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2021-01 Biorefineries With CCS

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2021-01 Biorefineries With CCS

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IEAGHG Technical Report

2021-01
March 2021

Biorefineries with CCS

IEA GREENHOUSE GAS R&D PROGRAMME


International Energy Agency
The International Energy Agency (IEA), an autonomous agency, was established in November 1974. Its primary mandate was – and is – two-
fold: to promote energy security amongst its member countries through collective response to physical disruptions in oil supply, and provide
authoritative research and analysis on ways to ensure reliable, affordable and clean energy for its 30 member countries and beyond. Within
its mandate, the IEA created Technology Collaboration Programmes (TCPs) to further facilitate international collaboration on energy related
topics. To date, there are 38 TCPs who carry out a wide range of activities on energy technology and related issues.

DISCLAIMER
The GHG TCP, also known as the IEAGHG, is organised under the auspices of the International Energy Agency (IEA) but is functionally
and legally autonomous. Views, findings and publications of the IEAGHG do not necessarily represent the views or policies of the IEA
Secretariat or its individual member countries.

This report was prepared as an account of the work sponsored by IEAGHG. The views and opinions of the authors expressed herein
do not necessarily reflect those of the IEAGHG, its members, the organisations listed below, nor any employee or persons acting on
behalf of any of them. In addition, none of these make any warranty, express or implied, assumes any liability or responsibility for the
accuracy, completeness or usefulness of any information, apparatus, product of process disclosed or represents that its use would
not infringe privately owned rights, including any parties intellectual property rights. Reference herein to any commercial product,
process, service or trade name, trade mark or manufacturer does not necessarily constitute or imply any endorsement, recommendation
or any favouring of such products.
COPYRIGHT
Copyright © IEA Environmental Projects Ltd. (IEAGHG) 2021. All rights reserved.

ACKNOWLEDGEMENTS AND CITATIONS

This report describes work undertaken by VTT Technical Research Centre of Finland on behalf of IEAGHG. The principal researchers were:

• Ilkka Hannula
• Kristian Melin

To ensure the quality and technical integrity of the research undertaken by IEAGHG each study is managed by an appointed
IEAGHG manager. The report is also reviewed by a panel of independent technical experts before its release.

The IEAGHG manager for this report was: Jasmin Kemper

The expert reviewers for this report were:

• Kristin Onarheim, Aker Solutions


• Piera Patrizio, Imperial College London
• Sara Budinis, IEA
• Sara Giarola, Imperial College London

The report should be cited in literature as follows: ‘IEAGHG, “Biorefineries with CCS”, 2021-01, March 2021.’
Further information or copies of the report can be obtained by contacting IEAGHG at:

IEAGHG, Pure Offices, Cheltenham Office Park


Hatherley Lane, Cheltenham,
GLOS., GL51 6SH, UK

IEAGHG Technical Report


w w w. i e a g h g. o rg
BIOREFINERIES WITH CARBON CAPTURE AND
STORAGE (CCS)

The aim of this study is to provide a techno-economic assessment of biorefinery concepts with and
without carbon capture and storage (CCS) as well as a comparative assessment of 1st generation and
2nd generation biorefineries. The results of this study will be of interest to developers of biorefinery
and CCS projects and policy makers.

Key Messages

 The cost of adding CCS on the high-concentration streams of biorefineries varies between 22
and 24 $/tCO2. If CCS is extended also to flue gas streams, the cost of CCS varies between 27
and 66 $/tCO2. The wider range of cost is explained by differences between biorefineries in
the share of CO2 that needs to be captured from low-concentration streams.
 The lowest cost of CCS is achieved with gasification-based configurations using base case
CCS design (22 $/tCO2) followed closely by ethanol plants with base case CCS design (24-25
$/tCO2).
 Several of the cost estimates are developed for first-of-a-kind commercial plants and contain a
lot of uncertainty as they are derived from a small handful of demonstration projects. Cost
reductions could be achieved over the coming decades through learning from these
technologies at relevant scale.
 Biorefineries with CCS show potential for negative emissions. First generation corn ethanol
plants with CCS can only produce carbon negative fuels if natural gas inputs are switched to a
low-carbon energy source. For second generation biorefineries with CCS, based on woody
biomass, emissions range between -59 gCO2eq/MJ and -164 gCO2eq/MJ. The deepest
emissions reductions in comparison to the fossil reference are associated with second
generation wheat straw plants with CCS, which can achieve -274 gCO2eq/MJ in the maximum
capture configuration.
 Biorefineries with CCS seem very attractive, especially for decarbonising the hard-to-abate
transport sector. On the other hand, the cost of biofuel is currently too high to compete with
petroleum fuels and out of the examined configurations only two have currently been
demonstrated at commercial scale.
 Recommendations for further work include:
 Implementation of large-scale demonstration projects in order to reduce risk and
increase investor confidence.
 More data should be made available from projects in order to refine the techno-
economic assessment of biorefineries with CCS and reduce uncertainties.

i
Background to the Study

Negative emissions technologies (NETs) feature in many climate models that comply with 2°C
scenarios; and efforts to aim towards a 1.5°C target, as outlined in the Paris Accord, have drawn
further attention to the need for options that reduce the overall stock of emissions in the atmosphere.
Negative emissions are also an important tool for offsetting residual emissions from the hard-to-abate
sectors like aviation, cement and steel industry, as well as agriculture to achieve overall carbon-
neutrality.

A range of plausible NETs have been proposed, and some of them are currently more developed than
others, in terms of both technological maturity and the amount of CO2 removal that could potentially
be offered. As NETs are growing in prominence in energy planning, better understanding is needed of
the many trade-offs that achieving negative emissions have on cost, emissions and the required
resources.

Bioenergy with Carbon Capture and Storage (BECCS or Bio-CCS) is a NET that receives most
attention in integrated assessment model studies and in the latest IPCC reports. A key difference
between BECCS and fossil-based CCS technologies is that when CO2 produced as a by-product from
biomass processing is captured and securely stored in geological formations, the generated energy
could be characterised by negative net greenhouse gas (GHG) emissions, because of the storage of
biogenic CO2. However, the overall climate change mitigation potential of BECCS depends on a
number of factors (land use aspects, biomass procurement, performance of processing, share of CO2
capture, transportation of CO2 and the permanence of storage).

A closely related concept to BECCS is so-called Bioenergy with Carbon Capture and Utilisation
(BECCU). Here CO2 produced as a by-product from biomass processing is captured, but instead of
permanent storage, the CO2 is used as a feedstock in a way that produces value for the plant operator.
In most of these CCU applications, the CO2 is released into the atmosphere fairly quickly after its
utilisation, and therefore its climate change mitigation potential can be significantly lower than that of
CCS. However, possible displacement of fossil fuels and carbon intensity of the energy used to run
the CCU process can also play a decisive role in the overall climate impact. CCS technologies have
been used industrially over several decades for example in oil refining, and they can be considered
relatively mature.

Currently, the only large-scale BECCS process is the Illinois Industrial CCS facility that captures
annually up to 1 Mt of CO2 from the fermentation process of a Decatur corn ethanol plant and injects
it into a geological storage beneath the facility. The remaining four BECCS facilities operating today
are small-scale ethanol production plants that use most of the captured CO2 for enhanced oil recovery
(EOR).

Modern bioenergy plays an essential role in the International Energy Agency (IEA) 2°C Scenario
(2DS) providing nearly 17% of final energy demand in 2060 compared to 4.5% in 2015. Bioenergy is
important especially in sectors for which other decarbonisation options are not available.

Technologies for producing so called “first generation” crop-based biofuels like ethanol from sugar
and starch-based feedstocks, and FAME (fatty acid methyl ester) biodiesel from vegetable oils and
other lipid feedstocks (including wastes and by-products) are well-established, and provide most of
today’s transport biofuels.

In recent years, technology to produce HVO (hydrotreated vegetable oil), also known as renewable
diesel (including advanced biodiesel, naphtha and aviation fuels), has been successfully
commercialised. About 5 Mt/yr of HVO was produced globally in 2017 and production is expected to
increase to 6-7 Mt/yr by 2020 and continue to increase thereafter. HVO production is increasingly
based on waste and residue oil and animal fat feedstocks rather than oil crops. HVO has advantageous

ii
fuel characteristics compared to FAME, and can be used to produce so-called drop-in fuels, i.e. fuels
that can be used unblended in the existing vehicle fleet or distribution infrastructure.

The longer-term growth of transport biofuels in the IEA’s 2DS relies on the widespread supply of
novel advanced biofuels produced by processes that are generally not yet mature. Advanced biofuels
are sustainable fuels produced from non-food crop feedstocks that are capable of delivering
significant life-cycle GHG emissions savings without competing with food and feed crops for
agricultural land use. Advanced biofuels can also be called “second generation” (2G) biofuels, to
differentiate them from first generation crop-based biofuels.

The development and commercialisation of advanced biofuel technologies has been slow, however,
and most commercial-scale projects are currently on hold due to the high investment cost of pioneer
process plants combined with the lack of funding instruments that share the risk of scale-up.

The sustainable conversion of biomass feedstocks to biomass-derived fuels and chemicals are often
referred to as “biorefining”. In addition to biofuel, such “biorefineries” typically produce also by-
products and CO2 (see Figure 1). The CO2 from biomass processing is normally vented to atmosphere,
but if it were captured and securely sequestered in geological formations, the produced biofuel could
be characterised by net negative GHG emissions because of the storage of biogenic CO2.

Figure 1: Conceptual representation of a biorefinery coupled with CCS.

Scope of Work

IEAGHG commissioned VTT Technical Research Centre of Finland to carry out a techno-economic
assessment of different biorefinery concepts with and without CCS.

The scope of work comprises the following tasks:

1. A techno-economic assessment of 2nd generation biorefineries with and without CCS for a
select number of different feedstocks;
2. An estimation of the potential for negative emissions of such biorefinery with CCS concepts;
and
3. A comparison of a 2nd generation bioethanol plant with and without CCS to 1st generation
bioethanol plant with and without CCS.

iii
Findings of the Study

Methods and approach


Several technological pathways are available for converting lignocellulosic feedstocks to biofuels (see
Figure 2). Gasification represents a thermochemical processing route where the feedstock is first
converted to gas at elevated temperatures (800 – 1,200°C) and in the presence of an oxidising agent
(air, oxygen and/or steam). The gas is then cleaned and conditioned, and catalytically converted either
to hydrocarbon fuels (e.g. Fischer-Tropsch diesel or methane) or to fuel alcohol (e.g. methanol).
Alternatively, pure hydrogen can be produced by separation from synthesis gas using pressure swing
adsorption (PSA).

Figure 2. Schematic of possible processing pathways to second generation biofuels from lignocellulosic
biomass.

Another main thermochemical option is the direct liquefaction of biomass into bio-oil, using e.g. fast
pyrolysis process where solid biomass is heated up rapidly at around 500°C and the formed product is
recovered as bio-oil by condensation. The production of bio-oil for use in transport applications (such
as diesel and/or petrol/gasoline) requires significant upgrading by hydrogenation.

The main biochemical pathway involves the hydrolysis of biomass into sugars, followed
by fermentation into bioethanol. The bioethanol is separated from the fermented solution by
distillation. In addition, a lignin-rich by-product is obtained from the process.

Reference plants
The prospective cost and performance of advanced biofuels have been extensively investigated in
a series of “scoping studies”. However, results from these past studies are heterogeneous, and a
wide range of values has been proposed. In addition, scoping studies typically evaluate costs at some
future date based on the assumption of mature technology. Such Nth-of-a-kind (NOAK) cost
estimates are valuable for outlining the prospective long-term cost potential of biofuels, but are
less useful in assessing costs of first-of-a-kind (FOAK) plants, as conventional cost estimation
methods are found to routinely understate the costs of pioneering FOAK technologies.

iv
In recent years, however, a small amount of actual data on demonstration projects has surfaced,
allowing indicative cost and performance estimates to be derived for different emerging biofuel
technologies from empirical evidence. The following projects have been used to derive the reference
cases for this study:
 ADM corn ethanol plant, Decatur, Illinois, USA
 Inbicon demonstration plant, Kalundborg, Denmark,
 Fortum pyrolysis plant, Joensuu, Finland
 GoBiGas gasification plant, Gothenburg, Sweden

Performance analysis
The study analyses and compares the performance of different biorefinery configurations based on
mass and energy flows simulated with Aspen Plus®. Following helpful metrics are calculated to assist
the investigation. Fuel yield:

(1)
where ṁbiof is output massflow of biofuel (kg/s), Hbiof is lower heating value of biofuel (MJ/s), Hpetrol is
lower heating value of petrol (MJ/l), ṁbiom is input massflow of dry biomass (kg/tonne) and 159 stands
viii
for litres per barrel; and CO2 capture yield:

, (2)
where ṁCO2 is massflow of captured CO2.

GHG emissions analysis


Total emission from biofuel production are defined as a sum of upstream emissions (Eupstream) caused
by feedstock harvesting and transport, and nitrogen fertilisation to replace nutrients removed within
the feedstock; and process emissions (Eprocess) caused by the possible use of fossil fuels during
processing. Eupstream values are taken from the literature and Eprocess values are based on our process
simulation results. Emissions caused by manufacturing of the biofuel plants or other needed
infrastructure are excluded from the calculation. We also exclude emissions from producing the
catalyst needed in some configurations as they are found to represent less than a 0.1 % of total
emissions and thus have insignificant contribution to the overall results.

Table 1. Emission calculation parameters.


FOSSIL FUEL CARBON INTENSITIES, GCO2EQ/MJ
Natural gas 65.9
ERROR! BOOKMARK NOT
Fossil petrol/diesel 94
DEFINED.ERROR! BOOKMARK NOT DEFINED.

Fossil hydrogenERROR! BOOKMARK NOT DEFINED.* 93


DIRECT UPSTREAM EMISSIONS, GCO2EQ/MJ
Corn ethanol*** 25.5
Wheat ethanol 1.8
Delivered waste wood** 2.4
*calculated from natural gas emissions by dividing with thermal efficiency
of steam reforming of 71 % (lhv).
**upstream emissions for the delivered waste wood are converted to
upstream biofuel emissions by dividing with thermal efficiency of biomass
to biofuel (lhv).
***values from RED II (Edwards et al. 2019); values for wheat and wood
are lower due to being 2G residue feedstocks.

v
The functional unit under study is one megajoule (MJ) of biofuel produced, and emissions are
expressed as gCO2eq/MJ. All emissions are allocated to the main biofuel product, and electricity used
by some configurations is assumed to be procured from zero-carbon sources. CO2 emissions relative
to the fossil fuel comparator are calculated using the following equation:

(3)

where Efos is emissions from fossil fuel comparator. Fossil fuel carbon intensities and upstream
emissions used in the calculations are summarised in Table 1.
Cost analysis
The prospective costs of advanced biofuels have been investigated extensively in a series of scoping
studies. However, results from past studies are heterogeneous and a wide range of values have been
proposed. In recent years, however, a small amount of actual data on demonstration projects has
surfaced, allowing indicative cost and performance estimates to be derived for emerging biofuel
technologies from empirical evidence. Here, publicly available information from reference and
demonstration biofuel plants (see Table 2) are used to develop total capital investment (TCI) estimates
individually for each configuration examined. Exchange rates and Chemical Engineer magazine’s
Plant Cost Index (CEPCI) are used to escalate all demonstration plant costs to 2018 US dollars.

Table 2: Reference plant cost data.


REFERENCE PLANT CORN CELLULOSIC PYROLYSIS SYNTHETIC
TYPE ETOH ETOH OIL BIOFUELS
Reference plant name ADM Inbicon Fortum Joensuu GoBiGas
Decatur Demo plant pyrolysis plant
Location Illinois, Kalundborg, Joensuu, Finland Gothenburg,
USA Denmark Sweden
Biomass input, MW 371.8 16 50 30
Biofuel output, MW 278.5 4.6 30 20
Commissioning year 2011 2010 2012 2014
Total capital 127 M$ 180 M$* 27 M€ 1375 MSEK
investment
Adjusted TCI (m$2018) 131 216 36 210
*) Newer estimate to give more accurate estimate for near future 2G ethanol plants according to e4Tech

To minimise distortion caused by scale benefits in the cost results, the same biofuel output should be
used for all plants. However, as existing corn-based biofuel plants are much bigger than existing
cellulosic biofuel plants, a choice was made to set the scale of corn fed plants to 5,000 bblpe/d (petrol
equivalent barrels per day), and set the scale of lignocellulosic feedstock plants to 1,000 bblpe/d.

A cost-scaling exponent (k) was used to scale reference plant capital costs (C0) to a commercial scale
capacity (S) using the following relation:

(4)
where S0 is the scale of the reference plant and C the TCI of a FOAK plant at commercial scale.

The choice of capital investment scaling function and scaling parameter has a significant impact on
the estimated process economics. If the selected scaling exponent is small, it suggests that the
optimum plant size is very large and vice versa. An average value of 0.67 is used for k in this work.
Previous research indicates that the investment for biomass-based plants, especially for the

vi
biochemical route, could scale with higher values than this, but some ambiguity still remains
regarding capital investment scaling exponent for biorefineries.

For a summary of financial parameters, see Table 3.

Table 3: Financial parameters used in the work.


