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Energy Procedia 4 (2011) 1043–1050 Procedia
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GHGT-10

Using the Second Law of Thermodynamic to improve CO2 capture

systems
Yolanda Lara, Ana Martínez, Pilar Lisbona, Irene Bolea, Ana González, Luis M. Romeo*1
Centre of Research for Energy Resources and Consumption (CIRCE), Thermal Division , Mariano Esquillor Gómez 15, Zaragoza 50018, Spain

Elsevier use only: Received date here; revised date here; accepted date here

Abstract

Among the main challenges of Carbon Capture and Storage (CCS) technologies, the reduction of energy penalties associated
with the capture process and the integration of the new process in the design of a complex system - original power plant and
capture facility - are major issues. Traditionally, the Second Law of Thermodynamics is an essential tool for process optimization
through the application of exergy and exergy destruction (irreversibility) concepts. An exergy analysis provides a guide for
identifying those systems and equipments with larger irreversibility. Modifications in the design of these systems may lead to
reduction of thermodynamic inefficiencies in CO2 capture facilities, improving their performance and reducing costs. In this
work, some examples of the application of the Second Law of Thermodynamics are presented for postcombustion, oxyfuel
combustion and precombustion CO2 capture technologies. The main target is to identify the equipment with larger
irreversibilities and to propose items for future optimization.

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© 2011 Elsevier
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Open access under CC BY-NC-ND license.

Keywords: CO2 capture systems; exergy analysis; irreversibility; optimization; energetic eficiency

1. Introduction

It is accepted that CCS will play an important role in the reduction of greenhouse gasses emissions in a medium-
long term. Some of the main challenges are the reduction of energy penalties associated with the capture process and
the integration of the new facility in the design of a complex system which includes the original power plant and the
new process. A tool for optimizing the energy consumption is the utilization of the Second Law of Thermodynamics
through the exergy and exergy destruction concepts. As exergy is the maximum theoretical useful work from an
energy carrier, the loss of exergy means loss of potential work and system inefficiency.
The information given by the exergy assessment is a guide to reduce the thermodynamic inefficiencies of CO2
capture systems and to improve their performance. Moreover, less exergy destruction and lower losses associated
with the integrated system (CO2 capture and power plant) corresponds to a higher yield of the overall system and a
minimization of CO2 capture cost. Due to the novelty of CCS, there is a lack of information and literature related to
the exergy analysis of these systems. Nevertheless, recent research has focused on the use of exergy analysis for the

Corresponding author. Tel.: +34-976-762-570; fax: +34-976-732-078.
E-mail address: luismi@unizar.es

doi:10.1016/j.egypro.2011.01.153
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identification of equipment with larger irreversibility and has proposed items for optimization [1-9]. The target of
this work is to show the results of the exergetic analysis of six different CO2 capture options and to identify the
weaknesses of any of these schemes to reduce inefficiencies, energetic penalties, and hence, the operational cost of
these systems.

