Journal of Cleaner Production 274 (2020) 122871

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Journal of Cleaner Production

journal homepage: www.elsevier.com/locate/jclepro

Comprehensive 3E analysis and multi-objective optimization of a

novel process for CO2 capture and separation process from syngas
Yinglong Wang a, b, Xiaobin Liu a, Hongru Zhang a, Yigang Liu a, Peizhe Cui a, *,
Zhaoyou Zhu a, b, Yixin Ma c, Jun Gao c
a
College of Chemical Engineering, Qingdao University of Science and Technology, 53 Zhengzhou Road, Qingdao, 266042, PR China
b
Shandong Collaborative Innovation Center of Eco-Chemical Engineering, Qingdao University of Science and Technology, Qingdao, 266042, PR China
c
College of Chemical and Environmental Engineering, Shandong University of Science and Technology, 579 Qianwangang Road, Qingdao, 266590, PR China

a r t i c l e i n f o a b s t r a c t

Article history: The traditional synthesis gas (syngas) production process in the coal chemical field encounters the
Received 7 November 2019 problems of high cold energy consumption and difficulty in effectively capturing CO2. This limits the
Received in revised form clean production and sustainable development of coal chemical industry. To solve this problem, this
5 June 2020
paper proposes a novel process for capturing and separating CO2 from syngas using [bmim][Tf2N]. This
Accepted 13 June 2020
Available online 18 July 2020
process can effectively reduce the cold energy consumption and improve the CO2 capture efficiency,
which will help relieve the global concerns over CO2 emissions. Energy, economic, and environmental
Handling editor: Prof. Jiri Jaromir Kleme
s analyses of the process were conducted based on accurate modeling and simulation results. To balance
the conflict between the economic and environmental performances, the non-dominated sorting genetic
Keywords: algorithm II method was used for the multi-objective optimization of the process. The CO2 escape flow
CO2 capture and separation rate and total annual cost were the objective functions of the multi-objective optimization scheme and
Energy had values that were 5.9% and 1.5% higher than their minimum values, respectively. Moreover, the multi-
Economic objective optimization scheme for this process was compared with the Rectisol process and CO2 capture
Environmental
from syngas using [emim][Tf2N]. This work provided new ideas for clean production of coal chemical
Multi-objective optimization
industry, and also provided reference for the green sustainable development of relevant work.
© 2020 Elsevier Ltd. All rights reserved.

1. Introduction
Continuous industrialization has increased the concentration of
CO2 in the atmosphere. By 2017, the global atmospheric CO2 con-
centration had reached 408 ppm (Kumar et al., 2018). This is 45.7%
more than CO2 concentration in the pre-industrial period
(280 ppm) (Cao and Caldeira, 2008). If the CO2 concentration
continues to increase in line with current trends, it will exceed
550 ppm by 2100 (d’Amore et al., 2019). Thus, alleviating concerns
over CO2 emissions has gained worldwide attention.
Coal combustion is the main source of CO2 emissions (Davis
et al., 2010). It provides 29% of the world’s energy but contributes
to 44% of the world’s CO2 emissions (Li et al., 2016). Thus, reducing
CO2 emissions from coal-based industries is extremely important.
CO2 capture and storage, as a widely recognized and promising
greenhouse gas (GHG) emission reduction method, has attracted
* Corresponding author.
E-mail address: cpzmagic@qust.edu.cn (P. Cui).
extensive attention from researchers (Xiang et al., 2014). Zhou et al.
(2018) combined coal to liquid technology with CO2 capture and
storage and investigated the performances of five different carbon
capture and storage processes. Tola and Pettinau (2014) studied
three different technologies for coal-fired power generation with or
without CO2 utilization. The results showed that an ultra-
supercritical power plant with CO2 capture has higher energy
penalties, and an integrated gasification cycle combined with CO2
capture and storage is more efficient than the corresponding CO2-
free ultra-supercritical method. In the process of coal-to-natural
gas production, Liu et al. (2015) studied a process for H2S removal
and CO2 capture from syngas using methanol as a solvent. This
process was found to have better heat integration. However, the
process consumed a large amount of cold energy, which led to a
large amount of indirect CO2 emissions.
As a new type of green solvent, an ionic liquid has been used to
capture CO2 in recent years (Zhao and Baker, 2013). Wang et al.
(2018) designed a series of ionic liquids for CO2 capture using a
systematic computer-aided design method. They used the COSMO-

https://doi.org/10.1016/j.jclepro.2020.122871
0959-6526/© 2020 Elsevier Ltd. All rights reserved.
2 Y. Wang et al. / Journal of Cleaner Production 274 (2020) 122871

Nomenclature cw cooling water

DEH dehydration column
C cost ($) DIS distillation column
c unit energy price ($/GJ) E equipment
F escape flow rate (kmol/h) ele electricity
f correction factor env environment
h specific enthalpy (kJ/kg) FLA flash tank
M the cost exponent M materials
m_ mass flow rate (kg/h) op operational
N the service life of equipment P pressure (bar)
Q_ heat transfer rate (kW) PUM pump
S equipment size r revised
t time (h) T temperature (
C)
W_ power (kW) t time (h)
Z investment cost ($) tot total annual
1, 2, 3 state points
Greek symbols
a capital recovery factor Abbreviations
4 maintenance cost factor CBTL coal biomass to liquids
h efficiencies isentropic CEPCI the chemical economic plant cost index
COSMO-SAC the conductor-like screening model for the
Subscripts segment activity coefficient
ABS absorption column CTL coal to liquids
B base capital NSGA-II non-dominated sort genetic algorithm-II
COM compressor TOPSIS technique for order preference by similarity to an
COO cooler ideal solution
ce cold energy 3E energy, economic and environmental