Weighted avg. cost of capital (WACC) 8 %
Economic lifetime 20 years
Capital charge rate (CCR) 0.10 -
Annual operating and maintenance 4 % of TCI
Annual runtime 8,000 h/yr
333 days/yr
Corn price 150 $/tonne
Biomass price 60 $/tonne
Electricity price 50 $/MWh
Natural gas price 30 $/MWh
Value of DDGS as animal feed 75 $/tonne
CO2 transport and injection/storage costs 15 $/tCO2

LCOF (levelised cost of fuel) production is evaluated according to the following equation:

(5)
where
 F is the annual cost of biomass feedstock,
 E is the annual cost of electricity,
 C is the annualised capital charge, including return on equity and interest on debt,
 O is the annual operating and maintenance costs, and
 R is the annual revenue from selling by-product fuel gas.

The sum of these annual costs ($/yr) is divided by P, which is the annual output of fuel (GJ/yr) from
the plants. When defined in this way, LCOF ($/GJ) indicates the product sale price needed to break-
even under the technical and economic parameters assumed.

Summary of process configurations


Five different biofuel technologies are examined in detail, representing different approaches,
feedstocks, end-products and technological maturities, namely:
 1st generation ethanol via fermentation of corn,
 2nd generation ethanol via biochemical conversion of wheat straw,
 bio-oil via thermal fast pyrolysis of forest residues,
 Fisher-Tropsch liquids (FTL) via thermal gasification of forest residues, and
 hydrogen via thermal gasification of forest residues.

Each basic configuration is investigated with and without carbon capture and storage (CCS). Two
different CCS approaches are considered for plants that have more than one stream that contains CO 2.
The base case approach is to capture carbon only from high CO2 concentration streams, while an
alternative configuration CCS-MAX is developed for maximal CO2 capture (including also low
concentration streams). Combination of these designs results in thirteen configurations (see Table 4),

vii
each characterised by distinctive plant designs. These configurations are identified by acronyms that
identify both the biofuel production approach and the treatment of CO2:
 ETOH = Ethanol from corn,
 CE = Ethanol from lignocellulosic biomass,
 PO = Pyrolysis oil from lignocellulosic biomass,
 FTL = Fischer-Tropsch liquids from lignocellulosic biomass,
 H2 = Hydrogen from lignocellulosic biomass;
 V = Vent of biogenic-CO2 to atmosphere,
 CCS = Capture and underground storage of carbon from high concentration CO2 streams,
 CCS-MAX = Capture and underground storage of carbon from all streams that contain CO2.
Following capture efficiencies are assumed for different capture processes, depending on the CO2:
 100% direct capture of CO2 from fermentation by drying;
 97% capture of CO2 (and 100% co-capture of H2S) from synthesis gas by scrubbing with
chilled methanol;
 90% capture of CO2 from flue gas by scrubbing with amine solution (30% MEA).
Three different feedstocks are considered in this work:
 Corn for ETOH-V and ETOH-CCS,
 Wheat straw for CE-V, CE-CCS and CE-CCS-MAX, and
 Forest residues for FTL-V, FTL-CCS, FTL-CCS-MAX, H2-V, H2-CCS and H2-CCS-MAX.

All examined plant configurations are designed to be self-sufficient in terms of heat and steam (by
recovering heat from hot process streams), while electricity is balanced from the grid. Process models
are developed using Aspen Plus® process simulation software and used as a tool for carrying out
performance analyses.

Table 4: Summary of examined process configurations.


CASE FEEDSTOCK CONVERSION END CO2 CAPTURE
TECHNOLOGY PRODUCT TECHNOLOGY
ETOH-V Corn Fermentation Fuel ethanol -
ETOH-CCS Corn Fermentation Fuel ethanol Chemical absorption
CE-V Lignocell. residues Biochemical conversion Fuel ethanol -
CE-CCS Lignocell. residues Biochemical conversion Fuel ethanol Drying

CE-CCS- Lignocell. residues Biochemical conversion Fuel ethanol Drying and chemical
MAX absorption
PO-V Lignocell. residues Fast pyrolysis (+ HDO) Bio-oil -
PO-CCS Lignocell. residues Fast pyrolysis (+ HDO) Bio-oil Chemical absorption
FTL-V Lignocell. residues Fluidised-bed gasification FT-liquids -
FTL-CCS Lignocell. residues Fluidised-bed gasification FT-liquids Chemical absorption
FTL-CCS- Lignocell. residues Fluidised-bed gasification FT-liquids Physical and
MAX chemical absorption
H2-V Lignocell. residues Fluidised-bed gasification Hydrogen -
H2-CCS Lignocell. residues Fluidised-bed gasification Hydrogen Physical absorption
H2-CCS- Lignocell. residues Fluidised-bed gasification Hydrogen Physical and
MAX chemical absorption

viii
Process emissions
Mass and energy flows were simulated with Aspen Plus® for plants that produced either 5,000 bblpe/d
(from corn) or 1,000 bblpe/d (from lignocellulosic feedstocks) of biofuel. The carbon flows are
summarised in Table 5, together with calculated results for the upstream, conversion and total biofuel
emissions (gCO2eq/MJ) and R. The H2-CCS configuration captures the highest share of input carbon
to a concentrated stream of CO2 (97% and 90%), followed by CE-CCS-MAX (74%), FTLs (66% and
54%), PO-CCS (36%), ETOH-CCS (21%) and finally CE-CCS (10%).

Relative emissions (R) from the plants are negative for almost all examined configurations featuring
CCS due to the storage of the biogenic-CO2. ETOH-CCS is an exception due to the high upstream
emission, the use of natural gas as an energy source, and to the small share of CO2 being captured.

Table 5: Carbon distributions and biofuel emissions. R is relative biofuel emissions in comparison to the
fossil fuel reference. This study uses 94 gCO2/MJ for petroleum-derived diesel/petrol and 93 gCO2/MJ for
fossil hydrogen produced via steam reforming of natural gas.
OF FEEDSTOCK
CARBON THAT ENDS
UP
Direct Direct
Total direct
stored upstream process
vented in fuel emissions R
as CO2 emissions emissions
gCO2/MJ
gCO2/MJ gCO2/MJ
ETOH-V 0.0 41.9 0.0 25.5 26 51 54 %
ETOH-CCS 0.0 41.9 21.0 25.5 -10 16 16 %
CE-V 81.0 19.0 0.0 1.8 0 2 2%
CE-CCS 71.0 19.0 10.0 1.8 -37 -36 -38 %
CE-CCS- 7.1 19.0 73.9 1.8 -276 -274 -291 %
MAX
PO-V 40.0 60.0 0.0 4.2 0 4 4%
PO-CCS 4.0 60.0 36.0 4.2 -63 -59 -63 %
FTL-V 69.4 30.6 0.0 5.4 0 5 6%
FTL-CCS 15.5 30.6 53.9 5.4 -122 -117 -124 %
FTL-CCS- 3.1 30.6 66.4 5.4 -151 -145 -154 %
MAX
H2-V 100.0 0.0 0.0 4.1 0 4 4%
H2-CCS 10.1 0.0 89.9 4.1 -156 -152 -163 %
H2-CCS- 3.5 0.0 96.5 4.1 -168 -164 -175 %
MAX

Wheat ethanol with maximal CO2 capture is the most carbon negative product having emissions of -
291% relative to fossil petrol. This is caused by both the large share of CO2 being captured and the
relatively low conversion efficiency to ethanol. CE-CCS-MAX is followed by hydrogen plants having
emissions ranging from -175% to -163% relative to fossil hydrogen, followed by FT liquids from
154% to 124%, thermal bio-oil (-63%) and 2G ethanol with base case CO2 capture design (-38%).

Natural gas is one of the main process utilities used in corn based ethanol plant and replacing it with a
low-carbon alternative such as biogas, electricity etc. would lower the total biofuel emissions for
ETOH-V from 51 to 26 gCO2/MJ and for ETOH-CCS from 16 to -10 gCO2/MJ. In the latter case, the
switch from natural gas to a non-fossil energy source together with CCS would therefore negate direct
upstream emissions for the corn ethanol plant, making it a negative emissions technology.

ix
Between 1,881 and 1,753 kg of CO2 is captured for every tonne of biomass (dry) by H2
configurations featuring CCS. This is followed by FT-liquids with capture rate from 1,294 to 1,052
kgCO2/tbiom, CE-ETOH with capture rate from 1,240 to 168 kgCO2/tbiom, thermal bio-oil with 702
kgCO2/tbiom capture rate and 1G ethanol with 342 kgCO2/tbiom.

Ethanol configurations that feature base case CCS designs have the smallest CO2 capture rates as most
of the biomass carbon will end up in the by-products, either distiller’s dried grain solids (from corn)
or combustion feedstock (from lignocellulosic biomass). When CO2 from the by-product biomass is
also captured (CE-CCS-MAX), a substantial increase in capture rate is achieved. For thermochemical
configurations, base case CCS designs already capture most of the available CO2 from the process and
maximal capture designs contribute only a small addition to the total capture. Highest capture rates
are achieved with hydrogen configurations as all carbon from the process is in the form of CO 2 and
therefore available for capture.

Process economics
Finally, the contribution of different cost categories on the total cost of fuel ($/GJ LHV) and the cost of
CCS ($/tCO2) are presented in Table 6. Cost of carbon capture and sequestration ranges from 22 to 66
$/tCO2 depending on the examined configuration. Lowest costs are associated with ethanol and
gasification-based plants that feature CO2 separation already in the base (vent) configuration and the
cost of adding CCS is only 22 – 25 $/tCO2. A clear jump in cost can be seen for plants that
incorporate post-combustion capture design, being 66 $/tCO2 for pyrolysis where all CO2 is captured
from flue gas, and 50 $/tCO2 for CE-CCS-MAX, where part of the CO2 is captured at a lower cost
from fermentation. For the CCS-MAX configurations, the costs increase more moderately for
gasification-based configurations where only a small part of the overall CO2 is captured from flue gas.

x
Table 6: Cost comparison of examined process configurations. Results are given as $/GJLHV, if not
otherwise noted.

ELECTRICITY

COST OF CCS
TOTAL ($/GJ)
DISPOSAL
CONFIG. CAPITAL

($/TCO2)
STOCK

DDGS
FEED
O&M

CO2
NG
ETOH-V 1.6 0.6 15.6 3.2 -2.6 0.5 19.0
ETOH-CCS 1.7 0.7 15.6 3.2 -2.6 0.5 0.7 19.8 24
CE-V 15.1 5.9 13.3 -7.0 27.5
CE-CCS 15.3 6.0 13.3 0.6 -6.8 28.4 25
CE-CCS-
20.1 7.9 4.1 -5.0
MAX 13.3 40.4 47
PO-V 3.4 1.3 5.4 -1.1 9.0
PO-CCS 5.4 2.1 5.4 0.9 -0.6 13.2 66
FTL-V 26.0 10.2 7.0 -0.8 42.3
FTL-CCS 26.2 10.3 7.0 1.8 -0.2 45.0 22
FTL-CCS-
27.3 10.7 2.3 0.0
MAX 7.0 47.2 33
H2-V 26.0 10.2 5.4 0.8 42.3
H2-CCS 26.2 10.3 5.4 2.3 1.6 45.8 22
H2-CCS-
26.8 10.5 2.5 1.7
MAX 5.4 46.9 27

The main cost results (the levelised cost of fuel and the cost of CCS) are also visualised in Figure 3
for all examined plant configurations.

Figure 3: Levelised cost of fuels (dollars per petrol equivalent litres of biofuel) and cost of CCS (US
dollars per tonne of sequestered CO2) for all examined plant configurations.

The levelised cost of biofuel ranges from 0.3 to 1.5 dollars per petrol equivalent litre being lowest for
thermal bio-oil from pyrolysis and second lowest for corn ethanol. The low LCOF of pyrolysis plants
is mainly due to the general low investment, operating and feedstock costs of these plants. A clear
jump in costs can be seen when transitioning to other technologies. LCOF for wheat ethanol is
between 0.9 and 1.3 $/lpe (dollars per petrol equivalent litres) depending on the CCS design whereas
gasification based configuration has biofuel cost between 1.4 and 1.5 $/lpe.

xi
Sensitivity analysis
We then investigate the impact of plant scale on process economics. Chemical process technologies
are usually expected to benefit from a large scale, as doubling the plant output less than doubles the
capital investment cost. Biomass-based technologies are, however, limited in their scale by the
availability of biomass, which is a geographically dispersed resource that cannot usually be
economically transported more than 100 km. In Figure 4, the impact of plant scale on the cost of CCS
and levelised cost of fuel is examined for plants that process woody biomass (corn ethanol plants were
excluded from this analysis as they are operating at a much larger scales).

Figure 4: Impact of plant scale on the cost of CCS and on the levelised cost of biofuel.

According to the results, the plant size has modest impact on the cost of CCS for plants that
incorporate capture from fermentation and from synthesis gas, as the costs are associated only for the
compression and are therefore relatively low. For plants where most of the CO2 is captured from flue
gases by scrubbing with amine, the size of the plant has higher impact on costs. For example, for
pyrolysis plants the cost of CCS reduces from 78 $/tCO2 to 58 $/tCO2 when the scale of plant
increases from 500 to 2,000 bbl/d. The plant scale has a much more pronounced impact on the
levelised cost of fuel. For example, for gasification based configurations the cost of biofuel reduces
from about 1.8 $/lpe to 1.3 $/lpe when plant scale increase from 500 to 2,000 bbl/d level.

In Figure 5, the impact of feedstock cost on the biofuel production cost is shown. Here the corn
ethanol configurations are also excluded from the comparison as they are governed by different
feedstocks characteristics (both in terms for cost and availability) than plants operating on
lignocellulosic feedstocks.

xii
Figure 1. Impact of cellulosic biomass cost on the levelised cost of fuel.

Based on the results, the feedstock cost has lowest impact on the biofuel production cost for the
gasification-based configurations, and highest for the PO-CCS and CE-CCS configurations. This is
probably explained by the higher share of CapEx in the cost of gasification-based plants. For example,
an increase in the cost of biomass feedstock from 30 to 90 $/tonne increases the biofuel production
cost by 61% (from 0.7 to 1.1 $/lpe) for the CE-CCS plant, but only by 12% (1.4 – 1.6 $/lpe) for the
H2-CCS-MAX.

Expert Review Comments

Four reviewers from industry, academia and IGOs provided comments on the draft report. The
majority of the comments have been addressed by the contractor, including but not limited to:
 Restructuring of the report to allow better flow of reading and improve clarity (e.g.
underlying modelling assumptions have mainly been moved to an annex)
 Addition of an executive summary upfront in the report
 Addition of further references and contextualisation
 Addition of new illustrations and tables to better support the discussion
 Discussion of pulp mills has been shortened to only present information relevant to the report
 Removal/correction of inconsistencies

Conclusions

Five different biorefinery technologies have been examined and compared, representing different
technological approaches, feedstocks, end-products and commercial maturities. The base case capture
designs in this study capture CO2 only from high-concentration streams, while MAX designs feature
additional capture from low-concentration streams, i.e. flue gases.

The cost of adding CCS on the high-concentration streams of biorefineries varies between 22 and 24
$/tCO2. If CCS is extended also to flue gas streams, the cost of CCS varies between 27 and 66 $/tCO2.
The wider range of cost is explained by differences between biorefineries in the share of CO2 that
needs to be captured from low-concentration streams. The lowest cost of CCS is achieved with

xiii
gasification-based configurations using base case CCS design (22 $/tCO2) followed closely by ethanol
plants with base case CCS design (24-25 $/tCO2). However, up to ten times more CO2 (1,052 – 1,753
kgCO2/tbiom) is captured from the same amount of biomass by gasification configurations than by base
case ethanol configurations (168 – 342 kgCO2/tbiom). Only when the by-product lignin is fully
combusted and captured (CE-CCS-MAX) can similar capture rates be achieved for the biochemical
plants. However, this will significantly increase the cost of CCS to 47 $/tCO2.

Due to the capture and sequestration of biogenic CO2, biorefineries show potential for negative
emissions. The corn ethanol design ETOH-CCS is a notable exception to this rule, due to high
upstream emissions of corn and the use of natural gas as additional energy source in the process.
However, if natural gas would be switched to a low-carbon energy source, corn ethanol plants with
CCS would also produce carbon negative fuels. For biorefineries based on lignocellulosic biomass,
emissions range between -36 gCO2eq/MJ and -274 gCO2eq/MJ. The deepest emissions reductions in
comparison to fossil petrol are associated with CE-CCS-MAX, as it combines a large capture rate
with relatively small biofuel output, therefore leading to highly negative emissions per MJ of biofuel
produced.

On paper, biorefineries with CCS seem very attractive. They would contribute to decarbonising the
hard-to-abate transport sector, provide much-needed negative emissions at scale, and the cost of CCS
would be only a fraction of that when applied to traditional power plants. On the other hand, the cost
of biofuel is currently too high to compete with petroleum fuels, the location of a geological storage
formation does not always coincide with good availability of biomass, and out of the examined
configurations only ETOH-V and ETOH-CCS have been currently demonstrated at commercial scale.
However, responding to the Paris Agreement will ultimately require deploying negative emissions at
scale.

