Technium BioChemMed Vol. 2, Issue 2 pp.

28-38 (2021)
ISSN: 2734-7990
www.techniumscience.com

Physical and Geochemical Assessment of Limestone of Amran

Group in Arhab Area-North Sana'a for Industrial Uses

Ali M. Qaid1, Naji Alqubati2 and Ali M. Al-Hawbani3

1. Dep. of Civil Engineering technology, Al-Hajar (Qabitah) Community College/ Lahj,

E-mail: [email protected]
2. Geological Survey and Mineral Resources Board, Sana'a, E-mail: [email protected]
3. Dep. of Geology & Environmental Sciences, Faculty of Applied Sciences, Thamar University,
E-mail: [email protected]

Abstract

The present study is aimed to evaluate the potential of using limestone of Amran Group in
Arhab area in different industries. X-ray diffraction pattern revealed that the limestone from
Arhab is dominantly composed of calcite. The physical analysis showed that the bulk density is
ranging from 2.4-2.88 g/cm3, water absorption 0.4-2.32%, void ratio 0.01- 0.06, whiteness
87.78-90.2 and specific surface area 3900-4650 cm².g-1. Based on the XRF results, limestones
are pure and dominantly composed of calcium carbonate 97.52-99.06%. The concentration of
major oxide: CaO is ranging from 54.70 to 55.50 wt%, SiO2 0.20 - 0.80 wt%, Al2O3 0.2 – 0.4
wt%, Fe2O3 0.13-0.28wt% and MgO 0.40-0.60 wt%. The other oxides are present with low
concentration. Loss on ignition value varied from 42.40 to 43.16 wt% and exhibits strong
positive correlation with CaO which attributed to the highest concentration of CaCO3.
Geochemical data combined with Physical analyses data indicated that the limestone of Arhab
area is suitable to be raw materials for various chemical industries such as paint, papers,
ceramics, steel, pharmaceutical products and plastics after slightly modification of iron oxides
in some special industries.

Keywords: Amran Group, limestone, Arhab, calcium carbonate, physical analysis, XRD, XRF

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1. Introduction
The study area is located at about 10 km north of Sana'a, between 41573 5 - 434580 E and 1734960 -
1767993 N and covering about 650 km2 (Figure 1). Yemen is endowed with huge natural resources of
rocks and minerals. Limestone rocks are the most widely distributed rocks in Yemen. In this research
limestones of Arhab area were elected because of their high purity (high CaCO3 content), high
physical and mechanical properties, huge of quantities, and low cost of quarrying the raw materials
and transportation.

Study
Area

Figure 1. Satellite image (ASTER) shows study area

In Yemen, the applications of limestone are limited only to construction (aggregates, dimension, and
ornamental stones) and industrial purposes (cement, lime, animal feed, agriculture). That is due to of
the scarcity of applied studies of limestone rocks. Cement manufacturing is considered one of the
most important industries that depends on limestone rock, there are 6 plants currently working. For
other industries like paint, paper, medicine, etc., limestone is imported from outside the country.
Investigation of carbonate rocks in Yemen could be co-associated in the growth of a number of
industrial and agricultural fields that lead to urban development. Limestone is commonly defined as a
rock composed of calcium carbonate (CaCO3) however, most limestone rocks contain significant
amounts of magnesium, silicates, manganese, iron, titanium, aluminium, sodium, potassium, sulphur
and phosphorus. They are formed from the dissolved organic matter of calcareous organisms and
inorganic materials, which rely on their environmental deposits, and are then deposited and compacted
into rock by lithification process over geological time [1], [2]. They can occur in various depositional
environments, such as non-marine, shallow marine platforms and deep-sea environments [3]. The
majority of carbonate sedimentary rocks are deposited from seawater and made by bioclastic
accumulation of calcareous organisms [4], [5].
Numerous classification schemes for carbonate rocks have been proposed [6]–[13]. [6], described
limestone rocks in terms of discrete grains (such as biogenic fragments) or "allochems" dispersed to a
greater or lesser extent in a matrix of microcrystalline calcite ooze (micrite), or a crystalline cement

