-
The geothermal gradient indicated in this tian limestones beneath the foreland basin show
study of 310~ -1 for the preserved Lower broadly equivalent thermal conditions as for the
and Middle Coal Measures in the eastern half of overlying Coal Measures, but with one major
the South Wales coalfield, and the assumed even exception. This is in the southwest of the basin
higher gradient in the anthracite zone to the in the Swansea and Gower Peninsular area,
northwest imply high levels of heat flow, as where very high values of CAI have been
indicated by the following calculation: recorded (Austin & Burnett 1994) in an area
where the overlying Coal Measures show their
heat flow (m Wm -2)
lowest values of maturity. It is also broadly the
= geothermal gradient (~ km-1) site of the foreland basin depocentre (cf. Fig. 2).
The origin of this relationship is unclear, but it
x thermal conductivity (Wm -1 ~ -l) seems unlikely to have developed from normal
Thus, with an average thermal conductivity of burial maturation and may imply the passage of
Coal Measures of 0.9Wm -l ~ -l, a palaeo- fluids through the Dinantian limestones.
geothermal gradient of 310~ km -a implies that The correlation of excursions with in-seam
the South Wales Late Carboniferous heat flow thrust detachments suggests that the thrusts
was 295 m Wm -2. were fluid pathways. Evidence from the Car-
This level of heat flow is comparable with ibbean accretionary prism indicates that fluids
values associated with oceanic spreading ridges are expelled along the basal thrust detachment
(Sclater et al. 1980) and is completely unrealistic of the accretionary wedge (Bangs et al. 1990).
for continental foreland basins. Preliminary Similarly, thrust detachments associated with
attempts to model the situation in the South the destructive continental margin west of
Wales coalfield using the commercial basin Vancouver Island channel fluids and produce
maturity computer software package BasinMod abnormal heat flows (Westbrook et al. 1993). In
(Platte Rivers Associates 1996) suggest that such recent years there has been a growing recogni-
gradients are unlikely to have been generated by tion that thrusts are able to guide fluids into
burial alone, and it seems likely that the normal sedimentary basins (Lawrence & Cornford
continental foreland basal heatflow was 1995), and indeed the seismic action of the
enhanced by heat carried into the basin by thrusts may well have increased the rate of fluid
transient hydrothermal fluid flow. flow by seismic pumping (Sibson 1994). In the
case of the thrusts within the South Wales
coalfield it is clear that the strains associated
with thrust deformation has produced exten-
sional and contractional fracture systems that
Role of fluids in the South Wales coalfield
have allowed the volume surrounding the thrust
The recognition of excursions from Hilt's law in to become permeable and thus to allow fluid
the Lower and Middle Coal Measures of the ingress (Hathaway & Gayer 1996).
South Wales coalfield provides strong evidence
for localised increase in temperature at specific
stratigraphical levels. This is precisely the form Mineralization in the South Wales coalfield
of thermal depth profile to be expected where
heat has been transferred laterally into the basin The fracture systems in the coals of the South
along a permeable conduit (Duddy et al. 1994). Wales coalfield are extensively mineralized and
The temperature would have been raised to more than 50 different mineral species have so far

Fig. 9. Plots ofVm% (dmmf) against depth for 12 sites in the South Wales coalfield, located in Fig. 1 to show the
three main types of variation. See text for explanation. Calculated palaeogeothermal gradients between specific
seams are shown for seven data sets as follows: Coedely, 117-140~ -l (seams 91-13); Cwm 4, 133-
193~ km -l (seams 42-13); Nantgarw, 008-016~ km -1 (seams 91-31); Bedwas, 035-053~ km -1 (seams 91-13);
Mardy, 056-079~ km -1 (seams 42-13); Lady Windsor, 056~ km-1 (seams 40-13); Faldau, t33-164~ -1
(seams 42-13).
174 R. GAYER E T A L .

a)Volatile M a t t e r

-200

-250 91

-300

-350 8O

-400 65

4 6O
-450

-500
. _ 36

-550

-600

-650 I t
20 22 24 26 28 30 32 34
Volatile % d m m f

b)Phosphorous and Sulphur

-200

-250
91 ___...--4

-300

-350

-400

J
-450

-500 42 4o
37

-550

9 26 9
-600

-650 ! -- ,,, I
0 0.5 1 1.5 2 2.5 3 3.5 4
% Element

Fig. 10. Vm, sulphur and phosphorous variations with depth at Coedely colliery (located in Fig. 1). (a) Vm%
(dmmf), lines represent +1 standard deviation from the mean, and show two excursions from Hilt's Law.
(b) Variations in S (squares) and P (circles) showing similar excursions to those in (a).

been identified (Gayer & Rickard 1994). These also been discovered in the coal cleat system in
include an early carbonate and oxide phase some coals, associated with the late stage of the
consisting of Ca, Mg, Fe and Mn carbonates, earlier mineral paragenesis (Gayer & Rickard
Ba and Ca sulphates, clays (kaolinite, various 1994). It has been argued by Gayer et al. 1991
illites and mixed layer clays), and quartz, that this mineralization was a result of fluid
followed by a base metal sulphide and selenide movements along thrusts carrying exotic ions
phase consisting of Fe, Co, Ni, Cu, Zn, Mo, Cd into the basin and leaching elements from the
and lead sulphides and clausthalite. Gold has compacting sediments.
(a) Lianharan Colliery

-50

-100
Oe 37 repeat

-150 Llanharan Thrust

,.-.,
g -200

-250
42
-300 37 - 4~_0 it A36
3 1 G ~ O/~ Red
-350 30 A Amman
Yard. ~ 26
-400 13 = ~.

-450 ! t , I i :

32 33 34 35 36 37 38
Volatile % daf

(b) Park

42

-300
4O

37

-400

26

-50C t t I
12 13 14 15 16
Volatile % dmmf

Fig. 11. Plot of Vm against depth to show relationship between excursions from Hilt's law and in-seam thrust
detachments revealed by rashings bands, and the C o c k s h o t Rock sandstone; (a) L l a n h a r a n colliery, lines
represent +1 standard deviation from the mean; (b) Park colliery (located in Fig. 1).
176 R. GAYER ET AL.

Comparison with the Ruhr coal basin 3. The geothermal gradient within the Lower
and Middle Coal Measures of the eastern part of
It is interesting to compare the situation in the the coalfield is 310~ -1 and is presumed to
South Wales coal basin with that in the Ruhr be higher in the northwest of the coalfield.
coal basin, another coal-bearing foreland basin Preliminary thermal modelling of the basin
along the northern Variscan margin (Gayer et al. suggests that burial alone cannot be responsible
1993). Computer generated thermal models for for this gradient which would require Late
11 localities in the Ruhr coal basin of Germany Carboniferous basal heat flow values of
have suggested that the Ruhr Coal Measures 295 m Wm -2.
were buried beneath an additional 2.2-3.5 km of 4. Excursions from Hilt's law occur in locally
younger Carboniferous sediments that were developed zones associated with one or more
completely eroded before the deposition of the coal seams, and most commonly with seam 37
Mesozoic cover (Littke et al. 1994). In order to near the base of the Middle Coal Measures.
achieve a match between calculated and observed These excursions are observed in plots of volatile
geothermal gradients the Late Carboniferous matter variations with depth and are interpreted
heat flow was calculated to have been between 64 as localised zones of higher temperature. Ther-
and 83 m Wm -2, very high values for downflexed mal gradients associated with the excursions
continental crust in an orogenic foreland which vary from 8~ -1 to 193~ -I
in modern situations have low heat flow values 5. The excursions are correlated with in-seam
with average geothermal gradients of 22~ km -1 thrust detachments, seen as cleavage duplexes
to 24~ -l (Allen & Allen 1990). In the Ruhr and thrust duplexes in working opencast coal
coal basin the modelled average palaeogeo- mines and as rashings in the colliery records.
thermal gradient was between 36-47~ -~ 6. It is argued that fluids, associated with
but the observed gradient in the preserved Coal seismic activity along the thrusts, have carried
Measures succession is 63-65~ km -1, reflecting heat into the coal seams, causing a local increase
the lower thermal conductivity of the Coal in the heat flow and a resultant perturbation of
Measures (and the assumed higher thermal the thermal gradient. The fluids have also
conductivity of the now eroded cover). introduced minerals into the coals.
The above suggests that the Ruhr basin 7. Comparisons with the Ruhr coal basin
experienced high Carboniferous values of heat imply possible similarities as well as differences
flow and a thick Late Carboniferous cover, between the two basins. It is suggested that
subsequently eroded. This is in contrast to the thermal modelling of both basins may provide
South Wales basin where locally high heat flow the solution to an understanding of the thermal
values appear to be related to fluid inflow along histories of the Variscan foreland basins.
thrusts. In the Ruhr basin there is little evidence
for in-seam thrust detachments; the thrusts are The maturity data collated for this study were made
commonly ramps and are intimately associated available by the former British Coal Corporation. We
with the folds (Kunz & Wrede 1985). However, as are extremely grateful to British Coal Opencast and to
in South Wales, the coal rank was developed at Celtic Energy for allowing access to opencast coal
mines in South Wales and for providing plans and
the time of deformation. Excursions from Hilt's
sections from which the thrust structure within the
law have also been observed in the volatile matter South Wales coalfield has been deduced. The final
data, although it is unclear how these have been version of the manuscript has been greatly improved
interpreted Ouch 1991). It seems at least possible by suggestions made by Ron Austin and Chris
that fluid inflow has had some role in the develop- Cornford.
ment of the Ruhr basin. Computer generated
thermal modelling involving possible transport
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 Deep borehole evidence for a southward extension of the Early
Namurian deposits near N6m~i~ky, S. Moravia, Czech Republic:
implication for rapid coalification

J. D V O I ~ A K l, J. H O N I ~ K 2, J. P E S E K 3 & P. V A L T E R O V A 4

1 Czech Geological Survey, Leitnerova 22, 658 69 Brno, Czech Republic

2 Hongk Co. Ltd, Opavsk[t 4150/9, 70800 Ostrava 4-Pustkovec, Czech Republic
3 Faculty of Science, Charles University, Albertov 6, 12843 Praha 2, Czech Republic
4 Geofond, Kostelni 26, 170 O0 Praha 7, Czech Republic
Abstract: Unexpected Early Namurian (Namurian A) sediments were identified in several
boreholes in the vicinity of N6m6i~ky (the N6m6i~ky basin), south Moravia. Coal fragments
were recovered from the boreholes N6m 1, 2, 5 and 6. These fragments come partly from
in situ coal seams, partly from eroded coal seams and partly from coalified logs. Although
these fragments were recovered from depths of 2690.9 m (N~m 5) to 4803 m (N~m 1), their
mean reflectance (R0) is 0.57% up to 0.9% which corresponds to subbituminous to high
volatile bituminous coal. The very low rank of the coal at these depths argues for very fast
coalification of the coal fragments most likely during the Carboniferous. The rank of the
coal is believed not to have been affected by later burial beneath Jurassic sediments or by
tectonic burial under Carpathian nappes.

The presence of Early Namurian (Namurian A) natural gas in the vicinity of N6m~i6ky, SE of
sediments has been proved below the Car- Brno (Fig. 1). In addition to rocks, some of
pathian Flysch nappes at relatively great which strongly resemble sediments of the Czech
depths in several boreholes drilled by Moravsk6 part of the Upper Silesian coal basin, fragments
naftov~ doly Co. during exploration for oil and of isochronous coal were also identified. The

POLAND

..s

Fig. 1. Schematic geological map of Moravia-Silesian Devonian and Carboniferous. 1, unfolded rocks on the
platform; 2, volcano-sedimentary formations on the surface; 3, basinal formations below the flysch; 4, carbonate
formations on the surface or below the flysch and molasse; 5, Upper Silesian basin; 6, borehole Jablfinka 1.

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geologyand Technology,
Geological Society Special Publication No. 125, pp. 179-193.
180 J. DVOI~.AK E T A L .

Age Formation Member

Westphalian A Doubrava

Such~i Hubert fresh water group

of bands

Karvinfi

Saddle

Poruba Gaebler group of marine

bands

Jaklovec Barbora group of marine

bands

Namurian Ostrava Enna group of marine

bands
Hrugov
Frantigka group of marine
bands

Pet~kovice Main whetstone

horizon

1)hiatus

Fig. 2. Lithostratigraphical scheme of the Upper Silesian basin (A) and proved age of sediment filling of the
N6m6i6ky basin (B).

first record of fragments of Carboniferous coal coalified logs. The total length of the analyzed
found in drilling mud was that of the N6m 1 borehole section was from 4250 m up to 4535 m.
borehole (Reh/tk 1975). However, no systematic Palynological studies suggest a Carboniferous
coring of the boreholes was undertaken because age of the examined coal (Knobl-Jachowicz in
the programme was aimed at testing the oil I~eh~k et al. 1973).
and gas potential in the area. The discovery Another Carboniferous coal was found in the
of coal bearing Carboniferous strata was com- N6m 2 borehole. A bituminous coal seam,
pletely unexpected at such depths. The samples 1700mm thick, was penetrated by the borehole
obtained from the drilling mud were subjected to at a depth of 3374.30 to 3376m. Numerous coal
technological tests and petrological investigation fragments were also found in drilling mud in
despite some uncertainty about the true number addition to the above mentioned coal seam. The
of coal seams penetrated during the drilling. It is great thickness of the coal seam was the main
also possible that some fragments have come reason for detailed investigation of both the
from eroded and redeposited coal seams or from coal and adjacent sediments which were found
 EARLY NAMURIAN COAL-BEARING DEPOSITS, CZECH REPUBLIC 181

in the N~m 1 and 2 boreholes (Hon~k et al. deposition of dark, partly dolomitic, limestones
1978, Hon~k-Vrbovfi 1980, Hon6k et al. 1980, of the La~finky Limestones which grade into
Polick)-Fialovfi 1980) and in other boreholes light grey very pure Vil6movice Limestones.
(see below). Phytopalaeontological studies Both types of limestones belong to the Macocha
proved the Late Carboniferous age of these Formation which is of Givetian-lowermost
sediments (Early Namurian) which appear to be Fammenian age (Fig. 5). This formation is
the same age as the Ostrava Formation in the characterized by reef-building coral- and stro-
Upper Silesian basin. Specifically they appear matoporoid faunas. The thickness of this
isochronous with the upper part of the Ostrava formation is about 800 m in the west, gradually
Formation, commencing with the Enna marine thinning to 480 m in the east.
horizon and including the Jaklovec and Poruba A major regression occurred at about the
members (Purkyfiovfi 1978a, b). Palynological Middle Fammenian, following which the Vil6-
studies by Valterovfi (1978, 1982) also proved movice Limestones were karstified. Dark bio-
the Carboniferous age of the unit (Fig. 2). Later detrital Hfidy-l~i~ka Limestones, locally with
finds of coal fragments from the N6m 5 and 6 corals and brachiopods (Gigantoproductus) were
boreholes were studied to a lesser extent. deposited after a second marine trans-gression
No gamma-gamma logging was undertaken which occurred in the Late Vis6an. These
in the boreholes for technical reasons. Conse- limestones are about 120 to 130 m thick in the
quently, the true number of coal seams pene- west (N~m 2 and 5 boreholes) but thin out to
trated during the drilling remains unclear. The the east.
source of some coal fragments is also question- The Hfidy-l~i6ka Limestones are transitional
able. Despite this uncertainty, the results indi- toward the top into dark, locally calcareous silty
cate the extension of the Upper Silesian coal shales, which represent here the Myslejovice
basin into the area beneath the Carpathian Formation. The shales which were penetrated by
Flysch nappes and have important implications N6m 5, N6m 2 and N6m 1 boreholes were 23, 47
for the timing and process of coalification. and 38 m thick respectively.
The onset of coarse-grained sedimentation
which outpaced the basin subsidence occurred at
the boundary between the Early and Late
Geology of the N~m~i~ky area Carboniferous. A large body of coarse-grained
petromict (polymict) conglomerates about 500 m
The region under consideration belongs to the thick was deposited along the western margin of
M~nin block (cf. Dvof'fik 1993) which is the the rapidly subsiding eastern sub-block which is
southernmost part of the Paleozoic Drahanskfi only 150 thick in the N6m 2 borehole. These
Vrchovina Plateau, located south of the city of conglomerates are completely missing in the
Brno. The basement beneath its sediments N6m 1 borehole.
consists of the Precambrian Brno-granitoid The Early Namurian is represented by a cyclic
massif. Two sub-blocks (Fig. 3) were distin- series in which grey to black-grey sandstones,
guished in the area: the western sub-block locally with numerous fragments of fossil flora,
consists of the Basal Clastic Formation of Old are the dominant sediments. The N~m 1 bore-
Red facies resting on the granodiorites. This hole penetrated the following rock sequence
formation is more than 1400m thick and likely from the bottom to the top: greywacke sand-
Early Devonian in age. It is overlain by stone about 80m thick; pink arkoses about
relatively thin (400m) reef limestones (Middle 160m thick, and finally feldspathic sandstones
Devonian and Frasnian). more than 250 m thick which represent the last
The eastern sub-block has suffered greater member of the whole sequence terminating the
subsidence. The sedimentation also starts with sedimentation. Intercalations of black-grey silt-
terrestrial red-purple arkoses of the Old Red stones and shales and also coal seams, confined
facies, with unknown thickness. These were to the upper part of the sequence, are much less
deposited on weathered granitoids of the Pre- abundant. Intercalations consisting of tuffites,
cambrian Brno massif. The boundary between often mixed in sandstones, represent a typical
the sub-blocks is formed by a N-S trending fault constituent of this sequence. The N~m 5 bore-
which was penetrated by the N~m 5 borehole hole revealed also a layer of coarse-grained
(see Figs 3 & 4). conglomerates about 200m thick which must
The marine transgression recorded in the thin out towards the N6m 1 borehole. The
eastern sub-block reached this area at approxi- preserved thickness of the whole sequence
mately the boundary between the Eifelian and reaches 1100 m thick in the west. It is reduced
Givetian. The transgression was followed by to 600 m toward the N~m 1 borehole some 5 km
 182 J. DVOI~.,~K E T AL.

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184 J. DVO15,AK ET AL.

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upper 1
t Formation
............ _.........-"'5'~oJ
--''~'' 7 , o f"~//
I
I

Macocha Formation

Fig. 5. Lithostratigraphical scheme of the Devonian and Early Carboniferous of the Drahany Upland. O, Ostrov
Shales; B, Brezima Formation; K, Krtiny Limestones; D, Drazovice Formation.

ESE in which the thickness of Carboniferous The age of coal bearing sediments and
sediments is believed to be doubled due to an coal fragments
overthrust fault.
The Ostrava Formation in the vicinity of the Palynological and coal petrological investigations
N6m~i6ky boreholes forms the southernmost of coal fragments from the N6m 1 and 2 boreholes
and the youngest known alluvial fan belonging show clearly that these fragments are of Carbo-
to the Moravian Paleozoic (Dvo~fik 1995). niferous age (cf. Knobl-Jachowicz in I~,ehfik et al.
1973; l~ehfik 1975; Valterovfi 1978). However,
Elifig (1974) and Strakog-l~ehfik (1975) consid-
ered these fragments to have been redeposited
Comments on tectonics into Jurassic clastic sediments. In contrast, Rehfik
(1975) interpreted the coal fragments in N~m 1
The M~nin block has a tectonic boundary with borehole as evidence of the occurrence of seven
the Nesva~ilka block in the north. This fault coal seams whose properties, particularly their
trending NW-SE was active during the Devo- degree of coalification, correspond to the upper-
nian and Carboniferous sedimentation. The N-S most part of the Ostrava Formation (Early
fault within the M6nin block was active during Namurian), specifically to the Poruba Member
the deposition of the Ostrava Formation (Fig. 5). of the Upper Silesian basin, l~ehfik's opinion was
Many other normal faults and thrust faults can later supported by macrophytopaleontological
also be deduced on the basis of changes in mean (Purkyfiovfi 1978a, b) and microphytopaleonto-
reflectivity values (R0) which were measured on logical studies (Valterovfi 1978, 1982).
samples from the N6m 1, 2 and 6 boreholes.
Westerly verging thrust faults are thought to be
Neogene in age, accompanying the emplacement Macrophytopaleontological investigations
of the Carpathian nappes. Their existence has
been proved palaeontologically suggesting that Purkyfiovfi (1978a, b) found in the N6m 1 and 2
100-200m of the sequence has been repeated. boreholes twenty plant species some of which
The eastern part of the Jurassic autochthonous are of Late Vis6an to Early Namurian age and
sediments, together with the underlying Paleo- others are of Namurian and Westphalian age.
zoic, were also affected by thrust faults. The assemblage indicates that the sediments
 EARLY NAMURIAN COAL-BEARING DEPOSITS, CZECH REPUBLIC 185

belong to the uppermost Early Namurian which sediments found in several boreholes near
lithologically correspond to those occurring in N6m6i6ky. The occurrence of Early Namurian
the upper part of the Ostrava Formation, i.e. to clastics in the N~m-1 borehole, at depths of
the Jaklovec and/or Poruba members of Upper 4253-4704m, is supported by finds of the
Silesian basin. These units are characterized by following species of miospores: Bellispores
the occurrence of the following species: Lygi- (Artuz) Sullivan, Ahrensisporites Potonie et
nopteris larischii, L. bartonecii, L. cf. stangeri, Kremp, Savitrisporites Bhardwaj and Tripartites
Sphenopteris adiantoides, Rhodeopteris stachei, (Schemel) Jachowicz. A similar assemblage of
Pecopteris aspera, Neuropteris cf. bohdanowiczii, miospores was found at depths of 3274.95-
Sphenophyllum tenerrimum, Mesocalamites roe- 4402.0m in the N6m 2 borehole. Among
meri, M. costiiformis, Lepidodendron cf. velthei- important miospores, the following species
mii, L. cf. obovatum and L. cf. aculeatum. were found: Rotaspora Schemel, Schulzospora
Kosanke, Verrucosisporites (Ibrahim) Smith and
Butterworth.

Palynological studies
Valterov~ (1978, 1982) following earlier inves- Coal petrology
tigations by Knobl-Jachowicz (in l~eh~tk et al.
1973), provided palynological evidence for the The coal fragments from the N~m 1, 2, 5 and 6
Early Namurian age of coal fragments and boreholes are of various provenances:

Table 1. Relative proportions of macerals and microfithotypes in % in samples of a coal seam penetrated by the
Ngm 2 borehole

Maceral groups (%)

Sample Depth (m) V L I Note
T366 3374,30-3375,00 91,9 5,3 2,8 upper part of seam
1"367 3375,00-3375,50 77,6 12,4 10,0 middle part of seam
T368 3375,50-3376.00 78,6 9,4 12,0 lower part of seam
T783 3374,30-3376,00 80,0 10,7 9,3 average sample
T369 3375,60 81,0 10,1 8,9 lump sample

Macerals and minerals (%)

Sample Telinite Collinite V Macro- Micro- Resinite Cutinite Alginite L
Total sporinite spodnite Total
T366 1,8 87,3 89,1 0,3 4,5 0,1 0,2 5,1
T367 1,2 75,2 76,4 0,7 11,1 0,1 0,3 12.2
T368 1,6 72,2 76,8 0,8 8.5 -, 9,2
T783 1,0 77,3 78,3 0,8 9,4 0,3 10,5
T369 0:6 79,3 80,1 0,7 9.3! 0,1 t0,0
Sample Micdnite Semi- Fusinite Sdero- I Clay Sulphid~ Carbo- Other M
Macrinite fusinite Unite Total minerals nates miner. Total
T366 1,0 0,9 0,5 0,3 2,7 2,9 0,2 - 3,1
T367 4.6 3,1 1,7 0,5 9.9 1,5 -. 0,1 1,6
T368 3,9 2,8 4,3 0,8 11,7 1,9 0,2 0,1 2,2
"1"783 4,3 2,5 1,8 0,5 9,21 2,0 0,1 2,0
T369 1.4 2,6 4,4 0,4 8,81 1,0 0,1 1,1

Microlithotypes (%)
Sample Vitdte Liptite Inertite Clarite Dudte V'dd- Td- Cartx)- Shale
nertite macerite minerite
T366 67,0 17,5 0,8 1,1 7,3 6,3
T367 43,6 1,3 27,0 2,9 2,O 21,4 1,81
T368 45,1 2,1 16,0 1,0 3,2 29,4 3,2
"1"783 45.1 0,5 21,4 0,5 2,3 27,3 2,9
T369 45,9 2,7 29,7 -I 1,0 19,8 0,8
(a)

Fig. 6. (a)-(e) Relative proportions of macerals and microlithotypes in samples from a coal seam penetrated by
the N6m 2 borehole.
(c)

Fig. 6. (continued)
188 J. DVOI~AK ET AL.

Fig. 6. (continued)

(i) Coal fragments in drill cuttings were represent the true coal petrographic composition
brought to the surface in the drilling mud. from a specified coal seam. Samples from the
The coal particles were separated by wash- N6m 1 borehole show that macerals of the
ing the drill cuttings in a heavy liquid or by vitrinite group vary between 78 and 84% those
hand picking. These samples provided of the liptinite group between 10 and 16%; and
information on the average grade of the the inertinite macerals from 5 to 13%.
coal coming from a certain depth interval. Detailed analysis of coal samples from the
(ii) Thin bands or small coal seams or seam N6m 2 borehole show vitrinite group macerals
with a minimum thickness of 170 cm was ranging between 77.6 and 91.9%. Some samples
identified in the N6m 2 borehole and layers also show a slightly increased content of liptinite
of coal claystones to coal siltstones were group macerals (5.3-12.4%) but mostly a lower
recovered from drill cores. content of inertinite group macerals (2.8-12%)
(iii) Tiny fragments of organic substance (Table 1 and Figs 6a-e).
(organoclasts) in clastic sediments of core In contrast, a few isolated fragments from the
runs. These samples served almost exclu- drill cuttings of the N~m 2 borehole, examined
sively for the determination of their rank. as bulk samples, showed higher contents of
inertinite. One sample contained more than
Coal petrology was carried out on samples from 50% inertinite. This composition resembles coal
two boreholes. Drill cuttings samples from the of the Karvinfi Formation of the Upper Silesian
N~m 1 borehole were prepared by maceration. basin. Unfortunately, the depth from which these
The maceral composition corresponds to an particular fragments come from is unknown.
average petrographic composition of the coal
substance from a certain depth interval. By
contrast, the samples from the N~m 2 borehole Chemical-technological analyses
were from core and represent a coal seam. These
samples were examined by maceration combined The samples were subjected to basic technologi-
with microlithotype analysis. The results thus cal and chemical analyses. Samples showing ash
 EARLY NAMURIAN COAL-BEARING DEPOSITS, CZECH REPUBLIC 189

contents exceeding 10% A d were washed in a found in the N~m 1 borehole (82.84-84.32%),
mixture of trichlorethylene and bromoform lower contents were established in samples from
having a specifc gravity 1500kgm -3 in order the N6m 2 borehole (80.08-82.14%), whereas
to reduce the ash content. Only samples from the lowest concentrations were found in samples
the N6m 6 borehole were not washed because of of the N6m 6 borehole (78.89-83.01%) (Table 2).
their small volume and low coal content, i.e. The content of hydrogen in the volatile matter
analysed without reducing the ash content. This (H ~af) varies between 5.34 and 6.38%. The low-
affected the results of the chemical-technologi- est content of 4.81% was found in a sample
cal analyses particularly as far as the content of from the N6m 5 borehole (Table 2).
volatile matter, coking and other properties are The results of the technological tests indicate
concerned. that the Carboniferous coal from the vicinity of
However, the A s values of samples from the N6m6i6ky ranges from subbituminous to high
Nfim6i6ky area should be considered approx- volatile bituminous coal. This is in contrast with
imate only because only a part of the drill core the relatively great depth of about 3000 to
and coal fragments were sampled, the rest being 4000m from which the coal samples were
left for further investigations. The ash content of recovered. Only finds from the N6m 6 borehole
samples from the drill cuttings (the N6m 1 and 6 are from depths less than 3000 m.
boreholes) can be uses only for the recalculation
of analyses.
The chemical-technological analyses show Vitrinite reflectance
that the coal fragments were, in general, only
The low degree of coalification of the organic
slightly coalified. This is supported by the
matter established on the basis of technological
contents of volatile matter (V daf) which in
tests (V daf, cdaf) is supported also by the results
samples from the N6m 1, 2 and 5 boreholes
of vitrinite reflectance (R0) measurements. The
vary between 37.1 and 39.9%. Coal samples
minimum value of R0 is 0.57% (the N6m 5
from the N6m 6 borehole, in fact, showed a
borehole, depth 2690.9m) whereas the max-
greater range from 37.3 to 41.5% but these
imum value is 0.9% (the N6m 1 borehole, depth
samples were not washed to reduce the content
4803.5m). This sample together with a coal
of ash (see above). The maximum coalification,
fragment from the depth of 4801.5m comes
occurred in the coal fragments derived from the
from the Early Carboniferous basement of the
greatest depth in samples from the N6m 1
coal bearing unit. The majority of values of Ro
borehole. The minimum coalification similarly
vary between 0.6 and 0.85% (Tables 2 and 3).
occurred in samples observed from the N6m 5
According to Hilt's law, the rank of coal
borehole. Combustion heat values (Qdaf) of
increases with increasing stratigraphic depth.
samples from the boreholes N6m 1 and 2 vary
Graphic expression of this law is a general plot
between 32.69 and 34.81MJkg -~. The lowest
of coalification (Patteisky-Teichmfiller 1960).
value Q ~af
s was established in a sample from the
The plot of coalification for the Czech part of
N6m 5 borehole giving 31.14 MJ kg -1 (Table 2).
the Upper Silesian basin and its use for inter-
A very low rank of coal results in a worsening
pretation of faults in boreholes was established
of coking properties of the coal. Values of the
by Weiss (1976).
swelling index vary between 0.5 to 2.0. Only the
A palaeogeothermal gradient of between 70~
two deepest samples from the N6m 1 borehole
to 90~ per km has been calculated, using
showed negative expansion during the dilatation
Buntebarth's method, in the Jablflnka 1 bore-
test. The other samples showed only some
hole, situated on the axis of a Variscan foredeep
contraction.
(see Fig. 1). The borehole penetrated a coal-
Total sulphur contents Std in coal of all the
bearing formation of the Early Namurian and
samples are rather low, ranging between 0.35
also rocks of the Early Carboniferous and
and 0.96%. The sulphur content is high only
Devonian. Boreholes situated to the west show
exceptionally. Samples from 2692.3m in the
steeper gradients of Rmaxvalues (Dvo~fik 1989).
N~m 5 borehole, and from 3060-3080m in
the N~m 6 borehole showed 3.5 and 5.35% Std
respectively. These extreme values are believed Discussion
to have been caused by the possible occurrence
of nodules of iron disulfides (Table 2). Timing of coalification
The results of elemental analysis support the
character of coalification which follows from the The coal in the N6m6i6ky boreholes was coalified
contents of volatile matter: the maximum con- prior to burial beneath the Carpathian nappes
tent of carbon in volatile matter (C aaf) was because the nappe cover thickens towards the
190 J. D V O R A K E T AL.

9 ~ ~ ' - ' - ' ' - ~

I'-- ~ I"",,,l''~l~"'l"'~i ~

o"

0
o

o z

~ . .
O N , O O ~
o o

~ , ~

,?
~ 0 ~ ~ ~
~ ~ ~ ~
N o 0 0 ~

o" o ' I o ' o " o " o o o o o ~0 ~ 0 0 0 0 0 0 0

~e

N N I o o O h O '

c~

~ N ~ ~ l ~ i ~

~ ' ~ ~
a

~ h N ~ N h ~

o
. ,...~

N N h ~ ~ ~

0
4

N N',-" ~- ~- N 04 ~1 ' , - 04

9 "~ r r I1~ ~
I-I-

E :u :_u ~o~-~
E Eo~o ~oE E ,.~ 0 9
~ m

Z~x~
 EARLY NAMURIAN COAL-BEARING DEPOSITS, CZECH REPUBLIC 191

Table 3. Mean relectance (Ro) measured on coal fragments from the NYm 1, 2, 5 and 6
boreholes

Borehole I Depth R V'~ iI Borehole I Depth R V n=f

(m) (%) (~~176i1 I (m) (%) (%)
N~rnEi~,ky 1 4248-4250 0.75 37.2 ,NlmEiEky2 I 3862,30 0.83 35.3
4310-4325 0.80 36.0~ 13863.10 0.80 36.0
14495 0.77 36.7 ,, 14401.50 0.74 37:5
4524 0.76 37.9 n
3480.00 0.75 37.2
4530-4535 0.79 36.3 i,Nlm(EiEky 5 2690.90 0.58 9 40
4204.50 0.70 38.4 2692.20 0.57 9 40
4206.20 0.71 38.2 ~' 2692.20 0.57 > 40
4254.20 0.74 37.4 I I 2692.30 0.60 9 40
4316.90 0.78 36.5 F'N~mEi6J~ 3349.50 0.69 38.3
4317.00 0.81 35.8 I 3350.80 0.68 38.5
4319.50 0.79 36.3 I 3351.10 0.72 37.3
4382.60 0.83 35.3]: 1"3843.00 0.76 36.8
4434.80 .... 0.79 36.3 ,, 13060- 3080 0.58 ~, 40
4801.50 0.90 33.6 ,, 13095 0.60 9 40
4803.50 0,90 33.6 ,, 13105- 3110 0.61 9 40
N~m6iEky 2 3204.50 0.60 40.9 ,, 13145 0.63 9 40
13271.50 0.60 40.9 ,, 13160 3185 0.71 37.9
13370.10 0.68 39.2 ,, 13190-3250 0.74 37.2
[3373.50 0.63 40.2 ,, 13250 - 3300 0.77 36.5
[3375.50 &73 37.7 ,, t3300- 3315 0.76 36.7
13478.30 0.74 37.5 ,, i3315 0.78 36.3
[3481.00 0.70 38.5 13315-3325 0.79 36.1
13624.50 0.70 38.5 "'j 13330 - 3345 0.78 36.3
13625.80 0.74 37.5:1 13350-3365 0.77 36.5
[3740.20 0.84 35.1 1 J3510- 3525 0.77 36.5]
1385g.50 0.83 35.3 :i 13545-3550 0.79 36.1
13860.50 0.85 34.9 ,, . 13760 0.81 35.7 i
Values V daf are derived from relationship R0 - Vaar, established by Weiss (1976) for
the Czech part of the Upper Silesian basin.

ESE (Fig. 4) and this has no effect on the coal other boreholes (e.g. N6m 1, 5 and 6)
rank in the underlying Carboniferous (c.f Fig. 4 provided the majority of coal fragments
and Table 3). By analogy with the coalification found in drilling mud. Some of them likely
process in the Upper Silesian basin it is likely that represent redeposited coalified logs and
the rank was developed during the late Carbo- coal clasts eroded from coal seams. With
niferous. the exception of the coal seam identified in
the drill core from a specific depth in the
N~m 2 borehole the remaining coal frag-
ments brought up in drilling mud may not
Conclusions
have originated from the indicated depths.
The discovery of previously unknown Early (2) Lithological similarities between sediments
Namurian (Namurian A) sediments has been from the boreholes and those occurring in
proved palaeontologically in the N~m6i6ky 1, 2, the Upper Silesian basin indicate that Early
5, 6 boreholes, drilled in the search for oil and Namurian occurrences in the N~m6icky
natural gas in SE Moravia (Purkyfiovfi 1978a, b; basin were linked with the Upper Silesian
Valterovfi 1978, 1982). However, neither sys- foredeep.
tematic coring, because the program was aimed (3) Purkyfiovfi (1978a, b) considered that these
at testing the oil and gas potential of the area, nor sediments are isochronous with the Jaklovec
logging of the boreholes for technical reasons and/or Poruba Members of the Ostrava
was undertaken. Formation of the Upper Silesian basin,
suggesting an Early Namurian (Namurian
(1) The partially cored N6m 2 borehole pene- A) age. Palynological studies of coal and
trated part of a coal seam at a depth of sediments also support a similar age (Val-
3374.3-3376.0m. This borehole and some terovfi 1978, 1982).
192 J. DVOI~,h,K E T AL.

(4) Coal samples from the N6m 2 borehole 1989. Anchimetamorf6za ve varisk6m tektog6nu
show the following composition (data in st~edni Evropy -jeji vztah k tektogenezi. Vdstnik
parenthese show the composition of coal (/st(edniho ftstavu geologick~ho, 64, 17-20.
fragments from the N6m 1 borehole): 1990. Geology of Palaeozoic sediments of the
deep borehole Jablfinka 1 (Beskydy Mts, NE
vitrinite 77.6-91.9% (78-84%), liptinite
Moravia)- comparison with the deep borehole
5.3-12.4% (10-16%), inertinite 2.8-12% Mfinsterland- 1. Sbornlk geologick~eh vdd, 45,
(5-13 %). A few samples of drill cuttings 65-90.
analysed as bulk samples from the N6m 2 - - 1 9 9 3 . Moravsk~ paleozoikum. Geologie Moravy a
borehole (unknown depth) show an Slezska. Sbornik pfisp6vkfi k 90. v~,ro~i narozeni
increased content of inertinite, which in prof. dr. K. Zapletala, 41-58.
one fragment exceeds 50%. Their composi- 1994. Varisk~ flydovf~ v~voj v NizkOm Jesenlku.
tion corresponds to that of coal coming Czech Geological Survey, Special Papers 3.
from the overlying Karvin~ Formation of 1995. Moravo-Silesian Zone. Stratigraphy. In:
DALLAMEYER, R. D., FRANKE, W. & WEBER, K.
the Upper Silesian basin.
(eds) Pre-Permian Geology of Central and Eastern
(5) Basic technological parameters of the Europe. Springer, Berlin, 447-489.
coal fragments from the N6m 1, 2, 5 ELIAg, M. 1974. Mikrofaci~lni v~,zkum karbonfit6
and 6 boreholes are as follows: A a naftonad6jn~,ch oblasti na p[iklad6 autochtonni
5.8-37.9%, V daf 37.1-41.5% Qoaf S 31.14- jury jihov~,chodnich svahfi Cesk6ho masivu.
34.81MJkg -1, S d 0.37-5.35, SI 0.5-2.0. Zemni plyn a nafta, 19, 359-374.
(6) The mean reflectance (R0) measured on GAYER, R. & PEgEK, J. 1992. Cannibalisation of Coal
Namurian coal fragments is 0.57-0.81%. Measures in the South Wales Coalfield- signifi-
(7) Mean values of Rmax obtained from all cance for foreland basin evolution. Proceedings of
the Ussher Society, 7, 380-384.
layers of the Late Carboniferous pene-
- - , S~'KOROV,k,I. & VALTEROVA,P. 1996. Coal
trated by the N6m 1 borehole (total 11 clasts in the Upper Westphalian sequence of the
samples) are equal to 0.7%. The calculated South Wales coal basin: implications for the
gradient of all boreholes is 0.03% Rmax. timing of maturation and fracture permeability.
In: GAYER, R. & HARRIS, I. (eds) Coalbed
Coal fragments identified in the drilling mud Methane and Coal Geology. Geological Society,
from these boreholes and samples of a coal seam London, Special Publication, 109, 103-120.
penetrated by the N~m 2 borehole at a depth of HON~K, J. & VRBOVA, V. 1980. Chemicko-technolo-
3374.3-3376.0 m show that their reflectance (R0) gick6 a uheln~-petrografick6 vyhodnoceni kar-
corresponds to that of high volatile bituminous, bonsk6ho uhli z vrtfi N6m~i6ky 1 a N~m6i6ky 2.
and occasionally to subbituminous coal. The Sbornlk GeologickOho prdzkumu Ostrava, 21,
very low rank of coal found in these boreholes 51-77.
argues for very fast coalification of peat which is et al. 1978. Zhodnoceni vrtnf~ch jader paleozo-
ic~ch hornin z vrtu Ndmdidky 2. MS Geofond,
in agreement with coal clasts found both in the
Praha.
Ostrava Formation of the Upper Silesian basin --, POLICK?, J. & WEISS, G. 1980. Diageneze
which come from eroded Early Namurian coal karbonsk~ch hornin z vrtfi N6m6i6ky 1 a N6m-
seams and the Westphalian C and D units of the 8i6ky 2. Sbornik Geologickkho pr~tzkumu Ostrava,
South Wales basin (Gayer-Pe~ek 1992, Gayer 21, 77-79.
et al. 1996). The rank of coal from N~m6i~ky PATTEISKY, K. & TEICHMOLLER,M. 1960. Inkohlungs-
was not affected by the deposition of overlying Verlauf, Inkohlung-Masstabe und klassifikation
Jurassic sediments and a flysch cover nor by its der Kohlen auf Grund von Vitrit-Analysen.
burial under Carpathian flysch nappes. Very fast Brennstoff-Chemie, 41, 79-84, 97-104, 133-137.
coalification provides evidence that the tempera-
POLICKY, J. & FIALOVA, V. 1980. Petrografick~, a
litologick~ charakter karbonu ve vrtech N6m6i6ky
ture gradient in the Variscan foredeep varied 1 a N6m6i6ky 2. Sbornik Geologickgho pr~zkumu
between 70 and 90~ -1 (Dvo~'~tk 1990). Ostrava, 21, 49-51.
PURKY]qOVA, E. 1978a. F16ra svrchniho karbonu
(namuru A) v paleozoiku jv. svahfi (~esk6ho
References masivu u N6m6i6ky na ji~ni Morav6. Casopis
SlezskOho Muzea Opava, A27, 77-86.
BUNTEBARTH, G., KOPPEL, J. & TEICHMOLLER, M. 1978b. Makrofloristick~i korelace sedimentfi
1982. Palaeogeothermic in the Ruhr Basin. In: karbonu ve vrtech Zaro~ice - 1, Uhfice - 1 a 2
(~ERM~.K, V. & HAENEL, R. (eds) Geothermics and a N~m6i6ky 1 a 2. Zemnf~ plyn a nafta, 23,
Geothermal Energy, 45-55. 555-566.
DrolL&K, J. 1980. Geotectonic condition of the I~EHAK, J. 1975. Carboniferous coal from M~m6i6ky -
forming and the extinction of the reef complex, 1 deep borehole near Hodonin in southern
notably in the Devonian of Moravia. Vdstnik Moravia. Vdstnik (/st(edniho ~stavu geologick~ho.
Usoredniho fistavu geologick~ho, 55, 203-208. 50, 179-182.
 E A R L Y N A M U R I A N C O A L - B E A R I N G DEPOSITS, C Z E C H R E P U B L I C 193

-- et al. 1973. Zhodnocenl uhli z hlubokf:ch vrt~ v 1982. Zji~tdni karbonsk~ch miospor v hlubok~ch
okoli Velk~ch Pavlovic. MS Geofond, Praha. vrtech jv. svah~ Cesk~ho maslvu na jiYni Moravd.
STgAKO~, Z. & REHAK, J. 1975. Diskuse k vfskytu uhli Sbornik IV. uheln6 geologick6 konference P~ir-
karbonsk~ho st6?i na ji~ni Moravd. Sbornik II. odov6deck~ fakulty UK, 151-154.
uheln6 geologick+ konference Pfirodov~deck+ WEiss, G. 1976. K prfib6hu zm6n stupn6 prouheln~ni s
fakulty UK, 137-141. hloubkou v 6s. 6~isti hornoslezsk6 p~inve. Sbornik
VALTEROVA, P. 1978. Palynologick~ v2~zkum ve vrtu Geologick~ho pr~zkumu Ostrava, 11, 9-34.
N6m6i6ky 2. Zemnf: plyn a nafta, 23, 597-618.
 M6ssbauer spectroscopic investigation of low rank coal lithotypes
IRENA K O S T O V A l, K A L I N K A MARKOVA 2 & KRASIMIR KUNTCHEV 1

l Institute of Applied Mineralogy', Bulgarian Academy of Sciences,

92, Rakovska Str., 1000, Sofia, Bulgaria
2 St Kliment Ohridski University of Sofia, Tzar Osvoboditel Blvd 15, Sofia, 1000, Bulgaria

Abstract: Low rank coal lithotypes- xylain, humovitrain, semifusain, fusain and liptain
sampled from the Maritsa Iztok coal basin (Bulgaria) have been examined by M6ssbauer
spectroscopy with no pre-concentration procedures. The results are used to identify three
iron species in coal lithotypes and show that covalent iron (Fe n) related to pyrite, is the main
iron species in xylain, while in humovitrain ferric iron is dominant. The total quantity of
iron species in semifusain, fusain and liptain is about the same, but their distribution is
different. Ferric iron dominates in all the three lithotypes. Ferrous iron, although present in
smaller quantities, has a higher content in fusain than in semifusain. Our results illustrate
the type of oxidation processes which formed the coal lithotypes. A transformation of Fez+
to Fe 3+ has occurred out as a result of differing oxidation processes. The intensity of that
transformation increases during the destructive microbial oxidation and decreases during
thermal oxidation and direct oxidation processes. The opposite transformation of ferric to
ferrous iron has been achieved during both thermaloxidation and direct oxidation processes.

Detailed study of the mineral matter in coal is semifusain, fusain and liptain sampled from the
very important for the preservation of the Troianovo mine No. 1 in the Bulgarian Maritsa
environment since mineral matter may cause Iztok coal basin (Fig. 1) Their characteristics
air, water and soil pollution as a result of the are presented in Table 1. The investigated
combustion of coal. There are various techni- lithotypes belong to three genetic series. The
ques which have been used for the analysis of first genetic series is primary plant m a t t e r -
mineral matter in coal. X-ray diffraction, infra- x y l a i n - humovitrain; the second genetic series
red spectroscopy, thermal and microscopic is primary plant m a t t e r - s e m i f u s a i n - fusain;
analysis are the most commonly used techniques, and the third genetic series is primary plant
but in some cases, due to their low sensitivity, matter - liptain.
pre-concentration procedures are required. The coal lithotypes have been sampled
The high sensitivity and noninterference because of their more homogeneous nature
characteristics of the M6ssbauer effect allows it than the trivial coal molecular structure. This
to be used for the determination of several iron is the reason these petrographic ingredients
species without any pre-concentration proce- have been selected to develop a model in our
dure. Bituminous and subbituminous coal and study.
their lithotypes have been examined in detail
using M6ssbauer spectroscopy (Smith et al.
1978; Melchior et al. 1982; Martinez-Alonso
et al. 1987). M6~sbauerspectroscopy
We have used this method for the investiga-
tion of iron species in low rank coal lithotypes M6ssbauer spectra of the samples were obtained
which had not previously been attempted. The using a purpose-made spectrometer with con-
main iron-bearing minerals found in the Maritsa stant acceleration and a resolution of about
Iztok coal basin are illite, pyrite, siderite and 0.1 mm/s per channel. The radiation source used
was 57Co in a palladium matrix, while the isomer
dolomite. Some pyrite in coal is very unstable
and is converted into iron sulphates with shifts were measured with respect to the center
different number of hydrous water molecules. of the spectrum of a reference sample of c~-Fe.
Owing to the low content of iron in the samples
the spectra were accumulated to reach a signal of
10 6 counts per channel. To determine the line
Experimental method
parameters the spectra were processed by the
Coal samples computer program 'M6sspec' for iterative
approximation of the experimental points
The subject of the present study is coal through a sum of Lorentzian profiles using the
lithotypes of low rank: xylain, humovitrain, least-square method.

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 195-199.
196 I. KOSTOVA E T AL.

> k~ BULGARIA Varna et'/"J" ~

- - - ( . . . . . ..J
GREECE 45km

~'~ MaritsaIztokCoal Basin

Fig. 1. Location of Maritsa Iztok coal basin in Bulgaria.

Table 1. Characteristics of lithotypes

Lithotypes Proximate analysis (wt%) Elemental analysis (%)

Moisture Ash Volatile Carbon Hydrogen Nitrogen Sulphur Oxygen

content matter
Wa Ad V daf cdaf H daf N daf sdaf odaf

Xylain 7.2 2.6 61.1 68.7 6.8 0.7 4.7 19.1

Humovitrain 10.0 5.9 56.4 66.9 5.2 1.2 3.2 23.5
Semifusain 9.4 9.2 35.1 71.1 4.3 0.8 3.3 20.5
Fusain 8.8 4.4 17.0 87.2 3.1 0.8 1.9 7.0
Liptain 4.0 2.4 70.9 70.8 7.0 0.8 3.7 17.7

a, analytical; d, for dry basis; daf, for combustible basis.

Results two groups (a) and (b) with similar M6ssbauer

parameters. These groups have centre shifts
The results obtained from the M6ssbauer study (6 mm/s) and quadrupole splittings (A mm/s) as
of low rank coal lithotypes are presented in Fig. 2 follows:
and Table 2. Ferric (Fe 3+) and ferrous (Fe z+)
iron, including covalent iron (FeII) were estab- group (a) 0.32-0.42 and 0.62-0.85
lished in different quantities in the five examined group (b) 1.05-1.33 and 2.11-2.99
lithotypes - xylain, humovitrain, semifusain,
fusain and liptain. With Fe u we identify the Ferric or ferrous covalent iron, or a combination
covalent iron, connected with pyrite in contrast of both, belong to group (a). It is not possible to
to the other ferrous iron, which may be related to determine separately ferric and covalent iron
other mineral phases such as siderite and dolo- due to a covalent deposition of iron in pyrite on
mite, which have been detected with X R D the one hand and the close M6ssbauer para-
analysis, or organic compounds. The ferric iron meters (centre shifts of 0.32-0.35 and quadru-
is connected mainly with the clay mineral illite. pole splitting of 0.60-0.65mm/s) of both iron
The observed iron species can be subdivided in species on the other hand. An additional real
 LOW RANK COAL LITHOTYPES 197

(1)

(2)

(3)

..,~_
(-
-'1

.>
.1-,,
m (4)
fl)
n"

(5)

9 t I 1 I I ,,, 1 1 r [ I J I l I
-a -2 o 2 ~ (; +3 I0

Velocity (mm/s)
Fig. 2. M6ssbauer spectra of (l) xylain; (2) humovitrain; (3) semifusain; (4) fusain and (5) liptain. Velocity axis is
with respect to ~Fe.

difficulty is the insignificant content of iron in In the members of the second genetic series,
these samples. Ferrous iron belongs to group semifusain-fusain, iron of both group (a) and
(b). It may be related to the carbonate minerals, group (b) has been established. Fe 3+ and Fe 2+
siderite and dolomite, in coal. Iron from group can be clearly distinguished in semifusain
(a) has been established in xylain and humovi- (Fig. 2). A very small quantity of covalent iron
train in the first genetic series (Table 2). can be masked by Fe 3+. Ferrous iron is present
With the help of other parallel studies (XRD, in considerably smaller amounts (11.4%), and
SEM and TEM), and according to unpublished ferric iron predominates. It is very likely that
data it can be demonstrated that in xylain iron is Fe 2+ is connected with carbonates, siderite and
connected mostly with pyrite, i.e. covalent iron dolomite, which have been established in this
(FeII) dominates. The expected presence of Fe 3+ type of coal under X-ray diffraction and SEM
is in a subordinate quantity, about 8 to 10%. analysis. With the second representative of the
With the second representative of the genetic genetic series, fusain, the iron forms observed
series, humovitrain, because of the higher value coincide with those established in the semifu-
of quadrupole splitting, the iron present is Fe 3+ sain, but their quantities are different (Table 2).
(Fig. 2). The amount of Fe z+ is greater (group b), and the
198 I. KOSTOVA E T AL.

Table 2. M6ssbauer parameters a for lithoO'pes low rank

Sample Group b Centre shift c Quadrupole Line widthd

splitting

Xylain a 0.32 4- 0.05 0.62 4- 0.05 0.56 4- 0.08 100+8

Humovitrain a 0.35 4- 0.015 0.66 4- 0.1015 0.41 4- 0.025 100 4-4
Semifusain a 0.334-0.15 0.694-0.015 0.564-0.03 88.64-2
b 1.124-0.03 2.11 4-0.03 0.26+0.07 11.44-4
Fusain a 0.424-0.01 0.854-0.01 0.554-0.02 67.6 4- 3
b 1.334-0.01 2.994-0.01 0.424-0.02 32.4 4- 3
Liptain a 0.36 4- 0.06 0.65 4- 0.06 0.30 4- 0.08 80.04- 10
b 1.054-0.10 2.73+0.1 0.384-0.06 20.0 4- 10

a All parameters are in mm/s.

b a is assigned as pyrite (FeII) or Fe 3* or combination of both. b is Fe 2+.
c The centre shifts are reported relative to c~Fe.
d Width at half maximum of the peak.

amount of the iron of group (a) less (Fe 3+ or/ decomposition of the peroxides and hydroper-
and Fe n) in comparison with semifusain, as can oxides to free radicals:
be demonstrated by the high quadrupole split-
ting of the first peak (Fig. 2). The basic iron R O O H + Fe 2+ ~ RO" + Fe 3+ + OH" (1)
present (67%), is Fe 3+. If there is any admixture
These peroxides and hydroperoxides have been
of covalent iron, its amount will a be minimal, produced by the oxidation of organic matter.
(about 5 to 7%). One third of the iron The resultant free radicals RO" and OH" are
established in fusain is bivalent. In semifusain, very active and are the reason for the polimer-
and especially in fusain, an increased content of ization process (Kucher et al. 1980).
macropores is observed (Markova et al., 1992) The formation of lithotype maceral of the first
with 98.4% in semifusain and 99% in fusain. genetic series represents a continuation of the
A large proportion of the clay minerals and destruction by microbial oxidation (Si~kov 1988).
pyrite is found in these pores. The porous Therefore, the probable reason for the high
structure of these lithotypes is related to the Fe 3§ content in the final product of this genetic
high ash content (Table 1). It is likely that a series, humovitrain, is the continuous oxidation
great part of the Fe 3+ and Fe z+ is connected process represented by mechanism (1). Accord-
with mineral matter. In liptain, from the third ing to Sigkov (1977) this lithotype appears to be
genetic series, iron of both (a) and (b) groups a huminic polymer.
has also been established, Fe 3+ (80%) being The lithotypes of the second genetic series:
predominant (Table 2). semifusain - fusain contain both Fe 3§ and Fe 2§
These lithotypes are a product of fusanization
which has taken place as a result of thermal
processes in a strongly acidic medium with high
Discussion oxygen fugacity (Sigkov 1988).
Ferrous iron was found to be present in the low It can be assumed that due to this intensive
rank lithotypes of the first genetic series: oxidation process the peroxide and hydroper-
x y l a i n - humovitrain formed as a result of oxide groups have disintegrated under the action
gelefication under microbial oxidation destruc- of the salts of the transition metals by a
tion conditions (Sigkov 1988). However, in combination of reaction (1) and mechanism (2)
xylain covalent iron (Fe n) is dominant indicat- (Ivanov 1970):
ing pyrite. Pyritic iron in humovitrain is R O O H + Fe 3+ ---+ROO" + Fe 2+ + H + (2)
probably present at rather low concentration,
in the range 10-15 wt%. Salts of metals with However, our results indicate that the processes
variable valency have been identified in peat of formation of ferrous iron {mechanism (1)}
bogs (Garrels & Maskenty 1974). It is suggested are dominant not only xylain and humovitrain
that these salts have acted catalitically during the but also in semifusain and fusain. With the
 LOW RANK COAL LITHOTYPES 199

progressive increase in the fusanization process, thermal oxidation and direct oxidation pro-
from semifusain to fusain, the intensity of cesses. The opposite transformation of ferric to
reaction (1) decreases, while the intensity of a ferrous iron occurs during both thermal oxida-
mechanism (2) increases (i.e. the ferric iron tion and also direct oxidation processes.
content increases).
The lithotype of the third genetic s e r i e s -
liptain, which was formed under the direct action
of oxygen, contains both iron species - Fe 3+ and References
Fe 2+ but the ferrous iron predominates. Conse-
quently, it can be concluded that the peroxides GARRELS, P. & MACKENZY, F. 1974. Evolusia osa-
dachnix porod. Ser. Earth Sciences, Vol. 58, Mir,
and hydroperoxides produced by oxidation have
Moskwa.
been decomposed by the action of metals with IVANOV, S. 1970. Verishni radicalovi reactsii. Nauka I
variable valency according to the two mechan- izkustvo, Sofia.
isms as discussed above. The results illustrate the KUCHER, R.V., KOMPANETS,V. A. & BUTUZOVA,L. F.
processes of oxidation associated with the 1980. Structura iskopaemix uglei i ix osobenost k
formation of the coal lithotypes. okisleniu. Naukova dumka, Kiev.
MARKOVA, K., RADEV, G. & KOSTOVA, N. 1992.
Razpredelenie por v ugolnix litotipax niskogo
Concusions ranga. Ximia tv topliva, 3, 20-22.
MARTINEZ-ALONSO, A., GRACIA, M., GANCEDO, R.,
Low rank coal lithotypes contain three iron GONZALEZ-FLIPE, A. R. & TASCON, J. M. D.
species which can be identified using M6ssbauer 1987. The roles of organic and mineral matter in
spectroscopy without pre-concentration proce- aerial oxidation of brown coal. In: MOULUN,J. A.
et al. (eds) International Conference on Coal
dures. Covalent iron (Fe n ) related to pyrite is
Science 1987.
the main iron species in xylain. However, in MELCHIOR, D. C., WILDEMAN, T. R. • WILLIAMSON,
humovitrain ferric ison is dominant. Almost D. L., 1982. Mrssbauer investigation of the
100% ferric and ferrous iron in different transformations of the iron minerals in oil shale
quantities has been determined in the three during retorting. Fuel, 61, 516-522.
lithotypes - semifusain, fusain and liptain. SIgKOV, G. D. 1988. Teoretichni osnovi na biohimich-
Ferric iron dominates in all three. Ferrous iron nata vaglefikatsiya. Univ. Izd. St. Kliment
is present in smaller quantity but it increases Ohridski.
in fusain. SMITH, G. V., Liu, J. H. & SAPOROSCHENKO,M. 1978.
Mrssbauer spectroscopic investigation of iron
Our study demonstrates that a transformation species in coal. Fuel, 57, 41-45.
of Fe 2+ to Fe 3+ has been carried out as a result VOITKEVICH, G. V., KIZILTSTEIN,L. I. & HALODKOV,
of different oxidation processes. The intensity of J. I. 1983. Rol organicheskogo vechtestva v
that transformation increases during microbial konsentrasii metalov v zemnoi kore. Nedra,
oxidation destruction and decreases during Moskva.
 Comparison of solid state 13C NMR of algal coals/anthracite and
charcoal-like fusinites: further evidence for graphitic domains
P. I. P R E M O V I ( ~ , R. S. N I K O L I ( ~ & M. P. P R E M O V I ( ~

Laboratory for Geochemistry and Cosmochemistry, Department of Chemistry, University of

NiY, P.O. Box 91, 18000 NiY, FR Yugoslavia

Abstract: Carbon distribution in coals and coal macerals was studied by 13C NMR cross-
polarization (CP)/magic angle spinning (MAS) spectrometry. We examined two charcoal-
like fusinites from Serbia: the Jerma (Jerma mine) and Miro~ (mine 'Aliksar') seams. This
examination revealed that atomic H/C ratios calculated (on the basis of the CP/MAS
parameters) for fusinites studied are higher by 68% (Jerma) and by 64% (Miro6) than the
H/C values which are determined by elemental analysis. Calculated H/C values infer that
either more carbon or less hydrogen is required for the fusinite structures than is contained
in the samples. We conclude that the differences in the estimation of H/C for bituminous
charcoal-like fusinites between solid state 13C NMR and elemental analysis can be explained
by graphitic domains within the maceral 'invisible' in the CP/MAS experiment.

Coals have been subjected to many magnetic seams: Jerma (the Jerma mine) and Miro6 (the
resonance studies, and many parameters have Aliksar mine) with high maceral purity (>90%).
been measured to obtain information about coal For comparison, two fresh-water algal coals
molecular structure. During the last decade (torbanites) (Scotland and S. Africa) and,
researchers have focused their attention on marine algal coal tasmanite (Australia) and the
solid state 13C N M R spectroscopy with CP/ Vrgka Cuka anthracite (Serbia) were also
MAS because in principle this technique pro- examined.
vides a non-destructive way to measure the The earliest spectroscopic work of which we
aromatic/alkenic carbon fraction of coals fa (the are aware which discusses chemical structure of
ratio of aromatic/alkenic carbon Car to total algal coal-torbanites is that of Millais &
carbon C), one of the key parameters which Murchison (1969). These authors investigated
characterize the coal structure (Wilson & five torbanite samples from: S. Africa, France
Vasallo 1985). Usually in 13C N M R spectra of and Scotland. Their petrographic examination
most coals two broad lines can be distinguished indicates that these freshwater coals contain
belonging to the aromatic/alkenic and aliphatic alginite (maceral of the exinite group) in excess
carbon atoms respectively: fa of coal is defined as of 90% by volume. Cane & Albion (1971) have
the ratio of the integrated line intensity for proposed that alginite is an oxidative polymer of
aromatic/alkenic carbon atoms to the total straight-chain alkadiens of molecular formula:
integrated line intensity (Speight 1994). CH2 = CH(CH2),,CH = CH(CH2)4CH3 (n = 15,
In addition to aromaticity fa, dipolar dephas- 17 and 19). Allan et al. (1979) analyzed three
ing (DD) experiments provide estimates of other torbanites (S. Africa, Australia and Scotland)
structural parameters of coals including the using various geochemical and optical techni-
aliphatic (s) and the aromatic/alkenic (p) frac- ques. They concluded that the torbanites are
tion which are protonated (Wilson & Vasallo composed of polymeric materials which contain
1985). Yet major problems exist concerning the relatively high proportion of aliphatic structures.
use of solid state 13C N M R spectrometry in coal According to Allan et al. (1979) the evidence for
research. One such problem is that the 13C aromaticity is conflicting but the total Car is
N M R experiment gives inadequate quantitative suggested to be small on the basis of the
estimation of carbon distribution in coal which elemental analysis and infrared (IR) spectra.
strongly contradicts other geochemical data For a number of years, this laboratory has
(Premovi6 et al. 1992). This contributes to the been engaged in the structural elucidation of
difficulty in the unequivocal interpretation of the coals and kerogens. Premovi6 et al. (1987)
N M R data. The purpose of this report is to studied two torbanites from Scotland and S.
show that the estimation of H/C for fusinite Africa by both 13C N M R CP/MAS technique
(maceral.of the inertinite group) with solid state combined with DD experiments and 1H N M R
13C N M R is not in agreement with elemental MAS technique. This examination has shown
data. For the sake of clarity, we will consider that these coals have predominantly both
only two fusinite materials from two Serbian aliphatic carbon and protons ( > 9 5 % of total

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 201-205.
202 P. I. PREMOVI(~ E T AL.

organic carbon and hydrogen) incorporated into 1 K FIDS, acquired with a 3 ms contact time,
polymethylene (-CH2-) skeleton structures. 0.35 second recycle time and a rotor frequency
of c. 4 kHz, were zero filled to 8 K before Fourier
transformation. The pulse sequence employed
Experimental procedure for obtaining the dipolar dephasing (DD)
spectra is described elsewhere (Premovi6 et al.
The isolation procedure was similar to that used 1987).
by Premovi6 (1984) and Premovi6 et al. (1986). Proton N M R spectrum of tasmanite was
Powdered rock (50g) was extracted with ben- taken at 270MHz with MAS and BR-24 at
zene methanol (3:lv/v) for 96h in a Soxlet room temperature on an N M R pulse spectro-
apparatus. The residue remaining in the Soxlet meter constructed in the laboratories of the
thimble was treated with boiling hydrochloric Friedrich Schiller University, Jena (Germany)
acid (HC1, 4 M) to remove most of the carbo- (Premovi6 et al. 1987).
nates. Carbonate removal was checked by IR For F T I R analysis, the sample was mixed
analysis. The insoluble residue was further with anhydrous potassium bromide and pressed
demineralized by repeated treatment with boil- into the disc (2.5 mg/150 mg KBr) with a load of
ing hydrofluoric/hydrochloric acids (HF/HC1, 200 MPa. The spectra were recorded at room
22 M and 0.25 M, respectively). This acid mix- temperature on a Bruker ISF l13V F T I R
ture removes silicates and the removal was spectrometer.
checked by IR analysis. The final residue is the
coal sample. It contained only small traces of
inorganic minerals, including pyrite, as con- Results and discussions
firmed by the electron microprobe analysis.
Algal coals (Table 1) are of Permian age In addition to torbanites, we have studied by 13C
(about 250 Ma). The Vrgka (~uka antracite and CP MAS marine algal coal: tasmanite contain-
the maceral concentrates from Serbian seams ing more than 90% by volume sporinite
(Table lb) are of Jurassic age (about 200 Ma). (maceral of the exinite group). Figure 1 shows
All 13C N M R spectra of the coal samples were typical 13C and 1H N M R spectrum of tasmanite
recorded at 25.15 MHz on a Bruker CXP-100 as which indicate a presence of a strong aliphatic
previously described (Premovi6 et al. 1986). The carbon (Fig. l a) and proton (Fig. l b) bands

Table 1. Geochemical data on the coals." (a) algal coals," (b) bituminous coal macerals (Serbian seams) b
(a)

Location Maceral C H (O,N) a

H H
(mol/kg) )ca s C C

South Africa alginite 67 111 5 0.09 0.89 1.66* 1.61t

Scotland alginite 69 108 4 0.12 0.92 1.57" 1.62t
Tasmanite sporinite 60 92 1 0.10 0.90 1.53" 1.62t
(b)

Location Maceralc C H (O,N) a

H H
(mol/kg) fa S p C C
Vr~ka6uka vitrinite 76 19 0.7 1.00 0.00 0.25 0.25* 0.25~
Jerma inertinite 78 32 2 0.90 0.80 0.55 0.40* 0.66~
Miro~ inertinite 76 38 3 0.80 0.80 0.65 0.50* 0.85~

* Experimental.
t Calculated using expression 2.
Calculated using expression 1.
a Dry, ash-free corrected maceral data.
b Separated by sink-and-float procedures by heavy liquids starting with hand-picked lithotypes that were rich in
the desired maceral.
Predominant maceral (>95%) component.
 SOLID STATE 13C NMR 203

--CH 2--

~i = I

. 9 l , I ~ l i I , 1 ~ ! 1 , 1 9 1 ~ 1
160 140 120 100 80 60 40 20 0 -20
CHEMICAL SHIFT (Plan)

Aliphatlc

A 1 ~ 1 L
10 5 0
CHEMICAL SHIFT (ppcn)

Fig. l. 13C (a) and 1H NMR (b) spectra of the powdered sample of the Vrgka Cuka anthracite.

inferring that more than 95% of both organic value of: 2 for aliphatic portion and 1 for
carbons and protons are aliphatic. Thus these aromatic/alkenic part, we may write
results suggest that the tasmanite is an aliphatic
material which also contains a relatively high H = 2SCal +pCar
proportion of polymethylene chains and rather
were H is the total hydrogen of coal.
low amount of aromatic/alkenic groups in the
Combining these two equations we obtain
structures. It is likely that the best estimated fa
value for these materials is close to 0.10 H
(Premovid et al. 1987). ~ - = 2s(1 - f ~ ) +Pfa- (1)
If total coal carbon is apportioned to both
aliphatic (Ca0 and aromatic/alkenic carbons C~r, As N M R study indicates that fa values for the
then C = C a l + C a r assuming an overall H/C algal coals in question is small (c. 0.1) and that
204 P. I. PREMOVI(~ E T AL.

most of aromatic/alkenic carbons are non- in elemental data tend to imply) there is a
protonated (Premovi6 et al. 1987) then the good correspondence between experimental
product Pfa is small and can be neglected. In (obtained by elemental analysis) and calculated
this case, formula (1) is simplified into the form: (through NMR data) H/C ratios for algal
coals considered here.
H We have also studied the Vrgka Cuka
~ - = 2s(1 -fa). (2) anthracite using both the 13C N M R CP/MAS
(Fig. 2a), 1H N M R MAS (Fig. 2b). The results
The H/C values (calculated using the expres- show that this coal has predominantly polyaro-
sion 2) of algal coals studied are listed in matic structures withfa = 1.0 and consists chiefly
Table la. Unless the calculations are more of the vitrinite maceral (>90%). It has been
seriously in error (than the stated uncertainly suggested that all X3C atoms in these structures

Aromatic

I , I , I 1 , 1 , l , I , 1 ~ 1 , i
160 140 120 100 80 60 40 20 0 - 20
CHEMICAL SHIFT (ppm)

Aromatic

-*: 1 I ,
lo o
CHEMICAL SHIFT (OOm)
Fig. 2. 13C (a) and ]H NMR (b) spectra of the powdered sample of tasmanite.
 SOLID STATE 13C NMR 205

are not equally cross polarized with IH nuclear and elemental analysis can be explained by
spins. Most researchers of the subject now agree, graphitic domains* within these macerals invi-
however, that the number of ~3C atoms in these sible in the CP/MAS N M R experiment.
coal structures that are not observed by 13C
N M R is small (Speight 1994). This work is supported by a grant to PIP from
Since the anthracite is wholly polyaromatic, Ministry of Science (Serbia), Project 0206. Special
the total carbon can be expressed as C = C a r . If thanks to: the late D. Urogevi6 who supplied the
this is correct then the total hydrogen is given by fusinite samples (Serbia), the Vrgka Cuka mine
(Serbia) for providing the anthracite sample, and
H = pCar = pC. Buerau of Mineral Resources, Geology & Geophysics
(Australia) for supplying the tasmanite sample.
Hence p = H/C. The calculated value of H/C(= p)
shown in Table 1b is in excellent agreement with
the experiment. Table 1b lists atomic H/C ratios References
of Serbian (Jerma and Miro~) fusinite samples
computed using expression (1). An examination ALLAN, J., BJOROY, M. & DOUGLAS, A. G. 1979. A
geochemical study of the exinite group maceral
of this table reveals that calculated H/C values alginite, selected from three Permo-Carboniferous
for the fusinite samples are higher by 68% torbanites. In: DOUGLAS, A. G. & MAXWELL,
(Jerma) and by 64% (Miro6) than those experi- J. R. (eds) Advances in Organic Geochemistry
mentally determined values. Thus, the H/C 1979. Technip, Paris, 599-618.
values calculated on the basis of the CP/MAS CANE, R. F. & ALBION,P. R. 1971. The phytochemical
parameters suggest that either more carbon or history of torbanites. Journal of the Proceedings of
less hydrogen is required for the fusinite struc- the Royal Society New South Wales, 104, 31-37.
tures than it is contained in the sample. If this MILLAIS, R. & MURCHISON,D. G. 1969. Properties of
notion is valid then there are only two reasonable coal macerals: infrared spectra of alginites. Fuel,
48, 247-258.
explanations for the contradiction (between PANTIE, N. & NIKOLIC,P. 1973. Ugalj. Nau6na knjiga,
experimental and calculated H/C value given in Belgrade.
Table lb): (1) the fusinite carbons are extensively PREMOVlC, P. I. 1984. Vanadyl ions in ancient marine
substituted e.g. by O or N for which there is, carbonaceous sediments. Geochimica et Cosmo-
however, no persuasive geochemical evidence; chimica Acta, 43, 873-877.
and, (2) in the fusinite structures there are carbon --, PAVLOVIC, M. S. & PAVLOVIC, N. Z. 1986.
atoms which do not show their resonancies in the Vanadium in ancient sedimentary rocks of marine
13C N M R CP/MAS spectrum. origin. Geochimica et Cosmochimica Acta, 50,
In general, the CP/MAS experiment relies on 1923-1931.
, STOJKOVIC, S. R., PUGMIRE, R. J., WOOLFEN-
the presence of organic structures abundant in DEN, W. R., ROSENBEREG, H. & SCHELER, G.
protons in order to observe the 13C N M R 1987. Spectroscopic evidence for the chemical
resonancies. Consequently, the 13C N M R spec- structure of algal kerogens. In: RODRIGUEZ-
tra do not show signals from carbon atoms in CLEMENTE, R. R. & TARDY, Y. (eds) Proceedings
structural domains within coal lacking protons, of the International Meeting 'Geochemistry of the
such as graphite. On the other hand, physical, Earth Surface and Process of Mineral Formation '.
chemical and other studies indicate that the coal C.S.I.C., Madrid, 421-430.
fusinites are similar to natural charcoals which is , JOVANOVIC, Lj. S., & MICHEL, D. 1992. Solid-
consistent with the view that these macerals had State 13C and 1H NMR in kerogen research:
Uncertainty of aromacity estimation. Applied
been exposed to elevated temperatures and
Spectroscopy, 46, 16-18.
charred before incorporation in the sediment SPEIGHT, J. R. 1994. Application of spectroscopic
(Panti6 and Nikoli6 1973). If this concept is true techniques to the structural analysis of coal.
then fusinites as natural charcoal materials Applied Spectroscopy Review, 29(2), 117-169.
would undoubtedly contain a high amount of WILSON, M. A. & VASALLO, A. M. 1985. Develop-
graphitic components which are inactive for the ments in high resolution solid state 13C NMR
CP/MAS approach. spectroscopy of coals. Organic Geochemistry, 8,
Thus, we suggest that the differences in the 299-312.
estimation of H/C for charcoal-like fusinites
(Serbian seams) between solid state 13C N M R * Consists chiefly of amorphous charcoal.
 Composition and properties of North Bohemian coals

IVANA SYKOROV,~ l, J A R O S L A V ( ~ E R N ' ~ 2,

HELENA PAVLiKOV,~ 3 & ZUZANA WEISHAUPTOV,~ 1

l Institute of Rock Structure and Mechanics, Czech Academy of Sciences,

V HoleYovidk(tch 41, 182 09 Prague, Czech Republic
2 Department of Petroleum Technology and Petrochemistry,
Institute of Chemical Technology, Technickdt 5 166 28 Prague, Czech Republic
3 N M R Laboratory, Institute of Macromolecular Chemistry, Czech Academy of Sciences,
Heyrovskdho ndtm. 2, 162 06 Prague, Czech Republic

Abstract: This work presents the mean chemical, micropetrographic, surface and other
characteristics of coal seams from western, central, and eastern parts of the North Bohemian
brown coal basin. Attention was especially paid to the elemental composition, ash content,
content and forms of sulphur, occurrence of syngenetic and epigenetic sulphides, maceral
composition, and degree of gelification and decomposition of components in the huminite
maceral group. Some other coal characteristics were also assessed, such as pore texture,
extractability and solvent swelling of the coals.
The coals examined were huminitic with a variable xylite and detrite content. Huminite
reflectance varied between 0.33 and 0.39%. Substantial differences in pore texture of the
coals were found in the range of meso- and macropores. These differences largely affected
the extractability of the North Bohemian coals. The coals also exhibited extremely high
swelling ratios in basic solvents, such as pyridine.

The N o r t h B o h e m i a n basin is the most impor- The main coal seam belongs to the M i o c e n e
tant b r o w n coal basin in the Czech Republic. It Most F o r m a t i o n . The only mineable seam in the
is situated south of the Kru~n6 H o r y m o u n t a i n s N o r t h Bohemia coal basin is the m a i n coal seam
and has an area of approximately 1400 k m 2. with an average thickness of 30 m a n d m a x i m u m

i ,_.r-'/% ~,~
L

S'
'73.75"bs7 .+f'

@~ ..... ~"'"'"<,.<:.,. ,,

Fig. 1. Map of North Bohemian coal basin.

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geologyand Technology,
Geological Society Special Publication No. 125, pp. 207-217.
208 I. SS(KOROV~, E T AL.

thickness of 60 m. It consists mainly of humi- and in the deepest areas (Hrdlovka, Osek,
nites. Liptobiolites and liptodetrites occur rather Dfinov) even metatypes, of brown coal were
rarely. Very stable interlayers divide the seam formed in relation to their depth of burial. Coal
into a few, mostly three, beds of different quality varies across the basin. In open pit
quality. The seam is approximately subhorizon- mining, the whole seam is occasionally worked.
tal except where it was deformed by postsedi- In some open pit mines, remnant pillars from
mentary tectonism or where it is draped over deep mines are exploited. The average thickness
crystalline or volcanic basement. The seam is of the mined seam varies between 12 and 26 m
best developed at Most and in the western part Q~ between 11 and 20MJ/kg, ash content
of the basin near Chomutov (See Fig. 1). Coal between 7.4 and 39.8 wt% dry and total sulphur
with a higher ash content occurs in the main content between 0.4 and 2.9wt% dry (Pe~ek
seam in the vicinity of Chomutov. The lower 1993).
part of the seam has a higher content of pyrite Coal composition, huminite properties and
and so tends towards a pyritic coal clay. In the degree of gelification of North Bohemian brown
P6tipsy-~Zatec part of the North Bohemian coal coals were extensively studied in the 1960s
basin (Zatec delta), the main seam commonly and 1970s in relation to the coal processing and
splits into a few almost non-mineable leaves. In briquetting (Kurz 1981; Malfin 1962). Higher
the Bilina delta, the main seam is divided into liptinite content in coal increases the hydrogen,
more irregular beds. Sudden splitting, pebbles in carbon and volatile matter contents, heat of com-
coal and an increase in mineral matter content bustion and tar yield (Svoboda 1953; Zelenka
occur near the Kru~n6 Hory fault, (Elznic 1963). 1974) as well as the coal reactivity during
The seam is only rarely fully developed. Some gasification, pyrolysis, combustion, and lique-
parts of the seam, i.e. the highest part in the faction (Hrn6i~ & B~rta 1982; Dehmer 1989;
Most area and the basal part in the Teplice area, Furimsky et al. 1990; Martinez-Tarazona et al.
are uneconomic due to a high mineral content. 1994).
Generally, the main seam has a higher mineral Coal mined in the North Bohemian basin is
content in the south than in the north. The main used for the power industry. Previously, it was
seam, with a lower thickness is also known in used for low temperature pyrolysis to produce
some isolated deltaic lobes in the Doupovsk6 synthetic liquid fuels and gas. The aim of our
Hory and (~esk6 Sffedohofi mountains (Bou~ka work was to evaluate the composition and
et al. 1995). structure of North Bohemian coals. In addition,
Xylodetritic and semidetritic coals prevail in evaluations such as coal extractability, solvent
the North Bohemian coal basin. Less frequent swelling, pore texture, and spectroscopic analy-
are xylitic and detritic coals. The economic coals sis were carried out. Most of the coal samples
are massive, glossy and semiglossy soft coals, were from the main seam of the North
and partly oxyhumolites. Para- and orthotypes, Bohemian basin.

Table 1. Overview of samples and their description

Coal Coal description

Western part
Libou~ clay-like coal with strips of xylite, clearly visible sulphate forms
Nfistup xylitic-detritic coal, brown-black colour, low occurrence of finely dispersed sulphide, partly
weathered, whitish sulphate forms
Central part
Vr~any xylitic-detritic coal without apparent sulphides, isolated strips of clay mineralization
Sverma xylitic-detritic coal without massive and visually observable mineralization of sulphides and
clay minerals
(~SA 92 xylitic-detritic coal, partly clay-like, isolated tiny flat sulphide concretions
CSA 93 xylitic-detritic coal, brown-black colour, without visually observable sulphides
Le~fiky xylitic-detritic coal, brown-black colour, without visually observable sulphides
Bilina xylitic-detritic coal with isolated fusite strips, sulphides in the form of tiny flat concretions and
thin veins
Centrum xylitic-detritic coal without apparent mineralization
Kohinoor xylitic-detritic coal with sparse occurrence of sulphides in the form of flat concretions and tiny
massive fillings of cracks
Eastern part
Chaba~ovice xylitic-detritic coal without apparent mineralization
 NORTH BOHEMIAN COALS 209

Table 2. Technical analysis of North Bohemh~n coals

Coal wt%, dry Volatile Calorific

matter value
Ash Sd Sdo4 Sd Sdo (wt%, d a f ) (MJ/kg)

Liboug 32.9 0.9 0.2 0.4 0.3 51.0 27.5

Nfistup 8.6 1.8 0.5 0.2 1.1 50.5 28.0
Vrgany 15.7 2.5 0.1 1.2 1.2 49.8 28.1
Sverma 15.7 0.9 <0.1 <0.1 0.8 46.8 30.0
CSA 92 21.8 2.4 0.4 0.5 0.6 48.8 29.4
t~SA 93 4.7 0.7 <0.1 <0.1 0.7 55.9 32.1
Le2fiky 19.0 1.7 <0.1 0.8 0.8 49.1 29.0
Bilina 3.4 1.4 <0.1 0.7 0.6 47.9 29.8
Centrum 4.1 0.5 <0.1 <0.1 0.4 50.3 30.1
Kohinoor 8.6 1.5 <0.1 0.5 0.9 48.2 29.9
Chaba~ovice 3.7 0.3 - - - 48.3 28.8

Std, ado4 , S d and Sao denote the total, sulphate, pyritic, and organic sulphur, respectively.

Table 3. Elemental analysis of North Bohem&n coals (wt%, daf)

Coal C H N So O (diff)

Liboug 68.0 5.4 1.4 1.6 23.6

Nfistup 70.2 4.9 1.8 1.2 21.9
Vrgany 67.9 5.4 1.3 1.4 24.1
Sverma 71.5 5.9 1.0 0.9 20.7
(~SA 92 71.1 5.3 0.9 2.0 20.8
(~SA 93 74.6 6.2 1.0 0.9 17.3
Le~fiky 69.9 5.5 1.3 1.1 22.2
Bilina 72.1 5.4 1.0 0.7 20.9
Centrum 72.5 5.6 1.0 0.5 20.4
Kohinoor 71.7 5.6 1.2 1.0 20.6
Chaba~ovice 70.7 5.3 1.1 0.3 22.6

Table 4. Petrographic analysis of North Bohemian coals and characteristics of iron sulphides (%)

Coal R0 H L I MM Microscopic forms of FeS2

FeS2 dispersed clusters inclusions massive

Libou~ 0.33 64 5 1 30 3.1 1.8 1.3 0.0 0.0

Nfistup 0.35 87 4 1 8 2.2 0.8 1.2 0.2 0.0
Vrgany 0.33 78 6 1 15 3.6 1.4 1.9 0.3 0.0
Sverma 0.36 78 7 3 12 0.6 0.2 0.2 0.2 0.0
(~SA 92 0.38 71 6 1 22 0.4 0.4 0.0 0.0 0.0
(~SA 93 0.37 84 13 1 2 0.7 0.2 0.3 0.2 0.0
Le~fiky 0.35 74 5 5 4 0.6 0.2 0.2 0.2 0.0
Bilina 0.36 90 6 1 3 2.0 0.0 0.0 1.0 1.0
Centrum 0.39 86 10 1 3 1.3 0.3 0.7 0.3 0.0
Kohinoor 0.39 83 7 1 9 2.2 1.1 0.5 0.6 0.0
Chaba~ovice 0.37 88 6 1 5 0.3 0.3 0.0 0.0 0.0

R0, light relectance of huminite; H, huminite content; L, liptinite content; I, inertinite content; MM, mineral
matter content.
210 I. SYKOROVA ET AL.

Experimental procedure mines, and eastern part by the coal sample from
the Chaba~ovice mine. An overview of the
Samples samples is given in Table 1.

Samples represented the typical development of

the main seam in the North Bohemian coal
basin. The western part of the seam was Methods of examination of
represented by the coal samples from the the brown coal samples
N~stup and Libou~ mines, central part of the
seam by coal samples from the Vr~any, Sverma, The ash content (Ad), volatile matter (vdaf),
CSA, LO.~iky, Bilina, Centrum, and Kohinoor total sulphur (STY), individual sulphur forms

Fig. 2. Types of macerals in North Bohemian coals: a, ulminite; b, densinite; c, textinite; d, liptodetrinite;
e, inertinite; f, syngenetic pyrite.
 N O R T H B O H E M I A N COALS 211

( sd' Sdso4' Soa), heat of combustion, and bio- 1. crystals and framboids dispersed t h r o u g h
genous elements (C, H, N, S, O) in the organic the coal matter
matter were determined according to national 2. crystals and framboids forming clusters in
standards. the coal matter
Petrographic evaluation of the coal matter 3. microscopic fillings of cellular walls, com-
samples consisted of the determination of partments and microcracks
reflectance of gelified huminite macerals (R0), 4. macroscopic massive grains.
determination of maceral group contents of
huminite, liptinite, and inertinite, and determi- Microscopic and m i c r o p h o t o m e t r i c measure-
nation of the mineral content with emphasis on m e n t of the polished surface of the coal grains
the various forms of iron sulphides. U n d e r the was performed on an U M S P 30 Petro micro-
same conditions as the maceral analysis, the scope-microphotometer (Zeiss-Opton) in oil
syngenetic and epigenetic types of sulphide immersion ( n = 1.518) and in reflected light at
mineralization were determined based on the a wavelength of 546 nm. Total magnification
following four FeS2 classes (Grady 1977; Frankie was 450 • Fluorescence analysis was carried out
& H o w e r 1987; R e n t o n and Bird 1991; H o n 6 k with the same instrumentation using a halogen
1992; S~korovfi & Vodi6kovfi 1992): discharge lamp and an F109 filter set.

Table 5. Maceral composition of huminite (%) and factors of gelification and tissue preservation in North
Bohemian coals

Coal Attrinite Densinite Textinite Ulminite Gelinite Corpo- Huminite Gelification Tissue
huminite index preservation
index

Liboug 6 16 0 38 2 1 64 2.4 1.8

Nfistup 6 36 2 38 4 1 87 4.4 0.9
Vrgany 4 28 4 37 4 1 78 2.7 1.2
Sverma 19 8 2 47 1 1 78 1.1 1.8
CSA 92 9 15 1 46 1 traces 72 2.0 1.9
0SA 93 15 15 traces 48 4 2 84 2.0 1.5
Le~fiky 9 11 2 48 3 1 74 2.0 2.1
Bilina 6 24 2 50 6 2 90 3.7 1.5
Centrum 3 18 1 54 7 3 86 4.8 2.1
Kohinoor 3 21 0 50 8 1 83 3.9 1.6
Chaba~ovice 6 19 3 52 7 1 88 2.6 1.8

Table 6. Pore texture characteristics of the North Bohemian coals (daf bas&)

Coal Vmm Vmicro Smm Smicro Prmm Prmicro

(cm3 "g-l) (cm3 "g-l) (m 2 "g-l) (m 2 "g-l) (%) (%)

Libou~ 0.166 0.072 9.6 260 20.7 9.1

Nhstup 0.092 0.076 3.6 277 11.5 9.5
Vr~any 0.118 0.073 8.3 263 14.1 8.8
Sverma 0.122 0.063 10.8 224 14.4 7.5
~;SA 92 0.170 0.065 10.7 230 18.7 7.1
C;SA 93 0.222 0.051 21.6 180 25.3 5.9
Le~/tky 0.136 0.079 9.5 276 15.9 9.3
Bilina 0.094 0.074 7.8 259 10.7 8.5
Centrum 0.160 0.072 13.3 249 17.0 7.6
Kohinoor 0.105 0.067 11.2 238 11.9 7.6
Chaba~ovice 0.083 0.076 6.3 267 10.2 9.3

Vmm , m e s o - and macropore volume; Vmicro,micropore volume; Smm , m e s o - and macropore

surface; Smi.... micropore surface; Prmm, porosity based on meso- and macropores; Prmicro,
porosity based on micropores.
212 I. SS(KOROVA ET AL.

The apparent density (da), volume (Vmm),and absorptivities (Solomon & Carangelo 1988).
surface area (Smm) of mesopores and macro- 13C CP MAS N M R spectra were measured on a
pores were determined by high-pressure mercury Bruker MSL 200 spectrometer at a frequency of
porosimetry on a Carlo Erba Porosimeter 2000. 50.32MHz and a contact time of 1 ms. The
The volume of micropores (Vmicro) was deter- SP MAS spectra were obtained with a pulse
mined by the Dubinin-Raduskiewic method, delay of 100 s. About 3000 scans were acquired
which is based on a CO2 isotherm measured at to obtain an average spectrum.
25~ (Carlo Erba Sorptomatic 1800). The sur-
face area of micropores (Smicro) was calculated
by the Medek method. The true density (dr) was
calculated from the apparent density by sub- Results and discussion
tracting the pore volume from the total volume.
Coal extractability was examined by using Chemico-technological character&tics
Soxhlet extraction with chloroform, tetrahydro- o f the samples
furan and pyridine at the boiling point of the
respective solvent. Soxhlet extraction with The results of the chemico-technological ana-
methanol was applied after the coal had been lyses are consistent with the data of North
extracted with pyridine to remove pyridine from Bohemian coals obtained by Hub~i6ek (1964)
coal pores. Volumetric coal swelling in toluene, and Malkovsk~ et al. (1985). The composition
tetrahydrofuran and/or pyridine was determined and properties of the coals strongly reflect their
after an equilibration time of seven days. The mineralization, degree of coalification, and
height of dry and/or swollen coal in the tube was petrographic composition.
measured after centrifugation at 3000 rpm for In this work, mineralization of the samples
3 min. Swelling index, i.e. the ratio of swollen to was examined by measuring their ash content,
dry coal volume, was calculated on a daf basis total sulphur, individual sulphur forms, and by
using densities which resulted from porosimetric microscopic evaluation of the pyritic-marcasitic
measurements. Average density of minerals was mineralization. Generally, mineralization in the
considered as 2.3 g/cm 3. North Bohemian coal basin increases from
FTIR spectra of HC1/HF demineralized coals north to south (Malkovsk2~ et al. 1985; Havlena
in a form of KBr pellets were measured on a 1964). Data in Table 2 show that coals with a
Bruker IFS 88 spectrometer. One hundred scans high ash content, between 15.7 and 32.9wt%
were acquired at 2 cm -1 resolution to obtain an occurs in the western (Liboug) and central
average spectrum. Spectral intensity was adjusted (Vr~any, (~SA, Le2~iky) part of the basin. Most
to a sample concentration of 1 mg/cm 2. Quanti- abundant are clay minerals, quartz, and pelosi-
tative evaluation of FTIR spectra was done by derites; carbonates are less frequent (Bou~ka
an assessment of the 3000-2750cm -~ and 900- 1981). Mineral matter is finely dispersed through
700cm -a spectral regions using Solomon's the detrite, fills the cellular tissue compartments,

Fig. 3. Meso- and macropore distribution in the Fig. 4. Meso- and macropore distribution in the
Nfistup coal. Centrum coal.
 NORTH BOHEMIAN COALS 213

or forms distinct bodies. Iron sulphides are calorific value (between 29.0 and 32.1 MJ/kg,
stable mineralization components in the basin. Table 2) and somewhat higher carbon content
Increased total sulphur content up to 2.5 wt% (between 70.7 and 74.6wt%, Table 3). Brown
(Table 2) was found in samples from the western coal metatypes with higher calorific value and
and central parts of the basin. The sulphur carbon content frequently occur in that region,
content was mostly formed by organic (up to particularly at Osek (Zelenka 1973).
1.1 wt%, dry) and pyritic (up to 1.2wt%, dry) The petrographic composition, particularly a
sulphur. The sulphate content was low (below high liptinite content, is a further parameter
0.5 wt%, dry) and it was presumably associated affecting the chemical composition of coal
with the epigenetic oxidation of iron sulphides. (Wolfrum & Wawrzinek 1981). This is well
With respect to the ash content, the more documented by the CSA 93 coal, for which the
coalified coals are in the central part of the highest carbon and hydrogen content, calorific
basin, where the coals exhibited rather a high value and volatile matter content were found.

Fig. 5. Extractability of North Bohemian coals in Fig. 7. Extractability of North Bohemian coals in
chloroform. pyridine.

Fig. 8. Relationship between tetrahydrofuran

Fig. 6. Extractability of North Bohemian coals in extractability and surface of meso- and macropores for
tetrahydrofuran. North Bohemian coals.
214 I. SYKOROV,~ ET AL.

Petrographic characteristics of the samples microcracks and microscopic grains by massive

FeS2 were also classified as syngenetic iron
The samples examined were huminitic coals with sulphides. The macroscopic grains by massive
variable xylite, detrite, and mineral contents. FeS2 (Bilina) were classified as the epigenetic
Huminite reflectance varies from 0.33 to 0.39% type.
corresponding to the brown coal orthotype. Diessel (1986) has introduced two petro-
Huminite concentration varies from 64% to graphic indices, i.e. the gelification index (GI)
90% and is the most abundant maceral group and tissue preservation index (TPI). These
(Table 4). The macerals, ulminite (Fig. 2a) and indices well characterize a coal depositional
densinite (Fig. 2b) contributes to the high environment. In our study, slightly modified
huminite content (Tables 4 and 5), a character- GI and TPI (Kalkreuth et al, 1991; Whateley &
istic of orthotypic brown coals. The concentra- Tuncali 1995) were assessed for North Bohe-
tion ofattrinite and gelinite is substantially lower, mian coals, and they are presented in Table 5.
i.e. 3-19% and 1-8% respectively. Textinite Values of GI and TPI indicate that North
(Fig. 2c) and corpohuminite contents does not Bohemian coals had been developed in a
exceed 4%. Liptinite is formed by waxy and limno-telmatic and/or telmatic environment of
resinous substances. The maceral composition of deposition.
liptinite was determined by a fluorescence mea-
surement. Sporinite and liptodetrinite (Fig. 2d)
predominate particularly in the CSA 93 and Porometric analysis of brown coals
Centrum samples (Table 4). The remaining
liptinite macerals, i.e. cutinite, resinite, exsudati- The results of porometric analysis of the coals
nite, bituminite, suberinite, and fluorinite, are (Table 6) indicate that the values characterizing
accessory.Inertinite (Fig. 2e) is more abundant in the microporous texture, i.e. volume (Vmicro) and
only the Sverma and Le~fiky coals (Table 4), surface area (Smicro), oscillated within a very
where inertodetrinite and macrinite are found in narrow range. It confirms that the microporous
addition to sclerotinite and fusinite. texture is a characteristic of natural coals, in
The results presented in Table 4 indicate that which the microporous phase forms the basis of
the syngenetic pyrite type (Fig. 2f) with typical the coal matrix.
fine grained forms - euhedral crystals and fram- Appreciable differences in the porous texture
b o i d s - predominate in the coals. The crystals were found for meso- and macropores. Their
and framboids can occur dispersed through the maximum volume (Vmm) differs from the mini-
organic as well as inorganic coal matter. More mum value by a factor of three, their maximum
frequently, however, they form clusters which surface area (Smm) is up to sevenfold with
were rather extensive and compact in the coal respect to the minimum value. This indicates
samples from Liboug and Vrgany. The fillings of that different total porosity values, which are
19-31% of the coal volume (Table 6), primarily
mirror differences in the meso- and macropore
distribution. Except the N/tstup coal, the pore
distribution is almost identical for all coals with
25 - Pyridine O

"o 20-
Table 7. CoalswellingindexesJbr North Bohemian coals
0 0
~ 15 Coal Swelling index (daf) in solvent
-~ oC~ 6 ~
~.,
9 10 0 0 Toluene Tetrahydrofuran Pyridine
~- 0
0 Liboug 1.05 1.6 2.8
5- Nfistup 1.07 1.5 2.3
yrgany 1.04 1.8 2.5
uJ 0 I J t t Sverma 1.14 1.8 2.8
0 5 10 15 20 25 I~SA 93 1.19 2.2 3.0
Le2fiky 1.10 1.7 2.6
S u r f a c e of m e s o - a n d m a c r o p o r e s (m2/g daf) Bilina 1.07 1.9 2.6
Centrum 1.10 1.8 2.7
Fig. 9. Relationship between pyridine extractability Kohinoor 1.04 1.9 2.6
and surface of meso- and macropores for North Chaba~ovice 1.15 2.0 3.1
Bohemian coals.
 NORTH BOHEMIAN COALS 215

a maximum in the region of mesopores. The extractability is the Nfistup coal. This coal in all
Nfistup coal has an almost constant relationship cases gave the smallest extraction yield. When
between pore radius and pore volume. Compar- compared with porometric characteristics, the
ison of a typical pore distribution, represented extractability was in a close relationship with a
by the Centrum coal, with the pore distribution surface of meso- and macropores. The relation-
of the Nfistup coal is apparent from Figs 3 & 4. ship is presented in Figs 8 & 9 for tetrahydro-
furan and pyridine extractions. As expected, a
relatively close relationship was also found
Coal extractability between liptinite content and extractability of
coal in either solvent, because liptinite is known
As expected, the extractability of coals increased to consist of easily extractable material.
from chloroform to pyridine. The chloroform
extract accounted for 1.2 to 8.6 wt% daf of the
coal, for tetrahydrofuran and pyridine the Coal swelling
extract yields were found in the range 4.0 to
13.1wt% daf and 8.0 to 25.0wt% daf, respec- Coal swelling is an important investigative tool
tively. As evidenced from the broad yield ranges, into the thermodynamic interactions and physi-
large differences in extractability have been cochemical structure of coal. When simplified,
found between individual coals. Extraction swelling is a measure of the extent of some of the
yields are graphically presented in Figs 5 to 7 intermolecular interactions, which account for
for the respective solvents. The highest differ- crosslinking the coal macromolecular network
ences in extractability between coals were found (Quinga & Larsen 1988). For the North Bohe-
for chloroform. An average extractability was mian coals, extremely high values of coal swelling
found between 2 and 3wt% daf with an were found, especially in pyridine. Coal swel-
exception of the Sverma, (~SA and Centrum ling indexes for the coals are listed in Table 7.
coals. Chloroform mostly extracts highly alipha- It can be supposed that coal swelling has some
tic waxes and resins, whose composition is quite relation to coal extractability. For instance,
different from that of the bulk of coal. Stronger pyridine is known to break hydrogen bonding,
solvents, such as tetrahydrofuran and pyridine, which contributes to coal network crosslinking.
are able to extract compounds which are a part Simultaneously, it can liberate coal clusters
of the coal macromolecular network or can be bonded to the coal network only through
considered as clusters from which the coal hydrogen bonding and extract them from the
network is formed. Consequently, differences coal. It can be seen from Figs 10 & 11 that there
in pyridine extractability seem to be less than is a general tendency for increasing extractabi-
for chloroform, however, the (~SA 93 coal lity with coal swelling. However, the individual
still exhibited exceptionally high pyridine extrac- points are highly spread in the plots and the
tability. Another coal with an exceptional relationships are not good.