Recommendations

Based on the results and conclusions of this study it is suggested that future work should focus on:

 Implementation of large-scale demonstration projects in order to reduce risk and increase


investor confidence
 More data should be made available from projects in order to refine the techno-economic
assessment of biorefineries with CCS and reduce uncertainties

xiv
Biorefineries with CCS

Report for IEAGHG


September 2020

Ilkka Hannula and Kristian Melin


VTT Technical Research Centre of Finland
Contents
Executive summary............................................................................................................................................ 3
1 Background ................................................................................................................................................ 4
2 Introduction ............................................................................................................................................... 7
3 Materials and methods ........................................................................................................................... 11
3.1 Reference plants .............................................................................................................................. 12
3.1.1 ADM Decatur, Illinois, USA ................................................................................................. 12
3.1.2 Inbicon demonstration plant ................................................................................................ 12
3.1.3 Fortum Joensuu pyrolysis plant .......................................................................................... 13
3.1.4 GoBiGas gasification plant .................................................................................................. 13
3.2 Performance analysis ...................................................................................................................... 13
3.3 GHG emissions analysis ................................................................................................................... 14
3.4 Cost analysis .................................................................................................................................... 15
4 Process configurations............................................................................................................................. 17
4.1 Ethanol from corn (ETOH) ............................................................................................................... 19
4.2 Ethanol from lignocellulosic biomass (CE) ....................................................................................... 19
4.3 Pyrolysis oil from lignocellulosic biomass (PO) ............................................................................... 21
4.4 Fischer-Tropsch liquids from lignocellulosic biomass (FTL) ............................................................. 22
4.5 Hydrogen from lignocellulosic biomass (H2) ................................................................................... 24
5 Results ..................................................................................................................................................... 26
5.1 Mass and energy flows .................................................................................................................... 26
5.2 Process economics .......................................................................................................................... 33
5.3 Sensitivity to plant scale .................................................................................................................. 36
6 Discussion and recommendations........................................................................................................... 37
Annex I: Summary or process design parameters and feedstock properties ................................................ 39
Annex II: Block diagrams for examined process configurations with simulated stream data ....................... 43
Executive summary
We investigate the techno-economic feasibility of providing negative emissions from “biorefineries”,
i.e. from processes that convert solid biomass feedstocks into gaseous or liquid biofuels. Some CO2
is formed as a by-product of biofuel production, and it is normally vented to atmosphere. However,
if it were captured and securely sequestered in geological formations, the produced biofuel could be
characterised by net negative greenhouse gas emissions because of the storage of biogenic CO2.
Four different biorefinery technologies (corn ethanol, cellulosic ethanol, biomass fast pyrolysis and
biomass gasification) are examined and compared against each other in terms of performance,
emissions and costs. These technologies were chosen on the basis of adequate maturity, i.e. each
technology has been demonstrated at multi-megawatt scale, and sufficient amount of information is
publicly available from these projects allowing to derive performance and cost estimates at
commercial-scale. Three of the chosen technologies are considered “advanced” i.e. they use non-
edible lignocellulosic feedstocks, while the production of ethanol from corn was chosen as a
reference case as it is widely applied today in the US and as there already exists CCS (carbon
capture and storage) experience from a large-scale ADM Decantur plant located in Illinois.
Concerning end-products, following alternatives were included in the analysis: fuel ethanol, pyrolysis
oil, Fischer-Tropsch fuels and hydrogen. Together they span a wide variety of different biofuel
options with different characteristics and end-use sectors. To remove differences caused by varying
heating values (e.g. 27 MJ/kg for fuel ethanol, 120 MJ/kg for hydrogen), all results are reported on a
petrol equivalent (43 MJ/kg) basis.
Some biorefinery concepts, like those involving fermentation, feature high-concentration CO2
streams that could be captured and prepared for transport at a low cost. Some concepts feature both
high and low-concentration CO2 streams, and therefore pursuing more extensive capture also
increases the total cost of CCS. Our base case CCS designs capture CO2 only from these “low-
hanging” high-concentration streams, while CCS-MAX designs are developed to capture carbon
from all available CO2-containing streams.
The lowest cost of CCS was achieved with gasification-based biorefineries featuring base case CCS
design (22 $/tCO2), followed closely by ethanol plants (both corn and cellulosic) with base case CCS
design (24-25 $/tCO2). However, from three to up to ten times more CO2 (1052-1753 kgCO2/tbiom) is
captured from the same amount of biomass by gasification-based biorefineries than by comparable
ethanol plants (168-342 kgCO2/tbiom). Only when the by-product lignin is fully combusted and
captured (CE-CCS-MAX), can similar capture rates be achieved for the cellulosic ethanol plant.
However, this will increase the total cost of CCS to 47 $/tCO2.
Due to the capture and sequestration of biogenic CO2, biorefineries show deeply negative emissions.
The corn ethanol plant with a base case CCS design is a notable exception to this rule due to high
upstream emissions of corn and the use of natural gas as additional energy source in the process.
However, if natural gas would be switched to a low-carbon energy source, corn ethanol plants with
CCS would also produce carbon negative fuels. For biorefineries based on woody biomass,
emissions range between -36 gCO2eq/MJ and -274 gCO2eq/MJ. The deepest emissions reductions in
comparison to fossil petrol are associated with cellulosic ethanol plant featuring a CCS-MAX design
as it combines a large capture rate with relatively small biofuel output, therefore leading to highly
negative emissions per megajoule of biofuel produced.
Gasification-based biorefineries seem to be striking the best balance in terms of cost (22 $/tCO2),
CO2 capture rate (1052 kgCO2/tbiomass) and biofuel yield (268 litres/tbiomass). Unfortunately,
gasification-based biorefineries are also associated with the highest levelised cost of biofuel
(1.4 $/litre). However, any attempt to estimate the realistic cost of advanced biofuels is inevitably
limited by the small handful of actual projects, and so, more operational plants will be needed to
reduce uncertainties. Our cost estimates are also developed for first-of-a-kind commercial-scale
plants and significant cost reductions could be achieved over the coming decades through learning
from these technologies at relevant scale.

Table 1. Summary of abbreviations used in the work.

IPCC = Intergovernmental Panel on Climate Change


NET = Negative Emissions Technology
GHG = Greenhouse Gas
CCS = Carbon capture and storage
BECCS = Bioenergy with Carbon Capture and Storage
BECCU = Bioenergy with Carbon Capture and Utilisation
ETS = Emissions Trading System
RED2 = EU directive (2018 recast) on the promotion of the use of energy from renewable sources
RD&D = Research, Development and Demonstration
HVO = Hydrotreated Vegetable Oils
RD&D = Research, Development & Demonstration
2G = Second generation biofuel
TRL = Technical Readiness Level
FT = Fischer-Tropsch
PSA = Pressure Swing Adsorption

1 Background
In the latest Special report on the impacts of global warming of 1.5°C the Intergovernmental Panel
on Climate Change (IPCC) highlights the urgent need to reduce the atmospheric CO2 emissions.1
The report also identifies the importance of negative emissions, i.e. removing CO 2 already emitted
to the atmosphere, in order to limit the rise in global surface temperatures and to reach the emissions
reduction targets of the Paris Agreement.
Negative emissions technologies (NETs) feature in many climate models that comply with 2°C
scenarios;2 and efforts to aim towards a 1.5°C target as outlined in the Paris Accord, have drawn
further attention to the need for options that reduce the overall stock of emissions in the atmosphere.
Negative emissions are also an important tool for offsetting residual emissions from the hard-to-
abate sectors like aviation, cement and steel industry, as well as agriculture to achieve overall
carbon-neutrality.
Some authors have voiced their concern that emissions reduction strategies that place extensive
emphasis on NETs contain significant risks. Relying too much on negative emissions technologies
to meet emission targets may create a moral hazard problem, i.e., “why should we go through the
effort to reduce emissions now when we can deal with the problem later just by using NETs”?3
However, given the current trajectory of emissions and the remaining carbon budget, it is becoming
increasingly clear that NETs are not a substitute to defossilisation measures, but instead both
approaches need to be aggressively pursued. However, to satisfy the growing demands for food,

1
Summary for Policymakers. In: Global Warming of 1.5°C. An IPCC Special Report on the impacts of global warming of
1.5°C above pre-industrial levels and related global greenhouse gas emission pathways, in the context of strengthening
the global response to the threat of climate change, sustainable development, and efforts to eradicate poverty (IPCC,
2018)
2
Smith, P., Davis, S., Creutzig, F. et al. Biophysical and economic limits to negative CO2 emissions. Nature Clim Change
6, 42–50 (2016). https://doi.org/10.1038/nclimate2870
3
Anderson K. and Peters, G. The trouble with negative emissions. Science 354(6309), 182–183 (2016).
wood products, energy, climate mitigation and biodiversity conservation — all of which compete for
increasingly limited quantities of biomass and land — the deployment of mitigation strategies must
be driven by sustainable and integrated land management.4
A range of plausible negative emissions technologies have been proposed, spanning from dedicated
processes (capture of CO2 from bioenergy conversion, mineral carbonation) to land management
(afforestation/reforestation, soil organic carbon sequestration and biochar) and further to different
geoengineering solutions (ocean fertilisation, cloud treatment). Some NETs are currently more
developed than others, in terms of both technological maturity and the amount of carbon dioxide
removal that could potentially be offered. As NETs are growing in prominence in energy planning,
better understanding is needed of the many trade-offs that achieving negative emissions have on
cost, emissions and the required resources.5

Figure 1. Two scenarios for the by-product CO2 formed during biomass processing. In the base case
(BEVENT) scenario, by-product CO2 is vented to atmosphere. In the BECCS scenario, CO2 is
captured and safely sequestered to geological formations.

Bioenergy with Carbon Capture and Storage (BECCS or Bio-CCS) is a NET that receives most
attention in integrated assessment model studies and in the latest IPCC reports.6 A key difference
between BECCS and fossil-based CCS technologies is that when by-product CO2 from biomass
processing is captured and securely stored in geological formations, the generated energy could be
characterised by negative net greenhouse gas (GHG) emissions, because of the storage of biogenic
CO2 (see Error! Reference source not found. for illustration).7,8 However, the overall climate
change mitigation potential of BECCS depends on a number of factors, spanning from land use
aspects and biomass procurement to performance of processing, share of carbon capture,

4
Canadell, J., Schulze, E. Global potential of biospheric carbon management for climate mitigation. Nat Commun 5, 5282
(2014). DOI:10.1038/ncomms6282
5
van Vuuren, D.P., Hof, A.F., van Sluisveld, M.A.E, and Riahi, K. Open discussion of negative emissions is urgently needed.
Nature Energy 2, 902-904 (2017).
6
Torvanger, A. Governance of bioenergy with carbon capture and storage (BECCS): accounting, rewarding, and the Paris
agreement. Climate Policy 19 (2018). DOI:10.1080/14693062.2018.1509044.
7
Sanchez, D.L. and Kammen, D.M. A commercialization strategy for carbon-negative energy. Nature Energy 1, 15002
(2016).
8
Liu, G., Larson, E.D., Williams, R.H., Kreutz, T.G. and Guo, X. Making Fischer-Tropsch fuels and electricity from coal and
biomass: Performance and cost analysis. Energy Fuel 25, 415–437 (2011).
transportation of CO2 and the permanence of storage. Therefore, a comprehensive life-cycle
analysis is required to ensure carbon negativity. In addition, many low-carbon policies and
associated GHG accounting frameworks (e.g. EU ETS, California ETS) do not currently appropriately
recognise, attribute or reward negative emissions from Bio-CCS.9
A closely related concept to BECCS is so-called Bioenergy with Carbon Capture and Utilisation
(BECCU). Here by-product CO2 from biomass processing is captured, but instead of permanent
storage, the CO2 is used as a feedstock in a way that produces value for the plant operator. Possible
applications of CO2 utilisation include enhanced oil recovery, carbonation of beverages, CO2
fertilisation in greenhouses, and various industrial approaches for the production of fuels, chemicals,
plastics and building materials.10 In most of these CCU applications, the CO2 is released into the
atmosphere fairly quickly after its utilisation, and therefore its climate change mitigation potential can
be significantly lower than that of CCS. However, focussing only on the fate of CO 2 in the overall
concept can lead to incomplete understanding of CCU’s climate impacts, as possible displacement
of fossil fuels and carbon intensity of the energy used to run the CCU process often have a decisive
role in the overall climate impact.11
CCS technologies have been used industrially over several decades for example in oil refining, and
they can be considered relatively mature. This goes not only for the capture part, but also for CO2
transport and storage. CO2 is removed from gas streams using commercial technologies such as
physical (e.g. Rectisol®, Selexol®, etc.), or chemical absorption (e.g. amine) scrubbing systems.
Regarding transport, CO2 has been shipped regionally for over 20 years, while a 5,000 km pipeline
network has been operating in the USA for over 30 years for Enhanced Oil Recovery (EOR). CO2
storage projects have been operating successfully now for over two decades, e.g. at Sleipner
(Norway). However, despite these experiences, the deployment of fully integrated CCS projects have
stalled, and fallen considerably behind from levels originally set by ambitious technology roadmaps.12
Currently, the only large-scale BECCS process is the Illinois Industrial CCS facility that captures
annually up to 1 Mt of CO2 from the fermentation process of a Decatur corn ethanol plant and injects
it into a geological storage beneath the facility. According to a recent report by the Global CCS
Institute,13 The remaining four BECCS facilities operating today are small-scale ethanol production
plants that use most of the captured CO2 for enhanced oil recovery (EOR); including:

• Plane Kansas Arkalon


o Location: USA
o Size: 200,000 tonnes per year
o Transport method: compressed and piped.
• Bonanza CCS
o Location: USA
o Size: 100,000 tonnes per year
o Transport method: compressed and piped.

9
Kemper, J. Biomass and carbon dioxide capture and storage: A review. International Journal of Greenhouse Gas Control
40, 401-430 (2015). DOI:10.1016/j.ijggc.2015.06.012.
10
Naims, H., Olfe-Kräutlein, B., Lafuente, AML. and Bruhn, T. CO2 Recycling – An Option for Policymaking and Society?
Twelve theses on the societal and political significance of carbon capture and utilisation (CCU) technologies (Institute for
Advanced Sustainability Studies, 2015).
11
Koponen, K. and Hannula, I. GHG emission balances and prospects of hydrogen enhanced synthetic biofuels from solid
biomass in the European context, Applied Energy 200, 106-118 (2017). DOI: 10.1016/j.apenergy.2017.05.014
12
Reiner, D.M. Learning through a portfolio of carbon capture and storage demonstration projects. Nature Energy 1, 1-
7 (2014). DOI: 10.1038/NENERGY.2015.11
13
Consoli, C. Bioenergy and carbon capture and storage (Global CCS Institute, 2019).
https://www.globalccsinstitute.com/wp-content/uploads/2019/03/BECCS-Perspective_FINAL_18-March.pdf
• Husky Energy CO2 Injection
o Location: Canada
o Size: 250 tonnes per day
o Transport method: compressed and trucked
• Farnsworth
o Location: USA
o Size: Over 600,000 tonnes of CO2 (injection now ceased)
o Transport method: compressed and piped.

2 Introduction
Bioenergy is the main source of renewable energy today, providing five times the contribution of
wind and solar to global final energy consumption, when traditional use of biomass is excluded.14 In
addition to electricity, bioenergy provides heat for industry and buildings, and fuels for transport.
Modern bioenergy plays an essential role in the International Energy Agency (IEA) 2°C Scenario
(2DS) providing nearly 17% of final energy demand in 2060 compared to 4.5% in 2015.15 Bioenergy
is important especially in sectors for which other decarbonisation options are not available. For
example, in the transport sector bioenergy complements improved efficiency and electrification, and
is particularly important in aviation and shipping. According to the IEA, its contribution to the transport
sector should grow ten-fold between 2015 and 2060.15
Technologies for producing so called “first generation” crop-based biofuels like ethanol from sugar
and starch-based feedstocks, and FAME (fatty acid methyl ester) biodiesel from vegetable oils and
other lipid feedstocks (including wastes and by-products) are well-established, and provide most of
today’s transport biofuels. In the short-term, the deployment of first generation biofuels could be
boosted by RD&D focussed on improving conversion rates, costs and life-cycle GHG emission
savings, improving the production of co-products such as animal feed, and widening the feedstock
base to include those with limited land-use implications. The share of bioethanol could be further
increased either by adopting higher blend levels with petrol, or by promoting unblended use to
maximise GHG emission reduction16.
In recent years, technology to produce HVO (Hydrotreated Vegetable Oil), also known as renewable
diesel (including advanced biodiesel, naphtha and aviation fuels), has been successfully
commercialised. About 5 Mt/yr of HVO was produced globally in 2017 and production is expected to
increase to 6-7 Mt/yr by 2020 and continue to increase thereafter.17 HVO production is increasingly
based on waste and residue oil and animal fat feedstocks rather than oil crops. HVO has
advantageous fuel characteristics compared to FAME, and can be used to produce so-called drop-
in fuels, i.e. fuels that can be used unblended in the existing vehicle fleet or distribution infrastructure.
The longer-term growth of transport biofuels in the IEA’s 2DS relies on the widespread supply of
novel advanced biofuels produced by processes that are generally not yet mature. Advanced
biofuels are sustainable fuels produced from non-food crop feedstocks that are capable of delivering
significant life-cycle GHG emissions savings without competing with food and feed crops for

14
IEA Renewables Information: Overview (IEA/OECD, 2020) https://www.iea.org/reports/renewables-information-
overview
15
IEA Technology Roadmap – Delivering Sustainable Bioenergy (IEA/OECD, 2017).
16
IEA Technology Roadmap – Delivering Sustainable Bioenergy (IEA/OECD, 2017)
17
Landälv, I., Waldheim, L. and Maniatis, K. (Eds.) Technology status and reliability of the value chains: 2018 Update
(ART Fuels Forum, Continuing the work of the Sub Group on Advanced Biofuels for the RED II market deployment for
Advanced Biofuels)
agricultural land use. Advanced biofuels can also be called “second generation” (2G) biofuels, to
differentiate them from first generation crop-based biofuels.
The development and commercialisation of advanced biofuel technologies has been slow, however,
and most commercial-scale projects are currently on hold due to the high investment cost of pioneer
process plants combined with the lack of funding instruments that share the risk of scale-up.
Nevertheless, policy interest remains strong, notably in Europe (RED2 sets a 3.5% target for
advanced biofuels by 2030),18 and in the United States (Renewable Fuel Standard, California Low-
Carbon Fuel Standard).19,20
The sustainable conversion of biomass feedstocks to biomass-derived fuels and chemicals are often
referred to as “biorefining”. In addition to biofuel, such “biorefineries” typically produce also by-
products and CO2 (see Figure 2). The CO2 from biomass processing is normally vented to
atmosphere, but if it were captured and securely sequestered in geological formations, the produced
biofuel could be characterised by net negative GHG emissions because of the storage of biogenic
CO2.