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(spar). Although the wide distribution of calcium carbonate, white calcium carbonate is rare [14]. Iron
and manganese oxides, organic matter, and pyrit are the main dark substances that affect the whiteness
of calcium carbonate [14], [15]. With over a hundred industrial uses, limestone rock is probably the
most useful of all industrial rocks and minerals. These include building (aggregates, rail ballast and
dimension stone), mineral fillers (in paper, paint, plastic, rubber and pharmaceuticals), adhesives,
abrasives, fertilizers, food additives, environmental applications (acidity neutralization, flue gas
desulphurization, soil conditioning and stabilization), and production of cement and lime [16]–[23].
The widely used of calcium carbonate in industrial application because of their special properties: high
purity, whiteness, ease of access, average particle size and distribution, etc. [24]–[28]. Limestons are
usually used as inert fillers to complete a large variety of final properties without increasing the costs
through replacing a more expensive material with an inexpensive one. Fillers also improve the specific
characteristics such as hardness, brittleness, impact strength, compressive strength, softening point,
fire resistance, surface texture, electrical conductivity, and so on [29], [30].
Figure 2 shows the world lime production in 2019 in million tons [31]. China ranked the first
production in the world with the total amount of 300,000,000 tons and the second one is USA with
18,000,000 tons. [16], [17], [32], [33], classify the purity of limestone rocks according to carbonate
concentration to: > 98.5% CaCO3 very high purity, 97.0 to 98.5% high purity, 93.5 to 97.0% medium
purity, 85.0 to 93.5% low purity and 50.0 to 85.0% impure (Table 1). Very high purity limestone is
defined as carbonate rock that contains greater than 98.5% calcium carbonate (usually as calcite). The
British geological survey (BGS) has used this classification in all major limestone resource work
carried out in the UK and other parts of the world [34].

0 100 200 300 400

CHINA 300
UNITEDSTATE 18
INDIA 16
RUSSIA 11
BRAZIL 7.6
JAPAN 7.1
GERMANY 5.2
KOREA 4.7
TURKEY 3.6
ITALY 3.3
IRAN 2.7
POLAND 2.6
FRANCE 2.2
ROMANIA 2.1
UKRANIA 2.1
AUSTRALIA 1.8
SPAIN 1.8
CANADA 1.6
MALAYSIA 1.5
BULGARIA 1.4
UNITED KINGDOM 1.3
BELGIUM 1.2
SOUTH AFRICA 1.2
SOLVENIA 1.1
CZECHIA 1.1
KAZAKHSTAN 14
OTHER WORLED TOTAL 240

Figure 2. World lime production 2019 in million tons [31]

Table 1. Limestone purity classification according to [16], [17], [32], [33]

Purity Cao Possible industrial uses (grouped by minimum
CaCO3 wt%
classification wt% CaCO3 specifications)
Steel, white glass (subjected to trace elements), rubber,
Very high purity > 98.5 > 55.2
plastics, paint
High purity 97.0–98.5 54.3–55.2 Iron, ceramic,
High purity 97.0-98.5 54.3-55.2
Portland cement, whiting, chemical uses
Medium purity 93.5–97.0 52.4–54.3 Paper (subject to
Medium purity 93.5- 97.0 52.4-54.3
color), animal feedstuffs (subjected to level
47.6–
Low purity 85.0–93.5 Asphalt
52.4
Mineral wool, natural cements (subjected to silica/clay
Impure < 85.0 < 47.6
mineral ratio)

