Modular design and optimization of hydrogen-driven electrochemical CO2 capture systems

doi:10.11949/0438-1157.20250150

Abstract

Abstract:

Hydrogen-driven electrochemical carbon capture system (HECCS) is a new method for low-concentration CO₂ capture and separation. Due to limitations such as large-area membrane preparation, membrane performance, and electrode performance, the single-module carbon capture capacity of HECCS is limited. To enhance the carbon capture performance and economic efficiency of the HECCS, a modular design and optimization approach for the HECCS is proposed. Based on analyzing the operational performance of a single HECCS module, the carbon capture strategies and optimal operation methods for the modular HECCS are established. The structural characteristics of modular HECCS systems and the coordination and matching features between modules are elucidated. The results indicate that in specific scenarios for capturing CO₂ at low concentrations, different combinations of the modules within the modular carbon capture system significantly influence the carbon capture performance and economic efficiency. Under certain operating conditions, the series structure exhibits superior decarbonization effects compared to the parallel structure, while the multi-stage structures are favorable for reducing hydrogen consumption. The optimal number of stages for an HECCS system is significantly influenced by factors such as inlet and outlet CO₂ concentration, hydrogen price, and HECCS module cost, which is a trade-off between the operating expenses and investment costs of the system. This work provides the optimal design method for enhancing the performance and economic efficiency of modular HECCS systems.

Key words: electrochemical CO₂ capture system, hydrogen, modulization, system design, optimization

摘要：

氢气驱动的电化学捕碳系统（HECCS）是一种新型的低浓度CO₂捕集与分离方法。受大面积膜制备、膜性能和电极性能等限制，HECCS系统的单模块捕碳能力有限。为了提高HECCS系统捕碳性能和系统经济性，本文提出HECCS系统的模块化设计与优化方法，在分析HECCS系统单模块操作性能基础上，研究了模块化HECCS系统的捕碳策略及优化操作方法，阐明了模块化HECCS系统结构特性及单元模块之间的协调匹配特性。研究表明，在特定的低浓度CO₂捕获场景中，在模块化捕碳系统中，不同单元模块组合方式的HECCS模块化系统结构显著影响捕碳性能和经济性。在相同操作条件下，串联结构比并联结构具有更优的除碳效果，多级结构有助于降低系统氢气消耗；HECCS系统的最优级数受进出口CO₂浓度、氢气价格和HECCS模块价格影响显著，取决于系统操作费用和投资费用权衡。本研究可为模块化HECCS系统性能优化和经济性提升提供优化设计方法。

关键词: 电化学捕碳系统, 氢气, 模块化, 系统设计, 优化

CLC Number:

TQ 021.8

Shichang LIU, Yibai LI, Jing WANG, Yongzhong LIU. Modular design and optimization of hydrogen-driven electrochemical CO₂ capture systems[J]. CIESC Journal, 2025, 76(8): 4108-4118.

刘世昌, 李一白, 王靖, 刘永忠. 氢气驱动电化学捕碳系统的模块化设计与优化[J]. 化工学报, 2025, 76(8): 4108-4118.

Figures/Tables 10

Fig.1 Carbon capture mechanism and characteristics of HECCS

Fig.2 Structural diagram of hydrogen-driven modular electrochemical CO2 capture system

Table 1 Validation of the model A and B

性能	RMSE		R²		拟合范围
性能	Model A	Model B	Model A	Model B	Model A	Model B
除碳率	2.07%	3.95%	0.9706	0.9607	0~1	0~1
CO₂通量/( $k g C O 2$ ·(m²·h))	0.34%	0.61%	0.9968	0.9905	0~0.4	0~0.4
电子效率	1.23%	3.12%	0.9847	0.9730	0~1	0~1

Table 1 Validation of the model A and B

性能	RMSE		R²		拟合范围
性能	Model A	Model B	Model A	Model B	Model A	Model B
除碳率	2.07%	3.95%	0.9706	0.9607	0~1	0~1
CO₂通量/( $k g C O 2$ ·(m²·h))	0.34%	0.61%	0.9968	0.9905	0~0.4	0~0.4
电子效率	1.23%	3.12%	0.9847	0.9730	0~1	0~1

Table 2 Comparison of optimization results under series and parallel structures of HECCS

