Recent progress of molecular design for highly stable alkaline anion exchange membranes

doi:10.11949/0438-1157.20210020

Abstract

Abstract:

Energy conversion and energy storage processes based on anion exchange membranes (alkaline ion membranes) are very important, including alkaline membrane fuel cells, alkaline membrane electrolysis of water to produce hydrogen, etc. This type of electrical membrane process will have a profound impact on the future energy structure influences. Existing anion exchange membranes often suffered from problems of poor alkali resistance and short life span, which severely restrict the development of efficient energy storage and conversion technologies. Recently, researchers have carried out a lot of novel molecular design for alkaline membrane materials of highly chemical stability. This review is based on the two perspectives of alkaline anion exchange membranes and the polymer backbone and cationic groups, focusing on the molecular design strategies including polyolefin and poly-aryl backbone structure, as well as non-metal or metal cationic groups. Moreover, regular methods and current deficiencies of high-stability alkaline anion exchange membranes structural design is summarized, and new ideas for synthesis of next generation high-performance materials for energy conversion processes is also proposed.

Key words: alkaline anion exchange membrane, alkali resistance, polymer backbone, cationic group, fuel cell, water electrolysis

摘要：

以阴离子交换膜（碱性离子膜）为基础的能量转化与储能过程十分重要，包括碱性膜燃料电池、碱性膜电解水制氢等，该类电膜过程对未来能源结构会产生深远影响。现有阴离子交换膜存在耐碱性差、性能衰减显著的问题，严重制约高效能源储存及转化技术发展。为了获得高稳定的碱性离子膜，近年来，围绕耐碱高分子材料的分子设计开展大量工作。本综述从碱性膜材料的高分子骨架和阳离子基团两个角度出发，针对膜材料耐碱性，重点阐述聚烯烃和聚芳基的主链结构，以及非金属中心、金属中心，两类阳离子的分子结构设计策略，展望高稳定碱性膜的结构设计规律及主要挑战，为设计与合成高性能碱性离子膜，满足清洁能源转化与储能膜过程提供新思路。

关键词: 碱性离子膜, 耐碱稳定性, 高分子骨架, 阳离子基团, 燃料电池, 电解水

CLC Number:

O 658.6⁺8

Zi'ang XU, Lei WAN, Kai LIU, Baoguo WANG. Recent progress of molecular design for highly stable alkaline anion exchange membranes[J]. CIESC Journal, 2021, 72(8): 3891-3906.

徐子昂, 万磊, 刘凯, 王保国. 高稳定碱性离子膜分子设计研究进展[J]. 化工学报, 2021, 72(8): 3891-3906.

Figures/Tables 16

Fig.1 Schematic of anion exchange membrane fuel cell (a) and anion exchange membrane water electrolysis(b)

Fig.2 Annual journal article publications included by Web of Science from 2006 to 2020. Keywords: (a) “Anion Exchange Membrane” & “Fuel Cell”；(b)“Anion Exchange Membrane” & “Water Electrolysis”. The total number of articles for 2018—2020 is statistics until October 2020

Fig.3 Factors affecting the design of stable anion exchange membranes

Fig.4 FxC9N based on Z-N coordination polymerization[29](a) synthesis route;(b) AEMFC durability test

Fig.5 AAEM-17 based on ring opening metathesis polymerization[30](a) synthesis route;(b) stability test based on conductivity variety according to time

Fig.6 Chemical stable QB-g-F based on side chain engineering[40](a) synthesis route & chemical structure;(b) stability test based on conductivity variety according to time under 2 mol·L-1 OH-, 60℃

Fig.7 PAP-BP-x & PAP-TP-x with poly-aryl backbone prepared by superacid catalysis[46](a) structure of polymer; (b) alkaline durability based on NMR change; (c) conductivity variety according to time under 1 mol·L-1 KOH, 100℃

Fig.8 Yamamoto coupling polymerization for poly-aryl backbone PAImXY[48](a) synthesis route; (b) water electrolysis stability test under 6 mol·L-1 KOH

Fig.9 Reported cationic groups for AEMs applications

Fig.10 Possible degradation mechanism of quaternary ammonium salt of alkyl chain under OH- attacking

Fig.11 PDPF-Qui based on quinuclidium cation groups[56](a) chemical structure; (b) alkaline durability monitored by NMR

Fig.12 Spiro-ionenes AEMs based on N?spirocyclic quaternary ammonium group[60](a) chemical structure & photographs of AEM; (b),(c) alkaline stability under different condition monitored by NMR

Fig.13 Alkaline stability based on model structure of imidazolium cations[66]

Fig.14 Pyrazolium cross-linked PXm-Tn for OH- transportation highway[67](a) chemical structure & synthesis route; (b) chemical stability test based on conductivity variety under 1 mol·L-1 KOH, 80℃; (c) AEMFC durability test

Fig.15 H-AEM-OH based on cobaltocenium center[32](a) chemical structure & synthesis route; (b) chemical stability test based on conductivity variety under 1 mol·L-1 KOH, 80℃

Table 1 Conductivity and alkali resistance of AEMs with different cationic groups

类别	阳离子基团	AEMs名称	聚合物主链	IEC/ (mmol·g^-1)	电导率/(mS·cm^-1)	稳定性	文献
非芳香型季铵盐	DBACO型	CL-QDPEEKOH	聚醚醚酮	1.2	51(55℃)	50%电导率保持(2 mol·L^-1 KOH， 60℃，120 h)	[54]
	奎宁型	PDPF-Qui	超酸催化聚芳基	1.99	100(80℃)	91.2%电导率保持(5 mol·L^-1 NaOH，90℃，168 h)	[56]
	哌啶型	PAP-TP	超酸催化聚芳基	2.37	193(95℃)	97%电导率保持(1 mol·L^-1 KOH，100℃，2000 h)	[46]
	吡咯型	PyrPIB	超酸催化聚芳基	1.79	49.08(80℃)	64.8%电导率保持(1 mol·L^-1 NaOH，80℃，1050 h)	[59]
	螺环型	Spiro-ionenes	螺环-阳离子聚合物	4	120(90℃)(与聚苯并咪唑共混后)	NMR谱图无变化(1 mol·L^-1 KOH，80℃，1800 h)	[60]
芳香型季铵盐	胍型	M-PAES-TMG	含氟聚芳醚	1.03	36（80℃）	63.9%电导率保持（0.5 mol·L^-1 NaOH，80℃， 382 h）	[75]
	咪唑型	Syne-IM PPO	聚苯醚	1.60	34（80℃）	95%电导率保持（1 mol·L^-1 KOH，80℃，48 h）	[64]
	吡唑型	PXm-Tn	全交联聚芳基	0.91	111.6（80℃）	76%电导率保持（1 mol·L^-1 KOH， 80℃,720 h）	[67]
季盐	氨基季型	AAEM-17	聚烯烃	0.67±0.1	22±1（22℃）	81.8%电导率保持（1 mol·L^-1 KOH，80℃，22 d）	[30]
季盐	芳基季型	TPQPOH	聚醚砜	1.09	27（20℃）	100%电导率保持（1 mol·L^-1 KOH，80℃，48 h）	[69]
金属盐	二茂钴型	H-AEM-OH	聚烯烃	1.86	90（90℃）	95%电导率保持（1 mol·L^-1 NaOH， 1个月）	[32]
金属盐	配位金属型	DCPD AEMs	聚烯烃	1.4	28.6（30℃）	7%质量损失（1 mol·L^-1 NaOH，80℃，24 h）	[33]

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