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2. Geological Setting
Limestone of Arhab area belongs to Amran Group (Amran Limestone rock) which is one of the most
widely distributed sedimentary cover unit in Yemen. Geological Survey and Mineral Resources
Board-estimated the geological reserve of carbonate rocks in Yemen as: pure limestone 3.6 billion
cubic meters, limestone rocks 10 billion cubic meters, magnizite 58 million Cubic meters and dolomite
3.4 billion Cubic meters [35]. Amran Group is a thick series of dominantly calcareous sediments, but
locally including significant sequences of shale and evaporates; the carbonates are commonly massive,
fissured rocks (Figure 3). The Amran Group consists mainly of limestone, marly limestone, shale beds
and thick beds of evaporites (salt rocks and gypsum), characterized as the Sabatain Formation in
Shabwa “surface outcrops” and Safer “subsurface” areas [36]. The name of this group is derived from
Amran town, which in the sequence is very clear (best exposed). [37], classified Amran limestone into
two groups: the lower group (the Amran Group Middle-Upper Jurassic) and the upper group (the
Sabatayn Group upper Jurassic-lower cretaceous). The maximum thickness of Amran Group may
exceed 800 m. Amran limestone is a complex group, with two main depositional environment; a
neritic environment (limestone and marly facies) and a shallow-water environment (evaporitic
sequence). The tectonic effects on Amran Group at Arhab area is less comparing to other places
covered by Amran Group. Weathering and erosion also showed less effect. The elevation of Arhab
area ranges from 1735 to 2775 m above sea level (Figure 4).

Study
area

Wadids and outwash plain deposits gravel, sand, Quaternary basalt: Basic volcanic ash and lapilli;
silt and loess vitrophyric basalt; basaltic lava flow

Tawilah Sandstone: Sandstone, fine to coarse Amran Limestone; Lower Basin Facies: Limestone
grained; conglomeratic sandstone; interbedded and dolomite, intercalates sandstone; fine- grained
gray, green and reddish shales brownish patch reef; oyster debris
Amran Limestone; Shelf Facies; Limestone and dolomite, massive thick; alternating fossiliferous marl and limestone
Figure 3. Geological map of study area [39]

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Study
area

Figure 4. Digital elevation map showing the altitude of the study area
3. Materials and methods

Field work involved collection of representing rock samples with their locations using GPS and other
geological information. X-ray diffraction and physical analysis were carried out at Saudi Geological
Survey (SGS), Central lab of Geological Survey Board-Sana'a (GSMBR) and Faculty of Engineering,
Sana'a University. Samples for XRD were prepared by grinding without treatment to very fine
particles then testing using XD-2/ XD-3 Goniometer Type vertical: 00-2 θ scan: 0-θ scan high, single-
phase 508Z, 220V, max. 60 kw, rated powder 3Kw. This determines the presence and purity of calcite
and common impurities such as quartz, feldspars, clay minerals, pyrite and iron oxides etc. The
physical analysis including surface area, bulk density, water absorption, whiteness and void ratio were
carried out according to American Standard (ASTM). Chemically, whole rock geochemical analyses
for major oxides of part of samples were carried out using X-Ray Fluorescence Spectrometer (XRFs)
techniques, WDXRF 1Kw, S8 Tiger Pruker AXA, AG-RH tube at the central laboratories of GSMRB
and the other samples were analyzed in SGS. The pH measurement is the measure of the acidity or
alkalinity of a solution. The pH value was measured at room temperature using a pH meter.

4. Results and Discussion

The XRD analysis of studied samples of limestone from Arhab area indicates that the limestone is
pure and composed mainly of calcite (Figure 5). The Physical test results showed that the whiteness
value is ranging between 87.78-90.2. The slight decreasing of whiteness refers to the slightly
increasing of dark minerals especially iron oxides content [28]. The bulk density ranges 2.4-2.88
g/cm3, water absorption 0.4-2.32% and void ratio 0.01-0.06. The specific surface area is ranging from
3900-4650 cm2/g (Table 2). The result of the major oxide composition revealed that limestone rock of
Arhab is pure with high content of CaO which ranging from 54.70 to 55.50 wt% with an average of
55.22 wt%, accordingly the CaCO3 content ranging from 97.52 Wt%-99.06 Wt%. The other oxides are
present only with a small concentration (Table 2). SiO2 content varies widely ranging from 0.20 to
0,80 wt%, which is contributed by quartz, Al2O3 0.2-0.4 wt% and the total alkali value is regarded as

