变电吸附二氧化碳捕集技术研究进展

doi:10.16085/j.issn.1000-6613.2023-1040

摘要/Abstract

摘要：

基于变电吸附的碳捕集技术，通过“通电-断电”实现摆荡模式，利用电能焦耳效应产生热能，驱动吸附剂实现连续地吸附与再生。相对于变温吸附，其输入高品位电能，因此可驱动碳源、碳汇之间的大浓度差富集，近年来备受关注。然而，目前限制变电吸附碳捕集技术应用的主要问题是较高的能耗与较低的产率。据此，本文总结了近年来国内外变电吸附碳捕集技术的研究进展并提出了技术展望。首先讨论了变电吸附碳捕集的基本原理，其次综述了近十年变电吸附碳捕集技术中吸附剂、循环结构的研究进展及发展趋势，应用热力学第二定律效率对变电吸附碳捕集系统展开评价。最后，对变电吸附碳捕集技术发展趋势进行展望，变电吸附技术具备规模化竞争力的关键为：在改善吸附剂导电和捕集性能的基础上，改进吸附剂制备工艺，关注吸附剂的加热形式以及吸附腔体内的电阻分配，尝试与其他碳捕集技术耦合进行分级捕集，与可再生能源进行集成。

关键词: 二氧化碳捕集, 吸附剂, 解吸, 变电吸附, 循环结构, 性能分析, 热力学

Abstract:

The carbon capture based on electric swing adsorption (ESA) could achieve a swing cycle through on/off mode of power. Meanwhile, it employs Joule heating effect of electrical energy to generate heat and hence to drive the continuous adsorption and regeneration of the adsorbent. With the input of electrical energy in high-grade, an enrichment for a significant concentration difference between carbon source and sink could be achieved, leading to its recent widespread attention. However, the main challenges currently limiting the application of ESA for carbon capture are high energy consumption and low generation efficiency. This paper provided a literature review on research progress on ESA for carbon capture. Firstly, the fundamental principles of carbon capture technology using ESA were presented. Secondly, the research progress and development trends of adsorbents and cyclic construction of ESA for carbon capture over the past decade were reviewed. The performance evaluation of ESA for carbon capture was conducted through the second law of thermodynamics efficiency. Finally, the future development trends of carbon capture technology using ESA were discussed. The key to competitive scalability of such technology lied in improving the conductivity and capture performance of the adsorbent. The preparation technology of adsorbent should be improved. Attention should be given to the heating form of the adsorbent and the resistance distribution in the adsorption chamber. Additionally, coupling with other carbon capture technologies for hierarchical capture should be considered and integration with renewable energy sources should be explored.

Key words: CO₂ capture, adsorbents, desorption, electric swing adsorption, cycle structure, analysis of performance, thermodynamics

中图分类号:

王胜岩, 邓帅, 赵睿恺. 变电吸附二氧化碳捕集技术研究进展[J]. 化工进展, 2023, 42(S1): 233-245.

WANG Shengyan, DENG Shuai, ZHAO Ruikai. Research progress on carbon dioxide capture technology based on electric swing adsorption[J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 233-245.