Figure 2: Conceptual representation of a biorefinery coupled with CCS.

As already mentioned, the coupling of biomass conversion with CCS has been promoted as one of
the most promising candidates for a large-scale NET.21 Globally, Bio-CCS could potentially remove
10 billion tonnes of CO2 from the atmosphere annually by 2050– equivalent to a third of all current
global energy-related emissions.22 Given the relative difficulty of mitigating CO2 emissions in the

18
EU. Directive (EU) 2018/2001 of the European Parliament and of the Council of 11 December 2018 on the promotion
of the use of energy from renewable sources (recast). 2018.
19
https://www.epa.gov/renewable-fuel-standard-program
20
https://ww2.arb.ca.gov/our-work/programs/low-carbon-fuel-standard
21
Johnson, N., Parker, N. and Ogden, J. How negative can biofuels with CCS take us and at what cost? Refining the
economic potential of biofuel production with CCS using spatially-explicit modeling. Energy Procedia 63, 6770-6791
(2014). DOI:10.1016/j.egypro.2014.11.712.
22
Koornneef, J., van Breevoort, P., Hamelinck, C., Hendriks, C., Hoogwijk, M., Koop, K., Koper, M., Dixon, T. and Camps,
A. Global potential for biomass and carbon dioxide capture, transport and storage up to 2050, International Journal of
Greenhouse Gas Control 11, 117-132 (2012). DOI: 10.1016/j.ijggc.2012.07.027.
transport sector, biofuel production with CCS is expected to play a significant role in reducing
̊ scenarios. 23
the carbon intensity of liquid transport fuels in 2 C
As existing CCS technologies have been developed largely around the combustion of fossil fuels,
they may need to be adapted for use with biomass feedstocks. This is due to the different
characteristics of biomass feedstocks (e.g. high oxygen content, high amount of volatiles, low
volumetric energy density and fibrous structure),24 and because biomass-processing plants are
usually an order of magnitude smaller than comparable plants based on fossil fuels.
Capturing CO2 from bioethanol production has been studied by Laude et al. for midsize plants.25
They found that GHG emission of CCS retrofit on fermentation and natural gas fired cogeneration
could be decreased by 115 % compared to the case without CCS. Later both the GHG emissions
and economics of CCS connected to US corn ethanol production have been investigated by
McCoy.26,27 Also, the coupling of CSS to sugar cane based bioethanol production has been
investigated.28,29
Sanchez et al. (2018)30 estimated that 60 percent of all CO2 emitted annually through the production
of ethanol at the US 216 biofuel plants (about 1 percent of all CO2 emissions from the U.S.) could
be captured at low cost, under $25 per metric tonne of CO2. If credits for captured CO2 were set at
$60 per metric ton, it would incentivise the sequestration of 30 MtCO2/yr that would otherwise be
vented into the atmosphere.
Liu et al.31 examined various system configurations that involve gasification-based coproduction of
Fischer-Tropsch liquid (FTL) fuels and electricity from coal and/or biomass, both with and without
capture and storage of by-product CO2. This was followed by later studies,32,33 where similar
approach was extended to cover synthetic petrol (gasoline). Highly carbon-negative fuels (specific
emissions of -123 gCO2/MJLHV) were produced when biomass was the only feedstock, although this
meant significant constraints on the scale of the fuel production plants and resulted in higher

23
Muratori, M., Kheshgi, H., Mignone, B., Clarke, L., McJeon, H. and Edmonds, J. Carbon capture and storage across
fuels and sectors in energy system transformation pathways, International Journal of Greenhouse Gas Control 57, 34-41
(2017). DOI: 10.1016/j.ijggc.2016.11.026.
24
Wilen, C., Moilanen, A. and Kurkela, E. Biomass feedstock analyses (VTT Publications 282, 1996).
25
Laude, Audrey & Ricci, Olivia & Bureau, G. & Royer-Adnot, J. & Fabbri, Antonin. CO2 capture and storage from a
bioethanol plant: Carbon and energy footprint and economic assessment. International Journal of Greenhouse Gas
Control 5, 1220-1231 (2011). 10.1016/j.ijggc.2011.06.004.
26
McCoy S., The bioeconomy through the lens of carbon management, US Department of Energy DOE, 2017
https://www.energy.gov/sites/prod/files/2017/10/f37/mccoy_bioeconomy_2017.pdf

27
MCCoy S., The Value Proposition for Combining CCS and Ethanol Production, 2017, Betterenergy.org
https://www.betterenergy.org/wp-content/uploads/2018/03/McCoy-Ethanol-and-CCS_v1.pdf
28
Hudson Bolsoni Carminati; Raquel de Freitas D. Milão; José Luiz de Medeiros; Ofélia de Queiroz F. Araújo, Bioenergy
and full carbon dioxide sinking in sugarcane-biorefinery with post-combustion capture and storage: Techno-economic
feasibility, Applied Energy, 254, 2019, 113633
29
Restrepo-Valencia S, Walter A., Techno-Economic Assessment of Bio-Energy with Carbon Capture and Storage
Systems in a Typical Sugarcane Mill in Brazil, Energies 2019, 12, 1129; doi:10.3390/en12061129
30
Sanchez, D.L., Johnson, N., McCoy, S.T., Turner, P.A and Mach, K.J. Near-term deployment of carbon capture and
sequestration from biorefineries in the United States. Proceedings of the National Academy of Sciences 115(19), 4875-
4880 (2018). DOI:10.1073/pnas.1719695115
31
Liu, G. et al. Making Fischer-Tropsch Fuels and Electricity from Coal and Biomass: Performance and Cost Analysis.
Energy Fuels 25, 415–437 (2011). DOI:10.1021/ef101184e
32
Liu et al. Gasoline from Coal and/or Biomass with CO2 Capture and Storage. 1. Process Designs and Performance
Analysis. Energy Fuels 29, 1830−1844, (2015). DOI:10.1021/ef502667d
33
Liu et al. Gasoline from Coal and/or Biomass with CO2 Capture and Storage. 2. Economic Analysis and Strategic
Context. Energy Fuels 29, 1845−1859 (2015). DOI:10.1021/ef502668n
production costs (due to lesser scale benefits) than for plants that co-processed also fossil
feedstocks.
Van Álamo et al.34 studied the potential to apply CCS in biomass and waste gasification-based
routes. A considerable impact on the reduction of GHG emissions was observed, doubling the
amount of CO2 avoided for both routes, but leading to 10-14% increase in the cost of biofuel.
Storing carbon from pyrolysis as biochar to improve soil properties in agriculture has been studied,
as is the use of bio-oil as asphalt binder and as an additive to concrete and other building materials35.
However, carbon capture from flue gas of the fast pyrolysis process has not been previously
evaluated.
CO2 can be also captured from pulp mills from various flue gases using standard post-combustion
capture technologies, Recent estimates for CO2 avoidance cost in kraft pulp mills range between 52
– 66 €/tCO2.36 In the IPCC 1.5° special report, the role of BECCS varies between 0 to 16 GtCO 2/yr
by 2050.37 Current CO2 emissions from chemical pulp production are roughly 350 MtCO2/yr. By
2050, the BECCS potential from the pulping sector could be in the range of 200-400 MtCO2/yr and
could play an important role in providing negative emissions needed to achieve overall carbon
neutrality targets.
Some studies also exist about the application of CCU to the production of biofuels. Hannula
examined the “enhancement” of biofuels manufacture with additional hydrogen, and found that up
to 2.6 or 3.1-fold increase in biofuel output could be attained for enhanced plant configurations over
reference designs.38,39 In a follow-up study, Koponen and Hannula40 found that the emissions of
BECCU are largely governed by the specific carbon emissions of the used electricity and needs to
remain below 84–110 gCO2/kWh for the fuels to achieve more than 70% emission saving compared
to fossil fuels. Onarheim et al.41 studied the possibility to add CCU to pyrolysis-based biofuel
production. Their results indicated that utilising pyrolysis process off-gases to produce synthetic
natural gas could provide up to 48%-61% savings in biomass use when fully enhanced with an
external hydrogen source.
In this work, we investigate the techno-economic feasibility of coupling CCS with the production of
biofuels. In section 3, we summarise publicly available information from relevant biofuel
demonstration plants that we use to develop Total Capital Investment (TCI) estimates for our
biorefinery configurations, and discuss methods used to carry out our analysis. In section 4, the basic
principles of capturing CO2 from biorefineries are discussed and the examined biorefinery
configurations are presented. In section 5, we present our simulation results, discuss the economic

34
Álamo, G. et al. Implementation of bio-CCS in biofuels production. (IEA Bioenergy Task 33, 2018)
35
Schmidt H-. Anca‐Couce A., Hagemann N., Werner C., Gerten D., Lucht W., Kammann C., 2019,
Pyrogenic carbon capture and storage, Bioenergy, 11, 573–591, DOI: 10.1111/gcbb.12553
36
Onarheim, K., Santos, S., Kangas, P. and Hankalin, V. Performance and cost of CCS in the pulp and paper industry part
2: Economic feasibility of amine-based post-combustion CO2 capture. International Journal of Greenhouse Gas Control
(2017).
37
Global Warming of 1.5 OC: An IPCC Special Report on the Impacts of Global Warming of 1.5° C Above Pre-industrial
Levels and Related Global Greenhouse Gas Emission Pathways, in the Context of Strengthening the Global Response to
the Threat of Climate Change, Sustainable Development, and Efforts to Eradicate Poverty (IPCC, 2018).
38
Hannula, I. Co-production of synthetic fuels and district heat from biomass residues, carbon dioxide and electricity:
Performance and cost analysis, Biomass and Bioenergy 74, 26-46 (2015). DOI: 10.1016/j.biombioe.2015.01.006
39
Hannula, I. Hydrogen enhancement potential of synthetic biofuels manufacture in the European context: A techno-
economic assessment. Energy 104, 199-212 (2016). DOI: 10.1016/j.energy.2016.03.119
40
Koponen, K. and Hannula, I. GHG emission balances and prospects of hydrogen enhanced synthetic biofuels from solid
biomass in the European context, Applied Energy 200, 106-118 (2017). DOI: 10.1016/j.apenergy.2017.05.014
41
Onarheim, K., Hannula, I. and Solantausta, Y. Hydrogen enhanced biofuels for transport via fast pyrolysis of biomass:
A conceptual assessment. Energy 199 (2020). DOI: 10.1016/j.energy.2020.117337
feasibility of capturing CO2 from biorefineries, and carry out sensitivity studies for key input
parameters. Finally in section 6, we derive conclusions based on our results, and propose directions
for future work.

3 Materials and methods


Several technological pathways are available for converting lignocellulosic feedstocks to biofuels
(see Figure 3). Gasification represents a thermochemical processing route where the feedstock is
first converted to gas at elevated temperatures (800 – 1200°C) and in the presence of an oxidising
agent (air, oxygen and/or steam). The gas is then cleaned and conditioned, and catalytically
converted either to hydrocarbon fuels (e.g. Fischer-Tropsch diesel or methane) or to fuel alcohol
(e.g. methanol). Alternatively, pure hydrogen can be produced by separation from synthesis gas
using Pressure Swing Adsorption (PSA).

Figure 3. Schematic of possible processing pathways to second generation biofuels from


lignocellulosic biomass.

Another main thermochemical option is the direct liquefaction of biomass into bio-oil, using e.g. fast
pyrolysis process where solid biomass is heated up rapidly at around 500°C and the formed product
is recovered as bio-oil by condensation. For use in transport applications (as diesel and/or petrol),
the produced bio-oil requires significant upgrading by hydrogenation.
The main biochemical pathway involves the hydrolysis of biomass into sugars, followed by
fermentation into bioethanol. The bioethanol is separated from the fermented solution by distillation.
In addition, a lignin-rich by-product is obtained from the process.
3.1 Reference plants
The prospective cost and performance of advanced biofuels have been extensively investigated in
a series of “scoping studies”. However, results from these past studies are heterogeneous, and a
wide range of values has been proposed.42 In addition, scoping studies typically evaluate costs at
some future date based on the assumption of mature technology. Such Nth-of-a-kind (NOAK) cost
estimates are valuable for outlining the prospective long-term cost potential of biofuels, but are less
useful in assessing costs of first-of-a-kind (FOAK) plants, as conventional cost estimation methods
are found to routinely understate the costs of pioneering FOAK technologies.43,44
In recent years, however, a small amount of actual data on demonstration projects has surfaced,
allowing indicative cost and performance estimates to be derived for different emerging biofuel
technologies from empirical evidence. In the following paragraphs, we present a selection of
demonstration plants that we use later to derive cost estimates for different FOAK plants at
commercial scale.

3.1.1 ADM Decatur, Illinois, USA


The ADM Decatur plant produces fuel ethanol from corn. The plant is large, processing 600,000
bushels of corn per day (~21,100 m3/d). Fuel ethanol is produced via the saccharification and
fermentation route based on enzymes and yeast. In this process, corn is milled into meal and mixed
with water and enzymes to produce a liquid mixture called mash. The mash is heated in order to
liquefy the cornstarch, and more enzymes are added to convert it to light sugars during
saccharification. The sugar-rich mash is cooled down and sent to fermentation where yeast
processes sugars in the mash. Fermentation products include heat, ethanol and CO2. The CO2 is
separated from the fermentation step while the mash, now called beer, is distilled to separate ethanol
from non-fermentable solids. The CO2 resulting from the fermentation is relatively pure and will only
need to go through a dehydration and compression process in order to meet the quality requirements
for delivery to the wellhead as supercritical CO2.
In 2011, construction begun for a full-scale commercial CCS unit at the Decatur plant. The initial plan
was to capture and store 2 500 tons of CO2/day to the nearby 7,000 feet deep saline Mount Simon
Sandstone formation. The first three years of operation, led by the Midwest Geological Sequestration
Consortium of which ADM is part of, captured and stored around 1 Mt CO2. In 2017, ADM took a
step further from the 2011-2014 one-off project by starting operation of the USDOE funded ~1 Mt
CO2/yr Illinois Carbon Capture and Storage (ICCS) project. The project holds an operating permit
for five years, totalling a capture rate of up to 5.5 Mt CO 2. The ADM facility is the 12th large-scale
CCS facility to go online in North America, and the first in the world to apply CCS on biofuels
production.45

3.1.2 Inbicon demonstration plant


The production of cellulosic ethanol has been demonstrated at the Inbicon plant at the port of
Kalundborg, Denmark, where 4 t/h of wheat straw is converted into ethanol, lignin pellets and C5
molasses. The demonstration plant was commissioned at the end of 2010 and the produced
cellulosic ethanol is currently distributed to 100 filling stations in Denmark as “Bio95 2G” petrol. Lignin
pellets are sold to DONG Energy for use in power plant, and the C5 molasses are sold as biogas

42
Haarlemmer, G., Boissonnet, G., Peduzzi, E. and Setier, P. Investment and production costs of synthetic fuels – a
literature survey. Energy 66, 667–676 (2014).
43
Merrow, E., Phillips, K., and Myers, C. (1981). Understanding Cost Growth and Performance Shortfalls in Pioneer
Process Plants (RAND).
44
Ansar, A., Flyvbjerg, B., Budzier, A., and Lunn, D. Should we build more large dams? The actual costs of hydropower
megaproject development. Energ. Pol. 69, 43–56 (2014).
45
Gollakota S. , McDonald S., Commercial-Scale CCS Project in Decatur, Illinois –Construction Status and Operational
Plans for Demonstration, Energy Procedia 63 ( 2014 ) 5986 – 5993
boosters in local biogas plants. Continuous operation from straw bales to fermentation has been
demonstrated achieving a yield above 198 litres of ethanol per tonne of dry straw.