15
t~ Tetrahydrofuran 0 25- Pyridine 0
-o 12
20-
o
v
v o 0
"o 15-
"0 Q~ o
0
"~, 6 ~ 10-
o C 0
C o
o 0
o 3 - 5-
X
LU I I
w 0 I I 0
1.0 1.5 2.0 2.5 2.0 2.5 3.0 3.5

Swelling index Swelling index

Fig. 10. Relationship between swelling index Fig. 11. Relationship between swelling index
and tetrahydrofuran extractability for North and tetrahydrofuran extractability for North
Bohemian coals. Bohemian coals.
216 I. SYKOROVA E T AL.

Table 8. Structural parameters of North Bohemian coals derived from FTIR and solid
state 13C NMR

Coal fa,cv fa,SP HaLIR LH,IR faaH (H/C)al

Liboug 0.53 0.16 0.15

Nfistup 0.57 0.72 0.17 0.14 0.19 2.15
Vrgany 0.52 0.68 0.14 0.13 0.19 2.22
Sverma 0.50 0.14 0.14
(2SA 93 0.51 0.61 0.14 0.14 0.23 2.02
Le~iky 0.57 0.65 0.17 0.16 0.25 1.95
Bilina 0.55 0.70 0.17 0.15 0.21 2.18
Cen trum 0.50 0.68 0.14 0.13 0.19 2.24
Kohinoor 0.54 0.14 0.13
Chaba~ovice 0.58 0.69 0.16 0.14 0.20 2.13

fd, carbon aromaticity; Har, hydrogen aromaticity; fa,H, ratio of hydrogen bearing
aromatic carbon to total carbon; faaH, ratio of hydrogen bearing aromatic carbon to
aromatic carbon; (H/C)ab atomic H/C ratio in aliphatic structures.

Spectroscopic characteristics occur in the western and central parts of the

basin. The eastern part of the basin is character-
Quantitative spectroscopic characterization of ized by low sulphur content. Main organic
coal is rather a difficult task. It is a consequence components are formed by macerals of huminite
of a high heterogeneity of coal and its multi- and liptinite groups, of which ulminite, densinite
component nature. An attempt was made to and liptodetrinite occur most frequently.
assess some basic structural parameters of North Pore texture analysis of the coals showed very
Bohemian coals by FTIR and solid state 13C little differences in the range of micropores.
NMR spectroscopy. The latter was performed However, substantial differences were found in
by using the cross-polarization (CP) as well as the range of meso- and macropores. These
single pulse (SP) techniques. It should be noted differences and/or content of liptinite largely
that the 13C CP MAS NMR discriminates affect the extractability of the North Bohemian
against aromatic carbon in coals and the SP coals. The coals also exhibit extremely high
technique is often recommended instead. How- swelling ratios in basic solvents, such as pyridine.
ever, the SP technique is time-consuming and
acquisition of one coal spectrum can take over Authors gratefully acknowledge the financial support
24 hours. of the Grant Agency of Czech Republic (Grant No.
Quantitative FTIR spectroscopy deals with 104/94/1791) and the Grant Agency of Czech Acad-
problems of average absorptivities of CH bonds, emy of Sciences (Grant No. 246101 and 3046607).
especially aliphatic (Cern~ 1995). So, aromatic
hydrogen concentration was only evaluated
from FTIR spectra. Some structural parameters
derived from FTIR and solid state NMR spectra References
of North Bohemian coals are presented in
BOUgKA, V. 1981. Geochemistry of Coal, Elsevier,
Table 8. The values of fa and Hat parameters Amsterdam.
were directly obtained from the NMR and FTIR , PEgEK, J. et al. 1995. Mineralizace uheln~,ch sloji.
spectra, respectively. Other structural para- Report for Ministry of Environment, Prague.
meters were derived by using simple equations (~ERNV, J. 1995. Structural dependence of CH bond
without any assumption dealing with coal absorptivities in FTIR spectra of fossil fuels.
structure (Cern~ & Pavlikovfi 1995). Abstracts of the lOth Spectroscopic Conference,
Lanskroun, Czech Republic, p. M1-P-8.
- - & PAVLiKOVA, H. 1994. Structural Analysis of
Low-Rank-Coal Extracts and Their Relation to
Conclusion Parent Coals. Energy & Fuels, 8, 375-379.
- - & 1995. Quantitative solid state NMR and
The overall composition and properties of FTIR spectroscopy of low rank coals and
North Bohemian coals depend slightly on their reliability of structural parameters. In: PAJARES,
geological position in the basin. The analyzed J.A. & TASCON, J. M. D. (eds) Coal Science,
coals were orthotype brown coals. Higher Vol. 1, Proceedings of the 8th International
ranked coals were found in the central part of Conference on Coal Science, Oviedo, Spain.
the basin. Some coals with a higher ash content Coal Science and Technology, 24, 111-114.
 N O R T H B O H E M I A N COALS 217

DEHMER, J. 1989. Petrographical and organic geo- MALKOVSK~-, M. 1985. Geologie severo(esk~ hnddou-
chemical investigation of the Oberpfalz brown helnO pdmve a jeff okoli. Ust~edni Ust~av Geolo-
coal deposit, West Germany. International Jour- gick~, Praha.
nal of Coal Geology, 11, 273-290. MARTiNEZ-TARAZONA,M. R., MARTiNEZ-ALONSO,A.
DIESSEL, C. F. K. t986. The correlation between coal & TASCON, J. M. D. 1994. Characterization
facies and depositional environments. In: of common lignite, xylitic lignite and pyropis-
Advances in the Study of the Sydney Basin, site varieties of low-rank coals. Fuel, 73, 11,
Proceedings of 20th Symposium, University of 1723-1728.
Newcastle, 19-22. PEgEK, J., KOULA, J. et al. 1993. Refiln6 vyt~!teln6
ELZN1C, A. 1963. Severozfipadni omezeni chomu- z~isoby uhli v otev~en2~ch dolech v Cesk+
tovsko-mostecko-teplick6 pfinve. Reports of the Republice.(~ist II. Hn~d~ uhli. Uhll, Rudy, 2,
Central Geological Institute, 38, 245-251. 337-345.
FRANKIE, K. A. & HOWER, J. C. 1987. Variation in QUINGA, E. M. Y. & LARSEN, J. W. 1988. Solvent
pyrite size, form and microlithotype association in Swelling of Coals. In: Y~3RI3M, Y. (ed.) New
the Springfield (No. 9) and Herrin (No. 11) coals. Trends in Coal Science. Kluwer, Dordrecht,
Western Kentucky. International Journal of Coal 85-116.
Geology, 7, 349-364. RENTON, J. J. & BraD, D. S. 1991. Association of coal
FURIMSKY, E., PALMER, A. D. et al. 1990. Prediction macerals, sulphur, sulphur species and the iron
of coal reactivity during combustion and gasifica- disulphide minerals in the three columns of the
tion by using petrographic data. Fuel Processing Pittsburgh coal. International Journal of Coal
Technology, 25, 135-151. Geology, 17, 21-50.
GRADY, W. C. 1977. Microscopic varieties of pyrite in SOLOMON, P. R. & CARAYGELO, R. M. 1988. FTIR
West Virginia coals. Society of Mining Engineers, analysis of coal. 2. Aliphatic and Aromatic
AIME, 262, 268-274. Hydrogen Concentration. Fuel, 67, 949-959.
HAVLENA, V. 1964. Geologie uhelnf:ch lo3isek. 2. SVOBODA, J. V. 1953. Geologicko-petrografickdt studie
CSAV, Praha, 293-353. v hnddouheln~ oblasti komo(anskd. CSAV, Geo-
HON~K J. 1992. Fe-disulphides in the brown coal of technica, Praha, 17, 1-63.
the North Bohemian brown coal basin. Aeta SYKOROVA, I. & VODICKOV.h,,A. 1992. Microscopical
Montana, Praha, 86, 45-49. forms of Fe disulphides. Acta Montana, Praha,
HRN~il~, J. & BARTA, V. 1982. Macerfily skupiny 85, 93-104.
exinitu (liptinity)- vlastnosti, fluorescen6ni mik- WHATELEY, M. K. G. & TUNCALI, E. 1995. Origin
roskopie, chemickfi struktura a vztah ke zkapal- and distribution of sulphur in the Neogene
fiovfini. Hnddd uhli, 4, 31-38. Beypazari Lignite Basin, Central Anatolia,
HUaA~EK, J. 1964. Pasportizace a klasifikace hn6d~ch Turkey. In: WHATELEY, M. K. G. & SPEARS,
uhli (~SSR a jejich popelfi. Pr6ce (?stavu pro D. A. (eds), European Coal Geology. Geological
vfzkum a vyu3itl paliv, 9, 3-138. Society, London, Special Publications, 82,
KALKREUTH, W., KOTIS, T. et al. 1991. The geology 307-320.
and coal petrology of a Miocene lignite profile at WOLFRUM, E. & WAWRZINEK, J. 1981. Beziehungen
Meliadi Mine, Katerini, Greece. International zwischen petrographischen und chemischen
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KURZ, R. 1981. Eigenschaften der rheinischen Braun- kohle-Hefte, 11, 381-386.
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off. Fortschritte in der Geologic yon Rheinland und stupn6 prouheln~ni severo6esk6 hn~douheln6
Westfalen. Krefeld, 29, 381-425. pfinve. Uhli, 22, 59-63.
MAL~,N, O. 1962. Die Entwicklung der optischen 1974. Vliv voskfi a pryskyfic na chemicko-
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 Aliphatic biological markers in Miocene
Maritza-Iztok lignite, Bulgaria

MAYA STEFANOVA 1 & CAROLINE MAGNIER 2

l Inst. Org. Chem. Bulg. Acad. Sci. Acad. G. Bonchev str. bl. 9 Sofia 1113, Bulgaria
2 Inst. Francais du P~trole, 1 & 4, Av. de Bois-Pr~au, 92506 Rueil-Malmaison, France

Abstract: Chromatographic separation and mass spectral studies of bitumens extracted from
lithotypes (humovitrain, xylain, liptain and humoclarain) from the Miocene Maritza-Iztok
lignite reveal the following: (1) A preponderance of the c~-phyllocladane skeleton over the
pimaranes/abietanes. The variety of tricyclic diterpanes confirms that the generation biota
included gymnosperms; (2) The presence of dicotyledonous angiospermaes in the generation
biota is indicated by the occurrence of widely distributed des-A-lupane structure; (3) The
dominance of terpanes over steranes confirms the prevailing contribution of terrigenous
input; (4) The preponderance of C27f~hopane and the presence of/3/3 hopanes indicates a low
degree of thermal maturation.

The early to mid-Miocene 'Maritza-Iztok' lignite Experimental methods

is located in southeastern Bulgaria (see Fig. 1 in
Si~kov, this volume for location). It is described Ultimate and proximate analyses of the samples
as having the following maceral composition: under study are summarized in Table 1. The
92% huminite, 6% liptinite and 2% inertinite maceral composition of the lithotypes has been
(5]i~kov 1988). The basin is included in the 'A described in our previous study of the products
sub-group' of the petrological classification of after Nail treatment of the lithotypes (Velinova
Neogene deposits (Si~kov & Andreev 1987) et al. 1993; Stefanova et al. 1996).
characterized by an almost equal contribution Bitumens were exhaustively extracted by
to coal formation by gymnosperm and angio- CHC13 (1:10) and separated into aliphatic and
sperm plants with a slight dominance of aromatic portions by column chromatography
angiosperms. The vitrinite reflectance (R0) of using an analytical glass column (100 • 5 mm) dry
the lignite is 0.18 +0.02% (Si~kov et al. 1986). packed with silica gel (Davison, 100-200 mesh)
This study is of the humovitrain (I), xylain and previously washed with methylene chloride
(II), liptain (III) and humoclarain (IV) lithotypes (CH2C12). The adsorbent was activated for
and involves the acquisition of information 16 hours at 180~ Bitumen was dissolved in a
concerning the molecular composition of the minimum of CH2C12 and placed at the top of
aliphatic portions of the extracted bitumen. This the column. The sample was eluted with CH2C12
allows the possible plant precursors to the lignite (fraction 1), and MeOH/CHCI3/H20 (25:60:4 v/v)
organic matter to be determined. (fraction 2). The first fraction was subjected to

Table 1. Proximate and ultimate analysis of lithotypes

Characteristics I II III IV

Proximate analysis (wt%)

Moisture 16.0 9.2 6.9 16.9
Ash (db) 9.2 3.6 3.0 22.6
VM (daf) 52.8 58.5 68.1 60.5
Ultimate analysis (wt% daf)
C 65.8 67.3 72.1 65.1
H 5.5 6.1 7.2 6.5
N 1.0 0.9 0.8 1.6
S 4.0 3.3 3.4 3.8
Odi~ 23.7 22.4 16.5 23.0

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 219-228.
220 M. STEFANOVA & C. MAGNIER

thin layer chromatography (TLC) separation lithotypes. The highest bitumen content is in
for isolation of the paraffinic/naphthenic com- liptain (39wt%) with 2.34wt% saturates com-
pounds. TLC plates were developed with posed of branched/cyclic alkanes. As the content
CH2C12. Berberine sulphate (Fluka) in methanol of linear alkanes is low the total extract from the
was applied as a spraying reagent to make the liptain sample was not adducted.
bands visible in day light. The hydrocarbon Figure 1 shows the GC separations of
fraction was separated to branched/cyclic and extracted bitumens. The high peak of ct-phyllo-
normal alkane sub-fractions by molecular sieve cladane eluted by n-C20 alkane is recognized in
adduction (5A). Total hydrocarbon fractions all samples. Distribution curves for the homo-
and branched/cyclic alkane sub-fractions were geneous lithotypes, humovitrain (I) and xylain
characterized by gas chromatography (GC) and (II) are smooth and calculated carbon preference
by gas chromatography-mass spectrometry index (CPI) values are close to unity. A similar
(GC-MS). pattern of alkane distribution was determined by
GC analyses were conducted using a Varian Markova et al. (1993) for lithotypes from the
3600 instrument and a DB1 capillary column same deposit, n-alkane distributions without a
(30 m, 0 0.32 mm, 0.1 #m film thickness). The
program consisted of 50~176 at 10~
110~176 at 3~ rain, and isothermal hold for
20min. Samples were introduced with an on- 28
column injector heated from 50-300 ~ at 20~ a) 26
The detector was operated at 300~ and the 3O
data were acquired by a Hewlett Packard 1000 26
integrator. G C - M S analyses were conducted
using a Hewlett-Packard 5890 gas chromato- 22
graph coupled to a VG70-250SE mass spectro-
meter. Scans were acquired over the mass range 20
of 60-550da. Mass spectra were corrected for
background by subtraction. A DB-5 (30m,
,,[1
0.25mm, film thickness 0.5#m) fused silica
capillary column was used. GC conditions were:
column program 50~176 at 3~ flow rate
1 ml/min, splitless for first 80 s.

R e s u l t s and discussion
-r-
Table 2 summarizes the contents and composi-
tions of the extracted bitumens from different

Table 2. Characteristics of the bitumens from lignite

lithotypes c~
Content Lithotype 27
(wt%)
I II III IV 2325 ]2i31
Yield of bitumen 1.1 10.3 39.0 8.9
Saturates 0.06 0.29 2.34 0.38
Branched/cyclic
alkanes
* 50.3 54.9 98.0 53.8
** 0.03 0.16 2.29 0.20
PhyUocladane
* 1.10 1 5 . 0 37.10 2.76 TIME
** 0.0003 0.024 0.847 0.006
Fig. 1. Gas chromatograms of the total bitumen
* wt% from the sample subjected to separation; fractions of lithotypes (a) humovitrain; (b) xylain; (e)
**wt% from initial lignite lithotype; Lithotype I, humoclarain; (numbers over peaks refer to carbon
humovitrain; II, xylain; III, liptain; IV, humoclarain. numbers of n-alkanes).
 BIOLOGICAL M A R K E R S IN M I O C E N E LIGNITE 221

well m a r k e d odd/even p r e d o m i n a n c e have been registered, CPI = 1.6 (Table 3). The abundance
attributed to bacterial lipids (Chaffee et al. of t/-C25, n-C27, and rt-C26 is high and the
1986), while Disner & H a r o u n a (1994) assumed m a x i m u m is at n-C2s homologue, and is typical
that such patterns represent a signature of the for a contribution of epicuticular waxes from
contribution of non-flowering plants to coal higher plants (Chaffee et al. 1986; W a n g &
formation. Simoneit 1990).
In the heterogeneous lithotype, humoclarain, G C separations of the branched/cyclic alkanes
a preponderance of the o d d homologues is are d o m i n a t e d by o~-phyllocladane (Fig. 2, peak 3,

Table 3. Maturity parameters

Parameter Lithotype

I II III IV

CPI* 0.99 0.97 - 1.65

Pr/Ph 0.33 1.12 0.50 0.51
'bio'/N 'geo' hopanes ** 1.13 0.44 - 1.05
C279/, 6.43 3.02 - 6.60
Tm/Ts 2.86 1.71 - 3.67
C29~o~/o~/~ 1.41 0.66 -- 1.20
C3~c~/3[S/(S + R)] 0.17 0.53 - 0.20

* CPI = E % odd alkanes/E % even alkanes;

** E C29-C31/~/~/~ C29-C310!/~.
See Table 2 for Lithotypes.

- j
I~,3
a] ' c) ~,! i
!fl

I
ILl
I
t~
Z
C~ ~ E~s~b9
0
O-
f 800 i000 1200 i
t~
l.tJ
er"

~O0 600 900 zOO:) Z600 20O0 2200 Z~O0 2s~o 3OCO -~ZCO_.JOmO
~ 600 iO0 zOO0 1.200 Z4O0 ~6 0 ~ aO 2000 ~
22C0 ~ O0 2600 2SOO .~000 3~00

lad

bl d]
l--

n~

6111
oo s Boo 1000 !200 1400 160~i 1800 2000 2200 2r 2~E.O2~3~ ~2CC . : o 560 ~00 . ~1000
.~_~ _ L ~14CO _
Z200 ~ _ -ZSO0
ZeO0 - ~ ' . .ZOO0
- ~ - - k2ZOO
~ , 2400 Z600
_ 2~00 ~00~."~:o"

--- SCAN

Fig. 2. Total ion currance (TIC) of the branched/cyclic alkanes (a) humovitrain; (b) xylain; (e) liptain; (d)
humoclarain; (numbers over peaks refer to Table 4). Pr, pristane; Ph, phytane.
 Table 4. Compounds' identified by mass spectrometry in hydrocarbon fractions
Peak Composition Compound designation M+ Base peak Structure*

1 C19H34 norpimarane 262 233 I

2 C2oH32 isophyllocladene 272 120 II
3 C2oH34 c~-phyllocladane 274 123 III
4 C24H42 Des-A-lupane 330 123 IV
5 C27H46 17fl(H)-22,29,30-trisnorhopaane 370 149 V
6 C20H34 dihydrorimuene 274 259 VI
7 C15H26 methyl, perhydro-phenanthrene 206 191 VII
8 C]5H26 cedrane 206 82 VIII
9 C19H28 18-norabiatane-18,11,13-triene 256 241 IX
l0 C2oH32 AS'l~ 272 257 X
11 C19H34 fichtelite 262 109 XI
12 C2oH36 sandracopimarane 276 247 XII
13 C2oH34 #-phyllocladane 274 123
14 C2oH32 sandaracopimaradiene 272 257 XIII
15 C2oH34 ent-beyerane 274 123 XIV

* structures in Fig. 5.

12

Ph
i
! -
'56o 5gr 660 6~o 760 7So s6o 830 960 9g0 logo loso 111o?"11'50 1~oo

I o)
g_

21

t
ILl
22
o 23

i,
Z
o 19 N
I:l.. (' 22 o _B26
20 , 23 : 27 ";C19 I
I/1
ILl I : / I101/+ 1.
I

ll:
b0 ' " ~o'ob ' iz'o6 i4o6 " " i6'oo " t,'0o 2o'o5' ~2'ob ' ,, ~ o q

o22
iJ_l
>
21 123 b)

I,-

..,J
26
i,a_l
re"
~_ 19 22! 25 ~

I //
, 2
./'\ 6
12
11//'~,\ 13
~. ./\ .,,- ..... .

[L
.... 5~0 ' ' looo 15oc " 2~,'o~ 25co
" 3cac

SCAN
-- SCAN

Fig. 3. Mass fragmentograms m/z 183 of branched/ Fig. 4. TIC of tri/tetracyclic diterpanes (a)
cyclic alkanes (a) xylain; (b) humoclarain; 9 iso- humovitrain; (b) xylain; (e) liptain (numbers over
alkane; 0 , anteiso-alkane; Sq, squalane. peaks refer to Table 4).
 BIOLOGICAL M A R K E R S IN M I O C E N E LIGNITE 223

I. n o r p i m a r a n e II.imophyllocladene III.o-phyllocladane IV. D e m - A - l u p a n e

Me

V. 1 7 F ~ H ) - 2 2 , 29, 3 0 - VI. D i h y d r o r i m u e n e VII. M e t h y l , P e r h y d r o - VIII. C e d r a n e

Tri s n o r h o p a n e phenanthr ene

IX. 1 8 - N o r a b i a t a n e - X. A~'IO-rimuene XI. F i c h t e l i t e XII. Eandara-

8, 1 1 , 1 3 - t r i e n e coplm~rane

XIII. S a n d a r a c o p i mar a d i e n e X I V. e n t - B e y e r a n e XV. C - T r i c y c l i c

-- 23triterpane

XVI.C24 17, 2 1 - s e c o - X V I I 91 7 ~ ( H ) - 2 2 , ~ g , 3 0 - X V I I I . 18~x(H) -P2p 2 9 , 3 0 -

hopane trisnorhopane, C27 t r isnor neohopane, C27

EI X. 1 7 o ( H), 21 ~ H) - XX. 17F)( H ) , 21 ~ ( H ) - X X I . 1 7 t ? ( H ) p 21 ~ ( H ) -

Fx)mohopane. Csl homo~or et ane, C31 '~'-' h o . . , ~ h o p a n e , C31 t?~:

Fig. 5. Chemical structures cited.

224 M. STEFANOVA & C. MAGNIER

o)
E27

tlJ
I.,"I
Z
o

uq
u/

I,i C2~
12
>
C29 311~

_.J
,~i ~ ~,~, L%~, ~~
ILl

660 860 1000 1200 1400 1'60'0''i'80,0 2000 2200 2400 2600 28~00 3000 32100

t
ILl
b)

Z
o
a.
u~

1,1.,I
>

l,,,-

._J

r~
[27

I
10'00 12'00 1400 1600 1800 2000 2200 2400 2600 2800

S C A N -----
 BIOLOGICAL MARKERS IN MIOCENE LIGNITE 225

C2 7 c)

Vl
Z
0
IX.

n-

c29~k
L~
>

._J

SCAN
Fig. 6. Mass fragmentograms m/z 191, key ion for tricyclic terpanes, 17,21-secohopanes, pentacyclic triterpanes
(numbers over peaks refer to Table 4). O, tricyclic terpanes; O, 17,21-secohopanes; - - , 'geo' hopanes;
'bio' hopanes; (a) humovitrain; (b) xylain; (c) humoclarain.

Table 4, Str.III), already mentioned for the Fig. 4a, c, peak 6, Str.VI) and rimuene (Fig. 2c,
separations of the total extracts. ~-Phyllocla- Fig. 4b, peak 10, Str.X).
dane is less common in humovitrain than in Abietane structures are represented by fichte-
liptain in which it reaches 0.85 wt% of lithotype lite (Fig. 2c, d and Fig. 4a, b, c, peak 11, Str.XI)
(Table 2). and 18-norabiatane-18,11,13-triene (Fig. 2c,
Traces from n-C16 to n-Cl8 alkanes occur in peak 9, Str.IX).
the sample of non-adducted liptain (Fig. 2c). The preponderance of phyllocladane skeleton
Homologues are accompanied by the isopre- is obvious in all samples. Noble et al. (1986), in
noids pristane and phytane. These also occur in their study of tetracyclic diterpanes with ent-
xylain and humoclarain samples where iso- and beyerane, phyllocladane and e n t - k a u r a n e struc-
anteiso-alkanes are indicated (Fig.3). tures, noted that the ratios of C-16 epimers were
Figure 4 illustrates the regions of tri/tetra- dependent on maturity. Phyllocladane is a
cyclic diterpanes. The mass spectral identifica- common constituent in low rank coals and is
tions are based on published spectra (Philp, thought to be derived from phyllocladene
1985). In Table 4 some of the proposed struc- (Str.II) which is a component in a number of
tures, illustrated in Fig. 5, are gathered. conifers (ten Haven et al. 1992). Phyllocladane is
The pimarane/abietane structures are tenta- well studied and correlated with maturity by
tively assigned with a prevalence of pimarane Simoneit (1977), Alexander et al. (1987), Hazai
compounds: norpimarane (Fig. 2, and Fig. 4, et al. (1988), Hazai & Alexander (1991), Ten
peak 1, Str.I); sandaracopimarane (Fig. 2c, d, Haven et al. (1992), Disnar & Harouva (1994).
Fig. 4a, c, peak 12, Str.XII); and unsaturated The relative quantity of the thermodynami-
homologues, i.e. sandaracopimaradiene (Fig. 4b, cally preferred /3-phyllocladane increases with
peak 14, Str.XIII), dihydro-rimuene (Fig. 2b, thermal maturity. It is registered in negligible
226 M. STEFANOVA & C. MAGNIER

quantities compared to the a-partner (Fig. 2c, Calculated values for Pr/Ph, C27~/c~and C29flc~/c~/3
Fig. 4a, c, peak 13). Ent-beyerane (Fig. 4c, peak in the case of humovitrain and humoclarain
15, Str.XIV) coelutes with pimarane and con- are similar but those for xylain differ noticeably,
tributes to the creation of the asymmetric peak. moreover the content of hopanes in xylain is
Its retention time is a bit less than the value for
negligible compared with to the other two
pimarane. The overlapping of the two com- lithotypes.
pounds is obvious in Fig. 4c. In humovitrain, xylain and humoclarain a
The liptain sample contains a relatively large significant quantity of Des-A-lupane (peak 4,
amount of cedrane (Fig. 2c, peak 8, Str.VIII). Fig. 2 and Fig. 6, Str.IV) is determined. This
This sesquiterpenoid was found in the fossil sesterterpenoid is considered to be a photo-
resin retinellite, and in a montan wax by chemical or photomimetric degradation product
Grantham & Douglas (1980). The occurrence of certain 3-oxygenated triterpenoid precursors
of cedrane suggests that the liptain was origin- from higher plants (Wang & Simoneit 1990;
ally derived from plants of the family Cupressa- Stout 1992). Des-A-lupane accompanied by an
ceae (order Coniferale). unknown series of C24H40 species, was recorded
Mass fragrnentograms m/z 191, key ion for by the above cited authors in extracts from
tricyclic diterpanes and triterpanes reveal the Tertiary coal. Its occurrence indicates input of
following distributions of series (Fig. 6): material from higher (particularly dicotyledo-
nous) plants.
9 tricyclic terpane (Str.XV), C22-C26 , with a Coals with high proportions of terrestrial
maximum content of C23 homologue; input contain low quantities of steranes (Aref'ev
9 tetracyclic terpanes (17,21-secohopanes) et al. 1992). The m/z217 fragmentograms
(Str.XVI), C22-C24; and produced in this study do not indicate the
9 hopanes (Str.XVII-XXI), C27-C 31; occurrence of steranes.
The comparative study of the aliphatic com-
Triterpanes were not registered in the liptain pounds in the Maritza-Iztok lignite lithotypes
bitumen sample, which is a peculiarity of the reveals some peculiarities of their biomarker
lithotype. assemblage. A considerable difference was regis-
Pentacyclic triterpanes are indicated in the tered in the amount of extractable bitumens, the
m/z 191 fragmentograms (Fig. 6). Calculated highest content was determined for liptain, where
maturity parameters are shown in Table 3. All it reached 40% and the lowest- for humo-
distributions are dominated by C27/3 hopane, vitrain, as low as 1.1%. The values determined
trisnorhopane (Fig. 2, peak 5, Str.V). The ratios for xylain and humoclarain are comparable. A
C27/3/a are >>1, an indication that C27 hopa- similar relationship was recognized for the
noids are represented predominantly by the contents of saturates.
biologically synthesized constituent. C29/3/3 The GC separations of all branch/cyclic
hopanoid is the most abundant species, accom- alkane portions were dominated by the highly
panied by the converted C29/3a isomer. Calcu- expressed contents of a-phyllocladane and
lated moretane/hopane ratios (C29/3a/a/3) are amounted 0.85 wt% in the case of liptain. A pre-
higher in the humovitrain and humoclarain ponderance of the a-phyllocladane skeleton over
samples and half as great in the xylain sample. pimaranes/and abietanes was registered for all
Hopanes are divided into 'bio'- and 'geo'- samples. The variety of tricyclic diterpanes
hopanes. Biohopanes have /3/3 stereochemistry. indicated that the generation biota included
Increased maturity leads to the transformation gymnosperms. The presence of cedrane in liptain
of these to the more thermodynamically stable bitumen was an additional proof for the family
a/3 configuration of geohopanes (Tissot & Cupressaceae (order Coniferales).
Welte, 1984, Ourisson et al. 1987, Aref'ev et Our results have shown that n-alkanes dis-
al. 1992, Peters & Moldowan 1993) allowing the tribution depended on the type of lithotype. In
stereochemistry of hopanes to serve as an the case of the homogeneous lithotypes, humo-
indicator of degree of maturation. The values vitrain and xylain, the CPI was close to 1.0 and
higher than unity calculated for the ratios could be explained by bacterial lipids or non-
E 'bio'/E 'geo' hopanes in the case of humovi- flowering plants contributions. For the hetero-
train and humoclarain, supported by the high geneous lithotype, humoclarain, a preponder-
values for Tm/Tsand C31a/3[S/(S + R)] ratios are ance of odd homologues was registered. The
taken as an unequivocal indication of a low other maturity parameters were closer for
degree of geochemical transformation. Certain humovitrain and humoclarain, while according
differences among the hopane distribution are to them xylain could be described as being at a
reflected in the maturity parameters (Table 3). higher level of geochemical transformation.
 BIOLOGICAL MARKERS IN MIOCENE LIGNITE 227

A lack of hopanes was registered for the DISNAR, J. R. & HAROUNA,M. 1994. Biological origin
liptain bitumen. In the other lithotypes the of tetracyclic diterpanes, n-alkanes and other
hopane pattern of distribution is similar, deter- biomarkers found in Lower Carboniferous Gond-
mined by the dominance of C27~ hopane and wana coals (Niger). Organic Geochemistry, 21,
143-152.
relatively high contents of/3/3 a n d / 3 a isomers.
GRANTHAN, P. J. & DOUGLAS,A. G. 1980. The nature
The prevalence of hopanes with <30 carbon and origin of sesquiterpenoids in some Tertiary
atoms suggests C30-diploterol-like structures as fossil resins. Geochimica et Cosmochimica Acta,
a potential precursor of hopanes. 44, 1801-1810.
Des-A-lupane was detected in all lithotypes, HAZAI, I. • ALEXANDER, G. 1991. Occurrence and
and may represent equivocal evidence for transformation of tricyclic aromatic hydrocar-
the input of angiospermous organic matter bons in low rank coals. Fuel, 70, 971-978.
in lignite formation. The presence of 17,21- , ESSIGER, B. & SZEKELY, f. 1988.
secohopanes is supplementary proof for a identification of aliphatic biological markers in
brown coals. Fuel, 67, 973-982.
terrestrial contribution.
MARKOVA, K., STOYANOVA, G. & PEEVA, N. 1993.
The presence of tricyclic triterpanes, C22-C25, Study of the effect of autoxidation processes on
is an indication for microbial activity. Tricyclics alkanes from low rank coal. Oxidation Commu-
appear to be more stable thermally than penta- nication, 16, 289 298.
cyclic triterpanes. Thus with increasing maturity NOBLE, R. A., ALEXANDER,R., KAGI, R. I. & KNOX,J.
the ratio of tri- to pentacyclic can be expected to 1986. Identification of some diterpenoid hydro-
rise (Waples & Machihara 1991). The lithotypes carbons in petroleum. Organic Geochemistry, 10,
studied are at a low degree of maturation 825-829.
consistent with the negligible content of tricyclics OURISSON,G., ALBRECHT,P. & ROHMER,M. 1987. The
hopanoids. Pure & Applied Chemistry, 51,709-729.
compared with pentacyclic triterpanes.
PETERS, K. E. & MOLDOWAN,J. M. 1993. Terpanes.
In: The Biomarker guide to interpreting molecular
.fossils in petroleum and ancient sediments.
Conclusions Prentice-Hall, Inc. Englewood Cliffs, New Jersey,
142-264.
The aliphatic biomarker compositions of homo-
PHILP, R. P. 1985. Diterpenoid hydrocarbons. In:
geneous and heterogeneous lithotypes of the Fossil fuel biomarkers. Applications and spectra.
'Maritza-Iztock' lignite were studied by chroma- Elsevier, Amsterdam, 133-153.
tographic and spectral methods. Some of the SIMONErT, B. R. T. 1977. Diterpenoid compounds and
identified compounds confirm the previously other lipids in deep-sea sediments and their
described peculiarities of this deposit (Si~kov geochemical significance. Geochimica et Cosmo-
1988). Resinites derived from conifers are chimica Acta, 41,463-476.
frequently easily recognized in lignite by micro- SIgKOV, G. 1988. Taxonomic composition of coal-
scopic techniques. Our results confirm that forest forming plants. In: Theoretical fundaments of
biochemical coalification. University Press, Sofia,
and sedge-grass populations took part in the
29-35 (in Bulgarian).
formation of the lignite and indicate aspects of -- & ANDREEV, A. P. 1987. A way to reconstruct
the chemical composition of the plant debris. coal-forming paleoplant communities based on the
Aliphatic compounds, with precursors gymno- micropetrographic composition of Bulgarian neo-
sperms and angiosperms were detected in differ- gene coals. Compt. rend Acad. Bulg. Sci., 40, 77-80.
ent proportions depending on the lithotype. --, KEHAJOVA, M. & STAJKOVA, S. 1986. Brief
geological description of coal deposits in Bul-
garia. In: Coals and coal deposits in Bulgaria. A
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ALEXANDER, G., HAZAI, I., GRIMALT, J. O. & STEFANOVA, M., MAGNIER, C. & VELINOVA,D. 1995.
ALBAIGES, J. 1987. Occurrence and transforma- Biomarker assemblage of some Miocene-aged
tion of phyllocladane in brown coal from Nograd Bulgarian lignite lithotypes. Organic Geochemis-
Basin. Hungary. Geochimica et Cosmochimica try, 23, 1067-1084.
Acta, 51, 2065-2073. STOUT, S. 1992. AIiphatic and aromatic triterpenoid
AREF'EV, O. A., ZABRODINA,M. N., GULJAEVA,N. D. hydrocarbons in a Tertiary angiospermous lignite.
& PETROV, A1.A. 1992. Policiklicheskie biomar- Organic Geochemistry, 18, 51-66.
keri tverdich kaustobiolitov. Khimia tverdogo TEN HAVEN, H. L., LITTKE, R. & RULLKOTTER, J.
topliva, Bdd 1, 12-35. 1992. Hydrocarbon biological markers in Carbo-
CHAFFEE, A. L., HOOVER, D. S., JOHNS, R. B. & niferous coals of different maturities. In: MOLDO-
SCHWEIGHARDT, F. K. 1986. Biological markers WAN, J. M., ALBRECHT,P. & PnluP, R. P. (eds)
extractable from coal. In: JOHNS, R. B. (ed.) Biological Markers in Sediments and Petroleum.
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Elsevier, Amsterdam, 311-347. 142-155.
228 M. STEFANOVA & C. MAGNIER

TtssoT, B. P. & WELTE, D. 1984. Petroleum Formation brown coal in the Zhoujing mine Baise Basin,
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VELINOVA, D., LAZAROV,L. • ANGELOVA,G. 1993. significance. Fuel, 69, 12-20.
N.M.R. investigation of low-rank coal lithotypes WAPLES, D. W. & MACHIHARA,T. 1991. Biomarkers
pretreated with Nail. Fuel, 72, 991-996. as organic-facies indicators. In: Biomarkers for
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 Floristic characters of the upper coal-bearing formation
in the Transcarpathians

SVETILANA SYABRYAJ

Institute of Geological Sciences NASU, Chkalova srt. 55b, 252054 Kiev, Ukraine

Abstract: The results of palynological studies of samples from outcrops, boreholes and
mines in the Transcarpathians are presented. Megafloral remains from the Ilnitsa suite show
the age of the upper coal-bearing formation to be Romanian. The palynological analysis
allows the reconstruction of changes in the plant cover during the Romanian, and the
determination of the climatic and palaeogeographic conditions.

The Upper coal-bearing formation of the Trans- Iljinskaja (1968). Palynological studies on some
carpathians belongs to the Ilnitsa Suite of Late sections in the Neogene deposits of the Trans-
Pliocene age and consists of alternating aleur- carpathians have been published previously
olites, coaly clays, tuffites and five coal-beds. The (Chmarsky 1954; Shchekina 1960; Rybakova
clays and tuffites are characterized by ostracodes, 1964, 1968, 1975). The present author studied
some molluscs, leaf remains, wood, seeds and 13 sections from Ilnitsa, Rokosovo, Gorbki,
fruits. The megaflora remains were studied by Berezinca Veliky Racovets, Uzhgorod (Syabryaj

POLAND

SLOVAKIA

5
9Uzhgorod
%

Irshava ~ 1
._______J

HUNGARY

Rakhov ~

ROMANIA

Fig. 1. Location of boreholes and outcrops in the Transcarpathians; 1, Ilnitsa; 2, Veliky Rakovets; 3, Rokosovo;
4, Berezinka; 5, Vuzhgorod; 6, Gorbki.

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 229-236.
230 S. SYABRYAJ

1969, 1975, 1986) (Fig. 1). Sediment samples The second assemblage corresponds to the
were taken from numerous boreholes, outcrops first, second and third coal seams. The pollen
and mines. spectrum of these deposits is rather uniform, and
The Ilnitsa section is the most complete. It the pollen diagram (Fig. 2) presents a picture of
contains five coal seams with thicknesses as forest vegetation. Deciduous tree pollen is
follows: 0.11-5.0m; 0.1-2.1m; 0.25-1.4m; 0.4- dominant, but their proportion has diminished.
1.5m; 0.25-1.3m. Other localities contain one They are represented by Carya (the most
or two of the coal beds seen at Ilnitsa. The abundant), Juglans, Pterocarya, Quercus,
Ilnitsa section was used as a standard. Fagus, Castanea, the latter being single finds in
only a few samples. Quercus pollen is more
abundant and more varied in this assemblage
than in the lower one. Three species were
Palynomorph records identified: Q. cf. pubescens Will.; Q. cf. petrea
Liebl.; Q. cf. robur L.
The Upper coal formation contains two coal Ulmus and Zelkova were discovered in the
horizons. The lower one comprises the fourth same quantity as in the first assemblage, whilst
and fifth layers and the other three beds are in the Celtis decreased. No significant change was
upper horizon. Two different palynomorph noted in the composition of the Betulaceae.
assemblages were obtained. Both show a high Liquidambar incieased proportionaly and
proportion of angiosperm pollen but there is also became more diverse, as also happened with
an important component of coniferous pollen, Tilia, which is represented by three species: T. cf.
mainly belonging to the Taxodiaceae. tomentosa Moench., T. cf. cordata Mill., and
The first assemblage is from the fourth and fifth T. platyphylla Scop. The pollen of thermophile
seams. The pollen diagram (Fig. 2) presents a plants are rare. Single finds of Platycarya, Engel-
picture of forest vegetation with a high propor- hardtia, Magnoliaceae, Aralia, Ilex, Nyssa are
tion of deciduous angiosperm trees: Carya, recorded. Coniferous tree pollen is more abun-
Juglans, Pterocarya, Engelhardtia, Ulmus, Celtis, dant than in the first assemblage: Pinus, Picea,
Zelkova, Quercus, Fagus, Castanea, Liquidam- Tsuga (T. cf. canadensis (L.) Carr., T. cf.
bar, Alnus, Parrotia, Carpinus, Nyssa, Mag- diversifolia (Maxim.) Mast.), Abies (A. cf alba
nolia. There is a lower proportion of shrubs Mill.). Keteleeria is absent and Cedrus, Podo-
which are represented mainly by Myrica, carpus, and Ginkgo are represented with single
Moraceae, Rhus, Corylus, Cornaceae, Caprifo- finds. The Taxodiaceae are represented by
liaceae and Rosaceae. Coniferous tree pollen is Taxodium, Glyptostrobus, and Sequoia. The
also abundant. These are identified as Pinus first is the most abundant and the last is a single
(predominantly P.diploxylon), Picea, Abies, find. The proportion of sporomorphs of shrubs
Cedrus, Keteleeria (a single find) and Tsuga. is small and they are chiefly represented by
The Taxodiaceae are represented by Taxodium, Rhus, Cornaceae, Celastraceae, Caprifoliacae,
Glyptostrobus and Sequoia (the latter beeng Elaeagnaceae, Rosaceae, Myrica. Herbaceous
rare). Single finds of Ginkgo, Sciadopitys and forms are represented by numerous hydro-
Podocarpus pollen are reported as well. As and hygrophile taxa belonging to the
for the herbaceous plants, the representatives Gramineae, Labiatae, Caryophyllaceae, Planta-
of hydro- and hygrophytic group are the ginaceae, Ranunculaceae, Gentianaceae, Umbel-
most abundant. They belong to the Cyperaceae, liferae etc. Abundant and diverse polypodiacean
Hydroharitaceae, Sparganiaceae, Nymphaea- spores are found; their number increases in the
ceae, Typhaceae, Potamogetonaceae, and Gra- upper part of the formation. The spores of
mineae. In the coal bands of the fourth seam Osmunda, Equisetum, Salvinia, Lycopodium,
Rynchospora (Cyperaceae), was found to be Sphagnals, Bryales are also recorded. Lusatis-
abundant. This genus is characteristic of meso- poris punctatus Krutzsch and L. perinatus
trophic peat-bogs. Just in these spectra, Sphag- Krutzsch were found only in bands of the
num is most abundant. The pollen of other second coal seam. They appear to characterize
herbaceous plants (Plantaginaceae, Polygona- this coal seam.
ceae, Compositae, Chenopodiaceae, Legumino-
sae, Ranunculaceae) are relatively rare. Spore
finds are attributed to the ferns Osmunda, Discussion
Polypodium, Dryopteris, Onoclea. There are
also many fungi and diatoms. Most of these Analysing the composition of the two palyno-
algae are inhabitants of freshwater basins complexes we note that the first assemblage is
(Vodop'jan 1979). the more varied one. The second complex
 PALYNOLOGICAL STUDIES OF THE TRANSCARPATHIANS 231

~J
,s
II.J.d

~ ~ m ~

I . . . . T ~ ., m. . ira..,., d- . .n ~ . Z

. ,,..~

B ~,..d=.-" ., '.. o

~ II.,.,,! , h .--I
i r I ' I

~
8
8
8

[
,x, , - - i I II --= L, o
, i

.ll,--.d n,, d,n ~

N ~

~a_ilIM 9 I. .d I= =~ =eL. 9 .. dll

I I ' I ' i '

=! z
~} ,.,ILl. . ,,, I,.

I!i o
,,.'-r ,,,-., ~io .. . . . , . . , .-. ~ ~
9 8 ~ 8

I Ir~l,;:,i!i ==
_ =-- .. > _ =_-_. >_. > ~=

,-4
E
232 S. SYABRYAJ

Table 1. Comparison of the composition of mega- and microfloral remains from the Upper Pliocene of the
Transcarpathians

Pollen and spores Megaflora

Taxa Number of Taxa Number of

palynomorphs megafloral remains
1 2 3 4

Ilnitsa, mine N 1
Equisetum parlatorii 1
Polypodiaceae 2 Dryopteris denticulata 7
D. linneaneiformis 1
Osmunda 1 Osmunda heeri 5
Pinus 49 Pinus (wood)
Pinus cf. sylvestris 1
P. tertiaria 1
P. cf. strobus 1
P. cf. Baileyana 5
Picea 6
Picea media 1
Cupressinoxylon
Taxodiaceae Taxodium dubium 4
Glyptostrobus 4 Glyptostrobus europaeus 29
Sequoia langsdorfii 12
Sciadopitys 1
Poaceae 2 Phragmites oeningensis 4
Cyperacites zollikoferi 1
Liliaceae 2
Juglandaceae 2
Juglans 3
J. cf. cinerea 1
Carya 3
C. cf. aquatica 2
Alnus 21
Carpinuas 2 Betula 1
Quercus pontica miocenica 10
Zeilkova 1
Ulmus 6
Celtis 2
Liquidambar 1
Tilia cordata 2
Acer 21
Cercediphyllum crenatum 2
Alangium tiliaefolium 16
Cornaceae 1
Rosaceae 3
Oleaceae (Fraxinus) 1 Fraxinus paviifolia 18
Ericaceae 1
Gentianaceae 2
Loranthus 1
Veliky Rakovaets
Pinus 35
Picea 10
Abies 6
Tsuga 2
Taxodium dubium 1
Sciadopitys 2
Arundo anomale 1
Poaceae (cf. Phragmites) 2 Phragmites oeningensis 6
Potamogeton 1
Sparganium 3
Cyperus 1
Phyllites cf. Myrica 1
 P A L Y N O L O G I C A L STUDIES OF T H E T R A N S C A R P A T H I A N S 233

Table 1. (continued)
Pollen and spores Megaflora

Taxa Number of Taxa Number of

palynomorphs megafloral remains
1 2 3 4

Veliky Rakovats (continued)

Salix rozmarinifolius
S. varians
Juglans cf. regia 1
Juglans 5
Carya 15 Carpolites cf. Carya
C. cf. elegans 3
Pterocarya 5 Pterocarya paradisiaca
Betula 3
Alnus 22
Corylus 2
Fagus 17
Quercus 3
cf. Castanea 4 Aesculus hippocastanea 34
Celtis 9
Ulmus 9
Moraceae 2
Liquidambar 3
Elaeagnus 2
Tilia cf. cordata 2
Tilia 1
Acer integerrimum 4
A. subcampestre 27
A. trilobatum 17
A. campestre 3
Cedrella sarmatica 2
Alangium tiliaefolium 234
Fraxinus paviifolia 53
Rosaceae
Nymphaeaceae
Labiatae
Ranunculaceae
Urticaceae
Lythraceae
Franceniaceae
Primulaceae
Rubiaceae
Solanaceae
Berezinka
Polypodiaceae 4
Polypodium 1
Cyatheaceae 2
Pinus 44
Picea 3
Larix 1
Tsuga 2
Taxodiaceae 4 Glyptostrobus europaeus
Taxodium 2
Poaceae 1 Phragmites oeningensis 5
Typha latissima 1
Cyperus reticulata 2
Arundo goepperti 4
Salix Salix varians 25
S. subaurita 6
Salix 5
Populus rhamnifolia 2
234 S. SYABRYAJ

Table 1. (continued)
Pollen and spores Megaflora

Taxa Number of Taxa Number of

palynomorphs megafloral remains
1 2 3 4

Berezinka (continued)
Juglans 1
Carya 2
Alnus 4
Corylus 2
Betula 4
Quereus 2 Quercus pontica-miocenica 6
Fagus 13
Castanea 3 Castanea atavia 3
Ulmus 5 Ulmus longifolia 3
Moraceae 3
Nymphaeaceae 1 Nelumbo protospeciosa 8
Liquidambar 1 Liquidambar europea 3
Platanus aceroides 16
Nyssa 1
Rhus 1
Acer aegopodifolium 2
A. hungaricum 2
A. sancta-crucis 6
A. trilobatum 10
Acer cf. sinense 2
cf. A. pseudoplatanus 8
Trapa transcarpatica 13
Alangium tiliaefolium 6
Oleaceae 2
Fraxinus cf. ornus 1
Rosaceae 2
Legominiosae 1
Ranunculaceae 2
Valerianaceae 1
Thymeliaceae 1

contains a lesser quantity of thermophile plants of correlating these coal seams with the upper
and more abundant hydrophile angiosperms, as horizon. The presence of Luzatisporis punctatus
well as dark coniferous elements and more and L.perinatus in the Gorbki coal bed allows its
numerous herbaceous taxa. correlation with the second seam of Ilnitsa.
It is necessary to concentrate on the third coal The palynological contents of the Ilnitsa Suit
seam, which is poorer than the lower and upper can be compared with megafloral remains from
ones. It does not contain thermophile elements, the Berezinca, Ilnitsa, and Veliky Racovets
including light-dependent ones like Celtis and it localities. This comparison between the palyno-
shows fewer sporomorphs of angiosperm pollen logical and megafloral composition highlights
whilst Taxodium and Osmunda are abundant similarities on the generic level. However, the
(Fig. 2). The third seam may be regarded as the palynological contents are more diverse (Table 1).
boundary between the lower and upper hori- The general picture of vegetation throughout the
zons, but its palynological composition is more coal bearing formation shows generally a rather
akin to that of the upper horizon. The spectra of monotonous warm-temperate deciduous forest
the first, second and third coal seams are to be cover with some subtropical elements. However,
considered togather. coniferous forests existed in the Trancarpathians
The spectrum from the coal seam of Gorbki, as well as in marshy conditions as is shown by the
the upper seam of Uzhgorod, and several small presence of Taxodium, Nyssa, Alnus and
seams from Rocosovo are identical to the second Osmunda which were found to be widespread in
palynocomplex. The composition of taxa and some of the wetter areas. Sphagnales were
their numerical content is an argument in favour important in the swamps, especially during the
 PALYNOLOGICAL STUDIES OF THE TRANSCARPATHIANS 235

accumulation of the fourth coal seam. Some horizons shows marked similarities. The entire
species of pine also inhabited swampy grounds, as interval is referred to the Romanian.
can be seen in the contemporary Mshana swamp The climate was warm-temperate, rather
in the Transcarpathians. Brush swamps with humid with a tendency to become cooler prior
Myrica and Salix invaded the outer parts of to the Gunz glaciation.
marshes. Wet forests with Carya, Liquidam- The flora from the coaly sediments of the
bar, Pterocarya, Alnus, Acer, and Ulmus Ilnitsa suite formed different communities simi-
occured in the vicinity. Mixed and deciduous lar to the ones of the same age in neighbouring
forests with Pinus, Abies, Cedrus, Tsuga, Betula, areas.
Fagus, Quercus and Castanea developed in the
drier habitats on higher areas. Thanks are due to Dr. I. Iljinskaja for kindly providing
The climate was warm-temperate, rather the samples of the Ilnitsa Suite with megafloral
humid. Only when the third coal seam accumu- remains from the Berezinka, Ilnitsa and Veliky
lated did the broad-leaved forests become more Rakovets localities. I am grateful to the anonymous
impoverished. The third coal seam overlies a reviewers for suggesting several corrections.
thick volcanic ash band and the coal contains
much tuffaceous material. Volcanic activity
taking place immediately before the third coal
bed accumulated, evidently influenced the floral References
composition. Some thermophile and light-
CHMARSKY, N. Z. 1954. Some data about fossil
dependent elements (such as Celtis) vanished flora of the Tertiary of the Transcarpathians.
from the plant cover. However the volcanicity In: Scientific notes of Dnepropetrovsk Institute.
also had a positive influence. The broad-leaved Collected works of geol.-geogr, faculty and Insti-
forests on the Vigorlat-Gutin mountain ridge tute of Geol., 39, 127-132 (in Russian).
probably expanded due to the volcanic products ILJINSKAJA, I. A. 1968. The Neogene flora of the
accumulating at the foot of the volcanoes Transcarpathian region of the UkrSSR. Publ.
(Syabryaj 1991). Such processes can be observed house 'Nauka', Leningrad (in Russian).
today in areas of modern volcanic activity, e.g. RYBAKOVA, N. O. 1964. The new data about the
Kamchatka and Indonesia. Upper Neogene flora of the Transcarpathian
region of UkrSSR (by palynological study). Bull.
The enrichment of plant communities is Moscow Society of test of nature, Geol. Series, 64,
observed during the period of formation of the 241-245 (in Russian).
second and first coal seams, when volcanism - - 1 9 7 5 . Palynological description of the Miocene
diminished. Taxa such as Castanea, Platycarya, and Pliocene deposits in the Transcarpathians
Engelhardtia, Magnoliaceae and the light- (UkrSSR). Paleontol. collect., 1-2, N 12, 142-147
dependent Celtis reappeared in the deciduous (in Russian).
forests, and the area of Quercus communities SCHEKINA, N. O. 1960. History of the Neogene flora of
increased. Modern beech forests are of impor- the Ukrainian Carpathians and Precarpathians.
tance in separate regions of Carpathians and on Flora and fauna of the Carpathians. Publ. house
AS USSR, 58-74 (in Russian).
the Vigorlat-Gutin mountain ridge, where the SYABRYAJ,V. T., LEVITSKY,B. P., SYABRYAJ,S. V. &
rich original beech forests are preserved today as EMETS, T. P. 1969. Substantial and palynological
forest reservations. Only the marsh forests composition of coal-bearing formation of the geo-
remained unchanged during the period of sinclinal part of UkrSSR. Publ.house 'Naukova
Upper coal-bearing formation. dumka', Kiev (in Russian).
At the end of the Pliocene the flora became SYABRYAJ,S. V. 1975. Description of the Levantinian
poorer, but there were no fundamental changes flora and vegetation of the Transcarpathians.
in plant cover and its structure. The Late In: Flora. Taxonomy and Phylogeny of plants,
Pliocene flora of the Transcarpathians was 279-288 (in Russian).
- - 1 9 8 6 . Evolution of the Neogenian flora and
warm-temperate, essentialy wet, with predomi- vegetation of the Carpathians. Doct. hab.thesis
nantly thermophile deciduous forest elements, (in Russian).
producing swamp forests. Coniferous and mixed - - 1 9 9 1 . Vegetation and volcanism in the Neogene of
forests occurred in the mountain areas. the Transcarpathians. Palaeovegetational devel-
opment of Europe and region relevant to its
palaeofloristic evolution. Proc. PEPC. Vienna,
Conclusions 231-234.
VODOP'JAN,N. S. 1979. The diatoms in the Pliocenian
With regard to the floral composition, the entire deposits of the Transcarpathians. Ukr. Botan.-
period of coal formation of the lower and upper journ. 35, 141-146 (in Ukrainian).
 The distribution of sulphur in the Palaeocene coals of the
Sindh Province of Pakistan

S. R. H. B A Q R I

Pakistan M u s e u m o f Natural History, Garden Avenue, Shakarpyran, lslamabad, Pakistan

Abstract: 46 samples of coals were collected, representing eastern and western coalfields of
the Sindh Province of Pakistan to investigate any systematic quantitative changes in total
sulphur. The coal is Palaeocene in age and the number and thickness of coal seams decreases
from east to west. The sulphur content was determined as total sulphur on an elemental
analyser Carlo Erba model EA 1108 on a dry basis. The sulphur content displays systematic
variations and increases gradually from east to west. It is about 1.44% in the eastern
coalfields at Tharparkar, 2.55% in the central coalfields at Badin and 4.95% in the western
coalfields at Lakhra. The Palaeocene coalfields of the Sindh Province were deposited in
shallow continental lagoonal areas towards Tharparkar in the east and comparatively down
dip deeper areas with brackish waters (deltas, estuaries) towards the Lakhra in the west. The
distribution of sulphur displays a good theoretical example in the change of depositional
environment from fresh water to brackish waters environments. It is concluded that the
coalfields with low sulphur occur in the east as compared to the coalfields with high sulphur
in the west.

The Palaeocene coals of the Sindh Province of a source of the coal vegetation towards east
Pakistan occur in the Bara Formation and have where the Precambrian granitic basement rocks
been discovered from east to west at Tharpar- are also exposed at Nagarparkar. The Bara
kar, Badin and Lakhra (Fig. 1). Stratigraphi- Formation is unconformably overlain by Pleis-
cally, coal bearing Palaeocene sediments in the tocene conglomerates and sandstones of prob-
Sindh area have been studied by several able fresh water origin in the eastern coalfields
authors (Shah 1977). Frederiksen et al. (1989- (Tharparkar and Badin coalfields) and con-
90: in Shah et al. 1992) named the Palaeocene formably overlain by Eocene marls and clays of
rocks, from base to top the Khadro Formation, probable bracklish water to marine origin in
the Bara Formation, the Lakhra Formation the western coalfields, located in the Lakhra
and the Sonahri Formation (Fig. 2). The coal area. Figure 2 gives a generalized section of the
bearing Bara Formation consists of shales, Palaeocene rocks in the Lakhra Coalfield of the
sandstones, marls and coal bends in the western Sindh Province. The depths of the respective
side at Lakhra, while it consists of clays and samples are provided in Table 1 and the details
sandstones of probably fresh water origin in the about the locations drilling cores lithology etc
east at Tharparkar. The presence of marls and are provided by Shah et al. (1992). 46 coal
lenticular argillaceous limestone bands at samples were collected to investigate the total
Lakhra in the west (Fig. 2) reflect compara- distribution of sulphur and to understand the
tively more saline and deeper water conditions palaeo-environments of the depositional basin.
as compared to the east at Tharparkar. There The sulphur content was determined as total
are about 11 coal seams in the Tharparker sulphur in an elemental analyser carlo Erba
coalfield that range in thickness from 1.42 to model EA 1108 on dry basis.
27 m. In addition, there are numerous thin coal
partings intercalated with the shales. There are
three workable coal seams in the Badin area Distribution of sulphur
and the thickness varies from 0.55 to 3.1m
(Khan et al. 1992). Three coal seams have been Figures 3 and 4 and Table 1 give the distribution
reported from the Lakhra Coalfield which of total sulphur in two boreholes (TP-3, TP-4)
range in thickness from 0.3 to 3.00m. The in the Tharparkar area and in some coals
number and total thickness of coal seams from the Badin and the Lakhra coalfields. The
generally decrease from east to west, indicating sulphur in most of the samples is less than 1%

From Gayer, R. & Pegek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 237-243.
238 S. R. H. BAQRI

I '
72" L
6,~"
U.S.S. R

AFGHANISTAN
NW R#, - ~
::)NTIE~ ~ JAMMU
a
~'\'~:~3) KASHMIR
~,--~

~32"
/

,~'.~s ,6 ,7 ( PAN JAB

~1 ~9
,7 / /
, ~ ~ --.'~-.

BALUCHISTAN // Lf.,,.,..
IRAN (SINDH. / INDIA

24"...-
4 /~ 4 ~ ' / 4 /r

,-e~-.4 TP4

0 200 krn ~ J~
} I., 1
0 e.~. 200mi
I

Fig. 1. The location map of the coalfields of Pakistan. The circles display the locations of the samples collected
for the present work: 1, Indus East Badin; 4, Lakhra; 26, Tharparkar.

with the exception of eight samples and indicates indicates a good prospect for an area of low
the lowest concentration of sulphur in Pakistani sulphur coal. The distribution of sulphur with
coals. The average concentration of sulphur in depth in bore hole TP-3 does not show any
40 samples of the two boreholes in the Tharpar- systematic variation and probably reflects the
kar coalfield is about 1.44% and is the lowest of uniformity of the processes of deposition or
all coalfields of Pakistan (Baqri 1993). Figure 4 diagenesis. The distribution of sulphur in bore
and Table 1 show that the sulphur in most of the hole TP-4 is interesting and is not uniform. It
samples (with the exception of one sample) from does not show any systematic variation with
borehole TP-3 remains even less than 1% and depth but appears as a random distribution and
 S U L P H U R IN P A L A E O C E N E COALS, P A K I S T A N 239

MEMBER >-

U AND _
~.m
o o
I.d COAL ZONE :z: EXPLANATION
I,=-

OUJ Ru bbty time stone.

..=Z 9 'LI
Even be dded limestone
AI luvi urn :----;. 9 i
. . . . i
Calcareous shale
Calcar~ou s siltstone
Laki Limestone Calcareous sandstone
Shale and ctay stone
LIJ 100
;:.~:: Sandy shale
r,.) .. ; ...
_.:.-, Siltstonr and sift
Shaly sandstont
Meting Shale __
Sandstone sctr~d~
Coat
%-- Undorctay

Meting ZOO
Limr

i~ :z: TM'sohnaricoat zone ;~'i'~-L':~

i t 300

Coat zone :-..'-'--

W Upper Dhaduri - .....

Z ~
Ld Ohaduri ,
0 z Upper stra y~ C?'."" ~'-"
W o Inyatabad . . . . . . . 4100
~ i Upper Sonda
EL I Lower Sonda
Upper Wassi .,,~r..4~.~
~ Wassi .....
~[ , ": 9 .,,
n,.
Lower s t r a y
.-- ..

50O
7-::-
. . . . .
~-_
SCALE
9 ." . . ' . . . - .
".',-...
IN
NETERS

Fig. 2. The stratigraphic section of the Palaeocene/Eocene rocks from the Lakhra Coalfield in Sindh Province
240 S. R. H. BAQRI

Table 1. The weight percentage of sulphur (wt%) in Table 2 provides the average distribution of
Palaeocene coal samples with respective borehole sulphur in the Badin and Lakhra coalfields of the
numbers and depths in metres. Tharparkar (TP4, Sindh Province. The sulphur in the Badin
TP3) Badin (BN1) and Lakhra (LS4, SOs) coalfield is lower (2.55%) than the Lakhra
Sample Sample No and Sulphur (4.95%). The low sulphur in the Badin coal-
depth in metres (wt%) field is due to leaching of the sulphate ions
through meteoric waters, poor in sulphate ions,
1. LS4, 156.97-157.64 0.92 most likely fresh/brackish waters as the Bara
2. LS4, 190.98-191.28 6.27 Formation with intercalating coal seams is
4. BN1, 0.36m Bara Fm. 1.65 overlain by conglomerates and sandstones of
5. BN1, 101.7 5.29 Pleistocene age.
6. BN1, 122.85-123.31 0.73
7. TP4, 180.91-181.25 3.53
8. TP4, 181.25-181.6 7.81
9. TP4, 181.6-181.93 16.94
10. TP4, 192.05-193.02 0.43 Discussion
11. TP4, 193.2-193.58 0.43
12. TP4, 193.58-194.31 0.37 Querol et al. (1991) studied the total sulphur in
13. TP4, 194.51-195.16 0.42 coals of Teruel District, Spain and concluded
14. TP4, 200.68-201.12 2.97 that the distribution of sulphur in the coals is
15. TP4, 203.45-203.75 2.93 influenced by the depositional and diagenetic
16. TP4, 205.73-206.08 0.56 environments. Querol et al. (1989) carried out
17. TP4, 223.78-224.66 0.3
detailed investigations on the iron sulphide
18. TP4, 229.01-229.71 0.44
19. TP4, 229.71-230.18 1.36 precipitation sequence in Albian coals from the
20. TP4, 230.18-230.73 2.88 Maestrazgo basin, southeastern Iberian Range,
21. TP3, 148.6 0.82 northeastern Spain. They proposed five stages of
22. TP3, 153.92-154.22 0.71 iron sulphide precipitation which were con-
23. TP3, 154.22 1.36 trolled by the coalification evolution.
24 TP3, 155.7-156.72 0.85 The lowest concentration of sulphur in the
25. TP3, 156.72-156.97 0.71 coalfields is generally due to either their deposi-
26. TP3, 157.64-158.24 0.84 tion in the proximal part of the depositional
27. TP3, 158.34-158.94 0.69
basin (fresh water ponds, Fig. 5) or due to the
28. TP3, 158.52-160.02 0.72
29. TP3, 158.94-160.02 0.57 leaching of the sulphate ions during early or late
30. TP3, 161.52-162.42 0.62 diagenetic stage through the waters poor in
31. TP3, 162.42-163.07 0.69 sulphate ions. It is most likely that the eastern
32. TP3, 163.07-162.42 0.49 coalfields of the Sindh Province experienced
33. TP3, 164.30-164.75 0.66 both processes. The eastern coalfields were likely
34. TP3, 164.75-165.52 0.59 deposited in the proximal part (fresh water,
35. TP3, 165.52-166.11 0.54 Fig. 4) of the Palaeocene depositional basin,
36. TP3, 166.11-167.66 0.1 shallower in the east and comparatively deeper
37. TP3, 167.66-168.21 0.51
towards the west (representing brackish to delta
38. TP3, 168.21-169.21 0.59
39. TP3, 169.21-169.90 0.45 front environments). The basement rocks are
40. TP3, 169.90-170.72 0.2 still exposed further east at Nagarparkar in
41. TP3, 170.73-171.83 0.69 Tharparkar district. The second cause for the
42. TP3, 171.38-172.26 0.71 low sulphur concentration in the eastern coal-
43. TP3, 172.26-172.83 0.38 fields (Tharparkar area and Badin area) is due to
44. TP3, 172.93-173.83 0.58 the leaching of the sulphate ions by meteoric
45. TP3, 173.83-175.23 0.7 waters from the overlying Pleistocene conglom-
46. TP3, 197.25-198.35 0.76 erates and sandstones of probably fresh/brack-
ish water origin as compared to the western
coalfields at Lakhra where the Palaeocene rocks
are conformably overlain by Eocene marls, clays
and limestones of marine origin. Figures 3 and 4
therefore reflects probably variations during display the increasing distribution of sulphur
the depositional and diagenetic history. Seven from east to west and indicate a basin with its
samples contain less than 1% sulphur, five proximal end towards the east (Tharparkar) and
samples display sulphur between 1-4% and the distal end towards the west where more
only two samples display more than 7% sulphur sulphate rich waters acted during the deposition
(Table 1). of the Palaeocene coal field at Lakhra.
 S U L P H U R IN P A L A E O C E N E COALS, P A K I S T A N 241

Distribution of SuLphur

;"4

~3

m
2

0
WEST LAKHRA BADIN T H A R P A R K A R EAST

Fig. 3. The average distribution of sulphur in the Sindh coals from east to west (Table 2).

Distribution of sulphur in Sindh coots

I sulphur% )
17
16-
15-

13
12
I1
tO
8
8
7
G
5
/,.
3
2
1
0
12 3 4 5 6 7 8 9 101112131/,1516171M92021ZZ?..~/,2r 3~f33435363"/N 4243/,4/,S&6
WEST EAS~I
Seriol no of somples(Tobte | ) .

Fig. 4. The distribution of sulphur in the individual samples of coals from the coalfield of the Sindh Province.
242 S. R. H. BAQRI

Table 2. The distribution of sulphur in the Palaeocene 3. The sulphur in the eastern coalfields or the
coals of the Sindh Province Sindh Privince is low and therefore the eastern
coalfields are the g o o d prospects for low sulphur
Name of Average SD SE No of
coals and m a y be exploited for industrial
coalfield sulphur samples
(wt%) purposes.

Lakhra 4.95 3.55 2.05 3 I am grateful to the EEC for providing a financial
Badin 2.55 2.41 1.39 3 grant as a post-doctorate Marie Curie Senior
Tharparkar 1.44 2.85 0.45 40 Research Fellowship for the carrying out of these
studies. I wish to thank Professor Dr N. Hamilton,
SD, Standard deviation; SE, Standard Error. University of Southampton, for allowing me to
conduct these studies in the Department of Geology,
I am also grateful to Dr Bashir Ahmad Sheikh,
Chairman of the Pakistan Science Foundation,
Islamabad, for his encouragement and granting
Summaryand conclusions permission for me to carry out these studies in
the UK.
1. The sulphur content in Palaeocene coals of I am thankful to Dr Shahzad A. Mufti, Director
General, Pakistan Museum of Natural History, who
the Sindh Province increases from east to west.
encouraged the publication of this work. I am grateful
It is 1 . 4 4 w t % at T h a r p a r a k a r , 2 . 5 5 w t % at to Mr. Sher Akbari for his help in the laboratory.
Badin and 4.95 w t % at L a k h r a . Finally, I pay my regards to Dr John Marshall for his
2. The Palaeocene coals were deposited in keen interest, supervision and encouragement of these
fresh water p o n d s towards the east and in studies, and to Mr Abbas Ali Shah, Director,
comparatively m o r e saline brackish water con- Geological Survey of Pakistan for providing the
ditions towards the west. borehole samples for these studies.

17 3 Tidal flat= klangrovr swarr~Fre~

-~ wFre.ph
water
amp
,Fresh water
awamp j
, and . _..and water .f ~ -
Delta Front_ _ cnannets lid61- channel swam p / ~ :r ~" ~'

- .'-
ki~,. /
. H i g h w"a...........
........ ter =- " :" " ~.~ ~.'-_"~-'~_~.~. ~ . Z:~.:~'r..:~,=
" - ' i - : - ".~.~'~." C LAY
11 - :" ~ """'-'-"'-'~-'" "~'~: "~B A S E M E N T R 0 C K S
, . . . . . . ... 9 . . . . . ~

1-2 3 /. 5 6
West
7~
!1 l ' mm I Immmimmii=mmmm_-m._lm=mil
' mIO1112131/~lS16t711H920212223Zt,
m-I i--am
Z5262"/2~Z93031 32.~3635.,t6373839/.O41~&3~St,6
East

Serial no of sarnples ( T a b l e 1)

Fig. 5. The palaeoenvironments of depositional basin and the distribution of sulphur in the Palaeocene coals of
the Sindh Province of Pakistan.
 S U L P H U R IN P A L A E O C E N E COALS, P A K I S T A N 243

References , FERUANDEZ-TURIEL J. L., LOPEZ-SOLER, A.,

HAGEMANN, H. W., DEHMER, J., JUAN, R. &
BAQRI, S. R. H. 1993. Research progress report for Ruiz, C. 1991. Distribution of Sulphur in coals of
Marie Curie Bursary, No. B/Cl1"-923195, Uni- the Termel mining district, Spain. International
versity of Southampton, UK. Journal of Coal Geology, 18, 327-346.
KHAN, S. A., KHAN, I. A., ABBAS, S. G. & KHAN, SHAH, A. A., KHAN, S. A., TAGER,M. A., CHANDIO,
A. L. 1992. Coal Resources Potential of Pakistan. A. H. & LASHARI, G. S. 1992. Drilling and Coal
Information Release 533, Geological Survey of Resources Assessment in Southern Sindh, Pakistan.
Pakistan. Information Release 537, Geological Survey of
QUEROL, X., CHIUCHONS,S. • LOPEZSOLER,A. 1989. Pakistan.
Iron Sulphide precipitation sequence in Albian SHAH, S. M. I. (ed.) 1977. Stratigraphy of Pakistan,
coals from the Maestrazgo basin, Southeastern Memoir Geology Survey of Pakistan, 12, 138.
Iberian Range, northeastern Spain. International
Journal of Coal Geology, 11, 171-189.
 Sulphur distribution in a multi-bed seam
PAUL F. C A V E N D E R & D. A L A N SPEARS

Department of Earth Sciences, University of Sheffield, Sheffield $3 7HF, UK

Abstract: The Parkgate Seam (Langsettian) is an important seam for the coal industry in the
UK. It extends over a considerable part of the East Pennine Coalfield and a large database
of information on the seam has been complied by (the former) British Coal for the
Nottinghamshire area from many sampling locations. The seam has been subdivided into a
series of mappable units termed plies. This paper demonstrates how sulphur concentrations
may vary considerably on a vertical scale and that spatial distributions within individual
plies may be markedly different to other plies within the seam. Often seam sulphur maps for
industrial use are produced for a composite of the whole thickness of the seam, typically as
the whole seam-less-dirt. The neglect of the vertical variation in seam sulphur content may
lead to the production of maps which are of limited industrial use. Variations in sulphur
distributions also has implications for the origin of the sulphur in the coal. Distribution
maps have allowed the controls on sulphur in the Parkgate Seam to be investigated, and
these are dominated by complex depositional processes.

Mapping of geochemical variables (sulphur and trace elements in coal, based on the use of ICP-
chlorine contents), ash content, seam splitting AES (Cavender & Spears 1995b).
and, perhaps most importantly, seam thickness The present paper describes and discusses the
has been carried out throughout the history of mapping of sulphur in coal and investigates
the coal mining industry. This has been achieved the use of ply-by-ply mapping in contrast to the
by interpretation of data collected over the mapping of the whole seam, taking into account
period of exploration, development and mining also the vertical distribution of the sulphur
of seams, resulting in an in depth knowledge of content. It then goes on to discuss the controls
the seam both vertically and spatially. Data are on sulphur in the Parkgate Seam.
usually accumulated by seam sampling from
borehole cores or pillar sections; see Ward
(1984) for discussion of sampling techniques. The Parkgate Seam
Since economically viable seams are commonly
in excess of 1 metre in thickness, several samples The Parkgate Seam has been worked in the East
are usually collected and analysed. These ana- Pennine Coalfield, UK, and substantial reserves
lyses have allowed the accurate subdivision of remain at the present day. The seam was
seams, which are usually formed from a number regarded by (the former) British Coal as one
of distinctive, laterally persistent units, termed with an important future well into the next
plies. Historically data were manipulated by century. A considerable amount of data are
hand and profiles and isolines were then plotted available on the characteristics of the seam
by eye, rather than by a sophisticated technique. within the seam database (British Coal 1992a).
However, this work is now done as routine by Figure 1 shows the stratigraphical position of
computer, creating the opportunity of accessing the seam within the Westphalian, together with
and manipulating an extensive database in a way the subdivision of the seam as used in this work.
not previously feasible. Access to the British Seam plies are referred to by ply codes in the text
Coal database (British Coal 1992a) has allowed of this work and the reader is referred to Fig. 1
much investigation of the coal. The database for their intra-seam positions. The seam lies in
includes extensive information (on 3569 sam- the upper part of the Langsettian and is a
ples) resulting from the exploitation, observation considerable stratigraphical interval from any
and analysis of seams for many locations. marine sediments in the sequence, a common
The Parkgate Seam, from the Langsettian prerequisite for high sulphur coals (Williams &
(Westphalian A) of the Nottinghamshire Coal- Keith 1963).
field, UK, has been studied in detail and forms Several workers have discussed the deposi-
the basis for the work presented here. The seam tional environments of the coal-bearing deposits
is also the subject of other work on the pre- of the East Pennine Coalfield, the most notable
diction of sulphur in coal (Cavender & Spears recent publications being by Guion & Fielding
1995a) and an alternative analytical technique (1988), Guion et al. (1995) and Flint et al.
for the determination of forms of sulphur and (1995).

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 245-260.
246 P. F. CAVENDER & D. A. SPEARS

Westphatian L a n g s e t t i a n ( W e s t p h a t i a n A) Parkgate Seam

m- m-~ Clay Cross Marine Band

t s i (Vanderbeckei)
t ]right coal
t
C Bolsovian ,' , I DEEP SOFT
t ledium sulphur
/
t )cc. dirty bright
i , f PARKGATE
/
I ledium ash with
/ TUPTON / COCKLESHELL
t Ih ash coal,
THREEQUARTERS Dase
B Duckrnantian
i, occ. high
t
t
i ! SILKSTONE (YARD /
z
i
BLACKSHALE)
/ I bright and dull

~hur
' ~ KILBURN
1st / 2nd ]inly mudstone

3al, often dirty

A Langsettian UPPER BAND /

9m. m-~ Norton Marine Band ash content

- ' - ' - - 1 NORTON very high sulphur
FORTY YARDS . m- m-] Alton Marine Band
ALTON ( G a s t r i o c e r a s listeri) )yrite common
i
BELPER LAWN
- Pot Clay Marine Band
............... m . m -~ ( G a s t r i o c e r a s s u b c r e n a t u m )

Fig. 1. Stratigraphical position of the Parkgate Seam within the Westphalian of Nottinghamshire and the
simplified subdivisions of the Parkgate Seam (redrawn from Cavender & Spears 1995a).

Correlation of the Parkgate Seam (1967) when the Parkgate Seam (of Yorkshire)
and the 1st and 2nd Piper Seams (of Notting-
Before considering the sulphur distribution in hamshire and Derbyshire) where proved to be
the seam, the correlation of the seam is outlined, continuous. The seam is termed the Parkgate
both from a historical perspective and for the Seam in this paper.
purpose of this work. The most up-to-date and relevant correlations
The Parkgate Seam extends over a consider- of the Parkgate Seam in Nottinghamshire have
able area, and is present throughout the East been made by British Coal (1992a, b). These
Pennine Coalfield. Figure 2 shows the extent of correlations show differing terminologies with the
the seam and also the areas in which the intra- British Coal (1992a) division being used in this
seam correlation has been considered. It also work. This subdivision of the Parkgate Seam has
shows the main area of the study of this work, been made using a number of variables. Histori-
which lies in the northern part of the Nottin- cally, a number of samples have been collected by
ghamshire Coalfield. British Coal at each sampling location. The
Many workers have suggested subdivisions boundaries between the samples are selected by
for the Parkgate Seam over the whole East either changes in the character of the coal, the
Pennine Coalfield, and a summary of these presence of partings, or by a maximum sample
subdivisions is given in Table 1 together with thickness (usually around 200 mm). This means
references. It should be noted that the most that several samples may be collected from a
important and easily identifiable ply of the seam single ply of the seam.
is the l st/2nd Piper split (X2P), this subdivides The following information is recorded for
the seam into the 1st Piper (1P) and the 2nd each sample collected: the thickness; the coal
Piper (2P). Originally the 'Pipers' of Derbyshire lithology and characteristics; the ash content
were not considered to be the same seam as the and the total sulphur content. These variables,
Parkgate of Yorkshire. This was noted by together with the presence of seam splits are
Edwards (1951), who introduced the term used to define the individual plies of the seam
'Dukeries' coal which represented a composite and all of these data have been included in the
of the Deep Hard and 1st Piper Seams. This seam database by British Coal (1992a). The
term was subsequently dropped by Edwards seam subdivision is shown on Fig. 1, together
 S U L P H U R D I S T R I B U T I O N IN A M U L T I - B E D SEAM 247

1320 [340.^. o~sea_m...... ,= . . . . . . T ~- , ,, --.r-_

Be~;ercotes
,."':'"-':
~elbeck Colliery ; Colliery
,, ~100m i

2 /'/ Q_O erton Co ery s

Ba~nsley O' ', "" ; t Ollerton Colliery 3's
/ 9 Thoresby Colliery ;, ~'-' |
i '<' / '-)~
," Ollerton~Collierylg'sA&B
400 ," ,,,,,
i~,'t, I/
seam present at depth % ' ,t', 'Olierton-Col ery 18's
I
\, "!,"Bilsthorpe o) Pillar section
Borehole section
4 o~,O~ " S a m p l i n g p~176 .~utt'ne ~ w~ /

Z : ", !5 ,/

She,, ,d ",i /
380 ~ i ", 9 / 380

,.. Lr4
v~ j" 6 i ", /

.............
~ - - ~ erfie d i
......lil;iiiii!iiiiiiiii, iiiiiiiiii!iiiiiii [
i Main study !i::iiiiiiii!!i:i!i:i:il
} ~ ~! I !ii! i :::.iarea :h:i::ili::iiii::!ii::il
~ , seam present at depth

360 i Mansfield II
I|ii:iii ii:.i:.ii
1
i i : i!iii::ili :::iiii!i!!| 360

9~

i seam present at depth

) Nottingham
II 34O

\
. . . . . . . . . . . . . . . . . . . . . . ~ .

N /
0 10 ~ /
t | \ / 32_0
kilometres , --... _ ~ "- I"
I 1440 1460 I

Fig. 2. The extent of the Parkgate Seam in the East Pennine Coalfield showing the main area of study, areas
where correlations have been made (see Table 1) and sampling locations within the main area of study.
248 P. F. CAVENDER & D. A. SPEARS

i :' I
i

.~ i o~

i
-~ ~ ~, ~,.
E o ~ _ :
i

~ ~
.~ ~
o
~
:
I

e", E _o ~ ~ :: _o
(J leOO Jaddn
-~ , ',
.01
.... (:': ........ I
t- 9 ~
O

I'~.~ e-. h-- ~. E c-. 8

.~_ 9 ~
9- I
~iiill~ =~ -- _-_
!!!~ _
4.% I

"~
Z ::
sdoi Jaded ;s L Jedld Puz
, ::

o ~o ~ _~~ ~E ~"
1~-I2
9~ -

m ~
~
r- ~
~ ~ ~ ll

UJ : l
: i: :, 0 o.

"0
C eO~ ' ~ _ o e'" ~ "- ~?. : ~'go e,-
~ ,

~ ~. UaA!6 UO!S!A!pqns pel!e;ep ou c-. ,..,

i 03
9 T-
,_. .... ~,! ~ ,, ~ ~ ~ ..~- .
0.. : r ~ r ' ~ CO '-'~r ='

~- o h" ~ iE m a. -o I = o = | .~ = ~ .~

=" =,~1 is ~,- > , ~ - o ~ = _.e ,,=

9- ~ I ~ ~ ~ . - ~

" 1
 S U L P H U R D I S T R I B U T I O N IN A M U L T I - B E D SEAM 249

with a brief description of the characteristics of of plies (specified by the ply code, Table 2), data
each ply. The 1PUB and 1PM plies are difficult were extracted for a given variable, in this case
to distinguish where seam splitting is absent and the sulphur content. These r a n d o m l y spaced
therefore are considered together in this work. data were then gridded using the kriging
The 2nd Piper is c o m m o n l y split, but the splits technique (see Swan & Sandilands 1995) and
tend to be laterally impersistent and therefore then s m o o t h e d sulphur isolines were con-
the ply has not been subdivided. In addition to structed. All m a t h e m a t i c a l procedures a n d plot-
the plies m e n t i o n e d above a r o o f and a floor coal ting were carried out using a personal computer.
are sometimes present (Table 1), separated from If, as in m a n y cases, m o r e t h a n one sample had
the m a i n b o d y of the seam by splits. been analysed for an individual ply, then a m e a n
value for this ply was calculated using a
weighing related to the thickness of the indivi-
Generation of seam sulphur maps dual samples.

M a p s showing the distribution of seam sulphur

content have been p r e p a r e d using i n f o r m a t i o n Sulphur distribution in the Parkgate Seam
from the British Coal seam database (British
Coal 1992a). Table 2 shows an example of the The only sulphur data available in the seam
seam data for one sampling location within the database are for total sulphur contents and
database. F r o m the database, for a ply or g r o u p therefore distribution maps are for total sulphur

Table 2. Format of British Coal seam database

1 2 3
FLASH LANE 468 644 364 663

693.48 10 BRIT 1PUT 3.4 1.20

693.49 1 DULL 1PUT 3.4 1.20
693.59 10 BRIT 1PUT 3.4 1.20
693.78 19 BRIT 1PUT 3.2 1.69
693.79 1 DIRT 1PUXB 55.6 0.80
693.80 1 DBRT 1PUB 20.8 1.52
693.94 14 BRIT 1PUB 3.3 1.84
694.14 20 BRIT 1PUB 4.1 1.79
694.25 11 BRIT 1PM 7.1 2.07
694.26 1 DBRT 1PM 28.4 1.00
694.41 15 BRIT 1PM 3.7 2.01
694.44 3 DULL 1PH 8.1 0.91
694.65 20 BRIT 1PH 3.3 1.04
694.68 3 DULL 1PH 3.7 0.87
694.76 8 BRIT 1PH 4.9 1.00
694.81 5 DULL IPH 10.1 1.04
694.83 2 DBRT 1PH 15.6 1.30
695.04 21 DIRT X2P 79.5 0.62
695.14 10 BRIT 2PU 14.0 3.39
695.22 8 DIRT 2PXL 84.0 0.66
695.34 12 DBRT 2PL 16.1 8.70
695.40 6 DBRT 2PL 25.0 16.40
695.53 13 BRIT 2PL 10.9 3.02
695.57 4 DIRT XFC2P 53.0 1.09
695.70 13 BRIT FC2P 14.2 2.53

4 5 6 7 8 9

Table indicates data for one location. 1 - name of location, 2 - grid reference
(eastings), 3 - grid reference (northings), 4 - depth to the base of unit from
borehole origin, 5 - thickness of unit (cm), 6 - coal lithology code (BRIT -
Bright Coal, DULL - Dull Coal, DBRT - Dirty Bright Coal, DIRT - Dirt
Band), 7 - ply-code (see Fig. 1), 8 - ash content (%), 9 - total sulphur
content (%).
250 P. F. CAVENDER & D. A. SPEARS

distribution only. However, a number of sam- (1.09 + 0.36%). It has been suggested that organic
ples have been collected for this study and 80 sulphur increases with pyritic sulphur but to a
samples analysed, from all plies of the seam, in lesser degree (Wandless 1959). This relationship is
order to determine the forms of sulphur in the shown in Fig. 3b, but in this case the relationship
coal. Samples from seven complete seam sections between the forms of sulphur is unclear.
were collected from the northern part of the
Nottinghamshire Coalfield (see Fig. 2). Analysis
of the samples for forms of sulphur was made Vertical variation of total sulphur and forms
using an alternative technique, based on the of sulphur." analysed seam sections
British Standard method, but using ICP-AES to
determine sulphur in the digestion solutions Figure 4 shows the vertical distribution of the
prepared (see Cavender & Spears 1995b for forms of sulphur in the seam at the selected
details). Total sulphur was also analysed, using sampling locations (see Fig. 2). In all cases the
the British Standard high-temperature method 2P has the maximum total sulphur concentra-
(British Standards Institution 1977). tion, although in the Ollerton 18's (Fig. 4b),
The analyses have allowed the vertical dis- Ollerton 19's B and Thoresby sections, the total
tribution of the forms of sulphur within the seam sulphur is not as high as in the other sections.
to be studied. In addition the vertical distribu- Both the Welbeck (Fig. 4c) and Ollerton 3's (Fig.
tion of total sulphur for a wider area has been 4d) sections show very high concentrations of
studied using information in the seam database. total sulphur in the 2P, with a maximum at the
base of this ply (the base of the seam). In
addition to the 2P, the 1PUB/1PM ply also has
Forms of sulphur in the Parkgate Seam high total sulphur but this is much less
prominent than in the 2P. The 1PH ply shows
From the analyses carried out for this work, it has a low in the total sulphur profile. This ply is
been demonstrated that the variation in total mainly composed of banded bright and dull
sulphur in the Parkgate Seam is almost entirely coal, the latter often being consistent with a low
due to the differing concentration of pyrite sulphur content (Wandless 1959).
(Cavender & Spears 1995a). This relationship
can be seen clearly when total and pyritic sulphur
are plotted against each other (Fig. 3a), and also Vertical variation of total sulphur."
in individual seam profiles (Fig. 4). Table 3 shows seam database
the general distribution of the forms of sulphur
in the seam. Pyrite shows a considerable variation The vertical variation of total sulphur in the
(1.17• in the seam with very high seam is summarized in Figure 5. The results have
percentages in some samples being due to the been calculated as the mean of all the mean total
presence of pyrite nodules. Organic sulphur is sulphur contents at each location for individual
relatively constant with only a small variation plies. The results are similar to those obtained

(a) 10 (b) 10
r2=0.09
9 ~

8
7
~
i- 6
t~
-5 5
0 .tO
4
,r-
>,
3
2
9
1 ~
~o
9" ~ " 9
tr22 = 0.9596 ,~"" - ' . .9. t," "~ 9 9
L'~.,_
i i i [ ] i i I I I 0
0 1 2 3 4 5 6 7 8 9 10 11 12 0 1
total sulphur % organic sulphur %
Fig. 3. (a) Pyritic sulphur plotted against total sulphur for coal samples analysed (redrawn from Cavender &
Spears 1995a). (b) Pyritic sulphur plotted against organic sulphur for coal samples analysed.
 SULPHUR DISTRIBUTION IN A MULTI-BED SEAM 251

8
"5 r- 5,

~ E "S
rO

o o
I
3o
E

b
"-6
r,,,,,)

8
-~~
rl t., 4 -
iii! !!!! !!!i !!!!!!!!!!!!!!!!-iiiii~i-_iiiii]i!i Z!]iiiiii~
/
r-O
Q-~.

"6
+ ' rO
o

9
~"- .......................................................................... i-i}iii......i--ii--ii i ----ii ............
--ii
~. ..........................._._......................
__ jf~!!~!!~ i~ ~5 ~,~,~,~~{~~./~
I.- ~ en .,~ "r "r I.-- r ~

X X

"6
o

~ . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

~ ......................................................................

.~
2o
. . . . . . . . . . . . . . r21

~o ,......... P - - .... t
o ......................................................................................................................................... o
'S
~~'~] iiii
.........................................
............. iiiiiiiiiiiiiiiiiiiiiiiii-i 0

~6
~

. . . . n E
~ o
~,,=,
252 P. F. CAVENDER & D. A. SPEARS

T a b l e 3. Forms of sulphur in the Parkgate Seam (data greater number of samples ( n = 192 except;
from Cavender & Spears 1995a) 1PM, n = 179; 2P, n = 1 5 9 ) in the database.
The maximum sulphur content is at the base of
total pyritic sulphate organic the seam (2P). Many ply descriptions from
Mean 2.34 1.! 7 0.08 1.09 British Coal records indicated that pyrite
S.D. 1.83 1.79 0.11 0.36 nodules are commonly present in this ply,
Min. 0.84 0.00 0.00 0.12 emphasising the importance of pyritic sulphur
Max. 11.05 9.61 0.58 1.71 in this seam. The lowest concentration of
sulphur is seen the 1PH ply, with the 1PUT
n=75 ply also low in sulphur, and the 1PUT/1PM ply
with a mean of just over 3%.
from the seven analysed seam sections (above), From the analyses done for this work and also
although results from the latter are in all cases the information in the seam database it is clear
lower than the corresponding result from the that the vertical variation in the total sulphur is
seam database. It is likely that this is due to the considerable.

80
mean: 1.84
s.d: 0.55
1PUT
60

40

20

SOT ~ 1mean:3.15 1PUB

40 .: .

20
10
0 ~

50
mean: 3.25 1PM
40 s.d: 1.50
30
20
10
0 on IIINnn o . i

90 ] ~ - ~ m e a n : 1.51
1PH

25
mean: 4.19 2P
20
15
10
5
0 , ,

0
, ,

1
,
n
2
IIl!lOOnnnOn
3 4 5 6 7 8 9 10
total sulphur %

Fig. 5. Vertical distribution of total sulphur in the Parkgate Seam (data from British Coal 1992a).
 SULPHUR DISTRIBUTION IN A MULTI-BED SEAM 253

Ash-sulphur relationships in the where Spy is the percentage of pyritic sulphur in

Parkgate Seam the coal sample and 'ash' is the percentage of ash
in the coal sample. Since only total sulphur data
Although the data on the forms of sulphur within are available in the seam database the theore-
the Parkgate Seam are restricted to analyses done tical relationship between total sulphur and
in this work, a vast number of total sulphur ash is:
analyses exist for the samples in the seam
St = (0.8032 x ash) + So + Ss (3)
database. These samples also have been analysed
for ash content. This ash content, determined by where S t is the percentage of total sulphur in the
the high temperature ignition of coal, is a coal sample, So is the percentage of organic
reflection of the mineral matter present in the sulphur in the coal sample and Ss is the
coal in situ. The ash content is therefore con- percentage of sulphate sulphur in the coal
trolled by various mineral fractions. By X-ray sample. Since the values of organic and sulphate
diffraction analysis, the main components of the sulphur have been determined and they are both
mineral matter in the Parkgate Seam have been relatively constant in the Parkgate Seam (Table 2)
identified as quartz, illite, kaolinite and pyrite. they can be included in the theoretical equation:
Pyrite is transformed to iron oxide during the
ashing process, and the reaction may be described St = (0.8032 • ash)+ 1.18. (4)
as follows: Figure 6 includes this line (4) on a graph of ash
plotted against total sulphur, for all samples
4FeS2 + 1102 - - + 2Fe203 + 8SO2 (1) present within the seam database. Of note are
This reaction means that there is a minimum the very small number of samples which lie
possible amount of iron oxide within the outside this theoretical line (that is with high
resulting ash for a given amount of pyrite sulphur contents and low ash contents), indicat-
within a coal sample. This amount can be ing that equation (4) applies to the samples in
calculated and a theoretical relationship between the seam database. The outlying samples may be
ash and pyritic sulphur determined. This rela- due to abnormally high percentages of organic
tionship is: sulphur or analytical errors.
The plot also indicates another trend in the
Spy = 0.8032 x ash (2) data. The minimum amount of sulphur present

35
t h e o r e t i c a l line of m i n i m u m
ash a g a i n s t sulphur: .
30 y = O . 8 0 3 2 x + 1.09

25

o~
z,..
= 20
(.-

C~

O)

O
9 9

10

9 9 8 o 9
9 , 9 o
L , 9 ." *O* **
5 ] .. . . . . . .
/ .d~JSg~'~ ,4 .e. 9 9 9 9 9149

0 / ~ , " ......... , ......... ' " ;;~" . . . . . , "-" " ""

/

0 /20 40 60 80 100
p r o g r e s s i v e 'dilution' of s u l p h u r by
detrital fraction of coal ash ash %
Fig. 6. Total sulphur plotted against ash for data within the seam database.
254 P. F. CAVENDER & D. A. SPEARS

decreases with increasing ash content, in contrast Spatial variation of total sulphur
to the relationship already noted. In this case it is
clear that the increase in ash content is not due to Sulphur distribution maps have been produced
pyrite, although pyrite may still be present in for the main plies of the seam. A composite map
small amounts in these samples, but silicate of the whole seam-less-dirt sulphur (Fig. 7) is
minerals such as detrital clays and quartz. The shown in addition to the total sulphur in the
decrease in minimum sulphur content is caused 1PUT (Fig. 8), 1PUB/1PM (Fig. 9), 1PH (Fig. 10)
by the relative decrease in the amount of and 2P (Fig. 11) plies. These figures show data
carbonaceous material in the samples which are other than sulphur distributions and are referred
either dirty coals or from seam splits. to in the discussion of controls on sulphur in
Some samples on Fig. 6 show very high the seam.
percentages of total sulphur. These samples are The Parkgate Seam composite map (Fig. 7)
likely to include pyrite nodules and therefore shows a variation of sulphur contents from < 1
abnormally high values of are obtained (>25%). to >3%, with most of the seam being between

Fig. 7. The distribution of total sulphur in the Parkgate Seam (whole seam-less-dirt), showing fault trends.
Fig. 8. The distribution of total sulphur in the IPUT ply of the Parkgate Seam and the sandstone units above
the seam.

