Energy Conversion and Management 325 (2025) 119377

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Energy Conversion and Management

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

Theoretical and experimental validation of an electrochemical-mediated

integrated system for CO2 capture and compression
Yuanhao Mao a , Huifeng Fan a , Sayd Sultan a , Yunsong Yu a , Zaoxiao Zhang a,b,* ,
Xiaomei Wu a,*
a
School of Chemical Engineering and Technology, Xi’an Jiaotong University, No.28 Xianning West Road, Xi’an 710049, PR China
b
State Key Laboratory of Multiphase Flow in Power Engineering, Xi’an Jiaotong University, No.28 Xianning West Road, Xi’an 710049, PR China

A R T I C L E I N F O A B S T R A C T

Keywords: The carbon dioxide capture and compression processes represent the most energy-intensive stages in the carbon
CO2 capture capture and storage (CCS) process, which are usually treated independently in the existing studies. Integrating
Electrochemically mediated amine the CO2 capture and compression stages is a possible way to effectively reduce the compressor size and the total
regeneration (EMAR)
energy consumption of the CCS process. The recent development of electrochemically mediated amine regen­
Thermodynamic model
eration (EMAR) technology provides a promising approach for this integration due to the strong driving force of
Integrated system
Energy consumption the electrochemical reaction and the copper–amine complexation reaction. In this paper, we propose an
electrochemical-mediated integrated system for CO2 capture and compression and verify its pressurized opera­
tion performance both theoretically and experimentally. A thermodynamic model was developed to analyze the
energy performance of the system and a bench-scale flow-cell system was designed to verify its ability to output
CO2 under pressurized conditions. The thermodynamic modelling results indicated that the energy consumption
of the integrated system is significantly affected by different operational paths. At lower pressures, CO2 bubbles
are easier to form and the system tends to operate in 3-steps, higher pressures lead the system to function in 4-
steps. Furthermore, the total energy consumption of the CCS process can be reduced by releasing CO2 at a
suitable pressure. The results of the bench-scale flow system indicated that a 40% increase in release pressure
resulted in a nearly constant driving voltage and released CO2 amount, thereby demonstrating its capacity to
release pressurized CO2. In conclusion, the results demonstrate the feasibility of the electrochemical-mediated
integrated system, which provide an innovative low-energy pathway to support the achievement of global
carbon neutrality.

1. Introduction efficiency and low-energy consumption carbon neutrality technologies

has been a pressing necessity for mitigating CO2 concentration in the
The excessive amount of anthropogenic carbon dioxide (CO2) emis­ atmosphere [6–8].
sions has posed a serious threat to the global ecosystem [1,2]. As indi­ The post-combustion CO2 capture process based on the solid
cated in the International Energy Agency (IEA) report, the global adsorption and amine absorption is the most mature carbon capture
energy-related carbon emissions reached 37.4 Gt in 2023, representing method. However, its practical application is still limited by several is­
the highest level on record [3]. Concurrently, 2023 has been the hottest sues, such as high energy consumption and low adsorption capacity
year on record, with many climate scientists predicting that 2024 may [9,10]. In recent years, electrochemical carbon capture (ECC) technol­
witness even more extreme weather and climate crises [4]. In this ogy has attracted wide attention [11]. In contrast to the conventional
context, more countries are recognizing the necessity of mitigating thermal-based carbon capture technology, the ECC technology is pow­
environmental problems. At the United Nations Climate Conference ered by electricity instead of high temperature steam to facilitate the
(COP28) in 2023, nearly 200 countries collectively committed to taking regeneration of the absorbent, thereby eliminating the limitation of the
the necessary action to achieve the Paris Agreement target of limiting Carnot cycle caused by temperature swing (energy efficiency ≤ 22 %)
global temperature rise to less than 1.5 ◦ C [5]. The exploration of high- [12]. Moreover, the flexibility of the power system enables ECC

* Corresponding authors.
E-mail addresses: [email protected] (Z. Zhang), [email protected] (X. Wu).

https://doi.org/10.1016/j.enconman.2024.119377
Received 10 September 2024; Received in revised form 4 December 2024; Accepted 4 December 2024
Available online 16 December 2024
0196-8904/© 2024 Elsevier Ltd. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
Y. Mao et al. Energy Conversion and Management 325 (2025) 119377