图/表 14

表1 吸附材料性能

年份	材料	类型	比表面积 /m²·g^-1	总孔容积 /cm³·g^-1	平均孔径 /nm	温度 /℃	压力 /bar	入口气体成分	CO₂吸附量 /mol·kg^-1	电阻率 /Ω·m
2009	活性炭纤维 ^[13]	蜂窝整体	907	0.36	16.1	25	1	99.99%CO₂	0.91	—
	70%沸石/30%石墨^[14]	蜂窝整体	—	—	—	42	1.5	3.5%CO₂、96.5%N₂	1.2	—
2010	浸渍胺的聚合树脂^[9]	挤压颗粒填充	—	—	—	40	1	99.99%CO₂	3.7	—
2010	66%活性炭纤维/34% 酚醛树脂^[15]	蜂窝整体	998	0.6	1.6	20	1	99.99%CO₂	2.9	—
2011	沥青基球形活性炭 ^[16]	挤压颗粒填充	1205	0.59	—	30	0.15	99.99%CO₂	1.12	—
2013	氧化改性的酚醛树脂基炭^[17]	挤压颗粒填充	962	0.41	—	25	1	99.99%CO₂	2.7	—
2013	18%沸石/82%活性炭^[18]	挤压颗粒填充	—	—	—	22	1	7.6%CO₂、92.4%N₂	0.82	0.00144-0.000001T_s
2015	炭^[19]	蜂窝整体	—	—	—	30	1	0.3%CO₂	3.45×10^-3	5.02×10^-2
2016	石墨烯薄膜^[20]	片状薄膜	—	—	—	25	1	99.99%CO₂	11.59
2016	石墨烯气凝胶^[20]	片状薄膜	165	—	—	25	1	99.99%CO₂	21.36	—
2016	毫米级介孔碳球 ^[21]	挤压颗粒填充	36	0.13	30.1	75	1	15%CO₂、85%N₂	3.71	—
2017	22%酚醛树脂/78%H-ZSM-5-800^[22]	蜂窝整体	397	0.2	—	25	1.1	99.99%CO₂	2.2	5.8
2017	多孔炭（UGIL-900）^[23]	蜂窝整体	4200	2.41	2.3	25	1	99.99%CO₂	2.2	—
2017	活性炭^[24]	蜂窝整体	—	—	—	20	1	99.99%CO₂	3.5	0.00063-0.0000004954T_s
2018	70%沸石NaUSY/30%活性炭^[11]	蜂窝整体	460	0.26	—	20	0.15	99.99%CO₂	2.05	1.18×10^-2
2018	活性炭^[25]	蜂窝整体	—	—	—	—	—	—	—	0.0011-0.000000856T_s
2018	18%沸石13X/82%活性炭^[25]	蜂窝整体	—	—	—	—	—	—	—	0.0014-0.00000111T_s
2019	浸渍PEI的碳化硅纤维^[26]	中空管束	—	—	500	30	1	15%CO₂、85%N₂	0.886	0.00125
2019	沸石填充的碳纳米管^[26]	中空管束	—		1.6	30	1	15%CO₂、85%N₂	11.14	0.0003
2019	82%沸石H-ZSM-5/18%活性炭^[27]	蜂窝整体	—	—	—	20	0.15	99.99%CO₂	1.2	3.4423-0.0067T_s
2019	70%沸石13X/30%活性炭^[28]	3D打印整体	2028	0.648	—	0	0.15	99.99%CO₂	3.49	0.28
2020	50%沸石13X/50%活性炭^[3]	挤压颗粒填充	—	—	237	30	1	99.99%CO₂	3.2	0.57-0.0885(T_s-293)^0.3
2021	活性炭管^[29]	中空管束	—	—	—	35	1	99.99%CO₂	1.22	0.0108
2021	50%沸石13X/50%活性炭^[6]	3D打印整体	819	0.43	1700	27	0.15	99.99%CO₂	1.54	59.0619
2021	50%沸石13X/50%石墨^[6]	3D打印整体	316	0.15	1500	27	0.15	99.99%CO₂	1.38	7.5398
2022	47.5%沸石47.5%活性炭5％黏合剂^[30]	3D打印整体	1985	0.88	—	30	1	15%CO₂、85%N₂	1.5	—

表1 吸附材料性能

年份	材料	类型	比表面积 /m²·g^-1	总孔容积 /cm³·g^-1	平均孔径 /nm	温度 /℃	压力 /bar	入口气体成分	CO₂吸附量 /mol·kg^-1	电阻率 /Ω·m
2009	活性炭纤维 ^[13]	蜂窝整体	907	0.36	16.1	25	1	99.99%CO₂	0.91	—
	70%沸石/30%石墨^[14]	蜂窝整体	—	—	—	42	1.5	3.5%CO₂、96.5%N₂	1.2	—
2010	浸渍胺的聚合树脂^[9]	挤压颗粒填充	—	—	—	40	1	99.99%CO₂	3.7	—
2010	66%活性炭纤维/34% 酚醛树脂^[15]	蜂窝整体	998	0.6	1.6	20	1	99.99%CO₂	2.9	—
2011	沥青基球形活性炭 ^[16]	挤压颗粒填充	1205	0.59	—	30	0.15	99.99%CO₂	1.12	—
2013	氧化改性的酚醛树脂基炭^[17]	挤压颗粒填充	962	0.41	—	25	1	99.99%CO₂	2.7	—
2013	18%沸石/82%活性炭^[18]	挤压颗粒填充	—	—	—	22	1	7.6%CO₂、92.4%N₂	0.82	0.00144-0.000001T_s
2015	炭^[19]	蜂窝整体	—	—	—	30	1	0.3%CO₂	3.45×10^-3	5.02×10^-2
2016	石墨烯薄膜^[20]	片状薄膜	—	—	—	25	1	99.99%CO₂	11.59
2016	石墨烯气凝胶^[20]	片状薄膜	165	—	—	25	1	99.99%CO₂	21.36	—
2016	毫米级介孔碳球 ^[21]	挤压颗粒填充	36	0.13	30.1	75	1	15%CO₂、85%N₂	3.71	—
2017	22%酚醛树脂/78%H-ZSM-5-800^[22]	蜂窝整体	397	0.2	—	25	1.1	99.99%CO₂	2.2	5.8
2017	多孔炭（UGIL-900）^[23]	蜂窝整体	4200	2.41	2.3	25	1	99.99%CO₂	2.2	—
2017	活性炭^[24]	蜂窝整体	—	—	—	20	1	99.99%CO₂	3.5	0.00063-0.0000004954T_s
2018	70%沸石NaUSY/30%活性炭^[11]	蜂窝整体	460	0.26	—	20	0.15	99.99%CO₂	2.05	1.18×10^-2
2018	活性炭^[25]	蜂窝整体	—	—	—	—	—	—	—	0.0011-0.000000856T_s
2018	18%沸石13X/82%活性炭^[25]	蜂窝整体	—	—	—	—	—	—	—	0.0014-0.00000111T_s
2019	浸渍PEI的碳化硅纤维^[26]	中空管束	—	—	500	30	1	15%CO₂、85%N₂	0.886	0.00125
2019	沸石填充的碳纳米管^[26]	中空管束	—		1.6	30	1	15%CO₂、85%N₂	11.14	0.0003
2019	82%沸石H-ZSM-5/18%活性炭^[27]	蜂窝整体	—	—	—	20	0.15	99.99%CO₂	1.2	3.4423-0.0067T_s
2019	70%沸石13X/30%活性炭^[28]	3D打印整体	2028	0.648	—	0	0.15	99.99%CO₂	3.49	0.28
2020	50%沸石13X/50%活性炭^[3]	挤压颗粒填充	—	—	237	30	1	99.99%CO₂	3.2	0.57-0.0885(T_s-293)^0.3
2021	活性炭管^[29]	中空管束	—	—	—	35	1	99.99%CO₂	1.22	0.0108
2021	50%沸石13X/50%活性炭^[6]	3D打印整体	819	0.43	1700	27	0.15	99.99%CO₂	1.54	59.0619
2021	50%沸石13X/50%石墨^[6]	3D打印整体	316	0.15	1500	27	0.15	99.99%CO₂	1.38	7.5398
2022	47.5%沸石47.5%活性炭5％黏合剂^[30]	3D打印整体	1985	0.88	—	30	1	15%CO₂、85%N₂	1.5	—