3.1.3 Fortum Joensuu pyrolysis plant


Direct liquefaction of wood by fast pyrolysis has been demonstrated by several companies such as
Fortum and BTL-BTG, and commercial scale plants are currently being built. Fast pyrolysis oil can
be used as such to replace heavy fuel oil in the production of district heat or steam, but use as a
transport fuel requires significant upgrading by hydrogenation.
Our process design is inspired by the Fortum pyrolysis plant, located in Joensuu Finland. Start-up
of the plant was in 2013 and it produces 30 MW of pyrolysis oil (50 kt/yr) from 50 MW of lignocellulosic
residues.46 The pyrolysis plant is integrated with a co-located fluidised-bed boiler for the extraction
of hot bed material for the pyrolysis reactor. Downstream of the pyrolysis unit, the vapours are
separated and condensed while the sand and the by-products (char and permanent gases) are
returned as fuel to the fluidised-bed boiler.
The plant has been operated as a demonstration unit, using different kind of raw materials and
production parameters in order to develop and optimise the process. Final product has been used
for replacing Heavy Fuel Oil (HFO) and tested with several sizes of boilers, from 1MW to 300MW.
Hydrothermal liquefaction is another possible technology for direct liquefaction of biomass, but it was
not considered in this work due to lower TRL and therefore lack of information from demonstration
plants.

3.1.4 GoBiGas gasification plant


The production of synthetic biofuels from solid biomass residues has been demonstrated in Varkaus,
Finland (by Neste, Stora Enso and VTT); Chicago, USA (UPM, Haldor Topsoe and GTI); and in
Gothenburg, Sweden (GoBiGas). The Varkaus plant demonstrated the production of Fischer-
Tropsch fuels, while the production of synthetic petrol was demonstrated in Chicago and the
production of biomethane in Gothenburg. However, no commercial scale plants have yet been built.
The GoBiGas plant has been the biggest demonstration plant to date that represents gasification-
based 2nd generation biofuel technology. The plant was commissioned in 2014 by Göteborg Energi
in Gothenburg, Sweden; and features a 30 MWth dual fluidised-bed biomass gasifier that converts
pellets to raw synthesis gas. The syngas is purified with scrubbers and filters, and converted to
synthetic methane over a nickel catalyst at elevated temperature and pressure. The methane output
is 20 MW, suggesting about 67% (LHV) overall efficiency.47

3.2 Performance analysis


We analyse and compare the performance of different biorefinery configurations based on mass and
energy flows simulated with Aspen. Following helpful metrics are calculated to assist the
investigation. Fuel yield:

𝑏𝑏𝑙 𝑚̇𝑏𝑖𝑜𝑓 ∗ 𝐻𝑏𝑖𝑜𝑓


𝑌𝑓𝑢𝑒𝑙 ( 𝑡
) = ̇ ∗ 𝑚𝑏𝑖𝑜𝑚 ∗159
𝐻𝑝𝑒𝑡𝑟𝑜𝑙
, (1)

46
Siikanen L. https://www.cif-ifc.org/wp-content/uploads/2016/10/First-Commercial-Pyrolysis-Oil-Plant-_-DEMO-
2016_-Sikanen.pdf, 2016
47
Thunman H, Gustavsson C, Larsson A, Gunnarsson I, Tengberg F. (2019) Economic assessment of advanced
biofuel production via gasification using cost data from the GoBiGas plant. Energy Sci Eng. 2019;1-13.
https://doi.org/10.1002/ese3.271
where ṁbiof is output massflow of biofuel (kg/s), Hbiof is lower heating value of biofuel (MJ/s), Hpetrol is
lower heating value of petrol (MJ/l), ṁbiom is input massflow of dry biomass (kg/tonne) and 159 stands
for litres per barrel; and CO2 capture yield:
𝑚̇𝐶𝑂2
𝑌𝐶𝑂2 = 𝑚̇ , (2)
𝑏𝑖𝑜𝑚

where ṁCO2 is massflow of captured CO2.

3.3 GHG emissions analysis


We define total emission from biofuel production as a sum of upstream emissions (Eupstream) caused
by feedstock harvesting and transport, and nitrogen fertilisation to replace nutrients removed within
the feedstock; and process emissions (Eprocess) caused by the possible use of fossil fuels during
processing. Eupstream values are taken from the literature and Eprocess values are based on our process
simulation results. Emissions caused by manufacturing of the biofuel plants or other needed
infrastructure are excluded from the calculation. We also exclude emissions from producing the
catalyst needed in some configurations as they are found to represent less than a 0.1 % of total
emissions and thus have insignificant contribution to the overall results.40

Table 2. Emission calculation parameters.


Fossil fuel carbon intensities, gCO2eq/MJ

Natural gas48 65.9


Fossil petrol/dieselERROR! BOOKMARK NOT 94
DEFINED.48

Fossil hydrogen48ERROR! BOOKMARK NOT DEFINED.,* 93


Direct upstream emissions, gCO2eq/MJ
Corn ethanol48 25.5
48
Wheat ethanol 1.8
49, 2.4
Delivered waste wood **
*Calculated from natural gas emissions by dividing with thermal
efficiency of steam reforming of 71 % (LHV).

**Upstream emissions for the delivered waste wood are converted


to upstream biofuel emissions by dividing with thermal efficiency
of biomass to biofuel (LHV).

The functional unit under study is one megajoule (MJ) of biofuel produced, and emissions are
expressed as gCO2eq/MJ. We allocate all emissions to the main biofuel product, and electricity used
by some (ETOH and H2) configurations is assumed to be procured from zero-carbon sources. We
calculate CO2 emissions relative to fossil fuel comparator using the following equation:

48
Edwards, R Definition of input data to assess GHG default emissions from biofuels in EU legislation. (2019) JRC115952,
DOI: 10.2760/69179
49
Jäppinen, E., Korpinen, O., Laitila, J. and Ranta, T. Greenhouse gas emissions of forest bioenergy supply and utilization
in Finland, Renewable and Sustainable Energy Reviews 29, 369-382 (2014). DOI: 10.1016/j.rser.2013.08.101.
𝐸𝑢𝑝𝑠𝑡𝑟𝑒𝑎𝑚 + 𝐸𝑝𝑟𝑜𝑐𝑒𝑠𝑠
𝑅(%) = , (3)
𝐸𝑓𝑜𝑠

where Efos is emissions from fossil fuel comparator. Fossil fuel carbon intensities and upstream
emissions used in the calculations are summarised in Table 2.

3.4 Cost analysis


The prospective costs of advanced biofuels have been investigated extensively in a series of
‘‘scoping’’ studies intended to inform public policy discussions on their use. However, results from
past studies are heterogeneous and wide range of values have been proposed.50
In recent years, however, a small amount of actual data on demonstration projects has surfaced,
allowing indicative cost and performance estimates to be derived for emerging biofuel technologies
from empirical evidence. We use publicly available information from reference and demonstration
biofuel plants (see Table 3) to develop Total Capital Investment (TCI) estimates individually for each
configuration examined in this work. We use exchange rates and Chemical Engineer magazine’s
Plant Cost Index (CEPCI) to escalate all demonstration plant costs to 2018 US dollars. For a
description of reference plants, see section 3.1.
Table 3: Reference plant cost data.
Reference plant type Corn Cellulosic Pyrolysis oil Synthetic
ETOH ETOH biofuels

Reference plant name ADM Inbicon Fortum Joensuu GoBiGas


Decatur Demo plant pyrolysis plant
Location Illinois, Kalundborg, Joensuu, Finland Gothenburg,
USA Denmark Sweden
Biomass input, MW 371.8 16 50 30

Biofuel output, MW 278.5 4.6 30 20

Commissioning year 2011 2010 2012 2014

Total Capital 127 M$ 180 M$* 27 M€ 1375 MSEK


Investment

Adjusted TCI (M$2018) 131 216 36 210

*) We used a newer estimate to give more accurate estimate for near future 2G ethanol plants
according to e4Tech51.
To minimise distortion caused by scale benefits in the cost results, same biofuel output should be
used for all plants. However, as existing corn-based biofuel plants are much bigger than existing
cellulosic biofuel plants, a choice was made to set the scale of corn fed ETOH and ETOH-CCS plants
to 5000 bblpe/d (petrol equivalent barrels per day), and set the scale of lignocellulosic feedstock
plants to 1000 bblpe/d.
We use cost-scaling exponent (k) to scale reference plant capital costs (C0) to a commercial scale
capacity (S) using the following relation:

51
Chudziak C., Alberts G. and Bauen A., Ramp up of lignocellulosic ethanol in Europe to 2030, E4Tech,
6th International Conference on Lignocellulosic Ethanol, 2017.
𝑆 𝑘
𝐶 = 𝐶0 ∗ (𝑆 ) , (4)
0

where S0 is the scale of the reference plant and C the TCI of a FOAK plant at commercial scale.
The choice of capital investment scaling function and scaling parameter has a significant impact on
the estimated process economics. If the used scaling exponent is small, it suggests that the optimum
plant size is very large and vice versa. An average value of 0.67 is used for k in this work.52 Previous
research indicates that the investment for biomass-based plants, especially for the biochemical
route, could scale with higher values than this, but some ambiguity still remains regarding capital
investment scaling exponent for biorefineries.53
We calculate annual capital charges from the TCI using 0.12 capital charge rate, which is based on
10% WACC (weighted average cost of capital) and 20-year economic life for the biorefinery. The
yearly operating and maintenance (O&M) costs are assumed to be 4% of the TCI, and plants are
expected to run 8000 h per year (91% availability factor). The cost of feedstocks and electricity varies
greatly across time and geographic location. For the purpose of our cost analysis, following
representative values are used: 150 $/tonne for corn, $60/tonne (dry) for biomass and 50 $/MWh for
electricity. For designs incorporating CCS, CO2 is available at 150 bar at the plant gate. We assume
that the CO2 is transported 100 km from the conversion facility, and stored 2 km underground in
geological formations. The cost of transport and injection/storage of supercritical CO2 is valued at
15 $/tCO2.31 For a summary of financial parameters, see Table 4.

Table 4: Financial parameters used in the work.


WACC 8 %

Economic lifetime 20 years

Capital charge rate (CCR) 0.10 -

Annual operating and maintenance 4 % of TCI

Annual runtime 8000 h/yr

333 days/yr

Corn price 150 $/tonne

Biomass price 60 $/tonne

Electricity price 50 $/MWh

Natural gas price 30 $/MWh


Value of DDGS as animal feed 75 $/tonne
CO2 transport and injection/storage costs 15 $/tCO2

We evaluate the LCOF (levelised cost of fuel) production according to the following equation:
$ 𝐹+𝐸+𝐶+𝑂+𝑅
𝐿𝐶𝑂𝐹 (𝐺𝐽) = 𝑃
, (5)

52
Remer, D.S. and Chai, L.H. Estimate costs of scaled-up process plants. Chemical Engineering 97(4), 138, (1990).
53
Leboreiro, J. and Hilaly, A.K. Analysis of supply chain, scale factor, and optimum plant capacity for the production of
ethanol from corn stover, Biomass and Bioenergy 54, 158-169 (2013). DOI: 10.1016/j.biombioe.2013.03.021.
where

• F is the annual cost of biomass feedstock,


• E is the annual cost of electricity,
• C is the annualised capital charge, including return on equity and interest on debt,
• O is the annual operating and maintenance costs, and
• R is the annual revenue from selling by-product fuel gas.
The sum of these annual costs ($/yr) is divided by P, which is the annual output of fuel (GJ/yr) from
the plants. When defined in this way, LCOF ($/GJ) indicates the product sale price needed to break-
even under the technical and economic parameters assumed.

4 Process configurations
We examine five different biofuel technologies in detail, representing different approaches,
feedstocks, end-products and technological maturities, namely:

• 1st generation ethanol via fermentation of corn,


• 2nd generation ethanol via biochemical conversion of wheat straw,
• bio-oil via thermal fast pyrolysis of forest residues,
• Fisher-Tropsch liquids (FTL) via thermal gasification of forest residues, and
• hydrogen via thermal gasification of forest residues.
Each basic configuration is investigated with and without carbon capture and storage (CCS). Two
different CCS approaches are considered for plants that have more than one stream that contains
CO2. Our base case approach is to capture carbon only from high CO2 concentration streams, while
an alternative configuration CCS-MAX is developed for maximal CO2 capture (including also low
concentration streams). Combination of these designs results in thirteen configurations (see Table
5), each characterised by distinctive plant designs. These configurations are identified by acronyms
that identify both the biofuel production approach:

• ETOH = Ethanol from corn,


• CE = Ethanol from lignocellulosic biomass,
• PO = Pyrolysis oil from lignocellulosic biomass,
• FTL = Fischer-Tropsch liquids from lignocellulosic biomass,
• H2 = Hydrogen from lignocellulosic biomass;
and the treatment of carbon dioxide:

• V = Vent of biogenic-CO2 to atmosphere,


• CCS = Capture and underground storage of carbon from high concentration CO2 streams,
• CCS-MAX = Capture and underground storage of carbon from all streams that contain CO2.
Following capture efficiencies are assumed for different capture processes, depending on the CO2
source:

• 100% direct capture of CO2 from fermentation by drying;


• 97% capture of CO2 (and 100% co-capture of H2S) from synthesis gas by scrubbing with
chilled methanol;
• 90% capture of CO2 from flue gas by scrubbing with amine solution.
Table 5: Summary of examined process configurations.
CASE FEEDSTOCK CONVERSION END PRODUCT CO2 CAPTURE
TECHNOLOGY TECHNOLOGY

ETOH-V Corn Fermentation Fuel ethanol -


ETOH-CCS Corn Fermentation Fuel ethanol Chemical absorption

CE-V Lignocell. residues Biochemical conversion Fuel ethanol -


CE-CCS Lignocell. residues Biochemical conversion Fuel ethanol Drying

CE-CCS-MAX Lignocell. residues Biochemical conversion Fuel ethanol Drying and chemical
absorption
PO-V Lignocell. residues Fast pyrolysis (+ HDO) Bio-oil -

PO-CCS Lignocell. residues Fast pyrolysis (+ HDO) Bio-oil Chemical absorption


FTL-V Lignocell. residues Fluidised-bed gasification FT-liquids -
FTL-CCS Lignocell. residues Fluidised-bed gasification FT-liquids Chemical absorption

FTL-CCS-MAX Lignocell. residues Fluidised-bed gasification FT-liquids Physical and


chemical absorption
H2-V Lignocell. residues Fluidised-bed gasification Hydrogen -
H2-CCS Lignocell. residues Fluidised-bed gasification Hydrogen Physical absorption
H2-CCS-MAX Lignocell. residues Fluidised-bed gasification Hydrogen Physical and
chemical absorption

Three different feedstocks are considered in this work:


- Corn for ETOH-V and ETOH-CCS,
- Wheat straw for CE-V, CE-CCS and CE-CCS-MAX, and
- Forest residues for FTL-V, FTL-CCS, FTL-CCS-MAX, H2-V, H2-CCS and H2-CCS-MAX.
Feedstock properties for corn, wheat straw and forest residues are given in the appendix.
All examined plant configurations are designed self-sufficient in terms of heat and steam (by
recovering heat from hot process streams), while electricity is balanced from the grid. Process
models are developed using ASPEN Plus (Aspen) process simulation software and used as a tool
for carrying out performance analyses. The examined configurations are discussed in the following
sections, while main design parameters are summarised in the appendix.
4.1 Ethanol from corn (ETOH)

Bioethanol production from corn is a mature technology and mostly produced in the US. Between
2004 and 2014, US corn ethanol production increased from 13 to 54 billion litres per year.54
Production of bioethanol from corn or other starch-containing feedstocks involves a straightforward
and relatively low-CapEx process that achieves high yield to biofuel.

Figure 4: Block diagram of the ETOH-CCS process design.

In our 1st generation ethanol plant design (see Figure 4), the first step is milling of corn kernels to flour
needed to solubilise the polysaccharides in corn starch. If wet milling process is used, gluten meal
is often obtained as by-product. Water, enzymes, possibly lime to adjust pH and urea as nutrients
are added and the mixture is heated up to 88°C; the slurry is solubilised by cooking. After cooling in
the saccharification step the mixture is heated to 110°C help for 20 minutes and then cooled to 60°C,
pH is adjusted and enzymes are added to convert polysaccharides typically during 6 hours into
fermentable monosugars. The aqueous solution of monosugars are cooled and then fermented at
34°C during 46 hours to produce ethanol and CO2. The ethanol is separated by distillation at elevated
temperatures and subsequent water removal with molecular sieves55. The solution from ethanol
removal is evaporated and dried, while Distiller’s Dried Grain Solids (DDGSs) are separated and
typically used as feed for animals. The CO2 that is obtained from fermentation is washed with water
in order to remove traces of ethanol, and washed with glycol to remove residual water. Finally, CO2
is compressed to supercritical 150 bar pressure for transport.

4.2 Ethanol from lignocellulosic biomass (CE)


During the past 10 years, seven large-scale 2nd generation bioethanol plants have been
commissioned with design capacities between 10 and 114 million litres of fuel ethanol per year. Two
of these plants are integrated into or co-located with 1st generation ethanol plants, using corn and
sugarcane as raw material. The remaining five plants are stand-alone plants using different biomass
sources.

