聚酰亚胺薄膜在氢气分离中的研究进展

doi:10.16085/j.issn.1000-6613.2022-2040

化工进展 ›› 2023, Vol. 42 ›› Issue (10): 5232-5248.DOI: 10.16085/j.issn.1000-6613.2022-2040

聚酰亚胺薄膜在氢气分离中的研究进展

蔡铭威¹(), 王知¹, 卢小闯², 庄俊伟³, 吴嘉豪¹, 张诗洋¹(), 闵永刚¹()

^1.广东工业大学材料与能源学院，广东广州 510006
^2.慧迈材料科技（广东）有限公司，广东佛山 528000
^3.广州大学土木工程学院，广东广州 510006

收稿日期:2022-11-02 修回日期:2022-12-06 出版日期:2023-10-15 发布日期:2023-11-11
通讯作者: 张诗洋,闵永刚
作者简介:蔡铭威（1999—），男，硕士研究生，研究方向为气体分离。E-mail：2112102037@mail2.gdut.edu.cn。
基金资助:
广东省“珠江人才计划”引进创新创业团队项目(2016ZT06C412);广州红棉项目(HMJH-2020-0012);佛山引进创新创业团队(1920001000108)

Polyimide membranes for hydrogen separation: A review

CAI Mingwei¹(), WANG Zhi¹, LU Xiaochuang², ZHUANG Junwei³, WU Jiahao¹, ZHANG Shiyang¹(), MIN Yonggang¹()

^1.School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, Guangdong, China
^2.Huimai Material Technology (Guangdong) Co. , Ltd. , Foshan 528000, Guangdong, China
^3.School of Civil Engineering, Guangzhou University, Guangzhou 510006, Guangdong, China

Received:2022-11-02 Revised:2022-12-06 Online:2023-10-15 Published:2023-11-11
Contact: ZHANG Shiyang, MIN Yonggang

摘要/Abstract

摘要：

氢气是重要的工业原料和清洁燃料，极具经济和社会价值。氢气在利用前需进行分离提纯。由于膜分离技术具有高能效、简单和可连续操作等优点被广泛用于氢气分离。聚酰亚胺膜具有优良的气体选择性、机械性能、热稳定性、耐化学稳定性、耐水解和耐腐蚀等优点成为最具有潜力的膜材料之一。然而，传统聚酰亚胺膜存在自由体积小、气体渗透性和抗塑性差等缺点无法用于大规模H₂分离。因此，需要对传统聚酰亚胺进行改性以更好地分离氢气。本文综述了近年来聚酰亚胺薄膜在氢气分离的研究现状，总结了目前聚酰亚胺气体分离膜存在的关键问题，并从无机粒子共混、MOFs共混、聚合物共混、交联和超支化改性及单体结构改性六个方面，详细介绍了聚酰亚胺气体分离膜的改性研究成果，并展望了聚酰亚胺气体分离膜的发展趋势，为未来高效分离膜的研发提供参考。

关键词: 聚酰亚胺, 气体分离, 氢, 聚合物, 渗透率, 选择性

Abstract:

Hydrogen is important as industrial raw material and clean fuel, which shows great economic and social value. Hydrogen separation is necessary before hydrogen utilization. Membrane-based technology is a H₂ separation technology with features of high energy efficiency, simplicity and continuous operation. Polyimide (PI) membrane as one of the most promising materials has been widely applied in the fields of H₂ separation due to its excellent gas selectivity, mechanical properties, thermal stability, chemical stability, hydrolysis resistance and corrosion resistance. However, driven by some disadvantages of small free volume, poor gas permeability and plastic resistance, traditional polyimide membrane cannot be widely used for large-scale H₂ separation. Therefore, the traditional polyimide needs to be modified to separate H₂ preferably. In this review, the recent research status of polyimide film in hydrogen separation was reviewed, and monomer structure modification and the key problems of polyimide gas separation membrane were summarized. Focusing on six kinds of modifications of inorganic particle blending, MOFs blending, polymer blending, cross-linking, hyperbranching modification and monomer structure modification, the research achievements of polyimide gas separation membrane modification were introduced in detail, and the development trend of polyimide gas separation membrane was looked forward, providing a reference for the research and development of efficient separation membrane in the future.

Key words: polyimide, gas separation, hydrogen, polymers, permeability, selectivity

中图分类号:

TQ17

蔡铭威, 王知, 卢小闯, 庄俊伟, 吴嘉豪, 张诗洋, 闵永刚. 聚酰亚胺薄膜在氢气分离中的研究进展[J]. 化工进展, 2023, 42(10): 5232-5248.

CAI Mingwei, WANG Zhi, LU Xiaochuang, ZHUANG Junwei, WU Jiahao, ZHANG Shiyang, MIN Yonggang. Polyimide membranes for hydrogen separation: A review[J]. Chemical Industry and Engineering Progress, 2023, 42(10): 5232-5248.