technology to be implemented on different carbon sources, such as

centralized stationary large carbon sources (power plants, steel mills, Mn + + αAmine⇌M(Amine)nα + R2
cement factories, etc.) and small distributed sources (automotive, ship­ The EMAR technology has been developed for over a decade, during
ping, aerospace, ambient atmosphere, etc.) [13]. Currently developed which significant advancements have been made in reaction system
ECC systems include electrochemical pH swing, electrochemical gener­ optimization, system simulation, electrochemical reactor design and
ation of redox actives, capacitive adsorption, and electrolytically- system economic evaluation. The performance of single solvents in the
mediated amine regeneration (EMAR) process [14–17]. Among these, EMAR systems has been extensively investigated, including EDA (eth­
the EMAR technology is developed from the traditional amine-based ylenediamine), MEA (monoethanolamine), NH3 (ammonia) and MMEA
absorption process and thus has the potential to use the well- (2-(methylamino)ethanol) [21–24]. A long cycle operation with the CO2
established amine solvents. The absorption process is consistent with desorption energy consumption of 40–80 kJ/mol CO2 has been achieved
the traditional amine absorption process, with the main distinction in the Cu-EDA system [25]. Subsequent studies have demonstrated that
being the use of an electrochemical reaction to regenerate the amine using mixed solvents and surfactants can effectively enhance the sta­
absorbent. The EMAR technology is distinguished by its high absorption bility of the EMAR system and reduce the desorption energy consump­
capacity, high efficiency, and low energy consumption, which makes it a tion, which has expanded the scope of suitable absorbents in the EMRA
promising option for industrial applications. system [26–28]. Meanwhile, the thermodynamic modelling, multi-
The operation of the EMAR process is based on the reaction R(1) and physics field simulation and full-cost modelling have been employed
R(2). The oxidation state ions of some transition metals (such as Cu2+, to investigate the effects of operating conditions such as copper loading
Fe3+, Zn2+, Ni2+, etc.) can form strong complexes with amino groups and flow rate, as well as equipment investment and feedstock price on
(NH) in amine molecules [18–20]. These complexes exhibit consider­ the EMAR system [29,30]. The findings demonstrated that the optimized
ably higher stability than Amine-CO2, which indicates that R(2) plays a EMAR system can achieve a minimum energy consumption of 16 kJ/mol
dominant role in the solution. As the result, the metal ions occupy the CO2 with the cost of carbon capture reaching less than $50/tCO2 [31,32].
binding sites of organic amines, disrupting the structure of Amine-CO2 Despite the comprehensive development of the EMAR system, the
and leading to the release of CO2. In the cathode chamber, the released related research is still limited to identifying the optimal systems and
metal ions were electroplated under the applied electric field, which operating conditions to further reduce the energy consumption. The
facilitates the regeneration of the amine absorbent. practical operation of the system has yet to be fully investigated, and its
Amine + CO2 ⇌Amine-CO2 R1 full operational potential remains to be realized.
A full-chain CCS process encompasses carbon capture, transport, and
utilization/storage stages. In the CO2 utilization and storage process,

Fig. 1. Flowsheet for the CCS process. (a) Conventional CCS process; (b) Electrochemical CO2 capture and compression based on EMAR technology for CCS.

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Y. Mao et al. Energy Conversion and Management 325 (2025) 119377

CO2 is typically pressurized to a range of 7–15 MPa for refrigerants and Table 1
15 MPa for enhanced oil recovery (EOR) or geological sequestration The main reactions in the electrochemical-mediated integrated system.
[33–35]. As illustrated in Fig. 1, if the CO2 can be pressurized at the Reaction types Reaction equilibrium equation
capture stage, it could partially replace the function of compressor, ( )
Electrochemical Cu2(aq)
+
+ 2e ⇌Cu(s)
− RT C0
thereby reducing the energy consumption of the compression equip­ E = E0 −
nF
ln
CCu2+
ment, which is important for reducing the total energy consumption of Amine-CO2 formation EDA + CO2 ⇌EDACO2 KCO2 =
( )
the full-chain CCS project. Moreover, the high-pressure inlet gas can CEDACO2 P0
streamline the compression process, reduce the compression stages and CEDA PCO2
Cu-Amine Cu2+ + C Cu(EDA) 2+
minimize the size of the compressor, which is crucial for the operational [ 2]
complexation [
2EDA⇌ Cu(EDA)2
]2+ β = 2
CEDA CCu2+
stability of the compressor. It is fortunate that the EMAR technology is [ ]2+
Overall Cu(EDA)2 + 2e− + 2CO2 ⇌Cu(s) + 2EDACO2
characterized by pressurized operation. The electrochemical reaction
occurs in solution, and thus the reaction of metals to metal ions is nearly
unaffected by the ambient pressure. Moreover, the driving force of the
equilibrium equations.
reaction R(2) is significantly greater than R(1), facilitating the release of
In these equilibrium equations, Ci represents the concentration of
CO2 under pressure with only a small increase in the physically dissolved
species i. The Cu(s) is the solid Cu electrode, and its concentration (C0) is
CO2 in the solution [11]. Nevertheless, there is still a paucity of research
constant at a value of 1. The standard equilibrium potential (E0 ) of Cu/
investigating the performance of pressurized operation of EMAR system.
Cu2+ is 0.34 V vs. SHE, the Faraday constant (F) is 96485C⋅mol− 1 and
The concept of electrochemical compressor has inspired the inves­
the gas constant (R) is 8.314 J⋅mol− 1⋅K− 1. P0 is the reference pressure,
tigation of an electrochemical-mediated integrated system for CO2
which is equivalent to 0.1 MPa.PCO2 represents the partial pressure of
capture and compression based on the EMAR process. The electro­
CO2, which is determined by the operating conditions. The values of
chemical compressor technology employs electrochemical reactions to
these equilibrium constants can be found in reference [31].
pressurize gases, which has been widely studied in the fields of hydrogen
These equilibrium equations can be solved to determine the con­
(H2) compression [36]. Currently, the electrochemical H2 compressors
centration of each substance in the solution and its corresponding po­
can compress H2 from atmospheric pressure to over 5.0 MPa [37–39]. In
tential. In order to solve those equations, it is necessary to define the
contrast, the electrochemical NH3 compressors and electrochemical CO2
mass conservation equations for EDA, CO2 and Cu as follows:
compressors have received less attention. Existing studies used NH+ 4 and
CO2–3 as medium to achieve gas pressurization, requiring the assistance CEDA,tot = CEDA + CEDACO2 + 2C Cu(EDA) 2+ (1)
[ 2]
of H2 or O2 to complete the electrochemical reaction. Furthermore, the
2–
reverse diffusion of NH+ 4 and CO3 reduces the efficiency of the process CCO2,tot = CCO2 + C[EDACO2 ] (2)
and makes it more challenging to operate at high pressures [40,41].
Nevertheless, the aforementioned studies provided a comprehensive CCu,tot = CCu2+ + C Cu(EDA) 2+ (3)
theoretical framework and a valuable experimental basis for studying [ 2]