SAC model to study the effects of the functional groups and alkyl
chain lengths of ionic liquids on the removal of CO2 from flue gas.
Chau et al. (2016) developed a process that used [bmim][DCA] to
capture the CO2 in syngas. Under the assumption of a 40% CO2
concentration and 100
C, the purity of the CO2 in CO2 rich products
can reach more than 95%. Six different ionic liquids were synthe-
sized by Yunus et al. (2019), and it was found that the ionic liquids
with the butyrate anion and [BEHA] cation had high CO2 absorption
capacities.
Much work has been done by researchers to improve the per-
formance of the CO2 capture process using an ionic liquid. Xie et al.
(2014) compared the amounts of energy consumed for CO2 ab-
sorption using different ionic liquids. The results showed that the
energy consumption for CO2 capture using [bmim][Tf2N] was the
lowest. Farahipour and Karunanithi (2014) explored the life cycle
environmental implications of CO2 capture and sequestration from
a coal-fired power plant using [bmim][Ac] as a solvent. Compared
with the 75% life cycle GHG reduction provided by the
monoethanolamine-based CO2 capture and sequestration process,
a [bmim][Ac]-based CO2 capture and sequestration process with a
90% CO2 capture efficiency reduced the life cycle GHG emissions by
only 50%. Because of the increasing environmental requirements,
the CO2 removal in a process design should be as great as possible
(Yang et al., 2018). However, it is not appropriate to continuously
sacrifice the economic performance of a process to remove more
CO2. Therefore, a method that balances economic and environ-
mental concerns is required to optimize the process.
In recent years, much attention has been given to multi-
objective optimization, which is a scheme that is used for prob-
lems with multiple objectives (Luo et al., 2019). There are many
solutions based on the differences in the natures of multi-objective
problems. Based on the Pareto optimal set theory, a stochastic
multi-objective optimization algorithm has been used to determine
the optimal trade-off set between objectives (Mirjalili et al., 2017).
For a cascade absorption refrigeration system, Cui et al. (2019)
obtained a scheme with the goal of optimizing the total cost and
exergy using multi-objective optimization. The results showed that
the total cost and exergy were 5.9% (14.8%) and 4.5% (11.0%) higher
than minimum results in the multi-objective (single objective)
optimization scheme, respectively. Jain and Sachdeva (2017) used
this method to study the performance and cost of a vapor absorp-
tion heat transformer. The results showed that the total annual cost
and total exergy destruction of multi-objective optimization were
1.0% and 0.8% higher from their minimum results, respectively.
However, for single objective optimization scheme, they were 6.1%
and 2.4% higher than their minimum results, respectively. This
point out that multi-objective optimization is more comprehensive
advantages than a single objective scheme. For CO2 capture and
separation technology, Tang and You (2017) used multi-objective
optimization to analyze the environmental and economic perfor-
mances of a municipal solid waste incineration power plant. The
results showed that the system performance of pressure/vacuum
swing adsorption and oxy-fuel combustion was better than that of
monoethanolamine absorption.
Based on the above literature investigation, it can be found that
the use of ionic liquid to capture CO2 was a scheme worthy of study,
and the application of multi-objective optimization method to
balance the performance of multiple conflicting objectives of the
process was also meaningful for the process design. This study
designed a process for capturing CO2 and H2S in gas using [bmim]
[Tf2N] at 25
C. On the basis of reasonable thermodynamic
modeling, energy, economic, and environmental (3E) analyses and
multi-objective optimization were performed. The process perfor-
mance with this design was explored in comparison with the
process based on [emim][Tf2N] and the low-temperature methanol.
 Y. Wang et al. / Journal of Cleaner Production 274 (2020) 122871
2. Process description
The ionic liquid [bmim][Tf2N] was selected as the absorbent for
this process. The reasons for its selection were given in the previous
work (Wang et al., 2019). Fig. 1 shows the CO2 capture and storage
process using the ionic liquid [bmim][Tf2N]. The process uses a
dehydration column, an absorption column, a distillation column, a
throttle, flash tanks, compressors, pumps, and heat exchangers. The
syngas and dehydrating solvent (triglycol) first enter the dehydra-
tion column. The dehydrated syngas is cooled in cooler 1 and then
enters the absorption column, where CO2 and H2S are absorbed by
the ionic liquid. The purified syngas comes out of the top of the
absorption column, and the mixed solvent is obtained from the
bottom. Then, the mixed solvent enters flash tank 1 to recover the
CO and H2 (effective gases). A mixture rich in the effective gases
leaves the top of flash tank 1 and enters the compressor, where it is
pressurized to transfer to mixer 1. The mixed solvent flows through
the multiple heat exchangers and enters flash tank 2, where the CO2
and H2S are separated. The high-purity ionic liquid solvent flows
back to the absorption column through pump 1 and the multiple
heat exchangers. The CO2 and H2S gases from the top of flash tank 2
are cooled, compressed, and passed through the heat exchanger to
form the CO2eH2S solvent, which enters the distillation column.
The H2S product is obtained at the bottom of the distillation col-
umn. The CO2 product at the top of the distillation column is
heated, compressed, and condensed, and then transported and
stored using pump 2. The CO2 in the syngas could be captured using
this process.
3. Model
Some assumptions had to be made about the process before the
3E analyses. The specific assumptions are listed below (Grossman
and Wilk, 1994).
1. All the equipment was operated in the steady state for the CO2
capture and separation process.
Fig. 1. Flowsheet of CO2 capture and storage using [bmim][Tf2N].
3
2. The changes in the kinetic energy and potential energy were
ignored.
3. The variation in the pressure drop inside the equipment and the
loss from the heat exchanger to the environment were ignored.
4. The solutions from the dehydration column, absorption column,
flash tank, and distillation column were under equilibrium
conditions.
It is necessary to provide details about the role and necessity of
each assumption.
1. The process was performed under steady-state conditions,
where only three major equilibria for the process needed to be
considered, i.e., the material balance, energy balance, and phase
balance. Without the assumption of steady-state conditions,
dynamic time variables would need to be introduced. Consid-
ering the influence of time on parameters such as the pressure,
temperature, and concentration, this would significantly in-
crease the amount of calculation needed for the process.
2. To show the energy transfer and work of the system more
clearly, the changes in the kinetic energy and potential energy of
the process were ignored. If these changes were considered, it
would be necessary to increase the loss in the kinetic and po-
tential energy conversion process, which would affect the un-
derstanding of the calculation of work done in the system.
3. Every piece of equipment has a certain heat loss to the envi-
ronment and pressure drop in actual work. However, in the
steady-state simulation, these losses were ignored to accurately
calculate the energy conversion losses. If the heat loss and
pressure drop of the equipment were considered, the energy
loss would increase.
4. On the basis of the steady state model, the solution was set to be
in the equilibrium state during the operation, to facilitate the
calculation under the equilibrium model. If this assumption
were ignored, it would be difficult to calculate the components
with the coexistence of gas and liquid phases.
4 Y. Wang et al. / Journal of Cleaner Production 274 (2020) 122871