54
Jan Lewandrowski, Jeffrey Rosenfeld, Diana Pape, Tommy Hendrickson, Kirsten Jaglo & Katrin Moffroid (2019) The
greenhouse gas benefits of corn ethanol – assessing recent evidence, Biofuels, DOI: 10.1080/17597269.2018.1546488
55
McAloon A., Taylor F., Yee W, Ibsen K. Wooley R., 2000, Determining the Cost of Producing Ethanol from Corn Starch
and Lignocellulosic Feedstocks, National Renewable Energy Laboratory, NREL/TP-580-28893,
https://www.nrel.gov/docs/fy01osti/28893.pdf
The most recent plant, the St1 CellunolixTM facility in Finland, uses only wood processing side-stream
as raw material.56,57 The main pre-treatment technology in use is steam explosion or hydrothermal
pre-treatment, while other pre-treatment technologies are in development phase. We use publicly
available information from Inbicon demonstration plant producing bioethanol from wheat straw to
develop realistic mass and energy balances for our biochemical ethanol production route.58

Figure 5: Block diagram of the CE-CCS base case process design.

In our 2nd generation ethanol plant design (see Figure 5), wheat straw bales are cut into pieces and
the dry matter content of the feed is adjusted by recycling acetic acid containing condensate
recovered after the pre-treatment. Subsequently the biomass is kept at 180-200°C for 10-20 minutes
with steam.59 In aqueous solution at elevated temperatures and pressure, some of the
hemicelluloses are solubilised and after cooling, the solid residue can be converted into sugars more
easily in the enzymatic hydrolysis. The breaking down of the cellulose into fermentable sugars by
enzymes can take several days. The solid residue that contains mainly lignin is separated, dried and
combusted in a CHP plant to produce heat and power. The solution is subsequently fermented at
approximately 33°C and the formed ethanol is separated by distillation and further by dewatering
using molecular sieves. The fermentation gases containing mainly CO2 are washed to remove
ethanol and dried with glycol.
Finally, the pure CO2 is compressed to supercritical 150 bar pressure for transport. During
fermentation, especially C5 sugars remain partly unfermented (typically 0-20wt-%) and are
processed with anaerobic digestion to produce biogas. The biogas is burned together with lignin in
the CHP to heat and power.

56
Lynd, L.R.; Liand, X.; Biddy, M.J.; Allee, A.; Cai, H.; Foust, T.; Himmel, M.E.; Laser, M.S.; Wang, M. and Wyman, C.E.
2017. Cellulosic ethanol: status and innovation. Current Opinion in Biotechnology, 45, pp. 202-211. DOI:
10.1016/j.copbio.2017.03.008.
57
Yamamoto, M. 2018. St1 Cellunolix® process - Lignocellulosic bioethanol production and value chain upgrading.
Bio4Fuels Days, 12 October 2018, Oslo, Norway.
58
https://www.eia.gov/biofuels/workshop/pdf/paul_kamp.pdf, US energy Adminstration, 2012 accessed 29.4.2020
59
Larsen J., Østergaard M. H, Thirup L., 2012, Inbicon makes lignocellulosic ethanol a commercial reality, Biomass
Bioenergy 46, 36-45
Figure 6: Block diagram of the CE-CCS-MAX process design.

An alternative capture design CE-CCS-MAX is also examined (see Figure 6). The configuration is
otherwise similar to CE-CCS, but now CO2 from the combustion of by-products (lignin and biogas)
is also captured by scrubbing with amine wash. As the major part of feedstock carbon ends up in
lignin and biogas, significantly more CO2 can be captured by this design.

4.3 Pyrolysis oil from lignocellulosic biomass (PO)


Interest towards producing bio-oil (pyrolysis liquids) from biomass using fast pyrolysis process has
sustained already for several decades.60 Fast pyrolysis bio-oil (FPBO) is a complex mixture of
oxygenated hydrocarbons and contains around 20 - 30wt-% water, depending on the feedstock type
and pre-treatment approach. Consequently, FPBO is not directly compatible with current transport
fuel systems, but can be used to replace heavy fuel oil in boilers and kilns. Bio-oil can be further
refined to hydrocarbons via catalytic processing with hydrogen (hydro-deoxygenation, HDO) and
further distilled into diesel and petrol fractions that can replace petroleum distillates in transport use.61

Figure 7: Block diagram of the PO-CCS process design.

In our pyrolysis plant design (see Figure 7), processing starts with drying and pretreatment of forest
residues into small particles. Biomass is then fed to a thermal fast pyrolysis reactor where it is heated
rapidly to around 500°C typically in a fluidised bed. Major part of biomass (~80wt%) is vaporised and
recovered by quick cooling. The rest of the biomass in converted to char. The part of the vapour that

60
Oasmaa, A., Solantausta, Y., Arpiainen, V., Kuoppala, E., and Sipila¨, K. Fast pyrolysis bio-oils from wood and
agricultural residues. Energy & Fuels 24, 1380–1388 (2010).
61
Elliott, D.C. Transportation fuels from biomass via fast pyrolysis and hydroprocessing. WIREs Energy Environ., 2, pp.
525-533 (2013). DOI: 10.1002/wene.74.
condenses at approximately 30°C is called pyrolysis oil, while uncondensed gases are combusted
together with the char to produce heat. The generated heat is typically used internally in the process
and any excess is used to generate electricity. From flue gas, the CO2 is separated by scrubbing
with amines and the recovered CO2 is compressed to supercritical 150 bar pressure for transport.
The pyrolysis oil can be transported to an oil refinery where it is upgraded by hydrogenation into
transport fuels. Upgrading typically features several steps, and upgraded pyrolysis oil is usually co-
processed with petroleum fuels into transport fuels with a biofuel component.
Fast pyrolysis oil is not stable if stored at ambient or higher temperatures, as the share of water-
insoluble compounds, average molecular weight, and viscosity of bio-oil will increase over time. This
will also worsen bio-oil’s suitability for further upgrading, and imposes restrictions on the distance
between the pyrolysis plant and the refinery. However, aging can be slowed down by storing in cold
conditions, or with stabilisation methods like dilution, removing of alkali metals that catalyse aging
reactions, or adding antioxidants to stabilise reactive specimens.62

4.4 Fischer-Tropsch liquids from lignocellulosic biomass (FTL)


Gasification is a thermochemical conversion process that turns carbonaceous feedstocks into a gas
mixture rich in carbon monoxide and hydrogen, called product gas or synthesis gas depending on
the end-use application. Other major compounds include carbon dioxide, nitrogen, water, methane
and a rich spectrum of hydrocarbons and tars. A general objective of gasification is to maximise the
yields of light combustible gases and minimise the amounts of condensable hydrocarbons and
unreacted char. The exact composition of product gas depends on the type of process feeds, their
feed ratios, process parameters and the type of gasification reactor used. In contrast to coal
gasification, where char gasification reactions determine the overall yield, in biomass gasification the
devolatilisation stage of the feedstock and secondary reactions of primary pyrolysis products play
the major role.63 Once the feedstock has been converted to raw gas, it needs to be purified and
conditioned to meet the strict requirements of the downstream catalytic synthesis, which then
converts the gas to desired fuel depending on the choice of pressure, temperature and catalyst.

62
Oasmaa, A. Bio-oil stabilization, in Fast Pyrolysis of Biomass: Advances in Science and Technology. Royal Society of
Chemistry RSC, p. 138-159 (2017).
63
E. Kurkela, Formation and removal of biomass-derived contaminants in fluidized-bed gasification processes, VTT
Publications Vol.287, Technical Research Centre of Finland, VTT (1996).
Figure 8: Block diagram of the FTL-CCS process design.

Our gasification process design and the associated simulation model is validated with experimental
data derived from a 0.5 MWth PDU (process development unit) run circa 4000 hours in pressurised
oxygen-blown mode using various wood residues as feedstock.64 The model itself is described in
detail in Refs. [65,66]. The process (see Figure 8) begins with the drying of forest residues from
their initial moisture of 50 wt-% to 15wt-% with a belt dryer and fed to a fluidised-bed gasification
reactor operated at 880°C and 4 bar with a mixture of steam and oxygen (from a cryogenic air
separation unit, ASU). During gasification, the residues are converted to product gas containing CO,
H2, CO2, H2O, CH4, small amount of higher hydrocarbons and tars.67 The gas is cooled down to
820°C to facilitate removal of entrained dust by ceramic filter elements.68 Gas then enters a catalytic
reformer, where tars and hydrocarbons are converted to light gases.69 The tar-less gas exits the
reformer at around 950°C and is cooled down to 200-300°C while recovering sensible heat to
generate steam. The stoichiometry of the syngas (i.e. its molar H2/CO ratio, modulus) is then
adjusted by feeding a portion of the gas into a sour shift reactor where water-gas shift reaction is
catalysed. The outlet temperature of the adiabatic reactor is set to 400°C and minimum steam/CO
ratio of 1.8 is maintained with steam inputs located upstream from the reactor. The share of by-pass
gas flow is set to achieve a modulus of 2.1 for the combined stream. The shifted gas is then cooled

64
Kurkela E, Simell P, McKeough P, Kurkela M. Production of synthesis gas and clean fuel gas [Synteesikaasun ja
puhtaan polttokaasun valmistus]. VTT Publications 682, Technical Research Centre of Finland, VTT. 2008.
65
Hannula I, Kurkela E. A parametric modelling study for pressurised steam/O2-blown fluidised-bed gasification of
wood with catalytic reforming. Biomass and Bioenergy 2012;38:58-67.
http://dx.doi.org/10.1016/j.biombioe.2011.02.045.
Overcoming Barriers to Bioenergy: Outcomes of the Bioenergy Network of Excellence 2003-2009.
66
Hannula I, Kurkela E. Liquid transportation fuels via large-scale fluidised-bed gasification of lignocellulosic biomass.
VTT Technology 91, Technical Research Centre of Finland. 2013.
67
Kurkela E, Kurkela M, Hiltunen I. The effects of wood particle size and different process variables on the
performance of steam-oxygen blown circulating fluidized-bed gasifier. Environ Prog Sustain Energy 2014;33(3):681-7.
http://dx.doi.org/10.1002/ep.12003.
68
Simell P, Hannula I, Tuomi S, Nieminen M, Kurkela E, Hiltunen I, et al. Clean syngas from biomass e process
development and concept assessment. Biomass Convers Biorefinery 2014:1-14. http://dx.doi.org/10.1007/s13399-
014-0121-y.
69
Kaisalo N, Kihlman J, Hannula I, Simell P. Reforming solutions for biomass-derived gasification gas experimental
results and concept assessment. Fuel 2015;147:208-20. http://dx.doi.org/10.1016/j.fuel.2015.01.056.
to 200°C with heat recovery and fed to a two-stage water scrubber where it cools down to 60°C while
recovering sensible heat for feedstock drying. Finally, the gas is cooled down to 30°C to remove
syngas moisture. The dried gas is compressed and cooled down to enable removal of acid gases
(CO2 and sulphur species) from syngas by scrubbing with chilled methanol. The separated stream
of CO2 is compressed to supercritical 150 bar pressure for transport.
The ultra-clean synthesis gas is converted to Fischer-Tropsch syncrude using cobalt-based catalysts
in a boiling-water reactor. The reactor is operated at 200 °C and 25 bar and and reaction exotherm
is recoverd as saturated steam. The alpha value is set to 0.90 and selectivity to C5+ is 92%.70 The
pressure drop over the reactor is set to 1 bar. Input HO, CO, N as well as unreformed methane,
ethane and longer hydrocarbons are considered inert.
The C5+ and heavier oil fractions are recovered while lighter products (C1-C4) together with
unconverted syngas are recycled back to the synthesis reactor. A small amount of the recycle flow
is continuously purged to prevent accumulation of inerts and sent for combustion. The oil fraction
and wax (syncrude) is sent for refining to fuel-related products and the aqueous product (reaction
water) is treated as waste water.

Figure 9: Block diagram of the FTL-CCS-MAX process design.

Similarly to CE-CCS-MAX we also examine a maximal capture desing for the FTL technology. Here
additional carbon is captured from flue gas that originates from the combustion of purge from FT
synthesis and char from the fluidised-bed gasifier. Capture from flue gas is achieved by scrubbing
with amine. The combined stream of captured CO2 is then compressed to supercritical 150 bar
pressure for transport.

4.5 Hydrogen from lignocellulosic biomass (H2)


Hydrogen is one possible product from synthesis gas. In our hydrogen plant design (Figure 10),
forest residues are dried from their initial moisture of 50wt-% to 15wt-% with a belt dryer and fed to
a fluidised-bed gasification reactor operated at 880°C and 4 bar with a mixture of steam and oxygen.
The gas is then cooled down to 820°C to facilitate removal of entrained dust by ceramic filter
elements. Gas then enters a catalytic reformer, where tars and hydrocarbons are converted to light
gases. The tar-less gas exits the reformer at around 950°C, and is cooled down to 350°C with heat

70
Hargreaves, N. (2013). Velocys, Inc., Personal communication in February.
recovery. Syngas modulus (H2/CO ratio) is then maximised by two adiabatic sour shift reactors with
intermediate cooling. The maximum exit temperature from both reactors is set to 400°C and
minimum steam/CO ratio of 1.8 is maintained with steam inputs located upstream from the reactors.

Figure 10: Block diagram of the H2-CCS process design.

The shifted gas is then cooled down with heat recovery to 200°C and further to 60°C using two-stage
water scrubber that in the first stage recovers sensible heat for feedstock drying and in the second
stage further down to 30°C to remove syngas moisture. The dried gas is compressed to 20 bar and
fed to an acid gas removal unit where CO2 and sulphur species are removed by washing with chilled
methanol. The separated stream of CO2 is compressed to supercritical 150 bar pressure for
transport. The ultra-clean synthesis gas is then fed to a pressure swing adsorber (PSA) that
separates 86% of syngas hydrogen to a dedicated hydrogen stream with a hydrogen purity of
99.999vol%. Rest of the gas exits the PSA at an atmospheric pressure as off-gas. The off-gas is
combusted along with char from the gasifier in an auxiliary boiler.

Figure 11: Block diagram of the H2-CCS-MAX process design.


As an alternative to H2-CCS, we also examine a maximal CO2 capture design for the hydrogen
process H2-CCS-MAX. In addition to CO2 that is removed from pressurised syngas by scrubbing
with chilled methanol, additional CO2 from the combustion of PSA off-gas and char is captured from
flue gas by scrubbing with amine solution.

5 Results
5.1 Mass and energy flows
Mass and energy flows were simulated with Aspen for plants that produced either 5000 bblpe/d (from
corn) or 1000 bblpe/d (from lignocellulosic feedstocks) of biofuel. Main results are summarised in
Table 6. The highest fuel yield Yfuel (measured as petrol equivalent barrels per tonne of dry biomass)
is achieved with PO and H2 configurations (2.2 bblpe/t), followed by ETOHs (1.9 bblpe/t), FTLs (1.7
bblpe/t) and finally CEs (0.9 bblpe/t).

Table 6: Simulated annual mass and energy flows for the examined plant configurations.
Configuration Biomass, Electricity, Fuel, CO2 Yfuel
t/yr (dry) MWh/yr MWh/yr captured, (bbl/tonne)
tCO2/yr

ETOH-V 885 573 -84307 2 362 917 0


1.9
ETOH-CCS 885 573 -116077 2 362 917 302 576
1.9
CE-V 378 298 236679 472 583 0
0.9
CE-CCS 378 298 230329 472 583 63 490
0.9
CE-CSS-MAX 378 298 170359 472 583 469 193 0.9
PO-V 153 436 36825 472 583 0
2.2
PO-CCS 153 436 19919 472 583 107 684
2.2
FTL-V 197 982 28597 472 583 0
1.7
FTL-CCS 197 982 6735 472 583 208 207
1.7
FTL-CCS-MAX 197 982 1691 472 583 256 252 1.7
H2-V 151 856 -26210 472 583 0
2.2
H2-CCS 151 856 -54155 472 583 266 141
2.2
H2-CCS-MAX 151 856 -56202 472 583 285 643 2.2

Based on the simulated mass and energy flows, carbon flows are illustrated separately to all CCS-
configurations using Sankey diagrams. Easy comparison across different configurations has been
facilitated by normalising biomass input to 100 units of carbon for each process.
For ETOH-CCS (see Figure 12), 42 units of carbon end up in fuel ethanol while 37 C ends up in
Distiller’s Dried Grain Solids (DDGSs). The remaining 21 C of concentrated CO2 is captured at 100%
efficiency and compressed at the plant to 150 bar for transport.
Figure 12: Simulated carbon flows for plant producing ethanol from corn (ETOH-CCS). Some natural
gas is used in this configuration to regenerate glycol drying agent under high temperature. These
fossil carbon flows are not illustrated here, but have been included in the emissions calculations.

For CE-CCS (see Figure 13) 41 units of carbon continue with the pre-treated feed to fermentation
while 59 C end up in the solid residue stream. From fermentation 19 C end up into biofuel while 12 C
go to combustion together with the solid residue from pre-treatment as biogas. The remaining 10 C
of concentrated CO2 from fermentation is captured at 100% efficiency and compressed at the plant
to 150 bar for transport.

Figure 13: Simulated carbon flows for ethanol from lignocellulosic biomass (CE-CCS) configuration.