the electrochemical-mediated integrated system for CO2 capture and

where Ctot is the total concentration of the corresponding substance in
compression.
the solution and CCO2 is the concentration of physically dissolved CO2.
Inspired by the concept of the electrochemical compressor and based
Given the high stability constant of the Cu-EDA complex, it can be
on the EMAR system’s capability to operate at high pressures, this study
assumed that there are no free Cu2+ present in the solution with a suf­
proposes an electrochemical-mediated integrated system for CO2 cap­
ficient amount of amine [42]. Thus, the mass balance of Cu can be
ture and compression. The pressurized CO2 can mitigate the operational
rewritten as:
challenges associated with subsequent compression stages, thereby
enhancing the overall stability of CCS operations. A comprehensive CCu,tot = C Cu(EDA) 2+ (4)
[ 2]
thermodynamic model was established to assess the operational capa­
bility of the system. In this context, the gas–liquid characteristics of the For convenience, the ratio of EDA bound with Cu2+ to the total amine
anode outlet fluid of the system have been investigated separately in concentration is defined as the Cu2+ loading (δ), which is calculated by:
order to explain the effect of pressure on its operational performance.
2C Cu(EDA) 2+ 2C
Furthermore, the model was employed to validate the practical advan­ δ=
[ 2]
=
Cu,tot
(5)
tages of the system through a comparison of the total energy con­ CEDA,tot CEDA,tot
sumption for CO2 capture and pressurization to 15 MPa in a full chain Similarly, the CO2 loading is defined as:
CCS project. The subsequent section examined the operation of the
constructed bench-scale flow-cell system and demonstrated the practical CCO2 ,tot
x= (6)
operational capability of the electrochemical-mediated integrated sys­ CEDA,tot
tem. Our preliminary explorations will provide a new research direction Based on the above equations, the relationship between the open
for electrochemical carbon capture systems, which offer a practical circuit potential and the composition of the solution can be established
value to this green and low-energy carbon capture technology. as follows:

2. Materials and methods [ ( ) ( ( )1 ) (

RT C0 2C0 2
E = E0 + ln − ln (1 − δ) β + ln 1
F CEDA,tot δCEDA,tot
2.1. Modeling )]
PCO2
+ KCO2 (7)
P0
2.1.1. The thermodynamic model of the electrochemical-mediated
integrated system The open circuit potential at the CO2 partial pressure of
The electrochemical CO2 capture and pressurized process involves a 0 (PCO2 = 0) is chosen as the reference potential. Hence, the relative
series of reactions, including CO2 hydration, amine protonation, amine- potentials Er under various conditions are calculated as:
CO2 reaction, Cu electrode electrochemical dissolution/deposition and ( )
RT
Cu-amine complexation. Although each reaction contributes, the overall Er = ln 1 + KCO2 P̃CO (8)
F 2
performance of the system is controlled by some key reactions. Table 1
lists the main reactions within the Cu-EDA based system with their

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Y. Mao et al. Energy Conversion and Management 325 (2025) 119377