0.14

0.032

0.081

0.14

0.0055

0.081

0.0085

0.14

0.032

0.0010

0.022

除碳率

0.52

0.78

0.73

0.52

0.96

0.73

0.90

0.52

0.78

0.97

0.93

CO₂通量/(

k g C O 2

/(m²·h))

0.22

0.16

0.15

0.22

0.10

0.15

0.10

0.22

0.16

0.058

0.13

电子效率

0.67

0.47

0.50

0.67

0.31

0.50

0.31

0.67

0.47

0.17

0.40

总氢消耗/(mg/h)

15.42

15.58

14.34

15.42

14.70

14.34

15.29

15.42

15.58

11.84

15.26

单位CO₂耗氢/(

k g H 2 / k g C O 2

Table 2 Comparison of optimization results under series and parallel structures of HECCS

性能

Mode 1

Mode 2

Mode 3

Mode 4

Mode 5

Mode 6

出口CO₂浓度/%

0.14

0.032

0.081

0.14

0.0055

0.081

0.0085

0.14

0.032

0.0010

0.022

除碳率

0.52

0.78

0.73

0.52

0.96

0.73

0.90

0.52

0.78

0.97

0.93

CO₂通量/(

k g C O 2

/(m²·h))

0.22

0.16

0.15

0.22

0.10

0.15

0.10

0.22

0.16

0.058

0.13

电子效率

0.67

0.47

0.50

0.67

0.31

0.50

0.31

0.67

0.47

0.17

0.40

总氢消耗/(mg/h)

15.42

15.58

14.34

15.42

14.70

14.34

15.29

15.42

15.58

11.84

15.26

单位CO₂耗氢/(

k g H 2 / k g C O 2

)

0.040

0.045

0.053

0.052

0.049

0.057

Table 3 Optimal operating parameters and hydrogen consumption in typical scenarios

场景	级数	操作参数		出口CO₂浓度/%	平均电子效率	总耗氢量/(g/h)
场景	级数	电流密度/(mA/cm²)	温度/℃	出口CO₂浓度/%	平均电子效率	总耗氢量/(g/h)
S1	1	24.8	60	0.12	0.62	45.83
S1	2	10.7/10.0	60/60	0.12	0.74	38.21
S2	2	17.7/14.8	60/60	0.20	0.78	36.17
S2	3	10.0/10.2/10.0	60/60/60	0.20	0.85	33.60

Fig.3 Operating range under different stages for HECCS

Table 4 Economics of HECCS under different stages in Scenario 1 and Scenario 2

场景	级数	电流密度/(mA/cm²)	末级出口CO₂浓度/%	投资成本/元	操作成本/元	总成本/元	标准化成本/(元/ $t C O 2$ )
S1	1	24.8	0.12	1780.71	14050.75	15831.46	1446.51
	2	10.7/10.0	0.12	3561.43	11711.87	15273.30	1393.40
	3	10.0/10.0/10.0	0.053	5342.14	17355.62	22697.76	1508.25
	4	10.0/10.0/10.0/10.0	0.0072	7123.57	23295.12	30418.69	1708.96
S2	2	17.7/14.8	0.20	2140.71	11099.38	13240.09	1207.33
	3	10.0/10.2/10.0	0.20	3210.71	10297.87	13508.58	1233.41
	4	10.0/10.0/10.0/10.0	0.12	4281.43	13632.51	17913.94	1288.70
	5	10.0/10.0/10.0/10.0/10.0	0.049	5351.43	17262.87	22614.30	1371.60

Table 4 Economics of HECCS under different stages in Scenario 1 and Scenario 2

场景	级数	电流密度/(mA/cm²)	末级出口CO₂浓度/%	投资成本/元	操作成本/元	总成本/元	标准化成本/(元/ $t C O 2$ )
S1	1	24.8	0.12	1780.71	14050.75	15831.46	1446.51
	2	10.7/10.0	0.12	3561.43	11711.87	15273.30	1393.40
	3	10.0/10.0/10.0	0.053	5342.14	17355.62	22697.76	1508.25
	4	10.0/10.0/10.0/10.0	0.0072	7123.57	23295.12	30418.69	1708.96
S2	2	17.7/14.8	0.20	2140.71	11099.38	13240.09	1207.33
	3	10.0/10.2/10.0	0.20	3210.71	10297.87	13508.58	1233.41
	4	10.0/10.0/10.0/10.0	0.12	4281.43	13632.51	17913.94	1288.70
	5	10.0/10.0/10.0/10.0/10.0	0.049	5351.43	17262.87	22614.30	1371.60