In summary, the above assumptions were used for subsequent material are important factors that can change the equipment cost.
process analysis. Therefore, Eq. (4) (Sun and Qiu, 2006) needs to be corrected to meet
the actual production requirements. To prevent corrosion, stainless
3.1. Energy analysis steel was used in all the equipment. Eq. (5) (Kaushik and Arora,
2009) was revised and used to calculate the investment cost in
As the basis of an energy analysis, the law of the conservation of this work, and the correction factors are listed in Table 2.
energy includes the following formulasEqn 1,Eqn 2 (Zhao et al.,
2020). Zr ¼ ZE fM fP fT (5)
X
Mass balance: m_ ¼ 0 (1) where fM ¼ correction factor for construction materials.

X X X fP ¼ correction factor for design pressure

Energy balance: Q_ þ W_ þ _ ¼0
mh (2) fT ¼ correction factor for design temperature
Table 1 lists the results of applying the above equations to the
CO2 capture and separation process. The relevant calculation parameters of all components were
listed in Table 2 and the equipment cost is on the basis of 2015
(Carrasco et al., 2017). In order to make the equipment cost closer to
3.2. Economic analysis
current actual price, it was changed to the cost in 2019 by chemical
economic plant cost index (CEPCI) as shown in Eq. (6). The CEPCI of
Before a new process can be accepted by the coal chemical in-
2015 was 556.8 (Carrasco et al., 2017) and that for 2019 was 603.1
dustry, in addition to technological advancements, the economic
(Okoro and Sun, 2019).
benefits of the process should also be considered. The total annual
cost (Ctot) of a process includes the investment and maintenance
P CEPCI2019
costs ( Z) and the operational cost (Cop). It is calculated using Eq. Ze;2019 ¼ Ze;2015 (6)
(3) (Yang et al., 2020).
CEPCI2015
X The maintenance cost factor (4) was set to 1.06 (Jain and
Ctot ¼ Z þ Cop (3) Sachdeva, 2017.). The capital recovery factor (a) of the system was
calculated using the interest rate (i) and system life (N). The
detailed computational equations are shown belowEqn 7 (Moghimi
et al., 2018).
3.2.1. Investment and maintenance costs
The equipment investment cost (ZE) of a process is first calcu- ið1 þ iÞN
lated using Eq. (4) (Smith, 2016). a¼ (7)
ð1 þ iÞN  1
SE M
ZE ¼ ZB ð Þ (4) where i is 15% and N is 10 years.
SB
Therefore, the investment and maintenance costs can be
The equipment size, operating temperature, pressure, and calculated as followsEqn 8:

Table 1
Mass and energy formulas for all equipment in CO2 capture and separation process.

Component Mass equations Energy equations

Dehydration column m_ 1 þ m_ 33 ¼ m_ 2 þ m_ 3 Q_ DEH ¼ m_ 2 h2 þ m_ 3 h3  m_ 1 h1  m_ 33 h33