Fig. 9. The distribution of total sulphur in the 1PUB/1PM plies of the Parkgate Seam.
Fig. 10. The distribution of total sulphur in the 1PH ply of the Parkgate Seam and the relationship to seam
splitting (redrawn from Cavender & Spears i995a)

Fig. 11. The distribution of total sulphur in the 2P ply of the Parkgate Seam and the relationship to seam splitting
(redrawn from Cavender & Spears 1995a).
 SULPHUR DISTRIBUTION IN A MULTI-BED SEAM 257

2 and 3%. The spatial variation is considerable 12

with, for example, Ollerton Colliery showing a
generally lower sulphur content than Bevercotes 10
Colliery. However, this map does not accurately
represent the whole-seam sulphur as it would be i 9

mined since, it excludes the seam splits (dirt ~ 8 9 S~" *

bands). Maps of the main plies of the seam show ,- 9 oo 0
9 -

that the location of the area of maximum ~ 6 :.. ~ ~':

concentration of sulphur for each ply does not -~
:+ u s.-. 9
correspond. This is important since most maps -~ 4 4 _"~.~ 1'. .,,
used in the coal industry are usually composites,
indicating whole seam-less-dirt (e.g. Fig. 7). 2 +7,..
9 ,..'.--
Therefore these maps do not show the consider-
able vertical variation which may exist in seams 0
and hence, are of limited industrial use in multi- 1 2 3
bed seams of this type. total sulphur (1PH) %
Successful ply-by-ply mapping has been
achieved in most of the area studied due to the Fig. 12. Total sulphur in the 2P ply plotted against
high density of data points, however in some total sulphur in the 1PH ply of the Parkgate Seam
places (e.g. the easternmost extent of the 2P ply) (from Cavender & Spears 1995a).
data density is low and the distribution is
interpolated over several kilometres.
sulphur distribution in these plies are operating
differently, and therefore cannot relate to a geo-
Controls o n s u l p h u r c o n t e n t d i s t r i b u t i o n in logical structure which is geographically specific
the Parkgate Seam (Cavender & Spears 1995a). Plots of other
adjacent plies in the seam also show a similar
The fundamental controls on sulphur in coal relationship.
have been outlined by a number of authors Lack of control by faulting may be shown by
(Altshuler et al. 1983; Berner 1984; Casagrande, comparing the sulphur distribution with the
1987; Chou 1990; Calkins 1994). These are actual pattern of faulting. Figure 7 shows the
essentially the availability of sulphate, iron and faulting and the whole seam-less-dirt sulphur
organic matter. Sulphate is found naturally in content. Two sets of faults are observed,
sea water, and to a much lesser degree in trending WNW-ESE and NE-SW with varying
freshwater, therefore water salinity is an impor- throws of up to 60 m. Although fault planes may
tant factor affecting the sulphur content in peat provide pathways for pore waters within sedi-
and subsequently coal. Iron is required for the ments (Goodarzi et al. 1993), even the area with
fixation of sulphur in the form of pyrite, which as the most concentrated faulting shows no rela-
already indicated is an important fraction of the tionship to the pattern of sulphur distribution.
total sulphur in the Parkgate Seam. The presence The seam is not a horizontal unit varying
of organic matter, especially in a reactive form, from about 350 to 850m below O.D. over the
is necessary to control the bacterial reduction of area studied. Prominent within the area is the
sulphate, which converts the sulphate to a form crest of the Eakring Anticline (shown in Fig. 11)
in which it may be fixed in the sediment. which trends from the central southern part of
Both depositional and post-depositional con- the area to the NNW. If percolation of ground-
trois may effect the sulphur content within a coal water by structural processes occurs, it will
seam. The presence of pyrite nodules, which are encounter either the roof or the floor of the seam
of depositional origin, and pyrite in coal cleat, of first, and most likely the floor due to dewatering
clear post-depositional origin demonstrates this. of sediments lower in the succession. Figure 11
As indicated above little relationship is seen shows a sulphur high in the area of Bilsthorpe
between the sulphur contents of adjacent plies in Colliery in the 2P ply of the seam. This is near to
the Parkgate Seam (Fig. 12). This may be used the crest of the Eakring Anticline indicating a
to demonstrate the structural control on sulphur possible control. However other plies of the
in the seam is probably negligible. The two plies seam do not show a corresponding sulphur high
plotted are adjacent to each other in the seam in this area indicating that this control is
succession but are commonly divided by the unlikely.
X2P split. The lack of any linear trend in these Movement of porewater in sediments after
data indicates that the factors controlling the burial may be a potential source of sulphate to a
258 P. F. CAVENDER & D. A. SPEARS

coal seam (Spears 1991). A comparison of the seen. The 1PH (Fig. 10) ply also shows isolated
presence of permeable beds, such as sandstones, sulphur highs, where seam splitting occurs below
near or adjacent to the base of the seam and the it. These examples do not show a clear positive
sulphur distribution in the floor of the seam may relationship between sulphur content and seam
give some indication whether this process has splitting, although some indication of the role of
been in operation. Although not discussed in flooding events in controlling sulphur contents
detail here a study of sub-seam sandstone units is observed.
indicates that there is no apparent relationship Sandstone units above the seam may indicate
between their occurrence and the sulphur con- the presence of post-depositional channels which
tent in the 2P ply. developed after the cessation of peat accumula-
In most documented cases, depositional con- tion. These channels may have been a source of
trols are the most important on the sulphur sulphate allowing sulphur incorporation into the
distribution in the resulting seam. Although the resulting seam. Figure 8 shows the sulphur
depositional environment of the Parkgate Seam concentration in the uppermost ply of the seam
succession has not been discussed here, it has (1PUT), together with the sandstone channels
already been noted that previous publications and units above the seam (as mapped by British
indicate that there is apparently little marine Coal 1992b). However little relationship between
influence. The major seams in the Langsettian/ the sulphur content and the channels is seen.
Duckmantian succession of the coalfield have This is probably due to the fresh water nature of
mean total sulphur contents of between 1.3 and these channels which were thus an unlikely
3.0% (Allen 1995). source of sulphate. Figure 8 also shows the
The identification of depositional controls is trend of a swilley in the 1st Piper which also
complicated by the multi-ply division of the appears to have no influence on the sulphur
seam, and especially by the sulphur variations characteristics of the seam, this swilley is likely
from ply-to-ply. The base of the seam (2P) may to represent the course of a palaeochannel which
be expected to be influenced by the mire was later abandoned with the re-establishment
environment and geochemistry during peat of the mire (Elliot 1965).
accumulation, flooding events during and after The above discussion has excluded all post-
the cessation of peat deposition, and various depositional and a number of depositional
later diagenetic processes. The sulphur content controls as likely influences on the sulphur
in the 2P shows a great variation in sulphur distribution in the Parkgate Seam. However
content from <3% to >9%. The presence of although mappable depositional controls have
pyritic nodules, as noted earlier, would tend to not been identified complex controls which
suggest that pyrite is of a depositional stage operated in the mire are likely to have caused
origin, and is therefore related to processes the sulphur variations observed in the seam. At
operating in the mire. The occurrence of high the beginning of this discussion, sulphate avail-
sulphur contents at the base of seams, as shown ability was emphasised as a fundamental pre-
for the 2P ply has been noted by several other requisite for sulphur incorporation into a seam.
workers. Wandless (1959) indicates that sulphur Flooding of the coal-forming mire with sulphate
is often high at the roof and floor of a seam, as bearing waters therefore appears to be a likely
well as adjacent to dirt bands or seam splitting. control. Evidence for flood events is seen by the
This may be due to the less than optimum presence of seam splits within the seam and Fig. 1
geochemical conditions for peat accumulation and Table 1 show that a number of these exist
and organic preservation in these circumstances within the Parkgate Seam. However the flood
(Renton & Bird 1991). events which cause seam splitting may extend
The flood events which caused seam splitting beyond the mappable boundary of the split and
may have been possible mechanisms for the therefore their extent is difficult to map. These
incorporation of sulphate into the mire during flooding events may also be the source of Fe 2+ in
deposition, which may subsequently be fixed as detrital form, another important input for the
sulphur in the resulting seam. The presence of retention of sulphur in coal as pyrite. This does
seam splitting may therefore be a variable which not necessarily mean that coal with a high pyrite
can be used to demonstrate the occurrence of content will be high in ash. The Fe 2+ is likely to
high sulphur coal. A broad relationship is seen be sourced from other external sources such as
at the southern part of Fig. 11, with a greater porewaters, providing the right geochemical
sulphur concentration where seam splitting conditions persist (Spears 1991).
(X2P) has developed. However in the northern The swamp waters during this stratigraphical
part of the map where the split is in the form interval have commonly been suggested as being
of a 'channel' feature, no such relationship is of fresh-water fluvial type, with deposition in an
 SULPHUR DISTRIBUTION IN A MULTI-BED SEAM 259

upper delta plain environment (Guion & Fielding The authors wish to thank a number of people who
1988; Guion et al. 1995). However due to the low- have aided this research, especially John Rippon. Also
lying nature of this type of environment and acknowledged are Mike Cooke, Allan Goode and
nearness to base level there is a possibility of a John Raine. Acknowledgement is made to the British
Coal Utilization Research Association Ltd. and the
minor brackish influence, by mixing of saline and
UK Department of Trade and Industry for a grant in
fresh water inland from the base level itself. This aid of this research, but the views expressed are those
may be investigated further by using elements of the authors and not necessarily those of BCURA of
other than sulphur which are indicators of the DTI.
palaeosalinity. One such element is boron. In
the Parkgate Seam it has been demonstrated that
boron and sulphur show a high positive correla-
References
tion (Cavender & Spears 1995b). In addition
boron tends to be higher at the base of the seam ALLEN, M. J. 1995. Exploration and exploitation of
and sometimes the roof. Although boron is the East Pennine Coalfield. In: WHATELEY,M. K.
commonly in concentrations of < 5 0 p p m in the G. • SPEARS, D. A. (eds) European Coal Geology,
seam, representing fresh water influenced envir- Geological Society, London, Special Publication,
onments (Banerjee & Goodarzi 1990) some 82, 207-214.
ALTSHCULER,Z. S., SCHNEPEE,M. M., SILBER,C. C. &
samples have boron contents >100ppm and
SIMON, F. O. 1983. Sulphur diagenesis in Ever-
rarely >150ppm, indicating a brackish influ- glades peat and origin of pyrite in coal. Science,
enced environment. Therefore a rise in base level 221, 221-227.
may have caused the increased availability of BANERJEE, I. & GOODARZI, F. 1990. Palaeoenviron-
sulphate to the mire, from more brackish ment and sulfur-boron contents of Mannville
conditions, and resulted in plies with high (Lower Cretaceous) coals of southern Alberta,
sulphur contents within the seam. Canada. Sedimentary Geology, 97, 297-310.
The spatial variation within individual plies is BERNER, R. A. 1984. Sedimentary pyrite formation: an
more complex, since for example although the update. Geochimica et Cosmochimica dcta, 48,
605-615.
2nd Piper ply is generally high in sulphur
BRITISHCOAL, 1992a. Parkgate Seam database. British
content, there is a two to three-fold variation in Coal internal document.
the area studied. Intra-ply variations are likely to - - 1 9 9 2 b . Piper/Parkgate Seam, summary of geol-
be controlled by more subtle controls which are ogy. British Coal internal document (map).
unlikely to be preserved in the geological record BRITISH STANDARDS INSTITUTION, 1977. Methods for
as mappable features, such as palaeotopography Analysis and Testing of Coal and Coke, part 6.
and localized variations in iron availability and Total sulphur in coal. BS1016: Part 6: 1977.
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in coal: a review. Fuel, 73, 475-484.
CASAGRANDE,D. J. 1987. Sulphur in peat and coal. In:
SCOTT, A. C. (ed.) Coal and Coal-bearing Strata."
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Special Publication, 32, 87-105.
The initial part of this work demonstrates that CAVENDER,P. F. & SPEARS,D. A. 1995a. Assessing the
seams may be subdivided using different vari- geological controls on sulphur in coal seams:
ables into a number of plies and also that the progress towards predictive mapping. In: Desul-
distribution of sulphur in a seam plies may be phurisation, IChemE Symposium Series No. 138,
mapped given sufficient data points. This ply-by- 197-205.
ply mapping is of value since this study indicates -- & 1995b. Analysis of forms of sulphur in
coal, and minor and trace element associations
there is a considerable vertical and spatial
with pyrite by ICP analysis of extraction solu-
variation of total and forms of sulphur in the tions. In: PAJARES,J. A. & TASCON,J. M. D. (eds)
Parkgate Seam. Therefore mapping on a ply-by- Coal Science, 1653-1656.
ply basis will provide more in-depth information CHOU, C. L., 1990. Geochemistry of sulphur in coal.
than a composite map of the whole seam, which In: ORR, W. L. & WHITE, C. M. (eds) Geochem-
is commonly used in the coal industry. istry of Sulphur in Fossil Fuels. American Chemi-
It has been demonstrated that the sulphur cal Society Symposium Series No. 429, 30-52.
distribution in the Parkgate Seam is controlled EDEN,R. A., STEVENSON, I. P. & EDWARDS, W. N.
mainly by depositional processes, although some 1957. Geology of the country around Sheffield.
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late stage incorporation of sulphur does occur.
Wales). 3rd Edition.
These processes are highly complex and no EDWARDS, W. N. 1951. The Concealed Coal)qeM of
specific mappable controls have been identified. Yorkshire and Nottinghamshire. Memoirs of the
However these depositional processes are likely Geological Survey (England and Wales). 3rd
to be dominated by flooding events. Edition.
260 P. F. C A V E N D E R & D. A. SPEARS

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Memoirs of the Geological Survey (England and London, Special Publication, 82, 79-97.
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International Conference on Coal Science, Alberta, DUGAN, P. R., QUIGLEY, D. R. & ATRIA, Y. A.
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262 V. BOUSKA E T AL.

Table 1. Content of sulphur in the lignites of the North

NO. I =2.006 =1.578 min =0.030 __ normal. Bohemian Basin
4460 } =1.608 ~O =1,927 max -19.930 - - Iognorm.
Sample Ad Sd Sdo, Sd Sd
4014 I
3568 [ (%) (wt%) (wt%) (wt%) (wt%)
3122 I
Western part
2676 I Merkur
2230 I 3-333/94 17.59 5.99 2.11 2.26 1.62
7s4 I 1-332/94 8.18 1.68 0.09 0.09 1.50
1338 I 232/94 8.60 1.81 0.49 0.21 1.11
892 I 16-328/94 80.49 0.58 0.01 0.03 0.54
446 I 65/211 27.80 2.99 1.33 0.98 0.68
^
Liboug
2-342/94 13.30 2.87 1.22 0.32 1.33
66/211 25.50 3.64 1.38 0.81 1.45
A 67/211 34.09 2.93 1.52 1.25 0.16
N =11477 233/93 32.93 0.92 0.24 0.35 0.33
NO. I ~ -1.728 s -0.934 rain =0.O30 - - normal.
GD =1.774 max -19.930 - - Iognorm. Central part
2090 t 18.2 CM "1"4"85
CSA
46/211 10.93 5.19 1.51 3.13 0.55
1672 [
,,631
11'
/11 47/211 20.85 0.82 0.32 0.16 0.34
\ 48/211 29.52 8.67 2.35 4.45 1.87
1254
1045 [
I I II 234/63 4.69 0.73 0.01 0.05 0.67
Bilina
836 I
10-338/94 16.61 0.52 0.01 0.02 0.49
627 I
12/340-94 8.33 1.26 0.13 0.50 0.63
418 I 8-339/94 4.94 0.71 0.02 0.07 0.62
51/211 3.89 1.24 0.37 0.62 0.25
53/94 3.37 1.35 0.02 0.69 0.64
9
28-343/94 14.56 3.60 0.69 1.84 1.07
52/211 40.94 0.88 0.24 0.43 0.21
B Hlubina (1.M6j mine)
53/211 5.07 1.12 0.27 0.52 0.33
Fig. 1. Histograms of sulphur constructed for total
54/211 4.94 1.24 0.33 0.68 0.26
number of samples n = 14993 (A) and for the most
55/211 10.84 0.76 0.23 0.17 0.36
frequently occurring values (B). Sulphur values
57/94 4.13 1.45 0.04 0.52 0.89
correspond to wt%.
59/211 4.63 0.92 0.24 0.35 0.33
60/211 3.71 1.01 0.27 0.54 0.20
to occur within the whole basin but the lowest 61/211 27.29 0.87 0.25 0.50 0.12
contents are confined to the eastern and south- 58/94 8.59 1.45 0.04 0.52 0.89
eastern margin of the NBB (i.e. contents not 56/211 14.99 0.51 0.21 0.19 0.11
exceeding 1 wt% S in coal). Contents between 57/211 7.50 1.23 0.39 0.72 0.12
1 and 1.5 wt% S in coal are most frequent in the 58/211 2.83 1.39 0.40 0.69 0.30
southern segment of the central part of the NBB. Eastern part
Lower contents were also identified in the area 43-363/94 4.67 0 0 0 0
of the Zatec delta and its northern extension. In 44-364/94 14.60 0.24 0 0 0
contrast, high contents of sulphur (exceeding 62/211 5.66 0.36 0.21 0.11 0.04
54/94 3.65 0.30 0 0 0
1.5 wt%) occur along the northern margin of the
45-365/94 45.78 0.38 0 0 0
basin at the foot of the Kru~nhory Mts and in
the westernmost part of the NBB.
The content of the organic sulphur is rather
low (0.65-1.0 wt%; Hokr 1975) but an unusually 1981). Elemental sulphur was found only in
high content was reported from the Hrabfik burnt-out parts of the coal seam. Its origin is
mine (2.95wt%, Bou~ka 1981). Concentrations derived from reduction of iron disulphides at
of sulphate sulphur range mostly between high temperatures at the centre of the fire.
hundredths to tenths of a per cent, with a The largest component of sulphur in coal of the
maximum of 0.2wt%. Higher contents of NBB is pyrite (aggregates of microscopic dimen-
sulphate sulphur indicate local oxidation pro- sions) with a significant proportion of marcasite
cesses have occurred (Hubfi6ek 1964; Bou~ka (Zelenka et al. 1970). The content of sulphide
 ~345 OF IRON DISULPHIDES 263

sulphur varies considerably. Some local enrich- numerous volcanic bodies and pyroclasticsclose
ment with disulphides of iron has been observed to the basin (Doupovsk~ hory Mts, Cesk6
particularly in the lower part of the lower bench stfedohofi Mts). Volcanic activity preceded
of the coal seam. Another local enrichment and also followed the formation of lignite.
occurs in the upper bench in the central part of
the basin, along its northern margin. Higher
values of St~ were reported from the western part Iron disulphides confined to the coal seam
of the basin whereas in the eastern part, in the
of the NBB
vicinity of Chabafovice, the lowest concentra-
tions of St~ = 0.2-0.8 wt% occur (Zelenka 1993). Iron disulphides, the most abundant of which
Our data support this pattern (see Table 1). are pyrite and marcasite, occur in the coal seam
and are represented by three major genetic types
(Bougka 1981, Dubansk~ & Gottstein 1990):
Geological setting
(i) Synsedimentary type. The origin of disul-
The North Bohemian Basin (NBB) represents phides of this type is isochronous with the
the most important lignite basin in the Czech origin of coal. They originated during
Republic (Fig. 2). It is filled with Eocene to the biochemical and partly also geochem-
Miocene, exclusively continental, mostly fluvial ical stage of coalification (Bou~ka 1981,
and lacustrine sediments which were deposited Dopita et al. 1985). These disulphides are
in a subsiding rift zone on the Variscan therefore of syngenetic or early diagenetic
consolidated basement. A large peat bog devel- origin. Amorphous monosulphides were
oped in the North Bohemian Basin in the Early precipitated during this stage in the form
Miocene. A high to low volatile lignite seam, 30 of FeS.H20 or melnikovite, greigite,
to 40, locally even 60 to 70 m thick, was formed. mackinawite or even pyrite and marcasite.
Its formation was accompanied by extensive It is known that the bacterium Desulfovi-
mostly basic volcanism which gave rise to brio desulphuricans preferentially reduces

.r 9

f c ~ . , . t .''~

_ ,, ~

\ ,, ~\\\\ , ~ \ ~ ..~,~ '~'~,-~,>~J-" "kl\ '-'"~

~.~ " 0 50km

Fig. 2. Geological sketch map of the North Bohemian Basin and its vicinity: 1-4 Tertiary formations:
1, sediments of the Sokolov and Cheb Basins; 2, sediments of the North Bohemian basin; 3, effusive rocks and
pyroclastics of the Doupovsk6 hory Mts; 4, effusive rocks and pyroclastics of the (~esk6 stfedohofi Mts.
264 V. BOUSKA ET AL.

the lighter ion 32802- than the heavier ion accuracy -4-1.0% for total sulphur in lignite.
34802-. Consequently, the hydrogen Values of 634S of-0.6%0 correspond to pyrite
monosulphide which forms at the begin- and 634S of +3.2%o correspond to sulphate
ning of coalification is richer in the lighter sulphur. The amount of organic sulphur (0.85-
isotope of sulphur whereas the heavier iso- 2.9wt%) in lignite of the NBB is almost
tope concentrates in the residual sulphate negligible, and therefore the isotope 6348 value
solution. equal to +1.2%o is of little importance for the
Pyrite, in particular, represents the general assessment of isotopic composition of
characteristic synsedimentary variety of local sulphur.
disulphide. The mineral was identified by Dubansk~, & Gottstein (1990) indicated that
X-ray diffraction. It forms finely dispersed 634S values of synsedimentary and diagenetic
microscopic framboids and tiny veinlets types of iron disulphides in the NBB are similar
arranged mostly parallel with the bedding to each other. These authors believe that the
of coal and also layers of pyrite-bearing majority of disulphides in the NBB could have
sandstone which occur at the base of the originated through thiobacterial reduction of
coal seam in the western part of the NBB. sulphates. As the parent solution consisted
(ii) Diagenetic type. This disulphide formed of sulphates, then the disulphides showing
together with the coal seam, during its negative 634S values are considered to be
burial. Tiny veinlets of iron disulphides relatively younger than those exhibiting positive
usually filled desiccation cleats. 634S, thus higher values. However, these authors
(iii) Epigenetic type. This type is developed in do not provide an unambiguous explanation for
already formed coal seams in which the markedly negative 634S values found in epige-
iron disulphides were concentrated along netic disulphides among which marcasite is most
faults in form of marcasite twins and abundant. They assume that a sublimation
clusters of crystals or as crystalline aggre- process could have been involved. Rainswell
gates which filled cleats and fractures. (1982) considered that pyrite from Jet Rock,
which showed values -40%0 up to -43%0,
Dubansk2~ & Gottstein (1990) anticipated the formed through a reduction of sulphates in an
existence of iron disulphides of hydrothermal open marine environment with an unlimited
origin whose source was in the basement of the supply of sulphate ions. During the kinetic
coal seam. However, this type of iron disul- bacterial fractionation of sulphur isotopes the
phides has not yet been found in the coal seam
residual sulphates became isotopically heavier
of the NBB even though low-temperature (the 634Svalues of the residual sulphate and later
solutions could have occurred in the coal seam sulphides increase). The kinetic fractionation in
where some exothermal reactions might have a relatively fast low-temperature process of
taken place during the process of coalification bacterial reduction of sulphates causes pyrite
(Bougka 1981). Volcanic activity could have also originated through such a process to be depleted
played some role in accumulation of this type of in the heavier isotope of sulphur.
disulphide (Dubansk~, 1984).
The shift in isotopic composition of sulphur
between the source sulphate and the final
sulphides which originated through bacterial
Analytical methods reduction may vary considerably depending on
specific conditions; if the system for sulphate is
Separated samples of iron disulphides were closed or open, if there is enough nutrition for
oxidized under vacuum using CuO at a tem- bacteria, if the originating H2S is immediately
perature of 790~ The sulphur isotopic compo- fixed in sulphides or remains free, etc. In general,
sition of the generated SO2 gas was measured the major shifts in isotopic composition of
using a Finnigan MAT251mass spectrometer. sulphur between sulphate and sulphide are
Overall analytical error is +0.15%. characteristic of an open environment for sul-
phate or where there is unlimited supply of
sulphate ions (seas) which the bacteria drain to
form sulphides. In contrast to that, a minimum
Values of 6345 in lignite of the North shift, sometimes almost non-existant, can be
Bohemian Basin observed in the environment where the supply
of sulphate is limited, i.e. when all incoming
Hokr et al. (1972) provided the first data on sulphate is continually reduced. There is, of
isotopic composition of sulphur in coal of the course, a wide spectrum of various environments
NBB. They gave 634S values from - 1 to 0%0 with between these two extremes.
 ~34S OF IRON DISULPHIDES 265

Table 2. Variation in the sulphur isotopic composition o f the Krugnk hory Mts sulphides and sulphates and
disulphides of the North Bohemian Basin (NBB)

Samples (~348 range References

of values

Sulphides of the crystalline rocks of the Krugn6 hory Mts, -1 to +5%0 Smejkal et al. (1978)
Smr6iny and Slavkovsk~, les Mrs
Sulphates of the Miocene lake, thenardite (NazSO4) and +2 to +6%0 Smejkal et al. (1978)
gypsum as well as the sulfates of the Western Bohemian
Spa mineral waters
Estimated value for the sulphate supplying the Basin + 5%o Smejkal et al. (1978)
Volcanic sulphur from Cesk~ sffedohofi and Doupovsk6 ,-~0%o Smejkal et al. (1978)
hory Mts (estimate)
St for the coal of the NBB -1 to 0%o Hokr et al. (1972)
Pyrite from the coal of the NBB -0.6%o Hokr et al. (1972)
Sulfate sulphur from the NBB +3.2%o Hokr et al. (1972)
Organic sulphur in the coal of the NBB +1.2%o Hokr et al. (1972)
Synsedimentary (early diagenetic) pyrite (sample No. 23) -0.8%o this work
in claystone from the upper part of the coal seam,
Doly Bilina open-cast mine
Synsedimentary (early diagenetic) pyrite (sample No. 34) +0.8%o this work
in claystone from the upper part of the coal seam,
Doly Bilina open-cast mine
Framboids of synsedimentary pyrite (sample No. 65/291) -0.5%o this work
in coal, lower seam, Merkur open-cast mine
Very fine radially divergent aggregates of early diagenetic +0.5~ this work
pyrite (sample No. 37b) on the base of a big sandy lens,
Doly Bilina open-cast mine
Small crystals of synsedimentary pyrite (sample No. 37a) 0.0%o this work
on the base of a big sandy lens, Doly Bilina open-cast
mine
Synsedimentary pyrite, Velkolom (2SA open-cast mine -4.2%o Dubansk~ & Gottstein (1990)
Synsedimentary marcasites, +3.5%0 Dubansk~ & Gottstein (1990)
Velkolom CSA open-cast mine +2.8%o Dubansk~ & Gottstein (1990)
Diagenetic marcasites, - 3.1%o Dubansk~ & Gottstein (1990)
Velkolom CSA open-cast mine -3.3%o Dubansk~ & Gottstein (1990)
Diagenetic marcasites, M. Gorkij I, -3.3& Dubansk9 & Gottstein (1990)
Brafiany, today Doly Bilina open-cast mine -4.8%o Dubansk~,& Gottstein (1990)
Diagenetic marcasite, 1. M~ij mine, H~ije at Duchov, NBB -3.5%0 DubanskSI& Gottstein (1990)
Epigenetic layer of marcasite from the base of the sandy +4.2%o this work
clay layer (sample No. 39), Doly Bilina open-cast mine
Epigenetic pyrite concretion, the base of the 3 seam +5.8%o this work
(sample No. 42), Doly Nfistup Tu~imice, Libou~
open-cast mine, NBB
Crystals of marcasite (size up to 6 cm), Bilina tectonic fault +4.9~ this work
(sample No. 46), Doly Bilina open-cast mine
Radially divergent aggregate of epigenetic pyrite +11.5%o this work
(cubes of 2-3 mm, sample No. 33), Bilina tectonic fault,
Doly Bilina open-cast mine
Crystals of marcasite, near the Bilina tectonic fault +12.0%o this work
(sample No. 35a), Doly Bilina open-cast mine
Crystals of marcasite on the fine grained aggregate of + 12.6%0 this work
pyrite (sample No. 36), base of the coal seam, Doly
Bilina open-cast mine
Sulphate aerosols + flying ash from the power plant +0.1%o ~ern~, (1982)
Chvaletice -0.8%0 Cern~, (1982)
Sulphate aerosols + flying ash from the power plant -0.7%o Buzek & Sr~imek (1985)
Chvaletice
266 V. BOUSKA E T AL.

The isotopic composition of sulphur was thought to have been formed during later stages
studied on disulphides from the NBB, particu- of the whole process, i.e. during the diagenesis or
larly on pyrite and marcasite representing as epigenetic sulphides.
various genetic types which were examined by Smejkal (1978) estimated the ~534S values in
petrographic and geochemical methods prior to sulphates of a Miocene lake at the onset of
isotopic studies (Bou~ka & Pegek 1995). The sedimentation of the Cypris Formation in the
results obtained, together with other data are Cheb Basin to be +2 up to +5%o. Rather
summarized in Table 2 and Fig. 3. positive ~534S values in biogenetic pyrite of
The dissolved sulphate which supplied the the Cheb Basin, in comparison with those of the
NBB during the Miocene is believed to have been original sulphates, indicate that pyrite was
derived from weathered sulphides of the Krugn6 formed during an advanced stage of sulphate
hory crystalline complex, Smr6iny unit and reduction in a closed basin, most likely in an
Slavkovsk~, les region (Smejkal et al. 1974). undrained lake. Pyrites of the Cypris Formation
Consequently, based upon the knowledge of showed (see Smejkal et al. 1974) 634S values
isotopic composition of sulphides of these units varying between +7 and +45%0, the mean value
(-1 up to +5%o) and the fact that during being +16%o. In contrast to that, thenardite
syngeneous oxidation of sulphides no significant efflorescence and gypsum showed values exhibit-
shift in isotopic composition occurs, the sulphate ing a conspicuous peak between +5 and +6%0.
supplying the NBB should exhibit similar slightly These values are close to those of sulphates
positive 634S values. Volcanogenic sulphur is which occur in the majority of mineral waters of
considered to be less important. Its isotopic western Bohemia which argues for their similar
composition should be close to 0%o. The Teplfi- origin or source. Similar values were obtained in
Barrandian region, located to the south of the our samples no. 39, 42 and 46 (see Table 2).
NBB is characterized by accumulations of Some epigenetic sulphide types show higher
sulphides with low ~534Svalues averaging below ~534S values in the range from +4.2 to +12.6%.
0% (Smejkal et al. 1974). Obtained sulphur The formation of these sulphides is probably
isotopic compositions of sulphides from the NBB related to bacterial (or organic-matter related)
indicate that this unit was not the dominant reduction of the sulphate content of basinal pore-
supply of sulphur into the basin. waters. These pore-waters represent a residual
Shifts in the isotopic composition of sulphur sulphate reservoir already shifted to higher ~34S
in the studied samples compared with antici- values by previous stages of sulphate reduction.
pated values in source sulphates are rather small. Synsedimentary disulphides, mostly pyrites,
In general, the sulphides showing lower values which form microframboids or veinlets parallel
(around 0%0) were formed in larger reservoir of with bedding, show values close to 0%o (our
sulphates, and are believed to be of earlier origin samples no. 23, 34, 37a, 37b and 65/291- see
and synsedimentary. Sulphides exhibiting higher Table 2). These mostly control the overall
values were formed during later stages of isotope composition of sulphur in common
bacterial reduction when the isotopic composi- lignite samples. The synsedimentary disulphides,
tion of sulphates had already shifted towards showing various relative proportions, are dis-
higher ~348 values due to the previous drain of tributed through the whole section of the coal
sulphur isotopes into earlier sulphides. Conse- seam, except in the eastern part of the NBB
quently, the sulphides with high ~348 values are where they are less abundant.

Sulfide.s of the crys'(alline

I rocks (Kru~,n~ h.ory M~s]
Volcanic sulfur {Cesk~ st~edohoH,
Doupovsk~ hory M'(s)
Organic sulfur
Sulfate sulfur
Synsedimentary ( 'early
diagene'(ic) disulfides
I Epigene'dc disulfides
Aerosols *
flying ash, ChvaLe~ice
I J I t
910~ ~" S

Fig. 3. Diagram of plotted data from Table 2.

 ~34S OF IRON DISULPHIDES 267

The mean 6348 values established in the coal suggests that no considerable shifts in isotopic
of the NBB when compared with those of composition of sulphur take place during
atmospheric SO2 and sulphate ions in water, thermal oxidation process in power plants.
suggest that some fractionation and a certain
shift towards heavier values took place in the
atmosphere and water environments (Cern~, References
1982). Nevertheless, the combustion products
(ash and sulphate aerosols) of the Chvaletice BOUgKA,V. 1981. Geochemistry of Coal. Elsevier, New
power plant which burns lignite of the NBB York.
- - & PEgEK,J. 1995. Mineralizace uhelnf~eh slojL MS
showed /534S values equal to +0.1 and -0.8 Faculty of Science, Charles University, Prague.
(Cern~ 1982). Several measurements at the same BUZEK, F & SRAMEK,J. 1985. Sulphur isotopes in the
power plant (Buzek & Srfimek 1985) showed a studies of stone monument conservation. Studies
mean value of ~534S corresponding to -0.7%o in Conservations, London, 171-176.
which is close to the mean value of coal and (~ERN'I', J. 1982. Sledovdni pomdru stabilnlch izotopft
pyrite from the NBB. slry ve srd~kdch v Praze. MS Faculty of Science,
A certain but not too considerable shift may Charles University, Prague.
be caused by organic sulphur in the coal of the DOPITA, M., HAVLENAV. & PE~EK, J. 1985. Lo~iska
fosilnich paliv. SNTL, Prague.
NBB. However, the concentrations are small
DUBANSKY, A. 1984. Sulfidick~ mineralizace v uhli
and its isotope composition is known from only severo6esk+ hn6douheln~ p~nve. Uhli-Rudy, 32,
one measurement (Hokr et al. 1972). 223-231.
-- & GOTTSTEIN, O. 1990. Izotopick6 slo2eni siry
Fe-sulfidh z SHR. Uhli, 38, 301-305.
GOTrSTE1N, O. 1985. Vliv antropogenni (innosti na
Conclusions geochemii izotop~ siry. MS Institute of Applied
Geology, Czechoslovac Academy of Sciences.
Among the genetically different types (synsedi-
Report No II-6-2/03.102.
mentary, diagenetic and epigenetic) of iron HOKR, Z., KOHOUT, J., HLADiKOVA,J. 1972. ~34S v
disulphides (pyrite, marcasite) which occur in hnJd~ch uhllch severo(esk~ho baz~nu. MS Geo-
lignite of the North Bohemian Basin, the fond, Prague.
synsedimentary disulphides appear to be most RAINSWELL,R. 1982. Pyrite texture, isotopic composi-
abundant. They form fine dispersed microscopic tion and the availability of iron. American Journal
framboids or veinlets mostly parallel with of Science, Washington, 282, 1244-1263.
bedding. These disulphides show c534S values SME~KAL,V. 1978. Isotopic geochemistry of the Cypris
fluctuating around 0%0. Formation in the Cheb basin. VJstnik Ust(ednlho
flstavu geologick~ho, Praha, 53, 3-18.
These values when compared with those of
, HAUR, A., HLADiKOVA,J. & VAVIS.IN,I. 1974.
sulphur dioxide in gases of the Chvaletice power ISOtOpic composition of sulphur of some sedi-
plant, which burns lignite of the North Bohemian mentary and endogenous sulphides in the Bohe-
Basin, indicate that they correspond to mean mian Massif. Casopis pro Mineralogii a Geologii,
values of synsedimentary disulphides. This also Praha, 19, 225-237.
 Determination of different forms of sulphur in Yugoslav soft
brown coals
G. J A N K E S 1, O. C V E T K O V I ( ~ 2 & T. G L U M I ( ~ I C 2

1Faculty of Mechanical Engineering, University of Belgrade, 27.marta 80,

11000 Belgrade, FR Yugloslavia
2 IChTM, Center of Chemistry, Njegogeva 12, 11000 Belgrade, FR Yugoslavia

Abstract: This paper presents the results of determination of different forms of sulphur in
two Yugoslav soft brown coals, Kolubara (KOL) and Kostolac (KOST). The forms of
sulphur were determined as sulphate, monosulphide, pyrite and organic sulphur containing
compounds by step-wise oxidation with perchloric acid. The tests were carried out in an
inert atmosphere in Bethge's apparatus. KOL and Kost were quite different in sulphur
content, KOL containing 0.71wt% of sulphur and KOST 3.11wt%, as well as in the
distribution of each type of sulphur compound. Pyrite was dominant in KOST (1.89 wt%)
and organic sulphur in KOL (0.47wt%). The analytical method applied was simple and
good reproductivity of results was shown. It was important that all types of sulphur were
determined in a single and small sample, using the same oxidizing agent.

The Kolubara (KOL) and Kostolac (KOST) A number of techniques are available for SO2
deposits of soft brown coal are of utmost impor- control: (a) coal cleaning, (b) gasification (or
tance for electricity production in Yugoslavia. pyrolysis) with combustion and gas cleaning
They are located in northern and northeastern prior to combustion, (c) flue gas desulphuriza-
Serbia respectively (Fig. 1), over an area of tion, (d) combination of these techniques.
several hundred square kilometres. Geological Numerous commercial processes exist for each
research has shown that the carbonaceous layer of these tehniques. The price of electricity under
in Kolubara was formed sometime between the emission limit in force determines the
the upper and lower Pontian, on the edges of the possibility of applying these processes. Proper
Panonian sea, created from various types of choice depends on sound knowledge of the
marshland vegetation. The carbonaceous rocks quality and forms of sulphur in coal and possible
of Kostolac consist of two geological units, one ways of their transformation in different prosess
of them dating from the boundary between the conditions. There was a serious lack of informa-
Panonian and Pontian, while the other formed tion about this matter for domestic coals in
during the Pontian and early Pliocene. Accord- Yugoslavia.
ing to their chemical, mineralogical and petro- Sulphur compounds in coals are inorganic
graphic features, both are typical soft brown compounds, mainly sulphates, monosulphides
coals with a low degree of carbonation and a and pyrite, and organic compounds such as
variable petrographic composition (Petkovi6 & thiophenes, aryl-, cyclic-, aliphatic-sulphides,
Novkovi6 1975). as well as disulphides, which are minor compo-
There are six power plants located close to the nents (Atar 1978). Because of the diversity
Kolubara and Kostolac open cast coal mines of sulphur forms, estimation of various types of
near Belgrade, in the middle of an agricultural sulphur compounds in coal has always been an
and densely populated area. The total output of interesting, important and difficult analytical
these plants is 4860 MW and average emission problem.
of SO2 is 308 000 tonnes/year (Antic et al. 1992). Several analytical methods for the determina-
This means that the use of coal in electricity tion of inorganic forms of sulphur have been
production in the future will require limiting SO2 proposed (ASTM 1982; Tuttle et al. 1986).
emissions. There are no emmision standards in According to analytical procedures most often
Yugoslavia. At present emission standards for used, the monosulphide-type of sulphur was not
SO2, NO~, particulates, CO etc. are at a determined (its content was usually small). On
proposed stage, but their adoption has been the other hand, organic sulphur was always
postponed due to the existing economic situa- determined indirectly, as the difference between
tion. Currently, average SO2 emissions from total sulphur and the sum of inorganic forms
Kolubara and Kostolac coals exeeds the limits of sulphur.
determined by EEC environmental regulations In the determination of sulphur forms for small
(Federal Hydrometeorological Institute 1994). samples of KOL and KOST coals step-wise

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 269-272.
270 G. JANKES E T AL.

i i

L.~ ' ~ 0 50km

i
'~ 9
%
'I.
".,,.
.....

i
r.-.i
gOST ~'~

KOL

~,,r "~" ~,,

( -,%. ' 5 Cv
i 9 9 ".-

\ .7 ,r,
"~"% %
9 p- 9s " . . . .

k g
) ?
i9 .~./

Fig. 1. Map of Serbia showing the location of Kolubara and Kostolac coal fields.

oxidation with perchloric acid was used (McGo- size - 125 + 90 m. The characteristics of these
van & Markuzevski 1988) 9 The results are samples are given in Table 1 and the major
presented in this paper. constituents of the ash are presented in Table 2
(standard procedure according to the ISO 1171
was used for the ash analysis).
The same samples were prepared for wire-mesh
Experimental procedure devolatilization experiments where only 0.01 g of
coal was used for each test. Therefore, it was
The samples used in the experiment were important to determine the proportion of various
obtained from Kolubara and Kostolac coal forms of sulphur (sulphate, monosulphide, pyrite
mines and from coal seams which have been and organic sulphur-containing compounds) in a
for the past few years in exploitation. The very small sample 9This was done by successive
samples were obtained by a standard sampling treatment of the sample (300-500rag) with
method (ISO 5069-1), from the power plant perchloric acid solutions of different concentra-
conveyer belt. By means of a standard method tions, i.e. of different boiling points, as selective
of sample preparation (ISO 5069-2), 200 kg of oxidizing agents 9The tests were carried out in an
coal yielded 0.5 kg of sample each, with grain inert atmosphere (N2) in a somewhat modified
 FORMS OF SULPHUR IN YUGOSLAV BROWN COALS 271

Table 1. Characteristics of KOL and KOST 60 min. At the end of the reaction the content of
coal samples the flask was filtered and the filtrate was added to
the 30% solution of hydrogen peroxide. In all
Parameters Samples cases the concentration of sulphate was deter-
KOL KOST mined turbidimetrically and calculated as the
content of sulphur in the dry sample. Using this
Ash (wt%, dry basis) 35.12 37.12 method, all the types of sulphur compounds
Sulphur, total (wt% dry basis) 0.72 3.06 present were determined in a single sample with
Ultimate analysis (wt% dry ash free) the same oxidizing agent.
Carbon 54.81 52.70
Hydrogen 5.47 4.82
Nitrogen 0.80 0.79
Sulphur + oxygen (by differences) 38.92 41.69 Results and conclusions
Heating value (kJ/kg-1) The results of direct determination of sulphur
HHV 15880 14585 compounds in coal samples KOL and KOST are
LHV 15030 13625 presented in Table 3. They were compared with
the results of ultimate analyses of the same
samples presented in Table 1. The sum of all
sulphur forms determined by step-wise oxidation
Bethge's apparatus (McGovan & Markuzevski (Table 3) is assumed to be the total sulphur. This
1988). To determine the monosulphide and value for total sulphur ranged within the limits
sulphate forms of sulphur the samples were of microanalitical experimental errors. More-
treated with 40% HC104 at 115~ for 40min. over, the results were found to be reproducible
The hydrogen sulphide originating from mono- (McGovan & Markuzevski 1988; Cvetkovi6
sulphides, was introduced into 30% H202, where et al. 1995).
it oxidized and was determined as sulphate. It is shown that KOL and KOST are quite
Sulphate sulphur was determined from a filtrate different in sulphur content, as well as in
obtained by filtering and rinsing the sample at the distribution of each type of sulphur compound.
end of the reaction. Pyritic sulphur was deter- For example, KOL contains 0.71 wt% of sul-
mined in the sample residue. The oxidation was phur while KOST has 3.11 wt% (Table 1). The
carried out by 55% HC104 at 145~ for 90min. samples do not show significant differences in
The sulphur-containing gases were introduced ash content, but they are quite different in their
into 30% H20 2. After the termination of the content of pyrite, and organic sulphur (Table 3).
reaction the sample was filtered, rinsed and dried. The difference in total sulphur, as well as pyrite
The filtrate was added to the H2Oz-solution and sulphur content (KOL 25%, KOST 61% of
the sulphate content was determined in the total sulphur), in the samples analyzed may
combined liquid mixture. Finally, the organic point to difference in precursory matter and to
sulphur was determined by oxidation of the different conditions in the depositional environ-
residual sample with a mixture of 75% HCIO4 ment. A considerably higher content of pyrite
and concentrated H3PO4 (9: 1) at 200~ for sulphur (Table 3) and approximately identical

Table 2. Major constituents of ash (wt% )

Sample Constituents

SiO2 A1203 Fe203 CaO MgO K20 Na20 SO3 Total

KOL 55.8 22.4 11.3 4.7 2.0 0.4 0.5 2.9 100.0
KOST 45.9 20.9 16.4 9.2 2.8 0.4 0.3 4.1 100.0

Table 3. Sulphur forms in Yugoslav soft brown coals (wt%, d.b.)

Sample Monosulphide Sulphate Pyritic Organic Total

KOL 0.01 0.06 0.18 0.47 0.71
KOST 0.06 0.76 1.89 0.40 3.11
272 G. J A N K E S E T AL.

amounts of organic matter in both samples References

(Table 1) indicate that KOST coal was formed in
a more pronounced reducing environment than ANTIC et al. 1992. Study: Analyses of possible applica-
KOL coal. Regardless of the amount of Fe in tion of flue gas cleaning processes - FGD and NOx
the samples under consideration, which differs control (in Serbian). Mechanical Faculty, Uni-
significantly (Table 2), in the KOL sample most versity of Belgrade, Mining Institute, Belgrade,
of the sulphur (66% of total suphur) is bound to Energoproject, Belgrade
AYrAR, A. 1978. Chemistry, thermodynamics and
organic matter, because the reducing environ- kinetics of reactions of sulphur in coal-gas
ment was not as pronounced. reactions: A Review. Fuel, 57, 4, 201-212.
The results of organo-geochemical analysis of BERNER, A. R. 1984. Sedimentary pyrite formation:
aliphatic hydrocarbons isolated from the soluble An update. Geochimica et Cosmochimica Acta, 48,
part of the organic matter of the above coals 4, 605-615.
have also shown up difference in the character of CVETKOVI(~, O., GLUMI(~It~, T., DRAGUTINOVIC, V. &
the depositional environment. Reducing condi- VITOROWC, D. 1995. Determination of different
tions in the depositional environment are forms of sulphur in Aleksinac oil shale and
charactered by a predominance of phytane as evaluation of their pollution potential. I Regional
Symposium: Chemistry and Environment,
opposed to pristane, i.e. (Pr/Ph < 1 (Didyk et al. Vrnja6ka Banja, 107-110.
1978)). The ratio of Pr/Ph<_ 1 in the KOL DIDYK, B. M., SIMONEIT, B. R. T., BRASSELL,S. C.
sample, and Pr/Ph<< 1 in the KOST sample EGLINTON, G. 1978. Organic geochemical indica-
(Table 3) points to a more pronounced reducing tors of paleoenvironmental conditions of sedi-
condition in the depositional environment of mentation. Nature, 272, 216-222.
organic matter at KOST (unpublished results). FEDERAL HYDROMETEOROG1CAL INSTITUTE 1994.
Pyrite and organic sulphur transform to SO2 National review on strategy and policy of air
during combustion and contribute to air pollu- polution abatment in Federal Republic of Yugosla-
tion. The share of these two forms of sulphur via, Belgrade.
JANKES, G., CVETKOVIC, O., GLUMI(~I(~, T., MILOVA-
in total sulphur is 91% for KOL and 74% NOVIC, N. 1995. Rapid devolatilization of lignite
for KOST. The difference in suphur forms Kolubara (in Serbian), Chemical industry, Bel-
indicates different behaviour during combustion. grade, 49, 7-8, 317-321.
It also points, however, to different possible McGOWAN, W. C. & MARKUZEWSKI,R. 1988. Direct
desulphurization strategies. Pyrite sulphur, determination of sulphide, pyritic and organic
which predominates in KOST, indicates the sulphur in a single sample of coal by selective,
possibility of applying coal-cleaning techniques. step-wise oxidation with perchloric acid. Fuel, 67,
KOL, where organic sulphur is dominant, 8, 1091-1095.
PETKOVIC, K. & NOVKOVlC, M. 1975. Geology of
requires more detailed research into ways of
Serbia. VII Kaustobiolites (in Serbian), Faculty of
transforming the sulphur compounds. This Mining and Geology, University of Belgrade,
should provide necessary data for the selection Belgrade, 144-186.
of the gas desulphurization technique which TUTTLE, M. L. et al. 1986. An analytical scheme for
could be applied to achieve the required reduc- determining forms of sulphur in oil shales and
tion of SO2 emission. associated rocks. Talanta, 33, 953-961.
 Origin of vanadium in coals: parts of the Western Kentucky (USA)
No. 9 coal rich in vanadium
P. I. P R E M O V I C 1, N. D. N I K O L I C l, M. S. P A V L O V I C 2,
LJ. S. J O V A N O V I C 1 & M . P. P R E M O V I C 1

1 Laboratory for Geochemistry and Cosmochemistry, Department o f Chemistry,

University o f NiY, P.O. Box 91, 18000 Nig, FR Yugoslavia
2 Institute o f Nuclear Sciences Vin(a, 11000 Beograd, FR Yugoslavia

Abstract: The existence of vanadyl (VO2+)-non-porphyrins (P) in a thin band (enriched with
vanadium) of the Western (W.) Kentucky (KY) No. 9 coal seam was shown by electron spin
resonance (ESR). The ESR analysis indicates that VO2+-non-P are associated with the coal
organic insoluble fraction. ESR parameters show that VO2+ ion is in an environment with
approximately axial symmetry and chelated possibly by carboxylic/phenolic oxygen ligand
donor atoms. These parameters are compared with those of VO2+-fulvic acid complexes and
the model complexes with salicylic/phthalic acids reported by others. It is concluded that the
vanadylation of W. KY No. 9 thin coal band occurred during its diagenetic (peat-forming)
stage in the Pennsylvanian swamp. The extraordinary V enrichment of the top 15 cm,
relative to the lower parts of the W. KY No. 9 coalbed is interpreted by a high V
concentration of the past swamp water attained through a sudden and exceptional external
supply. The predominant source of the metal was probably volcanic ash on the land that
was weathered/leached of its vanadium. The association of V/Cr (together with their
enrichment in the top of the seam) and Ni implies that the volcanic ash was derived from
basalts. Abundant organic (humic) materials (with the high V enrichment factor) and low
rate of deposition were the primary factors responsible for the high vanadium content of the
coal. From the chemistry of VO2+, FeS2 and CrOH 2+ it is deduced that the oxidation
potential Eh and pH of the ancient peat interstitial water were approximately -0.2 to
-0.3 V and 5-6, respectively.

The presence of vanadium in US coals is well (LLM) limestone and Serpiano (Se) marl. Finally,
documented. Much analytical data (Zubovi6 Nissenbaum et al. (1980) detected VO2+-P in
et al. 1961; Zubovi6 1966; Cahill et al. 1976; the DS asphalt float (Israel) using ESR.
Swaine 1976, 1977; Valkovi~, 1983) have been The average V content of US coals is 20 ppm
compiled because the metal has a significant (Valkovi6 1983). However, the concentration in
effect on coal conversion processes (catalyst certain parts of some seams exceeds 2000 ppm
poisoning) (references in Maylotte et al. 1981). (Zubovi6 1966), e.g. the Western K Y No. 9
In addition, vanadium contributes to harmful seam. Recently, Maylotte et al. (1981) applied
physiological effects (e.g. lung disease) arising the V-XAFS to probe the chemical and struc-
from the industrial combustion of coal and the tural environment of V in the parts of this
resultant ejections of vanadium derivatives into coalfield (Providence mine, Union County,
the atmosphere (Rehder 1991). Fig. 2) enriched with V. According to these
The discovery of the ESR signals of voZ+-P in authors the metal exists as V 3+ and VO 2+ in
the petroleums and asphaltenes by O'Reilly both of which it is bound to oxygens. Maylotte
(1958) prompted researchers to apply the tech- et al. (1981) also found that the the predominant
nique for the detection and approximate quanti- form of V in the so-called heavy fraction of the
fication of low concentrations of VO2+-P in K Y coal (specific gravity>_1.4gcm -3) is very
various carbonaceous geological materials with- similar to roscoelite of V203 with V 3+ with
out recourse to extraction (Premovi6, 1978). octahedral oxygen coordination. On the other
Hocking & Premovi6 (1978) were the first to use hand, V in the light fraction (_<l.3gcm -3)
this technique to study voZ+-P in the coal/coal- appears to be predominantly as VO 2+ in an
like inclusions of the Athabasca tar sand. oxygen environment with no evidence for VO 2+
Premovi6 (1984) and Premovi6 et al. (1986) coordinated with N (such as voZ+-P) or S.
applied ESR to estimate the distribution of The purpose of the present report was to carry
VO2+-P in the bitumen and kerogen fractions of out a geochemical and other investigations of V
ancient shaly-type sediments: the La Luna Mara and VO 2+ ions (by ESR) present in the coal

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 273-286.
274 P. I. PREMOVIC ET AL.

parts (rich in V) of the W. KY No. 9 seam. distilled water to pH 7. After drying, the insoluble
It was expected that these studies might yield organic concentrate was again exhaustively
additional information of interest as a contribu- extracted with benzene/methanol azeotrope
tion to the general understanding of the origins until the solvent siphoning to the flask was
of the coals enriched with V. clear. Material was dried at 80~ and stored
in a desiccator.

Experimental procedure
Elemental analysis
Sample preparation and pyrolysis
Elemental analysis of the coal organic insoluble
The coal samples were ground to a fine powder fraction (Table 1) for C, H and N was done on a
(200-400 mesh) with a ball mill and Soxlet LECO Model 600 C H N Determinator while S
extracted exhaustively with benzene/methanol was determined on the L E C O Model SC 32
azeotrope to remove soluble organic material Sulfur Analyzer. O was determined by difference.
(bitumen). The extracted rock was treated with
20% hydrochloric acid (HC1) to remove carbo-
nates. After filtration and washing, the remaining Reflectance measurement
minerals were acid leached by digestion for 72
hours at room temperature using 1:1 by volume The coal sample was mixed with an epoxy binder
mixture of concentrated hydrofluoric acid (HF): in a plastic mould and cured overnight. The
48% and HCI: 20%. The mixture was filtered and grain mount was ground and polished. Max-
the residue washed successively with boiling imum reflectance measurement (%R0, max) was

Table 1. Geochemical analyses of KY 9

(a) Chemical analysis

Fraction Cold HCI* Boiling HCI HF* Organic

:kl% 16.5 3 3 77.5

Organic fraction soluble insoluble
+1% 6 94

* The HCI/HF fraction

(b) Distribution of V[-4-1Oppm], voe+[zklOOppm], Cr[-4-1Oppm] and Ni[+lOppm]

V VO2+ Cr Ni

Whole coal fraction 1000 500 70 40

HC1/HF 1800 n.d.* 135 130
Organic insoluble 800 650 50 15

* n.d. not detected

(c) Elemental analysis (+0.5%, moisturefree): organic insolublefraction*

C H H/C N S Mineral matter O (diff.)

67.5 4.5 0.8 1.0 7.0 5.0 13.0

* Total acidity 1 • 0.4 g eq kg -~

(d) M6ssbauer analysis

Form of Fe FeS2 Jarosite

+0.5% 96.0 4.0%

Sample number: 15
 ORIGIN OF VANADIUM IN COALS 275

carried out by means of a Zeiss MPM II nitrosodisulfonate (Fremy's salt) for which
microscope, fitted with white halogen/UV g=2.0055+0.0001 and the nitrogen hyper-
HBO light sources and using an Epiplan fine splitting, aN---1.3094-0.001mT (Faber &
(Neofluor) oil immersion objective (noil = 1.518 Fraenkel 1967). A quartz sample tube (approxi-
at 546nm). (%R0, max) was recorded on mately 2mm o.d., 0.8mm i.d.) was used for
vitrinite. Fremy's solution (c. 10-3 M) that was taped on
the exterior of the tube.

Acidity determination
Total acidity of the coal organic insoluble
Scanning electron microscopy ( S E M ) and
fraction was determined by exchange with electron microprobe analysis
barium hydroxide measuring the amount of
The coal sample was examined by SEM and
barium uptake (Schafer 1970).
energy-dispersive X-ray (EDX) spectroscopy
with a JEOL JSM 5300 electron microscope
equipped with a Link System QX 20003 EDX-
Acid leaching spectrometer. Operating conditions for EDX
analysis were 30 keV accelerating voltage, 0.1 #A
1 g of the coal organic insoluble fraction was beam current and a beam spot diameter of
refluxed for 30 days with 100 ml of 6 M HCI. The approximately 3 #m.
leached residue was removed by centrifugation,
carefully washed with distilled water (again by
centrifugation) until free of CI-, and then
thoroughly dried over P205 in a vacuum desic- X-ray absorption fine structure
cator at room temperature. The dried residue (XAFS) spectroscopy
was then analyzed for VO 2+ by ESR.
The S XAFS experiments were conducted at
beam-line X-19A at the National Synchrotron
Emission spectrometry Light Source (NSLS) at Brookhaven National
Laboratory (New York, USA). Electron ener-
A PGS-2 plane grating spectrograph (Carl Zeiss, gies were 2.53GeV and beam currents were
Jena) was used with an attachment for photo- typically 90-200mA. A silicon (111) double-
electric detection, an arc plasma excitation crystal monochromator was used to vary the
source, and a Bausch and Lomb diffraction X-ray energy from approximately 50 eV below
grating as the monochromator (Marinkovi6 & to 300 eV above the S K-shell absorption edge
Vickers 1971). (2472eV). The experiments were done in the
fuorescent mode, using a fluorescent ionization
detector described elsewhere (Huffman et al.
1991). Further details concerning XAFS are
Atomic absorption spectrometry (AAS) found in Huffman et al. (1991).
A Perkin-Elmer model 4000 atomic absorption
spectrometer was used with a Perkin-Elmer
platinum hollow-cathode lamp and a nitrous
oxide/acetylene burner head.
M6ssbauer spectroscopy
The M6ssbauer absorption spectrum was
obtained using a constant-acceleration M6ss-
Electron spin resonance (ESR) bauer spectrometer of standard design at
US Steel Corporation, Research Laboratory,
ESR measurements were performed on finely Monroeville (USA). The multichannel analyzer
ground powders of (unheated and heated) featured a dual-input module enabling simulta-
geological samples which were transferred to an neous accumulation of a sample and calibration
ESR quartz tube (4 mm o.d., 3 mm i.d.). Spectra spectrum of an Fe foil; isomer shifts were
were recorded on a Bruker ER 200D ESR measured with respect to metallic Fe at room
spectrometer employing 100kHz modulation temperature. Source consisted of c. 30 to 80 mCi
and a nominal frequency of 9.5GHz. The of 57Co in a Pd matrix. Further details concern-
g-values and hyperfine coupling constants were ing M6ssbauer analysis are found in Huggins &
determined relative to a solution of potassium Huffman (1979).
276 P. I. PREMOVIC ET AL.

Results and discussion

system formation
Depositional environments, and the coal
samples' thermal history z
D

The Springfield (W. KY) No. 9 coal of the 3[

Carbondale Formation (Middle Pennsylvanian, tY-
uJ
Fig. 1) in the W. KY coalfield (Fig. 2) of the o.
Illinois Basin (correlative with the Illinois No. 5
and Indiana No. V coals) is the most abundant
coal in the W. KY coalfield. The W. KY No. 9
coal was deposited when coastal/deltaic swamp Z :~
environment (peat-forming system) covered m

z
large areas of the W. KY Basin (Rice et al. <
>
1979). The climate at the time of the peat/coal .u -----'Carbondale' -KY9
>,.
deposition was tropical to subtropical (Hower &
Wild 1982). Coal rank varies from high volatile
A bituminous (hvAb) to hvCb bituminous.
V (and Cr) is enriched in the ash at the top of the Q,,,
coal in the western portion of the field. Ni, Zn,
..I
Cu, and Co can also be concentrated in the top
benches, but the trend is not as consistent as the z
V/Cr enrichment (Hower et al. 1990b). Hower <
n
et al. (1983, 1990a, b) considered that hydro- ft.
i
thermal metamorphism generated some of hvAb if)
coals in the Union coalbed (near the W. KY
Fluorspar District, Fig. 2) against the back-
ground of hvCb rank. In addition, these authors
suggested that the hydrothermal fluids deposited
relatively high concentrations of metals such as Fig. 1. KY 9 within the Pennsylvanian system.
Ba and Zn in this coalfield.
The coal samples used in this study came comm.). The elemental analysis of the coal is
from the top 15 cm of the W. KY No. 9 seam shown in Table 1. The coal is rich in vitrinite
at Providence mine containing 1000ppm V (around 80%). Vitrinite maximum reflectance
(Table 1). Parts of the seam are exceptionally measurement (%Ro, max=0.60) indicates that
high in V up to 1800ppm (Maylotte, pers. the coal under study belongs to hvCb rank.

Fig. 2. The W. KY and Illinois (Saline and Gallatin counties) coalfields (approximate (shaded) outline of the
lateral distribution of coal samples rich in V). KY: U(nion), W(ebster), H(opkins), D(avies), He(nderson),
Mc(lean), M(uhlenberg) and O(hio) counties; Illinois: G(allatin) and S(aline) counties.
 ORIGIN OF V A N A D I UM IN COALS 277

Throughout this paper the top 15cm part of the spectrum implies that the VO2+-non-P sites
the W. KY No. 9 coal (enriched with both V have axial symmetry, aside from any possible
and VO 2+) will be referred to as K Y 9 unless rhombic distortions much smaller than the
otherwise specified. linewidth of 1 mT. In this case all the spin-
Hamiltonian parameters can be derived from
this ESR spectrum using the axially symmetric
spin-Hamiltonian
E S R of VO 2+ and V-XAFS study
=/3o[gflHzSz + g• + HySy)]
Figure 3 shows the ESR spectrum of VO 2+
incorporated into the KY 9 matrix. One sees five + AII(S.Iz) + A• + Syly)
of the weak parallel components of the spectrum
at the extremites, two at low field and three at where gll, g• AIjand A l are the parallel (z) and
high field. The remaining ones are masked by perpendicular (x,y) components of g and 51V
the much stronger perpendicular components in hyperfine coupling tensors, respectively. Hi, Si
the centre of the spectrum. There are two and L represent the vector components of the
obvious points. First, all of the coal VO 2+- magnetic field, electron spin, and 51V nuclear
non-P sites have the same magnetic parameters spin along the i(= x, y, z) axes.
since there is only one set of lines in the Experimental ESR spin-Hamiltonian para-
spectrum. Second, the absence of any small meters for the VO 2+ compounds in KY 9 (given
splittings of the perpendicular components of in Fig. 3), however, differed significantly from

]S,v

~20 mT

I ..I , 1 51~11

Fig. 3. First derivative, room temperature, X-band spectrum of VO 2§ within the insoluble organic fraction
of KY 9. ESR parameters: All = 17.6 4- 0.2 mT, A• = 5.7 • 0.4 mT; gLL= 1.951 + 0.003, and g• = 1.985 :t=0.010
(for VO2+-P, Premovi6 1984); All --- 19.2 + 0.3 mT and A• = 6.9 + 0.5 mT; gll --- 1.937 • 0.005, and
. . - . ; ~ . ~ ~ . - " . , " .

~111_-11~931m~0a~d (Af~176 ~93ur~Tc Aa~d in7 t5hmT(f~ Te~ McBa~eel9~8~b);

AII = 19.9roT and A• = 7.5mT (for the VO2+-fulvic acid in the deep peat, Abdul-Halim el al. 1981); and
All -- 19.2 mT, A• = 6.8* mT (for the VO2+-phthalate/salicylate mixture, Templeton & Chasteen 1980).

* Calculated as mean value of hyperfine couplings (A:,x and Ayy) derived from a non-axial spin-Hamiltonian.
278 P. I. PREMOVIC ET AL.

those of VO2+-P (Fig. 3). It has been shown VO 2+ in VO2+-non-P. However, they are cer-
that these parameters are particularly sensitive tainly consistent with this interpretation.
to direct ligand substitution in VO 2+ complexes Further support for this notion comes from
(Holyk 1979). Thus, the differences in ESR XAFS investigation of V in KY 9 by Maylotte
parameters, especially All (which is the most et al. (1981). This study shows that there is no
sensitive parameter to the bonding) can repre- evidence of V in the N environment (such as
sent the differences in the bonding ligands voZ+-P). The limit of detection using the
around VO 2+ in a VO 2+ complex. Model V XAFS method was about 50 ppm for VO 2+.
compound studies have shown this to be valid Therefore, one may safely conclude that VO 2+-
(Holyk 1979). For this reason, a comparison of non-P are located within the KY9 organic
the spin-Hamiltonian parameters for VO 2+ in structure and that they are coordinated with
KY9 and voZ+-P of various bituminous the oxygen ligand donor atoms. These atoms are
sedimentary rocks (Fig. 3) implies that VO 2+ arranged in a nearly octahedral system with a
compounds in the coal are of non-P type. Our strong tetragonal compression along the V-O
ESR signal intensity indicates that the concen- bond of VO 2*. It is probable that coordination
tration of VO2+-non-P incorporated into KY9 is primarily by carboxylate/phenolate groups
is around 600ppm of VO 2+, that most of the with their four oxygen ligand donor atoms in the
metal (60%) resides in an organic-insoluble equatorial plane of VO2+-non-P, which concurs
phase and that 80% of this V is in the VO 2+ with the known chelating functional groups of
form (Table 1). unoxidized/oxidized coals. In the free axial
The high value for All (19.2mT, Fig. 3) position, perhaps, there is one water molecule/
indicates that the VO 2+ ion incorporated into hydroxyl ion (OH-).
KY9 coal is probably complexed with oxyge-
nated functional groups such as carboxylic/
phenolic. The All and A l of voZ+-non-P are Pyrite ( F e S e ) and other S compounds
very similar to those reported VO 2+ ions
incorporated into the structure of soil humic EDX analysis shows that the KY9 sample
acid (McBride 1978) and fulvic acid isolated contains relatively high Fe (_>2% of total
from either a podzol soil (Templeton & Chasteen sample weight); SEM and chemical analysis
1980) or an organic-rich deep peat (90% organic indicates that most of this Fe is in an unoxidized
matter, Abdul-Halim et al. 1981) (Fig. 3). It is form. M6ssbauer spectroscopy reveals that 96%
suggested by these authors that these ions are of total Fe present in KY 9 is pyritic Fe and only
bound to (carboxylic/phenolic) oxygen ligand 4% appears as jarosite (the iron sulphate
donor atoms in the humic/fulvic acid structures. mineral). This mineral is usually present in
It is interesting to note that most of V is weathered coals; presumably weathering product
concentrated in the fulvic fraction of modern of FeS2 (Huggins & Huffman 1979). According
peat (Cheshire et al. 1977). to Smith & Batts (1974) the Fe sulphates
In an effort to model the binding environ- (as weathering products of FeS2) in the coals are
ment, ESR spectra of many fulvic acid solutions only of significance in relationship to very recent
containing a variety of ligand mixtures were secondary processes.
studied by Templeton & Chasteen (1980). Very recently, we have initiated in situ XAFS
Particular emphasis was placed on the salicy- measurements of KY 9 part. Analysis of the data
late/phthalate mixture because, it is generally are still under way and only a few preliminary
thought that carboxylic/phenolic structures are results will be discussed here. The S K-edge
the probable functional groups present in fulvic XAFS spectrum of KY 9 (Fig. 4) can be resolved
acid. In addition, as these authors pointed out in terms of two major general form components,
the fulvic acid used in their investigation are unoxidized and oxidized. One of the unoxidized
characterized by a preponderance of such forms is the inorganic sulphide derived princi-
groups. For this reason the ESR (All and A• pally from FeS2 (associated with the organic
hyperfine parameters for this model salicylate/ insoluble part). The SEM and EDX analyses
phthalate complex are given in Fig. 3. The indicate that all macerals of KY9 contain
similarity in the (AlL and A• values (Fig. 3) substantial FeS2, especially inertinite in which
suggests that the ligand fields about VO 2+ are FeS2 is the dominant S form. The other
comparable for VO2+-non-P and for the fulvic unoxidized forms are aliphatic sulphides and
acid complexes on the model (salicylic/phthalate) aromatic thiophenes. Oxidized forms include
compound. The ESR data, of course, alone do sulphate which can conceivably be derived from
not constitute proof that carboxylic/phenolic both inorganic and organic S compounds. The
groups make up the first coordination sphere of fact that sulphate is present in KY9 (Fig. 4)
 ORIGIN OF VANADIUM IN COALS 279

t- Origin o f VO2+-non-P
Py T si4
O
L ul Coals have two major stages of formation:
,Q
(a) a diagenetic or peat-forming stage that is
,< controlled by biological activities; (b) coalifi-
cation stage in which temperature, time and
pressure are important. In the coalification
sequence: peat ~ lignite ~ subbituminous coal
---, bituminous (hvCb ---,hvBb ~ hvAb) coal the
Zo ,~" , i ' I ' I 11
i
115
content of oxygenated functional groups dra-
-8 -4 0 4 8
matically decreases, reaching its minimum with
Energy, eV (Elemental sulfur) bituminous material. Hence, the first three
Fig. 4. XAFS spectrum of S in KY 9: Py (FeS2); Su members of this sequence have a much higher
(sulphide); T (thiophene); and, 804 (sulphates). capacity of complexing VO 2+ ions from aqueous
solution than the fourth one (Szalay & Szilagyi
1967). Thus, VO 2+ ions could be incorporated
into KY 9 in any of these sequential phases.
strongly suggests that this part has been altered The hvb coals subjected to air oxidation at
by natural weathering or induced oxidation. moderate temperatures (< 150~ are character-
Experimental evidence suggests that primary ized with good cation-exchange properties. This
sedimentary FeS2 forms in anoxic depositional is attributed to acidic (carboxylate/phenolate)
environments provided that organic matter, groups (the cation-exchange sites) formed during
dissolved sulphate, S-reducing bacteria and a the oxidation process (Chandra 1982). In fact,
source Fe co-occur in sufficient quantities these groups are excellent coordinating sites in
(Berner 1970). Many authors have noted that the coal structure which would be rapidly filled
peats accumulating in brackish to marine by VO 2+ ions (and other cations) through uptake
environments tend to be enriched with S from aqueous solution under suitable physico-
content, while fresh-water, peat-forming systems chemical conditions. Preliminary measurements
tend to produce coal with a lower S content. indicate that total (carboxylic/phenolic) acidity
Studies of modern peat-forming environments, of the K Y 9 organic insoluble fraction is
however, show a substantial increase in the FeS2 1-t-0.4geqkg -1 (Table 1) which may (theoreti-
content of peats forming in marine-influenced cally speaking) bond up to 33 500ppm of VO 2+
environments (such as ancient W. KY swamp) ions from the aqueous solution.
(Casagrande et al. 1977; Altschuler et al. 1983). Hower & Davies (1981) estimated that the
A 150 to 600 mm thick marine bituminous shale W. KY Pennsylvanian coals attained maximum
overlies the W. KY No. 9 coal over much of its burial (2-3 km) by the end of the Permian and
extent. Since the marine sediment lies directly were uplifted to near the present surface by the
above the roof of W. KY No. 9 coalbed, it is middle of the Cretaceous. It is clear that
probable that encroachment by the sea occurred prolonged weathering of K Y 9 had to be
very soon after, or even terminated, the final initiated/advanced during this near-surface stage
peat-forming stage. In this event, the organic of its burial. In aerated natural (subsurficial/
material could be expected to be extremely meteoric) waters (such as those which have been
reactive and a very rapid and complete reduc- in contact with KY 9 since its uplifting by the
tion of sulphate to sulphide (HzS/FeS2) by middle of the Cretaceous), V is predicted to
organic/biological reactions could occur. It is, occur in the +5 oxidation state as the vanadate
also, probable that some sulphate necessary for H,VO~ -3 ion (Wanty & Goldhaber 1992). As a
bacterial production of HzS/FeS2 in the W. KY consequence, the V species involved in the
No. 9 ancient swamp had arisen as a result of adsorption process in an oxic milieu appear to
the downward diffusion of the dissolved sul- be anionic, resulting in a relatively low affinity
phate in the overlying seawater. High contents for the cation-exchange (carboxylate/phenolate)
of FeS2, VO 2+ and polyaromatic paramagnetic sites in the coal (Van der Sloot 1976).
structures (PPS): c. 45 x 1019 spins g-a in the At this stage it is more likely that the
coal, as determined by ESR, is consistent with vanadylation of KY 9 occurred during its peat-
this depositional model (Premovi6 1992; Pre- forming stage. It is unlikely that a process would
movi6 et. al. 1993). Thus it seems reasonable to be introduced via subsurface water during the
conclude that FeS2 is formed during early lignite/subbituminous phases of the coal-forming
diagenesis of KY 9, especially that incorporated process. The subsurface water contains no
into the maceral matrixes. appreciable amount of V, regardless whether
280 P. I. PREMOVIC ET AL.

the source of water is meteoric (including vadose), that there is no indication that the bituminous
connate or juvenile (White 1965; Overton 1973). shale which overlies W. KY No. 9 coal is a likely
Casagrande & Erchull (1977) in their study of source of the coal V enrichment. He argued that
metals (including V) in the subtropical Okefeno- this bituminous rock 'of comparable thickness is
kee (comprised of a wooded swamp environment) present throughout Illinois, but there is no
peat-forming system (Georgia, USA) pointed out comparable V enrichment of the underlying
that the peat-forming environment is of major coals'. Published analyses by Hower et al.
importance for the distribution of metals ulti- (1990b) show the V enrichment in the top
mately found in coal. It is well-established that the benches relative to lower benches at 42 of the
Okefenokee represents a suitable model system 44 sites of W. KY No. 9 coal where the bench
that approximates ancient peat-forming systems samples were collected. It is quite unlikely that a
that have ultimately given rise to coals. In fact, the source of V in the W. KY No. 9 coal was
tropical/subtropical low-land paralic swamps ordinary shallow (<100m) swamp waters (the
were at their maximum development in the from within theory). The levels of metals in
Pennsylvanian (Johnson 1980). the modern swamp (stagnant) waters are indeed
Under typical swamp/peat physicochemical very low (< 1 ppm) (Casagrande & Erchull 1976,
conditions, the most stable form of V in aqueous 1977). The principal arguments against the
solution is generally vanadate ions (HnVO~]-3) hydrothermal origin of V are: (a) hydrothermal
but the peat humic/fulvic components can reduce fluids contain a rather low concentrations of V
HnVO~]-3 to VO 2+ in an aqueous phase (Wilson similar to seawater (Wedepohl 1971; Jeandel
& Weber 1979). VO 2+ (and other V 4+) ions can et al. 1987); (b) numerous intensive hydrother-
then form stable complexes with many biogeo- mal sources are necessary to supply the metal for
chemical compounds (e.g. humic/fulvic acids, about 104 years (a time interval sufficient for the
lignins, porphyrins etc.) through chelation, metal deposition of the _<15cm of the coal for an
exchange reactions and redox reactions. The fact assumed coal deposition rate of 1-2cmky -1)
that >70% of VO 2+ ions are incorporated into over a large area (in the range of 5 • 10 4 -
the organic insoluble fraction of KY 9 infers two 105 km 2) which is quite unlikely; Fe oxides that
important points: (a) the swamp/peat milieu was precipitates from the hydrothermal fluids are an
highly reducing (see below) and with a high excellent sink for V (Dymond & Roth 1988;
reducing/complexing capacity through a media- Trefry & Metz 1989) and (c) it is difficult to
tion of its humic substances (i. e. highly enriched believe that a thin coal band, extending over ten
with humics); and, (b) VO 2+ ions must be bonded thousands square kilometres would be enriched
to geochemically stable oxygenated groups of the by (circulating) hydrothermal fluids while the
coal in order to survive both the coal-forming underlying (and much thicker) parts of the same
process (about 200 Ma) and prolonged weath- coal remain unaffected. Local hydrothermal/
ering (100Ma). The lack of change of All of surface-water activities, however, might have
voZ+(-non-P) upon prolonged (six months) caused some epigenetic enrichments. The coal-
heating at 100~ (and accompanied dehydrata- fields in Union and Webster counties are
tion) of KY 9, is evidence that VO 2+ is strongly adjacent to the W. KY Fluorspar District
bound to the coal insoluble organic structure. which is the known area of extensive hydro-
The fact that extensive laboratory leaching with thermal activities which occurred possibly as late
6M HC1 had no effect on the ESR signals as Upper Cretaceous (Brecke 1962).
attributed to voZ+-non-P incorporated into We must, therefore, postulate an (extra-
insoluble organic part of KY9 lends further ordinary) external supply of V of the past
support to this interpretation. swamp/peat water of the W. KY No. 9 coal.
We propose two views on the V source problem
which we term from below and from above.
Source o f V, volcanism and the origin According to the first concept, V was derived
of fusinites from either volcanic water or volcanic ash.
Extensive and intense volcanism is known to
Zubovi6 (1966) found that V was enriched in the have occurred in the Middle Carboniferous of
thin top block (generally _<15 cm) of six sites of North America. The other concept, perhaps
the Springfield (W. KY No. 9, Illinois No. 5) coal more actualistic, presumes that the surface
in a relatively large area (>50000km 2) of the (water) processes were adequate to extract,
southern Illinois Basin (KY counties: Union, concentrate and transfer V through weathering/
Webster, Hopkins, Davies, Henderson, McLean, leaching volcanoclastic materials from adjacent
Muhlenberg and Ohio; Illinois counties: Saline, land areas. This view was formulated by
Gallatin), (Fig. 2). Zubovi6 (1966) pointed out Premovi6 et al. (1986, 1993) to explain the
 ORIGIN OF VANADIUM IN COALS 281

abnormal V enrichment of some ancient sedi- location (Table 1). This erratic horizontal
mentary rocks of marine origin. The appeal to distribution of V in the top 15cm bench
volcanism as a source of V arises from the samples, which were accumulated in the same
presumed inadequacies of ordinary processes to freshwater basin though separated only by less
supply and transport V in sufficient quantities. than 10km (Hower et al. 1990b), suggests that
The evidence for a volcanic source is the perhaps the reducing/complexing capacity of
presumed close association in time and space humics in the particular locations of past
of the V enrichment in a particular sediment and swamp/peat forming basin may have played an
volcanism (Premovi6 et al. 1993). As far as we important role in concentrating V. This, on the
are aware, there is no direct mineralogical other hand, may reflect the local divergence of
(or other) evidence in favor of volcanism. vegetational cover within this area of ancient
However, the fact that this coalbed enriched forest swamp (Casagrande & Erchull 1977). In
with V cover an area of at least >50000km 2 addition, a sample of bituminous roof shale
(Fig. 2) may suggest a relatively intensive source. covering K Y 9 contains <100ppm of V, sup-
In this case, the main source of V would be the porting Zubovid's suggestion (Zubovid 1966)
ash containing the ejected materials which were that V in this and other V enriched coal(s) is not
carried downwind from the distant eruptive derived from this sedimentary cover.
centre. It is, then, the exception rather than the
rule to find these fine volcanic materials in
the conditions in which they were when freshly P r i m a r y and secondary V
deposited. Their porosity and the (physical/
chemical) instability of their constituents make As noted above, V occurs in high concentrations
them prone to alteration, especially in (chemi- at the top (<_150 mm) of the coalbed throughout
cally speaking) acidic environment such as the much of the western half of the coalfield.
swamp/peat-forming milieu (see below). A typical example is the V enrichment (1240 ppm)
Hower & Wild (1982) observed (macroscopi- in the 126 mm top bench at a site in the Hopkins
cally) the increase in fusinite in the top benches County, as opposed to the rest of six (lower)
relative to the middle/bottom benches. Many benches (total thickness c. 154 cm) in which the
authors consider that fusinites achieved their V content (Fig. 5) varies between 9 to 39 ppm
high carbon contents before deposition and (24 ppm used in discussion) (Hower et al. 1990b)
most probably by exposure to elevated tempera- and it is similar to the level of V (20ppm)
tures. A commonly held view of the origin of reported by Valkovi6 (1983) for the average US
some fusinites is that natural pyrolysis occurred coals. Thus, V (1240 ppm) in the top bench rises
as a result of forest fires, ignited by lightning or over the V level (24 ppm) in lower benches by a
meteorites. If this concept is adequate for the W. factor of >50. The most spectacular example of
KY No. 9 coal fusinites then it is difficult to the V enrichment (Zubovi6 1966) was in the top
escape the conclusion that forest fires swept 150mm section of the near-by Hopkins site,
through the ancient swamp of the W. KY Basin where it reached 2080ppm and dropped to
in the later stages (Des Moinesian) of the peat < 9 p p m below the top. Such enormous V
accumulation. It is clear, then, that these fires enrichments in the top portions of the W. KY
could be readily triggered by volcanic eruptive No. 9 coal could only be explained by an abrupt
materials. In addition, some of the erratic lateral and high influx of V into the W. KY Pennsyl-
trends observed for V (and Cr) distribution of vanian swamp/peat-forming system and its
the W. KY No. 9 coal could be due to the V subsequent localized chemical accumulation into
concentrating effects of the forest fires through the peat humics. This proposition, on the other
the formation of the charcoal/ash materials. hand, can only support the eruptive volcanism
The W. KY No. 9 coalbed at the Providence view. If this concept is correct then the volcanic
mine is about 210cm thick and has a marine event must have taken place during the Middle
black shale roof immediately on top of the coal Pennsylvanian (Des Moinesian) about 300Ma
(Maylotte, pers. comm.). According to this ago and therefore preceded the deposition of
author, only coal samples from the top 15 cm the uppermost portion of the W. KY No. 9 coal.
have high V content and even then not all The volcanic ejecta cannot, however, have
samples from that level showed it. For this stayed aloft for more than 6 months, and by
reason, we analyzed a coal sample of the top Stokes's Law should have settled through
10cm part from another (near-by) site. The <100m of the Pennsylvanian swamp water in
absolute value of the V (100 ppm) concentration less than one week. These time intervals are
(and, of course, VO 2+ content: < 10 ppm) in this much shorter than those assumed (c. 104 years)
sample is substantially less then at the first for the sedimentation of the top 150 mm section
282 P. I. PREMOVIC E T A L .

benches themselves: explosive volcanic activity

1400 I was at a minimum during most of the KY 9 time
and geochemical volcanic activity at a max-
1200 I imum. Had the activities been reversed the
uppermost portions of the W. KY No. 9 coal
1000 i would be associated with a relatively large mass
of volcanic ash. In brief, volcanic ash and V-rich
8O0
solution were the products of volcanic activity
during the KY 9 time; ash was product of brief
period (<1 year) of explosive activity; V-rich
solution was the product of long sustained
period (104-106 years) of geochemical activity.
12C
The ultimate cause of volcanic activity of a type
I resulting in large-scale discharge of ash rich in V
remains a volcanological problem.
The highest V contents (1000-2000ppm) in
the top benches of the W. KY No. 9 coal
c3 (Zubovi6 1966; Hower et al. 1990b; this work)
are much higher than those of average volcanic
40 ) ash-fall (200ppm, Leventhal et al. 1983). This
suggests that V in the Des Moinesian volcanic
ejecta was greater than normal and/or that the
humics of Pennsylvanian W. KY swamp/peat-
01 ~ . . . . . 5. . . . . . . . . . . forming basin had a great reducing/complexing
0 50 100 150
Thickness (crn) capacity for the corresponding V ions from the
swamp aqueous solution. Relative to ordinary
Fig. 5. The V/Cr distribution for benches at site 19, US coal (Valkovi6 1983), the top _<150mm
Hopkins County (Hower et al. 1990b): , V; portions of the W. KY No. 9 coal are enriched
..... , Cr by a factor >50 for V (Zubovic 1966; Hower
et al. 1990b; this work). If the 'normal' con-
centration of V in the Pennsylvanian swamp
of the W. KY No. 9 coal. When volcanic ash fell water was enhanced by a factor 100, most of the
weathering/leaching of the metal should have extraordinary V concentrations of these sections
occurred in 104-106 years (Zielinski 1979). That would be easily explained by involvement of
is, removal of V must have taken place during, three factors: (a) high V geochemical enrichment
geologically speaking, in a short time interval, factor (>50000: 1) of peat (Szalay & Szilagyi
relatively soon (104-106 years) after the Des 1967); (b) relatively low sedimentation rate;
Moinesian volcanism that produced the ash. (c) relatively high input of organic matter and V.
Consequently, the high V concentration in this Consequently, it is reasonable to assume that the
150ram top section apparently represents an V concentrations in this ancient swamp had not
admixture of primary V (derived directly from exceeded 0.2 ppm.
the primary ash fallout) and secondary V (which In general, volcanic ashes have a chemical
could be derived from other primary fallout composition similar to that of the igneous rocks
deposits and eroded from elevated land sites of the same family. Vanadium in these rocks is
near the W. KY Pennsylvanian forest swamp). present predominantly as V(III) which ionic
It seems reasonable to suppose: (a) both kinds of species are, however, relatively immobile. On the
V came from a single volcanic eruption and other hand, H,VO] -3 are readily soluble and
(b) the V contribution of the secondary ash can migrate far in the ash weathering/leaching
fallout to the total coal V is much larger than solution and over a wide range of pH. Thus
that of the primary material. we suggest that V reached reducing bottom
Thus, we suggest that the main mass of V in of ancient W. KY swamp/peat as HnVO] -3
the top benches of W. KY No. 9 coal appears to where it was reduced to VO 2+ by humic/
have been added to the Pennsylvanian swamp/ fulvic components of the peat (see above). The
peat basin as a product of volcanic activity fact that the HC1/HF soluble fraction of
mainly through geochemical alteration of volca- K Y 9 contains exceptionally high V content
nic ash. The absence of readily recognizable (1800ppm, Table 1) i.e. that 40% of total V
volcanic material (such as ash) explains, in a in the coal resides in this fraction (Table 1)
sense, the existence of these V-rich upper indicates that substantial amount of V(III)
 ORIGIN OF VANADIUM IN COALS 283

(initially located in ash-fall) was released and

altered into hydrated oxides and/or vanadates
which may be adsorbed on the clay particles or
precipitated in CaCO3 (Evans 1978). These
species are relatively labile and, as such, soluble
in cold HC1. The release and associated altera-
tion had to occur during the weathering/leach-
ing process of ash in the O2 saturated aqueous
solution. ~-O.
ul
O

Cr, V, Ni and basaltic volcanic ash

Apart from V, W KY No. 9 coal is also enriched I
I
in other metals, notably Cr. 60% of total Cr in
K Y 9 resides in the organic insoluble fraction 1,
(Table 1). Cr follows the V enrichment pattern in
"0'54 6 8
the top benches of the 42 sites of W. KY No. 9 pH
coalfield. For instance, there is a 15-fold increase Fig. 6. Eh-pH diagram for V O 2+ and its associated
of the Cr content in the top section (120 ppm) of humic/fulvic acid complexes in the presence of
the Hopkins site over the mean value (8 ppm) for molecular (FeS2) and ionic (CrOH 2+) species in the
six benches below (total thickness 154 cm, Fig. 5) Pennsylvanian W. KY swamp. Hatched area
(Hower et al. 1990b). In fact, V/Cr/Ni are expec- represents approximate stability field for interstitial
ted to be concentrated from basaltic volcanic water within the swamp/peat-forming system.
ashes (Wedepohl 1971). Thus, we tentatively
suggest that the V/Cr/Ni enrichment of the
HC1/HF soluble fraction of K Y 9 (Table 1) is
associated with basaltic volcanic activitity which
characterizes the Middle Carboniferous volcan- physicochemical conditions attributed to a peat-
ism of (Eastern) USA. forming system are close to natural conditions
i.e. those defined by Baas-Becking et al. (1960).
We may further restrict the Eh values by the
existence of FeS2 in natural marine (aqueous)
Physicochemical conditions of deposition of environments which should be in the region
Pennsylvanian W. K Y peat-forming system +0.1 V to -0.2 V for the pH range given above.
Thermodynamic data used for the FeS2 field are
Numerous Eh-pH diagrams for V are present in those reported by Wagman et al. (1982). The
the literature. A critical review of thermo- total dissolved element concentrations in the con-
dynamic data for aqueous V species has been struction of the FeS2 stability field are: 280 ppm
presented by Wanty & Goldhaber (1992). They of Fe (an arithmetic mean value for the swamp
focused their attention on the results of experi- waters of the Okefenokee system); and 90 ppm
mental studies of V chemistry, especially on of inorganic S (found in the average seawater)
those for which experimental physicochemical (Goldberg 1961). Although this diagram has
conditions are similar to naturally occurring been prepared for arbitrarily selected values for
conditions. According to Baas-Becking et al. V, Fe and S, the critical boundary between the
(1960), who made a thorough study of Eh and VO 2+ and FeS2 fields is not significantly affected
pH in many natural aqueous environments, the by modifying these values ten-fold in either
acidity of the swamp/peat waters and the inter- direction. Thus this diagram may be used to
stitial waters in the peat is unlikely to vary estimate possible physicochemical conditions of
outside the range pH 4-8. Moreover, they found the swamp/peat-forming system at the time
that the Eh values of most peat-forming systems when the Pennsylvanian W. KY peat is formed.
do not exceed +0.6V. We have constructed the It is apparent from Fig. 6 that VO 2+ species
Eh-pH diagram for total V concentrations of are stable thermodynamically only at high Eh
0.2 ppm (as previously discussed) in an aqueous conditions (>0V). Therefore, natural solutions
solution (Nikoli6 1993). This diagram is essen- with Eh lower than 0 V would not be expected to
tially identical to that of Wanty & Goldhaber contain VO 2+ or its complexes thereof. Never-
(1992) but, for the sake of simplicity, we present theless, such solutions may contain VO 2+ (down
only a part of the diagram (Fig. 6) for which to - 0 . 2 V ) because of the formation of stable
284 P. I. PREMOVIC E T AL.

complexes between VO 2+ and organic acid therefore difficult to reconstruct the physico-
ligands (such as salycylate) (Breit & Wanty chemical conditions of sedimentation in the
1991). It is quite certain that we may expect Pennsylvanian swamp of the W. KY Basin
similar enlargment of the VO 2+ stability field for when the geomorphology and climate were
voZ+-humic/fulvic acid complexes in the W. KY quite different.
Pennsylvanian swamp/peat water (Fig. 6).
Wilson & Weber (1979) observed that the
VO 2+ concentration in the reaction solution
containing a ten-fold molar excess of (soil) Conclusions
fulvic acid (under strictly anaerobic condi-
tions) is rather low due to the formation of 1. VO 2+-non-P in a thin coal band (rich in V)
minor (diamagnetic) (VOOH) and major solid of the Western KY No. 9 bed are detected
VO(OH)2 above c. pH4.5. In fact, their data by ESR.
fitted exactly the Francavilla & Chasteen (1975) 2. The ESR spectral parameters of VO 2+-
experimental curve obtained for VO 2+ in aqu- non-P indicate that this ion is bound to oxygen
eous solution in the absence of air O2. Although ligand donor atoms, possibly carboxylate/
there are some differences in the chemical phenolate groups.
behaviour/structure between soil fulvic acid 3. The vanadylation occurred during the
and the corresponding peat component, these peat-forming stage of coal formation in the
results clearly indicate that the peat is probably Middle Pennsylvanian swamp of W. KY.
the most effective for the VO 2+ complexation 4. The V enrichment in the top benches
at pHs < 6. relative to lower benches of the W. KY No. 9
Bacterial HzS production is pH dependent and coalbed is caused by abrupt and high influx of V
one of the main sulphate reducing bacteria is into the Pennsylvanian swamp of W. KY. It is
Desulfovibrio desulfuricans. These organisms are suggested that the main source of the metal was
predominantly active at pH 6.5-8.0 (Alexander from volcanic ash on the land by weathering/
1967), though there are a few cases where they leaching which remove V from the ash to the
grow at pH 5.5. The marine peat-forming milieu ancient swamp.
has a pH near neutrality (7), while the freshwater 5. From the chemistry of VO 2+, FeS2 and
swamp/peat is at pH4. Thus higher pH(5-6) CrOH 2+, it is deduced that the oxidation
may be the cause of high H2S production in potential Eh and pH of the ancient peat inter-
the ancient W. KY swamp/peat basin and of the stitial water was approximately -0.2 to -0.3 V
consequent higher FeS2 production. and 5 to 6, respectively during the W. KY No. 9
Under the deduced physicochemical condi- coal formation.
tions of deposition of W. KY No. 9 coal (Fig. 6)
the bulk of Cr present in the Pennsylvanian This research was supported by grant number 0206
swamp water should be present as CrOH 2+ ions. from the Ministry of Science (Serbia). We thank D. H.
The Okefenokee swamp waters contain <60 ppb Maylotte (KY) for supplying geological samples. We
Cr (Casagrande & Erchull 1977). If the Pennsyl- are grateful to G. F. Huffman and F. E. Huggins for
vanian swamp water of W. KY was enriched the XAFS and M6ssbauer analyses. We also thank M.
Miljkovid for SEM and EDX examinations, J. C.
with Cr by a mediation of the Des Moinesian Hower for providing us with reprints/copies of his
volcanic ash (likewise V) than it is quite reason- publications and Ana de Pablo for reviewing the
able to assume that Cr of this water exceeded manuscript with skill and patience.
>60ppb. On the other hand, much of the
stability field of Cr is occupied by insoluble
Cr203. This species dissolves to form CrOH 2+
below pH 5 for the Cr concentrations >1 ppb References
(Brookins 1988). Hence, physicochemical condi-
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Acta, 45, 481-487.
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 Environmental impact of minerals in UK coals
D. A. S P E A R S

Department of Earth Sciences, University of Sheffield, Brookhill, Sheffield $3 7HF, UK

Abstract: Both detrital and diagenetic minerals are quantitatively important in UK coals. The
detrital minerals include quartz, and the clay minerals illite, mixed-layer illite-smectite,
kaolinite and chlorite. The diagenetic minerals are dominated by pyrite/marcasite,
carbonates, mainly ankerite and calcite, and kaolinite. Pyrite makes an important
contribution to the S contents of the coals and is largely responsible for the variation in
total S. The S content of coals delivered to power stations could be reduced by selective
extraction during mining and improved physical coal-cleaning. Pyrite is a major location for
trace elements of environmental concern and the elimination of pyrite would reduce both SO2
and trace element emissions. Pyrite is also important in the weathering environment due to its
instability. Its breakdown in coal stocks and colliery discard heaps may lead to spontaneous
combustion. In discard heaps, pyrite breakdown is also responsible for acid porewaters and
toxic elements in solution which inhibit colonization by vegetation and thus hinder
reclamation of derelict land. If carbonates are sufficiently abundant, acid conditions may be
eliminated. Acid porewaters are one facet of the general problem of acid mine drainage, which
has a major impact on water quality, particularly in streams and rivers. In the UK acid mine
drainage is a problem of growing concern due to reduction of deep-mine pumping following
closure of collieries. Although pyrite breakdown in colliery spoil has an important influence
on porewater compositions, it does not greatly influence the engineering stability because the
major component, the mudrocks, contain very little pyrite. Upon exposure, the mudrocks
break down relatively rapidly due to sedimentary structures to form an aggregate. Loss of
interparticle bonding is a much slower process but there are a few mudrocks associated with
low rank bituminous coals with both a high mixed-layer clay content and porosity which
disintegrate rapidly during cycles of wetting and drying. There are also regional variations in
the relative proportions of the clay minerals which influence the engineering properties.
Kaolinite is dominant in the northern coalfields. This is also detected in the composition of fly
ash produced by coal-fired power stations. Fly ash is enriched in those trace elements which
have an environmentalimpact. The volatile elements, many of which were sulphide-associated
in the coal, are enriched on the surface of the ash particles where they are accessible to leaching
in the weathering environment, resulting in the contamination of natural waters.