2. Assumptions and simulations

Six CO2 capture processes are simulated and their results compared. The schemes of every studied systems are
presented in Figure 1, there are two post-combustion processes (a and c), one based on oxy-fuel combustion (b) and
the other three pre-combustion systems (d, e and f). All of them have a thermal input of 100 MWth and make use of
the same fuel (coal; C 0.72; H2 0.05; N2 0.015; O2 0.075; ash 0.14; dry basis, LHV 25 MJ/kg). The chosen reference
case is a traditional power plant with a gross efficiency of 41% (specific CO2 emissions 851 kg CO2/MWh). The
volumetric concentration of CO2 in flue gases is 14.2%v. The boilers in the post-combustion and oxy-fuel systems
are also simulated with these specifications.
Among the post-combustion processes assessed in this work one is based on chemical absorption.
Monoethanolamine solvent (MEA) is considered as absorbent, with a concentration of 30%w. Flue gases enter the
system at 55 ºC pollutants-free. The capture efficiency is set on 94%. The main drawback of this option is the high
amount of thermal energy required for solvent regeneration. An average value of 3.5GJ/tCO2 is taken, thus more
than 1.8 t of steam is needed per tCO2 captured. This leads to an important power plant efficiency reduction, linked
to steam bleeding from the low/medium pressure steam turbine. Some integration possibilities are studied in the
literature to overcome this penalty [10-13]. Concentrated CO2 stream from the stripper column is conducted to the
compression train at 106 ºC and atmospheric pressure. Overall scheme is showed in Figure 1a.
Carbonation-calcination looping cycles, Figure 1c, are considered a promising option since no flue gas pre-
treatment is required and energy penalties may be reduced by process integration [14-16]. Inputs for the capture
system are the flue gases leaving the boiler, the oxygen coming from the ASU and the coal for oxyfuel combustion.
A CO2 capture efficiency of 94% in carbonator is assumed, and, due to the exothermic carbonation reaction, a
quantity of energy can be recovered in carbonator. For the calcination, an important amount of energy is required
[17]. This heat requirement is assumed to be around 46% of the energy provided to the whole system. This energy is
supplied by oxycombustion of coal, with an oxygen excess of 2%. Carbon dioxide leaves the capture system at 925
ºC, and is cooled down to 150 ºC before the conditioning system prior to CO2 compression.
A simplified process flow scheme of an oxy combustion power plant, Figure 1b, consists of an air separation unit
(ASU), a power plant with O2 blown combustion, and a CO2 treatment unit. ASU is based on a cryogenic distillation
process, the only commercially available technology today to produce large quantities of O2 economically and at
high purity, in the range of 85-98% O2. The inlet air flow is considered according to the necessary oxygen quantity
for the oxy combustion process in the boiler. The main energy consumption in the process corresponds to
compression work and it is assumed to be 227.6 kWh/tO2 [18]. Increasing oxygen purity increases the power
consumption as well as capital cost, in this sense 90 % is considered the optimum oxygen purity. After the ASU a
simplified oxyfuel combustion boiler is modeled [19-20]. The steam power cycle is considered as any conventional
coal-fired steam power plant. The oxygen flow is introduced into the boiler together with the recycled CO2. After
the combustion the CO2 flow is cooled down and directed to the compression train.
CO2 capture in precombustion processes always presents an initial step to convert the fuel into a mixture of
hydrogen, light hydrocarbons and other products. For solid fuels, gasification is the thermal treatment applied to
obtain this mixture. In this work, steam and pure oxygen are fed into the reactor as gasification agents to avoid the
dilution with nitrogen of the generated CO2 stream. An ASU will be also required to produce O2. The reactions
considered in the semi-equilibrium model are Bouduard, water-gas shift, methanation and methane steam reforming.
Steam to carbon ratio (S/C) and oxygen to carbon ratio (O/C) introduced in the reactor are around 0.65 and 0.40
respectively, the gasifier operates at 26 bar and 1200 ºC. A shift reactor is required to maximize the hydrogen yield.
It is fed with the syngas produced in the gasifier once it is cooled down to 400 ºC [21-24]. After shift reaction, the
capture process to separate CO2 must be implemented. Several separation technologies such as adsorption,
absorption and membranes, can be applied in precombustion processes.
Adsorption may avoid energy consumption associated with syngas cooling and subsequent heating, since this
separation process can be carried out at high temperatures. In this context, temperature swing adsorption (TSA)
 Y. Lara et al. / Energy Procedia 4 (2011) 1043–1050 1045
Lara Y. et al./ Energy Procedia 00 (2010) 000–000 3

represents an important alternative to reduce energy penalties. However, vacuum pressure swing adsorption (VPSA)
offers simplicity, lower capital cost and less cycle time and sorbent requirement [29]. Therefore, a VPSA process is
a) Amine scrubbing b) Oxyfuel

flue
gases N2 B1
B1 w/oCO2 B2
air air O2
COMPRESSION
ASU BOILER CO2
BOILER AMINES CO2 COMPRESSION
CO2 W
fuel flue fuel CO2
gases
water steam reheat water steam reheat W B2
water
B7 water W B3