Fig.4 Variation of cost with the number of stages for electrochemical CO2 capture systems in S1 and S2

Fig.5 Optimal stage number under different inlet and outlet concentrations of CO2

Fig.6 Variation of the standardization cost with hydrogen prices and HECCS cost

References 32

[1]	Huang P, Fu J L, Qiu D Y, et al. Experimental and kinetic study on the cyclic removal of low concentration CO₂ by amine adsorbents in confined spaces[J]. Process Safety and Environmental Protection, 2023, 180: 417-427.
[2]	李俊华, 焦桂萍, 邓辉, 等. 潜艇大气环境控制关键技术研究现状与展望[J]. 中国舰船研究, 2022, 17(5): 116-124.
	Li J H, Jiao G P, Deng H, et al. Development and prospects of key technology for submarine atmospheric environment control[J]. Chinese Journal of Ship Research, 2022, 17(5): 116-124.
[3]	徐新宏, 江璐, 方晶晶, 等. AIP潜艇长航期间舱室环境中空气污染物分析[J]. 舰船科学技术, 2019, 41(21): 94-99.
	Xu X H, Jiang L, Fang J J, et al. Analysis of air pollutants in an air independent propulsion submarine[J]. Ship Science and Technology, 2019, 41(21): 94-99.
[4]	Georgescu M R, Meslem A, Nastase I. Accumulation and spatial distribution of CO₂ in the astronaut's crew quarters on the International Space Station[J]. Building and Environment, 2020, 185: 107278.
[5]	Zhang Z J, Jin T, Wu H W, et al. Experimental investigation on environmental control of a 50-person mine refuge chamber[J]. Building and Environment, 2022, 210: 108667.
[6]	Jacobson T A, Kler J S, Hernke M T, et al. Direct human health risks of increased atmospheric carbon dioxide[J]. Nature Sustainability, 2019, 2: 691-701.
[7]	王钰, 乔江波, 李灿, 等. 核潜艇舱室一体化空气再生系统技术设想[J]. 舰船科学技术, 2022, 44(1): 78-81.
	Wang Y, Qiao J B, Li C, et al. The technical concept of integrated air regeneration system for nuclear submarine[J]. Ship Science and Technology, 2022, 44(1): 78-81.
[8]	Bisotti F, Hoff K A, Mathisen A, et al. Direct air capture (DAC) deployment: a review of the industrial deployment[J]. Chemical Engineering Science, 2024, 283: 119416.
[9]	Sodiq A, Abdullatif Y, Aissa B, et al. A review on progress made in direct air capture of CO₂ [J]. Environmental Technology & Innovation, 2023, 29: 102991.
[10]	Bui M, Adjiman C S, Bardow A, et al. Carbon capture and storage (CCS): the way forward[J]. Energy & Environmental Science, 2018, 11(5): 1062-1176.
[11]	Brethomé F M, Williams N J, Seipp C A, et al. Direct air capture of CO₂ via aqueous-phase absorption and crystalline-phase release using concentrated solar power[J]. Nature Energy, 2018, 3: 553-559.
[12]	Lee J W, Ahn H, Kim S, et al. Low-concentration CO₂ capture system with liquid-like adsorbent based on monoethanolamine for low energy consumption[J]. Journal of Cleaner Production, 2023, 390: 136141.
[13]	Küng L, Aeschlimann S, Charalambous C, et al. A roadmap for achieving scalable, safe, and low-cost direct air carbon capture and storage[J]. Energy & Environmental Science, 2023, 16(10): 4280-4304.
[14]	赵俊德, 周爱国, 陈彦霖, 等. 吸附法CO₂直接空气捕集技术能耗现状[J]. 化工学报, 2025, 76(4): 1375-1390.
	Zhao J D, Zhou A G, Chen Y L, et al. Energy consumption of adsorption CO₂ direct air capture[J]. CIESC Journal, 2025, 76(4): 1375-1390.
[15]	Garcia J A, Villen-Guzman M, Rodriguez-Maroto J M, et al. Technical analysis of CO₂ capture pathways and technologies[J]. Journal of Environmental Chemical Engineering, 2022, 10(5): 108470.