Absorption column m_ 5 þ m_ 32 ¼ m_ 6 þ m_ 9 Q_ ABS ¼ m_ 6 h6 þ m_ 9 h9  m_ 5 h5  m_ 32 h32
Distillation column m_ 20 ¼ m_ 21 þ m_ 22 Q_ DIS ¼ m_ 21 h21 þ m_ 22 h22  m_ 20 h20
Flash tank 1 m_ 6 ¼ m_ 7 þ m_ 11 Q_FLA1 ¼ m_ h þ m_ h  m_ h
7 7 11 11 6 6
Flash tank 2 m_ 12 ¼ m_ 13 þ m_ 27 Q_ FLA2 ¼ m_ 13 h13 þ m_ 27 h27  m_ 12 h12
Compressor 1 m_ 9 ¼ m_ 8 W _
COM1 ¼ m _ 9 ðh8  h9 Þ
Compressor 2 m_ 23 ¼ m_ 24 W _
COM2 ¼ m _ 23 ðh24  h23 Þ
Compressor 3 m_ 14 ¼ m_ 15 W _
COM3 ¼ m_ ðh  h Þ
14 15 14
Compressor 4 m_ 16 ¼ m_ 17 W_
COM4 ¼ m_ 16 ðh17  h16 Þ
Pump 1 m_ 27 ¼ m_ 28 W_
PUM1 ¼ m_ 28 h28  m_ 27 h27
Pump 2 m_ 25 ¼ m_ 26 W_
PUM2 ¼ m_ h  m_ h
26 26 25 25
Cooler 1 m_ 4 ¼ m_ 5 Q_ COO1 ¼ m_ 5 h5  m_ 4 h4
Cooler 2 m_ 29 ¼ m_ 30 Q_ COO2 ¼ m_ 30 h30  m_ 29 h29
Cooler 3 m_ 24 ¼ m_ 25 Q_ COO3 ¼ m_ 25 h25  m_ 24 h24
Cooler 4 m_ 13 ¼ m_ 14 Q_COO4 ¼ m_ h  m_ h
14 14 13 13
Mixer 1 m_ 3 þ m_ 8 ¼ m_ 4 m_ 3 h3 þ m_ 8 h8 ¼ m_ 4 h4
Mixer 2 m_ 30 ¼ m_ 31 þ m_ 32 m_ 30 h30 þ m_ 31 h31 ¼ m_ 32 h32
Throttle m_ 19 ¼ m_ 20 m_ 20 h20 ¼ m_ 19 h19
Multi heat exchanger m_ 11 ¼ m_ 12 m_ 11 h11 þ m_ 17 h17 þ m_ 28 h28 ¼ m_ 12 h12 þ m_ 18 h18 þ m_ 29 h29
m_ 17 ¼ m_ 18
m_ 28 ¼ m_ 29
Heat exchanger 1 m_ 18 ¼ m_ 19 m_ 18 h18 þ m_ 22 h22 ¼ m_ 19 h19 þ m_ 23 h23
m_ 22 ¼ m_ 23
Heat exchanger 2 m_ 9 ¼ m_ 10 m_ 9 h59 þ m_ 15 h15 ¼ m_ 10 h10 þ m_ 16 h16
m_ 15 ¼ m_ 16
 Y. Wang et al. / Journal of Cleaner Production 274 (2020) 122871 5

Table 2
Parameters of equipment capacity delivered capital cost correlations.

Equipment Measure Base size (SB) Base cost (ZB/$) M fM fP fT

Dehydration column Capacity 0.1 (m3) 4.92  103 0.53 2.1 1.5 1
Absorption column Capacity 0.1 (m3) 4.92  103 0.53 2.1 1.5 1
Distillation column Weight 8.0 (t) 6.56  104 0.89 2.1 1 1
Sieve tray Diameter 0.5 (m) 6.56  103 0.91 2.1 1.5 1
Cooler 1 Heat exchange area 80.0 (m2) 3.28  104 0.68 2.4 1.5 1
Cooler 2 Heat exchange area 80.0 (m2) 3.28  104 0.68 2.4 1.5 1
Cooler 3 Heat exchange area 80.0 (m2) 3.28  104 0.68 2.4 1.9 1
Cooler 4 Heat exchange area 80.0 (m2) 3.28  104 0.68 2.4 1 1
Multi heat exchanger Heat exchange area 80.0 (m2) 3.28  104 0.68 2.4 1.5 1
Heat exchanger 1 Heat exchange area 80.0 (m2) 3.28  104 0.68 2.4 1 1
Heat exchanger 2 Heat exchange area 80.0 (m2) 3.28  104 0.68 2.4 1.5 1
Pump 1 Power 4.0 (kW) 9.84  103 0.55 2.1 1.9 1
Pump 2 Power 4.0 (kW) 9.84  103 0.55 2.1 1.5 1
Compressor 1 Power 250.0 (kW) 9.84  104 0.46 2.1 1.5 1
Compressor 2 Power 250.0 (kW) 9.84  104 0.46 2.1 1.5 1
Compressor 3 Power 250.0 (kW) 9.84  104 0.46 2.1 1 1
Compressor 4 Power 250.0 (kW) 9.84  104 0.46 2.1 1 1
Flash tank 1 Capacity 5.0 (m3) 1.15  104 0.53 2.4 1 1
Flash tank 2 Capacity 5.0 (m3) 1.15  104 0.53 2.4 1.3 1