(CuSO4⋅5H2O, AR), and sodium sulfate (Na2SO4, AR) were used to

̃CO = PCO2
P (9) prepare the electrolyte, which were procured from Sigma-Aldrich. The
2
P0
pure CO2 (99.99 vol%) was injected into the electrolyte to prepare the
The Henry’s law is used to calculate the relationship between CO2 CO2-rich solution.
partial pressure (PCO2 ) and the concentration of physically dissolved CO2
(CCO2 ), the relationship is shown as equation (10). It is assumed that the 2.2.2. Bench-scale operation of the electrochemical-mediated integrated
Henry’s coefficient in the amine solution is the same as that in pure system
water. The Henry’s coefficient is temperature-dependent, as expressed An electrically driven continuous flow system was developed to
in equation (11). This can be reformulated in terms of concentration achieve CO2 capture and pressurized release. The detailed diagram of
through equation (12) [43,44]. the bench-scale system was shown in Fig. 2.
CCO2 = PCO2 KH (10) In the electrochemical cell, an anion exchange membrane (Selemion
AMV, Japan) divides the flow channel into two parts. Within each
ln(Kh ) = 4.80 + 3934.40T − 1 − 941290.20T − 2
(11) chamber, a copper plate electrode (GB T2, 5 cm × 5 cm, ≥99.9 %) was
installed as the cathode and anode. Graphite plates were used to apply
1000ρH2 O uniform current to the copper electrodes. The transportation of the
KH = (12) electrolyte was facilitated by two peristaltic pumps (LEADFLUID,
expKh ⋅MH2 O
BT100S). A flask was used to stabilize the gas pressure, while a pressure
where T is the operating temperature, K. ρH2 O is the density of water, kg/ gauge was used to monitor the system pressure. Before the pressurized
L; and MH2 O is the water’s molecular mass, 18 g/mol. Based on equation operation experiment, the pipeline was purged with pure CO2 to reach
(10)-(12), the relationship between the total concentration of CO2 and the target pressure. The electrolyte solution consists of 4 mol/kg H2O
its partial pressure can be established as follow: EDA with a Na2SO4 concentration of 0.5 mol/kg H2O. The simulated
anolyte has a Cu-loading of 0.2, while the catholyte has a Cu-loading of
KCO2 P
̃CO
̃CO KH P0 0.8. During the experiment, the electrolyte’s temperature was main­
x = (1 − δ) 2
+P (13)
1 + KCO P
2
̃CO
2
2
CEDA,tot tained by the thermostat water bath.
Before the experiment, the electrochemical impedance spectroscopy
By combining equation (8) and (13), the relative potential Er of the
(EIS) was performed with frequency range of 100 kHz to 0.1 Hz at open
solution under different CO2 partial pressures, CO2 concentrations,
circuit voltage (OCP) to ascertain the various impedances present within
amine concentrations, and Cu2+ concentrations can be calculated. Ul­
the system. During the experiment, the voltage profiles corresponding to
timately, the thermodynamic energy consumption of the EMAR system
different currents and the amount of CO2 generated were recorded to
cycle can be calculated by the following formula:
calculate the electron efficiency and CO2 desorption energy consump­
∮ ∮
EdQ CEDA,tot ⋅F Edδ tion. For the pressurized operation experiment, excess sulfuric acid
W(kJ/mol CO2 ) = = (14) titration was used to determine the CO2 concentration of the electrolyte.
ΔnCO2 ΔnCO2
Here, the electron efficiency (η) presents the molar ratio of CO2 released
where Q represents the charge transferred in the electrochemical reac­ per mole of electrons. WCO2 is the practical energy consumption. The formulas are
tion, ΔnCO2 is the molar amount of desorbed CO2. provided as follows:
For comparison, the thermodynamic limit for separation CO2 from a
ΔnCO2
mixed gas with 15 % CO2 under ambient conditions can be calculated by η= ∫ (18)
Idt
the following equation [12]:
( ) ∫
PCO2 UIdt
Wlim = − RTln (15) WCO2 = (19)
P0 ΔnCO2

2.1.2. The energy consumption of pump and compressor where ΔnCO2 represents the amount of CO2 desorbed (mole); I is the
In the CO2 utilization or geological sequestration process, it is applied current (A) and U is the cell voltage (V); t is the desorption time
commonly necessary to increase its pressure to 15.0 MPa. The energy (s).
consumption of both compressors and pumps plays a significant role and
must be considered in energy consumption calculations. The energy 3. Results and discussion
consumption of compressors is related to the inlet pressure Pin, and the
formula is given as follows [45]: 3.1. Thermodynamic analysis of the electrochemical-mediated integrated
system
Wcomp = − 3.48lnPin + 14.85, 1 bar⩽Pin ⩽20bar (16)

Assuming the operation of the pump is a simple isothermal process, Based on the thermodynamic model established in Section 2.1, a
the power consumed by the pump for capturing each mole of CO2 is comprehensive study was conducted to analyze the relationship be­
given by the following empirical formula [46]: tween the energy consumption and its operating pressure of the
electrochemical-mediated integrated system. The realistic benefits of
Pop − PCO2 the system were validated by comparing the total energy consumption of
Wpump = (17)
CEDA,tot × ΔxCO2 a full-chain CCS process witch capture CO2 and pressurized to 15 MPa
for geological utilization or sequestration.
where Pop is operating pressure, MPa; PCO2 is the partial pressure of CO2
in flue gas, MPa;ΔxCO2 is the difference of CO2 loading between the 3.1.1. Model validation
anolyte and catholyte. Before calculation, model validation should be carried out to
demonstrate the accuracy of the calculation process. While theoretical
models of compressor and pump have been widely applied, the
2.2. Experimental electrochemical-mediated integrated system model based on the EMAR
process still requires comparative validation. The accuracy of EMAR
2.2.1. Materials process was validated through the simulation of the classical process
In the experiment, EDA (AR, 99 %), copper sulfate pentahydrate

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Y. Mao et al. Energy Conversion and Management 325 (2025) 119377

Fig. 2. The electrochemical-mediated integrated system. (a) Process schematic diagram; (b) experimental system.