For CE-CCS-MAX, CO2 from the combustion of by-products is also captured by using amine wash
with 90% capture efficiency. The carbon flows are the same as in the case of CE-CCS, however
instead of 71 C only 7 C are now vented. A small residual part of carbon remains in the liquid phase
after digestion. The feed to digestion is highly digestable and only a negliable amount (few percent)
of the carbon in the feedstock goes to the digestate. Therefore it has not been considered here.

Figure 14: Simulated carbon flows for ethanol from lignocellulosic biomass (CE-CCS-MAX)
configuration featuring both CO2 capture from fermentation and from flue gas.

For PO-CCS (See Figure 15) 60 units of carbon end up in thermal bio-oil during pyrolysis while 40 C
will end up to combustion as char and purge gas. The formed CO2 is then captured with 90%
efficiency and compressed to 150 bar for transport.

Figure 15: Simulated carbon flows for fast pyrolysis oil from lignocellulosic biomass (PO-CCS)
configuration.

For FTL-CCS (See Figure 16), 97 units of carbon are converted to gas and tars and 3 C to solid
char. From carbon contained in the synthesis gas, 41 units are fed to the FT unit where 31 C is
converted to FT liquids (syncrude) and 11 C to purge gas. The purge gas is combusted together with
char to form a stream of diluted CO2 for venting to atmosphere. Separation of CO2 by scrubbing with
chilled methanol captures 54 units of carbon (capture losses 2C) that are compressed to 150 bar for
transport.

Figure 16: Simulated carbon flows for Fischer-Tropsch liquids from lignocellulosic biomass (FTL-
CCS) configuration.

For FTL-CCS-MAX (Figure 17) additional 12 C from the combustion of char and FT purge is captured
increasing the total capture share to 66 C. Combined capture losses are 3 C for this maximal capture
design.

Figure 17: Simulated carbon flows for FTL-CCS-MAX configuration.


For H2-CCS (see Figure 18), 97 units of carbon are converted to gas and tars and 3 C to solid char.
After maximal shifting, the gas now contains essentially only hydrogen and CO2 with some residual
methane and carbon monoxide. Almost all carbon (90 C) is separated by washing with chilled
methanol (capture losses 3 C). Synthesis gas is then fed to a PSA unit where most of the hydrogen
is removed to a separate stream. The remaining off-gas (4 C) is combusted with char (3 C) from the
gasifier in an auxiliary boiler to form a diluted stream of CO2 with 7 C. The concentrated stream of
CO2 from PSA is compressed to 150 bar for transport.

Figure 18: Simulated carbon flows H2-CCS configuration.

For H2-CCS-MAX (Figure 19), additional 7 C following combustion of char and PSA off-gas is
captured by washing with amine. This increases the total capture share to 97 C. Combined capture
losses are 4 C for this maximal capture design (deviations from 100 caused by rounding).

Figure 19: Simulated carbon flows for H2-CCS-MAX configuration.


The carbon flows discussed above are summarised in Table 7, together with calculated results for
the upstream, conversion and total biofuel emissions (gCO2eq/MJ) and R. The H2-CCS
configuration captures the highest share of input carbon to a concentrated stream of CO2 (97% and
90%), followed by CE-CCS-MAX (74%), FTLs (66% and 54%), PO-CCS (36%), ETOH-CCS (21%)
and finally CE-CCS (10%).
Relative emissions (R) from the plants are negative for almost all examined configurations featuring
CCS due to the storage of the biogenic-CO2. ETOH-CCS is an exception due to the high upstream
emission, the use of natural gas as an energy source, and to the small share of CO2 being captured.
Table 7: Carbon distributions and biofuel emissions. R is relative biofuel emissions in comparison to
the fossil fuel reference. We use 94 gCO2/MJ for petroleum-derived diesel/petrol and 93 gCO2/MJ
for fossil hydrogen produced via steam reforming of natural gas.
OF FEEDSTOCK CARBON
THAT ENDS UP

Direct Direct Total direct


stored upstream process
vented in fuel
as CO2
emissions R
emissions emissions gCO2/MJ
gCO2/MJ gCO2/MJ
ETOH-V 0.0 41.9 0.0 25.5 26 51 54 %
ETOH-CCS 0.0 41.9 21.0 25.5 -10 16 16 %
CE-V 81.0 19.0 0.0 1.8 0 2 2%
CE-CCS 71.0 19.0 10.0 1.8 -37 -36 -38 %
CE-CCS-MAX 7.1 19.0 73.9 1.8 -276 -274 -291 %
PO-V 40.0 60.0 0.0 4.2 0 4 4%
PO-CCS 4.0 60.0 36.0 4.2 -63 -59 -63 %
FTL-V 69.4 30.6 0.0 5.4 0 5 6%
FTL-CCS 15.5 30.6 53.9 5.4 -122 -117 -124 %
FTL-CCS-MAX 3.1 30.6 66.4 5.4 -151 -145 -154 %
H2-V 100.0 0.0 0.0 4.1 0 4 4%
H2-CCS 10.1 0.0 89.9 4.1 -156 -152 -163 %
H2-CCS-MAX 3.5 0.0 96.5 4.1 -168 -164 -175 %

Wheat ethanol with maximal CO2 capture is the most carbon negative product having emissions of
-291% relative to fossil petrol. This is caused by both the large share of CO2 being captured and the
relatively low conversion efficiency to ethanol. ETOH-CCS-MAX is followed by hydrogen plants
having emissions ranging from -175% to -163% relative to fossil hydrogen, followed by FT liquids
from 154% to 124%, thermal bio-oil (-63%) and 2G ethanol with base case CO2 capture design (-
38%).
Natural gas is one of the main process utilities used in corn based ethanol plant and replacing it with
a low-carbon alternative such as biogas, electricity etc. would lower the total biofuel emissions for
ETOH-V from 51 to 26 gCO2/MJ and for ETOH-CCS from 16 to -10 gCO2/MJ. In the latter case, the
switch from natural gas to a non-fossil energy source together with CCS would therefore negate
direct upstream emissions for the corn ethanol plant, making it a negative emissions technology.
The calculated biofuel emissions are also illustrated in Figure 20 together with biofuel yields and CO2
capture rates for configurations featuring CCS. The biofuel yields are calculated as petrol equivalent
litres per tonne of dry biomass input, and the CO2 capture rates are calculated as stored kilograms
of CO2 per tonne of dry biomass input.
Between 1881 and 1753 kg of CO2 is captured for every tonne of biomass (dry) by H2 configurations
featuring CCS. This is followed by FT-liquids with capture rate from 1294 to 1052 kgCO2/tbiom, CE-
ETOH with capture rate from 1240 to 168 kgCO2/tbiom, thermal bio-oil with 702 kgCO2/tbiom capture
rate and 1G ethanol with 342 kgCO2/tbiom.
Ethanol configurations that feature base case CCS designs have the smallest CO2 capture rates as
most of the biomass carbon will end up in the by-products, either distiller’s dried grain solids (from
corn) or combustion feedstock (from lignocellulosic biomass). When CO2 from the by-product
biomass is also captured (CE-CCS-MAX), a substantial increase in capture rate is achieved.
For thermochemical configurations, base case CCS designs already capture most of the available
CO2 from the process and maximal capture designs contribute only a small addition to the total
capture. Highest capture rates are achieved with hydrogen configurations as all carbon from the
process is in the form of CO2 and therefore available for capture.

Figure 20: Biofuel yields, the amount of CO2 captured and biofuel emissions for the examined
biorefinery configurations that feature carbon capture and storage.
5.2 Process economics
Our FOAK estimates are summarised in Table 8 for each process configuration. The estimated
carbon capture and compression (CCC) investments are presented separately and added to Vent
configurations to arrive at an estimate on the TCI of CCS configurations. As separation of CO2 is
already included in the ethanol and gasification configurations, the additional investment needed to
realise a CCS configuration comprises only of the compression system to pressurise CO2 to 150 bar
for transport..
The cost for CO2 compression to supercritical pressure is based on Kreutz, et al.,71 who give a cost
of $14.8 million ($2002) for a CO2 dehydration and compression system (to 150 bar) at a scale of
13 MWe. Of this total, 36% is due to the dehydration equipment, which is not required in biomass
gasification based designs, as the CO2 emerges dry from the Rectisol process. Kreutz’s cost includes
BOP, indirect costs (15%), and contingencies (15%).
The investment cost of post-combustion capture plant is estimated according to Jones et al.72 The
total fixed investment cost for a 30 % Monoethanolamine (MEA) capturing 0.91 million tonne/annum
CO2 capture plant was $134.4 year 2011. All investment costs are given as 2018 costs.
Table 8: Investment cost (TCI) estimates
Configuration CCC, M$ TCI, M$

ETOH-V 136
ETOH-CCS 7 143
CE-V 253
CE-CCS 2 255
CE-CCS-MAX 83 335
PO-V 56
PO-CCS 33 89
FTL-V 434
FTL-CCS 3 437
FTL-CCS-MAX 22 456
H2-V 434
H2-CCS 4 437
H2-CCS-MAX 14 448

Using total capital investment estimates from Table 8 and financial parameters from Table 4, we
calculate annual cash flows for the examined configurations as shown in Table 9.

71
Kreutz, T., Williams, R., Consonni, S., and Chiesa, P. Co-production of hydrogen, electricity and CO2 from coal
with commercially ready technology. Part B: Economic analysis. International Journal of Hydrogen Energy
30, 769-784 (2005).
72
D. A. Jones, T. McVey, S. J. Friedmann, 2013 Technoeconomic Evaluation of MEA versus Mixed Amines for CO2
Removal at Near-Commercial Scale at Duke Energy Gibson 3 Plant, Lawrence Livermore National Laboratory,
https://pdfs.semanticscholar.org/16fb/87f2ea4136441baafa23c56a9aa375634922.pdf
Table 9: Annual cash flows for the examined plant configurations as M$(2018)/yr.
CONFIGURATION CAPITAL O&M CORN BIOMASS NG DDGS CO2 ELECTR. TOTAL
DISPOSAL REVENUE

ETOH-V 13.9 5.4 132.8 4.2 162


27 -22
ETOH-CCS 14.5 5.7 132.8 4.5 5.8 169
28 -22
CE-V 25.8 10.1 22.7 -11.8 47
CE-CCS 26.0 10.2 22.7 1.0 -11.5 48
CE-CCS-MAX 34.2 13.4 22.7 7.0 -8.5 69
PO-V 5.7 2.3 9.2 -1.8 15
PO-CCS 9.1 3.6 9.2 1.6 -1.0 23
FTL-V 44.2 17.3 11.9 -1.4 72
FTL-CCS 44.5 17.5 11.9 3.1 -0.3 77
FTL-CCS-MAX 46.5 18.2 11.9 3.8 -0.1 80
H2-V 44.2 17.3 9.1 1.3 72
H2-CCS 44.6 17.5 9.1 4.0 2.7 78
H2-CCS-MAX 45.6 17.9 9.1 4.3 2.8 80

Finally, the contribution of different cost categories on the total cost of fuel ($/GJLHV) and the cost of
CCS ($/tCO2) are presented in
Table 10. Cost of carbon capture and sequestration ranges from 22 $/tCO2 to 66 $/tCO2 depending
on the examined configuration. Lowest costs are associated with ethanol and gasification-based
plants that feature CO2 separation already in the base (vent) configuration and the cost of adding
CCS is only 22 – 25 $/tCO2. A clear jump in cost can be seen for plants that incorporate post-
combustion capture design, being 66 $/tCO2 for pyrolysis where all CO2 is captured from flue gas,
and 50 $/tCO2 for CE-CCS-MAX, where part of the CO2 is captured at a lower cost from fermentation.
For the CCS-MAX configurations, the costs increase more moderately for gasification-based
configurations where only a small part of the overall CO2 is captured from flue gas.
Table 10: Cost comparison of examined process configurations. Results are given as $/GJLHV, if not
otherwise noted.

CONFIG. CAPITAL O&M FEED NG DDGS CO2 ELECTR. TOTAL COST OF


($/GJ) CCS
STOCK DISPOSAL ($/TCO2)

ETOH-V 1.6 0.6 15.6 -2.6 0.5 19.0


3.2
ETOH-CCS 1.7 0.7 15.6 -2.6 0.5 0.7 19.8 24
3.2
CE-V 15.1 5.9 13.3 -7.0 27.5
CE-CCS 15.3 6.0 13.3 0.6 -6.8 28.4 25
CE-CCS-MAX 20.1 7.9 13.3 4.1 -5.0 40.4 47
PO-V 3.4 1.3 5.4 -1.1 9.0
PO-CCS 5.4 2.1 5.4 0.9 -0.6 13.2 66
FTL-V 26.0 10.2 7.0 -0.8 42.3
FTL-CCS 26.2 10.3 7.0 1.8 -0.2 45.0 22
FTL-CCS-MAX 27.3 10.7 7.0 2.3 0.0 47.2 33
H2-V 26.0 10.2 5.4 0.8 42.3
H2-CCS 26.2 10.3 5.4 2.3 1.6 45.8 22
H2-CCS-MAX 26.8 10.5 5.4 2.5 1.7 46.9 27

The main cost results (the levelised cost of fuel and the cost of CCS) are also visualised in Figure 21
for all examined plant configurations.

Figure 21: Levelised cost of fuels (dollars per petrol equivalent litres of biofuel) and cost of CCS (US
dollars per tonne of sequestered CO2) for all examined plant configurations.
The levelised cost of biofuel ranges from 0.3 to 1.5 dollars per petrol equivalent litre being lowest for
thermal bio-oil from pyrolysis and second lowest for corn ethanol. A clear jump in costs can be seen
when transitioning to other technologies. LCOF for wheat ethanol is between 0.9 and 1.3 $/lpe
(dollars per petrol equivalent litres) depending on the CCS design whereas gasification based
configuration has biofuel cost between 1.4 and 1.5 $/lpe.

5.3 Sensitivity to plant scale


We then investigate the impact of plant scale on process economics. Chemical process technologies
are usually expected to benefit from a large scale, as doubling the plant output less than doubles the
capital investment cost. Biomass-based technologies are, however, limited in their scale by the
availability of biomass, which is a geographically dispersed resource that cannot usually be
economically transported more than 100 km. In Figure 22, the impact of plant scale on the cost of
CCS and levelised cost of fuel is examined for plants that process woody biomass (we exclude corn
ethanol plants from this analysis as they are operating at a much larger scales).

Figure 22: Impact of plant scale on the cost of CCS and on the levelised cost of biofuel.

According to the results, the plant size has modest impact on the cost of CCS for plants that
incorporate capture from fermentation and from synthesis gas, as the costs are associated only for
the compression and are therefore relatively low. For plants where most of the CO2 is captured from
flue gases by scrubbing with amine, the size of the plant has higher impact on costs. For example,
for pyrolysis plants the cost of CCS reduces from 78 $/tCO2 to 58 $/tCO2 when the scale of plant
increases from 500 to 2000 bbl/d. The plant scale has a much more pronounced impact on the
levelised cost of fuel. For example, for gasification based configurations the cost of biofuel reduces
from about 1.8 $/lpe to 1.3 $/lpe when plant scale increase from 500 to 2000 bbl/d level.
In Figure 23, we examine the impact of feedstock cost on the biofuel production cost. Here the corn
ethanol configurations are also excluded from the comparison as they are governed by different
feedstocks characteristics (both in terms for cost and availability) than plants operating on
lignocellulosic feedstocks.
Figure 23. Impact of cellulosic biomass cost on the levelised cost of fuel.

Based on the results, the feedstock cost has lowest impact on the biofuel production cost for the
gasification-based configurations, and highest for the PO-CCS and CE-CCS configurations. This is
probably explained by the higher share of CapEx in the cost of gasification-based plants. For
example, an increase in the cost of biomass feedstock from 30 to 90 $/tonne increases the biofuel
production cost by 61% (from 0.7 to 1.1 $/lpe) for the CE-CCS plant, but only by 12% (1.4 – 1.6
$/lpe) for the H2-CCS-MAX.