Shirazi, 2013).
Zr;2019 ¼ 4aZe;2019 (8)
mCO2 ¼ ltop ðWCOM þ WPUM Þ (11)

where l is the emission conversion factor of electricity from pres-

3.2.2. Operational cost sure equipment, which has a value of 0.968 kg/kW h (Sanaye and
The operational cost of the CO2 capture and separation process Shirazi, 2013).
comes from the electricity consumption, cooling water consump-
tion, and cold energy consumption. The compressors and pumps
from the absorption unit, desorption unit, and CO2 liquefaction unit 3.4. Multi-objective optimization
were the main power consumers in the CO2 capture and separation
process. The consumption of cold energy was concentrated in the Multi-objective optimization is an excellent solution for the
distillation column. The price of electricity (cele), cooling water problem of target conflict. This method can be used to optimize a
(ccw), and cold energy (cce) were 0.11 $/(kW h), 0.35 $/GJ (Chen et al., process by simultaneously considering multiple conflicting objec-
2017), and 3.33 $/GJ (Messineo and Panno, 2011), respectively. The tives under multiple constraints (Jain and Bandyopadhyay, 2019). A
annual operating time (top) was 8000 h. The formula for calculating single solution cannot meet the objectives of multiple conflicts.
the operating cost is listed belowEqn 8b. Therefore, there is no unique optimal solution for a multi-objective
problem. The solution of this problem is obtaining a solution set
cele X X X (Pareto front), where each solution corresponds to different needs.
Cop ¼ top ½ ð WCOM þ WPUM Þ þ ccw  QCOO
0:0036
X The decision maker ultimately chooses the best solution for the
þ cce  QDIS  process based on a specific design.
The objective function, decision variable, and constraint condi-
(8b)
tion are three important factors in the multi-objective optimization
The calculation formula for the total annual cost is shown process. In this study, Ctot and the CO2 escape flow rate (FCO2 ) were
belowEqn 9. two objective functions. Based on these two functions, the optimal
X scheme based on the environment and the optimal schemes based
Ctot ¼ 4a Z þ Cop (9) on the economy and multi-objective optimization scheme were
determined for the CO2 capture and separation process. The
objective functions were minimized by changing the decision var-
iables. Information about the decision variables is given in Table 3.
3.3. Environmental analysis Based on the syngas purification process regulation, the constraint
conditions of the CO2 capture and separation process are listed
To reduce the CO2 emissions and global warming, the environ- below.
mental impact has become an important indicator to evaluate a
process. CO2 emissions can be an important factor to quantify this 1. The CO2 content in the purified gas was less than 3%, and the H2S
indicator. The CO2 emissions (Zenv) determined by Eq. (10) show the content in the purified gas was less than 0.1 vppm.
social cost (Aminyavari et al., 2014):