c) Ca looping d) Pre Adsorption

B4
B2 H2
ADSORPTION COMPRESSION
CO2 CO2
flue rich CO2
Gases
gases
B3
w/oCO2 W B5
water
air
CARBONATION B8
BOILER COMPRESSION SHIFT
flue CALCINATION CO2 CO2 B3
fuel gases

water steam reheat B2

fuel O2 B1 water W B4
N2 syngas

air O2
air
ASU ASU GASIFIER B1
N2 W
W

fuel B7

e) Pre Membranes f) Pre Absorption

B5
B4 H2
H2 ABSORPTION COMPRESSION
MEMBRANE COMPRESSION CO2
CO2 Gases
CO2 CO2
rich CO2 WSelexol
Gases
B4 W B6
W B5 water
water

B8
SHIFT
B3 B8
SHIFT
B3

B2
B2
N2 syngas
N2 syngas
air O2
ASU GASIFIER air O2
B1
W ASU GASIFIER B1
W
fuel B7
fuel B7

Figure 1 CO2 capture system considered in the simulations

1046 Y. Lara et al. / Energy Procedia 4 (2011) 1043–1050
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modelled based on the results obtained in [29] for the Hydrocalcite (HTC) sorbent. The process, Figure 1d, takes
place at 400 ºC and syngas feed pressure, but CO2 is released at atmospheric pressure. It is assumed a CO2 recovery
of 94.8% with 97.2% purity. An energy consumption of 354.2 kJ/kg CO2 is considered.
Solvent regeneration in absorption processes is possible by pressure reduction, usually through flash stages,
which means low energy stripping requirements. To model the absorption process, Figure 1e, gas entering the
process is considered to be at 24 bar, and it is cooled down to 40̶C for better absorption tower operation. A capture
efficiency of 85% is assumed as the optimum [26]. The overall energy requirements of the plant are estimated to be
120 kWe per CO2 mass flow unit [27, 28].
Metallic and porous inorganic membranes may also operate at high temperatures reducing energy penalties [30].
Moreover, hydrogen selective membranes provide a high temperature CO2 stream reducing compression
requirements related to transport and storage. Microporous inorganic membranes present an important potential in
terms of hydrogen flux and selectivity [31]. A 2 mm thick MFI zeolite membrane is modelled based on [31], Figure
1f. Its permeance is 4.2 m3(STP)m/m2sbar and its separation factor is 18. It is assumed to have a 100% separation
efficiency.
After the CO2 capture processes under study, a conditioning system for CO2 transport is required. Typical energy
requirements of these systems are 90-120 kWh/tonne CO2 [32]. For the CO2 compression train considered in this
work, 101.2 kWh/tonne CO2 power consumption is assumed. The net work required by compressors can be reduced
by means of multistage intercooling. An amount of 136 kWh/tonne CO2, which is low quality heat, must be
dissipated in cooling equipment or integrated within the system [12, 33]. In most cases, the gas leaving the system is
a mixture of CO2/H2O, so a previous drying stage is included. CO2 enters the first compressor at 30ºC, 1 bar.
Compression up to 36bar is achieved by a three-stage process, compressors with 3.3 pressure ratio and 80%
isentropic efficiency, with an additional compression stage to make CO2 stream pressure reach 120 bar. Only one
compression stage with 4.2 pressure ratio is needed after the capture system using membranes, since they operate at
very high pressure. Final conditions of CO2 are the same for the six configurations, 120 bar and 60ºC.