proposed by Wang et al [25]. As shown in Fig. 3, the computational recent years, the energy demand of the EMAR technology has been
result of 16.2 kJ/mol CO2 aligns with the value of 16.0 kJ/mol CO2 progressively decreasing, steadily approaching its theoretical energy
reported by Sara et al. [47], thereby validating the accuracy of our consumption. This trend provides confidence in the practical application
model. For comparison, we analyzed the thermodynamic limit con­ of this system.
sumption for separating CO2 from a mixed gas containing 15 % CO2
under ambient conditions, which was determined by Eq. (15) to be 4.7 3.1.2. The energy consumption the electrochemical-mediated integrated
kJ/mol CO2. Considering a separation efficiency of 90 %, the minimum system
energy consumption for CO2 separation from flue gas is 6.4 kJ/mol CO2. Based on the thermodynamic model established in Section 2.1.1, a
The theoretical energy consumption of the EMAR process is only 2.5 theoretical evaluation of the thermodynamic energy consumption of the
times the minimum energy requirement, highlighting the substantial electrochemical-mediated integrated system was carried out. During the
advantages of this technique. Additionally, Fig. 3 also illustrates the calculation process, the concentration of EDA was set at 4 mol/kg H2O,
energy consumption for CO2 desorption as reported in current labora­ the temperature was maintained at 50 ◦ C, and the Cu2+ loading was
tory systems. Due to the continuous research and improvements in varied between 0.2 and 0.8.

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Y. Mao et al. Energy Conversion and Management 325 (2025) 119377

(b) The three-step operational process

Following comprehensive experimental observations, it was deter­

mined that a two-phase flow phenomenon occurs at the anode outlet of
the electrochemical cell, as illustrated in Fig. 5. This indicates that CO2
gas can be released directly without flash operation. Consequently, a 3-
step electrochemical-mediated integrated system process was calculated
on the assumption that the electrolyte at the outlet of the anode is fully
gas–liquid separated. The schematic of the 3-step process is depicted in
Fig. 4 (b). The absorption and cathodic processes of the 3-step process
(Fig. 4 (b) step1 and step 3) are consistent with those of the 4-step
process (Fig. 4 (a) step 1 and step 4). However, there are notable dif­
ference that the gradual accumulation of dissolved CO2 in the anodic
electrolyte will separate at the target pressure, as shown in step 2 of
Fig. 4 (b).
Fig. 6 presents the theoretical energy consumption of the 4-step and
3-step processes. It demonstrates that there are notable discrepancies in
energy consumption between the various operational paths. The 3-step
Fig. 3. The theoretical carbon capture energy consumption vs. experimental process allows for timely CO2 release, resulting in lower energy con­
energy consumption under the same solution’s conditions. sumption at different operating pressures than 4-step operation when
the output pressure is less than 5 MPa. However, the increase in pressure
(a) The four-step operational process led to a significant rise in energy consumption of 3-step process. This
phenomenon can be attributed to the varying ease of CO2 bubbles for­
In previous studies, it was generally assumed that no visible CO2 mation at different pressures. According to Henry’s law, higher CO2
bubbles formed in the electrolyte at the anodic exit of the electro­ pressure increases its solubility in the solution, thus necessitating more
chemical cell. This implies that the gas–liquid separation phenomenon Cu2+ to drive the CO2 release during anode process of the
occurs in the flash tank. In this case, the electrochemical-mediated in­ electrochemical-mediated integrated system. Consequently, the energy
tegrated system cycle consists of four steps, as illustrated in Fig. 4 (a). consumption increases with increasing pressure. However, the 4-step
Step (1): The EDA absorbent containing a small amount of Cu2+ absorbs operational process assumes a pure liquid anode outlet, which means
CO2 to saturation in the presence of flue gas with a 15 % CO2 concen­ the energy consumption is less influenced by pressure and remains
tration; Step (2): The CO2-rich liquid is directed to the anode chamber relatively constant. It is noteworthy that at extremely high pressures (10
where Cu electrodes dissolved, resulting in an increase in Cu2+ loading; MPa), the dissolved CO2 concentration in the solution increases signif­
Step (3): Subsequently, the solution is transferred to a flash tank, in icantly. This phenomenon leads to a decrease in the potential difference
which the Cu2+ loading remained constant and the CO2 released from between the anodic and cathodic processes, reducing the energy con­
the cell at target pressure; Step (4): Following the flash tank, the solution sumption of the 4-step process. However, the CO2 output declines
is pumped to the cathode chamber where Cu2+ was electroplated onto significantly at this stage, adversely affecting the carbon capture pro­
another Cu electrode, reducing the Cu2+ loading in the solution and cess. When the pressure reaches a critical threshold, the CO2 gas cannot
regenerating its capacity to absorb CO2. Fig. 4 (a) illustrates the rela­ be released, indicating that the maximum operating pressure limit has
tionship between the relative potential (Er) and the composition of the been reached, as illustrated at 12.44 MPa in the Fig. 4.
electrolyte during the 4-step process. It should be emphasized that while CO2 bubbles form in the anode
chamber, this does not fully represent the CO2 desorption process. The

Fig. 4. Thermodynamic paths of the electrochemical-mediated integrated system. (a) 4-step process; (b) 3-step process. (The red dashed line represents a constant
CO2 loading line, the horizontal dashed line signifies a constant CO2 partial pressure line, and the curved line delineates the operation process of the integrated
system). (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)