In the British Coal Measures the bituminous impact and, as composition is closely related to
coals vary widely in ash content through the the origin and mode of occurrence, these aspects
seam. Minimum ash contents, measured at 850~ are summarized in this paper. Not considered
(HTA), are usually around 2%. However, major here are the impacts that minerals have
seams are usually complex, containing grada- on utilization processes such as their influence
tional carbargillites and inter-seam mud- on combustion properties.
rocks with high ash contents. Hence the coal
delivered to U K power generators averages
approximately 16% ash. Based on the chemistry Minerals in UK coals
of the ash and quantitative mineralogy of low-
Sulphides, carbonates and silicates are the
temperature plasma ashes (LTA) it is possible to
common minerals in the East Pennine Coalfields
demonstrate that the coal ash is essentially
but oxides and phosphates also occur (Spears
derived from the minerals in the coal (Pike
1987). Minerals may be dispersed or concen-
et al. 1989; Ward 1989). The connate fluids make
trated and the grain size ranges from clay to
a minor, but nonetheless significant, contribu-
sand-sized, but with some minerals aggregating
tion towards Na and C1, although it should be
to form megascopic concretions. The composi-
noted that C1 is volatilized in the ashing pro-
tion and mode of occurrence of the minerals are
cedure. The ash content of these coals is there-
a function of the origin.
fore a direct reflection of the mineral content.
This paper will briefly describe the main
minerals present in U K coals and their origins Detrital minerals
before dealing in greater detail with their envir-
onmental impact. The composition of minerals The composition of the detrital sediment incor-
is an important factor on the environmental porated into the peat in the swamp environment

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 287-295.
288 D. A. SPEARS

is comparable to that found in the mudrocks, were not of major importance. Regional differ-
siltstones and sandstones in the sequence as a ences in the clay mineralogy have been described,
whole. However, the coal precursor swamp was as, for example, in the work of Taylor & Spears
generally a low-energy depositional environment (1970), which showed kaolinite was dominant in
and consequently the detrital sediment was fine- the coalfields of Scotland and northern England.
grained consisting essentially of clay minerals Figure 1 is based on that X-ray diffraction study
with minor quartz present as silt-sized grains. of tailings samples from coal preparation plants
The composition of the clay fraction is a in all areas of the coalfields. These preparation
function of the climate and the bedrock compo- plants usually dealt with several coal seams from
sition in the source area from which the more than one colliery, and the tailings samples
sediment was derived. In the East Pennine are therefore representative and thus ideal for a
Coalfields, illite and kaolinite are the major study of regional variations.
detrital clay minerals with minor amounts of a
chlorite mineral. The illite is associated with Precipitate (diagenetic) minerals
mixed-layer illite-smectite. Discrete smectite has
not been identified. Rootlets in seatearths In low ash coal samples (<5% ash) kaolinite is
demonstrate that soil-forming conditions also usually the only clay mineral detected. Based on
existed in the basin of deposition and in a few textural evidence seen under the microscope this
cases extreme alteration has produced a kaoli- is thought to be diagenetic. The X-ray diffrac-
nite rich (fireclay) bed. tion traces show the structure is well ordered,
On the other hand, chlorite, which is suscep- unlike the fine-grained detrital kaolinite. In
tible to weathering, occurs in many seatearths high-ash samples the diagenetic kaolinite may
(Rippon and Spears 1989) and also in coals, thus be obscured by the detrital kaolinite.
demonstrating that clay transformations at the Pyrite and its dimorph marcasite are the most
time of deposition and during early diagenesis common sulphide minerals. Pyrite is present as a

7A Kaolinite
k 9 Scotland, Northumberland & Durham
l e Yorkshire & Lancashire
v East & West Midlands
i

10,/k Mica ML Illite-Smectite

Fig. 1. To show the clay mineral proportions in representative clay samples (tailings samples) from all coalfields
in the UK. Also shown are three mudrocks known to have engineering instability. Chlorite is a minor component
and is not illustrated, but its abundance is proportional to that of illite.
 ENVIRONMENTAL IMPACT OF MINERALS IN COALS 289

number of textural types which formed over a are capable of shattering the mudrock. Slaking
long period of geological time (Love et al. 1983; tests conducted in vacuo restricted, but did not
Kneller & Maxwell 1985; Frankie & Hower eliminate the breakdown indicating the presence
1987). The formation of FeS2 is controlled by of another controlling factor. This was identi-
the availability of iron and reduced sulphur fied as the intraparticle expansion of smectite.
species. The latter is linked to the concentration Although discrete smectite does not occur,
of sulphate in the water in the depositional smectite is present in mixed-layer clay minerals.
basin, not only for the early diagenetic pyrite but The presence of an effective porosity and a
also for the late diagenetic pyrite although the significant smectite component within the
links are less clear. mixed-layer clay mineral are both favoured by
A number of elements occur in the pyrite in a high clay content. During deep-burial dia-
both solid solutions and as discrete sulphide genesis porosity is reduced and mixed-layer
phases. A simple relationship of composition illite-smectites are progressively illitized, there-
with time of formation was not observed in the fore the stability of mudrocks is increased. It is
work of White et al. (1989). Sulphides other than for this reason that in the UK the unstable
iron do occur, and may even be recognized in mudrocks which created problems, particularly
hand specimens, as well as under the micro- in the coal preparation plans, are associated
scope. However their volumes are small com- with the lower rank bituminous coals. Three
pared with the iron sulphides. unstable mudrocks are shown plotted on Fig. 1.
The cleat carbonate consists of ankerite and For all three mudrocks not only is the relative
calcite. Textural relationships in thin section proportion of mixed-layer clay high, but as these
demonstrate a later stage of formation for the are clay-rich mudrocks the total clay content is
calcite compared with the ankerite (Spears & also high.
Caswell 1986). Based on the work of Fellows The shear strength of mudrocks is also a
(1979) and Caswell (1983) most of the carbonate function of rank. Taylor (1988, table 5) demon-
would appear to be in the cleat. Siderite occurs strated that the shear strength of British colliery
spasmodically in minor amounts in the coal but discards fell into three groups, which were also
not in the cleat. rank groupings. Exceptions to this grouping, as
for example with the Scottish samples (Fig. 1), are
thought to be related to the much higher kaolinite
Weathering of minerals associated with coals content in the more northern coalfields and the
more 'geotechnically' inert nature of kaolinite.
Physical weathering: influence on The relative clay mineral proportions influence
engineering stability the strength parameters, but an even more impor-
tant variable is the total clay content, particularly
Mudrocks are intimately associated with coal as an increase in the clay content means there is a
seams. The mudrocks extracted with the coal decrease in the quartz content.
are disposed of underground and on the surface
in discard heaps. The engineering stability of
the discard heaps is very much dependent on the
behaviour of mudrocks during weathering. The Chemical weathering. influence on
composition, classification and weathering beha- engineering stability
viour of Coal Measures mudrocks was compre-
hensively reviewed by Taylor (1988). Physical The detrital minerals were subjected to one or
breakdown of many mudrocks takes place more weathering regimes before they were depos-
rapidly and is largely controlled by sedimentary ited and have therefore achieved some measure of
structures. Mudrocks were observed to break chemical stability in the weathering environment.
down rapidly to conglomerate and sand-sized The minor diagenetic changes undergone by the
aggregates during emplacement on the discard detrital minerals do not fundamentally change
heap. Once the material was buried, further the stability. The detrital minerals will therefore
physical breakdown appeared minor. Sedimen- react slowly, if at all, during exposure in discard
tary textures are also important for some heaps. This does not, however, apply to the
mudrocks, particularly with respect to air-break- diagenetic minerals that formed in restricted
age and slaking. If fragments of mudrocks are chemical environments. Sulphides and carbo-
allowed to desiccate, air is drawn into voids in nates are all potentially reactive when exposed
response to negative suction pressures. On sub- to surface waters.
sequent saturation, the water drawn into the Pyrite oxidation takes place rapidly when
mudrock by capillarity creates pressures which exposed to weathering at the surface. There are
290 D. A. SPEARS

a number of steps in the oxidation of pyrite, some problem in the older parts of the coalfields. In
of which are catalysed by the Thiobacillus the UK there is considerable concern that the
bacteria. The reactions and their influence of widespread programme of colliery closures and
the engineering stability of mudrocks, including the associated cessation of pumping could widen
the effect of the acidity generated on carbonates the impact of acid mine drainage. The problem
and clay minerals, are reviewed by Taylor (1988) arises from the underground oxidation of pyrite
and Pye & Miller (1990). The latter authors noted by oxygenated waters originating from the
that chemical alteration of a Carboniferous surface. The pyrite reactions are the same as
mudrock was a rapid process and that significant those occurring in colliery discard and described
post-emplacement alteration had taken place in by Taylor (1988) and Pye & Miller (1990).
an embankment. This was mainly attributable to Furthermore, the associated reactions involving
the oxidation of pyrite and the knock-on reac- carbonates and clay minerals are also important
tions involving carbonates and clay minerals. The as they influence the pH and the composition of
sulphuric acid produced in the breakdown of the ochre precipitate.
pyrite is consumed principally by the dissolution The pyrite is present in the roof and floor
of carbonates and to a lesser extent by the clay measures and also in the residual coal left as roof
minerals. There is loss of interlayer K and supports. It has been noted (Morrison et al. 1990;
octahedral Mg, Fe and A1 from the illite, leading Younger 1994) that problems of acid mine
towards the formation of kaolinite. Gypsum drainage are mainly associated with coals depos-
and more complex sulphates such as jarosite ited in marine or brackish-water strata rather
are precipitated. The engineering properties are than with coals deposited in terrestrial fluvial
changed in the mineral transformations and environments. The association of pyrite with
textural changes. The pyritic Carboniferous marine conditions, and particularly the control
mudrocks considered by Pye & Miller (1990) of SO4 availability has been noted earlier in this
are marine whereas the Carboniferous mudrocks paper. Another aspect of the pyrite weathering
dealt with by Taylor (1988) are non-marine and the resultant acid mine drainage is the
and thus essentially non-pyritic. The latter are concentration of ions in solution. These may
from the Westphalian Coal Measures whereas indicate the involvement of other minerals in the
the pyritic mudrocks are of Namurian age. reactions, for example Ca and Mg from carbo-
This explains why in UK colliery discard nates and A1 from clay minerals, but on the other
heaps chemical weathering has been found hand pyrite is an important host for a number of
to be relatively minor and not therefore a trace elements, which will also be released into
major factor in the long-term stability of the solution under acid conditions. Coprecipitation
colliery spoil. of toxic metals with iron oxyhydroxides could
Pyrite is not restricted to marine shales and the create problems, for example in the functioning
colliery discard will often include nodular and of treatment facilities (Murdock et al. 1994).
other concentrated forms of pyrite such as
pyritized coal. If this material is isolated by inert
mudrocks, and particularly if movement of oxy-
genated surface-derived porewaters is restricted Restoration of derelict land
by compaction at the time of emplacement, there
should be minimum impact on the long-term Deep mining in the UK has created derelict land.
stability of the engineering structure. Pyrite Although such activity accounts for less than
weathering at Yorkshire Main discard heap, 20% of the total area of derelict land in the UK,
cited by Taylor (1988), was found to be restricted it is associated with regions of high population
even though tipping from an aerial ropeway density and therefore there is an awareness of the
meant that the optimum compaction had not environmental impact. Opencast mining in the
been achieved. With a more open structure there UK has not led to the same problems because it
is a risk of spontaneous combustion triggered by is a more recent development with, therefore,
the reactive and exothermic pyrite oxidation. greater concern for the environment. Colliery
Although burnt shales is more stable, combustion discard heaps are a major contributor to derelict
of discard heaps is highly undesirable. land, a significant fraction of which have been
reclaimed by colonization with vegetation, often
after regrading. Most of the problems associated
Chemical weathering: acid mine drainage with establishing a flourishing vegetation relate
directly to the nature of the colliery spoil and the
Acid mine drainage, that is pollution by acidic constituent minerals. The engineering behaviour
and/or ferruginous waters, is a long-standing of the material is clearly important for slope
 ENVIRONMENTAL IMPACT OF MINERALS IN COALS 291

stability. However the relative chemical stability S02 emissions and the role of pyrite
of the clay minerals, a factor noted in the
previous section, together with the inertness of In 1988 agreement was reached in Europe on the
the more carbonaceous material produces very Large Combustion Plant Directive (8/609/EEC)
little in the way of nutrients for plant growth which required a 60% reduction in SO2 emis-
(Bradshaw & Chadwick 1980). According to sions from existing plant in the U K by 2003. The
these authors, colliery spoil may become colo- planned flue gas desulphurization (FGD) capa-
nized with vegetation naturally, but there is not a city in the UK has been reduced to 6000 MW
classical ecological succession with more species (Cooper & Kyle 1995) in response to changes in
appearing as a function of age. The number the balance of fuels used, notably a decrease
of species present would appear to be more a in coal and increase in gas. In the European
function of pH, irrespective of age. As in acid Union as a whole, the 40% reduction in SO2
mine drainage, the pH of the porewaters is emissions achieved in 1990 compared with the
related to the breakdown of pyrite. level in 1980 is seen as a direct consequence of
Bradshaw & Chadwick (1980) note that not the sharp increase in F G D capacity (Bolt 1995).
only is it the amount of pyrite which is important According to Harrison (1995) F G D is cur-
but also the proportion of the more rapidly rently the only practicable solution for existing
reacting fine-grained pyrite. Ambient tempera- coal-fired power stations with respect to SO2
tures are also important as would be predicted emissions. This author also notes that, in the
and observed oxidation rates in summer months UK, although conventional coal-cleaning does
are 5-10 times higher than those recorded during significantly reduce the total sulphur content of
the winter months (Backes et al. 1993). The the coal, in principle only half of the sulphur is
discard is dark coloured, and therefore surface amenable to such treatment, as the other half
temperatures in direct sunlight will be higher, occurs as organic sulphur which can only be
creating a more inhospitable environment for the removed by more expensive chemical means.
establishment of the vegetation. The pH of the These organic S-pyritic S proportions are in
porewaters also depends on whether or not agreement with analyses obtained for the
carbonate is available to neutralize the acid Parkgate Coal in the East Pennine Coalfield
solution from the pyrite breakdown. If there is (Cavender & Spears 1995), where the average
an excess of reactive pyrite, porewaters within the organic S was 1.09+0.36% and the pyritic S
colliery discard will remain acid, releasing A1 into was 1.17 • 1.79 (n = 75). Sulphate S is a minor
solution from the alteration of the clay minerals. component, 0.08 +0.11% and the total S was
Even at very low concentrations A1 in solution is determined as 2.344-1.83%. Although the
extremely toxic to plant growth. The Mn released average organic S and pyritic S values are
from the carbonates is also toxic in low concen- comparable, the standard deviations are signifi-
trations. Bradshaw & Chadwick (1980) also note cantly different. The organic S varies over a
that some freshly deposited colliery discard relatively small range compared with the pyritic
shows salinity problems due to water soluble S and the latter is responsible for most of the
salts originating from groundwater. The resul- variation in the total S content. The samples
tant problems for plant growth are relatively analysed had a minimum total S value of 0.89%
short lived in a humid climate as the salts are and a maximum value of 11.05%, which cor-
rapidly leached. This problem is probably responds to the minimum and maximum pyrite
associated with the connate water and restricted S values. It therefore follows that improved
to deep mine, high C1 coals. physical coal-cleaning would reduce the S
There is a contrast: chemical weathering is content of many of the coal samples by rather
important in creating acid conditions within more than 50% suggested by Harrison (1995).
porewaters which adversely effect the vegetation However, to separate all the pyrite would
whereas chemical weathering apparently has require fine-grinding, as much of the pyrite is
little influence on the stability of the discard micron-sized and intimately associated with coal
heaps. However, the former is restricted to the macerals (Kneller & Maxwell 1985).
zone of root activity, essentially the surface of A representative collection of 22 U K coals
the discard heap, whereas the stability relates to (Burchill & Way 1993) has an average organic S
the behaviour of the whole. Also, chemical content of 0.82 4- 0.23% (broadly comparable
weathering of a minor component, and pyrite with the Parkgate Coal) and an average pyritic S
breakdown in particular, can dominate the content of 0.35 4- 0.31% - significantly lower
chemistry of the porewaters and have a major than for the Parkgate Coal. However, the coal
impact on the vegetation, whereas the bulk samples are not entirely representative because
engineering properties are little changed. mineral contents are untypically low. This is
292 D. A. SPEARS

demonstrated by the low ash contents which orders of magnitude better than can be obtained
average 5 . 3 6 i 4 . 1 0 % and 4.65+2.4% if one with an electron microprobe, the rela-
sample with a 20.4% ash content is excluded. The tively large beam diameter utilized in the SXRF
latter is a commercial coal grade more typical of at that time (~ 20 #m) meant that not all textural
that delivered to the power generators. Never- types of pyrite could be analysed. In particular it
theless the selected seam samples do demonstrate was not possible to analyse the micron sized
that the distribution of mineral matter through framboidal pyrite which is a major textural type.
seam profiles is less uniform than organic S, and Nevertheless the SXRF analyses of the sulphides
low pyrite S coals are present in most seams. demonstrated significant concentrations of
In some of the coals analysed the organic S is many of the elements listed by Finkelman
also low, which is a feature of specific coalfields. (1982). No systematic differences were noted in
In the work on the Parkgate Coal (Cavender & trace element concentrations between early and
Spears 1995), the S distribution has been mapped late diagenetic sulphides. This also suggests that
on a plie by plie basis through the seam and over the composition of the small framboids is
a wide geographical area. This has been done, comparable with other textural types. Arsenic,
not only to establish the geological controls on Se, Pb, Cu and Ni were detected in most sample,
the S distribution and thus improve prediction by T1 in about half and Zn and Mo in about a
an improved understanding of processes, but quarter. The analyses show log-normal distribu-
also to identify areas of high S coal which might tions with mean values influenced by extreme
be rejected in a mining strategy designed to values, probably due to sub-micron sized inclu-
reduce the average S content of the mined coals. sions of other sulphides such as galena, chalco-
The importance of pyrite to the total S variation pyrite and blende. White et al. (1989) noted a
also highlights the importance of improved highly significant correlation between As and Se,
physical coal-cleaning to separate pyrite and but not between other elements. This lack of
reduce the S content of the coal and consequent correlation can be attributed to the inclusion of
SO2 emissions. subsurface inclusions of other sulphides in the
analyses and also the inferred variability of the
solutions and the precipitation processes. In
The role of minerals on element emissions follow-up work by Spears & Martinez-Tarazona
from coal-fired power stations (1993) pyrite was concentrated using density
fractions and analyses comparable to those of
Finkelman (1982) listed the following elements White et al. (1989) were obtained. The analyses
with a potential sulphide association: Sb, As, Bi, also demonstrated that not only does pyrite
Cd, Co, Cu, Ga, Ge, In, Pb, Hg, Mo, Re, Se, Te, contain elements recognized as of environmental
Sn and Zn. A number of these elements are of concern, but that it is the main location for these
environmental concern, particularly linked to elements in the coal.
atmospheric emissions. It has been estimated on The importance of pyrite as a major host for
a global scale that the power producers are the trace elements of concern in the environment
largest source of Hg (38%), Ni (52%) and V is an additional factor which needs to be taken
(74%) and an important source of Sb (21%), Cd into account in a cost/benefit analysis for the
(9%) and Se (23%) (Clarke & Sloss 1992). Coal reduction of SO2 emissions. Although improved
is a major source of As, Cd, Hg, Sb and Se with physical coal-cleaning will in theory eliminate the
Ni, Sn and V mainly derived from oil combus- pyritic S, there remains the organic S and hence
tion. Elements of greatest environmental con- the requirement for FGD. While there could be
cern linked to coal utilization are As, B, Cd, Hg, less emphasis on increasing the efficiency of
Mo, Pb and Se, and of moderate concern Cr, pyrite removal prior to combustion if FGD is to
Co, Ni, V and Zn. It should be noted that a be fitted, the benefit is not only of additional S
significant number of these elements of concern removal prior to combustion but also in the
are thought to have a sulphide association and reduction of trace element concentrations in
therefore if globally the coal-derived input into combustion products and emissions.
the atmosphere is significant, then pyrite is an
important contributor.
In the work of White et al. (1989), synchrotron The influence of coal minerals on
radiation X-ray fluorescence (SXRF) was used combustion residues
for the direct determination of trace elements in
pyrite (n = 206) and marcasite (n = 25). The pre- The ash produced during combustion is essen-
dominance of pyrite analyses reflects its greater tially derived from the minerals present in the
abundance. Although detection limits are several original coal. It therefore follows that the ash
 ENVIRONMENTAL IMPACT OF MINERALS IN COALS 293

composition reflects the relative proportions and the gaseous emissions is a function of volatility,
compositions of the minerals. In a conventional thus the sulphide associated elements figure
coal-fired power station two forms of ash are prominently.
obtained, the furnace bottom ash (~20%) is a The on-land disposal of fly ash has environ-
high density aggregate whereas the fly ash mental impacts (reviewed by Carlson & Adriano
(~80%) mainly consists of fine-grained, sphe- 1993). Elements associated with the surfaces of
rical particles. Both forms of ash are in demand fly ash particles are liable to be leached in the
in the construction industry but there is an weathering environment and released into solu-
excess production of fly ash, which is disposed of tion in concentrations which are a function of the
in lagoons, landfill sites and mounds. In the UK availability and aqueous chemistry. Most studies
the excess, non-marketed, fly ash production have been conducted on fly ash lagoons because
was approximately 6.5 • 106 tonnes in 1990. of the immediate impact on the environment.
The composition of fly ash is a function of Those elements incorporated into the glass phase
furnace efficiency and the ash composition of the may also be leached but at much slow rates than
coal, which is directly controlled by the miner- the sublimates. Nevertheless, significant amounts
alogy. The level of unburnt carbon should be could enter porewaters over a period of time
very low, ideally zero, otherwise the fuel loss is and these too could contribute an anthropogenic
economically important. In the work of Hub- input into surface waters and groundwaters. The
bard et al. (1985) sampling of fly ash at 26 UK contamination of surface waters may be less
stations showed that while the ash composition critical because of dilution and dispersion.
was relatively constant at one location over a However, porewaters originating from fly ash
period of days, there were important regional disposal sites could have a significant impact on
differences. As noted earlier kaolinite is more groundwater quality. In the case of such point-
important in northern coalfields in the UK source contamination there is less opportunity
(Fig. 1). This means that in terms of chemical for dilution and groundwater remediation
composition A1203 is more important and K20 schemes are expensive. A study of a long-
less so. These chemical differences are inherited established ash mound (Lee & Spears 1995)
by the fly ash and thus the composition of the provided information on the longer-term weath-
new minerals and the glass is influenced. A high ering of PFA and potential input into aquifers
kaolinite percentage in the original coal is over a period of 17 years. Equilibrium with
equated with a higher mullite content in the respect to gypsum was noted in the deepest
ash, and the generation of cenospheres (most of and oldest porewaters, but the concentration of
the amorphous silicates) is largely the result of other elements in the porewaters increased with
partial fusion of illite (Hubbard et al. 1985). depth indicating continued reaction of the
According to these authors it is the amorphous fly ash and the non-attainment of equilibrium.
silicate component which constitutes a potential Trace elements which were found to increase
pozzolana (i.e. not having direct cementitious with depth were, with maximum concentrations,
properties but which will nevertheless react with As (--~50#g/1), Se (~40#g/l), Pb (0.6mg/1), Mo
Ca 2+ released during cement hydration to form (3mg/1), Ni (0.15mg/1), Li (Zing/l), B (20mg/1)
low solubility compounds of cementitious char- and Cr (0.2 rag/l). These elements are all thought
acter). The coal mineralogy therefore has a to be pyrite-associated in the coal with the
major influence on the use of fly ash in cement exception of Li, B and Cr.
and the elimination of a potentially waste by- The porewater in contact with the fly ash in
product. the cited study was slightly alkaline with a pH of
There is an important element fractionation 7.96+0.38 (Lee & Spears 1995). This alkaline
between furnace bottom ash and fly ash (Clarke pH is attributable to hydrolysis of the surface
& Sloss 1992). The latter is in contact with the Ca, Mg, Na and K (Talbot et al. 1978). Pre-
gas stream as temperatures fall. The volatile diction of the leachate pH has been based
elements depleted in the furnace bottom ash are on the (CaO + MgO) to (SO3 + 0.04 A1203) ratio
incorporated into the glass phase and precipi- in the bulk ash (Van der Sloot et al. 1985). With
tated on the surface of fly ash particles. Because the exception of Na derived from connate fluids
of the surface association element concentra- in the coal and part of the S originating from
tions are highest for the smallest fly ash organic S, all the other elements are primarily
particles, which are also the most difficult associated with the coal minerals; Ca and
particulate emissions to eliminate. Volatile ele- Mg originate from carbonates, K, A1 and some
ments, which are only partially retained by the of the Na comes from the clay minerals and
particulates, also contribute to atmospheric the non-organic S from pyrite. The pH is
emissions. The proportion of these present in very important in controlling the solubility of
294 D. A. SPEARS

many of the trace elements in leachates derived into porewaters over a longer time period. Fly ash
from fly ashes. Under alkaline conditions a is therefore a potential contaminant of surface
number of elements occur as soluble anionic and groundwaters.
forms including arsenate, selenate, molybate, 9. Pyrite is unstable in the weathering envir-
borate, chromate and vanadate whereas the onment. The rapid reaction may trigger sponta-
more metallic cations tend to precipitate as pH neous combustion in coal stocks and discard
increases (Hjelmar 1990). The porewater con- heaps. In general, the oxidation of pyrite in UK
centrations observed by Lee & Spears (1995) colliery discard does not create problems of
conform with predicted solubilities. engineering instability, mainly because pyritic
mudrocks are uncommon in the Coal Measures.
10. The near-surface breakdown of pyrite in
Conclusions discard heaps creates acid conditions in pore-
waters. Carbonates and to a lesser extent clay
1. Minerals are quantitatively important in minerals will react and toxic elements may be
UK coals and are responsible for the ash, which released into solution in addition to those
for power station coals averages approximately originating from the pyrite.
16%. 11. If the acid porewaters escape from the
2. Detrital minerals present include quartz, discard heaps, contamination of surface waters
illite, mixed-layer illite-smectite, kaolinite and results. This is one manifestation of the problem
chlorite and the non-detrital, diagenetic minerals of acid mine drainage. More important are the
include pyrite, kaolinite, and the carbonates acid discharges from abandoned underground
ankerite and calcite. workings, particularly in coalfields where pump-
3. The detrital minerals are relatively stable ing has ceased.
during chemical weathering with chlorite the least
stable, but the smectite component in the mixed-
layer clay is capable of expansion. This effect is
potentially greatest in clay-rich mudrocks asso- References
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porosities and greater propensity for air-break- Seasonal variation of pyrite oxidation rates in
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4. There are regional variations in the compo- BOLT, N. 1995. The overseas perspective on desulphur-
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UK coals. This is detected in the geotechnical ICHEME Symposium Series No. 138, 15-20.
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tion of Land. University of California Press,
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A well logging method for the determination of the sulphur content of
coal seams by means of deep gammaspectrometry

ViT GREGOR ~ & ANTONiN TI~2KY 2

1Podpgrova 5, Brno-Medl6nky, 62100, Czech Republic

2 Lacinova 2, Brno-l~edkovice, 62100, Czech Republic

Abstract: This contribution describes new spectral logging equipment developed at

Geofyzika Brno which is designed to remotely determine the sulphur content in brown
coal. The method is based on analyses of the prompt gamma ray spectrum induced in coal
seams by a neutron source. Theoretical studies have demonstrated the possibility of using
the 5.42MeV peak of gamma radiation from sulphur. The measured spectrum is analysed in
three independent parallel ways. The analyser is calibrated in the range from 0.6% to 10%
of sulphur by weight. The lower detection limit is believed to be 0.3-0.5%, and the
measurement sensitivity 0.1%.
The undesirable consequences of the presence of development of new mathematical methods of
sulphur in the raw materials of energy produc- interpretation of the spectra, with the purpose
tion are well known and therefore it is not of improving considerably the selectivity and the
necessary to explain the significance of such a accuracy of the measurements. In view of the
problem at a time when the ecological aspects of limited extent of this paper we do not publish all
the industry are being monitored very closely. At the data that form the basis of our conclusions.
the beginning of the chain of energy production This was done in the final publication of
from brown coal there is the emission of sulphur the project.
dioxide. Therefore the task arose how to
determine the amount of sulphur in specific
parts of brown coal beds. Only on the basis of Detection of sulphur concentration in coal
such information is it possible to decide whether seams: accuracy and representation
particular parts of coal seams are suitable for
mining and which method of desulphurization The basic consideration in the research of each
to use. The most convenient means of obtaining new measuring method must start from a known
this information is from geological boreholes. and/or hypothetical distribution of the material
Such direct measurement of sulphur has only to be measured in the volume under study, with
become feasible with the advance of the theore- a set target in terms of the quality of results of
tical and technical tools of nuclear physics the measurements to be achieved (accuracy,
during the last twenty years. Nargolwalla et al. reproducibility, sensitivity). If the interpreted
(1977) stimulated interest in the possibility of results of the measurements have to represent
such measuring equipment, but in spite of real properties of the volume under study with
verification of the principles of his method in sufficient accuracy the two above-mentioned
the laboratory, a successful field logging appli- conditions must be mutually dependent.
cation has not yet been realized. Information about the distribution of sulphur
In 1992 a special gammaspectrometer for in each ten-centimetre long segment of the coal
detection of the prompt gamma-ray spectrum bed in both the horizontal and vertical directions
generated by the capture of thermal neutrons was can be obtained from the following data, which
developed as the result of an initiative by VGP illustrate a one-metre long interval of the
(Borehole and Geological Prospection) Osek and randomly chosen coal seam. The concentrations
Geofyzika Brno. This spectrometer probe was of sulphur in the horizontal direction are (in %):
certified with very good results on artificially 1.9; 2.13; 2.28; 1.99; 1.27; 1.16; 0.83; 0.88; 1.05;
prepared laboratory samples. Research project 1.12 (the average concentration in the whole one
No. 105/93/1272, supported by the Grant Agency metre long interval is 1.5%-I-0.6%). The con-
of the Czech Republic continued in 1993 with the centrations of sulphur in vertical direction are (in
work mentioned above. The object of this project %): 2.96; 5.26; 4.49; 5.94; 7.12; 2.65; 4.15; 4.48;
was to develop a practical well-logging measure- 3.40; 2.21 (the average concentration of sulphur
ment system for the determination of the sulphur in the whole one metre interval is 4% •
content of coal beds. The project considers both From this data it can be seen that the individual
the field applications of the spectrometer and the values fluctuate considerably and the probability

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 297-307.
298 V. G R E G O R & A. TI~2K~:

(a) ..-.-.. S A M P L E S
SULPHUR ...... P R O B E
CONTENT (%)
12-

I0'

I
l ! i j. l J i l I , ! J j ! ! ! J ! J j i a
o I 2 8 4 5 0 7
DEPTH. (m)

(b) SAMPLES
SULPHUR PROBE
CONTENT (~)~

4-

I
\

2.

" ~ "~."~ ~_._~ ~Z~

0
0

HORIZONTAL DISTANCE (m)

Fig. 1. Sulphur distribution.

 SULPHUR CONTENT BY GAMMASPECTROMETRY 299

that any of them would represent the average boreholes. The ability to use logging technology
value of the sulphur content in the whole in uncored boreholes will lead to a considerable
one-metre segment is very low. In the case of reduction in costs and to an increase of the speed
five-centimetre segments, the representation of prospecting operations. In consequence it will
of individual values is much more unfavourable. be possible to carry out prospecting operations
For laboratory analyses on core samples it is using a denser net of boreholes and by those
typical to measure the investigated volume in means to obtain results that are more represen-
only the first cubic decimetre. Because of the tative of the actual sulphur concentration in the
lateral and vertical variations in the sulphur coal seams under study.
content of coal seams it is necessary to take To conclude this chapter it is necessary to
much bigger sections of the coal seam for emphasize the fact that any logging equipment
sulphur analyses. One result of the study is for the direct detection of sulphur content cannot
that through increasing the number of the be calibrated from the results of laboratory
analysed volumes a much better representation analyses of samples from boreholes drilled
of the results is obtained, because the average through a coal seam. From the point of view of
value of the sulphur concentration in such big accuracy it is also impossible to compare the
segments is more constant. This can be reached results of these two methods of sulphur content
in practice only by means of well-logging. measurements properly. These two methods have
Furthermore, it is unreasonable to consider as very different radii of investigation and operate
valid for seam quality evaluation those values in on different parts of the coal stratum. This fact,
lower orders than units of wt% of sulphur. This together with the above-mentioned variability of
is because of the real distribution of sulphur in sulphur concentration in the seam results in a
coal seams. very low degree of correlation of the results of
V. Prokop (1994, pers. comm.) carried out a these two methods. Carrying out the laboratory
statistical evaluation of the mutual dependence analyses is convenient in such a case, when we
of sulphur content data that were obtained from must know exactly the concentration of sulphur
laboratory analyses of cores and from well- in a given sample of coal. Well-logging brings a
logging of the same boreholes. Figure la shows result representing an average value of sulphur
the sulphur distribution in coal matter when concentration in the vicinity of the borehole.
sampling at equidistant depth steps was used.
There is an example of a function in the same
diagram which shows how well-logging mea-
surement with its better radius of investigation The physical basis of the method
reflects the same coal bed. Figure l b shows the
situation in horizontal direction of a coal seam The first experiments to determine coal seam
in a similar way (the samples were taken from a sulphur concentration carried out by means of
surface of the bed). Our own observations classic well-logging methods were unsuccessful.
confirm published information that coal seams At that time the best results were obtained by
are formed by layers in a predominantly magnetic methods, thanks to the connection
horizontal attitude. Such a geometrical relation- between sulphur content and the presence of
ship is another important reason for using a iron. Only some of the nuclear methods among
well-logging method which has a much larger which are included theoretical possibilities of
radius of investigation. sulphur detection remained in the complex of
The obtained evidence indicates the following logging methods. X-ray fluorescence analysis
design requirements. The tool used in well- seems to be of limited use due to the very low
logging for sulphur concentration measurements radius of investigation and its very high depen-
must provide results from approximately one- dence on a clean and mechanically sound
metre long segments of the coal seam. The borehole surface. The activation analysis has
concentrations of sulphur in coal beds of SHR its spectrum in a higher level but its count rates
(North Bohemia Coal Basin) vary within a range are very low. The application of spectral
from 0.1% to about 20%. The calibration range analyses of prompt gamma rays generated by
of the tool must cover this range. Also, the tool the capture of thermal neutrons proved to be the
must be capable of achieving reproducibility to most convenient method. In this method char-
within one tenth of one per cent of sulphur acteristic gamma rays of high energy, up to
content, which is one numeric order lower than 10MeV, and of significant count rates are
is necessary for interpretation purposes. It is emitted from the chemical elements under
assumed that the measurements will take place study. As a consequence of high-energy
both in dry and in water-filled, cored or uncored gamma radiation only a little loss of energy
300 V. GREGOR & A. Tt~ZKY

takes place and so an adequately large radius of full absorption, and two escape peaks. The
investigation is achieved in this case. distance between the full peak and the two
The atomic nucleus is excited by the absorp- escape peaks is one and two times the annihila-
tion of a thermal neutron and it returns to the tion energy respectively (so-called single and
stable state in nearly 10-14s with the simulta- double escape).
neous emission of gamma quanta. It is necessary (3) Besides the peaks of sulphur, which are
to note here that gamma quanta in a similar our main interest, peaks from other elements,
range of energies can also arise from the inelastic which are present in significant quantities in
scatter of neutrons on their path from the coal (for example Fe, Si, A1, Mn, Ti, H, Zn,
neutron source. Some publications (for example K, Ca), are included in the spectrum. These
Serra 1984) say that in the case of inelastic peaks have a different position and energy
scatter there are influences especially from such heights when compared with the spectra of
elements as C, O, Si, Ca and possibly Fe and S, sulphur.
which could complicate the analysis of the As the consequence of above-mentioned influ-
resulting spectrum in the general case. Using a ences there are significant interferences generated
252Cf neutron source, the excited neutrons have in the spectrum. These interferences cannot
average energies about 2.3MeV, which is be resolved without using complicated mathe-
probabilistically too low to cause inelastic matical procedures. These procedures will be
scatter. We have never observed peaks corre- described later. A particularly significant inter-
sponding to the energies of inelastic scatter, even ference is that between the full peak of sul-
in case of very high carbon concentrations. phur, corresponding to an emission energy of
The situation in the spectra corresponding to 5.42 MeV, and the escape peaks resulting from
the mechanism of thermal neutron capture, the presence of Fe. In particular we would men-
which we are detecting in coal beds is not quite tion the single escape of Fe, whose full energies
simple. The following particular influences are are 6.018 and 5.920MeV. Such a situation is
included here. shown in Fig. 2, which is a representation of a
(1) The peaks corresponding to separate spectrum which was measured from a coal seam
energies are not straight lines. The reason for with a high concentration of sulphur. Sometimes
this lies in the resolution power of the detector it is not possible to ignore the influence of the
used (in the case of detector BGO (Bi4Ge3012) contribution of Ti and Mn (There are no visible
2"• 2" the resolution power for 137Cs is peaks of Ti or Mn in Fig. 2.).
approximately 11%). The selection of detectors closely determines
(2) Each characteristic energy of the gamma the physical basis of the measuring method. The
rays emitted by the elements present is mani- range of detectors available for selection is very
fested in the spectrum by three peaks: a peak of limited by the working conditions of the logging

PULSES

i
= ** ~ ,o ',136 ' ',~d ' ' 'l~O ' ' 't~ ' ~"tl~ ' ' '2b," ' ' ' z ~ d :" '.'~a' '

CHANNEL

Fig. 2. Spectrum from a coal seam with high concentrations of sulphur.

 SULPHUR CONTENT BY GAMMASPECTROMETRY 301

probe. It is not possible to use a detector of coal matter. Another advantage is in the
unsuitable proportions, nor a detector requiring increase in detection efficiency of the system.
controlled operating conditions in order for it to There is a further important difference
function. In practice there are two types of between the probe made by Geofyzika Brno
spectrometric detectors, either a semiconductor and earlier probes: all the resulting spectrum is
or a scintilator. In spite of some advantages of measured directly in the borehole now. The
semiconductor detectors (amongst the advan- spectrum is sent in digital form by means of a
tages is a high-resolution power and a good serial channel directly to the computer after its
thermal stability of the spectrum); their use is less detection. A 256 channel analyser controlled by
convenient especially for the following reasons: a microcomputer is used for distinguishing the
all semiconductor detectors in current produc- energies of the impulses coming from the
tion need cooling in cryostats; the small volume detector in the logging tool. The analyser is
and density of the detector means that its equipped with a progressive correction for the
effectiveness is small particularly in the range of dead time of the converter and with a time meter
energies that need to be detected. In the case of for limiting the time of the spectrum measure-
scintillation detectors, crystals of either NaI(T1) ment. The analyser is controlled by the compu-
or BGO types may be considered. Crystals of ter via the serial channel. Such a system has two
NaI(T1) have much worse spectrometric proper- main advantages; the transmission of the analo-
ties in the prompt gamma rays energy range of gue signal from the logging tool to the surface is
interest (approximately 3-10MeV) and much eliminated reducing potential electronic inter-
lower detection efficiency in comparison with ference with the signal, and it is not necessary
crystals of BGO. For these reasons and also for for the probe to be linked to the surface with a
the reason of the limited diameter of the logging coaxial cable. In the case of transmitting the
probe, the 2 " x 2" crystals of BGO have been analogue impulses from the borehole to the
chosen for our working detector. surface the use of coaxial cable is a necessity,
mainly because of the large bandwidth of signal
carried. Using the customary four-wire, steel-
plated logging cables for the operation with our
The measuring equipment spectrometric probe is sufficient.
An important precondition for the successful
The equipment used in the research of a well- processing of the measured spectra by means of
logging method for sulphur detection was mathematical methods is perfect spectra stabili-
constructed at Geofyzika Brno continuing the sation. The equipment used carries out this
tradition of the manufacture of nuclear technol- stabilization by reference to the position of the
ogy in this company. A special spectrometric very expressive full absorption peak of hydrogen
logging probe, described in greater detail by at the energy of 2.223 MeV.
Gregor & Kagparec (1993, pers. comm.) became The measurement process for the interpreta-
the basis of the measuring equipment. The tion of sulphur content and for the data
equipment includes a surface module with manipulation are controlled by an IBM PC
power supply and an interface for serial com- computer (a notebook model). The software
munication with the probe, it also includes a runs under the MSDOS operating system which
computer for checking the measurements and is a further advantage of this equipment.
for spectra recording and processing.
On the basis of many considerations, calcula-
tions and practical experimental attempts we The methods of processing the spectra
chose the following elements for our work. For
the neutron s o u r c e - 252Cf and the scintiblock All the information pertaining to the radiation
with a 2 " x 2" BGO crystal (produced by that originated from the elements present in a
Bicron) as a detector. This crystal has a several coal seam is contained in the spectrum which
times greater volume than the crystals used must be correctly measured and placed on the
earlier at FJFI VUT (Faculty of Nuclear energy axis. Figure 2 shows an example of a
Sciences and Physical Engineering, Technical spectrum obtained from a coal seam with a high
University of Prague) and at GIP (Geoindustria concentration of sulphur. It can be seen that
Prague) - it is nearly 10 to 15 times bigger. This there is a full peak from sulphur over channel
fact gives another advantage: lower heights of No. 170, and it can further be seen that there is a
escape peaks in comparison with the full peaks. last significant peak from iron over channel
This results in a decrease in mutual interference No. 240 and over channel No. 70 there is a peak
between the peaks of the elements present in the from hydrogen. If we use only the count rates
302 V. GREGOR & A. TI~ZKY

from selected energy windows for the quantita- present in the ash) which are detected in a coal of
tive interpretation of the spectra we receive a known composition. Such a condition is fulfilled
very limited quality of the results - in the same by means of a set of standards with one
manner as Nargolwalla et al. (1977) and later component of the spectrum predominant in
Drahofiovsk~ et al. (1986). In the latter work each of the standards. Then every new spectrum
there is an assumption that the limit of detection analysed is fitted to these unit spectra to provide
of sulphur is about 2% (if the content of Fe is no a minimalization of the deviations of derived
more than 1%) in the case of using BGO linear combinations of unit spectra from the
detectors and where the sulphur concentration spectrum being analysed. By such a process we
is around 3% the relative accuracy of inter- can derive coefficients for each component that
pretation is expected to be in the range 20-30%. are proportional to the concentrations of the
Nargolwalla et al. (1977) came to a similar elements present in the coal. The main advantage
conclusion. In accordance with this conclusion it of this process is the opportunity it provides for
is possible to achieve the accuracy around 8% removing a significant amount of the mutual
with his equipment but only for sulphur contents interferences created by the various elements
greater than 1%. The goal is therefore to find a present. As the method makes it possible to take
method for the interpretation of the spectra broader ranges of spectra for calculations, and
which is capable of processing a more significant the quality of the fit increases as a consequence of
part of the information present in the spectra. improved statistics, there is a significant increase
A method involving additional mathematical the uniqueness of the solution. In such a manner
processing of the measured data will primarily we can lower the detection threshold to concen-
make a possibility of the elimination of inter- trations of sulphur in coal of under 1%. This
ferences between different elements and will method was successfully used by Geofyzika Brno
make possible the interpretation of such quanti- in solving the problem of determination of U, Th
tative changes in the spectrum that cannot be and K, and it is still used in their field gamma
detected by the usual process of evaluation. Our spectrometer model GS 256.
effort is directed towards obtaining and compar- (c) The method of spectra deconvolution is
ing the results from the following three methods based on theoretical calculations which are based
of mathematically processing the spectrum. on the unique physical/mathematical parameters
(a) The method of empirical correction of the of the detection system (present in the probe).
standardized areas of the peaks. (b) The multi- A matrix of the responses to all the spectral
component statistical analysis. (c) The method energies belonging to the isotropic field of the
of deconvolution of the spectra. emitter is calculated. By means of the deconvolu-
In detail they are as follows: (a) Minima tion we try to create undistorted primary spectra
values of the spectra of prompt gamma rays from the measured spectra which have been
induced in a coal seam can be expressed by a distorted by measuring tool influences. In an
polynomial function. The constants of such ideal case it means that the spectrum detected by
a function vary from one spectrum to another, means of the BGO detector will be changed by
especially the constant A0 which expresses the means of deconvolution into a line spectrum in
shift in the y-axis. The above-mentioned func- which the height of the lines is directly propor-
tion describes a basic line which is fixed on tional to the concentration of any given element.
characteristic minima of the real spectrum. The In the real situation the escape peaks and the
area of the analysed peak of sulphur is then interferences connected with them are removed
standardized by means of the function value of from the spectrum and a considerable increase in
the basic line in the x-coordinate under the the ability of the whole measuring system to
maximum of the peak. The value obtained is differentiate individual peaks is evident.
corrected further according to the height of the Common to all these methods is the problem of
nearest peaks in the spectrum. In this way it is standardization in respect of the intensity of the
possible to remove interference and to find the average flow of thermal neutrons which produce
corrected value of the peak corresponding to the gamma radiation in the rock matter under
sulphur. In practice the influence of Fe (5.920, study. This average flow depends on the activity
6.018MeV) and in some cases also that of Ti of the neutron source used, on the density and
and Mn is eliminated, which is of great moderating characteristics of the strata in the
advantage. vicinity of the probe, and on the borehole
(b) The multicomponent statistical analysis geometry in the vicinity of the probe. The average
is based upon the unit spectra of all those flow of thermal neutrons cannot be measured
components under investigation (one component directly with sufficient accuracy in the field. It is
is sulphur, the other components are elements considered that the only possibility of solving the
 SULPHUR CONTENT BY GAMMASPECTROMETRY 303

problem is by deducing this quantity directly gamma radiation detected from the separate
from appropriately chosen intervals of the models were used in the construction of calibra-
spectrum obtained. We have successfully verified tion curves for the three interpreting methods
this in principle whilst obtaining the first described above.
measurements from the models during the testing (a) The calibration curve for the method of
the logging probe (Gregor & Kagparec 1993). empirical corrections is shown in Fig. 3. There
In the case of two last methods of interpreta- the concentration of S (in %) is plotted on the
tion it will be possible to add to the data x-axis, and the standardized response read from
concerning the sulphur concentration some spectra on the y-axis. Also shown are the graphs
information about the concentration of other which represent an approximate line of the
elements in the ash, such as for example Fe, Si, calibration curves for the cases of logging in
and possibly Ti. dry and in water-filled boreholes. The points for
drawing these curves are based on average values
of the standardized responses read at the depths
Discussion of results achieved on artificially of samples for which the results of laboratory
prepared models and in the field analyses on sulphur lay in a narrow range close
to some chosen values of sulphur concentration.
The logging probe developed by Geofyzika Brno Experimental measurements took place at the
was calibrated according to the sulphur content experimental base at Most (the coal mine CSA).
on six artificially prepared models of coal It will be necessary to continue with these
material. Each of these models had a nominal experimental measurements to obtain better
and uniform concentration of sulphur through- accuracy of the calibration curves. We anticipate
out the volume. The values of the concentrations reaching an accuracy of interpretation of around
in the artificial models were between 0.33% and 0.3-0.5% in the range from 1% to 15% by
10% sulphur by weight. The spectra of prompt weight of sulphur content using the analogue

STANDARDIZED RESPONSE

1.4

1,3
models

1,2
1

dry well
I~

J
1.0 i I i I i I i I I i
0 i 2 3 4 5 6 7 8 9 I0
SULPHUR CONCENTRATION (%)

Fig. 3. Calibration curves - empirical corrections method.

304 V. GREGOR & A. TI~ZK'Y

method of evaluation with the calibration plot results it is necessary to consider increasing the
(Fig. 3). We expect much higher accuracies in the quality of the primary spectrum (in terms of its
case of computer interpretation. energetic stability), achieving a more precise
(b) The calibration graph obtained by means analytical expression of the energetic depen-
of the multicomponent statistical analysis is dence of the resolution power of the detection
shown in Fig. 5. The interpretation of the system, a more detailed study of the speed of
obtained spectra was carried out by I. Ka~parec convergence, and the removal of the influence of
(Geofyzika Brno). The concentration of sulphur irregular jumps at the ends of spectra.
in the artificial samples is plotted on the x-axis, Figure 6 shows an indisputable advantage of
similarly to the above-mentioned example. The this method. The primary spectrum obtained
sulphur concentration evaluated by means of from the model with a 10% concentration of Ti is
the given method is plotted on the y-axis. We shown in Fig. 6a and the same spectrum after the
evaluated four different sets of measurements deconvolution is shown in Fig. 6b. As we can see
of the spectra from the individual models. The from these graphs, the superposition of the
course of the calibration curve itself and the escape peak has disappeared from the spectrum
relatively small deviation of the data from and an increase in resolution power has occurred.
the line prove this analysis to be correct. We In consequence the status of the interval of the Ti
assume the lower limit of resolution is around peaks (6.76MeV and 6.42MeV) has closely
0.3% of sulphur concentration and the sensi- approached the form of a line spectrum. The
tivity of measurement is round 0.1%. This spectrum after deconvolution therefore raises the
method also enables the determination of the con- possibility of distinguishing and quantitative
tent of some other elements present in the ash - evaluating of more chemical elements than the
Fe, Si, Ti - because the concentrations of these primary spectrum.
elements are the remaining components needed The reproducibility of measurements is an
for calculations of the sulphur content. important criterion for the use of the equipment
(c) The calibration graph obtained by means in the field. A basic set of such attempts was
of the method based on deconvolution is shown made at the coal mine (~SA. It was found that an
in Fig.v4. Calculations were made by J.Klusofi acceptable reproducibility could be achieved if
(FJFI CVUT). To achieve higher accuracy in the the time of measurement of one spectrum was

RESPONSE

30-

20-

-,1..
10-

0 1 2 3 4 5 6 7 8 9 10

SULPHUR CONCENTRATION (%)

Fig. 4. Calibration graph - deconvolution method.

 SULPHUR CONTENT BY GAMMASPECTROMETRY 305

400 s. The stage of reproducibility will depend We have not been able to determine exactly an
on the method of processing the spectra. We accurate value of the radius of investigation
found that the reproducibility did not noticeable under field conditions. Besides the technical
decrease even if the time taken for the measure- parameters of the probe, an accurate value of
ment of one spectrum was shortening by a half, the radius of investigation depends to a sub-
to 200 s. The effect of statistical fluctuations on stantial degree on the physical properties of the
the spectrum becomes noticeable when the surrounding matter (density, chemical composi-
measurement time is reduced below 200 s. tion of the matrix, porosity, saturation). Nar-
We consider the fact that results from view- golwalla et al. (1977) considers the radius of
point of sulphur content determination obtained investigation to be in the range of 40-50 cm for
from both dry and water-filled boreholes are his probe, Serra (1984) considers the radius to be
apparently equivalent to be a relatively surpris- in the range of 25-37cm for his probe. We
ing one. Certain particular properties of the registered radiation from a distance of about
spectra (total number of impulses, the distance 50 cm during our experimental measurements.
of a chosen peak of sulphur from the base line) The sensitivity of measurements to changes
are different but the interpretation results are in the diameter of the borehole is also connected
practically the same in both cases. This fact, on to the radius of investigation of the probe.
its own, demonstrates that the probe receives Changes in the borehole diameter as it passes
data from a relatively large radius around the through coal seams are usually significant. Our
detector. A water filled borehole is, for neutrons, conclusions can be demonstrated on measure-
an environment with high moderation and ments taken in a water-filled borehole in the area
absorption ability, but in spite of that there is of Strup6ice. Spectral measurements were taken
no noticeable loss of important information from between 32.0m and 41.8m depth in the
from the vicinity of the borehole. Neither was borehole. The diameter of the borehole varies
there a decrease in the measure of correlation between 0.13m and 0.26m, the greatest dia-
between the measurements made in the same meters of between 0.21 m-0.26 m being recorded
borehole with and without water. in the pelitic parts of the profile. Two minimum

RESPONSE

10
_

8-

7-

6-

3
................................................................................................................................................................................

i l ! i

0 1 2 3 4 5 6 7 8 9 10
SULPHUR CONCENTRATION (%)

Fig. 5. Calibration graph - multicomponent statistical analysis.

306 V. GREGOR & A. TI~ZK'Y

(a)
PULSES
Ti 6, 7 6 M e V
6, 42. H e Y

.... .... ,
2~0 24 0
CHANNEL

(b)
Spectrum after deconvolution
CHANNEL RESPONSE
1OOOOO ! 9

i! "
fl

4OOOO

20000 ......

0
1 2 3 4 5
ENERGY (HeV)

Fig. 6. (a) Primary spectrum and (b) the same spectrum after deconvolution.

values in the range 0.13m-0.14m are in one recorded spectra. The shapes of spectra are
case in coal of good quality (at c. 36m depth) considered to be practically independent of
and in the second case in coal with high changes in borehole diameter. Changes in the
ash content (at c. 39.5m depth). It can be shifts of spectra along the y-axis may be
seen that the differences between cavitation in compensated by means of the standardization
good quality coal seam and that in overlying of spectra during its further mathematical pro-
and underlying pelitic rocks are significant and cessing. Other changes of a similar type resulting
that it therefore helps us to express our opinion from an unequal flow of thermal neutrons may be
on the influence of borehole diameter on the similarly compensated. Nargolwalla et al. (1977)
 SULPHUR CONTENT BY GAMMASPECTROMETRY 307

also indicated only a rather small influence stage of calibration curves. (a) The method of
exerted by the borehole diameter on the results empirical corrections of the standardized areas
of measurements. of the peaks based on the elimination of
influence of escape peaks of Fe and Ti from
the full absorption peak of sulphur. (b) The
Conclusions multicomponent statistical analyses based on
fitting of measured spectra from unit spectra of
The results obtained during the solving of analysed components. (c) The method of decon-
problem of sulphur content determination by volution of the spectra which solves the return to
means of well-logging measurements based on primary, undistorted by measuring instrument,
analyses of prompt gamma radiation generated spectra by means of mathematical processing.
by the capture of thermal neutrons may be 5. Achieved results confirm the possibility of
summarized in following manner. sulphur content determination from about 0.3 to
1. A deep gammaspectrometer working with 0.5wt% of sulphur with the sensitivity of 0.1%
detector BGO and with neutron source 252Cf and the variation coefficient of 0.2% provided of
was developed and constructed. Working geo- measurement in coal seams of a good quality
metrical and mechanical parameters of the (low content of ash material).
probe were optimized during the laboratory 6. The presence of significant peaks of Fe, Si,
and field experiments. Ti in measured spectra shows the possibility of
2. The physical basis of the problem of well- detemination of these elements concentrations in
logging sulphur content determination by means ash material in future.
of prompt gamma radiation was studied. The
peak of sulphur at 5.42 MeV energy was chosen
for evaluation.
3. An optimal method of measuring and References
processing of spectra was designed. (a) The DRAHOlqOVSKY,R. et al. 1986. Kvantitativni stanoveni
quality of results (sulphur content determina- siry v hn~d6m uhli SHR primo z karot~2niho
tion) seems to be equivalent both in dry and m6?eni. Geoindustria Tuchlovice.
water-filled boreholes. (b) The spectra do not GREGOR, V. & KASPAREC,I. 1993. V~voj karot~2niho
depend substantially on the borehole diameters analyz~toru obsahu siry v uhli. MS-Geofyzika,
under common field conditions (diameters in the a.s. Brno.
NARGOLWALLA, S. S. et al. 1977. Nuclear Melalog
range from 0.1 to 0.25 m). (c) With respect to Grade Logging in Mineral Deposits. International
considered technological conditions the mea- Symposium of Nuclear Technique in Exploration.
surements should be done stationary for the Vienna, Austria, March.
time from 200 to 400 s for each measurement. SERRA, 0. 1984. Fundamentals of Well-logging Inter-
4. Several ways of interpreting spectra were pretation. The Acquisition of Logging Data.
studied. Three methods were worked out to the Elsevier, New York.
 A logging correlation scheme for the Main coal seam of the
North Bohemian brown coal basin, and the implications for the
palaeogeographical development of the basin
KAREL MACH

North-Bohemian Mines JSC, OHMG of Bilina Mines, 418 29 Bilina, Czech Republic

Abstract: A method for correlating the Main coal seam in the North Bohemian brown coal
basin by interpreting borehole logs is described. The most important well log was the
gamma-gamma density log, but in some boreholes it was also necessary to use the natural
radioactivity and electric resistance logs or technological sampling of the core. All these
methods, at various levels of sensitivity, reflect changes in the amount of organic matter in
the borehole profile. Vertical changes of coal matter content characterize variations of
sedimentation conditions. In close boreholes gamma-gamma density logs are easily
correlatable so that changes of sedimentation can be correlated over great distances. The
method has been used to correlate the main seam along the axis of the basin. The main result
of this correlation is that coal-bearing sedimentation occurred uninterruptedly along the
main axis of the basin, with the development of swamp and lake conditions. During the
swamp conditions peat accumulated over the majority of the present basin area, whilst
during the shallow lake conditions the region of clastic sedimentation was controlled by the
distance from the inflowing sediment source. The coal-bearing sedimentation cycle started
by a levelling of the palaeorelief by infilling the depressions, and was followed an extension
of the sedimentation area. Compaction of the previously deposited layers affected the
ensuing strata. No significant variations in stratal thickness were found along the length of
the main borehole line nor in any of the auxiliary lines whole, indicating that tectonic
controls in basin subsidence were unimportant. Thus changes of sedimentation conditions
dominantly of climatic conditions caused water levels in the basin area to fluctuate. For
many reasons it is concluded that the correlatable boundaries are isochronal. The
correlation scheme represents the first really objective correlation of the main coal seam
over the area of the whole North Bohemian basin.

Variations in the physical properties of coal some rock types, and for that reason it may not
seams offer a broad range of possibilities for be possible to extend the analysis results far
correlating an individual coal seam across a coal from the sample point. A further problem is that
basin. Amongst the many measurable proper- of core recovery and core quality, in that the
ties, are coal micropetrography, analyses of ash core presented to the geologist often bears little
content, combustible matter, water, sulphur, relationship to the strata in the ground. The
arsenic and many other trace elements, micro- small number of boreholes from which samples
palaeontological analyses, isotopic analyses - all have been taken for analysis also makes
of which result from analyses of samples taken correlation of the seam by its properties difficult.
either from the drill core or from outcrop. The M a n y of the above-mentioned deficiencies may
main problem hindering successful utilization of be overcome by logging methods involving non-
this data for the purposes of a detailed correla- destructive 'sampling' of borehole walls. The
tion of seam strata is the degree of subjectivity subjectivity factors diminish here and the net-
involved in sample taking. The seam is usually work of logging bores within the framework of
sampled according to its macroscopically dis- the North Bohemian brown coal basin (NBB) is
tinct properties, and this process will often unify very dense.
microscopically distinct rocks into greater inter- Geophysical logging methods, in contrast to
vals, and thereby result in a loss of important sampling for analysis, are dependent on mea-
distinguishing detail. This practice is encouraged surement of such physical properties of rocks as
both by the instantaneous requirements of electrical resistance, magnetic susceptibility, nat-
production practice and by the pressure to save ural radioactivity, thermal conductivity, reaction
costs on the geological survey. Some of the to irradiation by various types of incident
sampling methods used do attempt to remove radiation etc. The basis of the interpretation of
the subjectivity by systematic sampling at set the geophysical logging records of holes from
intervals, for instance by chip samples. Such which no core was taken has to be the
point sampling methods will work only with geophysical logs of those boreholes from which

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 309-320.
310 K. MACH

core was taken for analysis. Only where such coal seam. Because of the problems of sub-
correlation is possible throughout an area can jectivity in core sampling it is considered that the
geophysical logging methods be used with con- determination of the variation in ash content
fidence as a method to replace coring. Because of through the seam section is more effectively
the utilization of coal from the NBB as a major achieved by the method of density gamma-
source of energy, there exists a dense network gamma logging. The network of density
of boreholes with analysis data relating to gamma-gamma logged boreholes is comparable
the energy generating properties of the coal, with the network of cored boreholes and the
e.g. ash content, water and calorific value. From interval of logging measurement in the seam is of
the usability standpoint for correlation, the the order of centimetres (compared to sampling
most suitable analyses result from the detailed intervals in the cored seam sections of the order
sampling for ash content (calorific value and of decimetres or metres). Fluctuations in seam
water content are to a certain measure functions ash content are therefore mapped with max-
of the ash content). Many other physical imum detail both in plan and vertically. For this
properties that are measurable by geophysical reason the method of comparison of curves of
logging methods are also a function of the the density gamma-gamma logs is used as the
components of the ash material in coal. These principal method of correlation of coal and non-
are above all the density and natural radio- coal strata in the coal seam in the NBB.
activity and to great measure the electrical The potential of the method is illustrated by
resistance. Other geophysical logging methods reference to several boreholes in the vicinity of
are complementary and their use is restricted to Bilina mine (Fig. 1). The profiles of the curves of
strata differentiation outside the coal seam. adjoining boreholes are very similar so that the
Observation of seam strata in any open pit correlation of single coal and non-coal strata is
indicates that attempts to achieve a detailed possible despite fluctuations in thicknesses of
subdivision of individual coal seams will be best individual strata. The factor that limits the
aided by those geophysical logging methods distance over which reliable correlation might
whose results are proportional to the ash be is the high variability of the thickness of the
contents. The changes of sedimentation condi- succession in which the coal occurs. In the NBB
tions in the NBB were recorded, above all, on the thickness varies from several tens to several
the basis of the changes in ash content of the thousand metres. The potential of the method

B B
PA179 E,AE5 JU535 JU$3? JU$t5 JU~li3 JU/e~ E3"T75 SS'l"/; LP237

Fig. 1. Opencast Bilina part (B-B ~) of logging correlation scheme (curves of density GAMMA-GAMMA logging
from several bores with marked corellatable boundaries): 1, various correlatable boundaries; 2, gamma-gamma-
density log (density growths to the left).
 NORTH BOHEMIAN BROWN COAL BASIN LOGGING CORRELATION 311

for correlation is limited by underground mining and for that reason the paper will summarize the
of the seam, tectonics affecting the seam, consequences of the scheme for our knowledge
and mining of the seam by opencast methods of the formation of coal-bearing strata in the
before geophysical logging was introduced. In NBB. The scheme produced is confined to the
such areas it is necessary to use whatever period of origin of the coal seam and for that
information is available from any of the other reason it does not represent later geological
above-mentioned methods (ash contents, electro- events (besides the diagenetically conditioned
resistance logging). compaction of the sediments). The main finding
is that it shows a significant palaeogeographical
basin infilling. The presence of similar logged
sequences of strata in adjacent boreholes and the
D a t a used ability to correlate these sequences over dis-
tances comparable with size of the whole
The course of the line of boreholes used for
sedimentary basin show that the vertical varia-
construction of the logging scheme section is the
tion in ash contents in the seam is not random
result of their selection from a great amount of
from borehole to borehole but systematic across
available data according to several conditions.
the NBB. Above all it is evident that the
The adjacent profiles of boreholes had to be
changing sequence of sedimentary conditions
distinctly correlatable, the line should cross the
that is correlatable across such great distances
major seam structures and at the same time, at
have isochronal character. In other words while
least by its branches, run through the mining
the occurrence of one clay or coal strata in the
areas of operating giant opencast mines. The
boreholes in the area does not need to be
seam sections in areas of underground workings
interpreted as the consequence of one palaeo-
were, as far as it was possible, determined from
geographical event since it can be accounted for
boreholes that intersected pillars. Areas of total
by a gradual facies change, the repeated
extraction of the seam, if they did not provide at
occurrence of such distinctly comparable strata
least the results of detailed sampling of drill
as that indicated by the scheme, forces such a
core, were left out. For tactical reasons the areas
conclusion. This conclusion is intended to
of so-called abnormal seam development at the
resolve a discussion that has for many years
Most-Bilina-Duchcov margin of the basin were
involved geologists engaged in determining the
not included on the main section line. Abnor-
geology of the NBB. The principle has for some
mally great thicknesses of the seam in these
time been acknowledged in the Chomutov area
areas often created coal bonanzas that attracted
of the NBB where the coal seam is divided by
the miners during the early stages of the coal
clay interlayers (Zima 1986; Hor6i~ka 1988;
mining industry in the NBB. Unfortunately, this
Ov6arov 1988). However, it is not as easily
early extraction of the thicker coal has lead to
seen in the area of 'uniform' development of the
great problems during the recent collection of
seam to the northeast of a line from Most to
survey data. In spite of this shortage of data
Albrechtice. The detailed development of the
comment is made in the conclusion. An attempt
coal seam is concealed here by the diminishingly
has been made to include on the section the line
small thickness of the clay interlayers visible in
of all the borehole profiles that are considered
the Chomutov area, and the geological context
to cover the coal-bearing strata down to the
is in places complicated by the above-mentioned
apparently pre-Miocene underlying strata. Most
'abnormal' seam development, both of which
boreholes in the NBB do not, however, fulfil this
have resulted in the formulation of incorrect
condition so that it was necessary to use also
hypotheses. Correlation schemes in this area, for
many incompletely drilled boreholes. The final
those reasons, mostly consider the seam to be
course of the section line after the fulfilment of
split into three leaves according to the technol-
all the conditions could not be a straight line and
ogy of 'mining' methods (Vficl 1989; Brus et al.
it approaches the axis line of the basin only in a
1987; Hokr in Malkovsk) 1985). This is not the
zigzag way (Fig. 2).
first attempt to apply the above-mentioned
principle in this area of the NBB, but the work
of specialist geophysicist has been overlooked by
Result of correlation - isochrons the volume of work of geologists (D/tfia in V~icl
1989). Information from the thousands of
The result of this study is the first objectively logging curves was consequently not properly
constructed correlation scheme of the main coal utilized in this area. The present correlation
seam across the entire NBB. The full section, scheme was only applied to this area in 1993,
because of its size, is not capable of publication and it is considered that the submitted scheme
312 K. MACH

--q'-,g" , .,

~:~sw,Tz.-..,._-..,*usTl'A4 .u,~A~v/ I '

ITALq ~ ~"~, i
~.~ ~ --~ ~"~
-" J 9 I 9 m,~ ., t,J

North-Bohemian brown-coal basin ~

o,

/1'

- ~-"-ZY-"~ ( r~ o ~o =,,,,

Fig. 2. Orientation map of North-Bohemian brown-coal basin map with marking of bore lines, used in submitted
correlation scheme: 1, territories of cities; 2, borehole used in scheme; 3, borehole profiles presented in this paper;
4, borehole profiles used in shorted scheme (Fig. 3). I-IX, other mine localities I, Bilina Mine; II, Nfistup mines;
III, Libou~; VI, Merkur; V, Sverma; VI, VrMny; VII, VCSA; VIII, Kohinoor; IX, Chabafovice. X-XIV, villages
X, Albrechtice; XI, Hole~ice; XII, Nov+ Sedlo; XIII, Kundratice; XIV, Vysok~t Pec; XV, Kfem~; XVI, VIII,
Marifinsk6 Rad6ice).

redresses previous imbalances in the considera- given strata ends when their thickness reduces
tion of the available data and resolves the long- to zero or their petrographical composition
term dispute in a satisfactory way. closely approaches that of the overlying or
The conclusion that the whole sequence repre- underlying strata.
sents a single depositional event presupposes that From the correlation scheme it is evident that
single strata that are part of the given sequence the thickness of each coal stratum is very
and can be correlated for great distances could be consistent over great areas while the thickness
considered as isochronous horizons. The profiles of non-coal strata can quickly fluctuate from
of the logging curves enable single strata to be centimetres to several tens of metres. It is also
traced from borehole to borehole even where the the case that the petrographical composition of
thickness changes. At the same time the gradual coal strata is more consistent. The coal strata
changes in the petrographical composition of consist of various types of coal, clay coal and
single strata do not prevent their being traced coal claystones. On the other hand, the non-coal
for considerable distances. The ability to trace strata cover the broad spectrum of clastic rocks
 N O R T H BOHEMIAN BROWN COAL BASIN LOGGING CORRELATION 313

AHIOO KB107 DO 31B7 PE.30 V1~194 DNZOO MR56 ,1O425 ~ 26 20~

. I,.ERKUR" ,, LIBOL~" OROUZtqOVICEPEer'ICE ,,, VR.~NY" .. ~.S~" , KOHINCX]R" ,, B ~ . I I ~ { ~ J ) " TEPLICE ., C H J ~ V I C E "

B E

• 2 ~ 7 ~o 72
111111115
NITt]I 773,
7--110

Fig. 3. Shorted logging correlation scheme of main coal seam of North-Bohemian brown coal basin: 1-9 typical
correlatable parts of coal seam (this dividing of coal seam is used by miners in central part of basin; 1, upper
bench; 2, upper part of middle bench; 3, 4, 5 - 1., 2. and 3. subbenches of lower part of middle bench; 6, upper
part of lower bench; 7, lower part of lower bench; 8, upper part of 'lower seam'; 9, lower part of 'lower seam';
10, thick stratas of lake phase sediments; 11, underground mining; 12, number of borehole; 13, name of locality
or 'name' of mine. Position of boreholes see Fig. 2.

from claystones to coarse sands including their strata in the coal-forming swamp, there was a
mineralized f o r m s - sandstones and pelocarbo- regular alternation between the more or less
n a t e s - and include types with varying content undisturbed accumulation of material of plant
of material of plant origin. The growth of origin and whole-area flooding of the area by
thickness of non-coal strata is directly propor- sediment bearing streams. During both the
tional to the increase in coarse clastic material in peatbog phases and the very shallow lake
the sediment. From a palaeogeographical view phases, the basin area was supplied by streams
the scheme illustrates growth and development whose catchment areas are relatively well known
of the coal-forming swamp that existed in the from the association of heavy minerals in the
NBB area during the Miocene Period. During clastic sediments (Cadek et al. 1985). The
the whole period of the formation of the seam dominant southerly source of clastic material
314 K. MACH

into the basin did not change during the life of the axis of sediment contribution is revealed by
the coal-forming swamp in significant detail. compression of the former over-sedimented
What did change, however, were the positions strata sequences. The most typical example of
of entry of the stream mouths into the swamp such filling of a channel can be seen in the
and lake. Libou~ part of the scheme section (Fig. 4). The
relationship between the sand-clay and the silt-
clay sediments in one such stratal thickening is
Progress of lake phases shown in Fig. 5.
Figure 5 shows that the attitude of the sand
The positions of channel inflows into the swamp bedding inside the interlayer is unconformable
during lake stages is shown by the maximum against the clay sediments. The stratification and
thicknesses of clay interlayers connected by sand composition of the sand sediments correspond
accumulation. At each clay interlayer there can to the filling of a channel cut below the level of
theoretically be found at least one such channel. the water into which the stream is flowing
The documentation from the mining locality of (Reineck & Singh 1973). So in the section we
Libou~ and the results of drilling operations in can see the filling of the channel that brought
the Sverma a r e a - w e s t (Ov6arov 1988) show into the basin the previously deposited clay and
that the inflows change their path in the same way silt material. The sand bed shows a distinct
as a meandering river. The maximum thickness tendency towards an increase in the proportion
of an interlayer is present in the channel so of coarse clastic material in the earliest filling

RC135 RC132 KBI08 KBI0? NS117 NSl14

A X

t0lOre
Fig. 4. Opencast Libou~ part (A- A') of logging correlation scheme (curves of density GAMMA~3AMMA
logging from several bores with marked well correlatable boundaries). Position of this part see Fig.2. *l, various
correlatable boundaries; 2, gamma-gamma-density log (density growths to the left).
 NORTH BOHEMIAN BROWN COAL BASIN LOGGING CORRELATION 315

0 20 ~0 60 m
I I I I ~1 V-I m 5 Czl6 U-d7
Fig. 5. Documentation of lake phase from the walls of coal faces of Liboug mine: l, sands; 2, sandy clays;
3, claystones; 4, coal claystones; 5, coal; 6, coalyfied stumps; 7, diagenetical faults.

that decreases downstream, with the gradual strata and over areas comparable in size with
filling of the channel as stream speed decreases. the NBB basin area it becomes a practical
The following depositional sequence can be impossibility. The length of tongues of psam-
deduced: mites is apparently directly proportional to the
length of time for which the lake phase lasted
(1) Flooding; Sedimentation of mostly clay
and indirectly proportional to the degree of
material with the occasional return of
compaction of the previously deposited strata.
peatbog conditions where the water level
The largest most complex tongue formation in
decreases;
the Holegice- Nov~ S e d l o - Kundratice line
(2) Just below the sand bed itself; Subaqueous
extended to Kundratice and Vysokfi Pec, even
erosion of already deposited material;
to the margin of the basin. The development of
formation of bed profile;
this inflow is substantially more complicated and
(3) Further advance of channel face; Sedimen-
less well documented than the inflow described
tation of channel filling; gradual decrease
from the Liboug locality. The greater complexity
of rate of bed cut-through;
is caused above all by the longer period of
(4) Channel choking up; Decreasing of inflow;
existence of this inflow. The lake stages were
start of peatbog conditions.
here suppressed many times by abundant
In a given area these processes repeat one vegetation and the psammite beds themselves
after another, with short periods of flooding as a result of this changed position and channel
followed by the deposition of an interlayer and dimensions several times. Although the single
sand tongue. The significance of this flooding beds here are often of greater dimensions and
was not great, however, but it documents, their filling more sandy, their construction is
together with the coal claystones, stump hor- very similar to others elsewhere and they show
izons, and horizons of pelocarbonate concre- all the features described from the Liboug
tions, the fact that against the background of a locality. Within the sand strata filling the beds
major flood phase there were many small it is common to find cross stratification, but in
fluctuations in the hydrological regime of the contrast to the Libou~ locality the sand sedi-
area. The grain, composition and granularity of ments also occur outside the channel beds
clay sediment, away from the channel on the themselves in the form of concordantly laid
bottom of the greater part of the lake are strata, passing laterally into silty claystones. The
indirectly proportional to the distance from the Vrgany sand-clay accumulations may then be
tongues of the psammites, which is the con- considered as the development of a few psam-
sequence of a loss of flow speed across the mite tongues and associated beds in the frame-
broader lake area. Apart from the differentia- work of one great lake phase.
tion of clastic material according to granularity, Generally, the described phenomena represent
the mineralogial differentiation of the clay a very specific case of a river delta. The specificity
minerals found in the sediments has been lies in the extreme shallowness of the basin
affected by the reaction between lake water reservoir, in the flow leads, and in the extremely
and inflow water, as has also the differential high compaction of the beds filling the base of
laying down of some chemical elements carried the reservoir. While the classic delta of the
in solution. This phenomenon significantly Mississippi type (Reineck & Singh 1973) builds
complicates the geochemical correlation of into a practically unlimited sedimentation area in
316 K. MACH

the form of a sea, the delta of a river leading into flow into the basin must have been reduced so
a coal-forming swamp in its lake phase had at its that the flora managed relatively quickly to
disposal only a several decimetres deep reservoir colonise the quite flat drying floor of the swamp.
and any further sedimentation area it formed The effect of water flows leading into the
itself by compaction of the previously deposited peatbog was changed. As a result of the rising
sediments, primarily the peats and clays. The mass of peat and plant cover only relatively pure
very low water level in the flooded swamp is water penetrated into the interior of the peat
indicated by the low height of the preserved swamp while the clastic material was laid down
stump of trees that were covered by the lake soon after inflow into the peatbog. In these
sediment in the form of very broad extensions of marginal areas, in the direction of the water
the intraformation breccias (Mach 1993a) inside inflow a ring ledge of finely mixed sediments
the single interlayers. formed at the tongue, indicating regular changes
The depth of the lake ranged from decimetres in sedimentation type. The lateral transition of
to a maximum of 2 metres. The occurrence of these sediments towards the basin into coal
intraformational breccias and coal strata at the strata of equivalent age is gradational and
same time attest to occasional fluctuations of the relatively rapid so that the borehole logs
lake level leading to the drying-up of extensive commonly note the sudden change. The char-
areas of the lake bottom. The dynamics of the acteristic signs of sediments of this continuous
water flow resulted in clastic material not being inflow are, besides the rhythmicity, the alterna-
deposited in some parts of the lake, so that in tion between clastic sediments and sediments of
those areas the individual coal strata are not mixed material. The latter are composed of plant
divided by a non-coal interlayer. In these cases fragments and clastics, with the presence of
the inundation event can sometimes be proved stump horizons, prints of water plants including
by coal micropetrography (Malfin in Vficl 1989; root parts, root soils, and the occasional tests of
Malfin in Zima 1986), which has revealed the fresh-water bivalves together with abundant
occurrence of thin strata of 'allochthonous coal' lenticular sideritic sections with thickness up to
at this horizon. Apart from this evidence it is 50 cm. The stump horizons are accompanied by
only the weathering of outcrops of the coal seam sub-horizontal to obliquely laid stem parts of
in opencast mines that demonstrates any strati- trees, bearing the evidence of a long-term of
fication in the seemingly monotonous coal. On decomposition in air (the charred stems are
detailed inspection there is usually nothing on hollow and lack the rind). From a palaeobota-
the strata boundary-line that would indicate its nical standpoint it is the growth which periodi-
presence, although a very thin stratum of more cally occurs on this tongue that stretches into
clayey coal or a thin horizon of 'breaking' bog and is the same as the growth on the
fusinite is occasionally found. The existence of a adjacent peatbog. The occurrence of these
clay interlayer over a great area or the continu- sediments laterally splitting the coal strata, was
ing of this interlayer as a 'non-visible boundary- found in the correlation scheme at two places.
line' between the coal strata demonstrates the However, only one can be demonstrated in
exceptionally flat surface of the swamp before outcrop at an opencast mine. At the present time
the flooding. The occurrence of allochthonous in the detailed borehole survey there is another
coal implies penecontemporaneous erosion of feature of this type in the foreland of Vr~any
minor elevations in the peatbog by wave activity mine. It is considered to be of the same character
in the encroaching lake. It is not easy to by analogy with the Bilina mine, where the
understand what caused the flooding of such phenomenon is observable over a length of
an extensive area of peatbog. And in order to do several hundred metres. The character of the
so it is necessary to return to the peatbog sediments is very similar; this inflow existed for a
(swamp) phase of the development of the coal- period several times longer and persisted over
forming swamp. many lake phases of swamp development. By
interpretation of the changes on the geophysical
logging curves it is possible to detect the
The progress of peatbog phases beginning of this type of sedimentation. The
reliable identification of the termination of this
The extensive development of most coal seams phase, however, is not possible without the
over great areas comparable with the area of the detailed description of drill core, because the
entire coal-forming swamp demonstrates the accumulation of sediment from permanent flows
practically continuous extent of peatbog across in the peatbog phase can pass without noticeable
the area of swamp. This requires a levelling change into the accumulation of sand-clay
activity of the preceding lake phase. The water material in the lake phase (and vice versa) and
 NORTH BOHEMIAN BROWN COAL BASIN LOGGING CORRELATION 317

this transition is not manifested in any way on changes in the erosion base of this outflow. No
logging curves. The behaviour of sediment in the such outflow is either visible in the present area
vicinity of such features during compaction of the basin, or has been reliably proved. With
under the load of overlaying strata causes the regard to the effect of tectonic phenomena on
development of obliquely bowed strata, diag- the course of coal-bearing sedimentation, much
enetical polished surfaces and other effects that has been written, but there is little evidence of
might otherwise be explained by erroneous their ability to effect the relatively quick changes
hypotheses. of sedimentation conditions within the frame-
work of the whole basin. Above all the fluctua-
Causes of regime changes tions in thicknesses of both coal and non-coal
strata are mostly explicable in other ways than
There still remains the question of why the quiet syngenetic tectonism in the underlaying strata,
peatbog regime is so often disturbed by the lake and it is clear that sudden regionally limited
regime. By analogy with some recent local peat fluctuations of stratal thicknesses would have to
swamps (Titov 1952) it follows that the devel- accompany these movements. The correlation
opment of a peatbog of a size corresponding to scheme, however, dooes not give a cover of the
the NBB area must be interrupted by occasional whole basin so that it cannot be completely
flooding for a very simple reason. The marginal excluded that there exist places where, during
parts of a peatbog are so efficient a preventing the coal-bearing sedimentation, such movements
the inflow of mineral nutrients to its interior that were manifested.
during the amassing of peat, nutrients become
exhausted and increments of plant mass are near
to zero. The degradation of plant cover leads to Climatic changes
changes in the rate of evaporation from peatbog
Briefly summarized, there is much evidence that
and to terrain differentiation, caused by small
changes in the hydrological regime of the
fluctuations in mineral contents in the substrate.
swamp, or in the watershed of the inflows into
The peatbog stagnates and on its surface lakes
the swamp, were the originators of changes in
form that become connected into great water
sedimentation conditions in the NBB. As a main
areas acting by surge erosion on the formerly
cause of such hydrological changes, climatic
relatively dry places. The increase of the area of
changes must be considered the most probable.
clear water surface further lowers the evapora-
Periodical and relatively radical changes of
tion rates from the area and the lake gradually
climate have been proved in the Quaternary by
extends to cover the whole area of the peatbog.
many methods (Cilek 1993) and it is unreason-
At this stage the inflow will still be divided from
able to believe that such changes did not occur
the lake by the barrier formed by that area of the
in the Miocene. Some hydrological factors such
swamp still provided with nutrients by the
as for example water evaporation could be in
inflow, but the breaking of this barrier could
many cases influenced by internal processes,
cause an increase of water level across the whole
caused by the stagnation of successive incre-
swamp area. The dimensions of the basin are
ments of plant mass, or from the insufficiency of
such that an insignificant growth of water inflow
mineral nutrients, or from fires of the peat
could also result in a substantial increase in the
swamp vegetation.
water level of the swamp. The long-term flood-
ing of the swamp floor covering the stump parts
of trees and scrub leads to their dying and to the Some applications
quick decomposition of those parts of the plants
that are above the water level. The final The alternations of peat swamp conditions with
destruction of the peatbog could be achieved very shallow lake conditions is accompanied by
by surge erosion by the lake. The thin uncon- the existence of coal-forming swamp from the
nected horizons of fnsinitic coal, often occuring initial formation of the NBB until the definitive
especially in profiles of seams without interlayers end. Some sections of the lines of the correlation
are considered to be the result of fires, and fire scheme objectively document the fact that the
could be added to the list of factors that might cyclical exchanging of both regimes in the coal-
lead to the destruction of the swamp vegetation forming swamp is accompanied by a gradual
mentioned above. If it was the case that the extension of the whole basin area. From logging
basin was not isolated and that an outflow profiles it can be seen that the lowermost strata
existed somewhere, discharging the water from are limited in the direction of increasing
the swamp, then it could be that the movements palaeorelief. This phenomenon is the natural
of water level in the swamp were caused by consequence of the gradual infilling of primary
318 K. MACH

depressions in the palaeorelief. It is assumed that detailed solution here, it is considered to be

the total thickness of peat mass and included beyond the scope of this paper.
strata of clay materials in the area of uniform Finally, with reference to the 'geochemical
development of the seam in the Most area isochron' proposed by Elznic et al. (1986), its
immediately before the end of the coal-forming position only locally follows some of the
swamp conditions reached 250 metres or seven boundary-lines on the proposed scheme section,
times the present seam thickness (Hurnik 1972). but over greater areas of the NBB the isochron
It is no wonder that the total area of the NBB and the boundary lines intersect. It is considered
was at that time much greater than today and that the given boundary line, marking the change
that the seam found in erosional relicts of this in contents of some chemical elements and at the
basin contains only its topmost elements. These same time a change in composition of clay
relicts occur in the Pohradice and K~em)2 area, minerals, characterizes not a change of source
in areas of volcanic elevations in the Most and area but rather a change of position of the inflow
Bilina area, but also in other areas. At Bilina source of clastic material relative to a given place.
mine this phenomenon has been documentated In consequence practically the whole area to the
directly in the coal face (Mach 1994). west of a line from Most to Albrechtice is above
From the correlation scheme presented follow this isochron and many areas of uniform
the answers to many questions concerning the development of the seam are below the given
course of coal-forming sedimentation. The fol- boundary line. In transitional areas this geo-
lowing represent some of the more important chemical boundary line lies within the seam
points: where and when the coal-forming sedi- strata and often it cannot be unequivocally
mentation began and when, where and how it placed. In this regard it is relatively well docu-
finished (Fig. 6). It is clear that the first coal- mentated that many chemical elements are either
forming swamps appeared in the areas of Mines bound to the mineral matter (the ash) or organ-
Nfistup Tugimice and in the Most area. The ically to the coal mass (Bougka et al. 1972) and
cessation of coal-forming sedimentation in the differentation of the clastic material in the
whole basin happened in three stages. The first process of sedimentation of clay minerals in
stage ended the existence of the coal-forming the basin can be considered as proved (Sloupskfi
swamp in the Chomutov area, the second in the 1985; Divokfi 1987; Ruck~, et al. 1990). It is
majority of the rest of the basin and the third considered very probable that the differentiation
destroyed the peatbog in the area of Most- of many chemical elements occurred at the same
Rad6ice. Another problem resolved by the time as the sedimentary differentiation of
scheme is the problem of areas of so-called various minerals during the lake stages of the
abnormal development of the seam which are a life cycle of the coal-forming swamp . Similar
special case of psammitic tongues, arising in the differentiation could also have occurred with
lake phases of the life of the coal-forming swamp. the development of some authigenic minerals
They owe their development to: (carbonates etc.).
It is to be hoped that the proposed scheme,
(1) their position on a divided basin margin;
intentionally presented without a new scheme of
(2) their position in the bottom part of the
seam; stage names, will be accepted as having proved
the technical aspects and will, with further
(3) that besides the period of tongue develop-
improvement, form the basis of any new division
ment of further lake phase they did not
of the NBB. It is hoped that the final products of
bring the greater sedimentation of clastics
this scheme will be a series of new palaeogeo-
('uniform development of seam');
graphical maps documenting the development of
(4) the concentration in these areas of the
the NBB and explaining much that is currently
mouths of inflows carrying the clastic
disputed. In perspective a further understanding
material that ended the coal forming
conditions. of the processes leading to the development of
coal seams can be seen to be closely connected
The differential compression of the underlay- with the geological processes in this scheme. In
ing strata of the coal seam, the close proximity this respect, a reinterpretation of existing studies,
of compacting sand-clay accumulations forming carried out in accordance with the proposed
the strata overlying the coal seam, and the scheme can bring not only the verification of
compression effect of the psammitic tongues of the scheme, but also increased precision and
these inflows led to horizontal movements of the enrichment of the submitted theory. There is no
partially consolidated peat mass in the early doubt that a mechanistic use of the scheme
stages of the end of coal-bearing sedimentation. method would reveal some mistakes in the detail
Although it would be possible to outline a of the correlation as result of insufficient data.
 R 6

Fig. 6. Main stages of rise of coal-bearing sediments in North-Bohemian brown-coal basin: 1, crystalline rocks;
2, Cretaceous sediments; 3, volcano-clastics; 4, volcanites; 5, underlying clastic sediments; 6, peat to coal;
7, overlying and coal seam clastic sediments; 8, direction of water stream; 9, water level; 10, peat forming swamp.
(a) Levelling of depression of palaeorelief; rise of first swamps. (b) The regime of coal-forming swamp; gradual
increasing of its area. (c) Supppression of coal-forming sedimentation by start of lake conditions.
320 K. MACH

Conclusions CADEK, J., DUSEK, P. & ELZNIC, A. 1986. Nov6

poznatky o geologick6m @voji komplexu mio-
Under the conditions of the NBB the interpreta- c6nnich sedimentfi severo6esk6 pfinve. - Sbor. V.
tion of g a m m a - g a m m a - d e n s i t y logs has proved uhel. konf. pfirodov, fak. (Praha), 21-25, Praha.
to be the most useful method of stratigraphic CILEK, V. 1993. V~,sledky ledov~ho vrtu SUMMIT v
correlation within the main coal seam. The Gr6nsku. Vesmir, 72/11,624-627, Praha.
qualitative character of logs gives the possibility DIVOKA, H. 1987. Zhodnoceni nerost6ho slo~eni
sedimentfi DJS z hlediska dobyvatelnosti.
of correlating logs measured under different VI)HU Most, Most.
conditions (various method of boring etc.) and ELZNIC, A. 1986. Problematika fizemniho 6len6ni
correlation of technologically unequal strata. severo6esk6 hnadouheln6 pfinve. Sbor. VII. uhel.
This method eliminates most of the potential konf. pfirodov, fak. (Praha), 71-74, Praha.
subjective aspects, which arise from sampling HOR(~ICKA, L. 1988. Dil6i zfiv6re6nfi zprfiva fikolu
core. The method with the best results reflects Prun6fov - Chomutov. Geoindustria, n.p. Praha,
variations of ash contents in vertical profiles of Praha.
the coal seam. This shows variations of sedi- HURNiK, S. 1972. Koeficient sednuti n6kter~ch sedi-
mentation conditions with time at the point of mentfi v Severoeeskb hnadouhelnb pfinvi. Casopis
pro mineralogii a geologii, 17/4, 365-372, Praha.
boring. Using this method in the NBB it is MACH, K. 1993a. Intraformaeni brekcie na VMG v
possible to determine isochronous horizons Bilinfi. Zpravodaj SHD, 3/1993, 11-16, VUHU
within the main coal seam stratigraphic interval Most, Most.
and thus derive more precise knowledge about 1993b. Korelace vrstev hlavni uheln6 sloje mezi
the internal structure of the coal deposit. lomy Bilina, Kopisty a V(~SA. Zpravodaj SHD,
4/1993, 31-40, VUHU Most, Most.
My thanks for help in acquiring logging documenta- - - 1 9 9 4 . Dokumentace rozgi~ov~.niuhlotvorn+ ba~iny
tion of boreholes and for accompanying me on visits to na VMG. Zpravodaj SHD, 3/1994, 24-30, VUHU
NBB mining localities goes to colleagues working in Most, Most.
various mining and NBB survey organizations; above MALKOVSKY, M. et al. 1985. Geologie severoeesk6
all to: I. Strbfifi, P. Sulcek, J. RehoL O. Jane6ek, hn6douheln6 pfinve a jejiho okoli. UUG, Acade-
F. Folt)n, P. Coufal and J. Prochfizka. Special thanks mia, Praha.
are due to J. Zima and L. Hor~i6ka for enabling me to REINECK, H. E. & SINGH, I. B. 1973. Depositional
have access to the adjusted sections of partial correla- Sedimentary Environments. Springer, Berlin.
tion logging schemes of some parts of the Chomutov OV(~AROV, K. et al. 1988. Zfiv6re6nfi zprfiva fikolu
NBB area, and assisting me in their elaboration. Sverma - zfipad. Geoindustria, st.p. Praha, Praha.
RUCKY, P., SLOUPSK.~,M. & THIELEV. 1990. Zhodno-
ceni dob~vac!ch podminek na lomu Vrgany do
roku 1990. VUHU Most, Most.
SLOUPSKA, M. 1985. Nerostn6 slo~.eni terciernich
References sedimentfi SHR. VI)HU Most, Most.
TtTOV, I. A. 1952. Vzaimod6jstvie rastit61nych soobg-
BOUSKA, V., JAKES, P., PACES, T., POKORN~"J. et al. 6estv i uslovij sredy. Sovjetskaja Nauka, Moskva.
1980. Geochemie. Academia Praha, Praha. VACL, J. et al. 1989. Zfiv6re6n/t zpr~tva fikolu velkolom
BRUS, Z., ELZNIC, A., HURN~K, S. & ZELENKA, O. Maxim Gorkij. Geoindustria, st.p. Praha, Praha.
1987. Geologie oblasti. - XXVI. Celostfitni kon- ZiMA, J. et al. 1986. Zfiv~re6nfizprfiva fikolu LibouL
ference CSMG,VUHU Most, Most. Geoindustria, n.p. Praha, Praha.
 Seismic monitoring for rockburst prevention
in the Ostrava-Karvinfi Coalfield, Czech Republic
KAREL HOLUB

Institute of Geonics, Academy of Sciences of the Czech Republic,

Studentskd 1768, 70800 Ostrava-Poruba, Czech Republic

Abstract: Seismic activity in the Ostrava-Karvinfi Coalfield is continuously monitored by

networks of seismographic stations located both underground and on the surface. Software
has been implemented for statistical analysis and various types of data display to aid
interpretation. Practical experience obtained in long-term seismic monitoring has proved
that it is an indispensable part of the rockburst prevention scheme applied in underground
mines in this region. Continuous seismic monitoring enables us to delimit seismically active
areas, observe the trends of seismic activity in time and space so that we can make more
accurate estimates of local rockburst hazard, and check the effectiveness of the rockburst
prevention methods used.

