氢气驱动电化学捕碳系统的模块化设计与优化

doi:10.11949/0438-1157.20250150

摘要/Abstract

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

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

中图分类号:

TQ 021.8

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.

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.

图/表 10

图1 HECCS捕碳机理及特性

Fig.1 Carbon capture mechanism and characteristics of HECCS

图2 氢气驱动的模块化电化学捕碳系统结构

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

表1 模型A和模型B的验证结果

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

表1 模型A和模型B的验证结果

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

表2 HECCS系统串并联结构下优化结果

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

表2 HECCS系统串并联结构下优化结果

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

表3 典型场景下的最优操作参数和耗氢量

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

图3 电化学捕碳系统不同级数下的操作范围

Fig.3 Operating range under different stages for HECCS

表4 场景一和场景二下不同级数对HECCS系统经济性影响

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

表4 场景一和场景二下不同级数对HECCS系统经济性影响

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

图4 场景一和场景二中电化学捕碳系统的费用随串联级数的变化

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

图5 不同进出口CO2浓度要求下的最优级数

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

图6 标准化成本随氢气价格和HECCS费用的变化

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

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