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low (Na2O + K2O) 0.06-1.50wt%. The low levels of Al2O3, K2O, Na2O, and SO3 related to the
decreasing spread of clays. MgO contents 0.4-0.6 wt%, the extremely low content indicates a weak
dolomitization process of the limestone. The Fe2O3 content is ranging from 0.13 to 0.28 wt% (Table
3), and varies from place to place due to the distribution of tectonic discontinuity, bedding planes and
clays. A slight increase in iron oxides could be related to surface sampling as iron oxides fill joints and
bedding planes. The loss on ignition value ranging from 42.40 to 43.16 wt% with an average 42.88%,
suggesting a high carbonate content for the limestone (Table 3). SiO2, Al2O3 and Fe2O3 contents show
strong negative correlation with CaO (Table 3 and Figure 6 a,b,c). The negative correlation between
CaO and SiO2, this is because of the fact that the CaO (from calcite) and SiO2 (from quartz) are from
two different mineral phases and they are not related [38]. LOI shows strong positive correlation with
CaO content which may be due to the reason that LOI is contributed mainly by the carbonate content
of calcite. It also shows negative correlation with SiO2 (Figure 6d,e and Table 4). Plotting limestone
samples on the Al2O3 – CaO – (MgO+FeOt) ternary diagram shows that all samples are rather pure
limestones with few Fe – Mg enrichment (Figure 7). The pH range of 8.3 to 8.6 indicates alkalinity
(Table 2).
Field observation, geological map, and satellite image (Figure 1,3) showed that the tectonic
discontinuity and cavities are less comparing to other limestone rocks in different places, that
associated with decreasing of impurities minerals and increasing the purity. Comparing properties of
limestone of Arhab area with [32], [33] classification Table 3 indicated that limestone marked in very
high purity to medium purity categories and that meet the requirements of different chemical
industries includes: paint, paper, pharmaceutical, ceramic, rubber, adhesive, sealants, agriculture and
animal feed with only slightly modification in iron oxide concentrations for some industries.

[AliQaid.txt] Date time:2020-11-21

1000 100

80
750
Intensity(Counts)

Intensity(%)
60

500

40

250
20

0 0
Calcite - CaCO3

10 20 30 40 50 60 70

Figure 5. XRD analysis for Limestone from Arhab

Table 2. Average of physical and chemical analysis of limestone from Arhab

Whiteness Bulk density g/cm3 Water absorption% Void ratio pH Surface area cm2/g
87.78-90.2 2.4-2.88 0.4-2.32 0.01-0.06 8.3 - 8.6 3900-4650

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Table 3. Chemical analysis of major oxides of limestone from Arhab

Sample no. CaO SiO2 Al2O3 Fe2O3 MgO TiO2 P2O5 K2O+Na2O LOI CaCO3
1 55.00 0.70 0.20 0.13 0.50 <0.05 0.01 0.06 42.72 98.16
2 55.33 0.40 0.36 0.26 0.42 <0.05 0.17 0.12 42.86 98.75
3 55.40 0.40 0.22 0.17 0.43 <0.05 0.09 0.10 42.98 98.88
4 54.70 0.80 0.40 0.26 0.60 <0.05 0.01 0.15 42.40 97.63
5 55.50 0.20 0.21 0.13 0.41 <0.05 0.05 0.11 43.06 99.06
6 55.50 0.25 0.26 0.15 0.44 <0.05 0.18 0.14 42.95 99.06
7 55.40 0.30 0.14 0.13 0.40 <0.05 0.11 0.10 43.16 98.88
8 55.20 0.43 0.21 0.19 0.41 <0.05 0.07 0.11 42.98 98.52
9 55.32 0.39 0.23 0.17 0.43 <0.05 0.10 0.10 42.95 98.73
10 55.32 0.35 0.26 0.26 0.53 <0.05 0.02 0.13 43.00 98.73
11 55.36 0.48 0.20 0.20 0.50 <0.05 0.03 0.10 43.08 98.81
12 55.12 0.65 0.29 0.21 0.51 <0.05 0.05 0.12 42.80 98.38
13 55.26 0.48 0.31 0.23 0.55 <0.05 0.04 0.15 42.80 98.63
14 54.64 0.69 0.32 0.28 0.60 <0.05 0.01 0.10 42.60 97.52
15 55.31 0.48 0.27 0.24 0.55 <0.05 0.04 0.14 42.92 98.72