图/表 15

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复合膜	渗透性/barrer			选择性
复合膜	H₂	CO₂	CH₄	H₂/CH₄	H₂/CO₂
Matrimid 5218/20% DDR^®[40]	34.9		0.093	375.27
Matrimid 5218/15% DDR^®[40]	29.37		0.095	309.16
PI/ZIF-7-III^[67]	322.01±28.66	74.08±1.73	1.87±0.07	172.24±8.50	4.35±0.29
PI/ZIF-7-I^[67]	921.44±100.46	407.41±50.05	13.67±1.20	67.42±1.45	2.26±0.03
25% ZIF-8/6FDA-BI^[68]	79.4±12.3		0.56±0.036	142.6±29.5
20% ZIF-8/6FDA-BI^[68]	78.5±5.84		0.35±0.033	223.9±16.7
6FDA-DAM:DABA(3∶2)/10% ZIF-8-90(30)^[69]	301	187	5.41	55.7	1.61
6FDA-DAM:DABA(3∶2)/10% ZIF-8-90(50)^[69]	276	174	4.74	58.3	1.58
2% A-SWNT^[58]	122±3	63±1	1.4±0.1	88±3	1.9±0.1
20%-COOH-PI/NH₂-UiO-66^[66]	1180	995	43	27.2	1.18
PSF/PI^[77]	348	86			4.04
PI/PBI^[78]	86	2.77			31
PI/TB 120℃，16h^[80]	77.1	18.4	0.16	481.8	4.19
PI/TB 150℃，16h^[80]	86.8	23.1	0.21	413.3	3.75

复合膜	渗透性/barrer			选择性
复合膜	H₂	CO₂	CH₄	H₂/CH₄	H₂/CO₂
Matrimid 5218/20% DDR^®[40]	34.9		0.093	375.27
Matrimid 5218/15% DDR^®[40]	29.37		0.095	309.16
PI/ZIF-7-III^[67]	322.01±28.66	74.08±1.73	1.87±0.07	172.24±8.50	4.35±0.29
PI/ZIF-7-I^[67]	921.44±100.46	407.41±50.05	13.67±1.20	67.42±1.45	2.26±0.03
25% ZIF-8/6FDA-BI^[68]	79.4±12.3		0.56±0.036	142.6±29.5
20% ZIF-8/6FDA-BI^[68]	78.5±5.84		0.35±0.033	223.9±16.7
6FDA-DAM:DABA(3∶2)/10% ZIF-8-90(30)^[69]	301	187	5.41	55.7	1.61
6FDA-DAM:DABA(3∶2)/10% ZIF-8-90(50)^[69]	276	174	4.74	58.3	1.58
2% A-SWNT^[58]	122±3	63±1	1.4±0.1	88±3	1.9±0.1
20%-COOH-PI/NH₂-UiO-66^[66]	1180	995	43	27.2	1.18
PSF/PI^[77]	348	86			4.04
PI/PBI^[78]	86	2.77			31
PI/TB 120℃，16h^[80]	77.1	18.4	0.16	481.8	4.19
PI/TB 150℃，16h^[80]	86.8	23.1	0.21	413.3	3.75

复合膜	渗透性/barrer			选择性
复合膜	H₂	CO₂	CH₄	H₂/CH₄	H₂/CO₂
6F-AP/DA-400^[119]	196.4±9.8	94.3±4.7	2.18±0.22	89.17	2.08
Co-80/20^[133]	380	261	6.7	57	1.45
Co-50/50^[133]	155	67	1.3	119	2.31
PES∶P84=75∶25^[147]	105.6	15.36	—	—	6.87
PDA∶BuDA=0.8∶0.2^[137]	91100	11619.89	—	—	7.84
Cross-linked P84^[151]	47	—	3.35	—	14
HBIN-Is^[176]	78.7	27.3	0.37	213	2.88
4MTBDA-PMDA^[177]	3300	—	390	8.46	—

复合膜	渗透性/barrer			选择性
复合膜	H₂	CO₂	CH₄	H₂/CH₄	H₂/CO₂
6F-AP/DA-400^[119]	196.4±9.8	94.3±4.7	2.18±0.22	89.17	2.08
Co-80/20^[133]	380	261	6.7	57	1.45
Co-50/50^[133]	155	67	1.3	119	2.31
PES∶P84=75∶25^[147]	105.6	15.36	—	—	6.87
PDA∶BuDA=0.8∶0.2^[137]	91100	11619.89	—	—	7.84
Cross-linked P84^[151]	47	—	3.35	—	14
HBIN-Is^[176]	78.7	27.3	0.37	213	2.88
4MTBDA-PMDA^[177]	3300	—	390	8.46	—

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聚酰亚胺薄膜在氢气分离中的研究进展

Polyimide membranes for hydrogen separation: A review

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