Zenv ¼ mCO2 CCO2 (10) Table 3

Decision variables for CO2 capture and separation process and their ranges.
In Eq. (10), CCO2 is the cost of the unit CO2 emissions, which
Decision variables Range of variables
varies from 0.002 $/kg to 0.130 $/kg for different countries. In this
work, the value of CCO2 was considered to be 0.008 $/kg Pressure of absorption column 9 bar < PABS < 12 bar
(Aminyavari et al., 2014; Carlsson et al., 2016). mCO2 stands for the Pressure of flash tank 2 0.09 bar < PFLA-1 < 0.4 bar
Temperature of flash tank 2 50
C < TFLA-2 < 90
C
CO2 emission mass, which is calculated using Eq. (11) (Sanaye and
6 Y. Wang et al. / Journal of Cleaner Production 274 (2020) 122871
2. The CO2 mole fraction in the CO2 products was greater than
98.5%.
3. The effective gas recovery ratio for the purified syngas was
greater than 99.4%.
4. The total amount of sulfur in the H2S products was greater than
25%.
The optimization process adopted the non-dominated sorting
genetic algorithm II (NSGA-II) technology (Deb et al., 2000), and the
pseudo code is provided in Appendix A. The tuning parameters of
the process are given in Table 4.
4. Case study
In this work, Aspen Plus (version 8.4) was used to simulate the
ionic liquid-based CO2 capture and separation process. The physical
property method was COSMO-SAC. The heat exchangers in the
process were designed using Aspen Exchanger Design and Rating
(version 8.4). The feed composition of the syngas was taken from
the actual industrial coal gasification process of Texaco. The accu-
racies of the simulation results and physical property method were
verified in previous work (Wang et al., 2019). The detailed infor-
mation about the simulation is listed in Tables 5 and 6.
5. Results and discussions
This section discusses the interaction between the design vari-
ables and parameters of the process, as well as the trade-off be-
tween the economic and environmental performances of the
process based on multi-objective optimization employing the
NSGA-II technology, along with a comparison between the use of
[bmim][Tf2N], methanol and [emim][Tf2N] as the solvent for the
CO2 capture and separation process. The results obtained through
the process are discussed below.
5.1. Sensitivity analysis
The effects of the operating variables on the gas capture ratio,
energy consumption, and investment and maintenance costs are
first analyzed. The capture ratio is the ratio of the gas flow rate from
the top or bottom of the distillation column to that of the syngas.
The pressure of the absorption column is the main operating
parameter affecting the result of absorption using ILs. The effect of
the pressure in the absorption column on the CO2 capture ratio is
shown in Fig. 2 (a). The CO2 capture ratio increases from 0.954 to
0.965 with an increase in pressure from 9 bar to 12 bar. Fig. 2 (b)
shows the effects of the pressure in the absorption column on the
energy consumption and investment and maintenance costs. The
energy consumption and investment and maintenance costs
increased from 842503.86 GJ to 870593.628 GJ and from
$1602469.23 to $1632337.58 with increasing pressure, respectively.
The pressure and temperature of flash tank 2 are considered to
be operating factors because they are the main factors affecting the
Table 4
Tuning parameters in the process of NSGA-II technology.
Tuning parameter Value
Population size 100
Maximum generation number 400
Mutation probability 0.01
Crossover probability 0.9
Tournament size 2
pressure and heat exchange equipment. They also influence the gas
desorption. Fig. 3 shows the results of the influence of the pressure
in flash tank 2 on the process. When the flash tank 2 pressure in-
creases from 0.09 to 0.4 bar, the CO2 capture ratio decreases from
0.9671 to 0.903 (Fig. 3 (a)). Similarly, the energy consumption de-
creases from 872036.43 GJ to 827529 GJ and the investment and
maintenance costs decrease from $1633053.06 to $1610595.73
(Fig. 3 (b)).
Fig. 4 (a) shows the effect of the temperature in flash tank 2 on
the CO2 and H2S capture ratio. When the temperature increases
from 50 to 90
C, the CO2 capture ratio increases from 0.96 to
0.9735. Fig. 4 (b) shows the influence of the temperature in flash
tank 2 on the energy consumption and the investment and main-
tenance costs. When the temperature increases from 50 to 90
C,
the energy consumption increases from 868328.06 GJ to
878894.19 GJ, and the investment and maintenance costs increase
from $1605748.13 to $1694930.30.
The distillation column plays a role in the separation that occurs
in the process. Thus, the distillation column pressure was selected
as the last factor affecting the process. When the distillation col-
umn pressure was increased from 1 to 5 bar, the CO2 capture ratio
remained at 0.965 according to the simulation results. Fig. 5 shows
the results for the influence of the pressure in distillation column
on the energy consumption and the investment and maintenance
costs of the process. When the distillation column pressure in-
creases from 1 to 5 bar, the energy consumption decreases from
929456.41 GJ to 864593.62 GJ, and the investment and mainte-
nance costs decrease from $1689657.43 to $1634278.98 (Fig. 5 (b)).
In summary, the temperature of flash tank 2 determines the
amount of CO2 desorption from [bmim][Tf2N], making it the first
key factor affecting the CO2 capture ratio. The second is the pres-
sure of the absorption column and flash tank 2. To separate the two
gases effectively, the pressure range of the distillation column is set
at 1e5 bar. For a fixed amount of CO2 capture, the pressure in this
range has little effect on the CO2 capture ratio, which is the last
factor. The order of the factors influencing the investment and
maintenance costs is as follows: temperature of flash tank
2 > pressure of flash tank 2, pressure of distillation
column > pressure of absorption column. The temperature of flash
tank 2 affects the gas expansion and further affects the equipment
size of flash tank 2. This leads to an increase in the investment and
maintenance costs. The order of the factors influencing the energy
consumption is as follows: distillation column pressure > flash tank
2 pressure > flash tank 2 temperature, absorption column pressure.
The pressure of the distillation column changes the amount of
cooling capacity required by the column kettle and the energy
consumption of the compressor and pump in the subsequent
compression process.
5.2. Multi-objective optimization
Based on the results of the sensitivity analysis, it is not difficult
to find that when the design variables change, the economic per-
formance and environmental performance of the CO2 capture and
separation process change in opposite directions. This proves that
they are in opposition to each other. In a case where both of these
performances should be considered, a multi-objective method is an
excellent scheme to weigh the problem with target conflict. This
work had the goal of optimizing Ctot and FCO2 . Fig. 6 shows the
Pareto front of the multi-objective optimization process.
To avoid the influences of the different units of objective func-
tions, Sayyaadi and Nejatolahi (2011) proposed replacing the actual
values with normalized forms. The normalized forms of the
objective functions are as followsEqn 12,Eqn 13:
 Y. Wang et al. / Journal of Cleaner Production 274 (2020) 122871 7

Table 5
Composition of syngas and simulation results.

Syngas conditions Purified syngas conditions CO2 conditions

Mole fraction (%)

H2 45.9 70.43 0.1
N2 0.3 0.46 Trace
CO 18.9 28.68 0.7
AR 0.1 0.15 Trace
CH4 0.2 0.25 0.1
CO2 34.2 0.03 99.1
H2S 0.1 0.589 ppb Trace
H2O 0.3 Trace 0
Total flow (kmol/h) 4237 2758.948 1413.936
Temperature (
C) 40 150 12.48
Pressure (bar) 36 12 150

Table 6
Input information for CO2 capture and separation process simulation.

Block Model Specification

Dehydration column Absorption column Stage: 20, PDEH: 34.0 bar

Absorption column Stage: 9, PABS: 12.0 bar
Distillation RadFrac Stage: 15, PDIS: 4.6 bar, Reflux ratio: 0.5
Flash tank 1 Flash PFLA-1: 3.1 bar, Duty: 0
Flash tank 2 PFLA-2: 0.1 bar, Duty: 0
Compressor 1 Compr PCPM-1: 12.0 bar, h: 0.85
Compressor 2 PCPM-2: 70.0 bar, h: 0.85
Compressor 3 PCPM-3: 1.0 bar, h; 0.85
Compressor 4 PCPM-4: 4.6 bar, h: 0.85
Pump 1 Pump PPUM-1: 12.0 bar, h:0.8
Pump 2 PPUM-2: 150.0 bar, h:0.8
Throttle Valve PTHR: 4.6 bar
Multi heat exchanger MHeatX TCold-outlet: 60.0
C
Heat exchanger 1 HeatX THot-outlet: 30.0
C
Heat exchanger 2 THot-outlet: 60.0
C
Cooler 1 Heater PCOO-1: 12.0 bar, TCOO-1: 25.0
C
Cooler 2 PCOO-2: 12.0 bar, TCOO-2: 25.0
C
Cooler 3 PCOO-3: 0.1 bar, TCOO-3: 20.0
C
Cooler 4 Vapor fraction: 0, PCOO-4: 10.0
C