Table 4. Correlation matrix of Pearson of major oxides of limestone from Arhab

Variables CaO SiO2 Al2O3 Fe2O3 MgO P2O5 K2O+Na2O LOI
CaO 1.00
SiO2 -0.90 1.00
Al2O3 -0.55 0.51 1.00
Fe2O3 -0.52 0.46 0.79 1.00
MgO -0.73 0.75 0.61 0.70 1.00
P2O5 0.58 -0.61 -0.08 -0.29 -0.71 1.00
K2O+Na2O 0.05 -0.07 0.61 0.51 0.34 0.11 1.00
LOI 0.89 -0.85 -0.78 -0.53 -0.73 0.41 -0.21 1.00

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0.45 a 0.90 b
0.40 0.80
0.35 0.70
0.30 0.60
Al2O3 wt%

SiO2 wt%
0.50
0.25
0.40
0.20 0.30
0.15 0.20
0.10 0.10
0.05 0.00
54.00 55.00 54.00 55.00
CaO wt% CaO wt%

0.30 0.90 d
c
0.80
0.25 0.70
0.60
Fe2O3 wt%

0.20
SiO2 wt%

0.50
0.15 0.40
0.30
0.10 0.20
54.00 55.00 42.00 43.00 44.00
CaO wt% LOI wt%

43.20 e
43.10
43.00
LOI wt%

42.90
42.80
42.70
42.60
42.50
42.40
42.30
54.00 54.50 55.00 55.50
CaO wt%

Figure 6. Diagrams of selected major oxides of limestone from Arhab (a) CaO wt%% vs.
Al2O3 wt%, (b) CaO wt% vs. SiO2wt%% (c) CaO wt%%% vs. Fe2O3 wt%% (d) LIO vs. SiO2
wt%% (e) CaO wt% vs. LOI%.

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Figure 7. Chemical analyses of samples of limestone from Arhab area plotted on

Al2O3–CaO–(MgO+FeOt) ternary diagram

5. Conclusions
XRD and chemical composition results showed that the limestone from Arhab area has very high -
high purity, mainly composed of CaCO3 with ranging from 97.52 to 99.06 wt% and the harmful
oxides SiO2, Fe2O3, MgO and Na2O3 are present with low concentration. The physical test results
include whiteness, void ratio, water absorption, surface area plain and bulk density show high
properties. In addition to chemical and physical specifications, there are many advantages of limestone
from Arhab such as huge outcrop, can be mined open cast with low cost, and their position near the
plants and markets.
Field observation, geological map, and satellite image revealed that the tectonic effects are less
comparing to the same rock in other places. Based on the geochemical and physical properties, the
limestone in Arhab can be used in a wide spectrum of industrial applications including plastic, glass
made, steel, ceramic, paper, paints, animal feed, and production of lime, etc. with slightly modification
for iron oxides in rare cases.
This is a preliminary study with limitations in industrial tests used (due to its currently unavailability).
The study emphasized the interest in local limestone, which is available in economic quantities with
very high quality that meet the requirements of many industries currently based on imported
limestone. It also stressed the importance of local limestone in industrial uses rather than construction,
which is extracted randomly.

Acknowledgements
The authors are grateful to the Dr. Mohammed Al-Wosabi, Dr. Khaled El-Selwi, Prfo. Mohamed
Abdel Wahab and Mr. Faroojan Khajeek for their value comments. Appreciation also is extended to
the chairman of the Geological Survey and Mineral Resources Board, as well as Eng. Abdel Fattah,
production manager of production of Atlas Factory - Taiz, for their cooperation.

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