3. Results

Energetic and exergetic balances of the streams illustrated in Figure 1 are calculated. Main results are presented
on Table 1. Three options, amine scrubbing, oxyfuel combustion and calcium looping cycle, use a boiler to produce
live steam (540 ºC-190bar/540 ºC-35 bar) with an exergetic efficiency of 39.95%. The product of the precombustion
technologies is a hydrogen stream at 400 ºC and a variable pressure and temperature depending on the option
simulated.
Equation 1 shows the definition of exergetic efficiency considered for calculations. It is obvious that, depending
on the criteria chosen for the selection of fuel and products, results could change completely. Moreover, different
schemes and streams could make difficult any comparison between them. In general, fuel in the Equation 1 is the
main fuel used in the boiler and products are the produced steam (in post and oxy technologies), or hydrogen stream
(in precombustion technologies) and waste energy coming from CO2 capture system. If a flux of heat is needed (i.e.
stripper requirements), it is deducted from the products as this energy have to come from other points of the
installation. Otherwise, an additional boiler (with typical low exergetic efficiency) has to be included and will
reduce the exergetic efficiency results. The same criterion is used for power requirements.
§ live_steam ·
product¨¨ ¸¸  waste_energy  heat  work required
PRODUCTS © hydrogen ¹ (1)
 ex
FUEL fuel
One of the important conclusions from the results is that exergy destruction in the combustion boiler is larger
than in any other CO2 capture equipment (52.34% of the 121.7 MW exergy input). Hence, the focus should be in the
reduction of this quantity because it will bring about overall system improvements. This was an expected result.
In regard to CO2 capture systems, in amine scrubbing, the heat exchanger that reduces flue gases temperature
from 150 ºC to 55 ºC before the absorber has an important exergy destruction of 3.5 MW. To minimize this number,
solvents with higher absorption temperature should be developed. In the absorption process, the exergy destruction
is about 5.9 MW and exergy losses in the flue gases without CO2 is 2.5 MW. 8.9 MW of exergy are necessary to
regenerate the solvent. Flue gases have to be conditioned and cooled before the CO2 compression. The exergy
 Y. Lara et al. / Energy Procedia 4 (2011) 1043–1050 1047
Lara Y. et al./ Energy Procedia 00 (2010) 000–000 5

destruction in the compression is low, 0.3 MW, due to an exergy recovery as heat of 0.7 MW. Although this process
is intensive in power requirements, the exergetic efficiency is high and there is no room for improvements (if heat is
recovered from intercooling compression). The exergetic content of compressed CO2 is 6.7 MW. To summarize,
there are 9.7 MW of exergetic losses caused by heat exchangers (3.5 MW, 36%), amine scrubbing process (5.9 MW,
61%) and CO2 compression (0.3 MW, 3%). The overall exergetic efficiency is 37.49% or 31.99% depending on
whether the compressed CO2 is considered or not a product.
The values in the case of the calcium cycle (carbonation-calcination) changes completely. One of the novelties is
the presence of an ASU to supply O2 for the CaCO3 calcination under oxyfuel conditions. Exergetic requirements
are important, 6.2 MWe, and also the exergetic destruction, 4.1 MW. For this reason, efforts should focus on the
improvement of O2 production. The capture process in this case is also different. More fuel is needed (coal, natural
gas) to calcinate the CaCO3, and the energy input for the whole system increases up to 104.3 MW. As a result, there
are several exergetic streams as heat that should be integrated in a new steam cycle. These are 14 MW coming from
carbonator exothermic reaction at constant temperature (650 ºC), and the exergetic content of flue gases and CO2
stream. 27 MW of flue gases exergy leave calcium cycle. There are 11.4 MW of recoverable exergy, 7.2 MW of
exergetic losses (as flue gases in the stack) and 8.3 of exergy destruction. In the CO2 stream (29.7 MW), the
recoverable exergy is 13.1 MW and the exergy of CO2 before compression is 8.5 MW. Exergy destruction in this
heat exchanger is comparable to previous one, 8.1 MW. Exergy destruction in compression, 0.5 MW, is higher than
in the case of amine scrubbing due to the CO2 stream is nearly doubled. To summarize, the exergy destruction is
61.1 MW, 16.4 MW due to heat exchangers (27.8%), 44.2 MW (72.3%) due to the capture process (Ca-looping) and
0.5 MW due to CO2 compression (0.9%). There are additional requirements, 6.2 MW of power for ASU and 104.3
MW of fuel for the calcium cycle. There are also new recoverable exergy as heat, 38.6 MW from carbonator, flue
gases at 650 ºC and CO2 at 925 ºC. It causes that overall exergetic efficiency is 39.33% or 33.45% depending on
whether the CO2 streams is included or not in the definition. It is nearly two efficiency points higher than amine
scrubbing system efficiency, mainly due to the exergetic recovery from the large amount of energy released in the
capture system.