The Ostrava-Karvinfi Coalfield is the south- Local and regional seismographic networks
western part of the Upper Silesian Coal Basin
which extends from southern Poland into the Original plans for the distribution of seismo-
Czech Republic (Fig. 1). This mining district is graphic stations were based on the expected
situated in a geologically complicated region lifetimes of mines in the regions prone to
around the contact between two large tectonic rockbursts. Since 1983, when the strongest
units, the older Bohemian Massif and the recorded rockburst occurred in the (~SA Mine
younger Carpathians Mountains. Seismic activ- (E-- 10 l~ J) the basic network has been gradu-
ity induced by underground mining in the ally expanded with new types of digital seismic
Ostrava-Karvinfi Coalfield has been observed systems. The automation of procedures for
since 1912, and is superimposed on a back- detection, recording and processing of seismic
ground of weak natural seismic activity in the events provided by these systems has made it
area. The foci of these weak earthquakes are possible to determine the locations of hypocen-
mostly concentrated in the Jeseniky Mountains tres and to quantify the seismic energy released
and in the neighbourhood of Opava and 0esk~ by individual events within a broad-band
T~in (K/trnik et al. 1954; Prochfizkovfi 1994), as energy scale.
shown in Fig. 1.
Long-term seismological observations using a
single recording station started in the Ostrava- Local seismographic network
Karvinfi Coalfield in 1977, and over the next
two decades 42 stations equipped with digital At present, this network of vertical seismometers
instrumentation were installed. Since seismolo- represents a widespread system which operates
gical monitoring started in this region, the in all mines except for the Franti~e and CSM
association between mining-induced seismic Mines (see Fig. 2). The seismometers are mostly
events and rockbursts causing great damage installed underground, although there are a few
to mine workings has been proved. Interpreta- on the surface. All stations are equipped with
tion of observations has made it possible to digital instrumentation for application auto-
develop new procedures for objective assess- matic procedures. These include data recording
ments of rockburst hazard, and consequently to at individual mines, and also determination of
apply rockburst prevention measures in under- arrival times and amplitudes of P and S-waves.
ground coal mines. After this pre-processing, the data are trans-
This paper reports on the procedures cur- mitted by modem connection to the operational
rently used as part of the rockburst prevention centre at the (~SA Mine. Further processing is
scheme applied by individual mines located done there to obtain the hypocentral coordi-
in the eastern part of the Ostrava-Karvinfi nates, estimated energy and origin time of
Coalfield. seismic events, which are then stored in a

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geologyand Technology',
Geological Society Special Publication No. 125, pp. 321-328.
322 K. HOLUB

% | % ~,

%% "%

--NMO VOS ES BASn

Fig. 1. Schematic structural map of the Bohemian Massif (after Dopita & Kumpera, 1993) also showing location
of the Ostrava-Karvimi Coalfield.

database. The data resulting from the final to a central laboratory. The results of contin-
interpretation are daily transmitted back to uous observations of a regional character are
individual geophysical and geomechanical used to create a database of current information,
laboratories at the respective mines. In parallel constraining arrival times of P and S-waves,
with the geophysical database, a technological hypocentral coordinates, seismic energy and/or
database stores data describing the daily posi- magnitude estimate of the recorded seismic
tions of the coal faces and the blasting opera- events. This database represents an essential
tions performed (location and explosive charge source of information for the geomechanical
sizes). A more detailed description concerning service of the Mine Survey and Safety institute,
the monitoring and analysis of induced seismi- based at Paskov, near Ostrava. First arrival
city observations is given by Holub et al. (1995). times of P-waves recorded by the regional
network are also included in the database for
the local seismographic network at the (~SA
Regional network Mine, and are used for hypocentral locations by
this monitoring system.
The regional network consisting of ten three-
component stations equipped with Lennartz
Electronic instrumentation covers the whole Long-term observations of induced seismicity
mining district. Three stations are situated
underground and seven are located at the surface Spatial distribution of hypocentres
(Fig. 2). The OKC seismic station, which
doubles as one of the ten monitoring stations Many major faults with different throws and
of this network, is located about 20 km west of dips, define a complicated block-structure of the
the centre of the mining area. The instrumenta- Ostrava-Karvin/t Coalfield. The blocks deli-
tion at each station provides for automatic data neated by these major tectonic faults were used
recording, pre-processing and radio transmission as elementary units in the planning of the layout
 SEISMIC MONITORING FOR ROCKBURST PREVENTION 323

! ?

/ ~'~ ~ ""- 9 9 .~. ,,

underground 9 9
o []
/ DOUBRAVA".] surface
/ 9 /........
,
F'"-" "
9 ! ; . . . . . i"
9 .-J . 01,~ SA ~.j": ..
\..
9
[30KC ./ ~_ . . . . . . . . "_...i" "x 9
/ 9 LAZY
.Zl . .~. . . . . . l,---, 9 !' " 9 9 D A R K O V I I . . . . . . . . . "-/" 7
i
'k 9 F 9 '"" 9 ''- 9.
j " N.

, ~ 9 9 e- ........ j , ,. \.
9 ] 0.
/ I I

i " / i i (~SM
L....DUKLA . F R A N T I ~ E K P i [3 \.
\
"'"( ---... ~.KV~TENI
0 .~km ""' 9 9 i ..... ,,2"
L , t I I I

Fig. 2. Distribution of seismographic stations in the Ostrava-Karvin~ Coalfield: 1, local seismographic network;
2, regional seismic network.

of mines. Each mine take consists of several impossible to infer the causes of individual
tectonic blocks, in which individual coal seams seismic events. This may imply that some
are gradually being mined by longwall methods 9 tectonically distinct blocks are combined in
In the mines of interest here, only longwall units of greater size in which mining-induced
retreat faces are used, either with caving and/or stresses interact, while other blocks demarcate
the low-pressure stowing method 9In contrast to self-contained areas within which seismic events
the distribution of earthquake hypocentres along are induced only by local mining activity.
tectonic faults, analysis of the hypocentres of
induced seismic events has proved that the great
majority of them were concentrated in areas of Temporal changes in the distribution of
current mining activity. Only rarely were hypo- hypocentres and release of se&mic energy
centres located in the vicinity of major faults, and
in those cases could the events be attributed to In addition to the spatial distribution of
tectonic movements induced by mining 9 hypocentres, the time-dependent changes in
According to the location plots from long- distribution provide very important complemen-
term observations over the whole region, areas tary information concerning the seismic regime.
with higher concentrations of hypocentres exist. Benioff graphs are usually used to show how
For the correct interpretation of a particular seismic energy release varies with time. In these
location plot, comparison with contemporary graphs, the so-called strain release is calculated
mining activities in the area investigated is as the square root of the amount of seismic
necessary. As a result, it has been possible to energy released, and is assumed to be propor-
identify isolated areas of seismic activity where tional to the amount of elastic deformation
the hypocentres are clustered around the active released from the rocks in the vicinity of each
mine workings within a single tectonic block, hypocentre. The overall trend is represented by
e.g. blocks 5 and 7 in the CSA Mine, blocks 2, 3 plotting the cumulative amount of strain release,
and 4 in the Dukla Mine, block 7 in the Lazy whilst the details are more clearly seen by
Mine and block 6 in the Darkov Mine (Fig. 3). plotting the daily amount of strain release 9
By contrast, there were other highly active areas Distinctively different patterns of seismic
which overlapped several tectonic blocks, e.g. in energy release occur as successive longwall
the vicinity of block 3 in the CSA Mine (Fig. 3). panels are worked 9 A particularly obvious
Under the latter circumstances, it was practically example is given in Fig. 4, during mining of
324 K. HOLUB

Fig. 3. Location plot of seismic event (E > 102 J) epicentres located during 1992. Mine takes and tectonic blocks
are demarcated by thick and thin lines, respectively. In the upper right corner the energy scale is given.

adjacent longwall panels in the 7th tectonic Another example of the process of seismic
block at the CSA Mine. Mining panel no. 17331 energy release during longwall operation comes
induced a very low level of seismic activity and from face no. 13933 at the CSA Mine (Fig. 5).
was completed without any occurrence of a large Without respect to the fact that this longwall
seismic event. In contrast, extraction of the panel was the first one, mined in the seam no.39
adjacent panel, no. 17332, induced a high level in the 3rd tectonic block, the situation from the
of seismic activity, manifested by a steep slope viewpoint of geomechanics was here very
on the graph of cumulative strain release, hazardeous, all preventative measures are inten-
exceeding the value of S l i m = 15 J1/2/day in the sified. It is worthwhile to mention that this area
graph of diurnal increment (Fig. 4) whose was affected by the strongest rockburst
definition will be given below. During coal (E=101~ which occurred in the whole
extraction by longwall face no. 17332, only a Ostrava-Karvinfi Coalfield in 1983. Further
single strong rockburst ( E = 107j) occurred, in details concerning this longwall panel operation
January 1992. Almost a month later, this long- and results of seismological observations have
wall face was stopped and the release of seismic been given by Kalenda et al. (1992).
energy rapidly decreased. This example is in
good agreement with general geomechanical
considerations, for the operation of the first Frequency-energy distribution
longwall in the appropriate tectonic block
usually proceeds without any problems. A This distribution can be described by a formula
higher degree of seismic hazard may be expected given by Gutenberg and Richter (1954), which
subsequently when mining neighbourhood long- for our purposes can be written as log N - - a -
wall panels, especially the third or fourth panels b l o s E where N is the cumulative number of
in an area when a substantial part of the coal events with energy within the prescribed
seam in the investigated tectonic block has been energetic window, E is the amount of seis-
extracted and the area affected has been mic energy released in a single event, and a
enlarged. and b are numerical constants. This formula
 SEISMIC MONITORING FOR ROCKBURST PREVENTION 325

Fig. 4. (a) Benioff graph and (b) its diurnal increment during mining operations for longwall faces nos. 17331 and
17332 in the 7th tectonic block at the CSA Mine. The period of working for each panel is shown in (a) by lines
parallel to the time axis.

represents a straight line, whose slope b char- A typical example of the time-space variation
acterizes the number of weak seismic events of b-values was the effect of mining operations
relative to the number of strong ones. For on seismic activity when the single longwall
fitting real data sets, two different approaches panel no. 13933 was mined in the 3rd tectonic
to b-value determination were applied. The first block at the (~SA Mine in 1990-1991 (Fig. 6).
method is based on the calculation of slope b An examination of the b-value variations has
of the straight line using least-squares regres- revealed that the higher b-values were found in
sion, while the other known as the maximum 1989 before starting the mining operations
likelihood method, was suggested by Aki ( b l - 0 . 7 4 - 0 . 8 0 and b 2 = 0 . 6 7 - 0 . 8 0 ) . After
(1965) and Utsu (1965) for analysing earth- coal winning started during 1990-1991, lower
quakes. The advantage of the latter method is values were established (b~--0.38- 0.55 and
that single strong seismic events (induced b 2 = 0 . 2 9 - 0.41). The b~-values were computed
events and/or earthquakes) have less influence by using least squares regression, and the
on the estimated slope b of the regression b2-values by means of the maximum likelihood
straight line. The software in use at the method.
operational centre enables the b-values for
different regions (the whole coal mine district,
mine, or tectonic block) to be calculated. In Utilization of long-term seismological
our computations, all data sets are strictly observations in geomechanical practice
limited to events having a minimum energy
value of 102j. Due to different approaches in In the Ostrava-Karvinfi coal mines, all seams
the b-value calculation, only slight differences and mine workings are classified in one of
in the resulting values appear to have occurred three categories of the rockburst hazard accord-
(Slavlk et al. 1992; Holub 1996). ing to the prevailing geological (e.g. type of
326 K. HOLUB

Fig. 5. (a) Benioff graph and (b) its diurnal increment for the 3rd tectonic block at the (~SA Mine before and
during mining of longwall panel no. 13933. The period of working is shown in (a) by a line parallel to the
time axis.

sedimentary rocks, tectonics, depth of the coal choice of mining equipment and others)
seam) and geomechanical (e.g. mechanical- which could prevent rockbursts occurrence
physical properties of sediments, mined out area and/or mitigate their consequences. The cri-
and edges of unmined seams in the roof, occur- teria for assigning areas to third category are
rence of the rockbursts in the past) conditions: not always in agreement with the real rock-
burst hazard, resulting in an overestimate
9 (1) Rockburst occurrence is not expected of the number of regions in this category.
during mining operations even if no pre- Therefore it was recommended that mine
ventative measures are applied workings should be classified for rockburst
9 (2) Rockburst occurrence cannot be hazard using the results of long-term seismo-
excluded during mining operations unless logical observations.
preventative measures are applied At present, applications of the seismic obser-
9 (3) Rockburst occurrence is to be expected vations are directed towards the determination
unless preventative measures are applied. of seismically active regions, monitoring the
This category includes mine workings development of seismic activity to assess rock-
where rockbursts have already occurred bursts hazard, and checking the efficiency of the
measures applied to prevent rockbursts. The
For mine workings in the third category, objectives of these efforts are:
extensive active preventative measures are
obligatory, e.g. destressing blasting in the 9 to determine regions where active and
seam, drilling tests, camouflet shotfiring of a passive preventative measures would have
large amount of explosives in the roof above a to be applied
longwall face, water infusion, and others. In 9 to check the effectiveness of the active
contrast to active preventative measures, the preventative measures applied
passive ones, are aimed at specific activities 9 to reclassify mine workings according to the
(e.g. mine design, mine field development, degree of rockburst hazard
 SEISMIC M O N I T O R I N G FOR ROCKBURST PREVENTION 327

1189 * 6189 [bl = 0,74_+ 0.07 I

3~
1bz=0.67 +-0.101 ,b: 0.80+0.19[
x x x }
2 x x x x

bl bz

I I I i ' ' ' ' ' ' ' '

"~ 2 3 4 5 6 1 2 3 4 5 6
log E ( J ) log E ( J )

7/9o. 12/s0 [ b l = 0.38 +_ 0.02

x x x
I b~bl = 0.44
"~176176176 + 0.03
0.37 _+0.04II
=
Z
I b2 = 0.29 + 0.03
x x X X X x

2,

0 , : : : : : ', : : ', t t I J i I I l [ I =

0 1 2 3 4 5 6 0 1 2 3 4 5 6
IogE(J) IogE(J)

1191 6/91 !
v9t. 12/91 [ bl = 0.55 __.0.03]
q

b~ = 0.48 + 0.03[
i

X
bz = 0.35 - 0.021 9
I b~ = 0.41 + 0,031
x x x x x x x ~
9 x x x

I t I * ~ I I I ( I ! I ! ', I ! ~ 1 ! :

1 2 3 4 5 6 0 1 2 3 4 5 6 7
IogE(J) log E ( J )

Fig. 6. Frequency-energy distributions of seismic events located in the 3rd tectonic block at the CSA Mine before
mining (January-December 1989) and during operation of longwall face no. 13933 (January 1990-December
1991). bl and b2 were calculated using least-squares regression and the maximum likelihood method, respectively.

On the negative side, all efforts aimed at be excluded and all active preventative measures
predicting the times of rockbursts with greater must be taken. Values of diurnal increment
precision are very questionable, in common with greater than 15j1/2/day were found in all areas
the general experience for earthquake prediction. where a rockburst had previously occurred
The analysis of long-term observations has (Holub et al. 1991). As an example of this
shown that for any region of the coalfield a approach, the reclassification of individual mine
value Sli m c a n be defined. This value represents workings into lower categories of rockburst
the maximum diurnal increment in strain release hazard has been proposed and in several cases
(in units of J1/2/day) for which the probability of this has been done. However, the diurnal
rockburst occurrence is negligible. It can gen- increments in strain release are not the only
erally be stated from our investigations of the parameter to be considered. When making such
Ostrava-Karvin~i coal mines, that the value of a decision, one take into account many factors,
Sli m is 15 j1/2/day, i.e. this is considered to be a such as the level of the seismic activity, location
safe value for continued mining provided that it plots, geological and tectonical situation, and
has not been exceeded during the two preceding the effects of old workings in adjacent areas.
months. Once the value S=15j1/2/day is Destressing blasting and camouflet shotfiring
exceeded, the occurrence of a rockburst cannot of a large amount of explosives are the principal
328 K. HOLUB

preventative measures employed to reduce rock- References

burst hazard. Their effectiveness can be checked
by using seismic methods. Whereas we have AKI, K. 1965. Maximum likelihood estimate of b in
primarily investigated the effectiveness of the formula log N = a bM and its confidence limits.
latter method, the investigations in Polish mines Bulletin of the Earthquake Research Institute,
are aimed at checking the effectiveness of Tokyo University, 43, 237-239.
destressing blasting with charges of up to 300 DOPITA, M. & KUMPERA, O. 1993. Geology of
the Ostrava-Karvinfi Coalfield, Upper Silesian
kg, as reported by Filipek et al. (1992) and
Basin, Czech Republic, and its influence on
Dubinski & Syrek (1994). For our work with mining. International Journal of Coal Geology,
camouflet shotfiring in the Ostrava-Karvinfi 23, 291-321.
coal mines, an empirical formula is used for DUBINSKI, J. & SYREK, B. 1994. The effectiveness of
estimating the efficiency of the large explosions destressing blasts performed in the Wujek Coal
(up to 3000kg): Mine. In: RAKOWSKk Z. (ed.) Geomechanics 93.
Balkema, Rotterdam, 59-62.
~7 = E s / 2 . 6 Q FILIPEK, M., MITREGA, P. & SYREK, B. 1992. An
attempt to assess the efficiency of destressing
where Es is the seismic energy in joules blasting performed in longwalls with caving under
determined by using interpreted data from high rockburst hazard conditions. Publications of
seismograms and Q is the amount of explosives the Institute of Geophysics of the Polish Academy
in kg. It is considered that if V > 3, then the of Sciences, M-16 (245), 319-332 (in Polish).
blasting has been effective in releasing accumu- GmowIcz, S. J. 1979. Space and time variations of the
lated strain energy. frequency magnitude relation for mining tremors
The application of b-value estimates to rock- in the Szombierki Coal Mine in the Upper Silesia,
Poland. Acta Geophysica Polonica, XXVII, No. 1
burst prediction in the Ostrava-Karvinfi coal
39-49.
mines is still under evaluation at the present GUTENBERG, B. & RICHTER, C. F. 1954. Seismicity of
time. Preliminary results have confirmed the the Earth and Associated Phenomena. 2nd edn,
general validity of the b-value criterion, which Princeton University Press.
hypothesizes lower values in regions of higher HOLUB, K. 1996. Space-time variations of the fre-
rockburst hazard. At this stage of investigation, quency-energy relation for mining-induced seis-
only qualitative changes in time dependent micity in the Ostrava-Karvinfi Mining District.
b-values have been established, as reported, for Pure and Applied Geophysics, 146, 265-280.
example, by Gibowicz (1979) and Holub (1996). - - , VAJTER, Z., KNOTEK, S. t~ TRAVNICEK,L. 1991.
Application of results of seismologic monitoring
during the operation of mine workings in the
Ostrava-Karvinfi Coal Basin. Publications of the
Concluding remarks Institute of Geophysics of the Polish Academy of
The advantages of long-term continuous seis- Sciences, M-15 (235), 219-228.
- - , SLAViK,J. & KALENDA,P. 1995. Monitoring and
mological observations for assessing rockburst
analysis of seismicity in the Ostrava-Karvin~t
hazard in the Ostrava-Karvinfi coal mines are Coal Mine District. Acta Geophysica Polonica,
as follows. XLIII, No. l, 11-31.
Routine application of rockburst prevention KALENDA, P., SLAVIK, J., HOLUB, K. ~r VAJTER, Z.
measures is based on reliable predictions of 1992. Statistical analysis of induced seismicity
hazardeous conditions within the rock mass for parameters in the Ostrava-Karvinfi Coal Basin
those mines where the rockburst hazard exists. with regard to the 3rd tectonic block of the CSA
All possible measures are taken to increase the colliery. Acta Montana, 84, 85-96.
safety levels in mine workings where rockbursts KARNiK, V., MICHAL, E. & MOLNAR, A. 1958.
Erdbebenkatalog der Tschechoslowakei bis zum
represent a serious threat.
Jahre 1956. Travaux Gdophysiques, 69, N(~SAV,
Efficient application of preventative measures Praha, 411-598.
at appropriate times minimizes stoppages in coal PROCHAZKOVA, D. 1994. Earthquakes in the Jeseniky
production, and represents substantial reduc- Mts. in 1986. Travaux Gdophysiques, XXXVI
tions in costs which have been confirmed by (1988-1992), Geophys. Inst. of CAS, Praha,
several individual mines. 28-38.
SLAViK, J., KALENDA,P. & HOLUB, K. 1992. Statistical
This work was carried out as part of research project analysis of seismic events induced by the under-
No.105/93/2409, which was financially supported by ground mining. Acta Montana, Series A, No. 2
the Grant Agency of the Czech Republic. This (88), 133-144.
manuscript benefited from critical and thoughtful UTSU, T. 1965. A method for determining the value of
review by N. R. Goulty. The technical assistance of b in formula log N = a - bM showing the magni-
J. Rugajovfi in the preparation of the manuscript is tude-frequency relation for earthquakes. Geophy-
also appreciated. sical Bulletin, Hokkaido University, 13, 99-103.
 An analysis of mining induced seismicity and
its relationship to fault zones
ZDENl~K KAL,~B

Institute of Geonics, Academy of Sciences of the Czech Republic, Studentskd 1768,

Ostrava-Poruba, 70800, Czech Republic

Abstract: Intense induced seismicity has resulted from long-standing mining activity in the
Karvin/t part of the Ostrava-Karvin~ Coal District, Upper Silesian coal basin.
Interpretation of mining induced seismic events in combination with other knowledge
(geological, tectonic, geomechanical, technological) aids the understanding of failure
processes in the rock mass. Seismological observations over a three-year period were
analysed. Four sets of mining-induced seismic events have been tested to evaluate the
seismicity of important fault zones. It follows from the analysis that the seismic activity on
important fault zones occurs only as a consequence of mining activities. Accumulations of
mining induced seismic events occur on stress concentrators, which may be geological and/
or anthropogenic structures.

The geological and tectonic structure of the rock In places, where the strength of the rock mass is
mass of a deposit is an important factor that exceeded, failure occurs and energy is emitted in
influences the origin of seismic events induced by the form of seismic events.
mining activities (henceforth referred to as Information gained from seismic interpreta-
seismic events). This influence is present in the tion (e.g. time of seismic event, origin, location
Czech part of the Upper Silesian basin, where of foci, energy, dimensions of the focal area,
the Ostrava-Karvinfi Coal District (OKR) is mechanism of the focus) and relation to the
located (Fig. 1). The underground mining of geological and tectonic structure of the area,
black coal has taken place for more than 100 the geomechanical situation and existing mining
years and during this period, a complicated activities produce a complex pattern of mining-
network of worked-out and caved mine spaces induced seismic activity in the area. These data
has been created. As a result, a complex induced can be used to provide information on the
stress field, variable with time, has been formed. importance of individual structures, the actual

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plan showing the position of collieries in Ostrava-Karvinfi Coal District in the K[ovfik co-ordinates
F i g . 1. A (in
km) (Collieries: 1, Doubrava; 2, Lazy; 3, Dukla; 4, CSA; 5, Darkov; 6, Franti~ek; 7-9, kv6ten; 8, CSM).

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geologyand Technology,
Geological Society Special Publication No. 125, pp. 329-335.
330 Z. KALAB

mechanism of the failure process and, signifi- geomechanical point of view, an analysis of the
cantly, the relation between seismic events and intensity of tectonic dislocations has resulted in
current geological and mining conditions. Subse- the following relationships (Rakowski 1989):
quently, this leads to the possibility of specifying
the probability of rockburst occurrences. 9 rockburst areas are situated usually in places
The aim of this paper is to observe the little affected by intrablock fault tectonics
connection of seismic activity with important 9 in areas with sudden changes in the intensity
fault zones in the area most affected by induced of tectonic dislocations, a greater intensity of
seismicity, i.e. the Karvinfi part of the OKR. rockburst events can be expected
9 in areas with a smaller intensity of intrablock
tectonic dislocation, the existence of tectonic
Tectonic and geomechanical situation discontinuous concentrators of stress and
residual tension cannot be excluded
The Czech part of the Upper Silesian basin is
formed by Carboniferous sediments (a detailed
description of the geological structure is given in
Dopita & Kumpera 1993). The Karvinfi part of Seismicity and mining situation
the OKR has the character of a basin with An analysis of mining induced seismic events, in
principal fault systems trending both in N-S and relation to mining activities, has proved the
E-W directions. It is possible to model the region existence of two important groups. The first is
as a partial block structure consisting of beds of closely connected in space and time with the
medium-thick psephito-psammitic layers that advance of mine openings, whereas, in the second
have a typically subhorizontal orientation. The group a more or less random relationship exists
thickness of individual beds ranges from metres between seismic events and mining activities.
up to 10-20m. Laterally, the dimensions of These seismic events are induced at greater
partial geological blocks vary from hundreds to distances and are likely to be the effects of several
several thousands of metres. The boundaries of workings. Moreover, shifts in time between
the blocks are usually formed by fracture mining activities and the initiation of events can
dislocations, largely filled with plastified materi- also occur (Gibowicz & Kijko 1994; Rudajev
als. Intrablock tectonics is not very marked, but 1989). An example where the development of
it exists and can divide the layers within the block seismic activity in a given area is influenced by the
into smaller partial blocks. Areas of varying driving of mine workings is presented by
intensity of tectonic dislocation differ in mining- Kone6n~, (1994).
induced seismic activity (Rakowski 1989). An empirical relationship between the process
A geological analysis of important tectonic of massif failure in a limited area and the
structures in the Karvin/l part of the OKR has probability of the origin of anomalous rock-
been made. From a geomechanical point of bursts can be established. This is based on the
view, the analysis has given the following results: relation between the number of mining-induced
9 the thickness of faults (fault zones) ranges seismic events, the amounts of emitted seismic
from several metres to some tens of metres energy and the intensity of coal fracturing. The
9 throws vary from metres to several tens of relationship is not simple because, in addition to
metres the effects of mining operations, it is necessary
9 the majority of faults (especially those with to take into account 'natural' factors. The
greater thickness), contain a filling consisting behaviour of all the factors given below must
of plastified cataclastic materials be studied to understand the development of
9 faults are commonly, although not always, seismic activity (Kone~n2~ 1989):
wet
9 the primary stress field and geological struc-
The detailed evaluation of both tectonic struc- ture (factors unaffected by human activity)
ture and palaeostress conditions has proved the 9 the geomechanical structure of the massif
existence of dominant structuro-dynamic condi- (given by natural factors, but partly influ-
tions favouring rockbursts. Critical sites were enced by active interference)
identified in the massif (e.g. the most important 9 the secondary stress field and changes in it
fault zones, hanging corner structures, sections (impacts of mining activity)
with a small frequency of faults and others)
where rockbursts could occur given the exis- From the above, it follows that for mining
tence of disadvantageous, especially mechanical purposes, it is desirable to study the develop-
conditions (Kumpera et al. 1991). From a ment of induced seismicity under the geological
 AN ANALYSIS OF SEISMICITY 331

and geomechanical circumstances of the primary energy greater than that corresponding to the
stress field by monitoring the stress changes that charge is recorded, the blasting operation must
occur as a result of mining activities. have initiated failure of the massif in an area
where stress conditions were close to critical.
To monitor the seismic activity in the OKR,
Seismological monitoring three levels of seismic networks are used. Local
seismic networks of individual collieries repre-
Induced seismicity results from anthropogenic sent a basic level of monitoring. The second level
activities causing changes in the rock massif that is ensured by a regional network named Seismic
lead to its failure. Failure is accompanied by the Polygon of the Ostrava-Karvinfi Collieries. The
generation of seismic waves that can be mon- station Ostrava-Kr~isn6 Pole, which is a part of
itored by seismic stations. Events due to blasting both the state and world seismological net-
operations have a special signifcance. If the works, is also situated in the Ostrava region. The
intensity of an event corresponds to the size of development of seismological monitoring in the
the charge, the seismicity simply recording the O K R as well as its utilization in the fight against
blasting operation. However, if an event with an rockbursts is described by Kalfib et al. (1994).

4.0 41 4.2 4.,344 45 46 47 48 49 50 51 52 53 54. 55 56 57 58 59 60 61 62 63 64. 65 66 67 68 69 70 71 72 7,3 74 75

E E
F" F
G G
H H
I I
d J
K K
L Nzmi l, ml L
M llmmmm an M
N lan lml N
0 immBnui 0
P
Q
s liOi P
Q
R R
S S
T T
U U
V V
W W
X X
Y Y
Z Z
M ,AA
BB BB
CC CC
DD DD
lEE EE
FF FF
C-~ GG
HH HH
II II
JJ JJ
KK KK
LL It
MM MM
NN NN
4.0 4.1 4.2 43 4.4 4.5 4.6 4.7 4.8 49 50 51 52 53 54, 55 56 57 58 59 60 61 62 63 64, 65 66 67 68 69 70 71 72 73 74. 75

Fig. 2. Intensity of exploitation Ik in the central part of the Ostrava-Karvin~t Coal District in 1990 (in square
250 • 250 m network; lines in network are the most important fault zones).
332 Z. KALAB

Modern methods of interpreting digital seis- event. The correlation ratio was determined on
mic data also test for tectonic effects. Seismic the basis of a 100kg charge for all blasting
events recorded only in the focal area are operations. The bulletins 'Seismologickfi aktivita
represented by data from the experimental OKR' (Seismological Activity in the OKR)
seismic network of a modular system in the processed at the seismological centre in the
Lazy Colliery with the possibility of connecting CSA Colliery served as the basic information.
with up to eight surface or underground A tectonic schematic map of the Karvinfi part
stations. The network monitors a seismically of the OKR was used to create a visual analysis
active part of the mine, covering an area of of the seismicity associated with tectonic zones.
about 3 km 2 (Knejzlik et al. 1992). The map was processed in the DPB Paskov
The layout of the stations of the Seismic company (Mine Exploration and Safety) by
Polygon of the OKD corresponds with its plotting the distribution of tectonic elements at
position as a regional network. Seven surface a depth of 500m. This depth corresponds
stations surround the Ostrava-Karvinfi District. roughly to the supposed z-coordinates of the
The remaining three stations are located in foci of seismic events. With regard to the fact
underground workings. The network covers an that the tectonic structure of the OKR is very
area of 200km 2, using Lennartz Electronic complex, only the most important fault zones
GmbH equipment. were taken into account. Nevertheless, it is not
The Fren~tfit Seismic Polygon is an autono- possible to determine unambiguously, whether a
mous unit situated about 30 km southwest of the given seismic event originated or did not
Karvinfi part in an area of the Fren~t~it colliery originate on an existing tectonic plane. To
under projection. It contains five surface obtain unambiguous results, it would be neces-
stations that are telemetrically connected with sary to establish data sets, in which the focal
the central recording station (Knejzlik & depth is also known to test whether the
Zamazal 1992). dislocation plane contains the focus. This will
soon be possible using data recorded by seismic
networks which provide three-component digital
Data sets records of the wave patterns of seismic events.
For the purpose of assessing the extent of
To evaluate the seismicity of significant tectonic mine activities, synthetic maps of mining inten-
zones in the Karvinfi area, four sets of mining sity for the observed and previous periods were
induced seismic events have been identified: produced. The intensity of exploitation was
evaluated by means of the Ik index (Kone6n~,
9 all recorded mining induced seismic events
1989), which represents the thickness of the
9 intense rockbursts
seam that could be extracted provided that
9 mining shocks
exploitation is realized across the whole area
9 intense seismic events induced by blasting
under evaluation (in accordance with the mine
operations
network, a square 250 • 250 m network is used,
The sets cover seismic events that occurred from see Fig. 2). Worked-out areas are determined
1989 to 1991. from the mine maps within individual time
Altogether, the localizations of about 14000 intervals.
mining induced seismic events with an energy
E > 100J (according to the energy scale in the
OKD) were used in the first set, but due to Discussion of results and conclusions
limited data, the focal depths were not defined.
The second set contained rockbursts with an As a consequence of potential inaccuracies,
energy E > 105 J. There were 94 events within the (e.g. in the localization of faults, the determina-
three year period. The set of mining shocks tion of their dip and the focal depth of the
(weak surface shocks) comprises 183 records. seismic event) a non-quantitative method was
This set is spatially inhomogeneous because it is used to assess the seismic activity of significant
based upon weak seismic events that can be fault zones in the Karvinfi part of the OKR.
observed on the surface and reported by the A visual comparison of the horizontal position
public to the processing centre. The last set of the focus with the fault at a depth of 500 m
consists of seismic events induced by blasting was used as a basis. In contrast to research
operations when 'shooting a charge'. The energy in areas without mining-induced seismicity
of these seismic events was higher than that (Prochfizkovfi 1985) in this area, it is necessary
stated because of the correlation between the to consider induced stresses that are variable in
charge weight and the energy of the induced time. These arise as a result of mining activities.
 AN ANALYSIS OF SEISMICITY 333

Data from individual sets were, with half-year This is valid also for the set of intense
intervals, compared with the tectonic sketch rockbursts that are not connected directly
plan and the intensity of mining in the area with mining activities. If an important fault
under study (e.g. see Figs 3 & 4). The data can zone occurs in the vicinity of the face, seismic
be interpreted as follows: events do not originate preferentially on
it or in its surroundings. This result contra-
9 No seismic event of natural origin (e.g. tec- dicts the results of Spi~fik & Zimovfi (1988)
tonic earthquake) has been identified in the which suggested an increased seismicity
data under analysis. No mining-induced along some fault zones. However, the
seismic event has been recorded which was authors warned that actual mining activities
located within an area of a significant fault and the distribution of worked-out spaces
zone, where no mining activity had occurred. were not considered.
9 The induction of seismic events is wholly Significant concentrations of seismic events
dependent upon the space-time distribution are observed in areas, where mining opera-
of mine workings, especially of active faces. tions took place under extremely complicated

40 41 42 43 44 45 46 47 48 4.9 50 51 52 53 54 55 56 57 58 59 60 61 62 63 64 65 66 67 68 69 70 71 72 73 74- 75
E
F
G
H
I
J
K
L
M
N
0
P P
O Q
R R
S S
T T
U U
V V
W W
X X
Y Y
Z Z
AA M
BB BB
CC CC
DD DD
EE EE
FF FF
C,(; GG
HH HH
II II
Jd JJ
KK KK
LL LL
Mkl MM
NN NN
4.0 41 42 4.3 44. 4.5 4.6 47 48 49 50 51 52 53 54 55 56 57 58 59 60 61 62 63 64 65 66 67 68 69 70 71 72 73 74 75

Fig. 3. Number of mining-induced seismic events (data set No. 1) in central part of the Ostrava-Karvinfi Coal
District in 1990 (in square 250 • 250 m network).
334 Z. KALAB

40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 61 62 63 64 65 66 67 68 69 70 71 72 73 74 75
" /I ~ - , . . -. -"~'-,.[]/i . " " r
oF'E: -~/\~. \ ~--'"i
' , -- -"\ 'I '-'/Yk~ I"- "'\ ~ , t;F
H / "\. \ . ~ - - < W - - ":%:~ v ] H

d ~ \_~. ,

J "-.-~ : . . .

M " ~ / // // "k ~J( I\M

o / ::,\ i
p / --,),--~,II ~ /i )! k\ i~ P
Q / i\ $/ ) '1 7 2 2 1 k Ii I I Y,, 311 t o
R / \ ~ / ... 3 6 L3:-:.;L ) ./~Zc:!/ R
s / \ - ?i~'Y"~7"--% " ].'I " ~s

u / "X I ~:.... \ "_'>Lq- ' / u

v / \ / I i,:. ) / /:\~\ \v
w / \~ / Xts k r ~.q: i w

z- "7/... ~_....--" :/7~-.:~._ :~: ~ z

ee /11 / 3/ BB

DD \ l/ r I :i :\ : ~ :'/ / DD
EE 2 N / ff ' I I ii i// . . . . Ii ' I EE

oo i/ I~, ~ . .,:-"'-,. . . ' ~ i'~ oo

, :'-~ // "
(~ 1 "
\ ~ "
(---' li

KK ~ / \ I..~i..,.- ~ I KK
u.-~ ,-...__ / "------f : , .. J u.
: .. ;

NN [
-'-" --Z.~ ..._ [ ] " NN
40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 61 62 63 64 65 66 67 68 69 70 71 72 73 74 75

Fig. 4. Number of rockbursts (data set No. 2) in central part of the Ostrava-Karvinfi Coal District in 1990 (in
square 250 x 250 m network).

geological, geomechanical and technological blasting operation was undertaken (release

conditions. These concentrations are con- of stress in the roof). In only a very small
nected with the existence of important stress number of seismic events has a shift of foci
concentrators, on which seismic events are towards fault zones been demonstrated. It is
induced. often not possible to distinguish a seismic
9 The connection between mining shocks and manifestation of the blasting operation from
tectonics has been studied previously (Mtiller an induced seismic event.
1989; Veseki 1993). The results are not
Analysis of the data recorded within the three-
unambiguous, there is no demonstrable
year period from 1989 to 1991 by the stations of
significance in the concentration of foci of
mine network showed:
these shock. It is possible to produce similar
results as for previous studies. 9 No incidence of the generation of seismic
9 Seismic events induced by blasting opera- events on important fault zones or in their
tions in workings are usually localized in the close vicinities has been proved in areas
rocks overlying the working, in which the where no mining operations have occurred.
 AN ANALYSIS OF SEISMICITY 335

9 Significant sources of induced seismicity are 1994. Mining induced seismicity in the Czech part
generated in zones of stress concentration of Upper Silesian Coal Basin depending on
where the spatial distributions of both geolo- mining conditions. In: RAKOWS~I, Z. (ed.) Geo-
mechanics 93 Proceedings. Balkema, Rotterdam,
gical and anthropogenic structures is critical.
63-68.
9 The influence of the characteristics of the KUMPERA, O., GRYGAR, R., KALENDOV,~,J., ADAMU-
massif on the generation of mining-induced SOV~,,M. & VONDRAKOVA,J. 1991. The evaluation
seismic events, can be determined by inter- method of structure and tectonic setting and
preting the digitally recorded data, with palaeostress conditions in relation to rockbursts
particular emphasis on assessing the depth prognosis. MS Report, Technical University,
of the focus and parameters of the plane of Ostrava (in Czech).
dislocation, or other physical parameters MI2LLER, K. 1989. Location of mining shock in
of the focus (see e.g. Swanson 1992; Tepper Karvinh part of OKB. In: Seismology in engineer-
ing and mining practice. Proceedings, Technical
et al. 1992).
University, Ostrava, 33-36 (in Czech).
The author acknowledges financial support from the PROCHAZKOVA, D. 1985. Space-and-time pattern of
Grant Agency of Czech Republic (reg. No. 105/93/ seismicity. Proceedings of symposium, Geophysical
2904 and 105/95/0474) and from the Czech-American Institute of CAS, Prague, 46-53.
Scientific and Technical Program (reg. No. 930 65). RAKOWSKI, Z. 1989. The conception of a physical
model of rockburst prone areas in Ostrava-
Karvin~ Coal Basin. Proceedings of symposium,
References ECE of the United Nations, Ostrava, Czechoslo-
vakia, A21.
DOPITA, M. & KUMPERA, O. 1993. Geology of the RUDAJEV, V. 1989. Major causes of rockbursts and the
Ostrava-Karvin~ coalfield, Upper Silesian Basin, role of seismology in their research. Proceedings
Czech Republic, and its influence on mining. of symposium, ECE of the United Nations,
International Journal of Coal Geology, 23, 291-321. Ostrava, Czechoslovakia, A23.
GIBOWlCZ, S. J. & KIJKO, A. 1994. An Introduction to SWANSON, P. L. 1992. Mining-induced seismicity in
Mining Seismology. Academic, San Diego. faulted geologic structures: An analysis of seismi-
KAL,~B, Z., KNEJZL]K, J. & M~LLER, K. 1994. city-induced slip potential. PAGEOPH, 139,
Seismological monitoring in Ostrava area. No. 3/4, 657-676.
Exploration Geophysics, Remote Sensing and SPIC,~K, A. & ZIMOV,/k, R. 1988. Seismic activity in
Environment, 1, 26-33. Karvin6 part of OKB and its reasons. MS Report,
KNEJZLiK, J., GRUNTORAD,B. & ZAMAZAL,R. 1992. Geophysical Institute of CAS, Prague (in Czech).
Experimental local seismic network in the A. TEPER, L., IDZIAK,A., SAGAN,G. & ZUBEREK,W. M.
Z~tpotock~, Mine of the Ostrava-Karvin~ Coal 1992. New approach to the studies of the rela-
Field. Acta Montana, 84, 97-104. tions between tectonics and mining tremors
-- & ZAMAZAL, R. 1992. Local seismic network in occurrence on example of the Upper Silesian
southern part of the Ostrava-Karvin~ Coalfield. Coal Basin (Poland). Acta Montana, Ser. A, 88,
Acta Montana, 88, 211-220. 161-178.
KONE~N~, P. 1989. Mining-induced seismicity (rock VESEL,~, V. 1993. An elementary analysis of mining
bursts) in the Ostrava-Karvin6 Coal Basin, Czecho- shock. In: KALAB, Z. (ed.) Seismology and the
slovakia. Gerlands Beitr. Geophysik, Leipzig, 986, Environment. Proceedings, Institute of Geonics,
525-547. CAS, Ostrava, 146-152 (in Czech).
 Comparison of structures derived from mine workings and those
interpreted in seismic profiles: an example from the Ka~ice deposit,
Kladno Mine, Bohemia
STANISLAV OPLUSTIL, JIl~I PESEK & JIl~i SKOPF,C
Faculty of Science, Charles University, Albertov 6, 128 43 Prague 2, Czech Republic

Abstract: Five seismic profiles across the Ka6ice coal deposit were reinterpreted and
compared with observations in mine galleries. The comparison shows that approximately
80% of normal faults with displacement exceeding 5 m detected on the seismic profiles really
exist. In contrast, in only two cases have mine workings shown faults (vertical displacement
10-15m) that have not been identified by seismic measurements. Discrepancies may be
mostly explained by: (i) misinterpretation of the fault with slope of the presedimentary
palaeorelief accompanied by differential compaction; (ii) virgation of faults and
misinterpretation of a fault zone composed of several small faults individually below the
detection limit but whose aggregate displacement is detected, giving the appearance of a
single fault; (iii) faults which die away toward the overburden indicating synsedimentary
movements in the deposit.

Reflection seismic has become a common and Moreover, at the end of 1970s and the begining
useful method of exploration of coal-bearing of 1980s, reflection seismics was carried out in
deposits in the central Bohemia, especially in the the central and northern parts of the deposit.
coalfields of the Kladno Basin (Kadle6ik et al. Advanced exploitation allows us to compare
1979, 1985, 1986). However, almost none of these observations in the galleries with the results of
coalfields has been mined until now. Exploitation seismic interpretation.
of the Ka~ice deposit is the only exception which
enables comparison between seismically derived
tectonic interpretation and reality.
Stratigraphy of the Kladno Basin and
Kadice deposit
History of the deposit
The Kladno Basin with the Kladno Coalfield
For more than 150 years, thick coal seams of including the Ka6ice deposit in central Bohemia
the Radnice Member have been exploited in the is only a small part of a WSW-ESE elongated
Kladno coalfield located along the southern complex of Upper Carboniferous continental
margin of the Kladno Basin. Later, in the mid- and partly coal-bearing sediments, which extends
1950s the Ka6ice deposit was discovered NW of from western through central to eastern Bohemia
Kladno coalfield, beyond an area of postsedi- with a length exceeding 250kin (Fig. 1). In
mentary erosion of the coal seams (Fig. 1). western and central Bohemia, the Carboniferous
Exploratory drilling of the deposit during the sediments are divided into four lithostratigraphic
1960s (Salava 1960; Richter 1964, 1966, 1969) formations. From the bottom these are: Kladno,
allowed its opening in 1969 through a gallery T~,nec, Slan~, and Lin6 Fins based on alternation
from the Kladno Mine. Consequently, coal of red and grey sediments. Deposition began in
exploitation followed from 1975. The annual mid-Westphalian and, including several hiatuses,
coal production from the deposit has varied lasted at least to the end Carboniferous. The coal
between 400 and 450 x 103 tons during 1980s, reserves of the Kladno Basin are concentrated
however, in 1994 it was only 311 • 103 tons. mainly within the Radnice Member at the base of
From 1986 to 1992, refractory claystone was the Carboniferous infill. It contains up to five
mined, but its exploitation was abandoned due mineable coal seams grouped into the Radnice
to economic reasons. (with Lower and Upper Radnice seams) and
During the last 20 years of exploration and younger Lubnfi (with Lower, Middle and Upper
exploitation of the Ka6ice deposit a large Lubnfi seams) group of seams. Most of them
amount of new data has been collected, the have been mined in the study area. There are no
concentration of which is greater than for any other workable seams in overlying units.
other part of the Kladno Coalfield (results until In the area of the Ka~ice deposit only the
1980 are summarized in Spudil et al. 1980). Kladno and T~nec Fins are fully present, whilst

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 337-347.
338 S. OPLUSTIL E T AL.

~>i'ONIcE DEPRESSION

150km A
VE LVARY RIDGE

BILICHOV RIDGE RIDGE

(LADNO N
Y

~2 Y ls ,o ,,Skm
B
Fig. 1. Generalized map the Upper Carboniferous deposits in the Czech Republic (A) and location of the study
area within the southern part of the Kladno Basin (B) in Central Bohemia (after Klener 1982, modified). 1,
Kladno Basin; 2, other Carboniferous deposits in the Czech Republic; 3, coalfields; 4, outcrop of the Proterozoic
basement; 5, present distribution of the Radnice Member. Numbers represent the names of different coalfields
and deposits (1, Rynholec coalfield; 2, Ka6ice deposit; 3, Brand~sek d.; 4, T~ebusice d.; 5, Jan d.; 6, Minice d.;
7, Kokovice d.)

only the basal part of the Slan2~ Formation has with variable directions into the Ka6ice Deposit
been recognized. The preserved thickness of the itself. The slope of the elevations commonly
Upper Carboniferous deposits varies from 450 m reaches 10-20 ~ locally even more.
to 650 m depending on palaeotopography, ero- In the Ka6ice Depression the coal-bearing
sion and tectonics. These deposits are underlain Radnice Member is dominated by siltstones and
by Upper Proterozoic basement composed mudstones with four mineable coal seams
mainly of a monotonous complex of folded (Fig, 2). Near the base, mudstones commonly
shales and uncommon volcanic rocks and cherts. interfinger with breccia derived from weathered
Deep erosion of the basement created a sig- basement surrounding the depression. In the
nificant palaeotopography with differences in upper part of the Radnice Member sandstone
elevation between the paleohighs and paleo- bodies also occur, the number and thickness of
valleys of up to 150 m in the study area and its these increasing significantly to the south. The
close vicinity (Oplu~til-Vizdal 1995). The axes of thickness of coals decreases upward; while the
the main elevations and depressions are in a Upper Radnice and Lower Lubn~i coals com-
good agreement with structural elements (folia- monly exceeds 3m (max. 7m) the remaining
tion, fold axes, cherts and volcanic belts) of the coals (Middle and Upper Lubnfi) rarely reach
basement and both follow a predominantly 2m. The thickness of the Radnice Member is
WSW-ENE direction which is the trend of the only erosional and varies greatly from 0 to 185 m
Kladno Coalfield itself. Workable coal seams are (average thickness around 90 m) within the study
developed in palaeovalleys. The Ka6ice depres- area and its close proximity.
sion is the northern protrusion of larger Kladno The overlying unit, the N~,~any Member, was
depression. It is surrounded by two significant deposited after a hiatus and reaches an average
palaeohighs from which protrude minor ridges thickness of 350m with only slight variations.
 STRUCTURES IN MINEWORKINGS AND SEISMIC PROFILES 339

Lrl (...)

._I L.,..
. . . . . - . . .
c . . . . . . . . . . . . . . . . . . . . . . . . . . .
->, Fli:r uloy M, . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

O Moteslce
;.--3::...::.?-:: :.72: ~ j c-:-~-1---<-3"-T:--'T- 7 7::, -. -:-- :5:-~-,-,-
g~ M
k. c L,._ JetenicaM, ,
...
-_-_-_-.-_-_-_-_-_ _ - ~-
. . . . _.-.~.- _. -._.-._ .- _.-._.- _ - _ - _ - _ - . --------'--UPPER LUBNA CDAL

c-
CI
-- E~ 2-'-'2:-'_. . . . . . . . . . . . . . . . . . . . .
q_. -~ i, i

/
. . . . . . . . . . . . . . . . . . . . . 7 .- .- T - - .~ . ~ . - .
"-----"--. T" - - . - " , - -. - 7 . 7 - -. - . - 7 . , ."-~ ~ 2 ~ o ~ ; o ; ~
~ ~ _ -2-_--_--_--7.-_-----_--_-_--_--Z~-1-..... ~
,- +,
L
U

0..,
/
s

/
1.-.

".>.,
.I
..Q
.t.a
I.--
/'
i
(D / LOVER LUBN~ COAL
/
(~ . . .

(_.) c-
o N~'any '
--
M. /
UPPER RADNICE COAL
c ~ I '
e-
o
n + g t"

i> LOVEP I~ADNICE COAL

CL m o Rodnlce
tn
(3
M.

, , , . ...... N N , II 8
' {t'
x<r
>'',

Fig. 2. Stratigraphy of the Kladno Basin and lithology of the Radnice M e m b e r in the study area. 1, mudstones;
2, (arkosic) sandstone; 3, (arkosic) conglomerate; 4, breccia; 5, refractory claystone; 6, tuff, tuffite; 7, coal;
8, basement.

The fluviatile sediments of the N)~any Member predominantly grey coloured mudstones it is
are arranged into cycles, the thickness of which very similar to the underlying T~Tnec Fro. and
varies between 1 and 10m. The lower parts of N~7~any Member.
the cycles dominate with medium-to-coarse- Within the study area, the Carboniferous
grained sandstones occasionally with conglom- sediments are covered by Upper Cretaceous
erates. These cycles are grouped into six 40 to deposits, the thickness of which varies in relation-
60m thick mesocycles which exhibit fining- ship to the pre-Cretaceous relief and intensity of
upward trends with a thin coal seam in the post-Cretaceous denudation. Usually, the Cre-
highest cycle of each mesocycle (Spudil 1982). taceous deposits are less than a few tens of meters
The following unit, the T2)nec Formation, thick. They are composed of continental fluvio-
shows a very similar lithology and sedimentary lacustrine sediments (conglomerates, sandstones
architecture to the previous unit, making it and mudstones, occasionally with a thin seam of
rather difficult to distinguish. It is composed dirty coal) at the base grading upward into
of three mesocycles with predominantly red marine sandstones and siltstone. They are over-
coloured sediments without coal seams. The lain by marl.
T)nec Formation passes gradually into the
Slan) Formation.
The Slan~, Formation is preserved only in the Coalfield
northern part of the Ka6ice Deposit with an The concentration of data in the area of the
erosional thickness of 30-40 m. Apart from the Ka~ice deposit is greater than that of the other
340 S. OPLUSTIL E T AL.

coalfields in the Kladno Basin. Since its discovery affecting the signal, on the thickness and
in the 1950s there have been more than 50 deep lithological stability of separate layers, etc.
boreholes drilled from the surface to the base- Since these factors are more or less variable,
ment and over 500 mining boreholes, penetrating the extent of such reflections is usually limited
usually only a part of coal-bearing succession of and the whole wave field can be characterized as
the Radnice Member. In addition, there are rather irregular.
47 kilometres of galleries, which have been the The amplitude of a reflected wave depends on
most useful for the construction of the tectonic the difference in physical properties on both sides
map of the deposit. An independently created of a given interface. In coal-bearing sedimentary
tectonic map has been derived from seismics. All basins, coal seams appear as layers of an
the galleries and mining boreholes are located in anomalous physical behaviour because of their
the approximatly 100 m thick basal coal-bearing low values of density and seismic velocity, which
complex. The remaining 350-500m of over- affects the reflection coefficient positively. There-
burden is known only from deep boreholes. fore, a group of beds containing coal seams is
usually characterized by strong reflections that
make it possible to determine fault positions
Reflection seismics where reflection horizons have been displaced.
This shift can vary from several hundred seconds
The commonly used borehole spacing is insuffi- to a few milliseconds and may not be observed at
cient to determine the fault tectonics of the all if the throw is too small.
Kladno basin. The CMP (common-midpoint) Seismic measurements in the Kladno Basin
method of reflection seismics can be used to aid were carried out in 1979 and 1983 by Geofyzika
the fault analysis. The important advantage of Brno. The Vibroseis measurements with 12-fold
the CMP method is its ability to detect separate coverage in the neighbourhood of Ka~ice village
horizonts even at a depth of several kilometres. were processed by using standard procedures
The results of the CMP method are commonly including wave migration. Strong reflections in
presented either as time or depth sections, where the coal-bearing basal Radnice Member have
continuous reflecting horizons are often clearly allowed the detection of faults which can be
visible. The irregularities that exist in the course compared with the results of later geological
of these horizons can be interpreted as evidence mapping.
of faults. Within the overlying sediments, the fault
The rocks filling a continental sedimentary structures affect the wave field less evidently,
basin may be developed as a cyclic sedimenta- causing local and disconnected shifts of rather
tary sequence consisting of many sandy and clay weak reflections.
layers. The lithological interfaces between neigh- As an example of traceable faults causing time
bouring sedimentary layers create reflecting shifts in the coal-bearing Radnice Member, the
boundaries for seismic waves generated at the part of seismic line 69/83 is presented in Fig. 3a.
Earths surface. The parameter describing the A number of normal faults with vertical throws
reflectivity of a medium is called the reflection of several tens of metres is obvious in the middle
coefficient, which can be defined as the ampli- part of the seismic depth section. In Fig. 3b, a
tude ratio of the incident and reflected waves. In part of seismic line 70/83 is shown, where the
practice the reflection coefficient is expressed as a sedimentary beds are only a little faulted by few
simple function of the densities and longitudinal minor normal faults. The time shifts are
wave velocities in the overlying and underlying negligible, but correspond to faults located in
media. the coal mine adits. On both figures, the different
In the case of a cyclic sequence, the time wave field can be observed for overlying
differences between separate reflections are so Carboniferous sediments and underlying shales
small that many of these reflections arrive within of Proterozoic age, while within the Carbonifer-
the time interval corresponding to the wavelet of ous beds the part containing the coal seams is
an individual reflection. Under such conditions, quite different from the overlying cyclic sedi-
instead of separated true reflections, rather ments without coal layers.
random interference patterns of numerous
reflections coming from the individual bound-
aries may be expected. The amplitudes of these Structure derived from mine
reflections are usually small, as are those from
the summary reflections. The total amplitude of The deposit is affected by post-sedimentary
the reflections depends not only on the reflection normal faults with a general N W - S E strike.
coefficient, but also on the number of reflections Faults with other strike directions are rare.
Depth
69/83
(m)

leg

ee@

1oo

2ee

3ee

4ee

.~88

Depth
(m) 70183

lee

eee

lee

2oe

3ee

4ee

500

Fig. 3. Part of the depth seismic profiles with interpreted faults. 3A, depth seismic profile 69/83; 3B, depth seismic
profile 70/83. For location see Fig. 6.
342 S. OPLUSTIL ET AL.

~D

0 0
~.~

\
\
'\
,,..I"
"x
,,,.,
~.~
/ ~m

/ .~

9..
f.
e~

o
7

~ I"~ 84 ~"

\
E~-
r- ~.1
~N ~ .~ .~.

~ ~ .~.

e6P!~l Aoqo!lJe
o~ \ \~ /i--.- ~.~
,~ "~ ~
.~ ~ z ~ \ \\
 STRUCTURES IN MINEWORKINGS AND SEISMIC PROFILES 343

Moreover, they have only small vertical dis- into several smaller faults, the downthrow of
placement with a maximum of a few metres. The which varies between 10 and 20m. They are
majority of these faults dip SW. Reverse faults traceable over a distance of 1 to 2 km in seismic
with throws exceeding several tens of centi- profiles and exceptionally in galleries.
metres have not been observed in the galleries. Another significant fault zone composed of
In the early 1960s, palaeo-ridges with a NW-SE two major antithetic faults limits the western
direction were misinterpreted in seismic profiles part of the Ka~ice Deposit. In the SW it creates
as normal faults, because until that time only a 70 m wide graben at the level of the Upper
those ridges running NE-SW had been known. Radnice Seam (about 50 m above the Carboni-
The throw of the normal faults varies greatly ferous basement). It has a throw of 6-10m.
from several centimentres to over a hundred Northward its vertical displacement increases up
metres. Approximately 80% of all documented to 80 m (eastern fault, cross cut 243) in NW edge
faults have throws less than 2m and only 10% of the deposit. A vertical displacement of about
exceed 5 m; thus they are around or above the 60 m on the western fault is estimated from the
detection limit of reflection seismics. discrepancy in basement altitude between two
Larger faults with more than 40m down- boreholes located in the upthrown and down-
throw occur at a spacing of about 1.5km in thrown blocks.
the Kladno Coalfield (Fig. 4). They dip at A similar graben is known from the south-
approximately 75 ~ (Spudil 1982) and extend to western margin of the deposit, where it con-
the Proterozoic basement but are truncated tinues from the Kladno Coalfield. In the Ka6ice
by the pre-Cretaceous surface. Smaller faults Deposit, however, only its eastern normal fault
(10-20m) are traceable for a distance of several was proved in the gallery.
hundred metres up to one kilometre and their
dip is usually 55-75 ~. They also continue into
basement but it is uncertain whether they reach
the top of Carboniferous sequence. They are Comparison of structures observed in the
typically sinuous. mine and those interpreted in seismic profiles
The faults often virgate. They commonly occur
as systems of antithetic faults, creating grabens Five reinterpreted seismic profiles are com-
several tens up to one hundred metres wide (near pared with the structural map derived from
the base of the Carboniferous) running across the mine. These profiles run mainly from WSW to
coalfield (Fig. 4). Small faults (throw less than ENE being more or less perpendicular to
10 m) usually do not disturb the whole section of prevailing direction of the faults. The location
the Radnice Member and diminish as they of all seismic fault indications in Fig. 6 if not
approach basement. stated, corresponds with the base of the
The most distinct reflection corresponds with Carboniferous.
the boundary between subhorizontally layered Seismic profile 1C/78 runs from SW to NE
undeformed Upper Carboniferous sediments of through the study area (Fig. 6). Two normal
various lithologies and the folded lithologically faults have been inferred in the area of mining
monotonous complex composed mainly of activity (vertical movement 20 and 5 m) and, just
Proterozoic shales. behind the eastern end of the galleries, a 200 m
The general dip of the basement surface is wide tectonic zone has been located. Within this
5-8 ~ to NNE. Therefore the shallowest occur- zone two principal normal faults have been
rence of this boundary is in SW part of the deposit recognized. A larger one (80 m) on its western
(borehole K6 11, -38.8m); whilst the average margin and a smaller one in its eastern margin.
altitude of the surface reaches 430 m. To the NE Both dip to the SW. These indications are in good
it falls to a depth below -280 m (borehole So 8, agreement both in size and dip with a significant
-287.7m surface 400m). In detail (Fig. 5), normal fault proved in a cross-cut at the SE
however, the general dip is superimposed on margin of the deposit as a non-branched fault.
the slopes angles of the pre-Carboniferous Seismic measurement supports the idea of their
ridges. Therefore the final angle may exceed 15~. virgation and gradual diminution to the NNW.
The study area is affected by three significant The remaining two indications correspond
normal fault systems. The largest one runs along only partly to observations in the mine. While
the eastern margin of the deposit where it the smaller one (5m) has been known from
continues from the Kladno Coalfield to the several galleries north of the profile, the larger
south. The vertical displacement reaches 100 m one (c. 20m) dipping NE probably has no
in the SE corner of the Ka6ice Deposit. Further equivalent in the mine. However, the distance
north the fault gradually diminishes and virgates between the detection site and the closest gallery
344 S. O P L U S T I L E T AL.

-12

80'

\ \
-60 ! \
/ Le3\

N
\\\\\ \
\ \

I/I/

~oX~ LADN0
O

\ ~" #~l~ JILt el~~~~~~ o ~oo

N ~u3~
' "7

Fig. 5. Tectonic sketch of the study area and contours of the surface of the Late Proterozoic basement; 1,
contours of the surface of the Proterozoic; 2, significant normal faults observed in mine; 3, borehole.
 S T R U C T U R E S IN M I N E W O R K I N G S A N D SEISMIC PROFILES 345

Le| 6
t
I
t
t
I
I
| \
t, /8: \
, z~ z~ , Le 3
\ 70183
\
\ 83
\

\
\ 1183

\\~0
' t
N

| \
, []
%3
\

\
\
:/78
\

/ 9 ~
L/;g V~ n 1 8 3
2,2
soz t
|
L
i 0 ~m
l a ,.J

\ ~,5 >.3
\
32

\
\
\ K~12
\
\
\
\
\
\
. . . .

Le 3 l
4 , |

Fig. 6. Comparison of structures derived from mine with those interpreted in seismic profiles. 1, normal faults
observed in gallery and its expected continuation; 2, indication of normal faults in depth seismic profiles the
existence of which have been proved (simple frame) and which have not been proved (double frame) in mine;
3, depth seismic profiles, thick part corresponds with location of profiles depicted in Fig. 3; 4, borehole.
346 S. OPLUSTIL ET AL.

in the direction of the fault is 500 m and it has The second indication without a proved
been observed that a 5m fault may terminate equivalent is an east-dipping normal fault
over a distance of 100m. Nevertheless, larger with an estimated displacement of c. 5-10m
faults are usually more persistent. Detection of (Fig. 6). It is situated in a zone with an increased
the fault in seismic profile through the whole number of small normal faults whose aggregate
Carboniferous sequence excludes misinterpreta- displacement may resemble a single fault in
tion due to the vicinity of a pre-sedimentary seismic profile.
ridge or sudden facies changes within the Seismic profile 70/83 crosses the northern part
Radnice Member. of the deposit from WSW to ENE. Five
Seismic profile 69/83 crosses the middle part indications of normal faults have been recog-
of the deposit in a WSW-ENE direction. The nized within the seismic profile. Their throw
two westernmost indications lie outside the area varies from 5 to 25 m. Four of them are situated
proved by the galleries. They are interpreted as in the mining area and have been observed in
antithetic normal faults with vertical displace- galleries. The fifth indication is located behind
ment of about 20-30 m. They match well with the eastern margin of the galleries in the
the hypothetical continuation of the graben proximity of borehole Le 3. It is interpreted as
proved in the mine l k m to SE. Its eastern an east-dipping normal fault with estimated
limit, which is well known from several galleries, throw of 25m. Probably on the same fault,
has been detected 240 m further east. gallery 1008 terminated at the NE margin of
250 m further east on the profile a large fault the deposit.
(up to 100 m at the base of the Radnice Member, The second indication from the east has been
c. 30-50 m about 90 m higher) dipping eastward detected only at the base of the Carboniferous
has been detected. This normal fault has no (throw c. 10 m); it seems to be absent higher but
equivalent proved in the surrounding galleries is indicated again around the boundary of
(distance 100m). It is believed, that this dis- the Kladno and the T~nec Fms approximately
crepancy is induced by close proximity of a 400 m higher.
pre-sedimentary ridge protruding into the Seismic profile 71/83 runs NNW-SSE along
deposit from the west. The inclination of its the eastern margin of the deposit, just behind
slope probably exceeds 20 ~ (locally 30 ~ or more) the eastern end of the galleries. It is nearly
as it results from palaeo-relief reconstruction. parallel with the main faults of the study area.
Moreover, misinterpretation could be affected Therefore all of the indications belong to the
also by rapid facies and thickness changes main fault (fault zone) of the Kladno Mine.
within the Radnice Member near the ridge They dip either to the W or to the E due to
and also by compaction. It is supported by a undulations of a fault with a low angle of dip,
decreasing value of the throw to the top of the 30-40 ~. Their throw decreases gradually north-
Radnice Member. ward from 20 to 10m.
There are seven other indications with sizes
varying from 5 to about 15(20)m. Only two of
them (throw 5-10m) remain unproven in the Conclusion
mine. They probably correspond to a narrow
fault zone composed of small normal faults Comparison of structures interpreted in seismic
under the detection limit, the aggregate throw of profiles with those observed in mines show good
which could affect the seismic reflections. agreement. Approximatly 75% of seismic indi-
Seismic profile 70A/83 runs SW-NE c. 300- cations correspond with the observations in
500m north of profile 69/83. There are seven mine galleries in both dip and throw. The
indications of normal faults with vertical dis- seismic data have indicated nearly all of the
placements between 5 and 15 m. Only two of observed normal faults above the detection
them probably do not correspond to the fault limit, which in the central and western Bohe-
system proved in the mine. The westernmost mian Carboniferous is between 5 and 10m. The
indication dips westward with an estimated number of normal fault indications in seismic
throw of about 10(15)m. Its parameters are l:rofiles slightly exceeds the number of observed
comparable with the normal faults observed in faults. Most of them are around the detection
the mine, but, c. 80-100 m eastward at the level limit. However, in one case a large fault with a
of the Lower Lubnfi Coal, i.e. 50m above the throw of several tens of metres has been
basement. It is believed that this discrepancy interpreted with no equivalent in the mine. The
could be due to different stratigraphic levels. possible explanations for most of the discrepan-
Otherwise the faults proved in the mine lack any cies between seismic data and observations in
indication on the seismic profile. mine are as follows:
 STRUCTURES IN MINEWORKINGS AND SEISMIC PROFILES 347

9 misinterpretation of the slope of a presedi- References

mentary ridge, which could exceed 150m
elevation accompanied by sudden facies KADLE~iK, J., SKAROV,~, M. & JIHLAVEC, F. 1979.
Geofyzik6lnY - geologick6 zhodnoceni reflexnYseis-
change. The influence of presedimentary
mickfwh pracl S R B technologii VIBROSEIS na
palaeotopography and different compaction ~kolu Peruc-Slapanice. Written final report.
could persist up to the level of the T~nec Fm. Archives Geofond, Brno.
(Spudil et aL 1980) -- et aL 1985. Seismickf: prdzkum na lo~isku Slanj~ v r.
9 several smaller faults under the detection 1983-1985. Written final report. Archives Geo-
limit whose aggregate throw is interpreted as fond, Brno.
a single fault. et al. 1986. Z6vJre(nd zprdva o reflexnJ-
seismick6m prdzkumu SRB v oblasti Peruc-
Kokovice v r. 1983. Written final report. Archives
The apparent discontinuous character of some Geofond, Brno.
faults in seismic sections can be induced by the OPLUSTIL, S. & VIZDAL, P. 1995. Pre-sedimentary
coincidence of the throw of the normal faults palaeo-relief and compaction: controls on peat
with the thickness of the cycles. The result- deposition and clastic sedimentation in the
ing reflections appear to be uninterrupted. Radnice Member, Kladno Basin, Bohemia. In:
It could be a common phenomenon in the WHATELEY, M. K. G. & SPEARS, D. A. (eds),
N ~ a n y Member and the T2?nec Formation European Coal Geology. Geological Society,
London, Special Publication, 82, 267-283.
where the average cycle thickness varies between RICHTER, V. 1964. Kadice. Zdvdrednd zprdva pJredb~n6
7 and 10m. etapy prdzkumu. Written final report. Archives
In one case a normal fault dying out towards Geofond, Praha.
overlying beds indicates an occurrence of - - 1 9 6 6 . Dopln~k zdv#rednd zprdvy Kadice. Written
synsedimentary movements in the deposit. final report. Archives Geofond, Praha.
Despite the above mentioned discrepancies, 1969. Dopln~k zdvgredn~ zprdvy Ka~ice sever.
reflection seismics has been proved to be a Written final report. Archives Geofond, Praha.
useful method for exploration of new coalfields SALAVA,J. 1960. Z6vYre?n6 zprdva Ka?ice. Vyhleddvaci
in the Upper Carboniferous coal basins of etapa. Written final report. Archives Geofond,
Praha.
western and central Bohemia. It indicates that
SPUDIL, J. 1982. Strukturn6 geologickfi charakteristika
a proper density of seismic profiles allows the lo2iska Ka6ice. In: HAVLENA,,V.,~ PESEK,J. (eds)
construction of a reliable structural plans Sbornik IV, uhelng geologickd konference pFidovY-
where even faults with small vertical displace- deck~ fakulty, Praha, 133-142.
ments can be indicated by the geophysical et al. 1980. Z6v~re?n6 zpr6va ~kolu Ka{ice.
method. Written final report. Archives Geofond, Praha.
 Improvements in direct coal liquefaction using
beneficiated coal fractions
J. B A R R A Z A , M. C L O K E & A. B E L G H A Z I

Coal Technology Research Group, Chemical Engineering Department, University o f

Nottingham, Nottingham NG7 2RD, UK.

Abstract: Beneficiated coal fractions from Point of Ayr coal (North Wales) were liquefied in
order to determine their effect on conversion, product and metal distribution in coal extract
solutions. The coal fractions were obtained in a dense medium cyclone separation unit, using
aqueous solutions of Ca(NO3)2, as medium, of relative density 1.26. The original coal and
the coal fractions were liquefied in an autoclave with hydrogenated anthracene oil (HAO) as
solvent. Liquefaction results show an improvement in conversion for the overflow fractions
over the feed coal, together with a shift in the net product distribution toward higher oils
content and lower asphaltenes and preasphaltenes material in the liquid products. A marked
decrease in the proportion of A1, Mg, Mn and Si was found in the extracts using overflow
coal. However, Ti and Ca, which are deactivating elements of the hydrocracking catalyst
used to upgrade the coal liquids, increased their proportion.

During the last decade, work has been carried before the hydrocracking process. Cloke (1986),
out in order to separate and concentrate reported that an increase in the digestion
macerals for use in liquefaction processes pressure produced a significant reduction in the
(Dyrack & Horwitz 1982; Cronauer & Swanson extract ash levels. Also, the addition of toluene
1991). Investigators seem to agree that the coal before the filtration process, precipitates heavy
characteristics, particularly petrographic and organics producing extracts of low concentra-
mineral compositions are important parameters tion in mineral matter (Cloke et al. 1993).
in the coal liquefaction process, affecting overall However, very little work has been reported in
conversions, product and metal distribution in order to attempt to decrease the metal content in
the coal liquids. It has been established (King coal extracts using beneficiated coal fractions,
et al. 1984; Steller 1987) under a wide range of which are simply clean coal fractions with high
liquefaction conditions that the more reactive concentration of organic matter and low con-
maceral is liptinite followed, in decreasing order, centration of mineral matter.
by vitrinite and inertinite. Also, some studies The purpose of this study was to ascertain the
(Keogh & Poe 1987; Oner et al. 1994) have effect of liquefying beneficiated coal fractions,
shown that the presence of mineral matter in obtained by a dense medium cyclone unit, on
coal has a catalytic effect towards oils produc- conversion, product distribution and element
tion in liquefaction carried out in the presence of content in the extract solutions.
hydrogen and at conditions of high severity.
One of the liquefaction techniques which
could process coals of a wide range of maceral
Experimental
and mineral compositions is the British Coal
two-stage coal liquefaction. In the first stage, the Materials
coal is digested in a hydrogen-donating solvent
in the absence of hydrogen, at a low pressure A bituminous coal from Point of Ayr (North
(20-30 barg), and the resulting mixture is filtered Wales) was used in the study. Coal samples, run-
to produce a low-ash extract solution. In the of-mine and uncrushed, were supplied by British
second stage the extract solution is catalytically Coal. The dense medium used for the separation
hydrocracked in the presence of hydrogen to up- was an aqueous solution of Calcium Nitrate
grade the products. Tetrahydrate, obtained from Berk Ltd, UK.
Catalytic deactivation, during the hydrocrack- Advantages of this medium include that: it can
ing stage was found (Robatt & Finseth 1984; produce solutions of a wide range of densities; it
Kovach et al. 1978) due to the deposition of has low toxicity; and it is moderately inexpensive
metals such as titanium, calcium and magne- (Rhodes et al. 1993). The solvent used for the
sium. Because of this, attempts have been made liquefaction was a process-derived Hydroge-
to reduce these undesired elements in the extract nated Anthracene Oil (HAO), supplied by the

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 349-356.
350 J. BARRAZA ET AL.

British Coal Liquefaction Project. Standards overflow and the under flow fractions. The
and controls used to determine the metal product of the digestion was filtered to produce
element concentration were made from B.D.H. a filter cake and a coal extract solution. Details of
'Spectrosol' solutions. the liquefaction procedure has been previously
reported in the work of Cloke et al. (1987).

Procedures
The fresh coal was crushed, wet screened, filtered Analysis
and air-dried at room temperature to obtain coal
samples of particle size -250 + 63 #m. Coal Analysis for moisture and ash were carried out
samples were processed in a dense medium using the Standard BS1016 methods, while
cyclone unit, which is a closed circuit sump- maceral analysis was performed by the proce-
pump-cyclone. A diagram of the process is dure described elsewhere (Cloke et al. 1994). The
shown in Fig. 1. Water and Calcium Nitrate coal extract solution was analyzed for hexane,
(powder) were added to the feed sump and the toluene and tetrahydrofuran (THF) insoluble, in
density determined and adjusted. A relative order to determine the product distribution. In
density of 1.26 was used in the experiment, the present study, the product distribution is
which was obtained by increasing the medium defined as: oils, (100-hexane insolubles); asphal-
concentration or diluting it with tap water. The tenes, (hexane insolubles- toluene insolubles);
coal was added to the media, producing a slurry, preasphaltenes, (toluene insolubles - THF inso-
which was agitated with a stirrer driven by air. lubles) and heavy organics, (THF insolubles).
The slurry was pumped (2 barg) to the cyclone The coal conversion (on a dry mineral matter
and samples of overflow and underflow were free, dmmf, basis) is defined in terms of coal ash,
collected. The recovered samples were filtered filter cake ash and quinoline insoluble. The
and air-dried in the laboratory at room tempera- extract solution and filter cake were analyzed for
ture ready to liquefy. ash content at a temperature of 815~ in
Liquefaction runs were made in a 2 litre platinum crucibles. Nine elements (A1, Ca, Fe,
autoclave with HAO as solvent in a ratio K Mg, Mn, Na, Si and Ti) concentrations were
HAO/Coal: 2/1, w/w. Approximately 350g of determined in the original coal, overflow, under-
coal (as received) was fed to the autoclave. The flow, coal extract liquid and HAO, using a
liquefaction was carried out for 1 hour and a Perkin-Elmer model 2380 Atomic Absorption
temperature of 420~ Digestion pressures of Spectrophotometer. The metal concentrations
10barg and 40barg were used for the original were determined on the basis of the work of
coal, while a pressure of 40 barg was used for the Hamilton (1986).

Overflow
Gaugepressure T---~
(~ d---~~ ] - - - Cycloneunit

Air IJ Underflow I /
Coal+ medium i~
! Stirrer Cleaj, |
'\,,, // ReceptorMedium
\, /' Tank

SumpTank J ~///
Recirculation
Feedp u ~ pump
9
Fig. 1. Diagram of the dense medium cyclone process.
 DIRECT COAL LIQUEFACTION 351

Results and discussion a positive effect to concentrate the organic

matter and to decrease the mineral matter in
Dense medium cyclone separation the overflow fraction. The higher concentration
of liptinite in the overflow fraction would be of
Mass yields, ash, macerals and element analysis benefit to the liquefaction process, while the
of the original coal and coal fractions obtained higher concentration of non-reactive macerals in
in the separation are shown in Table 1. Results the underflow would be detrimental.
show that the overflow fraction gives a lower Results of concentration of the elements in
vitrinite concentration than the original coal, ashes of coal samples show that in general, the
however, it has the lowest ash content and the elements with the highest concentration are Si,
highest concentration of liptinite. By contrast, Fe, A1, Ca and K. In order to analyze changes in
the underflow fraction shows the lowest vitrinite the concentration of the elements in the overflow
and the highest inertinite content. Clearly, the fractions relative to the original coal fed to the
findings indicate that the cyclone separation had cyclone, the concentrations are expressed in
terms of proportions. Figure 2 shows the
proportion values. In the overflow, it was
Table 1. Ash, maceral and major element analysis of found that Ca has the highest increase followed
coal samples
by Na and Ti, while Fe and Mg show the same
Coal samples as received proportions, and the rest of the elements show a
decrease. The above results suggest that Ca, Na
Original Overflow Underflow and Ti have a tendency to be associated with the
organic matter, and A1, Si, K and Mn with the
Relative Density 1.26 1.26 mineral matter. In agreement with our results, a
Yield mass (% w/w) 43.0 57.0 previous study (Barraza et al. 1994) has shown
Ash (%, db) 14.5 1.2 24.0
that Ca shows organic affinity using float-sink
Maceral analysis, separations. The above changes in the concen-
mmf (% v/v) tration proportion suggest that some elements
Vitrinite 80.9 77.0 73.6 have been removed more than others. In order
Liptinite 10.1 15.7 7.7 to examine this trend, the results are evaluated
Inertinite 9.0 7.3 18.7 in terms of the masses of the elements present in
Element analysis in the original coal, overflow and underflow.
ash (% w/w) Results of the elemental masses obtained in
A1 9.31 7.85 9.07 Table 2 show that the biggest decrease of all the
Ca 2.94 8.40 3.10 elements occurs in the overflow fractions, how-
Fe 8.70 9.00 9.10 ever some elements show greater reductions than
Mg 2.46 1.22 2.61 others. In order to compare the removal of the
Mn 1.69 1.65 1.89 elements, the masses were transformed into
K 0.13 0.02 0.16
proportions, relative to the original coal feed.
Na 0.34 0.85 0.23
Si 30.16 18.74 29.38 Figure 3 gives the mass proportion of elements
Ti 0.69 1.35 0.67 for the overflow coal fraction. Ca, Na and Ti
have the highest proportion, which in terms of

3.00 1

2.50 -'

2.00

1.50

1.00

0.50

0.00 -[ 1- r ,
AI Ca Fe K Mg Mn Na Si Ti
Element
Fig. 2. Concentration proportion of elements is ashes of overflow relative to original coal.
352 J. BARRAZA E T AL.

Table 2. Global and major element mass in original feed and the coal fractions. The overflow fraction
cyclone, overflow and underflow coal fractions produced the highest conversion, while the
underflow fraction gave the lowest conversion.
Coal samples
The highest conversion from the overflow
Original Overflow Underflow fraction would be associated with its high
concentration of reactive macerals (liptinite+
Global mass (g) vitrinite) as well as to its low mineral matter
Mass (g) 232.56 100.00 132.56 content, and the lowest conversion in underflow
Ash (g) 33.72 1.20 31.81 may be due to the high inertinite level. These
results are consistent with those reported for
Element mass (g)
Element Parkash et al. 1985; Joseph et al. 1991.
AI 3.14 0.09 2.89 Performing the digestion at higher pressure
Ca 0.99 0.10 0.96 appears to produce a slight increase in conver-
Fe 2.93 0.11 2.39 sion in the original coal. Higher content of light
K 0.83 0.01 0.73 compounds, which were not released from
Mg 0.57 0.02 0.55 the autoclave, may explain this increase in
Mn 0.04 0.00 0.04 conversion.
Na 0.11 0.01 0.09 Despite the high conversion values obtained
Si 10.17 0.22 9.47
from the overflow fraction, it gave lower oils
Ti 0.23 0.02 0.20
content and higher heavy organics material in
Basis: 100.00g of overflow as received. the coal extract liquid compared to the original
coal and the underflow fraction. The digestion
pressure appears to affect the oils level in the
removal means that they were partially removed, original coal. Oils concentrations are higher
while A1, K Mn and Si show a significant degree at 10barg than 40barg, however the latter
of removal. Again, the notable proportion of Ca pressure, appears to reduce the concentration
and Ti in the overflow is observed. These of asphaltenes and preasphaltenes in the product
variations in the mass of the elements suggest from the overflow fraction. Low heavy organics
that they may show different behaviour during content in the underflow compared with the
liquefaction. overflow fraction also was achieved.
The product distribution obtained above
includes the oils from the HAO and the oils
Liquefaction o f original coal and produced from coal. HAO represents a large
coal fractions amount of the oils in the final product and it
would have affected the distribution obtained.
Results of conversion and product distribution Therefore, an analysis is carried out on the basis
in the coal extract liquids are shown in Fig. 4. of products formed from the coal alone. In order
Note that the oils figure includes the original to evaluate the net product distribution, a mass
HAO solvent. Differences were observed in balance is performed taking as basis 100kg of
liquefaction conversion from the original coal coal, which was separated into an overflow

0.12 - -

0.10

~- 0.08

0.06

0.04

0.02

0.00 I I i [ ] t , r--1 I 1[
A1 Ca Fe K Mg Mn Na Si Ti
Element

Fig. 3. Mass proportion of elements of overflow fraction relative to original coal.

 DIRECT COAL LIQUEFACTION 353

100
90

80 u

70

60
50
m
! ! ji DciOn.ois
...
I nll Asphaltens
40
30 ~' L mHeavy Organics

20

10

0o
Feed lO
N
0 Feed-dO

Fig. 4. Conversion and product distribution.

Feed to autoclave
i
OF-I 26 40 UF-I26-40

fraction and then liquefied in the autoclave. For the lowest oils percentage value. These results
this mass balance, it was assumed that the show that the overflow fraction has a beneficial
amount of gas produced is 2% of the coal effect towards production of oils.
converted and all the HAO during the liquefac- With regard to the element distribution
tion finish as oils. Results of the net product during the digestion process, results of the
distribution are presented in Fig. 5. These concentration of the elements and ash content
findings show that, in general, the overflow of the coal extracts are shown in Table 3. The
fraction produced the highest net percentage of concentration of the element and ash of the
oils, with small reductions in the asphaltenes and HAO are also reported in the same table. These
preasphalteues. However, the heavy organics findings show that for digestion at higher
content is the highest. The underflow produced pressure, a reduction in the ash content for the

50.0

45.0
r'loils
40.0 mAsphaltenes
mPreasphaltenes
mHeavy Organ es
35.0

,5 30.0

g~ 25.0
1. Original coal, 10 bar
2. Original coal, 40 bar
~' 20.0 3. Overflow, 40 bar
2 4. Underflow, 40 bar
15.0

10.0

5.0

0.0
! 2 3

Feed to auloclave

Fig. 5. Net products distribution oi] a basis of 100kg as received.

354 J. BARRAZA E T AL.

Table 3. Major element analysis in ashes of coal extract liquids and HAO

Feed to autoclave Original Overflow Underflow HAO

Digestion Pressure, bar 10 40 40 40

Extract ash value, % w/w 0.045 0.023 0.048 0.041 0.003

Concentration of element
in ash (% wt)
A1 2.96 1.76 0.37 0.55 8.11
Ca 17.26 17.53 22.24 20.83 1.65
Fe 5.9 9.9 9.4 10.5 10.9
K 0.04 0.05 0.03 0.03 1.07
Mg 4.6 0.62 0.22 0.65 0.67
Mn 0.52 1.9 0.18 1.17 0.16
Na 0.42 0.35 0.19 0.22 1.85
Si 1.21 2.92 1.21 0.59 15.2
Ti 1.37 1.09 1.37 0.68 N/D

N/D: Not detected.

extract solution from the original coal is proportion in extract solution from the original
achieved. These findings are in agreement with coal digested at 10 barg. With regard to Na and
the results obtained by Cloke (1986). Thus, a Mg, both show a high proportion in the extract
digestion pressure of 40 barg was used with the liquid from the original coal and a low propor-
overflow coal fractions, since it was expected tion in the extract from the overflow. Ti and Fe
that this would give a low ash content in the coal do not show variations, while A1, K and Si give a
extracts. However, the results of ash content in great reduction in the majority of extract
the extracts from the coal fractions show that solutions. Kovach et al. (1978), have shown
the beneficiated overflow did not produced a that the alkali metals, Ca and Na, and the acidic
coal extract with ash content lower than the coal metals, Ti and Si, are greater deactivators of the
extract from the original coal. This may be due hydrocracking catalysts used in a two-stage
to the differences in heavy organics material liquefaction process. In the present study, a
content in the coal fraction as is shown in Fig. 5. reduction in the concentration of these elements
Differences in the proportion of elements found using overflow fractions has been achieved,
in the extracts, defined as the concentration of which would be beneficial in prolonging the
the element in the ash of the extract divided by hydrocracking catalyst life.
the concentration of the element in the ash of the The above results show that there are changes
feed to the autoclave, are shown in Fig. 6. Ca in the major element proportions between the
and Mn show the highest increase in all the coal extracts produced using different types of feed to
extract liquids, however, Ca gives the lowest the autoclave. In order to examine this trend the
proportion in the extract solution from the results are recalculated in terms of the masses of
overflow fraction, while Mn has the lowest the elements in each extract and coal samples fed

16.00
[] Original10
~9 14.00
t~ ii I~1Original40
s 12.oo
IlllOF 1.2640
10.00
[] UF 1.26 40
~ s.oo
6.00 _ _ _

4.00
o 2.00
0.00
AI Ca Fe K Mg Mn Na Si Ti
Element

Fig. 6. Concentration proportions of elements in coal extracts relative to feed autoclave.

 DIRECT COAL LIQUEFACTION 355

Table 4. Mass of major element in coal extract solutions

Feed to autoclave Original coal Overflow Underflow

Digestion Pressure, bar 10 40 40 40

Mass of coal converted, dmmf (g) 65.90 71.60 88.63 62.98

Mass of extract (g) 260.58 266.16 282.86 257.72
Mass of element in extracts (mg)
Element
A1 3.47 1.08 0.50 0.58
Ca 20.24 10.73 30.20 22.01
Fe 6.92 6.06 12.76 11.09
K 0.05 0.03 0.04 0.03
Mg 5.39 0.38 0.30 0.69
Mn 0.61 1.16 0.24 1.24
Na 0.49 0.21 0.26 0.23
Si 1.42 1.79 1.64 0.62
Ti 1.61 0.67 1.86 0.72

to the autoclave. For this, a basis of 100g of coal Si. However, Ti, Ca and Fe have the highest
fed to the autoclave was used and the material increase and K and Na show approximately the
vented was estimated 2% of the coal converted. same proportions. It indicates that the elements
The results for each type of coal fed to the Ca, Ti and Na, which are considered to be the
autoclave are shown in Table 4. Differences were deactivating elements of the hydrocracking
observed in both the amount of coal converted catalyst, were not reduced in the extracts using
and the mass of the elements in the extracts. The the overflow fraction compared to the original
highest mass of coal converted was obtained coal. These findings again may suggest the
with the overflow fraction, which is due to the association of Ca and Ti with the organic
high conversion achieved. Also, it was found matter, such as has been shown in other studies
that the majority of masses of the elements show (Robatt et al. 1984; Cloke 1986)
a decrease in the extracts from the original coal
as the pressure is increased. However at 40 barg,
the masses of some elements in the extract from
the overflow were not reduced compared to the Conclusions
masses of the same elements in the extract from
the original coal. Therefore, in order to analyse 1. The dense medium cyclone unit produced
which elements give a reduction in the extracts an overflow coal fraction of high concentration
from overflow relative to the original coal, the in organic matter and low concentration in
masses of the elements are transformed into the mineral matter.
proportions shown in Fig. 7. Results show a 2. In general, liquefaction results show an
decrease in the proportion for A1, Mg, Mn and improvement in conversion for the overflow

J
2.5

1.5
~- 1

0.5 +--F
, [---] ~
0
AI Ca Fe K Mg Mn Na Si Ti
Element

Fig. 7. Mass proportion of element in extract from overflow relative to extract from original coal.
356 J. BARRAZA E T AL.

fractions over the original coal. By contrast, the References

underflow fraction gave the lowest conversion.
Given the high mineral matter content to BARRAZA, J., GILFILLAN,A., CLOKE, M. & CLIFT, D.
1994 International Coal Conference on Coal Bed
remove in the filtration process, the underflow
Methane, Cardiff, Wales, September.
fraction is not a material desired for liquefaction CLOKE, M. 1986. Fuel, 65, 417.
purposes. - - 1987. PhD. Thesis, University of Nottingham
3. A shift in the net product distribution - - , BELGHAZI,A., MARTIN, S., KELLY, B., SNAPE,
towards higher oils and lower asphaltenes and C. E., MCQUEEN, P. & STEEDMAN, W. 1993.
preasphaltenes were obtained in the liquid International Conference on Coal Science, Banff,
product using the overflow fraction. However, Canada,
it gave the highest heavy organics content, which - - , CLIFT, D., GILFILLAN,A., MILES, N. & RHODES,
would be detrimental for the hydrocracking D. 1994. Fuel Processing Technology, 38, 153.
CRONAUER, D. & SWANSON, A. 1991. 201 ACS
stage.
National Meeting, Atlanta, Georgia, 14.
4. The beneficiation did not reduce the ash DYRKACK, G. R. & HORWlTZ, E. P. 1982. Fuel, 61, 3.
content in the filtered coal extract solution HAMILTON, S. 1986. Thesis M. Phil, University of
compared to the ash content in the extracts Nottingham.
from the original coal. However, the quantity of JOSEPH, J. T., FISHER, R. B., MASIN, C. A., DYRKACZ,
mineral matter to be removed at the filtration G. R. & BLOOMQUIST, C. A. 1991. Energy and
stage was reduced. Fuels, 5, 724.
5. Reduction in the proportion of masses of KEOGH, R. A. & POE, S. H. 1987. International
A1, Mg, Mn and Si, in the extracts from the Conference on Coal Science, The Netherlands,
289-294.
overflow relative to the original coal were
KING, H. H., DYRKACKZ, G. R. & WlNANAS, R. E.
obtained. However, some of the strongest 1984. Fuel, 63, 341.
deactivating elements such as Ti and Ca show KOVACH, S. M., CASTLE, L. J. & BENNETT,J. V. 1978.
a large increase in proportion. Industrial and Engineering Chemistry; Production,
Research and Development, 17, 1 62-67.
The authors gratefully acknowledge the award of a ONER, M., ONER, G., BOLAT, E., YATIN, G., KAVLAK,
grant in aid of research from the European Coal and C. & DINCER, S. 1994. Fuel, 73, 10.
Steel Community (ECSC), the Colombian Institute of PARKASH, S., LALI, K., HOLUSZKO,M. & DU PLESSIS,
Science and Technology (COLCIENCIAS), the British M. P. 1985. Liquid Fuel Technology, 3, 3.
Coal Utilization Research Association and the United ROBBATT,A., Jr., FINSETH, D. H. & LETT, R. G. 1984.
Kingdom Department of Trade and Industry. The Fuel, 63, 1710-1714.
assistance of British Coal Liquefaction for provision of RHODES, D., HALL, S. T. & MILES, N. J. 1993. XVIII
samples is acknowledged. The views expressed are International Mineral Processing Congress, 23-28.
those of the authors and not necessarily those of the STEELER, M. 1987. International Conference on Coal
funding bodies. Science, The Netherlands, 115-118.
Conversion of low rank coal into liquid fuels by direct hydrogenation

B. R. A L E K S I ( ~ ~, M. D. E R C E G O V A C , O. G. C V E T K O V I ( ~ 3,
B. Z. M A R K O V I ( ~ ~, Y. L. G L U M I ( ~ I ( ~ 3, B. D. A L E K S I ( ~ ~
& D. K. V I T O R O V I ( ~ 3
'IChTM, Center of Catalysis and Chemical Engineering, NjegoYeva 12,
11000 Belgrade, FR Yugoslavia
2 Faculty of Mines and Geology, University of Belgrade, DjuYina 7,
11000 Belgrade, FR Yugoslavia
3 IChTM, Center of Chemistry, Njegogeva 12, 11000 Belgrade, FR Yugoslavia

Abstract: A study of low-rank coal conversion into liquid products by direct catalytic
hydrogenation was undertaken. A soft brown coal from the 'Tamnava' field of the Kolubara
mines characterized by a huminite reflectance of 0.27+0.03%RR, ash content of
10.4wt%(db), carbon content of 64.0wt% (daf), and volatiles ca. 50wt%(db), was
submitted to liquefaction in a batch reactor. The effect of reaction parameters on both the
yield and nature of liquefaction products was studied for temperatures ranging from 365 to
440~ and pressure from 13.5 to 16.5 MPa, with process duration from 1 to 8 hours. The
total coal conversion was high at all applied reaction conditions (84-93%, daf coal basis),
pointing to a high reactivity of this coal. The yield of particular liquid products varied
markedly depending on temperature and residence time. The yield of light-oil (n-heptane
soluble products) increased and that of asphaltenes decreased by increasing the temperature
and prolonging the residence time. Changes in petrographic composition of the coal were
examined by microscopic analysis. At more severe reaction conditions the content of semi-
coke and coke increased. With the increase of temperature at mild conditions, the
proportions of both the reacted coal and granular residue increased, while the cenospheres
and mineral matter decreased.The nature of the changes observed in the organic and mineral
components of the coal grains was used to correlate the degree of coal conversion with the
experimental conditions.