Fig. 2. Influence of pressure in absorption column on CO2 capture ratio (a) and energy consumption, and investment and maintenance costs (b).

annual costs, respectively; Ctot,nf is the normalized total annual cost;

Ctot  Ctot;min FCO2 ;min andFCO2 ;max are the minimum and maximum CO2 escape
Ctot;nf ¼ (12) flow rates, respectively; and FCO2 ;nf is the CO2 escape flow rate after
Ctot;max  Ctot;min
normalization.
The Pareto front obtained by normalizing the functions is shown
FCO2  FCO2 ;min in Fig. 7. All the points on the Pareto front are the optimal condi-
FCO2 ;nf ¼ (13)
FCO2 ;max  FCO2 ;min tions for the CO2 capture and separation process. The final optimum
solution depends on how decisions are made. To determine a multi-
where Ctot,min and Ctot,max are the minimum and maximum total objective optimal solution, researchers have proposed the
8 Y. Wang et al. / Journal of Cleaner Production 274 (2020) 122871

Fig. 3. Influences of pressure in flash tank 2 on CO2 capture ratio (a) and energy consumption, and investment and maintenance costs (b).

Fig. 4. Influence of temperature in flash tank 2 on CO2 capture ratio (a) and energy consumption, and investment and maintenance costs (b).

Fig. 5. Influences of temperature in absorption column on CO2 capture ratio (a) and energy consumption, and investment and maintenance costs (b).

technique for order preference by similarity to ideal solution (Jain et al., 2016). However, the ideal point is actually a virtual non-
(TOPSIS) method for the decision-making process. The concept of existent point. Therefore, based on the TOPSIS method, the nearest
an ideal point is proposed in this method. Two objective functions point to the ideal point on the Pareto front is chosen as the optimal
have the minimum value (Ctot;nf ¼ 0, FCO2 ;nf ¼ 0) at an ideal point solution. The black line in Fig. 8 represents the distance from the
 Y. Wang et al. / Journal of Cleaner Production 274 (2020) 122871 9

Fig. 6. Pareto front for CO2 capture and separation process.

Fig. 7. Pareto front obtained by normalizing functions.

point on the Pareto front to the ideal point. It can be seen that the
horizontal and vertical coordinates of the minimum distance point
are 0.406 and 0.336, respectively. Therefore, this point is deter-
mined to be the optimal solution. Fig. 8 shows the optimal scheme
based on the environment (Ctot;nf ¼ 1 and FCO2 ;nf ¼ 0), and the
optimal schemes based on the economy (Ctot;nf ¼ 0 and FCO2 ;nf ¼ 1)
and multi-objective optimization scheme (Ctot;nf ¼ 0.402 and
FCO2 ;nf ¼ 0.338). In Fig. 8, the Pareto front is divided into two parts.
The left side of the optimal solution is the scheme based on the
economy, while the right side is the scheme based on the envi-
ronment. The Ctot ,FCO2 Ctot;nf , and FCO2 ;nf values for these three
schemes are given in Table 7. Table 8 gives the decision variables for
the three schemes.
The minimum value for FCO2 (50.03 kmol/h) was found under
the optimal scheme based on the environment. In contrast, the FCO2
value for the optimal scheme based on the economy was 17.6%
higher than this minimum value. The optimal scheme based on the
economy had the minimum Ctot ($15264865.31), whereas the Ctot
for the optimal scheme based on the environment was 4.4% higher
than Ctot,min. Because of the conflict between the economic per-
formance and environmental performance, if one performance is
determined to be in the optimal condition, the design will not be
able to meet the optimal condition for the other performance. The
FCO2 and Ctot values for multi-objective optimization scheme were
5.9% and 1.5% higher than their minimum values, respectively.
Therefore, multi-objective optimization scheme could more
comprehensively meet the process parameter requirements, which
was the optimal result for the CO2 capture and separation process
design.
5.3. Comparison with previous work
The optimal CO2 capture and separation process using the ionic
liquid [bmim][Tf2N] was compared with the Rectisol process (Liu
et al., 2015) and CO2 capture from syngas using the ionic liquid
[emim][Tf2N] (Taheri et al., 2019) in relation to the environment
and energy consumption. The comparison results are shown in
Table 9. In terms of the CO2 capture ratio, the present work was
similar to that of Taheri et al. and the result was 6.34% higher than
that of the Rectisol process. The effective gas recovery ratios of
three processes are basically similar. The Rectisol process has the
lowest electrical energy consumption of the three processes. This is
10 Y. Wang et al. / Journal of Cleaner Production 274 (2020) 122871

Fig. 8. Distance from Pareto front point to ideal point.

Table 7
Annual total costs and CO2 escape flow rates of different schemes.

Optimization scenario Ctot ($/year) FCO2 (kmol/h) Ctot;nf FCO2 ;nf

Optimal scheme based on economy 15264865.31 58.82 0.0 1.0

Multi-objective optimization scheme 15486463.17 52.98 0.402 0.338
Optimal scheme based on environment 15928889.42 50.03 1.0 0.0

Table 8
Decision variables of different schemes.