图1 活性炭材料的可行几何结构[35]

图2 四步ESA循环

图3 五步VESA循环

图4 六步ESA循环

图5 七步ESA循环

图6 八步ESA循环

表2 ESA碳捕集系统热力学性能分析总结

年份	材料	循环结构	CO₂进料体积分数/%	回收率/%	纯度/%	生产率 /kg·s^-1·kg^-1	能耗 / $G J · t C O 2 - 1$	η /%	η_2nd^① /%
2006	活性炭纤维^[13]	五步VESA	50	73.00	—	—	18.04	—	0.32
2008	活性炭^[38]	四步ESA	4.51	89.52	16.36	1.54×10^-3	7.23	—	3.02
2009	70%沸石/30%石墨^[14]	六步ESA	3.5	79.50	78.93	—	2.04	—	11.03
2009	80%沸石13X/20%活性炭^[62]	七步ESA	3.5	70.00	89.70	—	1.90	—	11.52
2010	66%活性炭纤维/34%酚醛树脂^[15]	四步ESA	10.75	95.00	—	—	3.00	—	5.76
2011	沥青基球形活性炭 ^[16]	五步VESA	15	95.00	—	—	3.50	—	4.36
2013	18%沸石/82%活性炭^[18]	六步ESA	8.1	81.40	46.60	—	33.30	32.70	0.53
2015	炭^[19]	四步ESA	0.3	95.00	—	—	33.10	64.00	1.15
2017	分子筛13X ^[44]	八步ESA	3.96	89.90	95.10	—	9.05		2.50
2017	活性炭^[24]	四步ESA	15	76.00	52.00	—	5.64	47.00	2.42
2017	70%沸石13X/30%活性炭^[63]	四步ESA	3.5	90.00	—	—	5.47	—	3.62
2017	70%TRI-PE-MCM-41/30%活性炭^[63]	四步ESA	6.4	90.00	—	—	3.67	—	5.40
2018	80%沸石13X/20%活性炭^[60]	八步ESA	3.96	91.20	94.70	9.60×10^-3	13.05	—	1.74
2018	80%沸石13X/20%活性炭^[60]	八步ESA	7.26	93.60	95.60	1.38×10^-2	9.64	—	2.02
2018	70%NaUSY沸石/30%活性炭^[11]	四步ESA	15	80.00	44.00	3.47×10^-4	2.50	75.00	5.57
2018	活性炭^[11]	四步ESA	15	80.00	53.00	5.86×10^-4	4.43	18.40	3.14
2018	活性炭^[25]	四步ESA	10	—	—	—	4.57	34.67	3.57
2018	18%沸石13X/82%活性炭^[25]	四步ESA	10	—	—	—	3.20	39.51	5.34
2018	70%沸石NaUSY/30%活性炭^[25]	四步ESA	10	—	—	—	2.78	56.22	6.15
2019	浸渍PEI的碳化硅纤维^[26]	三步ESA	15	62.00	81.00	—	14.50	—	0.89
2019	沸石填充的碳纳米管^[26]	三步ESA	15	62.00	81.00	—	9.20	—	1.40
2019	82%沸石H-ZSM-5/18%活性炭^[27]	五步VESA	15	72.00	33.00	4.80×10^-4	2.04	—	6.58
2021	50%沸石13X/50%活性炭^[6]	—	15	—	—	—	—	19.00	—
2021	50%沸石13X/50%石墨^[6]	—	15	—	—	—	—	34.00	—
2022	47.5%沸石47.5%活性炭5％黏合剂^[30]	—	15	—	—	1.98×10^-4	—	—	—
2022	50%硅酸钾/50%活性炭^[64]	四步ESA	30	92.10		—	19.90	—	0.53