Contrary to the previous conception that only The work presented here was aimed at
bituminous and subbituminous coals might be obtaining information on the behaviour of soft
used for liquefaction, much research effort has brown coal from the 'Tamnava' field of the
recently been directed toward determining the Kolubara mines (Serbia) during liquefaction by
susceptibility of low-rank coals to liquefaction. direct catalytic hydrogenation. The effect of the
It has been reported (Derbyshire & Stansberry reaction parameters on the changes in the coal
1987; Mondragon et al. 1988) that certain soft petrographic composition was examined and
brown coals liquefy more readily than high-rank correlated with the changes observed in the
coals. There is a number of research papers degree of coal conversion and in the liquefaction
dealing with the correlation between liquefaction product yields.
behaviour and various properties of coals,
especially coal petrography (Artemova et al.
1989; Given et al. 1980; Hower et al. 1991;
Parkash et al. 1984), but there is a lack of Experimental method
generally valuable correlations. One of the
reasons is the chemical and petrographic hetero- Liquefaction of pulverized coal (< 160 #m) slurry
geneity of coals within the same rank. The other in tetralin in the presence of a granulated cobalt-
reason might be the complex interaction of coal molybdenum hydrodesulphurization catalyst
mineral components with the organic part of was performed by a stream of hydrogen in a
coal during liquefaction. Therefore, data batch reactor. The reaction parameters were
obtained under certain experimental conditions varied in the following ranges: temperature,
of a particular coal liquefaction cannot be from 365 to 440~ pressure, from 13.5 to
considered reliable for other types of coals or 16.5 MPa; residence time in the reaction condi-
even for the same coal treated by a different tions, 1 to 8 hours. The choice of particular
liquefaction procedure (Tischer & Utz 1983). parameters was based on preliminary experi-

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 357-363.
358 B. R. ALEKSIC E T A L .

mental work. After cooling, the liquefaction reflectance, 0.27 + 0.03% RR, and volatiles,
products were separated according to a pre- 49.5 (wt%, dry basis), the average coal sample
viously established procedure (Vitorovi6 et al. belongs to soft brown coals, designated as M2
1991). After filtration the solid residue and the coals (Ercegovac 1986) with a xylite content of
catalyst were rinsed several times with the filtrate 42.0 wt%.
itself, then the catalyst was separated by sieving The liquefaction yields representative of dif-
and dried to constant weight at 300~ The ferent reaction conditions (temperature, T;
liquid liquefaction products were separated from pressure, p; residence time, rr) are shown in
tetralin by distillation. The light oil was dis-
solved in n-heptane, the undissolved part con-
sisting of asphaltenes. The liquid products were
characterized by ultimate analysis and gas Table 1. Characteristics of Tamnava coal sample
chromatography (30m Supelco capillary SPB-1
column). The solid residues were characterized Equilibrium moisture (wt%) 12.3
by ultimate and micropetrographic analyses. Ash (wt%, dry basis) 10.4
Sulphur, total (wt%, dry basis) 1.0
The methods have been described in more Fixed carbon (wt%, dry basis) 26.1
detail elsewhere (Vitorovi6 et al. 1991, 1994). Volatiles (wt%, dry basis) 49.5
The degree of coal conversion (X) was calcu- Ultimate analysis (wt%, dry basis, ash free)
lated on the basis of the dry, ash free solid Carbon 64.0
residue (R) according to: X = lO0(mo-R)/mc, Hydrogen 5.7
where mc denotes the initial mass of the coal Nitrogen 1.3
(dry, ash free). Oxygen (by difference) 29.0
Microscopic examination of the solid residues Heating value (kJ kg-1) HHV 19 327.3
LHV 18 425.5
and the initial coal sample was carried out on
Macerals and minerals (vol%)
two polished blocks prepared from each sample, Huminite 67.0
involving 1000 measurements according to ICCP Textinite 25.0
standards (1963, 1971). Ulminite 21.0
Atrinite 11.0
Densinite 4.0
Gelinite 6.0
Results and discussion Liptinite 3.5
Inertinite 6.0
The characteristics of the initial coal sample are Minerals 23.5
given in Table 1. The coal substance of the Clay 20.0
'Tamnava' coal sample is in a relatively low Pyrite 2.5
stage of humification and gelification (0.73). The Carbonates 1.0
Gelification index 0.73
proportion of the non-gelified macerals is Huminite reflectance, RR (%) 0.27
42.0vo1%, and that of gelified (homogenous) Xylite (wt%) 42.0
macerals 31.0vo1%. According to huminite

Table 2. Liquefaction yields (wt% daf coal) and coal conversion (%)

Test Reaction conditions Products Conversion

No
T (~ p (MPa) rr (h) Oil Asphaltenes Solid residue

1 365 13.5 1 22.6 25.5 15.7 84.3

2 365 13.5 4 21.8 26.3 11.5 88.5
3 365 13.5 6 16.8 17.0 14.5 85.5
4 365 13.5 8 16.5 15.7 6.7 93.3
5 365 16.5 4 22.2 27.0 10.3 89.7
6 400 13.5 4 26.6 27.8 13.8 86.2
7 400 16.5 4 25.5 23.5 15.3 84.7
8 420 15.0 4 52.5 7.2 9.2 90.8
9 440 13.5 4 68.2 7.8 11.5 88.5
10 440 13.5 8 74.4 5.1 11.3 88.9
11 440 15.0 4 65.4 6.2 10.8 89.2
12 440 15.0 8 73.0 3.3 13.6 86.4
 C O N V E R S I O N OF LOW R A N K COAL INTO L I Q U I D FUELS 359

Table 3. Petrographic composition and optical characteristics of liquefaction residues of Kolubara coal ("Tamnava')

Test 1 2 3 4 5 6 7 8 9 10 11 12
No
Categories of grains T (~ 365 365 365 365 365 400 400 420 440 440 440 440
(vol%) p(MPa) 13.5 13.5 13.5 13.5 16.5 13.5 16.5 15.0 13.5 13.5 15.0 15.0
No. 7-r (h) 1 4 6 8 4 4 4 4 4 8 4 8

1 Unreacted and partly - - 0.5 - 0.5 0.5 2.0 - 1.0 0.5 1.0 1.0

reacted coal
2 Reacted coal 12.5 13.0 40.0 12.0 ll.0 23.0 27.0 ll.5 28.0 24.5 18.0 10.5
3 Isotropic humoplasts 4.0 6.5 tr. 0.5 6 . 0 - - 1.0- tr. tr. tr.
4 Asphaltenes (pitch-like 0.5 tr. 0.5 - 0.5 1.5 1.0 - 2.0 - - -

material)
5 Cenospheres (Iso.) 10.0 5.5 2.5 1.0 3.5 tr. 1.5 2.5 tr. 2.0 3.0 4.5
6 Semi-coke (Iso.) 1.0 - - 1.5 1.5 - 5.0 3.5 - 2.0 2.0 ll.0
7 Coke (Aniso.) - - - tr. - tr. 0.5 0.5 - 4.0 1.0 4.0
8 Isotropic grains 2.0 0.5 1.0 2.0 2.0 3.0 1.5 2.5 2.5 0.5 tr. 1.0
(porous, A-type)
9 Homogenous isotropic 1.0 0.5 3.5 0.5 - 1.0 0.5 tr. 0.5 0.5 0.5 0.5
grains (high % RR)
10 Granular residue 42.0 45.0 35.5 47.0 61.0 54.0 44.0 69.0 52.0 46.0 61.0 59.0
(partly porous
structure)
11 Fragments 3.0 2.0 3.5 1.0 2.0 4.0 4.5 1.0 3.0 7.5 0.5 1.5
(<0.010ram)
Mineral Clay 21.0 24.0 12.0 31.5 9.0 9.5 8.0 4.5 8.0 9.0 9.5 3.0
12 Matter Pyrite 3.0 3.0 1.0 3.0 3.0 1.5 2.5 4.0 1.5 3.5 3.5 4.0
Carbonates . . . . . 2.0 2.0 - 1.5 - - -

Table 2. High coal conversion was observed at 1994) as follows: unreacted and partly reacted
all investigated conditions but the relative yields coal (cat. 1; up to 2.0 vol%), reacted coal (cat. 2;
of liquefaction products varied. By prolonging 10.5-40.0vo1%), isotropic humoplasts (cat. 3;
the residence time at lower temperature and traces to 6.5 vol%), asphaltenes (pitch-like mate-
pressure (test 4 vs. test 1) the a m o u n t of solid rial; cat. 4; traces to 2.0 vol%), cenospheres (iso.,
residue decreased, the conversion was higher, cat. 5; traces to 10.0 vol%), semi-coke (iso., cat 6;
but the relative yields of liquid products 1.0-11.0 vol%), coke (aniso., cat. 7; traces or
decreased probably due to formation of gases. 0.5-4.0vo1%), isotropic grains (A type; cat. 8;
At m o r e severe reaction conditions (tests 9-10 traces to 3.0vo1%), h o m o g e n e o u s isotropic
and 11-12), the yield of n-heptane soluble liquid grains (cat. 9; traces to 3.5vo1%), granular
product (oil) increased as a result of a higher residue (partly porous structure; cat. 10,
degree of h y d r o g e n a t i o n of coal particles dissol- 35.5-69.0vo1%), fragments ( < 0 . 0 1 0 m m , cat.
ving at the beginning of the process. The effect 11; 0.5-7.5vo1%) and mineral matter (cat. 12;
o f temperature m a y be seen if tests 2, 6 and 9 are clay, 3.0-31.5vo1%; pyrite, 1.0-4.0vo1%; and
compared. The overall coal conversion and the carbonates, max. 2.0vo1%). The microscopic
solid residue did not change markedly, but appearance of the solid liquefaction residues is
the yield of oil increased, at the expense of shown in Figs 1 & 2.
asphaltenes whose yield decreased. Results The effects of residence time and temperature
of tests 2 and 5, or 9 and 11, respectively, on the proportions of the particular grain
showed that the effect of pressure on the categories are shown in Tables 4 & 5 respec-
liquefaction yields was less pronounced. tively. The extended time o f liquefaction (from
The categories of grains presented in Table 3 1 to 8 hours) at mild conditions (365~ and
were identified and estimated by micropetro- 13.5 MPa) (Table 4 tests 1, 2 and 4) affected the
graphic analysis of the solid residues. The residue coal petrographic composition as follows: the
grains were placed in different categories (Guyot proportions of the reacted coal and semi-coke
& Diessel 1981; Ercegovac 1986; Vitorovi6 et al. plus coke did not change greatly; the a m o u n t of
360 B. R. ALEKSIC E T AL.

Fig. 1. Microscopic view of solid liquefaction residues of Kolubara coal, field Tamnava: (a) partly reacted coal,
the beginning of decomposition of huminite (test 6); (b) reacted coal with pitch-like material (? asphaltenes) and
small inclusion of inertinite (test 9); (c) huminite plasticity and the beginning of formation of humoplasts after
batch hydrogenation (test 1); (d) individual and coalesced humoplasts (solvent affected material) and granular
residue with fine grained mineral matter (heat affected material - test 2); (e) isotropic humoplasts with higher
reflectance (test 12); (f) fused and partly carbonized material with degasification pores (test 7); (g) granular
residue (down) and reticulated isotropic cenosphere with thick wall (test l); (h) mixed grains: reacted coal (upper),
granular residue (left) and weak - anisotropic semi-coke (test 12); (i) highly reflecting isotropic homogenous grain
(left), porous weak - anisotropic semi-coke and highly reacted coal (gray) (test 7). Reflected light, oil, • 360.
 C O N V E R S I O N OF LOW R A N K COAL INTO L I Q U I D FUELS 361

Fig. 2. Microscopic view of solid liquefaction residues of Kolubara coal, field Tamnava: (a) characteristic view of
specific category of oxidized grains with cracks (isotropic grains - type A; test 7); (b) same category of grains with
a carbonized outer wall (aniso.; test 7); (c) porous isotropic grain showing development of vacuoles (black
holes) - 'transition stage' to semi-coke formation ? (test 6); (d) "transition stage' to semi-coke, formation between
the granular residues (test 12); (e) porous isotropic semi-coke (test 12); (f) highly anisotropic grain of coke with
high degree of reflectance (test 12); (g) specific art of agglomeration of reacted coal grains (test 11); (h) mixed
grains: simple cenosphere and pyrrhotite between the granular residues (test 1); (i) mixed grains: slightly altered
huminite particle displaying indications of partial softening, single thin walled cenospheres and pyrite-pyrrhotite
agglomerate between the granular residues (test 1). Reflected light, oil, x360.
362 B. R. ALEKSIC E T AL.

Table 4. Change in petrographic" composition of the solid residues with the residence time at different reaction
conditions

Categories of grains (vol%) A. T= 365~ p-- 13.5 MPa B. T= 440~ C. T= 440~

p = 13.5 MPa p = 15.0 MPa

Tr= 1h rr=4h rr=8h rr=4h Tr=8h Tr=4h Tr=8h

Test No.

No. 1 2 4 9 10 11 12
2 Reacted coal 12.5 13.0 12.0 28.0 24.5 18.0 10.5
5 Cenospheres (Iso.) 10.0 5.5 1.0 tr. 2.0 3.0 4.5
6+ 7 Semi-coke & coke 1.0 - 1.5 - 6.0 3.0 15.0
10 Granular residue 42.0 45.0 47.0 52.0 46.0 61.0 59.0
12 Mineral matter 24.0 27.0 34.5 11.0 12.5 13.0 7.0

Table 5. Change in petrographic composition of the solid residues with temperature

Categories of grains (vol%) A. Tr=4h; p = 13.5MPa B. r r = 4 h ; C. % = 8 h ;

p = 15.0 MPa p = 13.5 MPa

T= 365~ T=400~ T= 440~ T=420~ T=440~ T= 365~ T=440~

Test No.

No. 2 6 9 8 11 4 10
2 Reacted coal 13.0 23.0 28.0 11.5 18.0 12.0 24.5
5 Cenospheres (Iso.) 5.5 tr. tr. 2.5 3.0 1.0 2.0
6 + 7 Semi-coke & coke - tr. - 4.0 3.0 1.5 6.0
10 Granular residue 45.0 54.0 52.0 69.0 61.0 47.0 46.0
12 Mineral matter 27.0 13.0 11.0 8.5 13.0 34.5 12.5

isotropic cenospheres decreased considerably By increasing the temperature at mild condi-

(from 10.0 to 1.0 vol%); both the granular tions, the proportions of both the reacted coal
residue and the amount of mineral matter and the granular residue increased, while those
increased, in accordance with the observed of cenospheres and mineral matter decreased
higher conversion of the organic part of coal at (Table 5, tests 2, 6 and 9). Semi-coke and coke
longer residence time (Table 2). The effect of the were not observed at these conditions. These
residence time at the most severe conditions results were in accordance with the increase of
(440~ and 15.0 MPa) was demonstrated by an oil yield with temperature (Table 2, tests 2, 6
increased formation of semi-coke and coke and 9). At a higher pressure, semi-coke and coke
(Table 4, tests 11 and 12). The observations appeared at higher temperatures (Table 5, tests 8
confirmed the postulated mechanism of coal and 11).
liquefaction (Shinn 1984). The observed By increasing the pressure from 13.5 to
decrease of the mineral matter content was due 16.5 MPa an effect was observed at mild condi-
to the increaase of the amount of coke and semi- tions (365~ 4 h) in tests 2 and 5 (Table 3). The
coke in the liquefaction residue. In contrast to maceral composition of the two residues was
experiments at mild conditions, the prolonged similar except for the higher proportion of
residence time at higher temperature and pres- granular residue and the lower proportion of
sure caused a slight increase in the cenosphere mineral matter in the sample obtained at higher
content. The mechanism of particular maceral pressure. It is interesting to note that an increase
changes during the coal liquefaction is poorly in the proportions of mezophase products,
understood at present. Therefore, it is difficult especially the semi-coke and coke, was not
to draw any definite conclusion on the experi- observed by increasing the pressure at mild
mental conditions promoting formation or conditions. However, at more severe reaction
decay of cenospheres. conditions the proportion of semi-coke and coke
 CONVERSION OF LOW RANK COAL INTO LIQUID FUELS 363

increased probably as a result of simultaneous References

effects of the temperature, pressure and resi-
dence time (Table 3 tests 10 and 12). The high ARTEMOVA, N. J. KASATOCHKINA, L. J. CHIZHEVS-
yield of oil and the low yield of asphaltenes, KAYA, V. R. & SHULAKOVSKAYA,L. V. 1989. The
effect of the petrographic composition of coals on
observed at 440~ and 13.5 or 15.0MPa, their hydrogenation. Khim. Tverd. Topl. (Chem.
indicated that polymerization of dissolved Solid Fuels), 4, 75-79 (in Russian).
and partly hydrogenated coal fractions did not DERBYSHIRE, F. & STANSBERRY,P. 1987. Comments
occur even during a prolonged reaction time. on the reactivity of low-rank coals in liquefaction.
Hence, the coking was a solid particles process, Fuel, 66, 1741-1742.
involving the remaining carbonaceous part of ERCEGOVAC, M. 1986. Brown and black coal hydro-
the coal. genation in comparative studies of their petro-
The results obtained indicate that at 440~ the graphic composition and solid residue. An. Gdol.
reactions in coal yielding liquid and gaseous de la P~nins. Balkanique, 50, 419-441 (in Serbian).
GIVEN, P. H., SPACKMAN,W., DAVIS, A. & JENKINS,
products (dissolution, volatilization, decomposi- R. G. 1980. Some proved and unproved effects of
tion of the coal substance) end in a period of coal geochemistry on liquefaction behaviour with
time shorter than four hours, under the applied emphasis on U.S. coals. In: WHITEHURST, D. D.
experimental conditions. During prolonged (ed.) Coal Liquefaction Fundamentals. American
retention time, hydrogenation of the liquid Chemical Society Symposium Series, 139, 3-34.
phase and thermal processes in the remaining GUYOT, R. E. & DIESSEL,C. F. K. 1981. Petrographic
solid phase continue with no signs of any studies on insoluble residues of hydrogenated
significant interaction. At lower temperatures coals. International Journal of Coal Geology, 1,
and pressures the conversion of coal did not 197-207.
HOWER, J. C., KEOGH, R. A. & TAULBEE,D. N. 1991.
seem to have been terminated during the applied Petrology of liquefaction residues: maceral con-
residence times. Further investigations are centrates from a Pond Creek durain, eastern
necessary for a more reliable correlation of Kentucky. Organic Geochemistry, 17, 431-438.
petrographic compositional changes of the ICCP - Internationales Lexikon ffir Kohlenpetrologie
'Tamnava' coal during the liquefaction process 2. Ausgabe, Paris, Centre National du Recherche
with the liquefaction yields. Scientifique, 1963. und Erg~inzungen Band zur 2.
Ausgabe, 1971, Paris.
MONDRAGON, F., QUINTERO, G., ACOSTA, R. &
Conclusions
JARAMILLO, A. 1988. Liquefaction characteristics
of some Columbian coals: 1. Reactivity in
A high degree of conversion (>84%) of the soft catalytic hydrogenation. Fuel, 67, 1709-1711.
brown coal 'Tamnava' was observed during PARKASH, S., DU PLESSIS, M. P., CAMERON,A. R. &
KALKREUTH, W. O. 1984. Petrography of low
liquefaction by direct catalytic hydrogenation.
rank coals with reference to liquefaction poten-
Varying the reaction conditions (the tempera- tial. International Journal of Coal Geology, 4,
ture, pressure and residence time), high yields of 209-234.
liquid products were obtained. The high reac- SHINN, J. H. 1984. From coal to single-stage and two-
tivity of the coal was confirmed by petrographic stage products: a reactive model of coal structure.
analysis which showed that there was no Fuel, 63, 1187-1196.
unreacted coal in the solid residues with most TISCHER, R. E. & UTZ, B. R. 1983. Comparison of
of the liquefaction runs. The petrographic normal and rapid heat-up modes in a batch
composition of the residues depended on the screening test for coal liquefaction catalysts.
Industrial and Engineering Chemistry, Product
reaction conditions, but a more reliable correla-
Research and Development, 22, 229-233.
tion requires additional investigations. Never- VITOROVI(~, D., ALEKSIC, B. R., KONTOROVIC, S. I.,
theless, petrographic analyses produced valuable ALEKSIC, B. D., ERCEGOVAC, M., MARKOV1C,
data concerning the changes in the 'Tamnava' B. Z., BOGDANOV,S. S. & CVETKOVlC,O. G. 1991.
soft brown coal during liquefaction. Liquefaction of brown coal prepared by grinding
under different conditions. Fuel, 70, 849-855.
This work was supported in part by the Research VITOROVIt~, D. K., ALEKSIt~, B. R., ERCEGOVAC,
Fund of Serbia (Project No 0816). The authors are M. D., ALEKSI{~, B. D., KONTOROVIC, S. I.,
grateful to the Kolubara Mine for providing the coal MARKOVlC, B. Z., CVETKOVI~, O. G. &
'Tamnava' samples. MITROVSKI, S. M. 1994. Liquefaction behaviour
of Kolubara soft brown coal. Fuel, 73, 1757-1765.
Desulphurization of low-rank coals by low-temperature carbonization
R. A S M A T U L U , N. A C A R K A N , G. O N A L & M. S. C E L I K

Istanbul Technical University, Mining Engineering Department, Coal and Minerals

Processing Section, Ayazaga, 80626 Istanbul, Turkey

Abstract: A lignite sample from the Istanbul region with 14.18% inherent moisture, 11.01%
ash, 1.86% total sulphur, 47.24% volatile matter, 41.75% fixed carbon and 5590kcal kg-1
calorific value as dried basis has been subjected to a set of systematic low-temperature
carbonization tests. The tests have been carried out as a function of particle size,
temperature and heating time. A semicoke product containing 15.22% volatile matter,
16.67% ash, 68.04% fixed carbon contents with 63% desulphurization on the basis of total
sulphur has been obtained under the optimum conditions of 650~ temperature and
50 minutes of heating time. The product has a calorific value of 6403 kcal kg-1 but does not
have enough strength for use as a fuel and thus needs to be improved by briquetting.

Istanbul, one of the major populated cities in the 1993). Low-temperature drying processes have
world, is currently encountering a severe air been employed since 1920s and the first patents
pollution problem in the winter season, partly by Fleissner appeared a few years later (Fleissner
caused by the burning of low-rank coals. The 1927 and 1928). In this process hot air or gas is
better quality coals extracted from coal mines in sent to accomplish drying of either surface or
the vicinity of Istanbul are generally not inherent moisture of coal. Since the inherent
upgraded by coal preparation processes. These moisture in low-rank coals is distributed in the
coals are produced about 200-400mm in size form of very fine capillaries, high temperatures
with 30-40% moisture, 35-40% volatile matter, are necessary. This leads to fragmentation and
1-3% total sulphur contents and calorific values consequently production of fines. Also, the dried
of 2400-3800 kcal kg -1 as received basis. coal is sensitive to spontaneous combustion.
Coal used for household heating makes up Work done in this area in the last two decades
about 60% of the total heating requirement in (Koppelman 1977; Cole & Ness 1977; Verschuur
Istanbul. Lignites produced from the Istanbul et al. 1976; Wash 1977; Evans & Sieman 1979)
region constitute about 80% of this total have focused on steam or hot water drying.
consumption. The high moisture, volatile The use of hot water or steam drying has
matter and sulphur contents are the major advantages of (i) production of low moisture
causes of coal-based air pollution in Istanbul. coal, (ii) reduction in the tendency of coal to
High moisture not only leads to low combustion reabsorb moisture, and most importantly,
efficiencies but also the discharge of unburned (iii) reduction in fragmentation and spontaneous
fines into the atmosphere. In addition, since ignition. A pilot plant erected in Wyoming in
domestic boilers and stoves are not specifically 1992 and Ceska Palivova commercial plant built
designed for burning low-rank coals, the volatile now in the Czech Republic working under
matter is emitted into the air before it is fully 80 atmosphere pressure and 400~ represents
burned. This problem results in hydrocarbon the most up to date technology in this area
and particulate matter emission. (Gentile 1995).
All these problems mentioned above led to the It is the objective of this study to conduct low-
development of new technologies for the mini- temperature carbonization tests on a typical
mization of air pollution originating from coal. Istanbul region lignite with the aim of reducing
Since sulphur is a major pollutant endangering the sulfur levels in the coal.
the human life, various desulphurization techni-
ques, i.e. desulphurization prior to combustion, Table 1. Analysis of the lignite sample on dry basis
desulphurization during combustion and, post-
combustion desulphurization processes need to % Moisture 32.50
be systematicaly tested (Celik & Somasundaran % Ash 11.01
1994). One of these processes involving low % Total sulphur 1.86
temperature carbonization at temperatures in % Combustible sulphur 1.05
% Volatile matter 47.24
the range of 400-700~ aims to reduce the
% Fixed carbon 41.75
sulphur content of coal (Gazanfer 1983; Lowry Upper calorific value, Kcal kg-1 5590
1945; Von 1982; Onal et al. 1995; Sciazko et al.

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 365-369.
366 R. ASMATULU E T AL.

Experimental procedure volume of 1500 cm 3. The discharged gases were

transferred to a cooling system via a screwed
Materials gate. The interior volume of the retort limited
the upper size of the coal sample to 50 mm. The
Low-temperature carbonization tests were car- tests were conducted with 500 g samples brought
fled out on representative samples taken from to an inherent moisture of 14%. The furnace
Istanbul-Yenikoy region lignites. The complete was preheated to desired temperature and the
analysis of the lignite sample on dry basis is sample placed for a certain period. After the
presented in Table 1. The original sample of sample was taken out and cooled, the weight
minus 100mm in size was crushed below 50ram loss, volatile matter and total sulphur contents,
and then classified into three size fractions. The size analysis, and drum strength measurements
analyses of these size fractons are shown in were performed (Table 2).
Table 2. The experiments were performed as a func-
tion of particle size ( 1 9 x 5 0 , 10x 19, and
Methods 1 x 10mm), temperature (400-700~ and heat-
ing period (20-120min). The physical and
The carbonization tests were performed in a chemical properties of the semicoke product
10 cm diameter cylindrical retort with an interior were also determined.

Table 2. The analysis of coal sample on dry basis as a function of particle size

Size fraction % by weight % volatile % fixed % total % ash calorific

(mm) matter carbon sulphur content value
(kcal/kg)

19 x 50 69.8 47.82 41.88 1.80 10.30 5598

10 x 19 16.2 46.47 41.85 1.84 11.68 5470
1 x 10 14.0 45.60 41.44 2.10 12.96 5270

Table 3. Total sulphur contents in semicoke products under different conditions

Temperature ( ~ Heating time (min) Size (mm)

19x50 10x 19 1 x 10

400 20 1.84 1.91 2.29

40 1.76 1.83 2.22
60 1.61 1.76 2.10
80 1.57 1.64 2.03
100 1.51 1.51 1.98
120 1.44 1.42 1.85
500 20 1.77 1.83 2.17
40 1.56 1.67 2.07
60 1.42 1.53 1.92
80 1.36 1.38 1.89
100 1.31 1.31 1.80
120 1.25 1.28 1.68
600 20 1.70 1.74 2.11
40 1.61 1.59 1.98
60 1.39 1.45 1.85
80 1.32 1.39 1.65
100 1.27 1.28 1.52
120 1.2 1.21 1.46
700 20 1.44 1.60 2.06
40 1.31 1.50 1.94
60 1.28 1.42 1.80
80 1.21 1.31 1.58
100 1.14 1.18 1.41
120 1.06 1.10 1.35
 DESULPHURIZATION OF LOW-RANK COALS 367

Results and discussion 400~ even after 120 min only about 50% of the
desulphurization is attained. The slope of the
The total sulphur contents obtained upon low curves in Figs 1-3 also shows this trend, i.e. the
temperature carbonization of Yenikoy lignite at slope increases with increasing the temperature.
three different size fractions (19 x 50, 10 x 19, The results reveal that at low temperatures and
and 1 x 10mm) are presented in Table 3. The initial heating periods only the removal of
percent sulphur removal for each size fraction is moisture is achieved. Only above 400~ does
respectively illustrated in Figs 1 through 3 as a the volatile matter and sulphur begin to separate
function of heating time. The most important from the solid. The sulphur removal at 700~
factor in the carbonization and also in the and 120 min of heating attains its peak value of
desulphurization process appears to be the level about 69.4%. Carbonization of coal is generally
of temperature. For instance, while a 60% found to exhibit a parallel behaviour to that of
desulphurization is achieved on the semicoke desulphurization. For instance, the fixed carbon
product at 700~ after 40 rain and this accounts level of 41% has been raised to 66-70%
for about 90% of the total desulphurization, at with calorific values in the range of 6300-
6500 kcal/kg upon carbonization. At this level
100 of carbonization about 70% of sulphur removal
.... 15 9 V.M.
-50+19 mm is achieved.
9O o 400 ~ l All the three size fractions exhibit a similar
o 5 0 0 *C J
80 zx 6 0 0 *C ] trend in that at 400~ and in the beginning of
>
0
heating the sulphur removal remains at low
70 levels and increases with increasing temperature.
i,i
r~ The lower sulphur removal levels from the finer
60
rY A particle sizes can stem from two contributing
u_
_J
5O effects. First, as the coal bed used is fixed, the
~o 40
diffusion of heat through the particle takes some
p- time and in such cases, coarser particles are
Z 3O more advantageous. Second, the systematic
0
n- 2O increase in the fixed carbon content as a function
L~
IX. of size and temperature indicates that with
I0 increasing the temperature coal becomes more
amenable to sudden shocks which in turn lead to
20 40 60 80 1 O0 120 higher carbonization levels. This difference is
CARBONIZATION TIME, rain. minimized as the temperature decreases (Asma-
tulu et al. 1995). The net affect appears to
Fig. 1. The percent sulphur removal of coal as a
function of heating time for 19 • 50 mm size fraction. govern the results presented in Figs 1-3.

100 / 1oo F
. . . . 15 % V.M.
-19+10 rnm 15 ~ V . l d . / I -i0+1 mm
90 o 400 90 o 400 ~
D 500 I a 500 ~
iI
.< 80 "- 600 ,~ 80 ~, 600 ~c
> 0 700 > O 700 ~
0 o 7o
"~ 70
i,i
r
_

60 6O

u_ 50 2 5o
_J ._J

40 (/3 40

~: 3o ~ 30
0 u
U C)
~ 20 20
n

10 10

0 0-
0 20 40 60 80 IO0 120 0 20 40 60 80 1O0 120

CARBONIZATION TIME, rn[n. CARBONIZATION TIME, rain.

Fig. 2. The percent sulphur removal of coal as a Fig. 3. The percent sulphur removal of coal as a
function of heating time for -19 + 10mm size function of heating time for -19 + 10ram size
368 R. ASMATULU E T AL.

Table 4. Physical and chemical properties of the semicoke product obtained at 650~

Size Moisture Ash CombustibleTotal Volatile Fixed Calorific Drum test Oversize Ignition
fraction (%) content sulphur sulphur matter carbon v a l u e oversize (%) temp.
(mm) (%) (%) (%) (%) (%) (kcal/kg) (%) (~

-50 + 19 3.87 19.95 0.37 1.39 15.01 69.04 6459 11.28 52.41 320
-19 + 10 3.94 17.20 0.34 1.41 15.99 66.33 6324 40.91 65.41 300
-10 + 1 4.02 19.59 0.62 1.79 15.37 65.04 6221 90.55 90.63 290

Coal undergoes fragmentation upon carboni- lignite. The experiments showed that if semi-
zation due to the removal of moisture and volatile coking is continued until 15% volatile matter
matter from coal. This is strongly dependent remains, the tar in Istanbul Region lignites is
upon the particle size and temperature. For fully removed. Another important advantage of
example, the 19 • 50 mm size fraction treated at carbonization is that in addition to upgrading of
400~ for 20min resulted in fragmentation coal in terms of moisture and volatile matter, a
producing only 13% below 19 mm, whereas at significant portion of the combustible sulphur is
700~ 45.6% of the coal passed below 19mm also removed. Under optimum conditions 63%
after 20 min heating. The fragmentation of coal of desulphurization is achieved. The released
also reduces the strength of coal. Low tempera- gases can be purified for further use as a utility
ture coking on non-coking Mckinley and Crown gas or portion of it can be recycled as an energy
lignites has been tested at 600-700~ and found source for the process itself.
to increase the fixed carbon content from 45 to A disadvantage of the low-temperature car-
66%. These tests were performed in the size range bonization process is the fragile nature of the
of -75 + 20 mm. 20% of the coal was found to semicoke product. It is possible to use the plus
pass below 20 mm. Similar results have been also 10 mm fraction for household heating while the
obtained on German and Turkish lignites (Lowry finer fractions can be utilized in cement and
1945; Von 1982; Onal et al. 1995; Asmatulu et al. ceramic industries. However, if feasible, the fine
1995). Low temperature coking of Polish bitu- product can be briquetted both to improve its
minous coals is now exploited on commercial strength as well as its utilization.
scale (Sciazko et al. 1993).
Low-temperature carbonization increases the
Conclusions
calorific value of coal from 5200 kcal kg-I to
6000-6600kcalkg -1, depending upon the tem- Low-temperature carbonization studies con-
perature and residence time of the process. The ducted on the desulphurization of the Istanbul
results reveal that 650~ and 50 rain are respec- region lignite sample can be summarized as
tively the optimum conditions for Istanbul follows.
Region lignites. The physical and chemical prop- 1. The Istanbul region lignite is amenable to
erties of the semicoke product obtained under low-temperature carbonization tests. Tests con-
optimum conditions and for different particle ducted as a function of temperature and heating
sizes are given in Table 4. time revealed the optimum conditions to be
Coals with high moisture and volatile matter 650~ and 50 min of heating time.
contents such as Istanbul Region coals usually 2. A semicoke product containing 15.22%
cause air pollution when burned in simple volatile matter with 6403kcalkg -1 has been
combustion systems. Combustion of such coals obtained.
must be done in specially designed systems in 3. The sulphur removal increases with
order to minimize air pollution or else lignite increasing the temperature and reaches a value
should be converted to a semicoke product by of 63% at 650~
low-temperature coking. The optimum condi- 4. Coal undergoes fragmentation upon car-
tions established in this study is only valid for bonization process due to the removal of
fixed bed coking furnaces. The mode of coking moisture and volatile matter from coal. This is
and the dimensions of the furnace certainly strongly dependent on the particle size. As the
affect the time and temperature of the carboni- particle size increases the tendency for particles
zation process. to fragment increases and this in turn reduces
An important consideration from the view- the strength of coal. The strength can be
point of air pollution is the removal of tar in improved by briquetting of coal.
 D E S U L P H U R I Z A T I O N OF L O W - R A N K COALS 369

References GENTILE, R. H. 1995. Clean Fuel Technology: The

Contribution of K-Fuel. Proceedings of 3rd Coal
ASMATULU, R., ACARKAN, N., ONAL, G. & CELIK, Technology and Utilization Seminar, Cayirhan,
M. S. 1995. Upgrading of low-rank coals by low- Turkey.
temperature carbonization. Proceedings of Tech- KOPPELMAN, E. 1977. Process for Upgrading Lignite-
nologies for Mineral Processing, Baia Mare, type Coal as a Fuel. U.S. Patent 4.052,168,
Romania, 29-35. October 4, 1977.
CELIK, M. S. • SOMASUNDARAN,P. 1994. Desulfur- LOWRY, H. H. 1945. Low-Temperature Carbonization
ization of coal. In Kural, O. ed., Coal: Resources, Chemistry of Coal Utilization. Wiley, New York.
Properties, Utilization and Pollution, Kurtis Press, ONAL, G., MUSTAFAEV,I., ASMATULU,R., YILDIRIM,I.,
Istanbul, 253-269. ACARKAN,N. 8s CELIK, M. S. 1995. Desulphuriza-
COLE, E. L. & NESS, H. V. 1977. Treatment of tion of Turkish Lignites by Low temperature
Solid Fuels. U.S. Patent 4,018,571, April 19, 1977 Coking, ECOS'95, July 11-14, Istanbul, 640-645.
and U.S. Patent 4,052,169, October 4, 1977 SCIAZKO, M., KUBICA, C. & RZEPA, S. 1993. The
(Texaco). Smokeless Fuel-Properties and Testing Metho-
EKINCI, E. 1982. Production Methods of Metallur- dology. Fuel Processing Technology, 36, 123-128.
gical Coke and Smokeless Fuel and its Appli- VERSCHUUR, E. et al. 1976. Thermal Dewatering of
cation to Turkish Coals (In Turkish). Proceedings Brown Coal, U.S. Patent 3,992,784, November 23,
of International Coal Technology Seminar, 1976 (Shell).
127-137. VON, H. H. 1982. Thermich Veredelung Der Kohel
EVANS, D. G. & SIEMAN, S. R. 1979. Separation of mit Ausnahme von Kokereien Technische Mittei-
Water from Solid Organic Materials. U.S. Patent lunge 75. Jahrgang, Heft 2/3, p. 117-128.
3,552,031, January 5, 1979. WASH, E. J. 1977. Upgrading Subbituminous Western
FLEISSNER, H. 1927-1928. Drying of Coal. U.S. Patent Coal. Canadian Patent 1,020,477, November 8,
1,632,829,1927 and U.S. Patent 1,679,078, July 1977.
31, 1928. ZIELINSKI, H., KACZMARZYK, G., SCIAZKO, M. &
GAZANEER, S. 1983. Smokeless Fuel Experience of SECULA, M. 1992.2nd Int. Cokemaking Congress,
Seyitomer Lignites. International Coal Utilization London, 28-30 Sept. 1992, Inst. Mater., London,
Conference, Sept. 6-10, Istanbul. 551-554.
 Amelioration of high organic sulphur coal for
combustion in domestic stoves
M I C H A E L K. G. W H A T E L E Y 1, Z A F E R G E N C E R 2 & E R T E M T U N C A L I 2

1Geology Department, University of Leicester, Leicester LE1 7RH, UK

2 Directorate of Mineral Research and Exploration (MTA), Ankara, Turkey

Abstract" Despite the proximity to Ankara, raw coal mined in the Beypazari basin cannot
be used as a domestic fuel in Ankara because the high combustible sulphur content would
add to the already severe pollution problems in that city. This study investigated a method
of reducing the SO2 emissions by adding lime (CaO) to the coal prior to combustion.
Sorbent, as lime, was added to the combustion chamber (a domestic stove), by pretreating
the coal by mixing crushed coal with lime and molasses and turning the coal into briquettes.
Lime was added to lump coal for comparative purposes. The ratio of Cafree : S was varied for
a series of combustion tests, and the heating efficiency and the amount of sulphur fixed in
the ash were determined. The results of the tests show that optimum sulphur retention and
heating efficiency were obtained when the Cafree :S molar ratio was between 0.95 and 1.15
for the briquettes and between 1.00 and 1.25 for the lump coal. For lump coal, 50% of the
total sulphur could be fixed in the ash and at least 75% of the heating efficiency retained.
During combustion of the briquettes, at least 57.5% of the sulphur could be fixed in the
ash and at least 85% of the heating efficiency could be achieved. This suggests that the addition
of lime to briquettes may be a feasible way of reducing the SO2 emissions for domestic stoves.

Ankara, the capital of Turkey, has a population and nitrous emissions from these stoves creating
of around 3.25 • l06 people, most of whom rely an e n v i r o n m e n t a l hazard ( D u r m a z et al. 1993).
upon coal as a domestic fuel supply for cooking As m u c h as 0.8 M t of coal is b r o u g h t into
and heating. The climate is such that in winter A n k a r a from s u r r o u n d i n g areas a n d from out-
temperature inversion on the high level plateau side T u r k e y to supply the domestic market. As
(elevation 1500m) often traps the sulphurous far as is possible, low sulphur coals are used, but

{ ~ Miocene
Neogene sedimentaryunits
,t:t Jit:t:t:t t~~:t:[:t:l%, v v - v
Teke volcanics
:: : v v v Palaeocene{ ~ Kizil~zayGroup

,
9
i
: 9
V V Late Jurassic
F ret
: Taceous
:TTIc I~

l ~
Ophiolites
Nardin Formation
(flysch)
So'uk~ am
limestone
"~ "~ ~ " ~ ' ' (~aylrhan
"" "" "~ \ lignite field// + ~ + \ PalaeozoicI ~ Granite
% "" ,~, "~ "~)liKg~ unfa~'l~l-] I++
[ [-~'-] Mh;at;:~ics

0 lOkm

Fig. 1. Location of the Beypazari basin showing the position of the (~ayirhan lignite field and the main rock units
in the region (from Whateley & Tuncali 1995b, modified after Yagmurlu et al. 1988).

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 371-377.
372 M. K. G. WHATELEY E T A L .

most of Turkey's cheaply mined lignites have a desulphurization (FGD) plant, which effectively
high sulphur content. To alleviate this problem, removes 99% of the SO2 from the flue-gas.
low-sulphur coal is imported into Turkey from FGD is economic at this scale, but would
USA, South Africa, Italy, Colombia and Aus- probably be inefficient and not cost effective on
tralia, some of which is transported to Ankara. domestic stoves.
Importation and transportation costs result in This study was designed to determine whether
raised prices of domestic fuel. the Beypazari lignite could be beneficiated with
One potential source of lignite for the Ankara the addition of lime to the coal in order to
market lies in the Beypazari basin (Fig. 1), only reduce the SO2 emissions from domestic stoves
100 km NW of Ankara. Coal, of Miocene age, is to acceptable levels.
known in two areas of the basin, namely the
~ayirhan and the Koyunagili lignite fields
(Fig. 1). Coal from the (~ayirhan field only was Lignite characteristicas
used in this study. The (~ayirhan field contains
some 400 Mt of coal, which is currently mined to There are two separate lignite seams in the
supply a 300 MW thermal power station (TPS). (~ayirhan lignite field (Fig. 1). The lower lignite
Unfortunately, this lignite is characterized by seam was deposited in the lower part of the
high sulphur content (maximum 8.2% on an air ~oraklar Formation (Fig. 2). It has variable
dried basis), up to 75% of which has been shown thickness, is laterally impersistent and is of
to be combustible sulphur (Whateley & Tuncali very poor quality. It was not used in this
1995a). The TPS is fitted with a flue-gas study. The thicker, economically important,

AGE FORMATIONS LITHOLOGY

J __ Z __ - - - - 9
claystone,
~ Kirmk-rgormaation~ mudstone & gypsum
limestone

conglomerate, sandstone

-
claystone, mudstone,
fine-grained sandstone

Upper
Miocene silicified claystone
& limestone, chert
....... _ =i i --
HirkaFormation ' ~ .... --b ~'~ shale, bituminous shale,
Upper ligniteseam . . . . .... _.,--/ trona & tuff

(~oraklar Formation ~ ~(~ ~ Vv "E cross-bedded conglomerate,

9 0

o Lowerlignites e a m ~ ~ sandstone & mudstone

"~ "~ + > v

Metamorphics, ophiolites,
Pre- granites, limestones
Neogene f ~ Basementrock "'-'
% % & clastic sediments
~ + + +\ ".-, ",-, ,-,,_,
K-~-7~/ ~ , ) ~ ~ '-,..,,

Fig. 2. Schematic stratigraphic section of the ~ayirhan basin (from Whateley & Tuncali 1995b, modified after
Yagmurlu et al. 1988 and Inci 1991).
 AMELIORATION OF HIGH ORGANIC SULPHUR COAL 373

upper lignite seam was deposited at the top of Mineral matter chacteristics
the formation. It is laterally persistent and has a
reasonably uniform thickness of about 3.0 m. A The inorganic fraction of the raw coal, the
one metre thick, tuffaceous, siltstone parting, mineral matter, was examined using XRD and
with cherty nodules, splits the upper seam into SEM EDX analytical techniques. The major
two lignite beds, referred to as the first (Tv) and minerals present are the zeolites, analcime and
second (Tb) seams (Whateley & Tuncali 1995a) clinoptilolite, and pyrite, with variable amounts
Detailed descriptions of these two seams are of minor minerals such as gypsum, albite/
given by Whateley & Tuncali (1995a), who anorthite, marcasite, quartz, illite, dolomite
examined proximate and ultimate analyses, and apatite. Vertical variation between the top
calorific value, combustible sulphur and pyritic and bottom seams is recognized because of the
sulphur contents, palynological descriptions, almost exclusive presence of clinoptilolite in the
petrographic analysis, reflectance values and first seam, with minor amounts of analcime and
ash oxide analyses derived from coal samples almost exclusively analcime in the second seam,
collected from boreholes and underground mine with minor amounts of clinoptilolite. Most
faces. Reflectance measurements (Rmax [%]) Turkish lignites contain quartz, kaolinite, illite,
varied from 0.34 to 0.38, putting the coal into smectite and pyrite as the main minerals with
the lignite rank category. The first and second varying minor amounts minerals which include
seams are mined and mixed together for calcite, dolomite, hydromuscovite, feldspar,
combustion in the TPS and Table 1 gives the barite, celestite and marcasite. No other Turkish
average quality of both seams. lignite is known to contain the abundance of
zeolites found in this coal.
Table 1. Average values of the proximate, ultimate,
sulphur, calorific value and ash oxide analyses from the
upper seam in the Beypazari basin, Turkey
Ash characteristics
As received Air dried
results results When coal is burnt the inorganic residue is
referred to as the ash and is measured as a
Proximate analyses percentage of the original mass of the raw coal,
Moisture content (%) 23.38 9.00 either on an as received or air dried basis. The as
Ash content (%) 23.27 35.88 received ash content changes vertically both in
Volatile matter (%) 28.74 29.12 and between the first (Tv) and second (Tb)
Fixed carbon (%) 24.61 26.00 seams at Beypazari (Whateley & Tuncali 1995b).
Sulphur analyses The average ash content of the second seam is
Combustible sulphur (%) 2.52 3.81 27.4%, compared to the first seam which
Sulphur in ash (%) 0.84 0.77 averages only 19.2%.
Total sulphur (%) 3.38 4.58 The ashes were analysed by ICP-AES after
sample digestion. The oxide analyses were
Ultimate analyses
Carbon (%) 31.12 40.37 tabulated and correlation coefficients presented
Hydrogen (%) 2.39 2.98 by Whateley & Tuncali (1995a, Table 5). They
Nitrogen (%) 7.32 9.12 found that there was a strong positive correla-
Oxygen (%) 55.73 43.26 tions between CaO and SO3, of 0.84 and 0.87 in
Total sulphur (%) 3.44 4.27 the first and second seams respectively. This was
due to the anhydrite in the ash which developed
Calorific value
Calorific value (kcal kg- 1) during the combustion of the coal. The pyritic
2318 3391
and organic sulphur forms were oxidized and
Grindability index 64.21 the the SO2 combined with Ca found mainly in
the clinoptilolite, but also in the organic matter,
Ash melting point (~ 1250
to form the anhydrite. Whateley & Tuncali
Ash analyses (1995a) showed that an average of 28% of the
SiO2 (%) 41.99 total sulphur in the raw coal reported in the ash
A1203 + TiO2 (%) 16.32 in the first seam and 25% of the sulphur
Fe203 (%) 11.96 reported in the ash of the second seam. The
CaO (%) 8.71 remainder of the sulphur was reported as
MgO (%) 4.19 combustible sulphur, and was lost to the atmo-
Na20 (%) 4.95
K20 (%) 1.17 sphere as SO2.
SO3 (%) 9.30 Recent work has shown that the Beypazari
coal consists of the following forms of sulphur
374 M. K. G. WHATELEY E T AL.

(British Standard 1977), namely sulphate sul- and molasses. The Cafree:S molar ratio was
phur, 0.23%, pyritic sulphur, 2.34%, and varied for a series of combustion tests (Table 2).
organic sulphur 2.03%. The organic sulphur is The free Ca contained in the coal was not
contributing some 45% towards the total included in these ratios. A fixed mass of coal
sulphur. As more than 75% of the sulphur is (7kg) was burnt in each experiment and the
lost as combustible sulphur, this suggests that central grate and the flue gas temperatures were
the pyritic sulphur is contributing to the monitored continually (Fig. 3) and graphs of
combustible sulphur as well. The ASTM and these variations with combustion time were
British Standard tests for measuring the ash drawn (Figs 5 and 6). For clarity only the raw
content expect the coal to be ashed at between coal (L1 and B1) and the penultimate experi-
750 and 850~ At these temperatures pyritic ment (L5 and B5) are shown.
sulphur as well as the organic sulphur will The raw coal, both as lump coal and as
oxidize, resulting in the release of SO2. briquettes, burnt fiercely and within 25 minutes
It is apparent that the high sulphur coals in produced central grate temperatures as high as
Turkey that are used as domestic fuels, con- 1300~ The lump coal produced the highest
tribute to the SO2 emissions that are a major central grate temperatures, but the stove lost
factor in urban air pollution (Durmaz et al. heat rapidly. The briquettes retained their heat
1993). This project intended to establish whether longer (Fig. 4). In general there was not a great
a practical solution could be found whereby the difference in the combustion time between the
addition of Ca to the coal in forms other than lump coal and the briquettes in each experiment.
that found in zeolites and organic matter would As the Cafree :S molar ratio increased, so the
lead to a lowering of the SO2 emission from the time taken for both the lump coal and briquettes
Beypazari coals. to reach their maximum temperature increased,
e.g. 90 and 70minutes respectively in experi-
ment 5 (Fig. 4). The combustion time increased
Results of sorbent addition in the stove as the Carree:S ratios increased,
One of the most freely available forms of Ca is in
lime (CaO). Experimentation has shown (Gencer
1988) that in a domestic stove the coal burns at
an average temperature of about 780~
although the maximum may reach as high as
1300~ At these temperatures, sulphur is
released from oxidized pyrite and organic
material. The CaO reacts with the pyritic S
during combustion in the following way,
2FeS2 + 4CaO + 702 ~ 4CASO4 + 2FeO
resulting in capture of some of the sulphur as
anhydrite in the ash.
Sorbent, as lime, was added to the combustion
chamber (a domestic stove), firstly in briquettes
and secondly with the lump coal. The briquettes
were produced by mixing crushed coal with lime

Table 2. Cafree'S molar ratio used in the combustion

tests when lime was added to lump coal and briquettes of
Beypazari coal, Turkey

Briquettes Lump coal Cafree:S molar ratio

B1 L1 0 (no lime added)
B2 L2 0.50
B3 L3 0.75
B4 L4 1.00
B5 L5 1.50
B6 L6 2.00 Fig. 3. Photograph showing the domestic stove used in
the experiment.
 AMELIORATION OF HIGH ORGANIC SULPHUR COAL 375

1400 350 " '

1200 300

i 1000 o~ 250 Ls
800 ~ 200
B5
600 ~ 150
E L5 E

400t/t ~ 100
200 50
0 , '," , , L1, , 0 , , , , ,

0 25 50 75 100 125 150 175 0 25 50 75 100 125 150 175

Time (minutes) Time (minutes)
Fig. 4. Variations in the central grate temperature Fig. 5. Variations in the flue gas temperature with
with combustion time in a domestic stove burning coal combustion time in a domestic stove burning coal
from the Beypazari basin, Turkey. The graph shows from the Beypazari basin, Turkey. The graph shows
raw coal (L1 and BI) and coal mixed at a Cafree: S raw coal (L1 and B 1) and coal mixed at a Cafree: S
molar ratio of 1.5 : 1. molar ratio of 1.5:1.

e.g. up to 175 minutes in experiment 6 (Table 3). The flue gas temperatures decreased rapidly past
The average central grate temperatures ranged the maxima. As the Cafree:S molar ratio
from 924 to 506~ for the lump coal and increased, so the time taken for the lump coal to
between 856 and 702~ for the briquettes. reach its maximum temperature increased, e.g. to
There is no clear pattern to be seen in the grate 125 minutes in experiment 5 (Fig. 5). The flue gas
temperatures to compare the different fuel types, temperatures were raised rapidly when the
except that in general, the average central grate briquettes were burnt in experiment 5 (Cafree :S
temperatures decreased as the Cafree:S ratios ratio of 1.5:1), but the temperature dropped
increased (Table 3). more slowly past the maximum. In general, there
The flue gas temperatures increased rapidly was very little change in the average flue gas
to maxima of around 310~ when raw coal was temperatures as the Cafree:S ratio increased
burnt both as lump coal and as briquettes (Fig. 5). (Table 3). The average flue gas temperatures

Table 3. Results of combustion tests in a domestic stove for a series of Beypazari lignite (L) and
briquette (B) samples burnt with various amounts of lime (see Table 2)

Average temps Heat losses (%)

Sample Combustion time Stove Flue Heat loss Heat loss Heat loss Thermal Sulphur
No. (mins) grate gases by flue due to in grate efficienty fixation
gas CO in (%) (%)
flue gas

L1 105 790 200 21.76 7.69 4.94 65.6 20.7

L2 120 894 215 27.00 10.25 4.87 57.9 36.5
L3 130 798 215 30.29 4.27 6.94 58.5 40.8
L4 150 924 210 30.30 7.12 7.82 54.7 50.3
L5 170 793 215 35.25 3.42 21.00 40.3 59.1
L6 175 506 214 38.00 11.00 12.00 39.0 60.6
B1 145 856 205 25.50 5.78 0.63 69.1 20.9
B2 135 827 217 26.90 7.35 2.90 62.8 43.7
B3 140 833 224 29.80 5.30 4.20 60.7 52.5
B4 150 724 220 30.50 2.60 6.60 60.3 53.6
B5 160 736 225 33.60 6.00 3.20 57.2 63.7
B6 175 702 227 36.50 11.30 5.60 46.6 69.3
376 M. K. G. WHATELEY E T AL.

70 70
y=22.699x + 25.078 ./,,~~,,~
60 r = 0 . 9 4 7 8 ~ _ _ -
50-
~ 55" y=20.44 + 2s.078

= 50- y=-14.442x + 66.507 " ~ . ~ 40- r=0.9629 _

I--'c:45"
~ r-'-0"9843 ~ ~ ' ~ 30"
-3
f~ 20-
40 [] Lump coal samples
03
9 Briquette samples
10
35

3O
0 0.25 015 0.:75 i 1.25 1~5 1.75 2 o o.;,s ols o. ,s i 1.i,s lls 1.?s 2
Cafree :total S molar ratio Cafree:total S molar ratio

Fig. 6. Variations in the thermal efficiency of a Fig. 7. Variations in the sulphur retention in the ash
domestic stove burning coal from the Beypazari basin, plotted as a percentage of the total sulphur content of
Turkey, with respect to the Carree : S molar ratios of the the raw coal from the Beypazari basin, Turkey, with
various feeds. respect to the Carree : S molar ratios of the various feeds.

measured when the briquettes were burnt were, added both to the lump coal (from 21% to 37%)
on average, some 5 to 10~ higher than those and briquette fuel (from 21% to 44%). In both
measured when lump coal was burnt. fuel types the rate of sulphur retention in the ash
By measuring the temperatures in the grate slows beyond the 1.5:1 Carrel: S ratio. In all
and flue gases it was possible to calculate the cases the amount of sulphur retained in the ash
heating efficiency of the central stove during was greater when the lime was mixed with the
each experiment (Table 3 and Fig. 6). With the coal as briquettes.
addition of lime to the stove fuel, the heating
efficiency dropped markedly at the low Cafree : S
molar ratio of 0.5:1 (Fig. 6). The lump coal
dropped from 66% efficiency with raw coal to
Discussionof results
58% and briquettes dropped from 69% to 63% The time taken to reach the maximum tempera-
efficiency. Thereafter the rate of change slowed ture in the grate and in the flue gases increased
between ratios 0.5 : 1 and 1:1. At these ratios, the as the Carree :S molar ratio increased (Figs 4
variation in efficiency was between 58 and 55% & 5). The maximum temperature reached is
for lump coal and between 63 and 60% for the lower as the ratio increases. The high sulphur
briquettes. As more lime was added with the content of the coal meant that lime had to be
lump coal (1.5:1 ratio) the heating efficiency added in large proportions. This resulted in
dropped rapidly to 40%. A similar effect was reduced operating temperatures (Fig. 4) and a
seen with the briquettes, although the drop in reduced heating efficiency (Fig. 6). There is an
heating efficiency was less noticeable at the 1.5:1 immediate loss of heating efficiency as soon as
ratio (57%). The final heating efficiency lime is added to the coal, but between the 0.5:1
recorded was 47%. and 1 : 1 ratio of Cafree : S there is no significant
The ash was analysed for total sulphur change in loss of heating efficiency. This suggests
content and this was reported as a percentage that there is no additional benefit to be gained
of the total sulphur in the raw coal (Table 3 and by increasing the ratio of Carrie : S to more than
Fig. 7). This figure reflects the amount of 1:1 as far as heating efficiency is concerned.
sulphur retained in the ash. Graphs of sulphur Sulphur retention increased from a base level
retention plotted against Carr~ :S molar ratios of 21% when no lime was added to over 60%
(Fig. 7) show a rapid increase in the amount of when the Carrer : S molar ratio was 2:1 (Fig. 7).
sulphur retained in the ash immediately lime was The retention of sulphur in the ash when raw
 AMELIORATION OF HIGH ORGANIC SULPHUR COAL 377

coal is burnt and no lime is added is a function The authors wish to acknowledge their colleagues and
of the presence of the clinoptilolite/heulandite the Director at MTA, Ankara and their colleagues in
zeolites. The effect of the addition of lime was an the Geology Department, University of Leicester who
immediate increase in the amount of sulphur provided technical and scientific support during the
project. They would also like to thank the Director of
retained in the ash. The rate of retention
TKI, Ankara who gave permission for access to the
remained high between a 1: 1 and 1.5 : 1 ratio, coal site and the management and staff at the (~ayirhan
thereafter the retention rate slowed. This sug- mine for their assistance during the collection of the
gests that there is no particular gain in sulphur samples. Considerable help was given by Professor A.
retention beyond the 1.5 : 1 ratio of Carree : S. Spears and Dr X. Querol, who read and commented
From Figs 6 and 7 it can be concluded that on earlier versions of this manuscript. Their help is
the optimum sulphur retention and heating very much appreciated.
efficiency were obtained when the Cafree: S
molar ratio was between 1.00 and 1.25 for the
lump coal and between 0.95 and 1.15 for the References
briquettes. At these ratios for lump coal, 50% of BRITISH STANDARD1997. Analysis and testing of coal
the total sulphur could be retained in the ash and coke, Part I1, Forms of sulphur in coal,
and at least 75% of the heating efficiency BS1016, part 11.
achieved. During combustion of the briquettes, CHINCHON, J. S., QUEROL, X., FERNANDEZ-TURIEL.
at least 57.5% of the sulphur could be retained J. L. & LOPEZ-SOLER, A. 1991. Environmental
in the ash and at least 85% of the heating impact of mineral transformations undergone
efficiency could be achieved. The added advan- during coal combustion. Environmental Geology
tage of the reduced operating temperatures of and Water Science, 18, 11-15.
the stove once lime was added with the coal is DURMAZ, A., DOGU, G., ERCAN, Y. & SIVRIOGLU,M.
1993. Investigation of the Causes of Air Pollution
that the anhydrite in the ash would be more
in Ankara and Measures for its Reduction. NATO
likely to be retained in the ash and not broken Science for Stability Program.
down. Chinch6n et al. (1991) have shown that GENCER, Z. 1988. An Investigation of Methods for
anhydrite is stable up to temperatures of Fixation with Lime of Sulfur Dioxide Formed by
1060• 10~ beyond which anhydrite decom- the Combustion of Ankara-Beypazari Lignites.
poses into CaO and SO2. MSc thesis, Gazi University.
This study showed that significant reduction INCI, U. 1991. Miocene alluvial fan-alkaline playa
of the SO2 emissions could be obtained with the lignite-trona bearing deposits from an inverted
addition of lime to the raw coal which, during basin in Anatolia: sedimentology and tectonic
controls on deposition. Sedimentary Geology, 71,
combustion, would convert some of the SO2
73-97.
derived from oxidation of pyritic and organic WHATELEY, M. K. G. & TUNCALI, E. 1995a. The
sulphur in the coal into anhydrite in the ash. At origin and distribution of sulphur in the Neogene
the optimum Cafree : S molar ratios there was no Beypazari lignite basin, Central Anatolia, Turkey.
significant reduction of the heating efficiency of In: WHATELEY,M. K. G. & SPEARS, A. (eds)
the coal. The briquettes proved to be slightly European Coal Geology. Geological Society,
more thermally efficient and retained a greater London, Special Publication, 82, 307-323.
proportion of the sulphur in the ash than the & - - 1 9 9 5 b . Quality variations in the high-
lump coal and lime mixture. This suggests that sulphur lignite of the Neogene Beypazari Basin,
Central Anatolia, Turkey. International Journal of
by pretreating the Beypazari coal by crushing
Coal Geology, 27, 131-151.
and mixing the coal with lime and molasses to YAGMURLU, F., HELVACI, C. & INCI, U. 1988.
form briquettes for use as a domestic fuel, the Depositional setting and geometric structure of
SO2 emissions can be reduced without signifi- the Beypazari lignite deposits, Central Anatolia.
cantly reducing the heating efficiency of the fuel. International Journal of Coal Geology, 10, 337-360.
 The use of pulverized lignite/natural gas mixed fuels in the
high-temperature process of a cement rotary kiln
M. bIANOJEVIC', (5. JANKES', M. K U B U R O V I C ' ,
M . S T A N O J E V I C 2 & P. B L A G O J E V I ( ~ 2

1Faculty of Mechanical Engineering, University o f Belgrade, 27 marta 80,

11000 Belgrade, Yugoslavia
2 Beodin Cement Factory. Beodin, Yugoslavia

Abstract: This paper presents the results of industrial tests of low grade lignite combustion
in the 500t/day wet-process rotary cement kiln. For the use of pulverized lignite, the
following process characteristics are determined: combustion process parameters, flue gas
properties, and the influence of coal ash properties on clinker quality. Industrial tests have
shown that it is possible to substitute 50-80% of the natural gas with pulverized low-grade
lignite, while the output of the kiln, specific heat consumption, and the quality of cement
clinker remain unchanged.

The cement industry faced an increase in the step is performed in drying plants (near the open
prices of liquid and gaseous fuels used for coal fields) and the second in the factory's
clinker production after the energy crisis of drying-grinding plant. The coal ash remains
1973. This was the reason for the increasing as part of the clinker material, thereby reducing
introduction of coal as a fuel, which is the the amount of raw material. The chemical
dominant fuel in the West European cement composition and ash content of coal determine
industry today. Anthracites and other high- the necessary corrections in the raw material
quality coals are commonly in use. used for the required cement clinker quality to
The introduction of precalcination in new be achieved.
cement production technologies has enabled the
use of low-grade fuels, such as soft brown coal.
Soft brown coals (lignites) are the main energy Table 1. Production process parameters for cement
resource in Yugoslavia, and it was of great rotary kiln in Beodin cementfactory
importance to determine the conditions for their
use in cement rotary kilns. The investigation Nominal kiln output t/day 500
Range of output t/day 450-520
focused on determining all the necessary process kg/m 3h 15-17.2
Specific kiln output
parameters and technical limitations for the use Kiln dimensions:
of 'Kolubara' lignite. length (L) m 135
This paper presents the experimental results of shell diameter m 3.6-4.0
mixed lignite/natural gas fuel combustion for length-to-diameter ratio - 35
cement production, in a wet-process rotary kiln (L/D)
(in the 'Beo6in' cement factory). Inner volume m3 1260
Inclination % 4
Speed of the kiln rpm max. 1.2
Internal heat exchangers
Process and experimental details
(chain curtain):
The coal usually used in the cement industry length m 20
surface m2 1400
should comply with the following requirements m 2.6 x 14.9
Clinker grate cooler (Follax)
(Duda 1976): Fuel natural gas/
LHV: rain. 21 (MJ/kg) pulverized coal
Specific heat consumption kJ/kg el. 6000-6700
Ash content: 12-15 (wt%) ~ 550-600
Secondary air temperature
Volatile matter: 18-22 (wt%) Flue gas temperature ~ 150
Moisture content: up to 12 (wt%) as Outlet clinker temperature ~ 50
delivered. Flue gas dust content % 1.5
(% of raw material
The high moisture content of Yugoslav lignites consumption)
(up to 50%) requires two-step drying. The first

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 379-383.
380 M. STANOJEVI(~

Experiments were performed in the wet- material balance includes the following process
process rotary kiln in the 'Beo6in' cement parameters: consumption of natural gas, pulver-
factory. Technical data and process parameters ized lignite, and raw material slurry; natural gas
of this plant are shown in Table 1. The scheme composition; flue gas composition; raw material,
of the clinker production plant used for indus- dust, and cement clinker composition; original
trial tests is shown in Fig. 1. The plant consists and pulverized coal composition; dust concen-
of the following parts: wet-process rotary kiln tration in flue gas; flow of hot air for the tube
with combined fuel burner (for pulverized coal ball mill; primary air flow; moisture flow
and natural gas), a clinker grate cooler, and a separated from coal.
tube ball mill with a direct coal-drying system. Four industrial tests were carried out. The aim
The plant was originally designed for use with was to determine the influence of the coal/
high quality coal. natural gas ratio on the clinker production
The material balance scheme for this kiln is process. The quality and grain size of 'Kolubara'
shown in Fig. 2. The mathematical model of the dried lignite were different in each test. The

,-~ po21 to2ii~:o21k.~_

~01 l~

Fig. 1. The scheme of clinker production plant and the locations of measuring points. 1, rotary kiln; 2, grate
cooler; 3, flue gas chamber; 4, flue gas fan; 5, chimney; 6, burner; 7, chain curtain

VVA'IERVAI=,~
8EPARA'TEI:>
I=ROMr DU6T IN
FLLE~ A
I~. MILL
X=-
l
~ - - J

ROTARY KILN

I CLINKER ~-
r'~ COOLER
r r

AIR
Fig. 2. The material balance scheme of the wet process rotary kiln.
 P U L V E R I Z E D L I G N I T E IN C E M E N T R O T A R Y K I L N 381

m e a s u r e m e n t of characteristic parameters in The table shows that the moisture content of the
each test was carried out in steady-state condi- original coal varied from 28.5 to 30.5 w t % while
tion, which lasted a m i n i m u m of 6 to 8 hours. L H V varied between 13.7 and 15.7 MJ/kg. The
Seeing that the material remains in the kiln ash c o n t e n t in tests a b, a n d c where coal with
for a b o u t 2.4 hours the m e a s u r e m e n t periods particle size of - 15 + 0 m m a n d - 15 + 5 m m
were long e n o u g h to provide reliable data on the was used, turned out to be 9.8 to 13.8wt%; in
kiln operation. test d, using coal with a particle size o f
- 5 + 0 m m the figure was 1 8 . 4 w t % . The moist-
ure content o f the pulverized coal in tests a b,
and c r a n g e d from 12.1 to 1 2 . 4 w t % . In test d the
Results o u t p u t of the coal mill was reduced due to the
use of lower-quality coal, which resulted in a
The quality of the coal used in the experiment is moisture content of 9.8 w t % . The L H V of the
presented in Table 2. F o r each test, the table pulverized coal was r o u g h l y the same in the
gives data a b o u t the proximate and ultimate samples p r o d u c e d by tests a and d i.e. 18.2MJ/
analyses of coal as it enters the mill and of kg, for test b it was 19.3 MJ/kg, and for test c it
pulverized coal as it enters the b u r n e r of the kiln. had the highest value - 19.85 MJ/kg.

Table 2. Coal properties

Industrial test in roatry kiln: a b c d

Coal size distribution - 15 + 5 mm -15+0mm -15+5mm -5+0mm
(tube ball mill inlet)

Ultimate analysis of coal:

Carbon C wt% 38.61 40.14 41.92 36.84
Hydrogen H wt% 3.18 3.31 3.55 2.92
Oxygen O wt% 13.91 14.51 15.47 11.83
Nitrogen N wt% 0.54 0.35 0.54 0.44
S. comb. S wt% 0.31 0.36 0.22 0.32
Proximate analysis of coal:
Moisture wt% 30.45 29.54 28.50 29.27
Ash wt% 13.00 11.79 9.80 18.38
S. total wt% 0.90 0.89 0.73 0.96
S. in ash wt% 0.59 0.54 0.51 0.64
S. comb. wt% 0.31 0.35 0.22 0.32
Coke wt% 38.09 38.16 37.01 44.14
C~ wt% 25.10 26.37 27.20 25.77
Volatile wt% 31.46 32.30 34.49 26.59
Combustible wt% 56.56 58.66 61.70 52.36
Low heat value kJ/kg 14 342 14954 15 717 13 698
Ultimate analysis of pulverized coal:
Carbon C wt% 48.64 50.10 51.41 47.10
Hydrogen H wt% 4.01 4.13 4.35 3.73
Oxygen O wt% 17.52 18.11 18.97 15.12
Nitrogen N wt% 0.68 0.44 0.67 0.56
S. comb S wt% 0.39 0.43 0.27 0.41
Proximate analysis of pulverized coal:
Moisture wt% 12.39 12.07 12.31 9.59
Ash wt% 16.37 14.72 12.02 23.49
S. total wt% 1.13 1.11 0.89 1.23
Coke wt% 47.98 47.62 45.39 56.42
Cfax wt% 31.62 32.90 33.37 32.94
Volatile wt% 39.63 40.31 42.30 33.99
Combustible wt% 71.24 73.21 75.67 66.93
Low heat value kJ/kg 18 171 19284 19845 18209
382 M. S T A N O J E V I C

Table 3. Rotary kiln process parameters

Industrial test in rotary kiln: a b c d

Coal size distribution (tuble ball mill inlet) -15+5mm -15+0mm -15+5mm -5+0mm

Pulverized coal
Low heat value kJ/kg 18 171 19 284 19845 18209

Natural gas
Low heat value (at ~ kJ/m 3 35466
Raw material slurry
Moisture content % 43.32 44.62 44.70 44.00
Specific consumption kg/kg cl. 2.7850 2.8546 2.8678 2.8234
Consumption t/h 58.82 58.63 57.36 60.00

Dry raw material

Ignition loss % 34.01 34.11 34.32 34.12
Specific consumption kg/kg cl. 1.5785 1.5809 1.5859 1.5811

Clinker
Production t/h 21.12 20.54 20.00 21.25
Fuel consumption
Natural gas ma/h 1741 1323 714 1396
m 3/kg cl. 0.0824 0.0644 0.0357 0.0657
Pulverized lignite kg/h 3390 3918 4768 4245
kg/kg cl. 0.1605 0.1907 0.2384 0.1998
Specific energy consumption
In natural gas kg/kg cl. 2922 2 284 1266 2330
In pulverized lignite kg/kg cl. 3004 3 678 4731 3637
Total kg/kg cl. 5926 5962 5997 5967

Natural gas/pulverized lignite ratio

Natural gas % 49 38 21 39
Pulverized lignite % 51 62 79 61

Table 4. Cement clinker properties

Industrial test in rotary kiln: referent a b C d

Natural gas/pulverized lignite ratio 100/0 49/51 38/62 21/79 39/61

Mineralogical composition:
3CaO.SiO2 wt% 66.66 51.23 66.11 50.35 67.28
2CaO.SiO2 wt% 15.26 32.76 15.90 29.88 16.82
3CaO.A1203 wt% 3.76 2.93 5.99 5.18 3.50
4CaO.A12OyFezO3 wt% 11.02 9.05 9.50 11.29 10.98

Oxides content:
ignition loss wt% 0.6 0.4 0.52 0.33 0.34
SiO2 wt% 20.77 21.05 21.10 21.15 21.25
A1203 wt% 5.67 5.67 5.93 5.80 5.80
Fe203 wt% 3.45 3.45 3.45 3.45 3.45
CaO wt% 66.36 65.80 65.66 65.65 66.22
MgO wt% 2.13 2.13 2.13 2.13 2.13
free CaO wt% 0.54 0.84 0.69 1.08 0.72

Characteristic modules:
hydraulic module (HM) - 2.22 2.18 2.15 2.16 2.17
aluminate module (AM) - 1.64 1.64 1.72 1.68 1.68
silicate module (SM) - 2.28 2.30 2.25 2.28 2.29

Bulk density kg/m 3 1428 1383 1398 1388 1502

 PULVERIZED LIGNITE IN CEMENT ROTARY KILN 383

Rotary kiln process parameters determined in During the experiment the natural gas sub-
industrial tests are given in Table 3. It is shown stitution ratio was 50-79% of total energy
that the energy from coal in total energy without affecting clinker production. The use
consumption for all industrial tests was 50 to of pulverized lignite did not affect specific energy
80%. The factors limiting the substitution of consumption in the clinker production process.
gas by coal were: a decrease in temperature in This could lead to the conclusion that the main
the kiln sintering zone, and the output of the process features, such combustion quality, heat
coal mill. transfer, and kiln output remained within the
In order for the required clinker quality to be limits which did not influence the overall kiln
maintained, it is necessary to have a temperature production process.
of 1550~ to 1650~ When only natural gas was Higher substitution of natural gas with
used, the mean temperature was around 1600~ pulverized lignite was not possible during the
dropping to 1540 to 1590~ in tests with coal, industrial experiments. The main reason was the
i.e. the maximum temperature drop was 60~ insufficient output of the tube mill and the
In tests a b, and d the degree of substitution of pneumatic transport system which had been
natural gas by pulverized coal was determined constructed for the use of high-quality coal.
by this maximum drop in temperature. In test c The results of the described experiment have
the quality of pulverized coal was such that the shown that high-quality coal is not the only solid
degree of substitution reached (79%) was not fuel utilisable in clinker production, and that
accompanied by a drop in temperature below there is a future for carefully pretreated low-
the above limits. However, a higher degree of grade lignite as the main fuel for the Yugoslav
substitution was impossible to attain due to cement industry. The same is possible for other
limitations in the mill's output. coals of similar quality.
Specific energy consumption and the rotary
kiln output shown in Table 3 were roughly the
same in all tests. They were similar to mean References
values attained when only natural gas is used.
Table 4 shows clinker quality (as defined by DUDA, W. 1976. Cement Data Book. Bauverlag
GmbH, Wiesbaden and Berlin, 279-283.
mineralogical composition, bulk density, free
PERKOVlC, B., STANOJEVIC, M., DOKI~, S. 1994.
CaO, characteristic modules) for all coal tests Industrial Tests of Substitutions of Anthracites
and the test which used only natural gas. All with Dry Pulverized Lignite 'Kolubara' in Cement
parameters indicate that clinker quality in coal Factory Beo(in, Final Report. Mining Institute,
test remained unchanged compared to the Beograd, Faculty of Mechanical Engineering,
natural-gas test. Beograd.
STANOJEVI(~, M. & KARAN, M. 1994. The Use of
Yugoslav Solid Fuels (Lignites) in Rotary Kilns in
Cement Industry. International Conference
'Energy for industry '94', Beograd, Proceedings,
Conclusion 218-223.
, PETROV,A. & KUBUROVId:,M. 1993. Influence of
The industrial tests of drying and grinding of lignite 'Kolubara' properties on the production of
lignite were performed in the factory's existing pulverized lignite. Termotehnika, Beograd, XIX,
tube ball mill, and the pulverized lignite, 1-2, 55-64.
together with natural gas, was used in the VULETII~,g. 8r STANOJEVIC,M. 1987. Possibilities and
500 t/day wet-process rotary kiln. conditions for the use of lignite 'Kolubara'.
Mining Journal, Beograd, 1, 64-67.
 The possibility of underground gasification of
Bulgarian Dobrudja's coal
DOUCHKO DOUCHANOV & VENECIA MINKOVA

Institute of Organic Chemistry, Bulgarian Academy of Sciences,

Acad.G.Bonchev str., bl.9, 1113 Sofia, Bulgaria

Abstract: The gasification of coal within underground coal seams and using the combustible
gas as a fuel is an idea that has attracted scientists for many years. Some success in gasifying
thick coal seams near the surface has been demonstrated in recent experiments in the USA.
Tests on underground coal gasification in Belgium and France have been carried out
supported by the Energy Commission of the European Communities since 1978. The latest
tests at Thullin, Belgium carried out by a joint Belgium and German team are thought to be
promising. The depth of the seams has been selected as representative of Southern European
and some Mid-European coals as an essential first attempt before moving to a further stage,
at around 900-1000 metres depth. Work on this programme is at an early stage and its
progress will be watched with much interest. For Bulgaria it is of vital importance to develop
underground coal gasification on Dobrudja's coal (1.5 109 t ) - as an important energetic
strategy and the possibility of environmental utilization of this resource.

The first tests on underground coal gasification following composition: CO, 13.4%; He, 13%;
(UCG) were performed in 1912. They were CO2, 11.8%; CH4, 3.6%; CnHm, 0.1%; 02, 0.2%;
followed by a number of tests in the former H2S, 0.01%; N2, 57.9%.
USSR and France. However, these attempts on The U C G station at Shatsky, built in 1959
U C G were discontinued due to the low calorific (lignite seams of 2.9 m thickness, lying at a depth
value of the gas produced and the difficult control of 40m), has produced 200 x 106 m 3 gas/year at
on the combustion processes and the chemical a calorific value of 800 kcal/m 3. Initially this gas
reactions in the underground gas generator. After was used mainly for local plants after which it
the experiment carried out in Gorlovka (1932), was employed to drive two 1 2 M W turbo-
the former USSR re-commenced the U C G tests. alternators in an electricity power station.
Following the completion of the test period, at The station at Angren is situated on lignite
the end of the 1950s, a series of U C G stations was coal seams that are 20m thick, at a depth of
built in: Tula (130kin south of Moscow), l 1 0 - 1 5 0 m and dipping at 30 ~ The area of the
Yushno-Abinsk (Kuznets mine basin, Siberia), coal deposit is 150 km 2 and the coal ash is 11%.
Shatsky (80 km southeast of Tula) and Angren The station has produced 600-800 x 106 m 3 gas
(120kin southeast of Tashkent). These stations at a calorific value of 700-800 kcal/m 3. The gas,
were designed to use lignite coals. The U C G whose composition was: CO, 5.6%; H2, 15.2%;
installations at Lisichansk (Donets basin) and C02, 19%; CH4, 2.5%; CnHm, 0.2%; O2, 0.5%;
Kamenskaya (130 km from Rostov) operated in H2S, 0.4%; N2, 56.1.% (Lavrov et al. 1971) was
bituminous and anthracite coals. The gas station used mainly for electricity generation in a
at Tula operated in lignite coals in horizontal 200 M W power-steam station.
seams between 0.3 and 5 m thick, lying at a depth The station at Kamensky(Rostov) has oper-
of 50m. In 1958 a total of 400 x 106m 3 of low ated in coal seams dipping at an angle of 40-50 ~
calorific gas (750-850 kcal/m 3) was produced. Its with a gas production rate of 2 x 106 m3/day at a
composition is as follows: CO, 5.5%; H2, 13.5%; calorific value 900kcal/m 3 and that at Lisi-
CO2, 17%; CH4, 1.6%; CnHm, 0.2%; O2, 0.5%; chansk has operated in coal seams which are
HzS , 1.0%; N2, 60.7%. 0.5-1 m thick, with a dip of 30-40 ~ and a gas
The seams developed in Yushno-Abinsc were production rate of 100-120 x 106m3/year at a
8-22 m thick at a depth of 250 m and with a dip calorific value of 850 kcal/m 3 (Skafa 1960). The
of about 45-70 ~ (Antonova et al. 1967). In this stations at Yushno-Abinsk and Angren were the
installation a total of 100 x 106 m3/year gas at a only ones remaining in operation after 1980.
calorific value of 1000 kcal/m 3 was produced and Parallel to the experiments on U C G in the
it is known that about 700 engineers and 3000 former USSR in 1945-1965, tests in USA,
technicians were involved in its production in England, Belgium, Poland, Czechoslovakia
1957. The gas produced is characterized by the (Prasek & Koranda 1989), in the Tatabanya

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geologyand Technology,
Geological Society Special Publication No. 125, pp. 385-390.
386 D. DOUCHANOV & V. MINKOVA

mine in Hungary during 1979-1980 (Szechy et al. steam-powered stations, and thirdly the UCG
1988), Italy, Japan and Morocco (Djerada, tests carried out in the Reno Junction, Wyoming
1947-1950) were carried out. The tests per- by the Atlantic Richfield Company (ARCO).
formed in England (Newman Spinney 1949)
and in USA-Gorgas, Alabama (1946-1958)
gave the most promising results.
In USA the development of underground coal The present UCG situation in Europe
gasification is considered as a prospective trend.
Taking into account the fact that the coal In Northern Belgium, between the Campine
reserves of USA amount to 87% of the mineral Basin and the border with Holland the hypothe-
resources, the eventual realization of UCG could tical coal reserves amount to 15-20 gigatonnes
increase almost threefold the exploitation of the which is equal to the total amount of coals
coal reserves. The oil crisis in the 1970s has produced in Belgium for the last 150 years. The
initiated again experiments on UCG in USA. German geologists consider that coal reserves in
The Energy Center of USA undertook gasifica- the Ruhr lying at a depth of 1200 m and those
tion experiments in Hanna, Wyoming to test the at a depth up to 5000m are 10 and 1000
possibility of underground gasification of 10m gigatonnes, respectively. Holland possesses
thick subbituminous coal seams, lying at a depth 1500 gigatonnes coal resources, with the major-
of 120 m. The coal permeability in the seams was ity of them lying at a depth of 1500-3000 m.
enhanced by hydrofracturing. In 1973 a total of On the basis of preliminary studies of the
0.24 x 10 6 m 3 gas/day was produced using air as National Mine Institute (NMI)-Belgium and
a gasification agent. A team at the Energy those of Professor Wenzel from AIX University
Center-Laramie has carried out UCG tests in in Germany a joint project between Belgium and
Hanna for 55 days. The gas composition Germany was agreed in 1986. In Thullin
in vol% is as follows: H2, 17.3; CO, 14.7; (Belgium) UCG tests were carried out at
C02, 12.4; CH4, 3.3; C2H4, 0.6; 02, 0.5; HzS, 0.1; depths of 860 m. Air was used as a gasification
N2, 51.0; At, 0.6. The Lawrence Livermore agent in the underground gas generator and a
Laboratory at Wyoming has performed a low calorific generator gas was produced. The
number of tests on UCG in seams that are utilization of oxygen-steam mixture at a pres-
15 m thick, at a depth of 150-900 m by applying sure of 10-20 MPa yielded a product with mean
a steam-oxygen mixture feeding. The gas C H 4 content (32.6% without N2). This content
production rate was 5 x 104 m3/day at a calorific is two times higher than that obtained in the
value of 2350 kcal/m 3. The Morgantown Energy pilot installation 'Ruhr-100' of the Lurgi Com-
Technology Center (METC) has carried out pany, Germany. Thus after CO removal the
underground gasification on 2m thick bitumi- calorific value of the gas has attained a value
nous coals, at a d e p t of 275 m, in West Virginia similar to that of natural gas.
(Strickland 1977). The gas production rate was Figure 1 shows the principal scheme of
0.1 x 10 6 m 3 at a calorific value of 1100 kcal/m 3. operation of this installation. The air supplied
It should be noted that this experiment has a by compressor 2 enters the basic seam layer
dual importance. On the one hand, the reserves through the pressure hole 3; the low calorific gas
of bituminous coals amount to 817 gigatonnes produced by UCG, is released through the outlet
and on the other, about 30% of these reserves hole 4. The latter is cooled to protect it from
are found at a great depth. In addition the excessive increases in temperature and a water
majority of these reserves are highballast and steam is produced simultaneously as a result of
their exploitation by deep mining would result in the heat of the removed gas. The low calorific
serious environmental problems (Clean Act, gas reaches the surface at high pressure with a
USA, 1970). These experiments on U C G in the temperature of about 250-300~ after which it
United States should be supplemented by three is washed in scrubber 5 before its inlet into the
additional tests. Firstly, he results obtained by combustion chamber of the steam generator 6.
the Los Alamos Scientific Laboratory (LASL) in The gasification of the base coal layer yields a
the Fruitland mines (New Mexico) on the high calorific gas (grison) which is contained in
separate runs of the two processes accompany- the upper layers.
ing UCG, i.e. pyrolysis and semicoke gasifica- In the programme described above the
tion in different areas of the mine, aimed at following partners participate: from Belgium-
reaching an optimal control on the processes. The Geological Department at Brussels, the
Secondly, the UCG performed by the Basic Department of Chemical Engineering at the Uni-
Resources Inc. in Fairfield (Texas), following a versity of Liege, the Mining Department at
Soviet pattern, in order to build two 20MW Mons Polytechnic, Distrigaz, Brussels; from
 REVIEW OF HISTORY OF UNDERGROUND COAL GASIFICATION 387

Ai~ Ex h~ ~,~////////////////"

'/.--6
5; E
- - O

:-_ ,--

.z

"///t~//////-///z///~'~
O

,r-

i g:

Fig. 2. Scheme of UCG carried out in Pas-de-Calais,

France: 1, existing mine gallery at a depth of 1000m;
2, injection hole; 3, internal hole diameter (60 ram);
4, external hole diameter (110ram); 5, closing valve;
6, gas removal hole; 7, coal seam; 8, metal grid;
9, intrusion of water under 800 bars pressure.
Fig. 1. Scheme of UCG carried out in Thullen,
Belgium: 1, motor; 2, compressor; 3, injection hole;
4, gas removal hole; 5, scrubber for low calorific gas removal) at a depth of 170m, separated by
purification; 6, steam boiler with combustion chamber;
7, alternator; 8, turbine; 9, heat-exchanger; 65m drilled in a 1.2m thick coal seam. The
10, condensation vessel; 11, pump; 12, grison outlet; experiment proceeded in the following stages:
13, scrubber for high calorific gas purification: first, water injection (hydrofracturing) at a
14, coal seams. pressure of 100-300 bars, followed by air
feeding for expansion of the hole, in the third
stage electrocombustion is carried out and in the
Germany - Rheinisch-Westfalische Technische last stage oxygen is supplied to produce a
Hochschule (AIX), Saarberg-Interplan (Saar- substitute of the natural gas (SNG) (Fig. 2).
brucken), Bergbau-Forschung GmbH (Essen- The very first objective of the Belgium and
Kray), Messerschmitt (Munchen). French projects was to produce a low calorific
England and the former USSR were among gas for electricity generation. Further it was
the first to show great interest in development of aimed to produce a gas at a calorific value of
UCG. Thus after a 30 years interruption the 2600kcal/m 3 which after concentration could
National Coal Board undertook in Newman substitute for the imported natural gas (SNG)
Spinney (1949) the production of gas by UCG with a calorific value of 9500 kcal/m 3.
for electricity generation in a 100-200MW In Bulgaria, since the discovery of the Dobrud-
steam-power station. ja's coal basin, intensive geological investigations
In France, a research group for underground on the origins and petrographic composition of
coal gasification, i.e. Groupe d'Etude de la the coal have been carried out. Detailed study of
Gaz~ification Souterraine (GEGS) including the coalification of this coal has revealed the
Charbonnage de France, Gas de France and presence of a thick series of bituminous coals.
Institut Fran~ais du P~trole was founded in Ultimate and proximate analyses of the coals
1976. Its goal was the development of coal show that according to the degree of coalification
reserves amounting to 2 x 109 tonnes at a depth they are all volatile coals (V daf =35-40%;
of more than 800m. In the 1980s about 22 C d a f = 80-83% and swelling i n d e x - 1 ) . On
million dollars were ensured for the realization average coals are characterized by a low sul-
of this project. For the first stage which was phur content-0.6-1.5% and a low content of
carried out in Bruay-en-Artois (Nord-Pas-de- mineral matter-Ad = 6-12%. Individual seam
Calais) about 4.3 million dollars were spent samples have a higher content of mineral
(Ferreti 1982). The first stage of the test began matter-A d = 13-31%, sulphur = 0.8-4.2% and
from a derelict mine tunnel at a depth of 1000 m volatile matter yield V daf = 3 7 - 4 5 % . The in-
and with two boreholes (injection and gas creased content of volatiles (up to 45%) and
388 D. DOUCHANOV & V. MINKOVA

r 3 I Gas
2.1 l r

Fig. 4. Countercurrent combustion in UCG:

~-a b " ~ d ' e 1, injection hole; 2, gas removal hole; 3, compressor;
4, coal seam; 5, combustion flow direction.
Fig. 3. Electrolinking method: 1, electrodes;
2, injection and removal holes; 3, insulation:
ab,de-highly conducting channel sections, c-unheated environmental problems such as the air pollu-
coal seam region. tion caused by various chemical derivatives
evolved during U C G should be also considered.
In Table 1 are shown data from the studies on
of cdaf-76-80% shows that some of the samples the pollution during U C G testing in Hoe Creek,
can be referred to high volatile bituminous coals Wyoming, USA (Mead et al. 1977). During
(Minkova et al. 1983). In the 1970s it was U C G at greater depths, as will be required for
considered that these volatile coals could be used the Bulgarian coal, similar pollution has not
in a mixture (up to 55%) for coking in the been registered: the clays, for example, take part
Kremikovtsi Metallurgical Plant (Trayanov, in the neutralization of H2S and NH3.
1979). However, it turned out that the coal It should be noted that the coal seams in
deposits are situated at a depth of 1500 m which Europe are characterised by great depths and
requires large investments for mining. small thickness. Under these conditions the
The gasification of coal seams at shallow and successful performance of U C G requires that a
intermediate depths can be undertaken by number of technical difficulties are overcome
directional drilling whereby the interaction such as: the effective linking in the coal seam; the
between neighbouring holes (for injection and impeded control of the gasification front; and
gas removal) is a result of the natural coal the control of the multistage gasification process
permeability. Often the latter is enhanced by: as a whole.
water feeding (hydrofracturing); air injection The reaction agents and the basic products
under pressure (electrolinking) (Fig. 3); blasting used in UCG, as in all gasification processes of
(Klimentov, 1964), or by using derelict mine coal, besides coal are: oxygen, water, hydrogen,
tunnels from which holes of up to 200m are carbon oxides, methane, hydrogen sulphide, etc.
drilled, etc. The most complicated problems in (Douchanov & Angelova 1982). The composi-
this respect are: the realization of the linking tion of the gas produced is influenced by
along the coal seam whereby the countercurrent catalytic reactions which occur on the surface
combustion ensuring sufficient gas flow between of the coal matrix and the inorganic salts which
the holes is most often employed for its are found in abundance around the under-
stabilization (Fig. 4); the pack compression of ground gas generator. The coal characteristics,
the rocks disturbing hermeticity facilitates the the geometry of the coal seams (depth, dip, etc.),
water penetration from the water-carrier layers; the amount, type and the quality of the
the control of the gasification front flow from gasification agent, its pressure and temperature,
the injection to the gas removal hole, etc. Some the geometry of the holes are some of the basic

Table 1. Study of the pollution by UCG during the Hoe Greek test
Pollution Pregasification Inside burn zone Outside burn zone Permissible
species value concentration
(mg/l) Concentration increase Concentration increase limit
(mg/1) (mg/1) (mg/1)
Phenols 0.001 0.1 100K 500 5 • 105 0.001
CN- 0.01 0.4 40K 300 3 K 10 4 0.20
NH~- 0.5 20 40x 70 100• 0.5
Pb 2+ 0.001 0.001 - 0.04 40 K 0.05
SO~- 200 2000 10• 1000 5K 250
 REVIEW OF HISTORY OF UNDERGROUND COAL GASIFICATION 389

parameters that determine the effectiveness of to a 'new edition' of the interest towards this
the UCG process. All these complex interactions huge resource. This project includes the follow-
indicate the necessity for various models and ing participants: the Mine Geological Techno-
mathematical modelling (Gunn & Whitman logical Institute in Madrid, the ENDESA and
1976) to optimise conditions prior the realiza- OCICARBON Companies, the English Nuclear
tion of the underground experiments. Energy Board and the Belgium Council for
The financial aspects of the problem are also UCG research.
of essential importance. The cost of a hole in the The main area of coal mined in Bulgaria
1980s was two million French francs. The belongs to the lignites from the M a r i t s a - East
greater distance between the two holes (injection field. They are the main feed stock of the
and gas removal) is decisive for the optimal thermal power plants. It is envisaged that
amount of the burned coals utilized by them. during the next 5-10 year the Elhovo lignite
This distance, imposed by the experiment, has a field (500 x 106 tonnes) will be set into operation
basic meaning for evaluating the economical (Douchanov & Angelova 1982). The character-
efficiency of the process. French scientists istics of the coal from the aforementioned
(Pottier & Chaumet 1978) have derived the so deposits are as follows: Marits-East (W, 50-
called 'integral coefficient t(L)' (Fig. 5) which 60%; A d, 30-60%; S d, 4.0-5.0%; C daf, 64%;
reveals the relationship between the following H daf, 6.8%; Combustion heat of working
parameters: Q, E, L, S. As seen from Fig. 5, fuel, 6.6 MJ/Kg) and Elhovo (W, 55-55%; A d,
these are: the amount of the coal utilised by a 30-37%; S d, 7.0-8.0%; C dar, 62%; Combus-
pair of holes (injection and gas removal) tion heat of working fuel -6.3 MJ/Kg).
Q = 6000 tons, coal seam thickness E of 2 m During recent years, stand-tests were per-
burned coal seam area S = 2 5 0 0 m 2 and the formed for coal gasification in a fluidized bed, at
distance between the pair of holes L = 60 m the pressures of 1-2 MPa, both with steam-air and
integral coefficient t(L), is 0.7. steam-oxygen mixes (Lazarov 1986). Besides the
The fact that in 1991 (Furfari 1992) the advantages, these experiments have certain
Energy Council of the European Communities shortcoming. For example, during gasification
decided to invest 18 million ECU in a large-scale of high-ash coal, agglomeration of the particles
Spanish-English-Belgium test on UCG in the and disturbance of the normal fluidized bed in
Alcorisa region of Spain with a depth of the the gas generator might occur. Such phenomena
holes of 600 and 900 m, points unambiguously have been observed with steam-air gasification

"d':O,~ ~-0,6 7"=0J3 "U=I,0

l 90

1/111I ~ 5 7 9 11 13 15
t(L) #' Ill / I n~3 I ,' f " ,', '. I ~ f I | f
S ( 1000 m 7)

1,0 OH 0,6 04
9
15
21
27
i .-1

10~ 5 E t~E 3 E 2

O,[x1OOOf/ pair h o l e s )

Fig. 5. Curves for calculation of the integral coefficient t(L): Q, quantity of the coal matrix utilized by a pair holes
(injection and gas removal); E, thickness of the coal seam; L, distance between the holes.
390 D. DOUCHANOV & V. MINKOVA

of the Elhovo coal in a quasi boiling layer, under DOUCHANOV, D. & ANGELOVA,G. 1982. Issledvane
pressure, at gasification temperatures of 920- vazmozchnostite za intenzifikatsiya na gazifikat-
930~ (Lazarov & Douchanov 1988). Due to the siyata na vuglischtata, Izvestiya na BAN, 15,
lower reactionability, compared to the Maritsa- 393-399.
DOUCHANOV,D., LUTSKANOV,L., MARINOV,S. P., MIN-
East coal the gasification of the Elhovo coal KOVA, V. & YOSSIEOVA,M. 1997. Catalytic effect
does not run at a satisfactory speed when the of ZnC12 in the pyrolysis of lignites, Fuel, in press.
temperature is below 950~ DOUCHANOV, D., MINKOVA, V., MARTINEZ-ALONSO,
To clarify the possibility of overcoming the A., PALAClOS, J. M. & TASCON, J. 1993. Low
particle agglomeration during gasification of temperature ashing of Bulgarian lignites, Erdol
Elhovo coal, the following studies were per- und Kohle, 12, 461-467.
formed: (i) on the cause of particle agglomera- GUNN, R. & WHITMAN, D. 1976. Packed-bed models
tion (Douchanov et al. 1993) and (ii) on the for the in situ gasifier, Laramie Energy Research
impact of some catalysts. The results from Center, Reprint No LERC/RI-762.
FERRETI, M. 1982. La valorisation du charbon, Paris,
study (i) on the Elhovo coal during gasification
219-237.
in the fluidized bed with a steam-air blow, FURFARI, S. 1992. Gasification and 1GCC within the
under pressure, confirm the necessity of run- European Communites, Erdol und Kohle, 45,
ning the process at a lower temperature and at 292-293.
conditions avoiding local overheating, i.e. at KLIMENTOV, P. P. 1964. Gidravlicheskii razriv dlya
intensive quasi-boiling layer. The effect of podzemnoi gazifikatsii zalezchei uglei, Izvestiya
some catalysts on increasing the speed of visshikh uchebnikh zavedenii-geologicheskaya raz-
gasification of the Elhovo coal was tested at vedka, Moskva, 1097-105.
temperatures below 900~ The results LAVROV, N. B., KULAKOVA,M. A., KAZACHKOVA,
S. T., ZHIRENYI,A. E., ANTONOVA,R. I. & VOLK,
obtained, indicated that the carbonates of the A. F. 1971. O podzemnoi gazifikatsii angrenskogo
alkaline metals are active catalysts during burougolnogo mestorozchdeniya, Khirniya tver-
gasification of the Elhovo coal at 750-800~ dogo topliva, Moskva, 1, 73-76.
(Angelova & Douchanov 1983; Douchanov & LAZAROV, Y. 1986. Habilitazionen trud, MIN-
Lutskanov, 1996). PROEKT, Sofia.
Since proposals for mining the Dobrudja's LAZAROV, L., DOUCHANOV, D., MARINOV, S. P. &
coal basin have been abandoned, underground STEFANOVA, M. 1988. Agglomeration of Elhovo's
coal gasification remains an important strategy coal in the pressurised fluidized bed gasifier,
for utilizing this resource. During the past Symposium 'Physico-technical problems of ener-
getics', Moscow, Reprint 12.
decade and particularly in the last few years a
MEAD, S., CAMPBELL,J. H. & NTEPHENS,D. R. 1977.
revitalization in the interest in U C G has Environmental tests in Hoe Greek UCG. Proc. of
occurred both in the United States and in 3rd Annual Underground Coal Conversion Sympo-
other countries. Considering the large reserves sium, Lawrence Livermore Laboratory, Reprint
of the Dobrudja's coal basin amounting to 770652, 475-489.
about 1.5 x 109t and the insufficient resources MINKOVA, V., ANGELOVA, G., GORANOVA, M. &
of petrol and natural gas in Bulgaria, we RAZVIGOROVA, M. 1983. Varhu khimicheskiya
conclude that ways should be investigated sastav na vaglischtata na Dobrudjanskiya basein,
including cooperation with other countries with Khimiya i industriya, Sofia, 5, 207-210.
POTTIER, M. & CHAUMET, P. 1976. Gaz6ification
experience in this field, to carry out research, souterraine profonde du charbon; problemes et
mathematical modelling and pilot experiments perspectives, L'Industrie du P~trole, 498, Septem-
on U C G in the Dobrudja's basin. bre, 53-57.
PRASEK, K. & KORANDA, J. 1989. Stav vyzkumu
pdzemniho zplynovani uhli, PLYN, Praga, 69/5,
References 141-145.
SKAFA, P. V. 1960. Podzemnaya gazifikatsiya, Gos-
ANGELOVA,G., DOUCHANOV,D. & RAZVIGOROVA,M. gortehizdat, Moskva, 110-115.
& LAZAROV, L. 1983. The role of catalysts in STRCLAND,L. 1977. In situ gasification of West
intensifying the process of gasification of lignite to Virginia coal by 'long wall generator', Proc. of
produce synthesis gas, Seminar on Chemical from 3-rd Annual Underground Coal Conversion Sym-
Synthesis Gas, Economic Commission for Europe, posium, Lawrence Livermore Laboratory, Reprint
Geneva, Chem/Sem. 12, R. 17. No 770652, 81-85.
ANTONOVA, R. I., GARKUSHA, I. S., GERSHEIV1CH, SZECHY, G., KISS, J. & AZENBEGI, J. 1988. Under-
E. G., KREININ, E. V., LAVROV,N. V., SEMENKO, ground Gasification of Coal, MagyarKemikusok
D. K. & FEDOROV,N. A. et al. 1967. Issledovanie Lapja, Budapest, 8, 289-295.
nekotorikh zakonomernostei protsessa podzem- TRAYANOV B. 1979. Kam Voprosa za Termichnata
noi gazifikatsii uglei. Khimiya tverdogo topliva, Podgotovka na Vuglischtata za Koksuvane, PhD
Moskva, 1, 86-90. thesis, Sofia.
 Coalbed methane migration in and around fault zones

E. L. B O A R D M A N & J. H. R I P P O N

International M&ing Consultants Limited, PO Box 18, Common Road,

Huthwaite, Sutton-in-Ashfield, Nottinghamshire, NG17 2NS, UK
Abstract: One of the characteristics of all operating coalbed methane fields is the
considerable variation in producibility success within these fields and even between
adjacent wells, suggesting that very site-specific controls are operating. The most likely
control in many coalfields is geological structure, particularly faults, which can divide the
ground into fluid migration pathways and zones with bypassed, retained gas. Apart from the
faulted zone itself adjacent ground will have been subject to dilational or contractional
strain, and the strain profiles on either side of the fault will have their own individual
permeability characteristics which may be further modified by subsequent burial history.
Although any one well will be site-specific, this introductory paper seeks to describe the
general ways in which modern understanding of faults and their associated strained ground
can contribute to better well spacing and detailed siting and therefore a greater proportion
of successful completions.