Table 1 Exergy analysis results (MW)

Amines Ca looping Oxyfuel Pre Adsorption Pre Membranes Pre Absorption
Fuel 121.7 121.7+104.3 121.7 121.7 121.7 121.7
Steam or H2 48.7 48.7 48.7 72.0 71.3 69.0
B1 0.9 14.0 1.2 9.3 9.3 9.3
Products (+)

Work Heat Waste energy

B2 0.9 11.4 0.7 12.1 12.1 12.1

B3 0.7 13.1 - 3.8 3.8 3.8
B4 - 1.5 - 1.3 7.4 8.6
B5 - - - 0.7 0.3 0.04
B6 - - - - - 0.6
B7 8.9 - - 4.2 4.2 4.2
Products (-)

B8 - - - 6.6 6.6 6.6

WASU - 6.2 8.5 2.2 2.2 2.2
Wcomp 3.5 6.8 3.5 3.1 1.0 2.8
WSelexol - - - - - 1.0
CO2 stream 6.7 13.3 6.9 6.1 6.0 5.4
ex (%) 37.49-31.99 39.33-33.45 37.33-31.66 73.23-68.23 79.23-74.1 75.62-71.20
Exergy destruction

Boiler 63.8 63.8 64.3 - - -

Gasifier - - - 13.2 13.2 13.2
Shift reactor - - - 4.8 4.8 4.8
ASU - 4.1 5.7 0.9 0.9 0.9
CO2 separation 5.9 44.2 - 4.3 3.9 3.3
Heat exchangers 3.5 16.4 4.5 1.9 1.5 0.06
CO2 compression 0.3 0.5 0.2 0.2 0.1 0.3
Exergy losses 2.5 7.2 1.5 6.9 0.5 5.3
1048 Y. Lara et al. / Energy Procedia 4 (2011) 1043–1050
6 Author name / Energy Procedia 00 (2010) 000–000