6 Discussion and recommendations


CCS technologies have for long been considered as an essential tool to meet climate mitigation
targets in the power and industrial sectors. In recent years, however, as the need to remove
substantial amounts of carbon dioxide from the atmosphere has become imminent, the prospect of
coupling CCS with bioenergy has regained interest.
Five different biorefinery technologies have been examined and compared, representing different
technological approaches, feedstocks, end-products and commercial maturities. Some process
configurations, like those involving fermentation, feature high-concentration CO2 streams that could
be captured and prepared for transport at a low cost. Some concepts feature both high and low
concentration CO2 streams, and therefore a higher share of capture would also lead to higher cost
of CCS. In the present work, our base case capture designs capture CO2 only from high-
concentration streams, while MAX designs feature additional capture from low-concentration
streams, i.e. flue gases. Here, our pyrolysis design represents an exception, as CO2 is only available
in flue gas, and therefore the base case capture design is also the MAX design.
Based on our results, the cost of adding CCS on the high-concentration streams of biorefineries
varies between 22 and 24 $/tCO2. If CCS is extended also to flue gas streams, the cost of CCS
varies between 27 and 66 $/tCO2. The wider range of cost is explained by differences between
biorefineries in the share of CO2 that needs to be captured from low-concentration streams. The
lowest cost of CCS is achieved with gasification-based configurations using base case CCS design
(22 $/tCO2) followed closely by ethanol plants with base case CCS design (24-25 $/tCO2). However,
up to ten times more CO2 (1052 – 1753 kgCO2/tbiom) is captured from the same amount of biomass
by gasification configurations than by base case ethanol configurations (168 – 342 kgCO2/tbiom). Only
when the by-product lignin is fully combusted and captured (CE-CCS-MAX) can similar capture rates
be achieved for the biochemical plants. However, this will significantly increase the cost of CCS to
47 $/tCO2.
Due to the capture and sequestration of biogenic CO2, biorefineries show deeply negative emissions.
The corn ethanol design ETOH-CCS is a notable exception to this rule, due to high upstream
emissions of corn and the use of natural gas as additional energy source in the process. However,
if natural gas would be switched to a low-carbon energy source, corn ethanol plants with CCS would
also produce carbon negative fuels. For biorefineries based on woody biomass, emissions range
between -36 gCO2eq/MJ and -274 gCO2eq/MJ. The deepest emissions reductions in comparison to
fossil petrol are associated with CE-CCS-MAX as it combines a large capture rate with relatively
small biofuel output, therefore leading to highly negative emissions per megajoule of biofuel
produced.
On paper, biorefineries with CCS seem very attractive. They would contribute to decarbonising the
hard-to-abate transport sector, provide much-needed negative emissions at scale, and the cost of
CCS would be only a fraction of that when applied to traditional power plants. On the other hand, the
cost of biofuel is currently too high to compete with petroleum fuels, the location of a geological
storage formation does not always coincide with good availability of biomass, and out of the 13
examined configurations only ETOH-V and ETOH-CCS have been currently demonstrated at
commercial scale.
However, responding to the Paris Agreement will ultimately require deploying negative emissions at
scale. Given the current slow progress in deploying both biorefineries and CCS, the main goal in the
near term should be to develop successful large-scale demonstration projects that reduce risk and
increase investor confidence towards these emerging technologies. Any assessment of the
prospective performance and cost of biorefineries with CCS is inevitably limited by the small handful
of actual projects, and so, more operational plants will be needed to reduce uncertainties and to start
learning from these technologies at relevant scale.
Annex I:
Summary or process design parameters and feedstock
properties
All process design parameters used in the Aspen simulation models are listed separately for
biochemical, fast pyrolysis, and gasification configurations in Table 11. In addition, equipment
common to all designs are described at the end of the table.

Table 11: Summary of design parameters used in simulation models.


Item Design parameters
Biochemical configurations

Corn to Ethanol Equal molar amount of CO2 and ethanol are produced, corresponding to a mass
ratio of 1.054 between ethanol and CO2. Ethanol yield = 452 litres (357 kg) of
ethanol per metric tonne dry matter of corn feedstock.

Ethanol from Equal molar amount of CO2 and ethanol are produced, corresponding to a mass
lignocellulosic biomass ratio of 1.054 between ethanol and CO2. Mass yield of ethanol assumed to be
16.7 wt-% according to data reported in the Inbicon demo plant.73 Lignin residue
and produced biogas are combusted at a nearby CHP plant.
Fast pyrolysis configurations
Mass yield of pyrolysis oil based wood dry matter 77 wt-%, based on experimental
pilot test at VTT in the 4REFINERY project. Mass of CO 2 produced in combustion
of char and gases in pyrolysis process 79 wt% of the dry biomass feed.
Gasification configurations
Pressurised steam/O2- Heat loss = 1 % of biomass LHV. ∆p = -0.2 bar. Carbon conversion: 97 %. Modelled
blown fluidised-bed in two steps with RStoic and RGibbs using Redlich-Kwong-Soave equation of state
gasifier with Boston-Mathias modification (RKS-BM). Hydrocarbon formation (kmol/kg
of fuel volatiles): CH4 = 6.7826, C2H4 = 0.4743, C2H6 = 0.2265, C6H6 = 0.2764. Tars
modelled as naphthalene: C10H8 = 0.0671, All fuel nitrogen converted to NH3. All
other components assumed to be in simultaneous phase and chemical
equilibrium. Inlet pressure 4 bar, outlet temperature 880°C.
Ceramic hot-gas filter ∆p = -0.05 bar. Inlet temperature 820 °C.
Catalytic autothermal Modelled as RGibbs using Redlich-Kwong-Soave equation of state with Boston-
partial oxidation Mathias modification (RKS-BM). Phase and chemical equilibrium conversion for
reformer C2+ and tar. Ammonia conversion restricted to 50 %. Outlet temperature 957°C,
CH4 conversion 95 %. ∆p = -0.4 bar
Sour-shift reactor(s) Steam/CO = 1.8 mol/mol, ∆p = -0.2 bar. Modelled as REquil using Redlich-Kwong-
Soave equation of state with Boston-Mathias modification (RKS-BM).
Equilibrium reactions: CO + H2O = CO2 + H2, T appr = 10 K. COS + H2O = CO2 +
H2S, T appr = 0 K. HCN + H2O = CO + NH3, T appr = 10 K.
FTL designs: one adiabatic WGS reactor, T out = 400°C, bypass adjusted to
achieve H2/CO = 2.1 (mol/mol).
H2 designs: two adiabatic WGS reactors. T1out=400°C and CO conversion 75%,
T2out=250°C and CO conversion 79%; combined CO conversion 95%.
Syngas scrubber Scrubbing liquid: water. Tinlet 200 °C. Two-step cooling: T1 = 60 °C, T2 = 30 °C.
cooler Complete ammonia removal. Modelled as Flash using Soave-Redlich-Kwong
(SRK) equation of state model.
Acid gas removal (pre- 97 % capture of CO2, 100% capture of H2S. Utilities: Electricity (other than for
combustion capture) refrigeration) =1900 kJ/kmol(CO2 +H2S); Refrigeration 3 x duty needed to cause -
12 K temperature change in the syngas; 5 bar steam = 6.97 kg/kmol (H 2S+CO2).
Low-temperature Treaction = 200°C, Pfresh feed = 25 bar, ∆p =-1 bar, Boiling-water reactor using cobalt
Fischer-Tropsch catalysts modelled with REquil using Redlich-Kwong-Soave equation of state with
synthesis Boston-Mathias modification (RKS-BM). Per-pass CO conversion depending on
the configuration. 0.90 α value and 92 % C5+ selectivity. Input H2O, CO2, N2 as
well as unreformed methane, ethane and longer hydrocarbons considered inert.

73
Larsen J., Østergaard M., H. , Thirup L., Inbicon makes lignocellulosic ethanol a commercial reality, Biomass and bio
energy, 46 ( 2 0 1 2 ) 3 6 -4 5
Pressure Swing Inlet: 25°C and 20 bar. Pressure drop 0.2 bar for product stream, off-gas at
Adsorption ambient pressure. Hydrogen separation efficiency 86%.
Common equipment
Post-combustion Regeneration of 30 wt-% MEA CO2 absorption solvent is assumed to require 3.9
capture GJ/tCO2 absorbed, thus appr. 31.9 MW of heat is needed for regeneration.
When 3.9 MW of heat is supplied as 4.5 bar steam instead of 2 bar district heat,
the estimated reduction in power production for case ETOH-CCS-MAX is 1.0 MW
based on process simulation.
When 3.9 MW of heat is supplied as 4.5 bar steam instead of 2 bar district heat,
the estimated reduction in power production for case PO-CCS is 0.2 MW based
on process simulation.
CO2 compression The outlet pressure of each compression stage is specified (polytropic efficiencies
in parentheses) as follows: compression stage 1: 4.35 bar (80 %) stage 2: 18.65
bar (80 %) and stage 3: 80 bar (75 %). After the third stage, the supercritical CO 2
is pumped to the suggested final pressure of 150 bar. All compressor drivers have
an efficiency of 95 % giving specific electricity requirement of 0.36 MJ/kgCO 2 for
the pressurisation of CO2 from near atmospheric level to 150 bar.
Heat exchangers74 ∆p/p = 2 %; ∆Tmin = 15°C (gas-liq), 30 °C (gas-gas). Heat loss = 1 % of heat
transferred.
Compressors75 Stage pressure ratio <2, ηpolytropic = 0.85, ηdriver= 0.92, ηmechanical = 0.98.
Multistage Stage pressure ratio <2, ηpolytropic = 0.87, ηdriver = 0.92, ηmechanical = 0.98, Tintercooler =
compressors (>4.5 35 °C, ∆p/p intercooler = 1%.
kg/s)76
Multistage Stage pressure ratio <2, ηpolytropic = 0.85, ηdriver = 0.90, ηmechanical = 0.98, Tintercooler =
compressors (<4.5 35°C, ∆p/p intercooler = 1 %.
kg/s)ERROR! BOOKMARK NOT D
EFINED.

PumpsERROR! BOOKMARK N ηhydraulic = 0.75, ηdriver = 0.90.


OT DEFINED.

74
G. Liu, E. D. Larson, R. H. Williams, T. G. Kreutz, X. Guo, Supporting information for making Fischer-Tropsch fuels and
electricity from coal and biomass: Performance and cost analysis, Energy & Fuels 25 (1). doi:10.1021/ef101184e.
75
P. Chiesa, S. Consonni, T. Kreutz, R. Williams, Co-production of hydrogen, electricity and CO 2 from coal with
commercially ready technology. Part A: Performance and emissions, International Journal of Hydrogen Energy 30 (7)
(2005) 747–767. doi:10.1016/j.ijhydene.2004.08.002.
76
A. Glassman, Users manual for updated computer code for axial-flow compressor conceptual design, Tech. rep.,
University of Toledo, Toledo, Ohio (1992).
Table 12: Properties of the biorefinery feedstocks used in this work.

Corn Wheat straw Forest


residues77
Proximate analysis, wt%, d.b.*
Fixed carbon 18.8478 1879 25.3
Volatile matter 70.89a 74.89a 70.8
Ash content 1.27a 7.1a 3.9
Ultimate analysis, wt%, d.b.
Ash 1.27a 7.1a 3.9
C 44.4480 45.8a 53.2
H 6.22a 5.96a 5.5
N 0 0.16a 0.3
S 0 0.45a 0.04
O (difference) 49.34a 40.13a 37.06
Other properties
Composition analysis wt% d.b* Not needed for
thermochemical
process
calculations
Starch 72.081
Hemicellulose/ totally 26.582
Cellulose 10.0a 37.8a
Protein 9.5a 4.3a
Oil 4.5a
Sugars 2.0a
Lignin 17.5a
HHV, MJ/kg 16.687 18.4988 20.67
Moisture (in to process), wt% 9 11.1 15
*wt% d.b. = weight percent dry basis.l
a) same source as above

77
Wilen C, Moilanen A, Kurkela E. Biomass feedstock analyses. VTT Publications 282, (VTT, 1996).
78
Phyllis 2 - ECN Phyllis classification, 2020, https://phyllis.nl/ corn shelled (#1973), accessed 31.08.2020
79
Phyllis 2 - ECN Phyllis classification, 2020, https://phyllis.nl/ wheat straw (Danish) (#1302), accessed 31.08.2020
80
https://phyllis.nl/Browse/Standard/ECN-Phyllis#corn, corn strach #2793 , accessed 31.08.2020
81
Andrew McAloon, Frank Taylor, and Winnie Yee, Determining the Cost of Producing Ethanol from Corn Starch and
Lignocellulosic Feedstocks, U.S. Department of Agriculture,2000
82
Rob Bakker, Wolter Elbersen, Ronald Poppens, Jan Peter Lesschen, Rice straw and Wheat straw Potential feedstocks
for the Biobased Economy , 2013
https://english.rvo.nl/sites/default/files/2013/12/Straw%20report%20AgNL%20June%202013.pdf
Annex II:
Block diagrams for examined process configurations with
simulated stream data
Configuration: ETOH-CCS

Stream 1 2 3 4 5 6
p (bar) 1 1 1 150 1 1
T (°C) 25 25 25 25 25 32
ṁ (kg/s) 7.0 2.1 2.2 2.0 21 2.1
ṅ (kmol/s)
LHV (MJ/kg) 16.4 26.9
Massfractions
Biomass 0.85
CO2 1 1
ETOH 0.995 0.1
H2O 0.15 0.005 0.1 0.9
DDGS 0.9
Configuration: CE-CCS

Stream 1 2 3 4
p (bar) 1 1 150 1
T (°C) 25 25 25 32
ṁ (kg/s) 6.4 0.9 0.9 0.9
ṅ (kmol/s)
LHV (MJ/kg) 15.0 26.9
Massfractions
Biomass
CO2 1 1
ETOH 0.995
H2O 0.15 0.005
Configuration: CE-CCS-MAX

Stream 1 2 3 4 5 6
p (bar) 1 1 150 1 1 1
T (°C) 25 25 25 120 32 40
ṁ (kg/s) 6.4 0.9 6.7 0.6 0.9 5.8
ṅ (kmol/s)
LHV (MJ/kg) 15 26.9
Massfractions
Biomass 0.85
CO2 1 1 <0.15 1
ETOH 0.995
H2O 0.15 0.005
Configuration: PO-CCS

Stream 1 2 3 4
p (bar) 1 1 1 150
T (°C) 25 30 120 25
ṁ (kg/s) 2.8 0.9 0.1 1.0
ṅ (kmol/s)
LHV (MJ/kg) 17.3
Massfractions
Biomass 0.5
CO2 0.5 <0.15 1
ETOH
H2O 0.25
Organics 0.75
Configuration: FTL-CCS

Stream 1 2 3 4 5 6 7
T (°C) 25 880 957 35 200 40 25
p (bar) 4 4 3 26 25 1 150
ṁ (kg/s) 1000 1927 2169 1711 926 199 1083
ṅ (kmol/s) 85 106 81 71 1 25
LHV (MJ/kg) 19.6 8.5 6.7 8.3 22.3 44.0 0.0
Molefractions
CO 0.214 0.234 0.218 0.291
H2 0.242 0.283 0.457 0.574
CO2 0.199 0.169 0.309 0.027 1.000
CH4 0.054 0.002 0.003 0.055
C2H4 0.007
C2H6 0.002 0.005
C6H6 0.002
C10H8 0.001
NH3 0.002
H2O 0.268 0.302 0.002 0.000
N2 0.009 0.008 0.011 0.041
H2S 0.00014 0.00011 0.00015
COS 0.00001 0.00000 0.00000
C5+ 1
Configuration: FTL-CCS-MAX

Stream 1 2 3 4 5 6 7
T (°C) 25 880 957 35 200 40 25
p (bar) 4 4 3 26 25 1 150
ṁ (kg/s) 1000 1927 2169 1711 926 199 1351
ṅ (kmol/s) 85 106 81 71 1 31
LHV (MJ/kg) 19.6 8.5 6.7 8.3 22.3 44.0 0.0
Molefractions
CO 0.214 0.234 0.218 0.291
H2 0.242 0.283 0.457 0.574
CO2 0.199 0.169 0.309 0.027 1.000
CH4 0.054 0.002 0.003 0.055
C2H4 0.007
C2H6 0.002 0.005
C6H6 0.002
C10H8 0.001
NH3 0.002
H2O 0.268 0.302 0.002 0.000
N2 0.009 0.008 0.011 0.041
H2S 0.00014 0.00011 0.00015
COS 0.00001 0.00000 0.00000
C5+ 1
Configuration: H2-CCS

Stream 1 2 3 4 5 6 7 8
T (°C) 25 880 957 35 40 35 40 25
p (bar) 4 4 3 21 20 30 1 150
ṁ (kg/s) 1000 1926 2168 2008 198 93 105 1805
ṅ (kmol/s) 0 85 106 98 57 46 10 41
LHV (MJ/kg) 19.6 8.5 6.7 6.8 68.3 120.0 22.6 0.0
Molefractions
CO 0.214 0.234 0.013 0.023 0.125
H2 0.242 0.283 0.548 0.947 1.000 0.716
CO2 0.199 0.169 0.424 0.010 0.054 1.000
CH4 0.054 0.002 0.002 0.004 0.022
C2H4 0.007
C2H6 0.002
C6H6 0.002
C10H8 0.001
NH3 0.002
H2O 0.267 0.301 0.002
N2 0.009 0.008 0.009 0.015 0.083
H2S 0.00014 0.00011 0.00015
COS 0.00001 0.00000 0.00000
Configuration: H2-CCS-MAX

Stream 1 2 3 4 5 6 7 8
T (°C) 25 880 957 35 40 35 40 25
p (bar) 4 4 3 21 20 30 1 150
ṁ (kg/s) 1000 1926 2168 2008 198 93 105 1937
ṅ (kmol/s) 0 85 106 98 57 46 10 44
LHV (MJ/kg) 19.6 8.5 6.7 6.8 68.3 120.0 22.6 0.0
Molefractions
CO 0.214 0.234 0.013 0.023 0.125
H2 0.242 0.283 0.548 0.947 1.000 0.716
CO2 0.199 0.169 0.424 0.010 0.054 1.000
CH4 0.054 0.002 0.002 0.004 0.022
C2H4 0.007
C2H6 0.002
C6H6 0.002
C10H8 0.001
NH3 0.002
H2O 0.267 0.301 0.002
N2 0.009 0.008 0.009 0.015 0.083
H2S 0.00014 0.00011 0.00015
COS 0.00001 0.00000 0.00000
IEA Greenhouse Gas R&D Programme
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Cheltenham, Glos. GL51 6SH, UK

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