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Y. Mao et al. Energy Conversion and Management 325 (2025) 119377

Fig. 5. The anodic outlet of the electrochemical cell.

actual operation of the EMAR system falls between the 3-step and 4-step
processes. At lower releasing pressures, CO2 bubbles are more likely to
form, causing the system to behave more like the 3-step operation, with
the energy consumption increasing significantly as the pressure rises. As
the pressure continues to increase, CO2 bubbles become difficult to form
in the solution, and the system prefers to the 4-step operation, with
energy consumption remaining relatively stable. Further increasing the
pressure results in the complete dissolution of CO2 in the solution,
causing the system to malfunction, as observed at a maximum pressure
of 12.4 MPa in the 4 M EDA absorbent. In this study, calculations were
conducted for both limiting cases. While the energy consumption of the
3-step process increases with rising pressure below 5 MPa, the energy
consumption of subsequent compression equipment must be considered,
which will be discussed in detail in Section 3.1.3.

3.1.3. The total energy consumption of the full-chain CCS process

In a full-chain CCS process, the CO2 typically needs pressurization for
geological utilization or sequestration. The actual benefits of the inte­
grated system were validated by comparing the total energy consump­
tion of the full-chain CCS process. Here, the final system pressure was set
as 15 MPa.
Fig. 6. The energy consumption of the electrochemical-mediated inte­ As shown in Fig. 7. The transfer of liquids becomes more challenging
grated system. with increasing system pressure, leading to an increased energy con­
sumption of the pump. However, as the output pressure increases, the

Fig. 7. The total energy consumption of the integrated system at different release pressure. (a) 4-step process; (b) 3-step process.

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Y. Mao et al. Energy Conversion and Management 325 (2025) 119377

compressor energy consumption decreases significantly, with over a 50

% reduction observed at 1.0 MPa. The notable decline in compressor
energy consumption effectively offsets the rise in pump energy con­
sumption. This indicates that pressurized CO2 output is an effective
strategy to reduce the energy consumption of compressor.
For the 4-step process, when the out pressure is below 1 MPa, the
reduced energy consumption of the compressor effectively offsets the
impact of increased pressure on both the pump and the electrochemical-
mediated integrated system. Therefore, the total system energy con­
sumption is lower. At pressures exceeding 1 MPa, the diminished energy
consumption of the compressor is insufficient to offset the augmented
energy consumption of the pumps and the integrated system. Conse­
quently, the total energy consumption of the proposed CCS process
increased. This phenomenon is particularly evident in the 3-step pro­
cess, where the energy consumption of the 3-step process rises signifi­
cantly with pressure. This increase obscures the effect of reduced
compressor energy consumption. However, there is no significant in­
crease in total energy consumption when the output pressures of CO2
capture section are ≤ 0.5 MPa, which demonstrates the 3-step operation
remains competitive at lower release pressures. It should be noted that
the system tends to operate in the 3-step process at lower pressures, Fig. 8. Nyquist plots of the EIS experiment of the flow-cell without flow. (The
resulting in minimal changes in total energy consumption at system CO2-saturated electrolytes contain 4 mol/kg H2O EDA and 0.5 mol/kg H2O
pressures below 0.5 MPa. Given that the actual operation of the Na2SO4. The initial Cu2+ loading is 0.2 and 0.4 in anolyte and catholyte. The
electrochemical-mediated integrated system is between the 4-step and experiment was conducted at a temperature of 50 ◦ C).
3-step processes, it can be deduced that the total energy consumption of
the full-chain CCS process is advantageous at appropriate output pres­ in the flow cell is low, and diffusion is the main limiting factor, which is
sure (< 0.5 MPa). Even if the total energy consumption remains similar consistent with the performance of the flat-plate EMAR system reported
after using the electrochemical-mediated integrated system, the system by Stern et al [48].
still remains advantage. This is due to the system can reduce the
compressor stages and compressor size of subsequent compression 3.2.2. The selection of operation current density
equipment, thereby reducing the investment costs. The operating current density is a crucial parameter influencing the
Overall, the energy consumption of the different parts of the full- electrochemical-mediated integrated system. A suitable operating cur­
chain CCS process has been carefully evaluated through the thermody­ rent density can mitigate the overpotential, thereby reducing the energy
namic model, demonstrating the potential for low-energy operation of consumption, which is significance for the integrated system. The per­
the electrochemical-mediated integrated system. It should be empha­ formance of the flow-cell was evaluated at the current densities ranging
sized that the model estimates the minimal energy consumption dictated from 50 A/m2 to 100 A/m2. The experiment was conducted at 50 ◦ C with
by thermodynamic constraints and ignores some resistance during the peristaltic pump speed of 40 rpm (the electrolyte flow rate of
actual operation. Nevertheless, we are optimistic that with continuous approximately 10 ml/min).
enhancements, the system can be optimized to approach the lowest The response voltage–time curve, stabilized cell voltage, electron
theoretical energy consumption. efficiency and desorption energy consumption were analyzed to inves­
tigate the effect of current density on the performance of the flow-cell
3.2. Experimental validation of the electrochemical-mediated integrated system. Fig. 9 (a) shows the monitored cell voltage at the current den­
system sity of 50 A/m2 for 1 h. At the initial stage, the cell voltage exhibits a
sharp rise, followed by a gradual decline to a stable value. The sudden
The results of the thermodynamic modelling had demonstrated that increase in voltage can be attributed to two main reasons: (a) the
the energy consumption of the electrochemical-mediated integrated possible presence of a copper oxide film during anodic oxidation, which
system is closely related to the practical operating process of the system. hinders the reaction of Cu to Cu2+; (b) the difficulty of directly utilizing
In order to verify the actual operating capability of the proposed system, active substances on the electrode surface. As a result, the cell voltage is
a comprehensive experimental study was carried out in this section, the rapidly increased to facilitate the reaction process. As the electro­
experimental set up was shown in Fig. 2. chemical reaction continues, the oxide film on the anode begins to
rupture; concurrently, the liquid flow provides an adequate supply of the
3.2.1. The resistances in the electrochemical cell active substance. This results in a gradual decrease in the cell voltage,
The electrochemical impedance spectroscopy (EIS) technique was which ultimately reaches a stable value. Fig. 9 (b) demonstrates that
conducted to quantify the potential resistances within the electro­ increasing the current density results in a nearly linear increase in the
chemical reactor. The frequency sweep was performed in the range of cell voltage. There is no significant increase in voltage over the selected
10 kHz to 1 Hz and the voltage was set to the open circuit voltage with a current density range, suggesting that no additional overpotential is
sinusoidal voltage wave amplitude of 10 mV. The Nyquist plot of the EIS presented. This phenomenon is consistent with the EIS analyses pre­
results is presented in Fig. 8. The intersection of the arc in the high- sented in Section 3.1, indicating that active substance diffusion is the
frequency region with the x-axis represents the ohmic impedance control step within the flow-cell. As the current density increases, the
(RΩ), which is indicative of the solution resistance, membrane resistance electronic efficiency decreases gradually, as illustrated in Fig. 9 (c).
and any potential contact resistances within the system. Due to the Theoretically, 1 mol of electrons should produce 0.5 mol of Cu2+, which
substantial amount of supporting electrolyte and the relatively narrow then combine with 1 mol of EDA molecules to form [Cu(EDA)2]2+
cathode–anode spacing, the ohmic impedance was found to be 0.65 Ω. complexes. The zwitterion mechanism has demonstrated that the molar
The low-frequency region of the Nyquist plot displays a linear trend with ratio of CO2 to EDA is 1:1. Consequently, it is theoretically possible for 1
a slope of 0.46, which suggests a significant limitation in material mol of electrons to release 1 mol of CO2, thereby achieving 100 %
transfer within the electrochemical cell. Overall, the ohmic impedance