Decision variables Optimal scheme based on economy Multi-objective optimization scheme Optimal scheme based on environment

Pressure of absorption column (bar) 9 10.4 12

Pressure of Flash tank 2 (bar) 0.4 0.14 0.09
Temperature of Flash tank 2 (
C) 50 61.3 90

Table 9
Comparison of different CO2 capture and separation methods.

Solvent CO2 capture ratio Thermal energy (GJ/t CO2) Electrical energy (GJ/t CO2) Solvent loss (kg/t CO2) Effective gas recovery ratio Sourse

[bmim][Tf2N] 96.34% 0 0.718 0.0059 99.6% Present study

Methanol 90% 0.25 0.40 1.6831 99.56% Liu et al.
[emim][Tf2N] 96.68% 0.033 0.754 0.0239 99.6% Taheri et al.

because the Rectisol process sacrifices the CO2 capture rate to save
electric energy. Because the process of Taheri et al. was similar to
the Rectisol process, heat energy was still consumed. The process
proposed in this paper adopts flash evaporation to recover the
solvent, and the solvent loss rate is the lowest. This proves that it
has reasonable energy utilization.
6. Conclusions
This paper presented a novel CO2 capture and separation pro-
cess based on an ionic liquid for the clean production of coal
chemical industry. The results of 3E analyses of the process were
also presented. The total annual cost and CO2 escape flow rate were
targeted for CO2 capture and separation process optimization. The
following conclusions could be made based on the analysis and
optimization results.
(1) A new CO2 capture and separation process using ionic liquid
[bmim][Tf2N] with multi-objective optimization was
designed in this paper. The effective gas recovery ratio was
99.6% and the CO2 capture ratio was 96.34%. Under the
condition of high efficiency capture of CO2, the production of
high purity syngas is realized, which provides the basis for
the clean production of the following coal chemical process.
(2) A study of the influences of the design variables on the
process parameters showed that a higher acid gas capture
ratio led to a higher energy consumption and equipment
investment. Therefore, not only the impact of economic
factors on the process, but also the effect of the environ-
mental performance of CO2 emissions for the sustainable
development of the process should be considered.
(3) The FCO2 and Ctot values of the multi-objective optimization
scheme were 5.9% and 1.5% higher than their minimum
values, respectively. This reflected that this scheme can
better balance the production cost and sustainable devel-
opment performance of the system.
(4) The process investigated in this work had high electric en-
ergy consumption. One of the future research directions is to
 Y. Wang et al. / Journal of Cleaner Production 274 (2020) 122871 11

improve this process through clean energy and renewable

energy power generation, or to extend it to other CO2 capture
processes. For example, low-temperature waste heat could
be used as an energy source, and a two-stage organic
Rankine cycle could be used for power generation. Among
them, the cold utility, which was not fully utilized in the CO2
capture and separation process, could be used to recycle the
organic Rankine cycle to realize the coupling of the two
processes.
(5) The results of this study showed that it is feasible to use ionic
liquid as absorbent to remove acid gas from the syngas in
clean production of coal chemical industry. In the future, the
application of the ionic liquid can deepen the research of gas
purification in coal chemical industry field or other in-
dustries, and contribute to the green and sustainable devel-
opment of industry.

CRediT authorship contribution statement

Yinglong Wang: Writing - original draft, Writing - review &

editing, Conceptualization, Supervision, Validation. Xiaobin Liu: Fig. A1. Computation process of NSGA-II.
Resources, Data curation. Hongru Zhang: Data curation, Visuali-
zation. Yigang Liu: Software, Formal analysis. Peizhe Cui: Funding
acquisition, Writing - review & editing. Zhaoyou Zhu: Resources,
Funding acquisition. Yixin Ma: Project administration. Jun Gao:
Visualization, Investigation.

Declaration of competing interest

The authors declare that they have no known competing

financial interests or personal relationships that could have
appeared to influence the work reported in this paper.

Acknowledgements

This work is supported by the National Natural Science Foun-

dation of China (No. 21808117), Talent Fund of Shandong Collabo-
rative Innovation Center of Eco-Chemical Engineering (XTCXQN03)
and supported by the State Key Laboratory Base of Eco-chemical
Engineering (STHG1803).

Appendix B. Supplementary data

Supplementary data to this article can be found online at Fig. A2. Pseudo code of NSGA-II.
https://doi.org/10.1016/j.jclepro.2020.122871. The selection process is divided into three steps.

Appendix A 1. Randomly produce an N-sized parent population, and then

The NSGA-II technology was obtained by improving the NSGA
technology. It has three advantages.
1. It has a non-dominated fast sorting algorithm, which can reduce
the computational complexity.
2. By adding an elite strategy, the sample space is effectively
enlarged.
3. The introduction of the crowding degree and distance ensures
the diversity of the population and offspring.
The selection process of this technology is shown in Fig. A1. The
pseudo code is given in Fig. A2 (Deb et al., 2002).
produce an N-sized offspring population from the parent pop-
ulation. A new 2N-sized population is formed by mixing these
two populations.
2. The 2N-sized population is calculated using a non-dominated
fast sorting algorithm. The crowding degree and crowding dis-
tance between individuals are obtained by calculations. Suitable
individuals to compose a new parent population are then
selected based on the calculated information.
3. The crossover and mutation functions of the genetic algorithm
are used to produce the offspring population. Then, a new
population is obtained by mixing this population with the
population formed in step 2. The previous steps are repeated
until the final conditions are met.
12 Y. Wang et al. / Journal of Cleaner Production 274 (2020) 122871

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