Oxyfuel combustion also has an important power consumption in the ASU, 8.5 MW, higher than calcium cycle
due to higher fuel input in the boiler. As explained above, exergy destruction in ASU, 5.7 MW, is large and, in this
case, is an essential issue to improve. Boiler exergetic destruction is similar to the exergy destruction assumed in the
reference boiler, it only increases 0.5 MW. In this case, there is no flue gas conditioning previous to the CO2
separation process (as amine scrubbing). Thus, there is no exergetic destruction in heat exchangers. Flue gas
conditioning prior to CO2 compression has more exergetic losses than amine scrubbing due to water condensation, it
amounts to 4.5 MW. Summing up, there are 10.9 MW of exergetic losses, 52.3% from ASU, 41.3% from heat
exchangers, 4.6% from oxy-boiler and 1.8% from the CO2 compression. Overall exergetic efficiency is similar to
amine scrubbing efficiency, 37.33% or 31.66% depending on the choice of CO2 definition.
In precombustion technologies the efficiency varies since the product is neither heat nor steam production but
hydrogen production. There are several common processes (ASU, gasifier and shift reactor) and the differences lie
in the selected CO2 separating technology. In these cases, ASU requirements are 2.2 MW and exergetic destruction
amounts to 0.9 MW. Gasifier demands 4.2 MW of exergy as steam and releases 9.3 MW of exergy as heat. Its
exergy destruction is 13.2 MW (10.8% of input as fuel). Shift reaction is exergetically more efficient due to
destruction is 4.8 MW, and there are two heat streams that totalize 15.9 MW. All these processes have an exergetic
destruction of 18.9 MW mainly due to gasifier (69.8%). Hence, the attention has to be focused in this equipment to
improve the overall system.
There are 4.3 MW of exergetic destruction in the adsorption process, and H2 stream has an exergetic content of
72.0 MW. Flue gases exergy losses are 6.9 MW and CO2 rich-stream has to be cooled down, recovering 1.3 MW of
exergy but destroying 1.9 MW. CO2 compression is exergetically efficient and losses amounts to 0.2 MW, with
similar power requirements as in previous options. Summing up, exergetic losses and destruction are 13.2 MW in
the gasifier, flue gas exergy losses 6.9 MW, shift reactor 4.8 MW, adsorption separation 4.3 MW, heat exchangers
1.9 MW, ASU 0.9 MW and compression 0.2 MW. Overall efficiency is 73.23% and 68.23% depending on the
choice of CO2 definition.
Membrane separation produces a high exergy CO2-rich pressurized stream with exergetic destruction slightly
lower than adsorption, 3.9 MW. Also the product has lower exergy, 71.3 MW. Heat exchanger before CO2
compression destroys 1.5 MW while compression only 0.1 MW due to the higher pressure of CO2 at membrane
output. Compression energetic and exergetic requirements are lower, 1.0 MW minimizing losses. For this system,
the overall exergetic efficiency is 79.23% or 74.30%. This is the higher efficiency achieved in the precombustion
capture systems.
The absorption process is simulated with Selexol, so the power requirements amount to 1.0 MW. Exergy
destruction is similar to previous precombustion options, 3.3 MW. Exergetic losses are 5.3 MW and the product has
lower exergetic content, 69 MW. The exergy destruction in compression process is similar to that in the other
systems, 0.3 MW with a power consumption of 2.8 MW. The exergetic content of the H2 that leaves the system is
lower than in the other two precombustion systems since its temperature is 40 ºC instead of 400 ºC.

4. Conclusions

Exergy analysis is a guide for reducing thermodynamic inefficiencies. Particularly in CO2 capture systems it
could be useful to detect, study and achieve proper integration and, hence, minimization of additional energetic
requirements which finally reduce the operational capture cost. The estimation of exergy destruction and losses for
integrated systems (CO2 capture + power plant) could support detailed analysis and efficiency improvements.
The exergetic analysis of different CO2 capture technologies has shown that the main cause of exergetic
inefficiency is the classical boiler, which is out of the capture system. Therefore, the classical analysis of power
plant improvements continues being an option to improve the performance of the whole system. Although energetic
requirements for CO2 compression are important, the exergetic destruction is very low in all cases. Hence, taking
advantage of compression intercooling energy there are no scope for improvements. For amine scrubbing the
development of solvents with higher operational temperature (increasing absorption temperature) and lower
regeneration temperature will reduce the exergetic destruction associated with heat exchanger that is the most
important one in this case. For oxyfuel option the improvement should be focused on ASU performance because
most of exergy destruction occurs in this system. Calcium looping analysis has revealed an excellent overall
 Y. Lara et al. / Energy Procedia 4 (2011) 1043–1050 1049
Lara Y. et al./ Energy Procedia 00 (2010) 000–000 7

efficiency due to the integration of waste heats from the capture system. In this case the system is enlarged with
additional fuel for CO2 capture but it entails still good efficiency. In the case of precombustion technologies the
system improvement should be focused on gasifier and shift reactor because most of the exergy destruction is
located in these equipments, specifically it would be desirable to reduce the changes of temperature in the main
stream. The efficiency of the CO2/H2 separation is another topic of interest since it affects directly the system
improvement. In any case, all the studied options have showed very good exergetic efficiency results.

Acknowledgement

The work described in this paper was supported by the R+D Spanish National Program from Ministerio de
Ciencia e Innovación, MICINN (Spanish Ministry of Science and Innovation) under project ENE2009-08246.
Financial support for A. Martínez during her Ph.D. studies was provided by the FPU programme of the Spanish
Ministry of Science and Innovation.

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