Methane from coal seams (coalbed methane) is anticline in the Grand Valley Field in the central
potentially an important source of natural gas part of the Piceance Basin, Colorado (Stevens
worldwide given the large volumes of gas 1993). The detailed geology and hydrology of
contained in the coals and associated rocks in this reservoir are still not well understood and it
the world's coal basins. To date successful is clear that a better understanding of cleat
economic production of coalbed methane from geometry and the structural controls on natural
virgin seams is limited to a few areas in the USA. fracturing will help to improve characterization
More recently attention has turned to other of the coals in terms of gas producibility.
coalfields, particularly in the United Kingdom, Coal seams constitute unconventional natural
eastern and western continental Europe, China, gas reservoirs. They not only store gas but they
South Africa, France, Spain and Australia. are also a source of gas. They are a more
A common feature of coalbed methane pro- complex form of reservoir than a 'conventional'
duction has been the co-existence of both low natural gas reservoir both in terms of their
and high production wells in the same field and geology and in the mechanisms involved in gas
often in close proximity to one another. Current production. Gas producibility from coal seams is
activity in the USA is addressing the problems of generally controlled by the interplay between the
poorly producing wells, in particular focusing following factors: coal distribution, rank, gas
attention on why certain wells are not producing content, permeability, hydrogeology, deposi-
at their perceived potential even though many tional and structural setting. Local variations
are located near to high productivity wells. For in the geology and reservoir characteristics must
example, a well in the Cedar Grove Field of the be expected to influence the feasibility of
Black Warrior Basin, which has been in produc- producing methane from them. One of the key
tion since March 1990 and currently averages local conditions will be permeability. It is aspects
100 000 cuft/day (CFD) has offset wells in the of local variation that are addressed by this
same area producing between 200000 and paper, in particular the way in which faults and
225 000 CFD (Kuuskraa et al. 1994). Surveys in their associated strain zones may impose varia-
the wells have provided evidence that some of the tions in the permeabilities and connectivities of
perforated horizons have taken little or no sand the coals and their surrounding rocks. The paper
during hydraulic fracture treatment and some is based largely on mining experience in the
perforations are blocked by coal fines. The extent United Kingdom Carboniferous coalfields but is
to which these factors are controlled by variation considered to be generally relevant.
in the coal and strata properties or whether these No single paper can adequately address all
are purely mechanical/treatment problems is not productivity settings with respect to faults. This
known. However, in other areas, increased gas contribution is seen as a general introduction,
production is attributed to the proximity of wells and discusses general concepts that can then be
to tectonic structures. Additional fracturing and considered for site-specific use. These concepts
enhanced permeability have been attributed to are based on the most up-to-date geological
the proximity of wells to the Crystal Creek models wherever appropriate. While compatible

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 391-408.
392 E. L. BOARDMAN & J. H. RIPPON

TECHNICAL
CONTROLS

INHERENT
GEOLOGY
* l
INVESTIGATION
AND
PRODUCTION WELL
1
INDIVIDUAL WELL
INTERPRETATION PATTERN COMPLETION DESIGNS

* discussed in this paper

Fig. 1. Controls on coalbed methane producibility. Apart from 'external' controls, eg financial regime and
marketing, a CBM prospecrs success will depend on the geology, and on the techniques involved in its
interpretation and engineering. Geological interpretation is tabulated separately to emphasise the importance of
detailed understanding where the geology itself is very variable.

with these, it is the further intention of the paper provided by Kaiser et al. (1994). A British
to minimize descriptions and terminologies that contribution is provided by Baily et al. (1995).
are too detailed for an introductory paper. Figure 2 lists these controls in terms of geological
history, from original depositional setting,
Geological controls on coalbed through the varied phases of burial history, to
methane producibility the present stress setting. In any individual
prospect, producibility will frequently reflect
The ultimate producibility of any individual well several of these controls and their interactions.
will reflect both the site's geology and the design The depositional setting will determine the
and technology of the investigative and extrac- thickness, lateral extents, degrees of connectivity,
tive processes (Fig. 1). Individual well design is and vertical frequencies of the coals themselves,
beyond the scope of this paper. Many geological and also important inter-coal sediments particu-
controls may be considered significant for the larly sandstones, which can form associated
ultimate producibility and these are reviewed in conventional hydrocarbon reservoirs. Also, ulti-
the literature. A resum6, with particular reference mate coal strength and fracture permeability may
to two North American Cretaceous formations is be influenced by the nature and setting of the

I GEOLOGICAL CONTROLS I

I
I I H'ST~ I 'i I
L
I
associated
I
net coal
I
max.
1
uplift
I
folding igneous
i
fluid
I
joint
~ I
stress
i
interaction
conventional thicknees burial and effects migrations systems ratios with inherited
reservoirs and types depth unconformities and features
vectors
coat rank factors

permeability factors II.

retained gas content factors . ]=,,

* discussed in this paper

Fig. 2. Geological controls. Many geological factors interact to affect producibility. The present paper only
discusses fault systems in any detail.
 COALBED METHANE AND FAULT ZONES 393

Time
v

c o n t e m p o r a r y within contemporary w i t h overall post-depositional

depositional cycle coal measures deposition

SEDIMENTARY PROCESSES I IGNEOUS PROCESSES I TECTONIC PROCESSES 1

1 _ I I
I
faultlets
I
compaction
I
rotational
I
? delta lobe
I
(e.g)
I
gas phase
I
synsedimentary
1
post-depositional
faults slips features sill emplacement faults faulting faulting
faults

" growth faults "

Millimet r es Kilometres
Increase in m a x i m u m possible displacements "11,=._
(sedimentary and tectonic processes)

Post-depositional tectonic faulting is by far the m o s t

c o m m o n t y p e , and is the m o s t important economically

Fig. 3. Types of faulting in British Carboniferous Coal Measures. A large generic range is found, and each type
will have geometries and linkage characteristics which reflect the very different modes of origin.

precursor vegetation itself. Most identified geo- the broad aspects of migration through
logical controls relate to the long burial history unfaulted ground, specifically coal-bearing
that characterizes many hard coals, especially sequences. These are laid down in many deposi-
Carboniferous coals. As Fig. 2 illustrates, several tional settings and characteristically comprise
of these factors interact to give the coal rank, and very varied rock types, usually reflecting river
also the basic permeability of the deposit. The system migrations. The proportions and geome-
present stress setting provides a final control, tries of these rock types are also very variable. In
with the principal horizontal stress vector in most hard coal deposits, the sandstones can be
particular influencing the directional permeabil- significantly permeable via their well developed
ity of the inherited structure. joint systems, with the claystones acting as
Because of the many interacting geological aquicludes. (However, in some high rank coal-
processes, it is very unlikely that all relevant fields, claystones may themselves be upranked
factors presented by the geology of a particular sufficiently to allow passage of groundwaters at
prospect will be sufficiently known and under- depth). Coal can form another permeable rock
stood for complete analysis. Figure 1 therefore type, for example, in the near-surface where
includes both inherent geology and its investiga- destressed, and in the tensile strain zones caused
tion and interpretation, as separate controls; in by mineworkings; in general, in situ coals in the
other words, the suitability of investigative UK can only rarely be considered permeable at
techniques, and the applicability of the inter- any practical scale, particularly for water, but
pretation, will be critical in maximizing produ- also for methane. The sandstones can form
cibility. Of all the geological controls, the most reservoirs for conventional hydrocarbons, and
site-specific, and currently the least understood significant water inflows to mine workings
in terms of coalbed methane producibility is usually involve sandstones as either source or
considered to be faults and their associated migration pathway. As the sandstones are also
structures (Figs 3 & 4). the most intricate in geometry, fluid migration
pathways cannot successfully be modelled with-
out good borehole data control. A key factor in
Fluid migration through unfaulted ground fluid migration through coal is the jointing; this
includes 'cleat' and 'slip' in the British coalfields.
Before considering the effects of fluid migrations Pervasive cleating usually lies roughly normal
in faulted ground, it is suitable to refer briefly to to the coal bedding, with fracture densities
394 E. L. BOARDMAN & J. H. RIPPON

|FAOL;"SYSTEMS
I
..,
j I
,, MODE
[ L ~ I 'DAMA!E ZONE L I
LINKAGES

I
normal
I
reverse
1
thrust
l
sWike
I
"blind"
1
intersects gouge fracture number
I
relay
I
volumetric
I
subsidiary
slip free rocks linkages o zones variations faults
surface sealing / trends fault joint
non-sealing populations densities
(fault densityl orientation
rnineralisation

Fig. 4. Fault system attributes. Those factors which describe the compartmentalization of the ground by faulting
and which affect the general permeability. See text for details.

sometimes several tens/m; cleat densities vary these fractures, the density of which is typically
according to structural setting, and also with coal much less than cleating, perhaps 1/m being
lithotype and rank. The high rank coalfields of characteristic. Similar slip has been recorded
southern England and South Wales have greater locally in other British coalfields, mainly adja-
cleat densities than those to the north. In general cent to large faults.
terms, the cleat orientations tend to reflect Fluid migrations through coal-bearing
Variscan compressional trends, with deviations sequences will also depend upon bedding dip,
from the regional on the approach to individual hydraulic gradients, and any mining extractions
faults. The degree of mineralization reflects the that have modified the sequence through voids
geological history of each coalfield, and in the U K and associated strains.
can vary from the well mineralized cleats (carbo-
nates and sulphides) of the eastern Pennine Basin
to the poorly mineralized coal of South Wales. Faults and fault zones
Many detailed cleat studies of British coals
were undertaken in the 1950s and 1960s as part There is a very extensive geological literature on
of studies on the introduction of plough coal faults and fault zones, both general and also
cutters; these commonly recorded all cleats in highly technical. The intention of the present
terms of density, orientation, and relationship to paper is to discuss those aspects which relate to
coal lithotypes for a variety of seams and fluid migration and/or retention, specifically
geological settings. However, there has been coalbed methane. Figure 4 tabulates the fault-
little published on cleat in British coals, and for related factors. Faults may originate in various
an overall geological appreciation of cleating, ways, some relating to the depositional processes
and jointing in general, reference may be made of the host formation but the majority being
to the wider geological literature, e.g. Rawnsley tectonic and post-depositional. These are invari-
et al. (1992). Further comment on cleat is ably categorized as normal, reverse/thrust or
provided later, with respect to Longannet mine strike-slip depending on the dominant slip
in Scotland. direction with respect to the fault plane. How-
Regarding slip, this is typically a fracture ever, this is very much a simplification, especially
system lying at around 45 ~ to the coal bedding when discussing zones of faults. For example a
and characteristic of the southern British coal- strike-slip fault zone may include many appar-
fields of Kent and South Wales. These fractures ently normal and reverse faults. Individual faults
are usually unmineralized, and form conjugate may well show both dip-slip and strike-slip
sets with fracture strike tending to parallel the characteristics giving oblique slip with extension
local 'cross faults' - i.e. those of overall normal or contraction. Normal, reverse and strike slip
fault mode which intersect the Variscan com- faults and their variants grow in response
pressional trends of these coalfields at a high to changes in the magnitude and ratios
angle; however, variations from this parallelism of the principal stresses. These may themselves
are known. Although often polished, there is alter throughout the geological history of a fault,
only rarely minor displacement of the seams at from it initiation to its final extent, producing
 COALBED METHANE AND FAULT ZONES 395

variations in fault plane dip and curvature. the following features are seen to affect the
Events in subsequent geological history may permeability of the fractured and strained
reactivate a fault, quite possibly under a different ground.
stress regime.
The fracture or fracture zone itself will reflect
these formative and subsequent stresses together Fault plane and damage zone
with the physical characteristics of the host
rocks and any lubricating clays and fluids. A Apart from the simple juxtaposing of permeable
wide 'damage zone' may result, with a hierarchy and impermeable formations, structural traps in
of interlinked faults with rotated or crushed conventional hydrocarbon reservoirs frequently
pieces of host rock; alternatively a single neat depend on the sealing characteristics of a fault
fracture with minimal damage zone width may damage zone; oil and gas may be retained by a
result. In particular contexts, there may be a clay-rock dominated 'gouge', or may have
relationship between fault throw and the width migrated by leakage through 'windows' pro-
of the damage zone (e.g. Robertson 1983; Knott vided by, e.g. the fault juxtaposing sandstones,
1994). In this paper the term 'damage zone' with minimal clay-rocks in the gouge (see e.g.
refers to the immediate faulted volume across Lindsay et al. 1993). Sandstone-to-sandstone
which there is measureable displacement and situations may, however, still have reduced
which includes the gouge and the normal drag. communication across the fault because of
For a simple fault, the variation in throw (in grain size reduction/recrystallization. Such con-
normal faults, throw is the vertical component siderations apply to water migrations as well as
of the displacement) is known to be systematic, conventional hydrocarbons. The sealing char-
with the greatest throw - ideally corresponding acteristics will, however, be very site-specific and
to the point of initiation - located centrally on a will depend on the following main factors: the
fault plane that has essentially ellipsoidal limits lithologies actually present within the faulted
when viewed in strike projection (e.g. Rippon sequence; the number of faulting events and
1985; Barnett et al. 1987; Walsh & Watterson their style; the diagenesis of the faulted rocks;
1990). Figure 5 illustrates the general principle, and the displacement relative to the thickness of
showing contours of displacement, the fault the bed in question. Potential migration along
limit (tip line) being zero displacement. Follow- the fault zone itself will depend on similar
ing from Fig. 5 it should be noted that a fault considerations. However, there will be differ-
cannot be viewed as a fracture independent of ences in the special case presented by coalbed
the adjacent ground. The variation in throw methane, where the reservoir rock is coal, the
across the fault necessitates a related strain in permeability of which may be very low by
the rock volume; in the simplest case of an comparison with sandstones, and in which
isolated normal fault, the upper hangingwall producibility commonly requires direct stimula-
and lower footwall of an ideal normal fault will tion. In this case, the fault plane and damage
be dilated above regional stratigraphic thickness zone will aid methane depletion over geological
with a corresponding compression in the lower time if the actual fracture pattern extends
hangingwall and upper footwall. Such strain laterally into the coal seams for a significant
zones will approximate to ellipsoidal volumes, distance, i.e. tens of metres.
and for large faults (hundreds of metres) may
show very significant volumetric differences
between adjacent hangingwalls and footwalls. The adjacent strained volume
Within these strains, the rock fabric will also
vary and the most obvious variable is likely to be The general nature of the strained volume (Fig. 5)
joint densities. Again, using the idealized simple was discussed above, with the potential for extra
fault (Fig. 5) the upper hangingwall and lower joint permeability identified for the upper hang-
footwall may be expected to have much better ingwalls and lower footwalls of idealised normal
developed joints; this may or may not translate faults. Although many examples of these strained
into enhanced fracture permeability depending volumes are known, actual field observations of
on geological history. the necessary rock fabric changes are rare. At
Longannet mine in Scotland, a number of large
(tens to hundreds of metres throw) faults are
Fault modification of fluid migration intersected by the mineworkings, and proved/
imaged by boreholes and high-resolution reflec-
From the above introductory account of faults tion seismic. Integration of all these data has
and their associated damage and strain zones, allowed the mapping of the practical limits of the
396 E. L. BOARDMAN & J. H. RIPPON

fault-adjacent strained volume, at mined hori- obvious visible effect. Figure 6 illustrates the
zons. Overall, this is expressed as prominent extents of the mappable strains adjacent to one of
dilation/contraction of the hangingwall and these, the Abbey Craig East Fault, an essentially
footwall as appropriate, together with some isolated structure which is well-proved by mine-
extra minor faulting, mainly in the footwalls; workings and by explorations. Changes in the
gradient change at the mined horizon is the most coal, in terms of strength and joint orientation/

T "--" "'I-- ...... ~ A

9-----" i I" l 9"9 B Ptan of fault intersecting
I 1 I I successive horizons,
I I I I A,B,C
I I ~. 1" tool 1
I I~ I', I c
t t ti
. : ~ c , ement (fault ~ line"

v / / I"" I " " .~. \ \

B / / - i ~ .\ .L X '\ / n---/:'~g7 J
' ; / f ~'--"~ ..~ ' /hangi / B
-h- _ , _ w . , , , - ,oo,- /
" \ ---I--" " / f / wa~l 1
\\ x /~ /./ // _ /
/

//~ Contours of displacement Cross-section of fault and

//// Projection of fault displacement data on to a adjacent strained ground.
/ / ~ : r t i c a l p l a n e , with horizons A , B , C p l o t t e d for
, the footwall intercept.

\\

./ "~._ ._~.__~ '\,

/ Normal )'\,
( tensional \}~

\
Fig. 5. Idealized simple normal fault. The fault's mapped intersections with three horizons, A B, C are shown in
plan view; as projected onto a vertical plane and contoured for displacement; and as a cross section which
illustrates the strain in the adjacent ground necessitated by the logically varying displacement.
(Displacement = throw/cosine hade).
 COALBED M E T H A N E A N D FAULT ZONES 397

o
,i,-

:l
1,1.1 | .,

7"
~<~

//
,,~/'
/
/
/
} ,

,~,.'~
, /

,'. ~,

/
/,
/
/
/"
/ ._
m
9 /t
.@
| o,1

.r

0 ',- ~

&

o~

.=
,- _~.=_ ] o o

(.~ ~

9 Q" " "

"~ t" N S 0

o~

oi~~~
~-~
'~-
~ "~.~'n
~Z
.,~.:
9 ~ g
~,!~! ~ :...~ m

~,= ~.~ ~
w
o
~Z
"!~.~ ~._~,,-.....~ t "? 0
~o~
...o ~ ~

~D

~ ' ~ o
398 E. L. BOARDMAN & J. H. RIPPON

e / .,<.,~.__-.---
I~ . - ~ ' -~ ~ --" ~--.c,,'~_,..
/ ?~f "~, "-<-->,.
,

-__.__._
9 /"
2' .J
.y ""-T
_._
", \
.~.',<, ",,,
/ o o '~. "\
/ .._z_.'~..~\.
/ ,<.t 9 ; T180m .~ '~ .,,.~
~,,>,..~/..----:_:~ / / ...~.\ .....-:.-.o0,,,
"---- "~ / - ' - 7 0-n,' . " / ~30.i \" ~\ ~ '" " -

9 / ,.,<-~ ~ .-._. ~ \',.. ....,,..

./ /-/- \\:-., .

-.__L ~_. / ------ ~o~:-.,..

9 ~.~
,7~ "~
~Lo~.._ ~ . . ~ - - ~ . ~ ~ ,,
c.~~.~. .---.-~.. ~. ~
~/ ~o-~--~ ~,. ">"~ ~ ~ ,,-'*
.... ,. .i m "' ....

a. -e-- Main m i n e r a l i s e d cleat "] e Borehole

all d a t a at
.-e-. Main c l e a t a d j a c e n t t o f a u l t s Upper Hirst horizon 1 km
( n o t all f a u l t s are s h o w n ) I . , I

o ; j~-~ -__
~ . . - 9

...v % \
....___. / 2 / 9.'I .~,,<,.,,~
/ o o "~. \
/" _~,~. CRAIG EA.S,~ ~-'~" ~ ' ~ . ~ ' ~ .
x / ~.~.~- ~'.-:-.-~.-~-LL~.-9- ~4,~OLv "---~-- "'~"~
~" ..6v. _.f.-..~" "~..~ ..._ ~. ,

9 |

' \i "
=~-___ ~ \ \ \ .~
ALLo~'.~...~................~ ..~.."Je~ . ~ - ~ . ~
~"~" ~ "~ . -'-- "~. -*~- e " "~"
1,. ...~ ~ ">,~.
" F~u~'E-" "~,~ ',~,
.. Im

b. ---)4- P r i n c i p a l h o r i z o n t a l stress away from faults o Borehole

I 1 km 1
 COALBED METHANE AND FAULT ZONES 399

frequency, are difficult to assess visually apart stronger and 'tighter' coals are to be expected,
from very local swings in the main cleat; however, probably with very good seismic propagation
there are signifcant character changes noted from and reflection characteristics. Unless modified
in-seam seismic transmission and reflection by later geological history, coals in these zones
surveys, and reduced integrity of surface seismic may be expected to have significant retained
reflectors is also prominent across these zones. methane, but also poor producibility because of
The example in Figure 6 is drawn at a coal reduced fracture permeability.
horizon, but it should be noted that the dilations/ The fracture aperture effects of these strains
contractions adjacent to these larger faults may are currently unknown, and will be difficult to
actually relate more to the prominent sandstones detect directly in mined exposures, where
and claystones that characterise the Longannet disturbance is inevitable. In general it must be
sequence, as, in bulk terms, these present the assumed that apertures will be greater where the
greater opportunity for modifications. In most fracture lies parallel to the local principal stress;
British coalfields, an increase in coal cleat density open jointing will be prone to mineralizations
is sometimes recorded in the immediate approach through later geological history.
to a significant fault. This is not always the case at
Longannet. The regional cleat trend there (Fig. 7)
subparallels the main fault trend, and is promi- Fault linkages and populations
nently mineralised with carbonates, the second-
ary cleat generally being subordinate in density The degree of connectivity of a fault fracture
and less mineralized. The situation at Longannet system will influence the potential for any fluid
is locally complicated by marked reduction in migration. Fault linkages may be considered in
cleat density in areas subject to mild thermal the following categories:
metamorphism, and by intense fracturing adja- (i) kinetically-related linkages, in which all the
cent to minor intrusions; however, the general fractures result from a common geological
picture shows only local increases in cleat density deformation phase;
on the approach to faults. Much more noticeable (ii) other linkages, in which faults from various
is that the main cleat orientation can swing geological deformation phases interact and
towards both smaller and larger faults, some- intersect to give a more complex situation.
times lying normal to the fault within a few
metres of it; this recalls the noding of fault- As with the fault-adjacent strained volumes
adjacent joints reported by Rawnsley et al. described above, there will be a fine balance
(1992). The Longannet descriptions are included between migration loss through fractures, a n d
here only to illustrate the potential geological ultimate producibility through stimulation of
relationships; there is no specific coalbed latent fractures. In these circumstances, it is
methane content. Given this background, it is proposed that particularly beneficial coalbed
assumed that for coalbed methane, fracture methane producibility may be found in those
permeability will be enhanced in the dilated zones where faults overlap. Fault overlaps
volumes in the coals, as well as the sandstones, (Peacock & Sanderson 1994; Childs et al. 1995)
but that the emphasized fracture systems in the occur where the overall deformation associated
coals will be more subtle. This probably repre- with an individual fault - including its adjacent
sents the best conditions for producibility, with strained volume - interacts with that of another.
good retention and a latent fracture system that Again, this particular form of 'linkage' may be
can be stimulated to encourage methane release. kinematically consistent, or not, with differing
Those zones adjacent to the fault which have detailed geologies as a result. Within these
suffered compressional strain should, by con- overlaps, ground strain may be considerable,
trast, have a much less pervasive fracture system. with changes in horizon dip, and fabric change
Field measurements of the bulk strength of including extra faulting and jointing. Such zones
in-place coals are notoriously difficult to stan- may therefore provide the required permeability
dardise, mainly because of fracture systems; for producibility, without the overall fracture
however, in such compressed settings, overall system depleting the methane over geological

Fig. 7. The Abbey Craig East Fault: coal cleat and present stress. This structure lies in the Scottish Midland
Valley, some 40 km northwest of Edinburgh: it is essentially an isolated fault allowing easy study of its
displacement and strain patterns. Fault displacement in metres. (a) The regional mineralised cleat shows general
parallelism with the gross fault trend except immediately adjacent to faults. See text for discussion. (b) The
present principal horizontal stress trend. See text for discussion; variations close to larger faults are known and
on-going work is seeking to define these.
400 E. L. BOARDMAN & J. H. RIPPON

time because the fracture pattern is not fully Fault zone burial history
linked. Figure 10 illustrates an overlap/relay
zone for a strike slip fault system. In UK coalfields, the main deformation and
The concept of fault populations, well known faulting phase is generally considered to be later
in coal mining for many decades, has recently Carboniferous/early Permian, with some later
been developed for the assessment of fracture reactivations. In certain coalfields, the later
patterns in conventional hydrocarbon reservoirs. movements have both complicated the existing
A fault population is a system of faults of all sizes faults and initiated new faults. By contrast in
in which there is some numerical relationship other coalfields, existing faults have been re-
between the size categories (e.g. Walsh & used, with renewed but essentially uncompli-
Watterson 1992). For tectonic faults, power law cated growth. These differences must partly
size distributions are sometimes applicable. reflect the orientation of the existing faults to
However, in the authors' experience there are the new stress pattern. In addition to reactiva-
significant gaps in fault size distributions in many tion, fault zones will be modified with respect to
British coalfields and power law size distribu- their permeability attributes by burial/uplift
tions may not be universally applicable. Ideally a history; and by regional fluid migrations and
fault population should be based on one mineralizations resulting from igneous replace-
geological deformation phase, but at least some ments, or driven by tectonic uplift (e.g. Daniels
published sets appear to include faults of several et al. 1990) or from other geochemical redis-
phases. The potential for describing conventional tribution mechanisms. It should be expected that
hydrocarbon prospectivity using fault popula- such fluid migrations in the geological past will
tion studies- in which fracture numbers below themselves have taken advantage of any struc-
seismic resolution are assessed from those turally controlled permeability patterns pre-
revealed by seismic- is very dependent on sented by a fault zone, to the extent that a key
choice of the most suitable mathematical fracture system, e.g. the main coal cleat, may
model, and is beyond the scope of this paper. be largely sealed by mineralization effected by
For coalbed methane, it is considered that fault these fluids.
population studies will rarely have applicability, The burial history of a fault zone should also
as they are essentially regionally-based whereas include consideration of the recent/continuing
coalbed methane producibility requires much present stress field. It is known from British
more site precision. Those aspects of fault coalfields that stress magnitudes and ratios can
population studies that may have coalbed vary over an area as small as one mine lease, and
methane application are as follows: also vary through lithology and stratigraphy.
For example, at Asfordby mine southeast of
(i) fault damage zone: specific fault hierarchies Nottingham (Whitworth et al. 1994), the varia-
and linkages making up the broken ground tions indicated some response to ground hetero-
itself; geneities produced at least partly by inherited, or
(ii) preferred faulted horizons: faults initiated 'fossil' fault structures. Current work by the
preferentially at a particular depth, and authors is investigating the response of the
propagating largely within a particular present principal horizontal stress to the fossil
depth interval. For example, Rippon & strain zones adjacent to the Abbey Craig East
Raine (1986) implied that fault populations Fault at Longannet mine (Fig. 6). As described
lay at differing preferred horizons (West- previously the strain zones have been investi-
phalian A/Westphalian B) at two adjacent gated and mapped for the mined horizon, and
collieries in Derbyshire, England. It is the volumetric differences between the lower
thought likely that such horizon prefer- footwall and hangingwall strains assessed using
ences are common in many coalfields, with their fabric differences, which are thought to be
each 'cell' having its own fracture char- largely joint orientations and frequencies. On-
acteristics (orientations, size relationships, going mapping aims to define any refractions of
preferred nucleation depths) on a scale of the stress vectors, both fossil and present, within
25 km2-100 km 2. the strain zones. The modifications produced by
'fossil' heterogeneities on the present stress field
From this listing of fault-related features, it will are not currently well understood, and again are
be seen that fluid migration and retention likely to be highly site-specific. However, the
characteristics are likely to vary significantly orientation of the principal horizontal stress
along, and adjacent to faults. However, any with respect to that of the inherited fracture
idealized pattern may well be modified by pattern will have considerable influence on well
subsequent geological history. design and producibility for coalbed methane.
 COALBED METHANE AND FAULT ZONES 401

Models for coalbed methane retention progressively greater subsidence towards the
and migration fault plane, directly influencing net coal thick-
ness on a very local scale. It should be noted that
One of the principles behind the present paper is in some circumstances, the greater coal thickness
that coalbed methane producibility is very site- might alternatively form in the footwall. For
specific and will be strongly affected by fault example, the hangingwall may be subsiding too
zones. However, it is appropriate to the under- fast for peat generation or retention, with the
standing of individual prospects and well sites footwall offering a better water-table balance
that the general principles be understood. This within an overall basin subsidence setting. The
can be attempted by combining the following: fault plane in Fig. 8.4 is shown as concave to the
hangingwall, or listric, only to illustrate another
9 idealization of normal, thrust, and strike slip
possible shape for normal faults. The listric
fault geometries;
shape is not essential for the 'growth' aspect-
9 assessing the physical changes imposed on
active during deposition - illustrated here. Also,
the adjacent rock ('fabric changes') with
the increasing inter-horizon thicknesses towards
special reference to fracture permeability;
the fault should be recognised as potentially
9 assessing any burial history particulars;
including both depositional increases and dila-
9 assessing the interaction between the 'fossil'
tional effects from subsequent fault growth.
fault structures and the present stress fields,
drawing upon mining experience.

Thrust faults and zones

Normal faults Reverse f a u l t s - taken here to have fault plane

dips characteristically greater than 45 ~ to bed-
Figure 8 illustrates some of the interactive d i n g - are considered by the authors to be
factors which will influence ultimate coalbed relatively rare except in strike slip fault zones
methane producibility. Given the very varied (see e.g. Fig. 10). They only rarely form in
geology of faults and fault zones already isolation, and very rarely form in regionally
described, only a few interactive factors can be integrated systems; some will be reactivations of
dealt with in such simplified drawings, which are originally normal faults. These are, therefore,
chosen more to illustrate general principles than not considered in any detail in this paper. Thrust
provide immediately usable templates. Figure 8.1 faults (Fig. 9) in the southern British coalfields,
illustrates an idealized normal fault. The stylized with Variscan deformation, typically have low
bedding is shown at a wider spacing across the fault plane dips, <_5~ commonly to 30 ~ with
faulted interval merely for clarity. In this simple steeper dips where the propagation of the
case, the fault is seen as essentially unmodified by fracture is through stronger rocks (ramps). In
later geological events; it did not intersect the strongly folded coalfields such as the Ruhr and
original free surface, and it is not exposed by the the Appalachians, thrust fault plane dips may be
present erosion level. The idealized distribution much more pronounced. A detailed considera-
of permeability characteristics, with respect to tion of thrust-related permeability is provided
coalbed methane migration, retention and pro- by Hathaway & Gayer (1996).
ducibility are described above. In Fig. 8.2 the A simple thrust is commonly associated with
upper part of the idealized fault has been eroded, folding in the immediate footwall and hanging-
with likely coalbed methane depletion in the wall (Fig. 9.1). Higher permeability is to be
upper hangingwall. It is thought that widespread expected in the hangingwall from well-developed
unconformities result in wholesale degassing cleating/jointing and maybe thrust-parallel
over significant vertical ranges (Creedy 1988). shears. Locally in the South Wales coalfield,
However, subsequent reburial by later basin the footwall is 'tight', presumably reflecting
development may allow secondary gas genera- downwards variation in displacement; such
tion (Fig. 8.3). The potential for retention of this settings may have characterised some of the
methane will depend on many burial history gas outburst situations in the western anthracite
aspects, including depth ranges, and the nature field. The detailed distribution of very low
of the unconformity and overlying formations. permeability anthracite in relation to thrusts or
Figure 8.4 shows a fault that was growing during gas outbursts is, however, not known and it
deposition of the coal-bearing sequence. Here, would be inappropriate to draw any definitive
coals are thickening into the fault on the conclusion. The great majority of thrust faults
hangingwall side, where vegetation growth and occur in linked systems as in Fig. 9.2. These may
preservation were able to keep pace with the be idealized in various ways, partly depending
402 E. L. BOARDMAN & J. H. RIPPON

1. Simple normal fault,

"blind", minimal linkages
to other faults, little degassing
(~) volume increase; increased
permeability
(| | (~ volume decrease; decreased
permeability
\J' .i- /

2. Erosion : essentially degassed,

I / / especially in upper hangingwaU (|
/,/I ? residual gas retention in lower
footwall ((~))

3. Early degassing by uplift / unconformity;

secondary gas generation from
subsequent reburial, with potential
retention in lower footwall

4. "Growth" fault w i t h thicker coals

along fault hangingwall, with
probably enhanced permeability (|
Probably low-permeability footwall
with generally thinner coals ((~))

Fig. 8. Normal fault examples. Many faults will undergo modifications over geological time and their related
permeability aspects will also be altered. Only some examples are illustrated. See text for further comment.

on the closeness to the contemporary free when intersecting a sandstone. Here it is

surface and on the lithologies involved. No suggested that the hangingwall coal, lying
work is known on the relative prospectivity of between the fault plane and a constraining
differing thrust systems. Because of their gen- strong sandstone, will be highly sheared, giving
erally low fault plane dips, thrust fault propaga- the possibility of coal-derived gas accumulating
tions are frequently modified by lithological in the sandstone as a conventional gas reservoir,
contrasts. Figure 9.3 shows a thrust ramping up assuming a suitable clay-rock cap.
 COALBED METHANE AND FAULT ZONES 403

1. Simple thrust displacing coal seam

(~) high permeability in hangingwall,
potential degassing
(~ reduced permeability in footwall
with potential for (gas) outbursts
|
(based on mining experience in
South Wales coalfield)

2. Thrust systems

imbricate fan;
? potential for degassing

thrust duplex;
? potential for gas retention

3, Lithological control on thrust

affected ground
impermeable cap ~..,.,,--0 (~) likely to be highly sheared;
? gas accumulation in
conventional reservoir

Fig. 9. Thrust fault examples. The permeability characteristics of the ground adjacent to thrust fault systems are
particularly poorly understood, reflecting conventional hydrocarbon interests in generally extensional regimes.
However, many permeability patterns may be envisaged. See text for further comment, and Hathaway & Gayer
(1996) for detail.

Strike-slip faults and zones vertical displacement, is rarely seen in British

coalfields, although well-documented examples
Strike-slip fault systems present very varied are known to the authors. More frequently,
patterns, both in map and section view. The identifiable strike-slip zones include a significant
simplest form, idealized as a vertical or near- dip slip displacement and fault plane dips at up
vertical fault plane, with very subordinate to 45~ with such attributes, their strike-slip
404 E. L. BOARDMAN & J. H. RIPPON

Maps of strike slip faults

'~~ ~ ~ ~o ~o
9~ ~ 1 7 6 "~ ~~176 ~
1. Early stage fault zone
with minimal linkage
but high strain / permeability
between individual faults,
potential high gas retention

9. . . 9 2. Highly linked fully formed

fault zone with potentially
extensive degassing

3. S c h e m a t i c strike slip s y s t e m ( m o d i f i e d f r o m W o o d c o c k and Fischer, 1986)

. . . .

- -

~
9

~
9 " releasing offset 9~ ", ~ " 'k
(relay zone) ~" ~s'=lIt

releasing bend "ly

restraining bend

.... ! 9 . .

/ r
/ i
Complex gas retention potential, probably maximissd in releasing offset
(high strain / permeability, with minimum linked system fractures)

Fig. 10. Strike-slip fault examples. A very wide range of fault styles will represent strike slip faults and zones, with
correspondingly very complex strains and permeability patterns. See text for comment.

character may be difficult to discern. In these respect to fluid migrations, and particularly
cases, individual component faults will appear to coalbed methane. Hence in Fig. 10, the dia-
be normal, or reverse (Fig. 10) with the overall grammatic map which is based on Woodcock &
zone showing prominent lateral movement. Fischer (1986) shows a range of fault settings. It
These differences may at least partly reflect was suggested above that the fault overlap zone
erosion levels, as the cross section of Fig. 10 illustrated by this may offer a greater produci-
implies. British coalfield fault mapping tends to bility, combining strained ground with no
record only the dip slip throw component, any through-going fracture. Depending on the rela-
strike-dip displacement being difficult to docu- tive depth of the fracture pattern with respect to
ment because of generally low bedding dips. the coal-bearing sequence, it is further suggested
Because of the complexity of many strike slip that the zones adjacent to the 'root' faults
zones and their considerable variation (see e.g. (see Fig. 10 cross sections) may also be prospec-
Naylor et al. 1986) it is difficult to generalize in tive. Strained volumes adjacent to strike slip
any useful way about their attributes with faults will be more difficult to identify unless the
 COALBED M E T H A N E AND FAULT ZONES 405

Fig. 11. Detailed interpretation of FMS. Detailed interpretations of image data, such as this example of FMS, are
routinely carried out to resolve seam boundaries, coal cleat, natural and induced fractures and sedimentary
features. For this coal seam, one individual cleat among many is shown bold, in the form of a 'sine' curve on the
'unrolled' image of the borehole wall.
406 E. L. BOARDMAN & J. H. RIPPON

bedding is steeply dipping, because of the absence Borehole surveys

or randomness of observable dip slip. Such a
fault will be mistaken for a normal fault of Downhole geophysical wireline logging in the
small throw, whereas its strike slip component UK coalfields was initiated in the 1950s when
may be hundreds of metres, with compatible several holes were logged using Schlumberger
large strains. resistivity, natural gamma and temperature
tools. It was not, however, until the 1960s with
the development of slim-hole tools by British
Plaster Boards (BPB) Instruments Ltd that
geophysical logging of boreholes became a
Investigative and analytical techniques routine feature of coal exploration. The early
Mining areas, sometimes with laterally extensive logging package comprised natural gamma,
workings, often at many levels, provide valuable density, caliper and sometimes a neutron log
data on the subsurface geology. The East and was primarily utilized to interpret seam
Pennine coalfield of the U K for example extends thickness and relative quality (principally ash
over an area of some 11000 km 2, the productive content).
Carboniferous coal measures attain a maximum A rapid expansion in coal exploration in the
thickness of about 1500m and contain up to early 1970s and the introduction of surface
30mineable seams in parts of the coalfield. reflection seismic into the industry to evaluate
Coalfields provide unique data sets on the geological structure was linked with the devel-
intensity, style and extent of faulting, and opment of dipmeter and sonic logs and the
detailed analysis is essential to an understanding running of seismic reference surveys to allow
of the controls on the subsurface flow of fluids. calibration of the sonic logs for synthetic
UK mining data sets result from a legal seismogram generation. The processed dipmeters
obligation on mining surveyors to record faults allowed detailed interpretation of structural
encountered underground, or in opencast mines. information from a borehole, which coupled
For most 20th Century mineworkings, these are with the surface seismic data led to the accurate
recorded on the detailed 1:2500 scale, with mapping of faults with throws above 10-20m.
smaller-scale plans for mine planning purposes The problem of the detection of minor structures
derived from these. It is thus possible to by downhole logging was, however, not resolved
investigate fault patterns to a very intricate until the later introduction of the Schlumberger
degree. At this scale of investigation, fault Formation Micro Scanner (FMS) in 1986. This
patterns and populations may be seen to vary was developed from the standard Schlumberger
significantly between mined horizons (Rippon & High Resolution Dipmeter (SHDT) by adding a
Raine 1986) and the need for specialist geologi- large number of small microresistivity buttons to
cal interpretation is emphasized. the SHDT pads. The data from these buttons are
now captured digitally which allows interactive
processing and interpretation to be carried out.
The detection of fractures and faulting from the
interpretation of FMS data sets has proved to be
Seismic surveys
very successful (Onions & Whitworth 1995). It is
Surface seismic reflection surveying has been only in certain lithologies such as weak seat-
used as an exploration tool in the British coal earths where detection has proved difficult.
industry for more than 20 years with very Several types of natural fractures have been
significant refinements in both acquisition and observed on the FMS. These include:
interpretation in recent years. Today the surface
(i) Coal cleat: orthogonal joint system specific
seismic technique is used for delineating the
to the coal seam consisting of closely
positions of sedimentary disturbances and fault
spaced subvertical fractures together with
throws that are little greater than seam thickness
any mineralization (Fig. 11).
in the best data areas. Faulting of less than 5 m
(ii) Fracturing and faulting: faulting identified
in throw has been imaged by modern 2D surface
when either a change in lithology occurs at
seismic lines and faults of around 2 m throw by
the identified feature or there is clear
recent 3D surveys. In virgin areas the surface
evidence of displacement of laminae.
seismic, often integrated with borehole geophy-
sical techniques, is used to reduce risk for Data sets already exist from boreholes which
immediate and long-term mine planning and penetrate faulted ground. It should be possible
provides an additional large source of detailed to analyse fracture intensity within faulted
structural coalfield data. volumes and compare the intensities both
 COALBED METHANE AND FAULT ZONES 407

within and outwith the faulted zone. In addition, data (on faults, joints, dips; field-mapped
in-situ permeability data from suitably located faults and seismic interpretations) with the
holes in similar situations could be acquired to most appropriate theoretical understand-
provide additional data from subsequently ing. Neither of these elements on their own
drilled holes. Downhole borehole testing equip- will give adequate understanding of any
ment is now available which can not only carry particular prospect.
out in situ permeability testing but can also be (v) It is unlikely that consistent success will be
used for in situ stress testing. Permeability tests achieved, particularly in Carboniferous
are carried out by isolating part of the formation prospects, without refined exploration
in the borehole by means of packers. The techniques, tailored to site conditions.
natural flow and pressures can then be mea-
sured, or injection of fluids can be undertaken to
measure permeability. Using higher pressures
the formation interval can be hydrofractured Conclusions
and measurements of in situ stress obtained. The The cost-sensitivities of many coalbed prospects,
orientation of induced fracturing and hence the and the intricacies of their geology, require
orientation of the principal horizontal stress detailed appraisal for optimized production.
direction can be subsequently derived from FMS This is particularly the case in faulted areas,
images run over the fractured part of the where juxtaposed sequences may have very
borehole wall. different structural and permeability character-
istics. It is hoped that the present introductory
paper will serve to stimulate interest in the
Discussion structural contribution to well siting.
Modern coal exploration techniques have
The foregoing introductory review has empha- been developed to an extent where it is now
sised the site-specific nature of many coalbed possible to resolve structural and permeability
methane well settings. A general interpretation data to a high degree of precision. Many existing
scheme is therefore inappropriate, but the data sets have already been acquired in areas
following principles result from the overall affected by faulting and it is considered that a
intricacies and interactions of various geological number of these could be subjected to detailed
factors. interpretation to provide information on the
fabric changes associated with different fault
(i) It is likely that, in faulted ground in settings.
particular, generalizations of practical The authors acknowledge the approval of
value will be inappropriate over areas International Mining Consultants Ltd for this
greater than 5 km 2. paper, and for the company's support in its
(ii) All aspects of coal geology (Fig. 2) should production. The Scottish Coal Company Ltd,
be considered for overall prospect apprai- and Rock Mechanics Technology Ltd are
sal, with their relative importances refined thanked for approval to use material related to
for individual wells, or groups of wells. Longannet Mine. R. A. Gayer, P. Gillespie and
Given the cost of data acquisition, it is T. Hathaway have suggested valuable modifica-
important to honour all available infor- tions to an earlier draft. Views expressed in this
mation. Extensive practical experience in paper are those of the authors and not
coal geology is required to achieve this. necessarily those of any of the above-mentioned
(iii) The integration of all data resources, from companies.
historical mine plans through to new
seismic reflection data, is also essential,
particularly where fault plane dips are low.
The construction of cross sections normal References
to the fault trends will often be necessary
to achieve this. These cross sections BAILEY, H. E., GLOVER, B. W., HOLLOWAY, S.
(1:5000 is suggested as suitable for such YOUNG, S. R. 1995. In: WHATELEY, M. K. G. &
SPEARS, D. A. (eds) European Coal Geology.
data integrations) constrain the interpreta- Geological Society, London, Special Publication
tions and allow accurate assessment of 82, 251-265.
throw variations and the extent of strained BARNETT, J. A. M., MORTIMER, J., RIPPON, J. H.,
ground. WALSH, J. J. & WATTERSON, J. 1987. Displace-
(iv) Specifically regarding faulting, interpreta- ment geometry in the volume containing a single
tion should seek to combine all available normal fault. AAPG Bulletin, 71, 925-937.
408 E. L. B O A R D M A N & J. H. R I P P O N

CHILDS, C., WATTERSON,J. & WALSH, J. J. 1995. Fault wrench faulting under different initial stress states.
overlap zones within developing normal fault Journal of Structural Geology, 8, 737-752.
system. Journal of the Geological Society, ONIONS, K. R. & WHITWORTH, K. R. 1995. Applica-
London, 152, 535-549. tions of electrical borehole imaging to mining
CREEDY, O. P. 1988. Geological controls on the design. Scientific Drilling, 5, 69-75.
formation and distribution of gas in British Coal PEACOCK, D. C. P. & SANDERSON, D. J. 1994.
Measures strata. International Journal of Coal Geometry and development of relay ramps
Geology, 10, 1-31. in normal fault systems. AAPG Bulletin, 78,
DANIELS, E. J., ALTANER, S. P., MARSHAK, S. & 147-165
EGGLESTON, J. R. 1990. Hydrothermal alternation RAWNSLEY, K. D., RIVES, T., PETIT, J. P., HENCHER,
in anthracite from eastern Pennsylvania: implica- S. R. & LUMSDEN,A. C. 1992. Joint development
tions for mechanisms of anthracite formation. in perturbed stress fields near faults. Journal of
Geology, 18, 247-250. Structural Geology, 14, 935-951.
GIBSON, J. R., WALSH, J. J. & WATTERSON, J. 1989. RIPPON, J. H. 1985. Contoured patterns of the throw
Modelling of bed contours and cross sections and bade of normal faults in the Coal Measures
adjacent to planar normal faults. Journal of (Westphalian) of northeast Derbyshire. Proceed-
Structural Geology, 11, 317-328. ings of the Yorkshire Geological Society, 45,
HATHAWAY, T. M. & GAYER, R. A. 1996. Thrust- 147-161.
related permeability in the South Wales Coalfield, - - & RAINE, J. D. 1986. Some methods of assessing
UK. In: GAYER, R. & HARRIS, I. (eds) Coalbed fault pattern variations in the East Midlands
Methane and Coal Geology. Geological Society, Coalfield. The Mining Engineer, April 1986.
London, Special Publication, 109, 121-132. ROBERTSON, E. C. 1983. Relationship of fault dis-
KAISER, W. R., HAMILTON, D. S., SCOTT, A. R., placement to gouge and breccia thickness. Mining
TYLER, R. & FINLEY, R. J. 1994. Geological and Engineer, 35, 1426-1432.
hydrological controls on the producibility of STEVENS, S. H. 1993. Coalbed methane - state of the
coalbed methane. Journal of the Geological industry, Piceance Basin, Colorado. Quarterly
Society, London, 151, 417-420. Review of Methane from Coal Seams Technology,
KNOTT, S. D. 1994. Fault zone thickness versus ll, 23-27.
displacement in the Permo-Triassic sandstones WALSH, J. J. • WATTERSON,J. 1990. New methods of
of NW England. Journal of the Geological Society, fault projection for coalmine planning. Proceedings
London, 151, 17-25. of the Yorkshire Geological Society, 48, 209-219.
KUUSKRAA,V. A., LAMBERT,S. W. & SCHRAUFNAGEL, & 1992. Populations of faults and fault
R. A. 1994. Black Warrior coalbed methane displacements and their effects on estimates of
productivity improvement project. Quarterly fault-related regional extension. Journal of Struc-
Review of Methane from Coal Seams Technology, tural Geology, 14, 701-712.
11, Nos 3, 4, 50-55. WHITWORTH, K.R 1994 (ed.) Investigation into the
LINDSAY, N. G., MURPHY, F. C., WALSH, J. J. & Effects of Lithology on the Magnitude and Ratio of
WATTERSON, J. 1993. Outcrop studies of shale in-situ Stress in Coal Measures. Commission of
smears on fault surfaces. Special Publication of the the European Communities, Directorate General
International Association of Sedimentologists, 15, for Energy, ECSC Agreement No. 7220-AF/845.
113-123. WOODCOCK, N. & FISCHER, M. 1986. Strike slip
NAYLOR, M. A., MANDL, G. & SIJPERSTEIJN,C. H. K. duplexes. Journal of Structural Geology, 8,
1986. Fault geometries in basement-induced 725-736.
 Geological research into gas sorbed in the coal seams of the
Carboniferous in the M~eno-Roudnice Basin, Czech Republic

V. HOLUB ~, M. ELI.AS l, P. H R A Z D I R A ~ & J. F R A N C U 2

1 Czech Geological Survey, Kldrov 3, Prague 1, 118 21, Czech Republic

2 Czech Geological Survey, Leitnerova 22, Brno, 602 00, Czech Republic

Abstract: In 1994 research in the Czech Republic began into coalbed methane (CBM). The
target of this research is the coal seams of the M~eno-Roudnice Basin, in the region
between M~lnik and Benfitky nad Jizerou. This region was chosen as a model area for
evaluating the CBM potential in the Permo-Carboniferous continental basins in the
Bohemian Massif. The first stage of the work was directed towards obtaining data for basin
analysis, the completion of lithological, stratigraphic and structural surveys particularly
concentrated on fault deformation of the basin filling. A general study was conducted into
the problem of the sorbed gases with respect to the occurrence of CBM. The latest
interpretation of laboratory analysis of the M61nik Main coal seam shows a methane
content of 4-10m3/t in the coal at a depth of 250 to 800m.

The Czech Geological Survey in collaboration of Prague. The M~eno-Roudnice Basin is shown
with Energie Kladno a.s., the Faculty of Natural in the map of the continental type of the Permo-
Science of Charles University, Prague and the Carbinerous basins of the Bohemian Massif
Institute of Geonics of the Academy of Sciences (Fig. 1).
of the Czech Republic, Ostrava, in 1994 began The crystalline basement of the Mgeno-
research into coalbed methane (CBM) potential. Roudnice Basin is predominantly composed of
The target of this research is the coal seams of the epi- to mesozonal metamorphosed Proterozoic,
M~eno-Roudnice Basin, in the region between which in the eastern and south-eastern parts of
M61nik and Benfitky nad Jizerou (Fig. 1). This the basin is partly overlain with slightly meta-
region was chosen as a model area for evaluating morphosed Ordovician rocks belonging to the
the CBM potential in the Permo-Carboniferous Caradocian. These units form a part of the
continental basins of the Bohemian Massif. This Bohemicum in the sense used by Mahel' et al.
paper presents the results of the initial stage (1984). A strip of volcanic rock of granodiorite
of research. to diorite type extends below the southern wing
of the Carboniferous basin, classified by Mahel'
et al. (1984) as Moldanubicum.
The sedimentation of the Late Palaeozoic in
Geological setting the major section of the M~eno-Roudnice Basin
began with the N ~ a n y Member (Westphalian D)
The M~eno-Roundnice Basin was chosen as a of the Kladno Formation. The strata sequence
model area because geophysically and through continues through to the Lin~ Formation
drilling it is currently the most extensively (Stephanian C to lower A u t u n i a n ) - as shown
investigated continental Permo-Carboniferous by the profile of the Zd6tin borehole Zd-1
basin in the Bohemian Massif, with total proved (Table 1).
geological coal reserves of 1 286922kt (Bosfik The Radnice Member was identified in only a
& Zbfinek 1992). The results of research into this small part of the basin, near its south-eastern
basin to date have been summarized by Holub border in the vicinity of M61nik. In most of the
& Tfisler (in Malkovsk~, et al. 1974), Holub & southern part of the basin, the N~[any Member
Tfisler (1981) and Bosfik & Zbfinek (1992). forms the basin fill but it wedges out to the north
In accordance with Holub & Pegek (1992) we and north-east. In this area, sediments of the
consider the M~eno-Roudnice Basin as one of T~nec Formation are the basal lithostratigraphic
the basins of the Central Bohemian region of the unit of the Carboniferous basin fill. The N~,[any
continental Late Palaeozoic basins of the Bohe- Member is the oldest coal-bearing unit in most of
mian Massif, lying to the east of the K l a d n o - the basin. The major development of the Slan~
Rakovnik Basin and to the west of the Formation distinguishes the M~eno-Roudnice
Mnichovo Hradi~t6 Basin. It is situated NNE Basin from the other regional-geological units

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 409-423.
410 V. HOLUB E T AL.

t .,~'7
i.~-" ~ - : . : : S ' ; --~ --.,~s
. . .-,._
<.....'.~ f , .-
~.~ , r -;. j -"~,~,~, " .
./'..:...: .~, ~ ~ ~.~

9. . . . : . - -...-r

,~..a,.~" ~ "~
. . - . ""/ -". ' ". .'+.'. ~~.- -o

r I?:".".-'/:-".": "~
.3 -'. " " ".'--."" "- ~,

9 .If!i-.'. -. :-.- .r
.~ L . / : : :.'.'." : : " - : "?."~
9 ,%_. :-.':-.: . : . :-.-.:-,:;
F'":: ~".'~- ".'::'!~, ~-

! ['::': : : , ' ~ 11t~--'+ IIIII U I b 2' a

t :';, A , . ~ ~llli." .
<r-;'~+.~-'~ ~1111%.

N
,'~ ~ +,. = -.,

J' -.Z'::.'.:~ 9..0 i

~:I9 ~- 9. .::..-..'~,,,d
9
. . --t )/,
." 0 " " p
z -, o
0
\ ~2 i _-
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E
.X
O.
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~. x-
-." / . _~-}"
H
(D.

O.

(D,
,I-

o
/
 GAS SORBED IN CZECH REPUBLIC COAL SEAMS 411

Table 1. Stratigraphy and coal-bearing sequences in the Zddtin (Zd-1) borehole (Mgeno-Roudnice Basin)
(Holub 1994)
I !
s~ra% i g r a p h y I
[
.... coal seams [ depth to)l thickness
general stratLgraph, scale I l o c a l s%ra%igr, scale (in metros) (fros - (in metres)
I I
Qua~er.! I o.o-i.3 I 1,3
C
I
! iIT I u p p e r
iu"
[ Teplice I 1~ 1 4,5
R i-- !
E I Ir[ m i d d l e Jizcra I 5,8-239,4 ti
T u lo - I! 233,6
A l P i r~! 1 . . . . B i lakn d Horn !
C
E -" lol , 1239.4-281,4 1 42,0
O r icier ne Xot'Tc~ny - ! I
U
S
!:!-*'*
I ~t ~resh-
Peruc ai nl et uerrocpael lai tt ieos n s
with coal
l
1281.4-289"1 I
l !
7~

subst.admixture [ !
I

' lower
iPermian !i lower Lln~ - 126901-583,6
!
!
I
!
f
294,45

u I'. I C I __
Kamenn~ Mos~ - ] 589,&-596,0 i 14.45
t.sl i I
l i m

r eI i Kounov barren e q u i v a l e n t i I
os ~he Kounov C o a l s 1598"0-613"4 i 15,35

e
'!i
I
I I
I
I
I
.
Ledce
.
-
m
] 1 . - -
)613,4-639,2 ]
u ~
25,80
r I I s Slant I Htedle - 1639,2-761', 8 I 122.60
b lal i - 761,'8-770,9 I 9,15
o inl !
n I I Jelentce u p p e r sea
I
770.90-771.78 (0,88)

I
!
!
I
I
1 c o o t s / gun punch c o r e
:768.30-796,25 (0.94)
l n t e r b ~ l c o a l seam
778.27-778,34 (0,07)
I

I
s I. ,
! coring gun punch c o r e
:77R,20-778060 (0,40)
770,9-841,0 70,1
I t main seam !
4 I i 7 8 4 , 2 7 - 7 8 7 , 6 2 (3,35)
l 1 c o r i n g gun punch c o r e (
I I f : 7 8 1 , 5 0 - 7 8 5 , 2 0 (3,70) I
I 1
T~nec 841,0-910.1 69,1 1

t ,Iel I '[
with barren I I
e(Dlivalents
' Iii
IPi ~ i *-~ Nttaay os t h e
Nt~any C o a l s
carbonised stems
(968,fl5-969,15) I
910,1-989,4

,
79,3 !
I

,.! i 1 i
I
t!
IPROTEROZOIC
i 989,4-1042,2 52.85

Fig. 1. Permo-Carboniferous basins in the Bohemian Massif (of continental character with the area studied)
(Holub 1994). 1. Permo-Carboniferous basins of the Sudetic region: a, Cesk~ Kamenice Basin; b, Mnichovo
Hradi~t6 Basin; c, Krokono~e-Piedmont Basin; d, Intra-Sudetic Basin; e, occurrences in the Orlick6 hory Mrs;
f, Orlice Basin. 2. Permo-Carboniferous basins of the Central Bohemian region: a, Plzefi Basin; b, Man6tin Basin;
c, Radnice Basin; d, Zihle Basin; e, K l a d n o - R a k o v n i k Basin; f, M~eno-Roudnice Basin; g, occurrences in the
neighbourhood of Krava~e. 3. Late Palaeozoic in the Krugn6 hory Mts: a, occurrence at Brandov; b, occurrences
at Teplice and Moldava. 4. Permo-Carboniferous sediments of the Furrows: a, Blanice Furrow; b, Boskovice
Furrow; c, Jihlava Furrow. 5. Researched area.
412 V. HOLUB E T AL.

of the Permo-Carboniferous of the central and Tectonic Pattern

western Bohemian region. Its oldest unit, the
Jelenice Member, is most fully developed in the An outline of the tectonic characteristics of the
Mgeno-Roudnice Basin of all the central Bohe- basin has been given in the previous section.
mian basins, both with respect to maximum Opinions concerning the fault structure of the
thickness and relative coal-bearing richness. The Mgeno-Roudnice Basin depend on the level of
most significant correlation horizon of the entire knowledge and the divergence in conceptual
Permo-Carboniferous filling is the Mgec Member approach of individual authors. The basic
which forms the roof of the M~lnik Coals. In the characteristics have been presented by Holub &
eastern section of the basin, the thickness of the Tfisler (1981). They distinguished two basic fault
upper part of the Slan~ Formation decreases systems: one striking NE-SW (transversal to
markedly; considering the nature of sedimenta- the structural lines and in places, especially to the
tion, it is clear that it is caused by the primary east of the studied area, twisting towards the
reduction of the later units of the Slan~ Forma- Rhine direction) and the other generally younger
tion strata. The Ledce and Kounov members than the Sudetic system (NW-SE, twisting in
which locally are only occasionally coal-bearing, places towards WNW-ESE) striking parallel
are reduced to only a few metres of coal-rich to or obliquely with the direction of the axis of
layers and the Kamenn2) Most Member is notably the basin.
reduced or, in some places, totally absent. Many faults are shown in the tectonic map by
The Lin~ Formation is the thickest lithostrati- E. Stanik (in Zbanek et al. 1991). In contrast
graphic unit. It forms the transition between the with the above outline there is a conspicuously
characteristic features of the Central Bohemian large number of faults trending W N W - E S E in
and Sudetic Permo-Carboniferous regions: in the the southern section of the basin.
eastern section rock types which are also char- A preliminary suggestion of the possibility of
acteristic of the Krkonoge Piedmont Basin can block dissection of the Mgeno-Roudnice Basin
be observed. In the lower section of the Lin~ into basement blocks was put forward by
Formation, the correlative Zd~tin Horizon St~p/mek (in Holub et al. 1994). Three basic
occurs. It is overlain by conglomerates containing zoned blocks are characterised by various levels
pebbles of Silurian and Devonian limestones of tectonic fractures, while one of the distin-
from the Barrandian area. In all formations of the guishing phenomena is also the varied homo-
basin the products of explosive volcanic activity genity of the Carboniferous basement. The
are present. These are found most frequently in eastern and western blocks are notable for the
the Lin6 and Slan~, formations, where they are presence of narrow trough structures restricted
predominantly of rhyolitic composition, and by steeply dipping faults in the Rhine direction.
rarely of intermediate to basic character. The central block is relatively less disturbed with
The Mgeno-Roudnice Basin is structur- fewer subsiding dislocations of both main
ally asymmetric with a basinal axis trending systems. The most eastern block is characterised
WNW-ESE. The cross section through the basin by greater morphological dissection of the base-
is shown in Fig. 2. ment with some crystalline uplifts with no
The Permo-Carboniferous basin-fill is tecto- Carboniferous cover. Partial depressions con-
nically disturbed by frequent faults, predomi- tinue to the eastern Mnichovo Hradigt6 Basin
nantly radial in character. Their vertical throw and, from a regional facies point of view, belong
ranges from tens to hundreds of metres. to the Sudetic region. The essential character-
The Permo-Carboniferous filling of the basin is istics of the tectonic structure of the Mgeno-
overlain by an Upper Cretaceous cover which Roudnice Basin based on a synthesis of knowl-
overlaps it with a slight discordant unconformity. edge to date, are shown in Fig. 3.
The Cretaceous sequence is stratigraphically
limited at its base by freshwater Cenomanian,
and at its roof by deposits belonging to the lower Coal deposits
Coniacian. Their lithology is very varied depend-
ing on the fact that the Cretaceous filling Bituminous coal seams occur in the basin at four
of the Mgeno-Roudnice Basin is located on stratigraphic levels. The most significant is the
the borders of four facies regions- Prague M61nik group of seams located in the Jelenice
(Vltava-Berounka), Lu~ice, Jizera and Labe. Member of the Slan~, Formation (Stephanian B),
The predominant section of the Cretaceous followed in importance by the N~,~any group of
basin-fill belongs to the sediments of the middle seams in the N2)~any Member (Westphalian D)
Turonian; the upper Turonian and Coniacian of the Kladno Formation; the Kounov group of
deposits occur only as denudation relics. seams (Stephanian B - upper section) was noted
 t~

I
l~l Z
'0 0
H
~§
E
E =~ i

+'4---
E
E
0

0
H
m ~ ~~ o
0
t~
I
o I ' ~ ~"-
o~ I,~;- ~

~D
~,~ 0 ~ 0

~..,~ ~ =
~'~ ~-~

"~ ~ 0 =.~
~ ~
-4"
'~ ~ ~ ~

~ ~ ~;-~
~ ~'~
f~

D
~ ~ ~
co ~ ~ 0 ~
414 V. H O L U B E T AL.

I
, t .i'

I
O
s
/
z~

, ,,,,~

t'-
~.Q,J
Z , , ~ . ~ . . , m
.a
 GAS SORBED IN CZECH REPUBLIC COAL SEAMS 415

in a small area. In the lower section of the Lin~ N and S borders of the basin (Bosfik & Zbfinek
Formation, thin coal seams occur in the Zd6tin 1992).
Horizon (see Table 1). The M61nik Interjacent coal seam was found
It is possible to divide the Mgeno-Roudnice in its usual thickness only in the SE section of
Basin into the three coal deposit areas: the the Benfitky nad Jizerou area, the M~lnik Upper
Mfilnik area, the central part of the basin and seam in the NW and NE sections of the M61nik
the Benfitky nad Jizerou area. area, and in maximum thickness in the southern
In the N)~any Member (Kladno Formation) section of the Benfitky nad Jizerou area. In the
it is possible, according to Bosfik & Zbfinek Kounov Member it is possible to delineate the
(1992), to recognize six groups of coal seams Kounov Coals with five seams. The Kounov
which they name N R 0 to N R 5 . Mostly these seam was located at its maximum thickness only
contain 1-2 thin coal seams, and in places only in the NW section of the M61nik region, and
coal representatives or coal seam equivalents. mainly after that in the centre of the Central and
Coal formation in the N ~ a n y Member gradu- Benfitky nad Jizerou areas.
ally extended from the SW section of the M61nik Scant coal formation was noted in the Zd6tin
district in a NE direction, so that the seam group Horizon of the Lin~ Formation in the lower
N R 4 has already expanded to cover almost the section of the strata unit. The Zd6tin Coals are
entire area. Seams N R 0, N R 2, N R 3, N R 4 are formed in five seams; however, only on the N W
identified as having a thickness greater than border of the M61nik area and in the Roudnice
0.4 m. Altogether, they are however without any section of the basin was the Zd6tin coal seam
great significance. found at maximum thickness. From an eco-
In the Slan~ Formation there are two coal- nomic point of view it is, however, insignificant.
bearing horizons: the M61nik and Kounov The remaining stratigraphic units of the
groups of coal seams. Permo-Carboniferous of the M~eno-Roudnice
Bosfik & Zbfinek (1992) zoned five groups of Basin are barren with respect to coal deposits.
coal seams within the M61nik Coals in the Rare thin seams occur only in the T~,nec
Jelenice Member. The base and lower M~lnik Formation and in the H~edle Member of the
seam had a greater thickness in the eastern part Slan~, Formation. They do not, however, have
of the Benfitky nad Jizerou area. The most significance as resource deposits.
important is the M61nik Main seam extending
regularly almost throughout the entire area
examined at a thickness of more than 1 m. Technological properties of coal
From the point of view of coal production as
well as of the occurrence of CBM, this seam is of Earlier technological exploration up to the
the greatest significance. It is lacking in only a present time was directed towards the character-
few places of the middle part in the deposit area ization of the coal from the viewpoint of classic
where it either was originally absent or has been mining and utilization. Technological character-
since eroded. Additionally, it was not found in i s t i c s - ash content, calorific value, specific
several boreholes at Kropfi6ova and M~lnickfi sulphur content with average values, review of
Vrutice, where it is most likely missing because the thickness of individual seams, as well as area
of faulting. Apart from this, the character of the and tonnage of recorded reserves of bituminous
M~lnik seam in the basin is regular. From its coal are shown in Table 2.
southern border, the basin slopes to the north at It should be noted that perhaps 40% of the
the southern border, it occurs at a depth of coal reserves are located in the protected water
between 160-200 m; in the north, it has a depth sources area.
of 900-1000m. At the southern border, it is From the point of view of a total technolo-
limited through erosion or tectonic faulting. In gical evaluation, the main resource is the M61nik
the W and N directions the seam slowly wedges Main seam, which is both the best in quality and
out or diminishes. The Jizera fault system has the most significant in quantity. Its quality is
probably contributed to its being restricted in mostly very good and raised sulphur content
the east part of the basin. So far it has not been occurs only locally.
possible to determine its continuation towards However, some harmful elements are present
the NW (towards the Lib~chov borehole), and in significantly high proportions, e.g. arsenic
further in the east from the borehole at Brodce (average content 154 g/t), zinc (average 307 g/t),
in the vicinity of Ben~itky nad Jizerou. A mercury (average 0.25 g/t) and fluorine (average
connection of the M~lnlk Main seam from the 0.018%).
M~lnlk area to the Benfitky nad Jizerou area was Technologically the coal is evaluated as
found in the central coal deposit-area along the energetic (useful for power plants), combustible,
416 V. HOLUB E T AL.

Table 2. Average technological parameters and coal geological reserves of individual seams in the MYeno-Roudnice
Basin (after Bos6k-Zbdmek et al. 1992)

Coal seams Average technological parameters Area Tonnage

(103 m 2) (kt)
Thickness Ash (Ad) Calorific value Specificsulphur
(m) (%) (Q ~MJ/kg) (g St/M J)

Zd6tin 0.42 51.35 13.13 1.30 2 544 1 818

Kounov 0.68 53.20 11.81 2.07 27 862 32 588
M61nik Upper 0.58 44.26 15.26 0.68 51 020 47911
M~lnik Intrabed 0.48 42.48 10.13 0.53 13 064 9 958
M61nik Main 2.22 31.98 19.26 0.95 308 618 1 010 044
M61nik Lower 0.49 32.31 19.16 1.30 12 851 9 308
M61nik Basal 0.44 17.97 21.21 0.37 1 918 1 140
N~,~any 4 0.58 34.81 17.82 3.44 71 249 62116
N~any 3 0.61 34.69 17.99 3.44 81 327 74428
N2~any 2 0.51 38.47 15.89 3.84 17866 14071
N~any 0 0.58 43.27 14.82 4.27 6 008 5 540

poorly sintering, commercial group V I A with than coal from the M61nik Main seam from the
average numeric code 622, easily adjustable, same locality. In contrast, coal from the
with good floatability, but without independent N ~ a n y seams is of higher rank than coal
coking capacity. It is predominantly susceptible from the M61nik Main seam in the same
to self-ignition and its dust is evaluated as locality. Analyses of coal seams and associated
explosive. The ash of the M~lnik Main coal rocks of the M61nik Coals from boreholes in
seam is of medium fusibility, with an average the Benfitky nad Jizerou area are presented in
value of around 1350 ~. Table 3.
Special exploration for natural gas or CBM The characterization of the coal properties
was not undertaken earlier in the M~eno- from samples taken all over the M~eno-Roud-
Roudnice Basin, as previous exploration was nice Basin is shown in the Table 4.
directed towards evaluation of the coal deposit The following properties were determined for
and its possible suitability for coal production. each sample: the thickness of the M61nik Main
The occurrence of methane in coal seams was seam; depth in the borehole; ash content;
observed only superficially and non-systemati- vitrinite reflectivity; maceral characteristic;
cally. The method used for setting technological volume of volatile matter; total volume and
and geochemical parameters did not enable the surface of pores; porosity; potential gas content
measurement of the sorption properties of the with respect to methane; pore size and perme-
coal seams, their porosity and other properties ability. To enable mutual correlation, all tests
essential to the evaluation of possible CBM were carried out on identical samples.
reserves. It was thus necessary to undertake Contour maps were constructed from the data
special research to measure the sorption proper- obtained:
ties of the coal seams, their porosity, perme-
ability and other properties essential for the (a) depth of deposition and the thickness of the
estimation of CBM reserves. M61nik Main seam;
The main target of the research was the (b) ash content in dry matter and the thickness
M~lnik Main seam. Samples of coal were taken of the M61nik Main seam;
from 23 exploration boreholes throughout the (c) porosity, potential gas bearing content and
area representing the variable quality of coal the thickness of the M~lnik Main seam;
from the M61nik Main seam over the entire (d) vitrinite reflectivity R0, content of volatile
studied area. Concurrently, samples of coal matter in combustible coal material and the
from the Kounov and N~,[any seams were also thickness of the M61nik Main seam;
taken from several of these boreholes. These (e) total pore volume, potential gas bearing
coal seams are found in only some sections of content and the thickness of the M~lnik
the basin and represent only completion of the Main seam;
coal reserves, with coal which has different (f) total pore surface, potential gas bearing
properties from that of the M61nik Main seam. content and the thickness of the M61nik
Coal from the Kounov seams is of lower rank Main seam.
 GAS SORBED IN CZECH REPUBLIC COAL SEAMS 417

Table 3. Analyses of coal seams and associated rocks of the MYlnlk Coals from boreholes in the vicinity of Benftky
nad Jizerou (Klibfni, NYmec et al. 1994)

No. of Collection Seam label Reflectance Mineral Maceral analyse

sample depth R0 part
Vitrinite (%) Inertinite (%) Liptinite (%)

1 686.5 overlying - 85 - - -
2 687.5 sandstone - 80 - - -
3 688.2 - 82 - - -
4 688.6 M61nikUpper 0.59 25 70 30 -
5 689 coal seam 0.59 30 65 35 10
6 691.7 sandstone - 79 - - -
7 692.2 M~lnik Main 0.56 35 70 25 5
8 692.3 coal seam 0.55 38 67 26 7
9 692.5 0.55 32 65 31 4
10 692.7 0.57 26 69 28 3
11 693 0.58 28 70 24 6
12 693.5 0.58 33 68 28 4
13 693.7 - 74 - - -
14 693.9 0.54 23 63 28 9

From the contour map of vitrinite reflectivity geological development of the basin. These are
R0 and volatile matter in combustible coal primarily the origin and development of post-
material it can be seen that with an increase in Carboniferous formations including heat, tec-
depth of the seam deposit there is a rise in vitrinite tonic and hydrogeological effects.
reflectivity and a decrease in the content of Concurrently with the geochemical evaluation
volatile matter in the combustible coal material of the coal samples from the M~eno-Roudnice
and vice versa. Basin, a complex evaluation of knowledge
Similarly it follows from the contour maps of obtained from an exploration borehole drilled
total porosity, total pore volume and surface at Zd6tin was also undertaken (borehole Zd-2).
area in relation to potential gas content of the The results showed that the Upper and Main
M61nik Main coal seam, that increase in depth M61nik seams at a depth of 690m represent a
leads to a significant reduction in the porosity of similar coal type and are differentiated from each
the coal material which is also associated with a other by ash content, which is in agreement with
lessening of the total pore volume and surface the results of borehole log measurement. The coal
area and simultanoeusly also of the potential cores obtained were tested not only for coal
gas-bearing property of the coal. These changes quality, but also examined in detail for the
in reflectivity, volume of volatile matter and evaluation of the quantity and quality of deso-
porosity of the coal material indicate changes in rbable gas ('container test'), from which was
coalification which increases with depth of the ascertained a gas-bearing value of 10.8m 3 t -1.
M~lnik Main seam. Where the M~lnik Main The composition of the desorbed gas was
seam can be found at shallow depth, which is in consistent with the composition of natural gas.
the south of the M~eno-Roudnice Basin, values The results of this desorption test in relation to
were obtained that showed greater porosity, the seam depth and other properties of the coal
lesser reflectivity and a raised content of volatile and in correlation with results obtained from
matter and simultaneously a higher gas content. analysis of the coal from the M61nik Main seam
The character of the coal material in the M61nik from further boreholes, suggests the existence of
Main seam, together with the values for reflec- prognostic reserves of methane held in the
tivity, total porosity and potential gas content M~lnik Main seam. Confirmation of this predic-
show that this seam has the necessary qualities tion is the subject of further research.
required for the sorption of CBM produced The results of the analysis of the coal seams of
during the coalification process. Whether that the M61nik Coals and associated rocks from the
quality of the coal material in itself is adequate newly-drilled borehole at Zd6tin, and samples
for the seam to hold a significant volume of taken from earlier boreholes drilled N of
producable methane (desorbable), depends on Benfitky nad Jizerou, are presented in Tables 3
factors which determined the presence and and 4.
418 V. HOLUB E T AL.

Table 4. Basic characterization of the coal properties from samples of the entire Mgeno-
Roudnice Basin (Klib6ni & N~mec 1994)

Sample Depth (m) Coal w a ( % ) Aa(%) vdaf(%) R0(%)

JB-1 Jabkenice 820 M61nik 2.01 9.8 41.43 0.62
823 M~lnik 2.11 18.77 39.93 0.69
BC-1 Brodce 515 M61nik 2.01 22.36 34.5 0.7
550 M61nik 3 12.6 38.18 0.69
770 N~any 3.13 20.71 45.33 0.73
Hu-1 Hrugov 460 Kounov 1.33 39.01 65.12 0.54
CHT-1 Chot~tov 1080 N2?~any 1.58 28.54 45.39 0.65
KBL-1 Kbel 250 M~lnik 3.08 18.8 43.66 0.57
SVK- 1 Sovinky 907 M61nik 3.12 16.03 48.46 0.66
927 M~lnik 0.75 18.57 67.66 0.62
SS-1 Su~no 724 M~lnik 1.07 53.15 46.94 0.71
745 M~lnik 2.33 26.94 41.92 0.7
749 M~lnik 1.83 13.47 43.21 0.68
907 NS,~any 1.71 18.04 38.28 0.75
DS-1 Dolni Silvno 288 M~lnik 3.25 35.09 43.07 0.53
315 M61nik 3.9 24.22 43.17 0.56
KV-1 Kropfi6ova Vrutice 490 N2}~any 2.31 22.77 44.92 0.57
MV-2 M61nik6 Vtelno 683 M61nik 2.29 18.16 41.96 0.59
825 N~,~any 3.43 20 42.77 0.62
SZ-1 Stfi~ovice 327 M~lnik 3.96 7.15 41.61 0.58
HS-1 Hostin 500 M~lnik 3.06 11.41 45.52 0.58
693 NS,~any 1.7 22.43 42.44 0.6
KRP-1 Krpy 284 M~lnik 2.73 11.14 44.24 0.53
CHO-1 Choru~ice 793 M~lnik 1.87 21.77 49.69 0.6
948 N~,~any 1.99 21.12 45.59 0.68
VUJ-1 VelkS,Ujezd 748 M61nik 2.76 36.84 45.36 0.57
RD-1 Radoufi 660 M~lnik 2.07 30.77 50.3 0.59
844 N~:~any 2.74 12.29 38.01 0.67
SI~-I St~emy 843 Kounov 1.17 38.81 35.04 0.73
1025 M61nik 2.23 27.16 47.03 0.72
1035 M61nik 0.65 34.28 47.58 0.7
VS-1 Vysokfi 944 M61nik 1.17 19.85 42.18 0.72
MUJ-1 Mal~: Ujezd 155 M61nik 4.46 12.52 43.56 0.48
LBL-1 Liblice 250 M61nik 4.71 24.36 53.33 0.52
LBL-2 Libllice 234 M61nik 4.58 22.59 44.09 0.53
BS-3 By,ice 241 M61nik 3.68 21 44.33 0.55
BS-4 By,ice 356 M61nik 3.97 31.07 41.83 0.55

Thermal history of the ture. If that led to a disturbance of balance, it

M~eno-Roudnice Basin could have caused desorption of gas from the coal
and its migration from the coal seams, or
Prognosis of CBM and its recognition for possible conversely it could have produced suitable con-
production requires detailed information con- ditions for its sorption into the coal material
cerning the properties of the seams and of the through migration. Although quantification of
surrounding rocks. A m o n g the required charac- these data is difficult, a rough model is proposed
teristics are particularly the physical qualities of to outline the trends of heat development, the
the environment (especially those which affect the maturing of organic material, the formation of
migration of fluid), and knowledge of the condi- gas and the progress of subsidence and erosion.
tions affecting the balance between the solid stage The model of of burial and thermal history of
(the coal material of the seam) and the liquid and the M~eno-Roudnice Basin is based on:
gas phases (methane, carbon dioxide, carbon
monoxide, and nitrogen etc.). Conditions for the (a) analysis of the thermal history of the
state of balance changed during geological devel- M~eno-Roudnice Basin (Francfi et al.
opment with changes of pressure and tempera- 1994, Kone~n~ et al. 1994),
 GAS SORBED IN CZECH REPUBLIC COAL SEAMS 419

(b) analysis of compaction of sediments on the Geothermal data are used from the borehole
basis of changes in the volume density and Sedlec MB-21, where the relationship between
porosity of rocks in the borehole profiles temperature (t) and depth (d) is expressed:
(Kone6n~ et al. 1994),
(c) analysis of bio-markers (Francfl et al. t = 0.0318d+ 9.5(~
1994).
and where the heat flow q --79.6mWm -2.
According to (~ermfik (in Ibrmajer, Suk et al. For construction of the model, the evolution of
1989), the M~eno-Roudnice Basin has, from the the basin was divided into 'events', which have
point of view of the regional character of the either the character of sedimentation, erosion or
heat flow of the Bohemian Massif, an increased without sedimentation. Each event is charac-
fluid temperature which is typical for the region terised by the thickness of the deposits, time
of the Lu~ice-Labe line. This can be seen from interval, lithology of the rock, hydro-chemical
depth-temperature data obtained during studies qualities of the water and palaeo-climatic data at
of the boreholes St~emy MB-7, Brodce BC-1, the interface between the sediment and the water.
Kropfi6ova Vrutice KV-1, M61nick6 Vtelno MV- The heat flow for the given section and its change
1 and Sedlec MB-21. with time is based on the geotectonic position of
This anomalous of the heat flow follows a the basin.
NW-SE (Sudetic) direction. The thermal gradi- To calibrate a model of the thermal history of
ent of the borehole MB-7 is 31.5~ km -l, of the the studied area of the M~eno-Roudnice Basin,
borehole MB-21 31.8~ -1 and of the bore- the thermal maturity of the organic matter was
holes BC-1, KV-1 and MV-1 33~ -l. These measured. According to these data, Francfi et al.
gradients are used as a starting point for the (1994) proposed a model of burial, erosion and
model of organic material and for orientational geothermal history of the Late Palaeozoic and
assessment of the sorption process in the Cretaceous sediments for the studied section of
methane-coal system. the basin (Fig. 4).

Well: HPivno- 1
B u r i a l history (thickness decompacted) Temperature (C)

Jurassic ,, us Plle0ge
I,~ W~lt seoUon t
1"~ K~T~Ih
~K~c
-3 rC2"sln

2- Cgtno
C:-nm
E

.10

g
r

|
Q ~]
IZ3
BELOW
30- 60
30"C
[~ 6 0 - B0
I]ITII! 90-12o
[~ 1 ~ 0 - 160

3OOO
noo 2~o 1~o lko ob o
Time (mabp) IE$

Fig. 4. Burial and thermal history of the Hfivno-1 borehole: Sedimentation in the Late Palaeozoic was followed
by erosion during the Permo-Triassic to the Late Cretaceous. Additional post-Turonian sedimentation is assumed
followed by erosion of these missing units (Francfl 1994). PDIT M software has been used.
420 V. HOLUB E T AL,

The basis of this model was analysis of 3. Thermal maturation of organic matter con-
organic material from rock and coal. From nected with the formation of hydrocarbons is
these samples, mineral and total organic carbon also evident in the distribution of extracted
was analysed and Rock-Eval pyrolysis was saturated hydrocarbons. With increasing depth
performed. Further analysis of bituminous there is a proportional increase in the content of
extracts with the aid of gas chromatography lighter homologues over heavier (C17-C21)/
and mass spectrometry was carried out on (C27-C31). It is therefore possible to deduce
selected samples. This analysis was directed that in the Carboniferous sequences, which are
towards identification of 'bio-markers', i.e. in today at a depth below 300 m the formation of
the group of organic materials, particularly the liquid hydrocarbons occurred. Conditions for
polycondensed structure of sterane and tri- their preservation were and are better than in the
terpane type. The main goal of this analysis shallower sediments of mainly Upper Cretaceous
was to identify the trend of maturation of age which are less influenced by compaction.
organic materials so that it would be possible Results from analysis of organic matter and
to test a model of the development of the studied from the model of the geothermal history of the
section of the Mgeno-Roudnice Basin from the studied section of the Mgeno-Roudnice Basin
point of view of the possible presence of CBM. can be summarized as follows.
Examples are given in Fig. 5 which shows the 1. According to the vitrinite reflectance and
maturity of organic material in relation to depth, the index of isomerisation of bio-markers, the
shown as the index of isomerisation of bio- level of maturity (coalification) increases with
markers. depth in the borehole. At the boundary between
The following conclusions can be derived. the Cretaceous and Permo-Carboniferous there
1. At the boundary between the Cretaceous is a jump in maturity from which it may be
and Permo-Carboniferous there is an obvious deduced that after deposition of the Permo-
partial jump in maturity. Carboniferous and before Cretaceous sedimen-
2. The increase of maturity with depth in the tation there was deep burial, and subsequent
Hfivno Hi-1 and Skuhrov Sh-1 boreholes shows erosion of a part of the section.
two parallel continuing trends in coalification, 2. Erosion in the SW part of the basin (in the
while the profile of the second of the examined vicinity of the Skuhrov Sh-1 borehole) appears
boreholes appears to be more uplifted and more to be greater than in the central eastern region
heavily eroded. (Hfivno Hi-1 borehole).

~ x~~ Skuhrov-1
200 --

_____X

Hrivno- 1
E
v i
"(:
9
<..., 400 '
EL
(D
a

<~~ Cretaceous
i.[] Carboniferous

800 i I ' I ' I '

0.00 0.20 0.40 0.60 0.80

22S/(22S+22R) ~13C31Homohopanes
Fig. 5. Biomarker maturity increase with depth in two boreholes: Hfivno-1 (in the E) and Skuhrov-1 (in the W)
(Franc6 1994).
 GAS SORBED IN CZECH REPUBLIC COAL SEAMS 421

3. Maturity of organic matter in the Cretac- Table 5. Geological and hydrogeological definition of
eous sediments reveals that these were also the MYeno-Roudnice Basin (elaborated by Hrazdira
buried to a greater depth than at present. 1994, after to the data by Boshk-Zbdmek et al. 1992)
4. The model of burial and thermal history of
Formation Member Coals Hydrogeological
the basin based on the above suggests the
unit
following events:
Kt Teplice
9 sedimentation of the N ~ a n y Member, T~nec Kj Jizera aquitard K1
and Slan~ formations (Westphalian D - Kb Bilfi Hora aquiclude K1-K2
Stephanian B) Kpk Korycany
9 sedimentation of a sequence perhaps 1400 m Peruc aquitard K2
thick (Stephanian C to Autunian) and its PC1 aquiclude K2-C1
erosion in the Upper Permian and Triassic PC s Kamenn~
and to a restricted degree in the Jurassic and Most
Cretaceous Kounov Kounov
9 sedimentation of the Peruc and Korycany Ledce aquitard C1
members and of the Bilfi Hora Formation H~edle
(Cenomanian - Lower Turonian), M~ec aquiclude C1-C2
9 hypothetical sedimentation of a sequence PC t Jelenice M~lnik aquitard C2
perhaps 1100m thick in the uppermost part aquiclude C2-C3
of Cretaceous, and its subsequent erosion. PC k N~any N~any aquitard C3
Radnice
5. The formation of hydrocarbons in the
deeper Carboniferous sequences took place PA o
mainly at the close of the Palaeozoic and also, PT
however, in part at the end of the Upper
Cretaceous. Legend: K t, Teplice Formation (Cretaceous); K j,
Analysis of the compaction of sediments of Jizera Formation (Cretaceous); K b, Bilfi hora Forma-
the Permo-Carboniferous (Konern~, et al. 1994) tion (Cretaceous); K pk, Peruc-Korycany Formation
led to similar results. (Cretaceous); PC1, Lin6 Formation (Permian and
Carboniferous); PC s, Slan~, Formation (Carbonifer-
ous); PC t, T2~nec Formation (Carboniferous); PC k,
Kladno Formation (Carboniferous); PAo, Ordovi-
Hydrogeology cian; PT, Proterozoic.
Knowledge of the hydrogeological relationships
of the M~eno-Roudnice Basin makes it pos-
sible to predict or to reject places as having a
likely concentration of CBM. The Permo- descending flow of groundwater is made
Carboniferous sedimentary filling of the basin more difficult by vertical and horizontal facies
can be hydrogeologically characterised as a changes, and by the decrease in permeability
collection of irregularly alternating rock strata of aquitards in relation to the depth of
of varying levels of permeability (from high rock deposition. Some hydrochemical properties
permeability, e.g. conglomerate and sandstone of groundwater in the Permo-Carboniferous
layers, to impermeable rocks: claystone and aquitards (e.g. low values of T.D.S. in compar-
siltstone). According to the hydrogeological ison with groundwater in Cretaceous aquitards)
properties of the rock there are restricted or higher values for rock filtration param-
hydrogeological aquitards and aquicludes in eters in aquitards indicating communication of
the profile of the basin (see Table 5) groundwater and CBM between hydrogeo-
Aquicludes prevent the communication of logical complexes. The migration of both
groundwater and CBM between aquitards. The groundwater and CBM via these communica-
comunication however permits tectonic distur- tional paths can be assumed.
bance and changeability of facies of the rock
complexes. In the hydrogeological aquitards
it is possible to predict the accumulation of Conclusions
CBM above all in aquitards within forma-
tions with M~lnik Coals. The enrichment of the After evaluation of the available geological data
Permo-Carboniferous aquitards occurs at and determining more precisely the lithostrati-
the aquitards outcrops outside of the basin. The graphic and tectonic structure with a view to the
422 V. HOLUB E T AL.

possible presence of CBM, it has been shown to 18%. With respect to sorption and desorption
be most important to concentrate attention on: changes, the volume of methane bonded to the
coal basically should not change. With a
9 the conditions for the formation and devel-
sufficient quantity of produced gas, the sorption
opment of CBM in coal seams dependent on
capacity, depending on the type of coal and
the geological conditions and the history of
coalification (coal rank), is roughly 9 m 3 t -1.
the Mgeno-Roudnice Basin, particularly
Starting from this point of evaluation, the
between M61nik and Ben/ttky nad Jizerou
difference between current gas volume and
area (lithology, tectonics, basin analysis)
sorbed gas volume may be considered to be
9 geochemical and mechanical properties of
losses caused by diffusion and transportation via
the M~lnik Main seam as a major source and
porous environments. It is not possible to
reservoir of CBM and on the characteristics
determine the dynamics of diffusion without a
of the surrounding strata as a sealing horizon
more detailed study of the transporting proper-
9 analysis of the hydrogeological relationships
ties of the rock. Calculations already made,
within the area with respect to the presence
however, show that uplift of the massif has
of CBM
occurred, and that therefore its permeability
A lithostratigraphic model of the filling of the may be also locally increased.
basin was produced and modifications were made
to the current tectonic model (Fig. 3). Stress fields During the preparation of the final version of this
in the basin were orientationally evaluated. work we used data supplied by the organizations
A basic contribution of this stage is the further which cooperated on the project of the Czech
Geological Survey, Prague entitled 'Geological
evaluation of post-sedimentational history of the
Research into Gas Sorbed in the Coal Seams of the
M~eno-Roudnice Basin using analysis: Carboniferous in the Mgeno-Roudnice Basin'. The
9 of compaction of sediments (evaluation of following co-workers of the following organizations
changes in the volume, density and porosity took part in the project: Energie Kladno, a.s. (Klibfini,
of rock at depth), L., N6mec, J., including Medek, Holub/t~, Dopita,
Kozfik, Kraus and H)ka), Faculty of Natural Science
9 thermal maturation of organic matter (bio- of the Charles University Prague (Hrfich, S. including
markers). Blecha, V., Kn~z, J., Kobr, M. and Skopec, J.),
Both methods show that on top of the Permo- Institute of Geonics of Academy of Science of the
Czech Republic, Ostrava (Kone6n~,, Petr, Martinec, P.,
Carboniferous, a sequence of strata roughly
Holub, K. and Kone6n~, Pavel).
1400m thick was deposited, and eroded before
sedimentation of the Upper Cretaceous
sequence. From the research carried out it was
further shown that the Cretaceous sequence References
reached a total thickness of perhaps l l00m. BOS,~K, P. & ZB,~,NEK, J. 1992. Geologiek~ pom~ry
Hydrocarbons were generated in the more lo(iska (erndho uhli M~lnik - Bendtky nad Jizerou.
deeply deposited strata of the Carboniferous Geologick2) Prfizkum. 1992, 11, 325-330. Praha.
mainly at the end of the Palaeozoic and also at FRANCU, J. et al. 1994. Anal/~za biomarker~ a model
the end of the Late Cretaceous. geotermickd historie sediment~t m~ensko-roudniekd
Primary attention was given to the deposi- pfnve. MS Archiv (;esk6ho geologick6ho fistavu.
tional and geochemical evaluation of the studied Praha.
region of the Mgeno-Roudnice Basin, from the HOLtJB, V. et al. 1994. Geologiek~ v~zkum sorbovanf~eh
viewpoint of the presence of CBM. 39 coal plynd v uhelnf~ch sloj[ch karbonu mYensko-roudniekd
pdnve. MS Archiv Cesk+ho geologick6ho fistavu.
samples were taken from 23 earlier-drilled bore- Praha.
holes, and these were fully studied geochemi- -- & PEgEK, J. 1992. H. Svrehni karbon a perm. In:
cally. Areal evaluation of these results is shown CHLUPA(~, J. & STORCH,P. (eds) RegiondJnd geo-
in the Table 4. logick~ dgleni Cesk~ho masivu na fizemi Cesk~ re-
Analysis of the condition for sorption and publiky (Regional geological division of the Bohe-
desorption of methane in coal is difficult because mian Massif on the territory of the Czech Repub-
of insufficient available data. Despite this, taking lic). 12as. Mineral. Geol., 37, 4, 263-267. Praha.
into consideration current work of similar -- & TASLER, R. 1974. Mladgipaleozoikum a spodni
trias v podloi Cesk~ kfidov~ p6nve (Late Palaeozoic
character, we can state that the effect of
and lower Triassic in the basement of the
reduction of pressure, e.g. as a result of erosion Bohemian Cretaceous Basin). In: MALKOVSK'I',
of the cover, is a reduction of the original et al. Geologie CeskO k(idovO p6nve a jejiho podloYi
volume by only 20%, while a reduction in (Geology of the Bohemian Cretaceous Basin and
temperature from 44~ to 20~ could by its basement). V~d. Ust~edni flstav geologiek~ v
contrast increase the sorption of methane by Academii, nakl. CSAV Praha.
 GAS SORBED IN CZECH REPUBLIC COAL SEAMS 423

-- & 1981. Geologie mgenskO p6nve a ?ernou- KONE(~NY,P. et al. 1994. Studium mo~nosti identifikace
heln~ch lofisek mezi M(lnikem a Ben6tkami nad stressovdho pole MYensko-roudnick~ pdmve. MS of
Jizerou. Sbor. geol. V6d, 1o~. Geol., Mineral., 22, the Institute of Geonics of Academy of Sciences
7-78. Praha. of the Czech Republic, Ostrava, Archiv Cesk6ho
HRACH, S. et al. 1994. Mgensko-roudnick6 p~mev. geologick6ho flstavu. Praha.
Hodnoceni st6vajlcich geofyzik6lnich pracL MS MAHEL, M., KODYM, O. & MALKOVSK'?, M. 1984.
Pfirodov~deck6 fakulty University Karlovy. Tektonick6 mapa CSSR. Geologick~, I0stav Dio-
Praha., Archiv Cesk6ho geologick6ho fistavu. n~,za St6ra. Bratislava.
Praha. MALKOVSKY, M. et al. 1974. Geologie (eskd k(idovO
IBRMAJER, J., SUK, M. et al. 1989. Geofyzikflni obraz p6nve a jejiho podlo~i. 0st~edni 0stav Geolo-
CSSR. Ust~edni lJstav Geologick~. Praha. gick~. Praha.
KLmANI, L., N~MEC, J. et al. 1994. V~skyt hoFlavOho ZB,~NEK, J. et al. 1991. Zdtv(re(n6 zprfva vyhled6vaciho
zemniho plynu v uhelnf:ch slojlch karbonu prdzkumu M ( l n l k - Benftky nad Jizerou. MS
Mgensko-roudnickd p6nve. MS Energie Kladno Geofond. Praha.
a.s., Archiv (~esk6ho geologick6ho fistavu. Praha.
 Method for estimating methane emissions from Polish coal mining

IRENEUSZ G R Z Y B E K 1, L I D I A G A W L I K 2,
WOJCIECH SUWALA 2 & RYSZARD KUZAK 3

1Polish State Mining Authority, ul. Poniatowskiego 31, 40-956 Katowice, Poland
2 Mineral and Energy Economy Research Centre, ul. Wybickiego 7 31-261 Krak6w, Poland
3 The Silesian University, Institute o f Earth Sciences, ul, B~dzihska 60,
41-200 Sosnowiec, Poland

Abstract: To improve the accuracy of estimations of methane emissions from coal mining, a
study of the Polish mine-specific method of methane measurement has been undertaken. To
carry out the study, the following assumptions have been made: (1) Methane emissions are
proportional to the gas content of coals; (2) The single mine average gas content is a
function of both exploitation depth and gas distribution; (3) The total volume of methane
released during mining is in proportion to the total gas content, while the volume emitted
from post-mining processes and from waste rock storage to the residual gas content. The
study has shown that: (1) There are four sources of methane emission from coal mining:
mining and post-mining processes, degassing systems and barren rocks storage; (2) Emission
from degassing systems should be measured directly, while the emissions from the other
sources could be estimated and characterized by release factors; (3) The release factors for
mining processes are described by parabolic equations, which have been defined by
comparing total measured emissions from venting and degasing systems with in-situ
methane content. For the remaining emission sources the factors are equal either to the
average residual gas content or to the total gas content, depending on the proportion of
residual to the total gas content; (4) Release factors and emissions, calculated for Polish coal
mining were found to be four times less than had been previously suggested.