[16]	Baek H M. Possibility of military service-regeneration of LiOH for submarines and improvement in CO₂ scrubbing performance of LiOH canisters[J]. Journal of Advanced Marine Engineering and Technology, 2022, 46(3): 115-121.
[17]	Panda D, Kulkarni V, Singh S K. Evaluation of amine-based solid adsorbents for direct air capture: a critical review[J]. Reaction Chemistry & Engineering, 2023, 8(1): 10-40.
[18]	An K J, Li K, Yang C M, et al. A comprehensive review on regeneration strategies for direct air capture[J]. Journal of CO₂ Utilization, 2023, 76: 102587.
[19]	Bouaboula H, Chaouki J, Belmabkhout Y, et al. Comparative review of direct air capture technologies: from technical, commercial, economic, and environmental aspects[J]. Chemical Engineering Journal, 2024, 484: 149411.
[20]	Zito A M, Clarke L E, Barlow J M, et al. Electrochemical carbon dioxide capture and concentration[J]. Chemical Reviews, 2023, 123(13): 8069-8098.
[21]	Fasihi M, Efimova O, Breyer C. Techno-economic assessment of CO₂ direct air capture plants[J]. Journal of Cleaner Production, 2019, 224: 957-980.
[22]	Li Y, Yuan Y P, Li C F, et al. Human responses to high air temperature, relative humidity and carbon dioxide concentration in underground refuge chamber[J]. Building and Environment, 2018, 131: 53-62.
[23]	Du Y, Gai W M, Jin L Z. A novel and green CO₂ adsorbent developed with high adsorption properties in a coal mine refuge chamber[J]. Journal of Cleaner Production, 2018, 176: 216-229.
[24]	Matz S, Setzler B P, Weiss C M, et al. Demonstration of electrochemically-driven CO₂ separation using hydroxide exchange membranes[J]. Journal of the Electrochemical Society, 2021, 168(1): 014501.
[25]	Shi L, Zhao Y, Matz S, et al. A shorted membrane electrochemical cell powered by hydrogen to remove CO₂ from the air feed of hydroxide exchange membrane fuel cells[J]. Nature Energy, 2022, 7: 238-247.
[26]	Rahimi M, Khurram A, Hatton T A, et al. Electrochemical carbon capture processes for mitigation of CO₂ emissions[J]. Chemical Society Reviews, 2022, 51(20): 8676-8695.
[27]	Matz S, Shi L, Zhao Y, et al. Hydrogen-powered electrochemically-driven CO₂ removal from air containing 400 to 5000 ppm CO₂ [J]. Journal of the Electrochemical Society, 2022, 169(7): 073503.
[28]	Sharifian R, Wagterveld R M, Digdaya I A, et al. Electrochemical carbon dioxide capture to close the carbon cycle[J]. Energy & Environmental Science, 2021, 14(2): 781-814.
[29]	Gubler L. Wire-free electrochemical CO₂ scrubbing[J]. Nature Energy, 2022, 7: 216-217.
[30]	Abbasi R, Setzler B P, Yan Y S. Material and system development needs for widespread deployment of hydroxide exchange membrane fuel cells in light-duty vehicles[J]. Energy & Environmental Science, 2023, 16(10): 4404-4422.
[31]	彭文波, 张诗, 李志印, 等. 回收液氧冷量冻结清除二氧化碳实现AIP潜艇节能增效[J]. 中国舰船研究, 2024, 19(5): 231-237.
	Peng W B, Zhang S, Li Z Y, et al. Recycle cold energy of liquid oxygen to clear carbon dioxide for AIP submarine[J]. Chinese Journal of Ship Research, 2024, 19(5): 231-237.
[32]	Tang Y, Li Y M. Comparative analysis of the levelized cost of hydrogen production from fossil energy and renewable energy in China[J]. Energy for Sustainable Development, 2024, 83: 101588.

Modular design and optimization of hydrogen-driven electrochemical CO₂ capture systems

氢气驱动电化学捕碳系统的模块化设计与优化

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