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Y. Mao et al. Energy Conversion and Management 325 (2025) 119377

Fig. 9. The performance of the flow-cell with different applied current at 0.1 MPa. (a) The V-t curve at the current density of 50 A/m2; (b) the cell voltage at steady
state; (c)the electron efficiency; (d) the desorption energy consumption. (200 mL CO2-saturated solution serves as electrolyte, which contain 4 mol/kg H2O EDA and
0.5 mol/kg H2O Na2SO4. The initial Cu2+ loading is 0.2 and 0.8 in the anolyte and catholyte, respectively. The experiment was conducted at a temperature of 50 ◦ C
for 1 h).

electron utilization. However, in practice, the generation of CO2 bub­ 0.14 MPa. Increasing the desorption pressure poses a significant chal­
bles, the re-saturation of the solvent, and the enthalpy change of the lenge to the liquid flow at the inlet of the anode electrolysis reservoir,
EDA-CO2 reactants consume some electrons, reducing the electrons especially under low liquid flow rate. Therefore, the peristaltic pump
available for CO2 release. Fig. 9 (d) demonstrates that the desorption speed during the pressurization operation was set at 80 rpm (the elec­
energy consumption increases from 86.4 kJ/mol CO2 at 50 mA/m2 to trolyte flow rate of approximately 20 ml/min).
153.67 kJ/mol CO2 at 100 mA/m2 as a consequence of the cell voltage To evaluate the performance of pressurized operation, the response
rise and the electronic efficiency decrease at high current density. voltage–time curve, the mount of CO2 desorbed and desorption energy
In summary, increasing the current density has a negative impact on consumption were recorded. Fig. 10 (a) illustrates the response volta­
the overall performance of the flow-cell, although it does accelerate the ge–time curves under different system pressure. It is evident that the
rate of CO2 release. Therefore, the operating current density should be response voltages at different pressures are highly similar. The response
selected carefully to ensure an appropriate balance between the reaction voltage changes by only 5 mV when the pressure increases by 40 %. This
rate and the flow-cell performance. Furthermore, it is important to note indicates that the proposed system can achieve stable CO2 output under
that the flow rate in the experiment is not optimized. The high liquid pressurized conditions. Fig. 10 (b) compares the CO2 release perfor­
flow rate results in a limited electrochemical reaction window, leading mance at different release pressure. The results show that the
to poor electron efficiency. Optimizing the liquid flow can effectively electrochemical-mediated integrated system can effectively release CO2,
improve the performance of the flow-cell. However, the objective of this and the pressure has almost no effect on the CO2 desorption perfor­
study is to evaluate the viability of the electrochemical-mediated inte­ mance. As shown in Fig. 10 (c), the energy consumption performance at
grated system. The optimization of the various parameters will be different output pressures is compared using the 0.1 MPa as a bench­
considered in our future research plan. mark. It was observed that an increase in output pressure does not cause
a significant rise in energy consumption, confirming the stability of the
3.2.3. Bench-scale validation of the electrochemical-mediated integrated integrated system.
system
As indicated in Section 3.2.2, a high current density leads to signif­ 4. Conclusions and outlooks
icantly higher energy consumption of the flow-cell. Consequently, the
applied current density in the pressurization experiments was set at 50 Based on the high-pressure operational capability of the EMAR
mA/m2. The operating absolute pressures were 0.1 MPa, 0.12 MPa and technology and the innovative concept of electrochemical compression,