表2 ESA碳捕集系统热力学性能分析总结

年份	材料	循环结构	CO₂进料体积分数/%	回收率/%	纯度/%	生产率 /kg·s^-1·kg^-1	能耗 / $G J · t C O 2 - 1$	η /%	η_2nd^① /%
2006	活性炭纤维^[13]	五步VESA	50	73.00	—	—	18.04	—	0.32
2008	活性炭^[38]	四步ESA	4.51	89.52	16.36	1.54×10^-3	7.23	—	3.02
2009	70%沸石/30%石墨^[14]	六步ESA	3.5	79.50	78.93	—	2.04	—	11.03
2009	80%沸石13X/20%活性炭^[62]	七步ESA	3.5	70.00	89.70	—	1.90	—	11.52
2010	66%活性炭纤维/34%酚醛树脂^[15]	四步ESA	10.75	95.00	—	—	3.00	—	5.76
2011	沥青基球形活性炭 ^[16]	五步VESA	15	95.00	—	—	3.50	—	4.36
2013	18%沸石/82%活性炭^[18]	六步ESA	8.1	81.40	46.60	—	33.30	32.70	0.53
2015	炭^[19]	四步ESA	0.3	95.00	—	—	33.10	64.00	1.15
2017	分子筛13X ^[44]	八步ESA	3.96	89.90	95.10	—	9.05		2.50
2017	活性炭^[24]	四步ESA	15	76.00	52.00	—	5.64	47.00	2.42
2017	70%沸石13X/30%活性炭^[63]	四步ESA	3.5	90.00	—	—	5.47	—	3.62
2017	70%TRI-PE-MCM-41/30%活性炭^[63]	四步ESA	6.4	90.00	—	—	3.67	—	5.40
2018	80%沸石13X/20%活性炭^[60]	八步ESA	3.96	91.20	94.70	9.60×10^-3	13.05	—	1.74
2018	80%沸石13X/20%活性炭^[60]	八步ESA	7.26	93.60	95.60	1.38×10^-2	9.64	—	2.02
2018	70%NaUSY沸石/30%活性炭^[11]	四步ESA	15	80.00	44.00	3.47×10^-4	2.50	75.00	5.57
2018	活性炭^[11]	四步ESA	15	80.00	53.00	5.86×10^-4	4.43	18.40	3.14
2018	活性炭^[25]	四步ESA	10	—	—	—	4.57	34.67	3.57
2018	18%沸石13X/82%活性炭^[25]	四步ESA	10	—	—	—	3.20	39.51	5.34
2018	70%沸石NaUSY/30%活性炭^[25]	四步ESA	10	—	—	—	2.78	56.22	6.15
2019	浸渍PEI的碳化硅纤维^[26]	三步ESA	15	62.00	81.00	—	14.50	—	0.89
2019	沸石填充的碳纳米管^[26]	三步ESA	15	62.00	81.00	—	9.20	—	1.40
2019	82%沸石H-ZSM-5/18%活性炭^[27]	五步VESA	15	72.00	33.00	4.80×10^-4	2.04	—	6.58
2021	50%沸石13X/50%活性炭^[6]	—	15	—	—	—	—	19.00	—
2021	50%沸石13X/50%石墨^[6]	—	15	—	—	—	—	34.00	—
2022	47.5%沸石47.5%活性炭5％黏合剂^[30]	—	15	—	—	1.98×10^-4	—	—	—
2022	50%硅酸钾/50%活性炭^[64]	四步ESA	30	92.10		—	19.90	—	0.53

图7 能耗与回收率、纯度关系

图8 能耗与CO2进料浓度关系

图9 热力学第二定律效率与能耗、浓度的关系

图10 变电吸附碳捕集技术改进路线

图11 使用Autodesk Fusion 3软件设计的（左）和3D打印结构的（右）蜂窝巨石[6]

图12 可再生能源辅助驱动ESA

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