Methane is one of the most aggressive green- factor (Win), which, multiplied by the amount of
house gases and a major source of its emission is coal produced (Q), enables evaluation of the
coal mining (Pyka 1993). Many attempts have global methane emission (E):
been undertaken to evaluate the amount of
methane emitted resulting from coal exploita- E = WmQ. (2)
tion. The assumption and results of those works
are described in detail in Smith & Sloss (1992) At first, the global average release factor for
and in the report of U.S. Environmental underground coal mines, evaluated on the basis
Protection Agency (EPA 1994). One of the best of American data, was assumed to be 27.1 m3/Mg
known is the evaluation by Boyer II (Boyer et al. (Boyer et al. 1990; OECD 1991). Then, after more
1990), the results of which are the basis of data were analysed (CIAB 1992), the suggested
the methodology of greenhouse gases emis- release factor for high emission (for mining and
sion evaluation approved by the Organization post-mining processes together) was 29m3/Mg
for Economic Cooperation and Development and for low emission 10.9m3/Mg (OECD 1991;
(OECD), during the Intergovernmental Panel on EPA 1994).
Climate Change (IPCC) in Paris (OECD 1991). In all of the above mentioned cases, when the
This methodology in its basic form assumes a basic form of OECD/IPCC methodology
linear relation between in situ methane content (termed 'global-average method') was applied
(G) and the so called 'release factor' (W), which to Polish coal mines (Boyer et al. 1990; CIAB
is a volume of methane emitted by a mass unit of 1992; Pilcher et al. 1991; Radwafiski et al. 1991),
coal exploited. This dependence is described by a the methane emission was overestimated. This
regression equation in the form: was, inter alia, the reason for undertaking the
development of the methodology of methane
W--- 2.04G + 8.16. (1) emission estimation on the basis of specific data
for individual Polish coal mines. As a result the
Where local data on the methane content are not so-called 'mine-specific method' has been devel-
available, the OECD/IPCC methodology sug- oped, and its theory and implications are
gests application of the global average release presented in this paper.

From Gayer, R. & Pe~ek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 425-434.
426 I. GRZYBEK E T A L .

Basic assumptions and the data used (1) Amount of methane emitted by a mass unit
in the study of coal produced, in all processes of coal
mining, is proportional to the average
In coal-bearing formations, methane is con- methane content of exploited coal seams.
tained both in coal seams and in surrounding (2) Average methane content of exploited coal
barren rocks. When coal is mined most of is a function of the depth-dependent dis-
methane is released, but some is retained in the tribution of methane content (Kotas 1994;
coal. The methane retained is termed residual Nie6 1993; Smith & Sloss 1992) and the
gas content. In coal, methane is mainly sorbed; depth of exploitation.
in barren rocks it exists as a free gas. In both (3) The difference in the rates of methane
cases the reservoir pressure is one of the release implies that during coal exploita-
principal agents in controlling gas content. The tion methane is released dynamically,
reservoir pressure can be assumed to be in whereas diffusion takes place after the
continuity between the coal and the surrounding mining process, from coal in post-mining
barren rocks (Tarnowski & Struzik 1978), so the processes and also from dispersed coal
amount of free gas in rocks is proportional to material in waste rock, mined together
the methane content in coal. Some examples with coal.
show that in Polish conditions the quotient of (4) Emission of methane from mining pro-
the methane volume contained in barren rocks cesses per mass unit of coal produced is,
(Vp) to the total volume of methane contained in therefore, proportional to the difference of
the coal formation (V) is similar to the quotient the average total methane content and the
of the residual methane content (Gr) to the total average residual methane content.
methane content (G) of coal: (5) Emission of methane from post-mining
activities and from waste rock heaps is pro-
Vp Gr portional to the residual methane content.
- (3)
V G
In the light of the above assumptions, to
Coal exploitation causes a decline in reservoir evaluate the emission from Polish coal mining
pressure in the area influenced by underground the following data were used: methane contents
workings. This results in methane emission from and residual methane contents of coal in Polish
rocks and coal. The methane contained in rocks is coal deposits, depths of coal exploitation in coal
released dynamically, with a rate that is propor- mines, amounts of coal produced, amounts of
tional to the gradient of pressure between the deposited waste rocks and the percentage of coal
underground opening and the unaffected rock material in the waste rock heaps. The evaluation
mass. Methane release from coal is somewhat was compared with data on emission, capture
different. At an early dynamic stage, its release is and use of methane in coal mines.
the same as from barren rocks (Grzybek 1993a). Data on the methane content and the rate of
When the pressure gradient approaches close to desorption - used to evaluate the residual
zero, the velocity of methane release depends on methane content (see below) were gathered
rate of diffusion through coal (Mazzsi 1992). from 25% of total available boreholes spaced
Usually, dynamic release is very quick, while the regularly in Polish coal basins (Fig. 1). Data
diffusion is very slow. It was estimated that the were collected only for those boreholes where
complete diffusion of methane from in situ coal the laboratory tests on gas content were made by
may take many years (Smith & Sloss 1992). In the same laboratory and where the methods
contrast, diffusion from crushed coal may only employed were: two-phase vacuum degassing
take tens of hours to tens of days (Gawraczyflski method (Kobiela et al. 1992) for methane
& Borowski 1986; Seidle & Arri 1990). The content tests and rate of desorption measured
amount of methane that is released from a mass in manometric desorbometer type DMC-2
unit of coal in the process of diffusion is usually (Grzybek 1993b).
comparable with the residual methane content Data on coal production, the amount of
(e.g. Grzybek et al. 1994). Therefore, the amount methane emitted by ventilation shafts ('ventila-
of coal released in the dynamic process (Gd) tion emission'), the amount of methane captured
corresponds with the difference between total and in degassing systems and the amount of methane
residual methane content: used, and also the maximum and minimum
depth of exploitation in each particular coal
Gd = G - Gr. (4) mine were collected for the years 1990-1992
directly from coal mines. Special attention was
Thus, in general, the following can be assumed. paid to the reliability of data concerning the
 ESTIMATION METHOD FOR METHANE EMISSIONS 427

,/ f........ "t

] \

.P-~-- ~ I - > ~ J "" - ~ P. Jl Y \~-~-\ ~ x_

i ~ I I ~ ~i" ( ""~.l. I I \ . "'~llloswu~c~M ~,j~.

' ",,
/ - . I / ,---.. "-"--<---__7 "'-.. '

/ / ,.., /I 0 i. I0
f' ~
t" * /I 9 ' 1-/r 2-.,J 3-" 4-~/ " 5 - " ~ 6 " - / " ~i. "~
7-~"
I IIl

Fig. 1. Location of boreholes chosen for analysis, location of coal mines and division of the Upper Silesian Coal
Basin into regions: 1, main faults; 2, main overthrusts; 3, boreholes; 4-6, borders of: the basin (4), coal mines (5)
and identified regions (6); 7, region number.

ventilation emission. The data on amount of gas Programme of research and the results
captured and used are fully reliable since each
degassing system is attached to high quality Bearing in mind the above mentioned assump-
measuring instruments; but the amount of tions, the following programme of research was
methane released by ventilation shafts is usually followed:
calculated on the basis of measurements of air
velocity in ventilation shafts and concentration (1) Identification of sources of methane emis-
of methane in the air, which are made only once sion in coal mining.
a month. The accuracy of those calculations (2) Analysis of the natural conditions under
depends, primarily, on the accuracy of methane which methane occurs and appropriate
concentration measurements, which is 0.01%. classification of parts of Polish coal basins
Taking into account typical volumes of air that into regions of uniform conditions.
usually go through ventilation shafts of a single (3) Depth standardization of the methane
mine (on average about 16 x 109m 3 per year) content distribution in each of the regions.
the expected, average calculation error is about (4) Evaluation of the average methane content
0.8 x 106 m 3 of methane per year and mine. So, and the average residual methane content.
for the purpose of this study, data on ventilation (5) Calculation of the specific emissions of
emission for 1990-1992 were taken into account those coal mines, in which ventilation
only from mines where the calculated emission emission had been assumed to be reliable.
was a minimum of two times the expected (6) Correlation and regression analysis of the
calculation error (i.e. no less than 1.6 x 106 m 3 specific emissions and the average methane
per year). contents.
Other data necessary to develop the mine- (7) Evaluation of the release factors from each
specific method of methane emission estimation source of emission.
were found and gathered from unpublished (8) Calculation of the total emission from the
reports of research institutes and the Civil Service. coal mining system for the 1992.
428 I. GRZYBEK E T A L .

Sources of emission in coal mining of methane content higher than 4.5m3/Mg

(Nied 1993). In 100metre intervals identified in
The system of hard coal mining includes the this way, the average and maximum methane
following technological processes during which contents were calculated for each region distin-
emission of methane may occur: guished and standardized distributions of aver-
age and maximum methane contents were
(a) The opening up of the coal deposit and
estimated (Fig. 2). The distributions for each
associated development.
region were compared with each other graphi-
(b) Exploitation of coal, its haulage and lifting
cally (Fig. 3) and using statistical methods
up to the surface.
(Kolmogorov-Smirnov test, two-sample test,
(c) Preparation, storage, transport and crush-
Spearman range correlation). As a result, on
ing of coal prior to its final use.
the basis of similarity, some regions could be
(d) Degassing of the deposit before, during and
merged. Further research was then carried out
after the exploitation.
(e) Storage of wastes (waste rock and prepara- for each region.
tion refuse).
The mining processes mentioned in points (a)
and (b) are carried out underground. Methane Evaluation of the total and residual
released in the course of those processes and not methane contents
captured by degassing systems is transferred to
the atmosphere through mine ventilation sys- Evaluation of the average methane content (GK)
tems. These ventilation emissions are thus the was made for each coal mine, by comparing the
first source of methane emission. The remainder standardized mines' exploitation depth interval
of the methane is contained in the extracted coal with the standardized distribution of average
and extracted waste rock and is released in the methane content in the region where the coal
course of post-mining processes mentioned in mine is located:
point (c) and at spoil heaps (point (e)). These are
the second and the third sources of methane ~ikl Gini (5)
emissions respectively. The fourth source of
methane emission is the degassing systems of
coal mines. They use only part of the gas where: Gi is the average methane content of the
captured; the rest is released to the atmosphere. ith 100-metre interval; ni is the number of
Emission of methane other than from the measurements of methane content in the ith
sources of hard coal production system men- interval of the distribution and k is the number
tioned above is likely to be very small. of intervals that lay in between minimum and
maximum depth of exploitation in any given
coal mine. The average residual methane con-
tents were established for each region. The
Classification of coal basins into regions and analytical method, described by Kandora &
standardization of the existing distribution of Grzybek (1992) was applied. The method is
based on observed correlation between rate of
methane content
desorption (AP2) and the total methane content
On the basis of the geological data from Polish (Fig. 4), where the coefficient a0 is equal to the
coal basins and available published material, residual methane content in the regression
a number of regions were distinguished, for equation:
which different gas conditions were expected.
The regions in the Upper Silesian Coal Basin G = a0 + al AP2. (6)
are shown in Fig. 1. In each region gas data The results of residual gas content calculations
were standardized to 100 metre depth intervals, have been partially published (Grzybek et al.
defined in relation to the roof of coal-bearing 1994).
Carboniferous formation, as well as (separately)
to the depth at which methane content for the
first time exceeds 4.5 m3/Mg of dry and ash free
coal (excluding of values of methane content Calculation of the specific emissions and
within zones of gas traps below the Carbonifer- release factors from each emission source
ous overburden; see: Kotas 1994). The choice of
the methane content value can be justified by Specific emissions (Wek) were calculated by
observed change in gas conditions for deposits dividing the sum of ventilation emission (Ew)
 ESTIMATION METHOD FOR METHANE EMISSIONS 429

. . .II i . .
4'4

0
" ..........
0
tF,,n
,,,. , , , '~. ":. '~.
[ ~ 'uoq.no jo ,loo~o~ ,.uo~!

= 9 =1 "~"
'

~ nlumnow~nm|nnn!
9- , ,~,~. 9
:l Ill ,,,il -t
!lmunnnn~lq||~,|l|~ 0

, ,. . . . . . P

:t "
8

~~
.~lumnw-,~l~lmltq, n.,!! m|muumn~qlU||t~n
.,.. , . , ":. "~.":. ~
430 I. GRZYBEK E T A L .

o) b)

0 4 O 12 18 G max 0 4 8 ~2 18 G I ' 1 1 0 1 [
I J ! | &

700' *700'
J ~ "~''"~v.
300. *300

-100, -I00

-500 -SO0
.,..~:. .......
-900 "900
z Z

c) d)

0 4 8 12 lS Gmox 0 /, 8 12 16 Gmox
t i , I I J l I , i !
~ I00, .10o

-200 -200
~,...:::.:...... i
-500 -50(>
.__(,,,.:..':~'~._
-800 .,,:~..-~
9 ., -800
/ "'--
-1100 -1100"

,. III .--- ~ . V
...... IV ..... u

Fig. 3. Comparison of standarized distributions of maximum methane content (Gmax,m3/Mg), defined in relation
to the roof of the Carboniferous (a & b), as well as to the depth at which methane content for the first time exceeds
4.5 m3/Mg (e & d); Z (m) is the relative depth, which is equal to zero for the roof of the Carboniferous (a & h) or
for the depth where Gmax ~ 4.5 m3/Mg for the first time (e & d); numbers below the figure explain particular
regions of the Upper Silesian Coal Basin.

plus the amount of methane captured by degas- and surrounding rocks dynamically and so,
sing systems (E0) of each coal mine (only reliable taking into account the equations (3) and (4),
measurements) by the coal mine output (Q): it is proportional to G.
On this basis, many variants of regression
Ew+E0 between the average methane content (GK) and
Wek - - - - (7)
Q the specific emissions (Wek) were analysed, and
finally the best regression equations were chosen
According to the assumption (3) of the work, the (Fig. 5) - those characterized by the least error
sum given in the numerator of equation (7) is the of ventilation emission estimation (5-15%).
amount of methane that is released from coal Estimated values of the specific emission were
 ESTIMATION METHOD FOR METHANE EMISSIONS 431

2e
G

10

0"
0 20 40 60 80 100 120 140 160 180 200
Ap,
Fig. 4. Distribution of rate of desorption (AP2, 1 • 10-3 m of H20) versus methane content (O, m3/Mg) in one of
the Upper Silesia coal mines.

assumed to be the release factors from under- assumed that all residual methane is released
ground (mining) processes (We). The resulting from coal before its final use, so the release
regression equation has the form: factors from post-mining activities are equal to:
9 residual methane c o n t e n t - in those coal
We = aa Gg~ + a2G~ (8) mines in which the average methane content
where: is higher than the residual methane content;
9 methane c o n t e n t - in the remaining coal
9 for coal mines of specific emission 14%k< mines.
10m3/Mg: al = 3.776 and a2 = -0.605;
9 for coal mines of specific emission Wek _> However the above assumption is not accurate,
10m3/Mg: al = 21.452 and a2 = -3.346. since there are no data to identity the volume of
methane burned during the final use of the coal.
In further work the established equations were The release factors for waste heaps were
extrapolated to all coal mines, with an addi- established taking additionally into account,
tional assumption that for coal mines of average that the calculated average content of dispersed
methane content lower than the residual coal material in waste rock is equal to 15%
methane content of the region, the final release (comp. Bolewski & Gruszczyk 1989; PIG 1988).
factor is twice as low as the one calculated by Release factors from degassing systems were
equation (8). also not estimated, as the amounts released to
Release factors from post-mining processes the atmosphere can be precisely measured in
and from waste heaps were not estimated. It is coal mines.
432 I. GRZYBEK E T A L .

a)
t
Wek
[m3/Mgl

5O
! 9

4 0 84

Wt" 21.542 G - 3.346 G :

30

~ _ 1,-----,"__'A"
_-----"--2"-7-:-'<-"
:" ,---
o 1 2 3 4
C,,,I,,,3/Mgl
b)
Wek /
/
[rn3/Mgl /
8

7 .
#
Wj" 3.7"/6 G - 0.60S G 3

6 . : .' "9 .

4-1

0 ----
o 1 2 ~' 4

Fig. 5. Comparison of the linear equation by Boyer et aL (1990) and Polish parabolic equations ilustrating
regression of specific emission (Wek, m 3/Mg) in relation to average methane content (GK, m 3/Mg) for Polish coal
mines of high (a) and low (b) emissions; dots sign data from particular coal mines for 1990 -1992, except those
where Wek < 1.6 x 106 m3/Mg.

Calculated release factors (in m3/Mg of coal Evaluation of total methane emission from
produced) for each emission source are: h a r d c o a l m i n i n g in P o l a n d

9 for mining processes: The estimated release factors for each source of
0,000-31.108 (average 6.005); methane emission were applied to equation (2)
9 for post-mining processes: in place of the global average release factor, and
0,000-1.907 (average 1.481); the emission from Polish hard coal system was
9 for deposition of waste rock: calculated. The amount of methane captured by
0,032-0.212 (average 0,065). degassing systems was subtracted from the
 ESTIMATION M E T H O D FOR M E T H A N E EMISSIONS 433

emission calculated for mining processes. Total GAWRACZYIqSKI, Z. & BOROWSKI, J. 1986. Zmiany
methane emission in 1992 was evaluated to be zawartogci metanu w czasie w pr6bkach pobra-
935.2 x 106m 3, out of which 697.65 x 106m 3 nych z urobionego w~gla. In: Metody rozpozna-
was emitted from mining processes. wania zagrokenia metanowego w kopalniach wcgla
kamiennego. Katowice, czerwiec 1986. Kato-
wickie Gwarectwo W~glowe- Zarz~d Oddziatu
SITG w Katowicach, Conference Proceedings,
Conclusions 135-150.
GRZYBEK, I. 1993a. Introduction to stimulation
The result of the presented research is the of coalbeds. Coalbed Methane Newsletter, 4-6,
development of a method of methane emission 10-14.
evaluation. The method is adjusted to the 1993b. The Polish methods of the coalbed
specific conditions that exist in Polish coal methane content testing and its reserves estimat-
mines. It is different from the global average ing. In: Proceedings of the 1993 International
Coalbed Metane Symposium, Birmingham, Ala-
method, suggested by OECD/IPCC, mainly due bama, USA, May 17-21 1993, I, The University of
to the application of a parabolic equation that Alabama, Tuscaloosa, 61-68.
describes release factors for mining processes. , GAWLIK, L., SUWALA,W. & KUZAK, R. 1994.
The form of the equation is different for coal Wst~pne wyniki implementacji analitycznej
mines of high and low specific emission and metody okreglania metanonognogci resztkowej w
proves that improvements introduced by GZW. In: Wcgiel kamienny- wtasnoJci, akumu-
OECD/IPCC in their methodology are in the lacja, uwalnianie i pozyskiwania gazdw kopalnia-
right direction. Nevertheless, the modified nych, Krak6w, 11-12 paddiernik 1994. Akademia
OECD methodology suggests linear regression G6rniczo-Hutnicza w Krakowie, Workshop Pro-
ceedings, 7-9.
equations, which under Polish conditions would KANDORA, P. & GRZYBEK, I. 1992. On the Criteria of
lead to improper evaluation of methane emis- the Possibility of Balancing and Exploitation of
sion. In the light of this new method of Polish Coalbed Methane. United Nations Economic
evaluation, the OECD methodology gives over- Comission for Europe Workshop on the Recov-
estimated results. The methane emission for ery and End-Use of Coal-Bed Methane, Kato-
Polish hard coal mining systems, estimated by wice, Poland. Gt6wny Instytut G6rnictwa,
the method presented here is four times lower Katowice.
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linear equations. E. • WRONA, B. 1992. The Methods of Sampling,
Laboratory Methods of Determining the Gas
Although the parabolic equation gives the Content in Coal Seams and Methods of Predicting
best approximation of methane emissions from Methane Emission in the Mine Workings Used in
the whole Polish coal mining operation, it does Poland. United Nations Economic Comission for
not explain the emissions from each coal mine. Europe Workshop on the Recovery and End-Use
It shows that emissions of methane are control of Coal-Bed Methane, Katowice, Poland. Gt6wny
led by unidentified factors, which are mine and, Instytut G6rnictwa, Katowice.
probably, coal basin specific. Therefore, the KOTAS, A. (ed.) 1994. Coal-Bed Methane Potential of
results of any global estimation of methane the Upper Silesian Coal Basin, Poland. Prace
emissions need to be interpreted with caution. Paflstwowego Instytutu Geologicznego, CXLII,
Warszawa.
MAZZSI, D. 1992. Cavity Stress Relief Method for
Recovering Methane from Coal Seam. United
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wienie opracowanych technologii i metod wyko- 1991. Uwarunkowania inwentaryzacji emisji i wych-
rzystania odpad6w. Polish Geological Institute wytu gaz6w cieplarnianych w Polsce w 1988 roku.
Report of CPBP 04.10.04 Subprogramme, Polish Foundation for Energy Efficiency Report.
Warszawa. SEIDLE, J. P. & ARRI, L. E. 1990. Use of Conventional
PILCHER, R. C., BIBLER, C. J., GLICKERT, R., Reservoir Models for Coalbed Methane Simula-
MACHESKY, L. & WILLIAMS, J. M. 1991. Assess- tion. International Meeting of the Petroleum
ment of the Potential for Economic Development Society of CIM and SPE, Calgary, CIM/SPE 90.
and Utilization of Coalbed Methane in Poland. SMITH, I. M. & SLOSS, L. L. 1992. Methane Emissions
U.S. Environmental Protection Agency Report, from Coal. Perspectives, IEA Coal Research.
EPA[40011-911032. TARNOWSKI,J. & STRUZIK,A. 1978. Opracowanie pola
PYKA, M. 1993. About the energy of methane. Silesian gazono~no~ci projektowanego obszaru g6rni-
Coalbed Methane Newsletter, 4-6, 18-26. czego. Przeglqd G6rniczy, 3, 95-105.
Methane emission and its utilization from Ostrava-Karvinfi Collieries
in the Upper Silesian coal basin, Czech Republic

G. T A K L A & Z. V A V R U S , ~ K

Ddlni prdzkum a bezpednost Paskov, a.s. (Underground Exploration and Mine Safety, Inc.)
73921 Paskov, The Czech Republic

Abstract: The Ostrava-Karvinfi part (OKR) of the Upper Silesian coal basin is the most
important hard coal basin in the Czech Republic. This basin extends over an area of
1600km2. The Carboniferous basin fill contains 255 seams with a net coal thickness of
150m. The methane content in the coal is estimated between 4.4 to 20m3/t. In the OKR,
about 120million cubic meters per year of methane are produced by gas drainage plants
from a number of collieries. The methane is used in local industries. Several measures have
been taken to increase the methane extraction in active mines and in areas of closed
collieries. Additionally, pilot projects for coalbed methane production have been started in
virgin coal bearing areas with no previous coal production. The authors' company is
progressing with such a pilot project, with the first coalbed methane wells completed
recently. Results to date are encouraging. All these activities are designed to increase the
safety in mines, to reduce methane emission to the atmosphere, and to develop new sources
of energy.

The hard coal reserves in the Czech Republic are by a release of methane averaging 589,000 cubic
found in one major and three minor coal mining metres per day. Historical data on coal produc-
districts areas: Ostrava-Karvinfi, Northeast tion and total methane released in the O K R are
Bohemia, Kladno and in West Bohemia. summarized in Table 1.
The Ostrava-KarvinS, Coalfield (OKR) con- In the course of the advance of mine mechan-
tains the most significant of the coal deposits. It ization and increase of coal mining intensity, it
covers an area of about 1600 km 2, within which became necessary to introduce a system of
about 335 km 2 belong to the mining claims of methane drainage to isolate part of the methane
individual collieries. Hard coal production in the liberated during coal mining, for safety reasons.
O K R represents more than 95% of the total In some longwalls, applying this method, it is
hard coal production in the Czech Republic. possible to reduce the amount of methane
More than 99.8% of methane emission from released into the atmosphere by up to 50% or
mines in the Czech Republic is related to mining more. During the 35 years of operating mine
operations in the OKR. methane drainage, an efficiency of about 30% of
Coal mining in the O K R started about 200 all the methane released has been reached. This
years ago. The earliest record of the quantity of means that about 30% of the total amount of
methane drained by mine ventilation relates to methane released from mining operations in the
the year 1910 when the coal production increased whole mining district is collected and drawn into
to 7.67 million metric tons per year, accompanied the methane drainage plants.

Table 1~ Coalproduction in OKR and methane exhalation

Year Coal production Methane content in Methane quantity Total methane
(106 t/year) outlet shafts drained recovery
(thousands m3/day) (thousands m3/day) (thousands m3/day)

1910 7.67 589 - 589

1920 7.59 856 - 856
1930 10.67 873 - 863
1940 16.25 869 - 869
1950 13.72 910 - 910
1960 20.87 957 32.9 989.9
1970 23.86 1526.4 553.7 2080.1
1980 24.69 1381.4 568.3 1949.7
1990 20.06 999.6 379.7 1379.1
1994 15.80 743.32 279.4 1022.6

From Gayer, R. & Pegek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 435-440.
436 G. TAKLA & Z. VAVRUS/~K

However, due to leakages in rock strata, mainly mine boreholes to this system. In addition
imperfection in the conductor casing strings of to these boreholes, abandoned mine and 'oldman'
boreholes etc., some dilution of the mine gas workings are connected to the system as well,
occurs. Because the whole system works below separated from active mine workings by seals.
atmospheric pressure, some air may be sucked in, From individual mine gas drainage plants,
so that the final methane concentration becomes pipelines feed into the main pipeline system. The
reduced to about 50-55%. gas mixture collected is then Oelivered to con-
Within a short period of time, after further sumers in local industry, mainly heating plants
development of the mine gas drainage network, and steelworks. The gas delivered consists of a
ways of using this source of energy were mixture of methane with air, with a methane
investigated. In most mines heating plants were content of about 50-55%.
modified in such a way to enable them to use The equipment used to burn this gas has to be
mine gas for heating and for the production of designed to account of this methane/air mixture.
hot water. For the remaining amount of mine The modification means that the equipment
gas, which reached up to 200 million cubic cannot be used for a different type of gas. The
metres per year, gas pipelines were laid, in typical gas mixture consists of 50-55% of
collaboration with regional gas utilities. Also, methane, 2-4% of carbon dioxide, 1-3% of
the use of methane in local industry was oxygen, and 38-47% of nitrogen. The heating
established, mainly in metallurgical plants and value of such gas is about 19-20 Megajoule per
power stations. cubic metre. The present gas pipeline network
forms a system of about 92km total length.
Figure 1 shows a schematic drawing of the gas
Overview of the present state pipeline system and mine gas drainage plants.
Table 2 gives an overview on the methane
At present, the mine gas drainage system in the production from mine gas drainage plants and
O K R consists of 21 individual mine gas drainage on the consumption of gas within the mines
plants with a total of 115 vacuum pumps themselves or in the regional industry.
installed. An extensive underground pipeline Due to the recent reduction in the intensity of
network connects about 5000 mine gas sources, coal mining and improvements in the efficiency

9 mNOV~- HU~"
9 OOUBRAVA CS~A ..~ KARVIN,A

/ -I - ... ..... ....

I - .......... ...... / \
~ I ~ " ........ FUC~Ky " " " ' '~ / M.
OOR*'vRo~./'"" .......... /G~.O.OUKLA " X,~.~....~csH

,.o0" '~ "~

e ......... SVOBOOA
,v, ov

@OSTRAVA
--OS TRAVA /
' "EXPLANATION " / mm I . ,.
9 GA$ORAINAGEPLANT N. J I" T STARi'C III.

~]1 METALLURGICAL
PLANT ~ PASKO~ ~
@ PASKOV
........ COALBEOt,,IETHANEPIPELINE
............. P I P E L I H E FOR COKE OVEN GAS

Fig. 1. Schematic drawing of pipeline system and mine gas drainage plants in OKR, Czech Republic.
 METHANE EMISSION FROM OKR MINES 437

Table 2. Methane production from mine gas drainage These programmes are based on a study initiated
and its utilization (in thousands m3/year) by the US Environmental Protection Agency
(EPA), Global Change Division. This study
Year Total Own Deliveries to Vented recommended an integrated approach to coal-
production utilization industry
bed methane recovery in the OKR.
1958 4300 - 2100 2200
1960 14300 - 12100 2200
1965 76233 542 61 966 13 725 Gas recovery from abandoned coal mines
1970 239713 41 617 127 907 70 189
1975 235700 61 158 168 970 5571 Due to the political and social changes since
1980 225028 69843 136533 18 652 1989/1990 in the Czech Republic, coal produc-
1985 207459 64230 120261 22969 tion has decreased as the coal industry was
1990 150395 65023 69085 16287
restructured and unprofitable coal mines were
1994 110324 52441 44977 12 905
closed down or are being closed. In the Ostrava
part of the mining district of the OKR, four
collieries have been closed. Mine claims over
these collieries cover an area of more than 100
of mine ventilation systems, the importance of
square kilometres extending partly over very
mine gas drainage for the safety of mine
densely populated parts of the city of Ostrava.
operations is gradually decreasing. In view of
After abandonment operations, the hoisting and
this development our company DPB, Inc. has
outlet shafts are being filled in. The ventilation
established new methods for collecting methane
systems, that diluted and vented the mine gases,
from active mines.
were shut down after more than 200 years of
Based on a detailed study of geological data,
mining operations. Water levels in the mines
new locations and rock sequences were explored,
would rise as predicted, gradually flooding the
where methane could have accumulated in
mine workings to the expected level. During this
greater quantities. At such locations specially
stage some mine gas may leak, out of control, to
designed and completed mine boreholes are
the surface via old mine shafts and other
drilled, leading to increases in total coalbed
potential leaks in their vicinity, and also via
methane production. Locations favourable for
natural migration channels, such as fissures and
methane production could be found in the upper
tectonic faults. This migration is also influenced
part of mine claims, in weathered Carboniferous
by rapid drops in atmospheric pressure which
strata, in faulted intervals, and also in areas with
lead to a pressure differential between the gas in
unconsolidated rocks covering coal mine areas.
the mine workings and the atmosphere above. A
According to results up to date, a development
risk of explosion or fire would occur, with such
of such opportunities could considerably
gas possibly finding its way into basements of
increase mine gas production from gas drainage
buildings or industrial plants in the densely
plants in active mines. In the mine CSM in
populated city of Ostrava.
Stonava for example, four mine boreholes of up
At three former mine sites, mine gas drainage
to 150 m depth were drilled into beds close to the
systems and plants had been in operation at the
top of the Carboniferous. After a few months of
surface before the decision to close the mines
operation, production of methane from these
was taken. The authors' company, DPB, Inc.,
holes rose to up to 12 000 cubic metres per day.
prepared a study, showing the necessity to
This new method is termed 'Supplementary
maintain mine gas drainage from shut-down
Mine Gag Drainage', because, unlike traditional
mines even after the termination of mining in the
mine gas drainage, it is not concerned mainly
OKR. For this reason the company bought mine
with mine safety.
gas drainage plants from two mines before their
Within less than two years of introducing this
closure. DPB is now converting these plants for
method the production from 16 boreholes with a
total length of 2563 m has reached 7.6 • 106 m 3 the permanent extraction of mine gas from
closed mine workings after the termination of
of methane.
coal mining in the area. Before the mine shafts
In addition to conventional gas drainage in
were filled in, boreholes were drilled at mine
coal mines, DPB has also been involved in
locations noted for their maximum presence of
two fundamental development programmes for
methane. These boreholes were connected to an
exploration, production and utilization of coal-
existing pipeline. Precautions had to be taken to
bed methane from
avoid damage of the mine gas pipeline while the
9 abandoned coal mines mine shafts were filled in. Some of the aban-
9 virgin coal seams doned shafts were selected to adapt them as gas
438 G. TAKLA & Z. VAVRUSAK

production shafts, by filling in their upper The wellhead pressure of our gob wells varied
section only and leaving the bottom parts open between 101.21-101.62kPa, depending on baro-
and connected to former mine working levels, so metric pressure. The technique of well testing
that those could act as a reservoir for mine gas. was therefore modified in such a way to take this
In the upper filled part of such shafts, pipes had peculiarity into account. A mobile vacuum
to be installed so that the mine gas collected pump was constructed by modifying a conven-
could be pumped into the mine gas drainage tional vacuum pump so as to create the under-
plant. pressure required to stimulate the flow of gas
DPB believes that mine gas of a quality from the gob zones.The vacuum unit consisted
sufficient for industrial use can be pumped out of a vacuum pump, a measuring line allowing
from closed mines of the Ostrava mining district. gas sampling, and an electric motor. The results
The methane content of the gas mixture of a short-term production test at the V-3 gob
produced varies from 40 to 80% but an increase well are given in Figure 2.
in methane content can be expected once the After the evaluation results of the short-term
filling of the abandoned shafts is completed. production tests, a flow line was laid connecting
A similar situation to the case described above the boreholes with the existing gas drainage
caused DPB in 1992/93 to put its first surface plants. Figure 3 displays the characteristics of
gob wells in operation in an area of abandoned the gas production from the V-3 well during its
coal mines, for the purpose of verifying: first year of operation.
The first pilot gob wells of DPB demonstrated
9 the possibility of recovering gas from aban- the feasibility of gob gas extraction from
doned coal mines, abandoned coal mines.
9 the technical and technological requirements
for drilling, completing and testing such
boreholes, and Coalbed methane development in virgin
9 the possibility of commercial use of this gas. coal seams
Gob wells in our project are wells extracting Coalbed methane (CBM) development in virgin
methane released from strata surrounding coal- coal seams in the Czech Republic dates back to
beds being mined and captured in the rock early 1992. This development was encouraged
massive in micropore-macropore structures and for several reasons:
fractures. 9 The occurrence of methane in active mines of
The gob wells were located in abandoned the OKR.
mine workings of Vrbice and Rychvald in the 9 The high density of previous exploration
Ostrava part of the OKR, where active mining throughout the OKR region, including explo-
was already discontinued in the 1950s. These ration wells, evaluation and assessment of
wells were drilled into the mined multiple coal coal reserves, studies of coal deposits, etc.
seams of the Ostrava Formation. 9 The government policy for the diversification
The design and technical performance of gob of gas resources.
wells fulfilled the following requirements: 9 The interest of the Czech Government and of
private companies regarding the exploration
9 Low drilling and completion costs in com- and production of coalbed methane.
parison to conventional gas wells, to ensure
profitability despite relatively low production According to Czech Mining Law, the area of
rates. virgin coal seams in OKR was divided among
9 Prevention of contamination of gob zones by four CBM concessionaires
drilling fluids.
9 D~lni prfizkum a bezpe6nost Paskov, a.s.
9 Maintenance of safety standards in drilling
(DPB, Inc.)
and production in accordance to regulation
9 Energie Kladno, a.s.
issued by the Czech Bureau of Mines.
9 Geologick~ prflzkum Ostrava, a.s. (GPO,
Inc.)
The gob wells were tested to yield funda-
9 Unigeo Ostrava, a.s.
mental information on production pressure,
volume of gas production and methane concen- A permit to explore for CBM was granted to all
tration, to allow estimates of profitability and to four companies. According to Czech Mining
provide a basis for planning to tie in the wells Law, the companies may expect to obtain a
into the production system of gas drainage production concession in the case of successful
plants already existing. results.
 M E T H A N E EMISSION F R O M O K R MINES 439

I ~-3 ~oa WELL II

+oo ~+.o.,,,,. ,,,oouc,.o..,,.

+o_ . . . . . . . .

150 - - - ; - - - / / i I. . . .

,oo....._.+//_. . . . . .

50 . . . . . ~ . ~/.:.4,+.+
" ~-~-wj
- w j ~ - - - ' - m -. - -. m. . . . . .. . . . m~--~-~.o__.__...~
, P- +, ~ _ = . . < d',--W_~l
.....

0 - IS" . . . . . . . . .
1 2 3 4 5 6 7 8 9 10
DAYS

WELLHEAD PRESSURE : CH4 C O N C E N T R A T I O N - " ~ - GOB GAS PRODUCTION

IkP-I I""I l"~'ml
"EJ-
9 UNDERPRESSURE -~-" ~ P R O D U C T I O N PERIOD
_ _
~p.] Imd'n~leel

Fig. 2. Short-term production test of the V-3 gob well.

IGV-3 GOB WELL

AS P R O D U C T I O N
Iio0. sc,,,It,J
100000

X
10000 - IIECALCULATEO TO 100% CH4 X

if( C:l----lil

, . , . ~ ~ --~" - " ' - +K-+-----I~----..#+_.+--~.--..~,~ .,.

1000
"%'~,: ..... X:

100
jl. .jk...~ 9 __" %" .I. .I. .t.. ....%'- 11= .Jl.. "+ ,lb.

10 i" ' ' i " I ! . . . . . .

7/93 0/93 9/93 10;931 lj93121931194 2/94 3/94 4/94 5/94 6/94' 71~14
' I ] ' '

MONTHS
- - , k - AVE.CI-14 C O N C E N T R . - - I - - AVE.UNDERPRESSURE - ~ . ' - A V E . C l I 4 PRODUCTION
I~1 I'+e'l I,,,,~/,+od
-I'~- TOTAL CH4 PRODUCT.

Fig. 3. Gas production of the V-3 gob well during first year of production.
440 G. TAKLA & Z. VAVRUSAK

According to the energy resource policy of the Each of the wells is continuously cored in the
Czech Government, CBM exploration is finan- Carboniferous interval to obtain primarily infor-
cially supported by the Ministry of Economy. By mation on the gas content in the rock sequence.
the end of 1994, nine CBM wells were drilled. Core samples of the coal are subjected to
Two of the wells were fractured, with promising standard canister desorption tests (according
results for future production. In April/May 1995, to the Standard of the US Bureau of Mines).
more four wells were fractured and long-term Simultaneously, coals and rocks surrounding the
pumping tests were started. Four to six new wells coal sampling points are tested to obtain
are expected to be drilled by the end of 1995. information required for the design and evalua-
DPB owns a concesion for CBM exploration tion of hydraulic fracturing of the coal. Drilling,
in ten prospection areas, covering a total of coring and completion are assigned to local
240km 2 of virgin coal fields that contain contractors, as is hydraulic fracturing of the coal.
4.1 • 10 9 tonnes of hard coal reserves. These The first pilot well was completed in the
areas are characterized by a high density of Karvinfi Formation's coal seams in the area of
exploration wells, drilled for coal, gas and water Ditmarovice at the begining of 1995. Successful
prospection on a spacing of some 1.5 km. hydrofracturing opened two coal seams (4.3m
Several geological evaluations and studies were and 1.4 m thick). A beam pump was installed to
carried out to assess the importance of the coal test water and gas production.
reserves and to build a database. Accordingly, The second pilot well in the Vficlavovice area
the coal deposits of these areas are well (Ostrava Formation's coal seams) did not realise
documented, with very good geological informa- the expected coal gas content and gas in place.
tion about each of the prospection areas. The third pilot well of DPB' s project is now
However, the occurrence of methane in virgin being drilled in the area of Fren~tfit (Karvinfi
coal seams is not well documented so far. For Formation). An additional one or two pilot
most of the prospection areas, data on gas wells are planned for spudding in 1995.
content of the coal are either not available at all,
or very incomplete at best. For this reason, a
CBM exploration campaign with a chance of Summary
success would first have to identify the most
favourable areas and coal seams by drilling pilot The paper presents information on some methods
wells. of coal gas processing and utilization in the
The CBM pilot project proposed by DPB, largest hard coal basin of the Czech Republic., i.e.
comprises six pilot test wells in the most the Ostrava-Karvinfi Mining District. Improve-
promising exploration areas, which are named ments in the methods of mine gas drainage,
as follows: increased recovery of methane from closed mines,
and new coalbed methane production from coal
9 D6tmarovice fields of the region could contribute to the world-
9 Petrovice - Vficlavovice wide aim at improving the use of clean energy
9 Pf'ibor - zfipad sources and reducing the emission of methane
9 T r o j a n o v i c e - Fren~t~it. into the atmosphere.
Methane emission and its utilization from Ostrava-Karvinfi Collieries
in the Upper Silesian coal basin, Czech Republic

G. T A K L A & Z. V A V R U S , ~ K

Ddlni prdzkum a bezpednost Paskov, a.s. (Underground Exploration and Mine Safety, Inc.)
73921 Paskov, The Czech Republic

Abstract: The Ostrava-Karvinfi part (OKR) of the Upper Silesian coal basin is the most
important hard coal basin in the Czech Republic. This basin extends over an area of
1600km2. The Carboniferous basin fill contains 255 seams with a net coal thickness of
150m. The methane content in the coal is estimated between 4.4 to 20m3/t. In the OKR,
about 120million cubic meters per year of methane are produced by gas drainage plants
from a number of collieries. The methane is used in local industries. Several measures have
been taken to increase the methane extraction in active mines and in areas of closed
collieries. Additionally, pilot projects for coalbed methane production have been started in
virgin coal bearing areas with no previous coal production. The authors' company is
progressing with such a pilot project, with the first coalbed methane wells completed
recently. Results to date are encouraging. All these activities are designed to increase the
safety in mines, to reduce methane emission to the atmosphere, and to develop new sources
of energy.

The hard coal reserves in the Czech Republic are by a release of methane averaging 589,000 cubic
found in one major and three minor coal mining metres per day. Historical data on coal produc-
districts areas: Ostrava-Karvinfi, Northeast tion and total methane released in the O K R are
Bohemia, Kladno and in West Bohemia. summarized in Table 1.
The Ostrava-KarvinS, Coalfield (OKR) con- In the course of the advance of mine mechan-
tains the most significant of the coal deposits. It ization and increase of coal mining intensity, it
covers an area of about 1600 km 2, within which became necessary to introduce a system of
about 335 km 2 belong to the mining claims of methane drainage to isolate part of the methane
individual collieries. Hard coal production in the liberated during coal mining, for safety reasons.
O K R represents more than 95% of the total In some longwalls, applying this method, it is
hard coal production in the Czech Republic. possible to reduce the amount of methane
More than 99.8% of methane emission from released into the atmosphere by up to 50% or
mines in the Czech Republic is related to mining more. During the 35 years of operating mine
operations in the OKR. methane drainage, an efficiency of about 30% of
Coal mining in the O K R started about 200 all the methane released has been reached. This
years ago. The earliest record of the quantity of means that about 30% of the total amount of
methane drained by mine ventilation relates to methane released from mining operations in the
the year 1910 when the coal production increased whole mining district is collected and drawn into
to 7.67 million metric tons per year, accompanied the methane drainage plants.

Table 1~ Coalproduction in OKR and methane exhalation

Year Coal production Methane content in Methane quantity Total methane
(106 t/year) outlet shafts drained recovery
(thousands m3/day) (thousands m3/day) (thousands m3/day)

1910 7.67 589 - 589

1920 7.59 856 - 856
1930 10.67 873 - 863
1940 16.25 869 - 869
1950 13.72 910 - 910
1960 20.87 957 32.9 989.9
1970 23.86 1526.4 553.7 2080.1
1980 24.69 1381.4 568.3 1949.7
1990 20.06 999.6 379.7 1379.1
1994 15.80 743.32 279.4 1022.6

From Gayer, R. & Pegek, J. (eds), 1997, European Coal Geology and Technology,
Geological Society Special Publication No. 125, pp. 435-440.
436 G. TAKLA & Z. VAVRUS/~K

However, due to leakages in rock strata, mainly mine boreholes to this system. In addition
imperfection in the conductor casing strings of to these boreholes, abandoned mine and 'oldman'
boreholes etc., some dilution of the mine gas workings are connected to the system as well,
occurs. Because the whole system works below separated from active mine workings by seals.
atmospheric pressure, some air may be sucked in, From individual mine gas drainage plants,
so that the final methane concentration becomes pipelines feed into the main pipeline system. The
reduced to about 50-55%. gas mixture collected is then Oelivered to con-
Within a short period of time, after further sumers in local industry, mainly heating plants
development of the mine gas drainage network, and steelworks. The gas delivered consists of a
ways of using this source of energy were mixture of methane with air, with a methane
investigated. In most mines heating plants were content of about 50-55%.
modified in such a way to enable them to use The equipment used to burn this gas has to be
mine gas for heating and for the production of designed to account of this methane/air mixture.
hot water. For the remaining amount of mine The modification means that the equipment
gas, which reached up to 200 million cubic cannot be used for a different type of gas. The
metres per year, gas pipelines were laid, in typical gas mixture consists of 50-55% of
collaboration with regional gas utilities. Also, methane, 2-4% of carbon dioxide, 1-3% of
the use of methane in local industry was oxygen, and 38-47% of nitrogen. The heating
established, mainly in metallurgical plants and value of such gas is about 19-20 Megajoule per
power stations. cubic metre. The present gas pipeline network
forms a system of about 92km total length.
Figure 1 shows a schematic drawing of the gas
Overview of the present state pipeline system and mine gas drainage plants.
Table 2 gives an overview on the methane
At present, the mine gas drainage system in the production from mine gas drainage plants and
O K R consists of 21 individual mine gas drainage on the consumption of gas within the mines
plants with a total of 115 vacuum pumps themselves or in the regional industry.
installed. An extensive underground pipeline Due to the recent reduction in the intensity of
network connects about 5000 mine gas sources, coal mining and improvements in the efficiency

9 mNOV~- HU~"
9 OOUBRAVA CS~A ..~ KARVIN,A

/ -I - ... ..... ....

I - .......... ...... / \
~ I ~ " ........ FUC~Ky " " " ' '~ / M.
OOR*'vRo~./'"" .......... /G~.O.OUKLA " X,~.~....~csH

,.o0" '~ "~

e ......... SVOBOOA
,v, ov

@OSTRAVA
--OS TRAVA /
' "EXPLANATION " / mm I . ,.
9 GA$ORAINAGEPLANT N. J I" T STARi'C III.

~]1 METALLURGICAL
PLANT ~ PASKO~ ~
@ PASKOV
........ COALBEOt,,IETHANEPIPELINE
............. P I P E L I H E FOR COKE OVEN GAS

Fig. 1. Schematic drawing of pipeline system and mine gas drainage plants in OKR, Czech Republic.
 METHANE EMISSION FROM OKR MINES 437

Table 2. Methane production from mine gas drainage These programmes are based on a study initiated
and its utilization (in thousands m3/year) by the US Environmental Protection Agency
(EPA), Global Change Division. This study
Year Total Own Deliveries to Vented recommended an integrated approach to coal-
production utilization industry
bed methane recovery in the OKR.
1958 4300 - 2100 2200
1960 14300 - 12100 2200
1965 76233 542 61 966 13 725 Gas recovery from abandoned coal mines
1970 239713 41 617 127 907 70 189
1975 235700 61 158 168 970 5571 Due to the political and social changes since
1980 225028 69843 136533 18 652 1989/1990 in the Czech Republic, coal produc-
1985 207459 64230 120261 22969 tion has decreased as the coal industry was
1990 150395 65023 69085 16287
restructured and unprofitable coal mines were
1994 110324 52441 44977 12 905
closed down or are being closed. In the Ostrava
part of the mining district of the OKR, four
collieries have been closed. Mine claims over
these collieries cover an area of more than 100
of mine ventilation systems, the importance of
square kilometres extending partly over very
mine gas drainage for the safety of mine
densely populated parts of the city of Ostrava.
operations is gradually decreasing. In view of
After abandonment operations, the hoisting and
this development our company DPB, Inc. has
outlet shafts are being filled in. The ventilation
established new methods for collecting methane
systems, that diluted and vented the mine gases,
from active mines.
were shut down after more than 200 years of
Based on a detailed study of geological data,
mining operations. Water levels in the mines
new locations and rock sequences were explored,
would rise as predicted, gradually flooding the
where methane could have accumulated in
mine workings to the expected level. During this
greater quantities. At such locations specially
stage some mine gas may leak, out of control, to
designed and completed mine boreholes are
the surface via old mine shafts and other
drilled, leading to increases in total coalbed
potential leaks in their vicinity, and also via
methane production. Locations favourable for
natural migration channels, such as fissures and
methane production could be found in the upper
tectonic faults. This migration is also influenced
part of mine claims, in weathered Carboniferous
by rapid drops in atmospheric pressure which
strata, in faulted intervals, and also in areas with
lead to a pressure differential between the gas in
unconsolidated rocks covering coal mine areas.
the mine workings and the atmosphere above. A
According to results up to date, a development
risk of explosion or fire would occur, with such
of such opportunities could considerably
gas possibly finding its way into basements of
increase mine gas production from gas drainage
buildings or industrial plants in the densely
plants in active mines. In the mine CSM in
populated city of Ostrava.
Stonava for example, four mine boreholes of up
At three former mine sites, mine gas drainage
to 150 m depth were drilled into beds close to the
systems and plants had been in operation at the
top of the Carboniferous. After a few months of
surface before the decision to close the mines
operation, production of methane from these
was taken. The authors' company, DPB, Inc.,
holes rose to up to 12 000 cubic metres per day.
prepared a study, showing the necessity to
This new method is termed 'Supplementary
maintain mine gas drainage from shut-down
Mine Gag Drainage', because, unlike traditional
mines even after the termination of mining in the
mine gas drainage, it is not concerned mainly
OKR. For this reason the company bought mine
with mine safety.
gas drainage plants from two mines before their
Within less than two years of introducing this
closure. DPB is now converting these plants for
method the production from 16 boreholes with a
total length of 2563 m has reached 7.6 • 106 m 3 the permanent extraction of mine gas from
closed mine workings after the termination of
of methane.
coal mining in the area. Before the mine shafts
In addition to conventional gas drainage in
were filled in, boreholes were drilled at mine
coal mines, DPB has also been involved in
locations noted for their maximum presence of
two fundamental development programmes for
methane. These boreholes were connected to an
exploration, production and utilization of coal-
existing pipeline. Precautions had to be taken to
bed methane from
avoid damage of the mine gas pipeline while the
9 abandoned coal mines mine shafts were filled in. Some of the aban-
9 virgin coal seams doned shafts were selected to adapt them as gas
438 G. TAKLA & Z. VAVRUSAK

production shafts, by filling in their upper The wellhead pressure of our gob wells varied
section only and leaving the bottom parts open between 101.21-101.62kPa, depending on baro-
and connected to former mine working levels, so metric pressure. The technique of well testing
that those could act as a reservoir for mine gas. was therefore modified in such a way to take this
In the upper filled part of such shafts, pipes had peculiarity into account. A mobile vacuum
to be installed so that the mine gas collected pump was constructed by modifying a conven-
could be pumped into the mine gas drainage tional vacuum pump so as to create the under-
plant. pressure required to stimulate the flow of gas
DPB believes that mine gas of a quality from the gob zones.The vacuum unit consisted
sufficient for industrial use can be pumped out of a vacuum pump, a measuring line allowing
from closed mines of the Ostrava mining district. gas sampling, and an electric motor. The results
The methane content of the gas mixture of a short-term production test at the V-3 gob
produced varies from 40 to 80% but an increase well are given in Figure 2.
in methane content can be expected once the After the evaluation results of the short-term
filling of the abandoned shafts is completed. production tests, a flow line was laid connecting
A similar situation to the case described above the boreholes with the existing gas drainage
caused DPB in 1992/93 to put its first surface plants. Figure 3 displays the characteristics of
gob wells in operation in an area of abandoned the gas production from the V-3 well during its
coal mines, for the purpose of verifying: first year of operation.
The first pilot gob wells of DPB demonstrated
9 the possibility of recovering gas from aban- the feasibility of gob gas extraction from
doned coal mines, abandoned coal mines.
9 the technical and technological requirements
for drilling, completing and testing such
boreholes, and Coalbed methane development in virgin
9 the possibility of commercial use of this gas. coal seams
Gob wells in our project are wells extracting Coalbed methane (CBM) development in virgin
methane released from strata surrounding coal- coal seams in the Czech Republic dates back to
beds being mined and captured in the rock early 1992. This development was encouraged
massive in micropore-macropore structures and for several reasons:
fractures. 9 The occurrence of methane in active mines of
The gob wells were located in abandoned the OKR.
mine workings of Vrbice and Rychvald in the 9 The high density of previous exploration
Ostrava part of the OKR, where active mining throughout the OKR region, including explo-
was already discontinued in the 1950s. These ration wells, evaluation and assessment of
wells were drilled into the mined multiple coal coal reserves, studies of coal deposits, etc.
seams of the Ostrava Formation. 9 The government policy for the diversification
The design and technical performance of gob of gas resources.
wells fulfilled the following requirements: 9 The interest of the Czech Government and of
private companies regarding the exploration
9 Low drilling and completion costs in com- and production of coalbed methane.
parison to conventional gas wells, to ensure
profitability despite relatively low production According to Czech Mining Law, the area of
rates. virgin coal seams in OKR was divided among
9 Prevention of contamination of gob zones by four CBM concessionaires
drilling fluids.
9 D~lni prfizkum a bezpe6nost Paskov, a.s.
9 Maintenance of safety standards in drilling
(DPB, Inc.)
and production in accordance to regulation
9 Energie Kladno, a.s.
issued by the Czech Bureau of Mines.
9 Geologick~ prflzkum Ostrava, a.s. (GPO,
Inc.)
The gob wells were tested to yield funda-
9 Unigeo Ostrava, a.s.
mental information on production pressure,
volume of gas production and methane concen- A permit to explore for CBM was granted to all
tration, to allow estimates of profitability and to four companies. According to Czech Mining
provide a basis for planning to tie in the wells Law, the companies may expect to obtain a
into the production system of gas drainage production concession in the case of successful
plants already existing. results.
 M E T H A N E EMISSION F R O M O K R MINES 439

I ~-3 ~oa WELL II

+oo ~+.o.,,,,. ,,,oouc,.o..,,.

+o_ . . . . . . . .

150 - - - ; - - - / / i I. . . .

,oo....._.+//_. . . . . .

50 . . . . . ~ . ~/.:.4,+.+
" ~-~-wj
- w j ~ - - - ' - m -. - -. m. . . . . .. . . . m~--~-~.o__.__...~
, P- +, ~ _ = . . < d',--W_~l
.....

0 - IS" . . . . . . . . .
1 2 3 4 5 6 7 8 9 10
DAYS

WELLHEAD PRESSURE : CH4 C O N C E N T R A T I O N - " ~ - GOB GAS PRODUCTION

IkP-I I""I l"~'ml
"EJ-
9 UNDERPRESSURE -~-" ~ P R O D U C T I O N PERIOD
_ _
~p.] Imd'n~leel

Fig. 2. Short-term production test of the V-3 gob well.

IGV-3 GOB WELL

AS P R O D U C T I O N
Iio0. sc,,,It,J
100000

X
10000 - IIECALCULATEO TO 100% CH4 X

if( C:l----lil

, . , . ~ ~ --~" - " ' - +K-+-----I~----..#+_.+--~.--..~,~ .,.

1000
"%'~,: ..... X:

100
jl. .jk...~ 9 __" %" .I. .I. .t.. ....%'- 11= .Jl.. "+ ,lb.

10 i" ' ' i " I ! . . . . . .

7/93 0/93 9/93 10;931 lj93121931194 2/94 3/94 4/94 5/94 6/94' 71~14
' I ] ' '

MONTHS
- - , k - AVE.CI-14 C O N C E N T R . - - I - - AVE.UNDERPRESSURE - ~ . ' - A V E . C l I 4 PRODUCTION
I~1 I'+e'l I,,,,~/,+od
-I'~- TOTAL CH4 PRODUCT.

Fig. 3. Gas production of the V-3 gob well during first year of production.
440 G. TAKLA & Z. VAVRUSAK

According to the energy resource policy of the Each of the wells is continuously cored in the
Czech Government, CBM exploration is finan- Carboniferous interval to obtain primarily infor-
cially supported by the Ministry of Economy. By mation on the gas content in the rock sequence.
the end of 1994, nine CBM wells were drilled. Core samples of the coal are subjected to
Two of the wells were fractured, with promising standard canister desorption tests (according
results for future production. In April/May 1995, to the Standard of the US Bureau of Mines).
more four wells were fractured and long-term Simultaneously, coals and rocks surrounding the
pumping tests were started. Four to six new wells coal sampling points are tested to obtain
are expected to be drilled by the end of 1995. information required for the design and evalua-
DPB owns a concesion for CBM exploration tion of hydraulic fracturing of the coal. Drilling,
in ten prospection areas, covering a total of coring and completion are assigned to local
240km 2 of virgin coal fields that contain contractors, as is hydraulic fracturing of the coal.
4.1 • 10 9 tonnes of hard coal reserves. These The first pilot well was completed in the
areas are characterized by a high density of Karvinfi Formation's coal seams in the area of
exploration wells, drilled for coal, gas and water Ditmarovice at the begining of 1995. Successful
prospection on a spacing of some 1.5 km. hydrofracturing opened two coal seams (4.3m
Several geological evaluations and studies were and 1.4 m thick). A beam pump was installed to
carried out to assess the importance of the coal test water and gas production.
reserves and to build a database. Accordingly, The second pilot well in the Vficlavovice area
the coal deposits of these areas are well (Ostrava Formation's coal seams) did not realise
documented, with very good geological informa- the expected coal gas content and gas in place.
tion about each of the prospection areas. The third pilot well of DPB' s project is now
However, the occurrence of methane in virgin being drilled in the area of Fren~tfit (Karvinfi
coal seams is not well documented so far. For Formation). An additional one or two pilot
most of the prospection areas, data on gas wells are planned for spudding in 1995.
content of the coal are either not available at all,
or very incomplete at best. For this reason, a
CBM exploration campaign with a chance of Summary
success would first have to identify the most
favourable areas and coal seams by drilling pilot The paper presents information on some methods
wells. of coal gas processing and utilization in the
The CBM pilot project proposed by DPB, largest hard coal basin of the Czech Republic., i.e.
comprises six pilot test wells in the most the Ostrava-Karvinfi Mining District. Improve-
promising exploration areas, which are named ments in the methods of mine gas drainage,
as follows: increased recovery of methane from closed mines,
and new coalbed methane production from coal
9 D6tmarovice fields of the region could contribute to the world-
9 Petrovice - Vficlavovice wide aim at improving the use of clean energy
9 Pf'ibor - zfipad sources and reducing the emission of methane
9 T r o j a n o v i c e - Fren~t~it. into the atmosphere.
 Index

References in italics are to Figures or Tables borehole diameter, changes in 305-6

borehole surveys 406-7
Abbey Craig East Fault 396, 397, 398-9, 399, 400 boron, positive correlation with sulphur 259
acid mine drainage 290, 294 British Coal database 245, 249
adjacent strained volume 395-9 Brno granitoid massif 181
Af~in-Elbistan deposit 93, 95 brown coal
air pollution 261,365, 368, 371,374 liquefaction by hydrogenation 357-63
A1, in solution, toxicity of 291 North Bohemian coal basin 208, 210-16
algal coals 201-6 Yugoslav, different forms of sulphur in 269-72
algal mats 72 see also lignite
alginite 56, 108, 110, 201 BS 1016 350
Alpine Orogeny 50 Bulgaria, low rank coals 141-8
Andano-Chulman coal-bearing region 149, 150, 151, genesis of coal macerals 145, 147
151, 153, 154, 155-6, 158 geology of neogene deposits 141-3
vitrinite reflectance 154-5 Dacian coal-bearing province 143, 147
ankerite 289 Sofia coal-bearing province 142, 147
aquitards and aquicludes, M~eno-Roudnice basin 421 Strimon-Mesta coal-bearing province 143, 147
Asagibelova Formation 118 Thracian coal-bearing province 142, 147
Askale coalfield 124 petrology of neogene coals 143-7
asphaltenes 358, 363 Biiyiik seam 118, 119, 120, 123, 126-7
atrinite 145

caking and coking properties

Badin coalfield 237, 240, 241, 242 G6kler coals 122
Baklan Granite 118 South Yakutian coals 153, 158, 159
B~lce~ti coal complex 131 calcite 69, 107, 124, 289
Bara Formation 237 camouflet shotfiring 326, 327-8
Barbora units 24 Can deposit 90-1, 93
basin-fill Turkey 90-1, 93
M~eno-Roudnice basin 412 Cfinde~ti Formation 131
S Wales coalfield 162, 164-5 carbargilite 144
Belgium, underground coal gasification 386-7 13C NMR spectroscopy (CP/MAS technique)
Ben~itky nad Jizerou area 415 201-5
Berbe~ti Formation 131 carbonates 53, 110, 287, 289
Berkakit Member 150, 151 carbonization tests, Istanbul-Yenikov region
Bevercotes Colliery 257 coals 366-8
Beypazari deposit 88-9, 91, 98, 124, 371, 372 carbons
Bey~ehir deposit 93-4, 95 aromatic/alkenic 201
Bicir Formation 94-5 and protons, aliphatic 201,201-2, 202-4
Bilfi Hora Formation 421 Carpathian Mountains 321
Bilfi Hora (nr Plzeh) Carpathian Nappes 184
sandstone/claystone, Fe-oxides 35, 39-40 catalytic deactivation 349, 355
tuffite, single-component remanence 33, 38-9 ~ayirhan lignite field 371,372, 372-4
Bilina delta 208 cedrane 226
Bilina mine 310, 310, 316, 318 cement clinker production plant 380, 380, 382, 383
Bilsthorpe Colliery, sulphur high 257 cenospheres 293, 362
biomarkers Central and West Bohemian Basins 29
aliphatic, Maritza-Iztok lignite 219-28 outline geology 33-5
M~eno-Roudnice basin 420, 422 C~sk6 Stredohofi Mountains 208, 263
bitumen 226 chalcedony 62
aliphatic and aromatic portions 219-20 channel inflows, lake stages, N Bohemian Basin 314
analyses, South Yukutian coal basin 155-8 charcoal see inertinite
bituminite, Selimoglu coal 110 chlorite 288
bituminous coal 36 Chukurov deposit 142, 145
former Czechoslovakia/Czech Republic 5, 5-7 Chvaletice power station 267
M~eno-Roudnice basin 412-17, 418 Cixerri Formation 52, 53, 53-4
Point of Ayr 349-56 clay 137
Selimoglu unit 107 clay minerals 144, 288, 294
UK, ash content reflecting mineral content 287, clean coal technology 10
292-4 cleat density, near to faults 399
Bohemian Massif 29, 32, 33, 321,322 cleat mineralization, late diagenetic 110
Namurian paralic basin 13-27 cleating 393-4
442 INDEX

coal cutinite 110

breccioid 124, 129 Cypris Formation, pyrites 266
clayey 137 Czech Republic
detrital (detric) 135, 137, 208 coal production and usage 3-12
effects of low-temperature drying 365 constraints on limits of mining 8-9
forms of sulphur in 261-3 energy policy 1-2
fragmentation upon carbonization 368 workable reserves, bituminous coal 6, 6-7
high organic sulphur, amelioration for burning in
domestic stoves 371-7 deformation 16, 47, 165
humic (huminitic) 153, 214 degassing 401,402
hypautochthonous 70 degassing systems, capture of methane 426, 430
low rank Dejdekar volcanics 104
Bulgaria 141-8 deltas, in coal-forming swamps 315-16
conversion to liquid fuels by direct hydrogenation dense medium cyclone separation 350, 351-2
357-63 conversion and product distribution 352, 353
desulphurization by low-temperature element distribution during digestion 353-4, 354
carbonization 365-9 overflow fraction 351, 351,352, 353, 355-6
low rank lithotypes 195-9 underflow fraction 351,352, 356
origin of vanadium in 273-86 densinite 145, 214, 216
as raw material for chemical industry 7 density gamma-gamma logging 310-11
stages of formation 279 depositional environments
sulphur compounds in 269 and coalbed methane producibility 392-3
xylite/xylitic 136, 137, 208 different, Kolubara and Kostolac coals 271,272
xylodetric and semidetric 208 KY 9 coal seam 276, 279-80
see also bituminous coal; brown coal; lignite derelict land, restoration of, UK 290-1
coal cleaning 269, 291 Des-A-lupane 226, 227
coal extractability 212, 213, 215 desiccation
coal facies, term 131 Eocene 72, 73
coal gasification 269, 385-90 Pontian Basin 143
coal liquefaction, improvements in 349-56 desmocollinite 103, 107-8, 110, 112
dense medium cyclone separation 350, 351-2 destressing blasting 326, 327-8
liquefaction, original coal/coal fractions 352-5 desulphurization 9, 272, 297
coal minerals by low-temperature carbonization 365-9
and element emissions from power stations 292 detrital minerals, UK coals 287-8, 289, 294
influence on combustion residues 292-4 detrite 214
coal mines, abandoned, gas recovery from 437-8 diagenesis
coal mining, methane emissions from, Poland deep-burial 289
425-34 early, formation of FeS2, KY 9 seam 279
coal rank 393 marine 63
S Wales coalfield 166, 176 replacement of evaporites 62
relationship to thrusting 161, 167-9 Sulcis coal basin 65-7
variations with depth 161, 169-71 and sulphur distribution in Sindh coals 240
coal strata, split by sediments 311,314, 315, 316 diagenetic minerals, UK coals 288-9
coal swelling 215 dipolar phasing (DD) experiments 201
coalbed methane Dobruja coal, possible underground gasification 387-8
development in virgin coal seams 391,438-40 Dolni Vlk~, siltstone 41, 42
geological controls on producibility 391,392, 392-3, dolomite 63, 66, 69, 124
399, 401,404 dolomitization 72
migration in and around fault zones 391-408 post-compactional 69
models for retention and migration 401-6 Doupovske Hory Mountains 208, 263
research in the M~eno-Roudnice Basin 409-23 Drahanskfi Vrchovina Plateau 181
secondary gas generation 401,402 Dukeries coal 246
coalification 279 Duraji Member 150, 158
Bulgarian low rank coals 147
increasing with depth, M~eno-Roudnice basin 420 Eakring Anticline 257
intensity, Upper Silesian Coal Basin 20-3, 26 East Pennine Coalfield 406
N~m~i6ky area 189, 190, 191 EEC, Large Combustion Plant Directive 291
Cockshot Rock 171,175 electrolinking 388
coking coal, high sulphur, G6kler coalfield 115-30 Elga coalfield 149, 152-3, 153, 155
colliery spoil, UK 290-1 Elhovo deposits/lignite 142, 147, 389
condont CAI values, S Wales 173 gasification in a fluidised bed 390
coquinas 56 engineering stability, and weathering 289-90
~oraklar Formation 88, 372-3 Enna marine horizon 181
corpohuminite 214 epigenesis 32
 INDEX 443

Europe, present underground gasification position Goze Delchev deposit 143, 147
386-90 graphitic domains 205
evaporites, Sulcis coal basin 63, 72, 73 gravitational sliding/slumping 50
exsudatinite greenhouse gas emissions evaluation 425, 433
Grkler coals 124, 125-6, 126 grison 386
Selimoglu coal 110 G(ines ophiolite 103
gypsum 107
fault damage zones 395, 400
fault linkages 399-400
fault populations 400 1H NMR MAS technique 201,204
fault systems 34-5, 343, 394, 415 Hfidy-Rirka Limestones 181
Mgeno-Roudnice Basin 412, 414 haematite 32, 38, 41, 43, 46
strike-slip 403-6 Hanioglu unit 103, 104
fault zones 129, 394-5 Hantepe unit 103
burial history 400 heat flow, S Wales coalfield 173
and induced seismicity 329-35 heavy industry, Czechoslovakia 3-5
faults/faulting 257, 394-5 Hilt's Law 189
antithetic 343 excursions from, S Wales 169, 171,174, 175, 176
detected on FMS data sets 406 Hirka Formation 88
Karice deposit 340, 342, 343, 347 Holodnican Member 151, 158
normal 50, 396, 401,402 hopanes 226, 227
reverse 343, 401,404 Hrabfik mine 262
strike-slip 404 H~edle Member 415
virgate 343 Hru~ov Member 24, 26
Fe-oxides 41 humic acid 278
FeS2, formation of 279, 289 huminite 144, 145, 219
see also iron disulphides; pyrite N Bohemian coals 208, 211,216
Ffos Las OCCS 165-6, 167, 167-9 huminite reflectance 147, 214, 358
Ffyndaff OCCS 165 humoclarain 219, 221,226
flood events, and seam splitting 258 humoclarite 144
flue gas desulphurization 1269, 291,372 humotelinite 137
fluid combustion 10 humovitrain 195, 196, 197, 198, 199, 219, 220, 226
fluid migration hydrofracturing 387, 388, 407, 440
fault modification of 395-400 hydrothermal fluid flow 173, 176
through unfaulted ground 393-4 hydrothermal fluids 276
fluorinite 110
fly ash 293, 294 Iberian Plate 50
foreland basins 14, 26 illite crystallinity 167
fracture systems, and permeability 399 Ilnitsa Suite 229
fractures, detected on FMS data sets 406 inelastic scatter 300
fragrnentograms 222, 225, 226 inertinite 110, 113, 136-7, 144, 188, 219, 278, 349,
France, underground coal gasification 387 351
Free Swelling Index (FSI) 119, 122 N Bohemian coals 211,214
Fren~tfit Seismic Polygon 332 South Yukutian coal basin 153, 159
fulvic acid 278 see also fusinite
furnace bottom ash 293 inertodendrite 110
fusain 144, 195, 196, 197, 198, 199 iron 257
fusanization 198, 199 ferric, ferrous, covalent 196-9
fusinite 201,205, 281,317 iron disulphide/sulphide 211,213, 214
6345 values in 261-7
gelification, huminite 211 diagenetic 264, 266, 292
gelification index (GI) 214 epigenetic 264, 266
geophysical logging 406 synsedimentary 263-4, 266, 267
Germany, underground coal gasification 386
gob wells 438, 439
Grc~iktepe sediments and alluvium 118 Jaklovec Member 16, 17, 21, 24, 181, 191
goethite 39, 41 jarosite 278
Grkler coalfield 115-30 Jelenice Member 412, 415
caking/coking properties of coals 122 Jerma seam, fusinite 201,205
geological setting 118-19 Jeseniky Mountains 321
iso-reflectance map/values 127-9 Jiu-Motru Formation 131
mineral matter of coals 122-4 Jizera fault system 415
G6kler Formation 118 jointing, and fluid migration through coal 393-4
seams in 118, 118-19 Juhta Member 150
444 INDEX

Kabakta Member 150, 151 limestone

Ka~ice deposit dolomitic 119
coalfield data 339-40 micritic 101, 103
history of 337-9 reef 181
post-sedimentary faulting 340, 342, 343 Lin6 Formation 337, 409, 412, 415
Ka6ice depression 338 lipids, bacterial 221
Kalbur~;ayiri Formation 94 liptain 144, 195, 196, 199, 225
Kammenn~, Most Member 412 bitumen content 220, 220
Kangal deposit 94-5, 96 liptinite 119, 144, 153, 159, 188, 219, 349, 351
kaolinite 124, 293 N Bohemian coals 211,214, 216
kaolinite precipitation 67 Selimoglu coal 103, 107, 108, 111, 113
Karacahisar volcanics 118 liptobiolite 208
Karadoruk Formation 88 liptodetrinite 110, 208, 214, 216
Karakaya fault zone 129 Litom6fice Deep Fault 35
Karliova deposit 96-8 Llanharan Colliery, excursions from Hilt's law 171,
Karsakatepe deposits 118 175
Karvin/t Formation 188 Llannon Disturbance 167, 167
Kerme Formation 85, 87 logging correlation scheme, N Bohemian Basin 309-20
Khadro Formation 237 Lom coal deposits 143, 147
Kjustendil coals 143, 144 Lom depression 143
Kladno Basin 6 Longannet mine, Scotland 395-9
reflection seismics 340, 341 Lubnfi seams 337, 338
stratigraphy of 337-9 Lu2ice-Labe line 419
Kladno coalfield 337, 342, 343
Kladno Formation 34, 337-8, 409, 412 Macocha Formation 181
Kladno mine 337-47 magnetic remanence
Kolubara coal/lignite 269, 270, 271, 271,272, isothermal (IRM) 37, 40-1
379 multi-component 39, 41, 46
Kolubara mines, 'Tamnava' field, brown coals, single-component 33, 38-9
liquefaction by catalytic hydrogenation magnetic remanence components, W Bohemia 29-47
357-63 magnetite 39, 41, 46
Kop~ivnice-T~inec uplift 26 magnetization
Korycany Member 421 chemoremanent/thermoremanent 32
Kostolac coal 269, 270, 271, 271-2 two-component 39
Kounov coals/seams 412, 415, 416 viscous 42
Kounov Member 412, 415 Main coal seam, Most Formation 207-8
Kozloduj coal deposits 143 logging correlation scheme for 309-20
Kozluca Formation 110-11 Main Ostrava Wetstone 19, 22, 25
Krugn6 Hory Fault 208 Malkara deposit 85, 88
Krugn~hory Mountains 262 marcasite 262, 263, 266, 288
supplying sulphate to N Bohemian Basin 266 marine facies, Ostrava Formation 24
Kru~n6hory piedmont coal basins 8 Maritza East deposit 142, 147, 389
KiJc[ik seam 118, 119, 120, 122, 123, 126-7 Maritza-Iztok coal basin 195-9
lignite, aliphatic biological markers in 219-28
maximum maturity temperatures, S Wales coalfield
lake phases, peat-swamps 313, 314-16 171, 173
Lakhra coalfield 237, 239, 240, 241, 242 megasequences, transgressive-regressive 51-2
Lakhra Formation 237 M61nik Coals 412, 415
La2finky Limestones 181 M61nik Interjacent coal seam 415
Ledce Member 412 M~lnik Main Seam 415, 415-16, 422
Ledce-Z;ilov, red claystone pit, two-component estimation of CBM reserves 416-17
magnetization 42-3, 44 Mengin deposit 85, 87
Leonard seam, lower whetstone 25 M6nin block 181, 184
Libou~ mine 314, 314 metamorphism 166-7, 276
lignite methane emission
Bulgaria 147 Polish coal mining 425-344
Czechoslovakia/Czech Republic 4, 4, 5 from mining processes 426, 428
Istanbul-Yenikov region, low-temperature from post-mining activities 426, 431
carbonization tests 365-9 utilization, Ostrava-Karvinfi coalfield 435-40
Kolubara, use in cement rotary kilns 379-83 methane release, from coal 426, 430
Maritza-Iztok coal basin 219-28 micro-karst 53, 56
Turkey 77-99 Mililolitic Limestone Formation 52, 67
lime, as sorbent for amelioration of high sulphur coal Mililolitic Limestones/Produttivo Formation
374-6, 377 boundary 53
 INDEX 445

mine gas drainage Northern Anatolian Fault Zone 124

from abandoned mines 437-8 N ~ a n y Member 338-9, 347, 409, 412, 421
Ostrava-Karvin~t coalfield 435-7 coal seam groups 415, 416
mineral alteration, South Yakutian coal basin 158-9
mineralization
Ogulbey Formation 103, 104
antimony, G6kler coalfield 115, 116, 117, 129
Ollerton Colliery 257
hydrothermal 129
Oltenia coal basin 131-9
S Wales coalfield 173:-4
main characteristics of coal facies 134
sulphide, syngentic and epigenetic 211
main coal facies and lithotypes
mining
aquatic macrophyte prairie 137-8
longwall, seismic energy release during 323-4, 325,
deciduous forest 135-6
326
forest swamp 136-7
opencast/opencut/open pit 998, 149, 151,208, 290
grassy marsh Carex spp. 135
Miro6 seam, fusinite 201,205
reed swamp 137
Miro~ov, 'Lomy na Janovr' quarries, siltstone 36, 40, 46
Orhaneli deposit 91-3, 94
Mn, toxicity of 291
orogenic trend, Variscan 24
Moesian Platform 143
Orta deposit 96, 97
monosulphides 269, 271
Ostrava Formation 13-14, 16-24
Moravian-Silesian Paleozoic Basin
changes in petrographic/geochemical composition
paleogeographic features 25-6
25, 26
paralic morasse 13-14, 16-24
Nrmrirky boreholes 181, 184, 191
partial troughs within 14-15
vertical changes in development of 24-5
Mrssbauer spectroscopy 195-9, 278
Ostrava-Karvinfi coalfield 13
Most Formation 207-8
induced seismicity related to fault zones 329-35
Motru coal complex 131
seismicity and mining situation 330-1
M~ec Member 412
seismological monitoring 331-2
M~eno-Roudnice Basin
tectonic and geomechanical situation 330
coal deposits 412-15
Karvinfi area
geochemical evaluation of samples 417, 418
evaluating seismicity of tectonic zones 332
technological properties of coals 415-17
fault systems in 330
geological setting 409-12
methane emission and its utilization 435-40
hydrogeology 421
coalbed methane development, virgin coal seams
research into coalbed methane 409-23
438-40
thermal history 418-21
gas recovery from abandoned mines 437-8
mudrocks
seismic monitoring for rockburst prevention 321-8
behaviour during weathering 289
induced seismicity, long-term observations 322-5
chemical alteration a rapid process 290
local seismographic network 321-2
Mu~la region (Yata~an-Milas) deposits 85, 87, 89
regional seismographic network 322
multicomponent statistical analysis 302, 304, 305
use of observations in geomechanical practice
Munzur limestones 110-11
325-8
Muratdagi Melange 118, 129
Seismic Polygon 331-2
Muratdagi region 122, 129
workable coal reserves 5-7
Myslejovice Formation 181
workable reserves 5-7
oxidation 198, 199, 289-90
Namurian paralic molasse, Bohemian Massif 13-27
oxides 287
natural gas, use of 10
oxyhumolites 208
with pulverized lignite in cement rotary kiln 379-83
Nrmri~ky area 13
age of coal bearing rocks/coal fragments 184-5 Pakistan, distribution of sulphur in Sindh coals 237-43
coal found in deep boreholes 179-81 palaeobiotopes 133, 134
coal petrology 185-9 palaeoclimate
geology of 181-4 Oltenia coal basin 133
S extension of Early Namurian deposits 179-93 Transcarpathians 234-5
Nerjungra Member 150, 151 palaeogeography
Nerjungry coalfield 149, 156 development of N Bohemian Coal Basin 311-20
Nesvarilka Block 184 of Oltenia coal basin 132-3
Netherlands, underground coal gasification 386 palaeogeothermal gradients, S Wales coalfield 161,
North Bohemian Coal Basin 207-17 169, 170, 171-3, 176
analyses, elemental, petrographic and technical 209, palaeomagnetic directions 43-4
212-16 palaeophyocoenoses, Oltenia coal basin 133-5
constraints on mining 8-9 palaeosalinity 259
634S values in iron disulphides 261-7 palaeosols 56
geological setting 263 palaeostress, Ostrava-Karvin~ basin 330
logging correlation, Main coal seam 309-20 palaeovalleys, containing coal seams 338
446 INDEX

palynomorph assemblages, Upper coal formation quartz mineral 122-4

230-6
parasequences, Produttivo Formation 54, 70-1
Park Colliery, rashings in New Shaft 171,175 Radrice (nr Plzefi)
Park Slip OCCS 165 claystone, multi-component remanence 39, 41
Parkgate Coal, S organic and pyritic 291,292 siltstone 40, 41
Parkgate seam 247, 248 Radnice Member 337, 338, 409
ash-sulphur relationships 253-4 fault detection in 340, 341
subdivisions, E Pennine Coalfield 248 'rashings' 171, 175
sulphur distribution 249-57 reflection seismics 406
controls on 257-9 common-midpoint method, Kladno Basin 340, 341
partial block structure, Ostrava-Karvinfi basin 330 reservoir pressure, controlling gas content 426
peat accumulation, Dacic Basin 131 resinites 110, 144, 227
peat mire, complex controls in causing sulphur rockbursts 330, 334
variations 258 seismic monitoring for prevention of 321-8
peatbog phases, peat swamps 313, 316-17 Rosice-Oslavany vasin 57
peatbogs rotary kiln, wet process 380, 380, 382, 383
final destruction of 317 Roudnfi (nr Plzefi), claystone, isothermal remanent
metal salts in 198 magnetization 37, 40-1
permeability, and coalbed methane production 391,
393
Peruc Member 421 sealing, by fault damage zones 395
Pet~kovice Member 16, 17, 20, 24 seam plies
phosphates 287 Parkgate seam 245, 258
phyllocladane 225 ply-by-ply mapping 257, 259
c~-phyllocladane 221,225, 226 seam splitting, and sulphur content 258
/3-phyllocladane, and thermal maturity 225-6 seam sulphur maps, generation of 249
Plzefi Basin 30-1, 34 sedimentary particles, petrography of, Sulcis Basin
pollution 4 62-5
by underground coal gasification 388, 388 sedimentation 310
see also air pollution coal-forming 311-20
polyaromatic structures 204-5 cyclic
porewaters 291 Early Namurian 181, 184
from fly ash sites, contamination source 293, 294 N~,~'any Member and T~nec Formation 339
potential source of sulphate to coal seams 257-8 Oltenia coal basin 132-3
a residual sulphate reservoir 266 influence of eustatic movements on 25
porosity, secondary, and feldspar dissolution 66-7 S Wales coal basin 162, 164
Poruba beds/Member 24, 181, 184, 191 seismic activity, natural and imposed 321
power industry, coal from N Bohemian coal basin 208 seismic monitoring for rockburst prevention 321-8
Produttivo Formation 50, 52, 67 seismic reflection surveying 406
diagenetic products 65-7 seismicity, induced, Ostrava-Karvin/t coalfield 322-5
intertidal facies 55-6 relationship to fault zones 329-35
overlying palustrine-lacustrine facies 56 seismological monitoring 331-2
parasequences in 54, 70-1 sources generated in stress concentration zones
regressive trend 60 335
subtidal facies 54-5 spatial distribution of hypocentres 322-4
supratidal facies 56 tectonic and geomechanical situation 330
Progressive Easy Slip Thrusting (PEST) 166 Sekk6y Formation 87
psammite tongues, N Bohemian Basin 315, 318 Selimoglu coal field 101-14
Pyrenean orogeny 50 geological setting and stratigraphy 102, 103-5
pyrite 107, 144, 197, 198, 199, 250, 257, 271,272, mineralogy 107
288 petrographic composition/depositional
containing elements of environmental concern 292, environments of coals 107-11
294 Selimoglu unit 103-4
framboidal 67, 110 semifusain 144, 195, 196, 197, 198, 199
G6kler coals 124 Seyit6mer deposit 90, 92, 124
in KY 9 seam coals 278-9 siderite 65, 67
massive 110 silicates 287
N Bohemian Basin 262, 263, 264, 266 silicification 129
oxidation of 289-90 diagenetic 72
and S02 emissions 291-2 Slan2~ Formation 34, 337, 339, 409, 412, 421
syngenetic 214 coal seam groups 415
underground oxidation of 290 slip, in UK coalfields 393, 394
see also iron disulphides smectite, inteparticle expansion of 289
 INDEX 447

smog, Czech Republic 9-10 sulphur 264, 266

Smr6iny unit sulphides 266 Beypazari coal 373-4
SO2 emissions 269, 374, 377 distribution
from pyrite and organic sulphur 272 multi-bed seam (Parkgate seam) 245-60
and Large Combustion Plant Directive 291 in Sindh coals 237-43
and role of pyrite 291-2 elemental 261,262
soft coal 208 forms of 261-3, 269-72
Softa-1 and Softa-2 formations 88 organic 261,269, 271,272, 291,374
Soma deposit 87-8, 90 pyritic 269, 271,291,374
Sonahri Formation 237 sulphate 261,271,291,374
sorbent addition, amelioration of high sulphur coal sulphide 261,262-3
374-6, 377 see also iron disulphide; pyrite
South Wales coalfield 161-78, 401 volcangenic 266
coal rank sulphur content
development related to thrusting 161, 167-9 affected by depositional and post-depositional
variation with depth 161, 169-71 controls 257-9
comparison with Ruhr coal basin 176 determined through gammaspectroscopy 297-307
metamorphism 166-7 high
role of fluids 173 Gfkler coking coal 115-30
stratigraphy 161-4 Selimoglu coal 107, 113
structure 164-6 Istanbul-Yenikov region lignite 366, 366, 367
South Yakutian coal basin, Siberia 149-60 Main coal seam (Most Formation) 213
bitumen analyses 155-8 N~m6i~ky area coals 189
Cretaceous flora 153 total, G6kler coals 121-2
geological setting and stratigraphy 150-3 /534S values, in lignite of N Bohemian Basin 264-7
Jurassic flora 151, 153 Susta marine unit 24
mineral alteration 158-9 swamp environment
proximate analyses and vitrinite reflectance values Dacic Basin 131-8
153-5 G6kler coal 122
Sozopol, Gulf of, coal deposit 142 N Bohemian brown coal 313-18
sparites 63 Selimoglu coal 107, 110, 111
spectra, processing methods 301-3 Syllach coalfield, bitumen anayses 155
spectra deconvolution 302, 304, 304, 306 syngenesis 32
spectrometric detectors 301
spectrometric logging probe 301 tasmanite (algal coal) 201,202-4
radius of investigation of 305 tectonic dislocations, Ostrava-Karvinfi basin 330, 332
sphagnales 234-5 tectonics
sporinite 110, 111,202, 214 extensional 50
G6kler coals 124-5, 126, 129 tectonic zones, Bulgaria 142, 143, 147
stable isotopes, Sulcis coal basin 67-70 telinite 159
steranes 226 telocollinite 103, 112, 119, 124
strain release, Ostrava-Karvinfi coal mines 327 textinite 214
stress fields 400, 422 Tharparker coalfield 237, 238, 240, 241, 242
primary and secondary 330 thermal demagnetization 36, 42, 42, 43, 45
subbituminous coal, Italy 49 thermal neutron capture, interferences generated in the
sublimation 264 spectrum 300
subsidence Thracian valley, coal formation in post-tectonic
basinal 25-6 depression 141
N6m6i6ky area 181 thrust detachments, Variscan 165-6, 171,173, 175, 176
Variscan intermontane area 34 thrust faults 184, 401-2, 403
Sulcis coal basin, SW Sardinia 49-75 thrust ramps 164, 165, 402, 403
depositional setting 70-3 thrusting, S Wales coalfield
diagenesis 65-7 relationship to coal rank development 167-9
facies spectrum and distribution 53-60 in seam 171, 173, 176
geological setting, palaeogeography and tissue preservation index (TPI) 214
stratigraphy 50-2 Tlustice (nr Zebr~ik), tuff-tuffite, two-component
petrography and geochemistry 60-5 magnetization 34, 39
revised depositional model 73 Tokin coal-bearing region 149, 151, 151, 152-3, 153,
stable isotopes 67-70 155, 158
sulphate 257, 269, 271,278-9 toluene, use of in coal liquefaction 349
reduction to sulphide 279 torbanites (algal coal) 201-2
sulphate ions, leaching by meteoric waters 240 trace elements, in fly ash 293-4, 294
634S values, in iron disulphides 261-7 transgressive cycles, Lower Eocene 70
sulphides 278, 287 trimacerites 144
448 INDEX

Trimsaron Disturbance 167, 167 KY peat-forming system, physicochemical

triterpanes 226, 227 conditions of deposition 283-4
Tunqbilek deposit 89-90, 92, 124 origin of VO2+-non-P 279-80
Turkey 89-90, 92, 124 origins of V from within and from above theories
Turgut Formation 87 280-1
Turkey, lignite deposits 77-99 primary and secondary V 281-3
Eocene lignites 80-1 pyrite (FeS2) and other S compounds 278-9
Oligocene lignites 81 vanadylation, of KY 9 seam 279-80, 284
Miocene lignites 81, 82-4, 85 ventilation emissions of methane 426, 428, 435
Pliocene lignites 85, 86 Vil~movice Limestones 181
named deposits described 85-98 virtual pole positions, Westphalian and Stephanian
T~,nec (Tinec) Formation 34, 337, 347, 409, 415, 421 rocks 43-4, 45, 46, 47
cyclic sedimentation in 339 vitrinite 153, 159, 188, 349, 351
Selimoglu coal 103, 107, 108, 113
vitrinite reflectance 129, 154, 167, 176, 276, 417, 420
UK Ffos Las OCCS 167-9
mining data sets 406 N6m6i6ky area coals 189, 191
underground coal gasification 387 volatile matter contents, G6kler coal 120-1
UK coals, environmental impact of minerals in 287-95 volcanic ash 235
ulminite 214, 216 volcaniclastic rocks, in Variscan foredeep 18-19
Upper coal formation, Ilnitsa Suite, floristic characters volcanism
of 229-6 Des Moinesian, and V in KY 9 seam 280-1,282
Upper Silesian Coal Basin 6, 179, 191 Neogene, Turkey 88-9
Beskydy piedmont area 3-5 Vrgany mine 316
lithostratigraphy 180 Vrganyvsand-clay accumulations 315
Polish 8 Vrgka Cuka anthracite 201,204-5
methane content and rate of desorption 426
regional division according to methane content 428, weathering 46
429, 430 minerals associated with coal 289-90
see also Ostrava Formation; Ostrava-Karvinfi well logging, and use of gammaspectroscopy 297-307
coalfield wireline logging 406
USA
coalbed methane production 391 xylain 144, 195
origin of vanadium, KY 9 seam 273-86 Maritza-Iztok coal basin 195, 196, 197, 198, 199, 219,
underground coal gasification 386, 388, 388 220, 226
Usmun coal-bearing region 149, 150, 151, 154, 155, xylite 214
158
USSR (former), underground coal gasification stations Yamadag lava flows 105
385 Yata~an Formation 87

Zatec delta 208, 262

Valea Vi~enilor coal complex 131 Zd6tin coals 415
vanadium, origin of in US coals (KY 9 seam) 273-86 Zd6tin Horizon 412, 415
depositional environments, and thermal history Zihle (red claystone pit), claystone, viscous
276-8, 279 magnetization 42, 43
 European Coal Geology
and Technology
edited by
R. A. Gayer (University of Wales, Cardiff, U.K) and
J. Pesek (Charles University, Prague, Czech Republic)

Despite the decline in the coal mining industry across Europe during
the last decade, coal continues to supply a major part of the growing
global energy requirements, particularly in the developing countries.
During this period there has been a shift in coal extraction techniques
from deep underground mines to open pit mines, reflecting cheaper
production costs in a market economy. It seems probable that the
European coal industry is now entering a period of stability. However, the
change to opencast mining has highlighted environmental issues and the
need to solve these problems.
This volume presents 39 papers written by coal scientists in the
forefront of European coal research. The papers cover a wide spectrum of
coal geology and technology, with sections on regional coal reserves,
coal basin tectonics and stratigraphy, coal petrology and palaeontology,
mineral matter in coal and the environment, mining geophysics, coal
technology and coalbed methane. Many of the studies describe coal
deposits from Central and Eastern Europe, some of which are not well
known in the west, so that the papers and included references will provide
an invaluable data source.
This book will be of value to all coal scientists in both the extraction and
energy industries and to academics. It will also be a useful reference for
students at both undergraduate and postgraduate levels.

• 448 pages

• 229 illustrations

• 39 papers

@ index
ISBN ! i.-;97799 86 1

Cover illustration: Rotating bucket excavator

(TC2-K800) of the North Bohemian Basin cutting
lignite of Main Seam in Vrsany Open Pit near Most,
Czech Republic.