9
Y. Mao et al. Energy Conversion and Management 325 (2025) 119377

this paper presents an electrochemical-mediated integrated system for

CO2 capture and compression. The system’s operational capability is
validated through theoretical and experimental analysis. This system
can stably release CO2 under pressurized conditions, significantly
reducing the compression difficulty of the subsequent compression
equipment. For the entire CCS process, this electrochemical-mediated
integrated system can reduce operational energy consumption and
improve process stability, which is of great significance for the practical
advancement and widespread adoption of carbon emission reduction
technologies.
Through simulations and experimental studies, several meaningful
conclusions have been drawn. Firstly, the results of the thermodynamic
modelling demonstrate that the energy consumption of the system is
significantly influenced by the operating path. At lower operating
pressures, CO2 bubbles are more likely to appear in the solution, and the
system tends to operate in the 3-step process, where energy consumption
is significantly affected by pressure. As the pressure increases, the sys­
tem shifts toward a 4-step operation. Since the actual process falls be­
tween 3 and 4 steps, the integrated system exhibits a competitive
advantage when the output pressure is below 5 MPa. Secondly, the
thermodynamic energy consumption calculations demonstrate that the
electrochemical-mediated integrated system with an outlet pressure
below 0.5 MPa could reduce the total energy consumption of the full-
chain CCS process, highlighting the practical benefits of the system.
Thirdly, the performance of the constructed electrochemical flow-cell
system shows that increasing the operating current density leads to a
decrease in the electron efficiency and an increase in the energy con­
sumption. At the applied current density of 50 mA/m2, the system ex­
hibits an energy consumption of only 86.4 kJ/mol CO2. Finally, at the
applied current density of 50 mA/m2, increasing the pressure from 0.1
MPa to 0.14 MPa did not result in significant changes in response voltage
and CO2 desorption amount, demonstrating the proposed system is
capable of stabilizing output CO2 under pressurization.
It is important to note that the main objective of this study is to verify
the operational capabilities of the electrochemical-mediated integrated
system. Our preliminary investigation has demonstrated the superiority
of the system. To further advance the system, future optimizations can
be pursued from several perspectives. (1) Due to the limitations of the
experimental conditions, the maximum operating pressure was limited
to 0.14 MPa. Therefore, a larger-scale verification of pressurization is
necessary in the future. (2) The flow rate of the electrolyte significantly
impacts the performance of the flow-cell, faster flow rates accelerate the
diffusion of active substances, thereby reducing the response voltage.
However, the limited electrochemical reaction window at high flow
rates hinders chemical reactions and reduces the electron efficiency. The
electrolyte flow rate should be optimized to achieve a balance with other
performance parameters. (3) The pressure is closely related to the for­
mation of CO2 bubbles. The generation of CO2 bubbles under high
pressure is difficult, which can potentially alleviate the uneven current
density distribution caused by these bubbles within the electrolyte.
Studying the bubble generation and movement under varying pressures
is crucial to further reduce the system’s energy consumption. It is
believed that through continuous research, the energy consumption of
the electrochemical-mediated integrated system will be further reduced
and its industrial application will be realized.

CRediT authorship contribution statement

Fig. 10. The performance of the flow-cell at different operating pressure. (a)
The V-t curve at the current density of 50 A/m2; (b) the amount of CO2 in 100 Yuanhao Mao: Writing – original draft, Methodology, Conceptual­
mL anolyte; (c) the relative unit energy consumption with 0.1 MPa as bench­ ization. Huifeng Fan: Investigation, Data curation. Sayd Sultan: Soft­
mark. (100 mL CO2-saturated solution serves as electrolyte, containing 4 mol/ ware, Data curation. Yunsong Yu: Methodology. Zaoxiao Zhang:
kg H2O EDA and 0.5 mol/kg H2O Na2SO4. The initial loading of Cu2+ in the Supervision. Xiaomei Wu: Supervision.
anolyte and catholyte is 0.2 and 0.8, respectively. The experimental tempera­
ture was maintained at 50 ◦ C, and a current density of 50 A/m2 was applied for
Declaration of competing interest
1 h.).

The authors declare that they have no known competing financial

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Y. Mao et al. Energy Conversion and Management 325 (2025) 119377

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