质子交换膜燃料电池中氧还原反应抗毒性电催化剂研究进展

doi:10.16085/j.issn.1000-6613.2022-2004

摘要/Abstract

摘要：

在质子交换膜燃料电池（proton exchange membrane fuel cell，PEMFC）中，出于成本和实用性等方面的考虑，氧还原反应所需氧气基本都来自于空气。而空气中存在的污染物，如SO₂、NO₂等都会导致阴极Pt催化剂中毒。因此，提高催化剂的抗毒性就成为推动PEMFC规模化实际应用的关键问题之一。本文介绍了PEMFC氧还原催化剂抗毒性的研究进展，并分析其抗中毒机理。目前，抗毒性阴极催化剂已取得一定的突破，其主要可分为铂基改性催化剂、非贵金属催化剂和非金属碳基催化剂，通过抑制毒化物与铂之间的电子作用、增强溢出效应、锚定金属原子、引入杂原子（如氮、磷）、采用不易中毒的金属等方式可增强催化剂的抗毒性。与此同时，抗毒性催化剂也面临一定的问题，如催化剂导电性下降、活性降低、制备复杂等。如何在保持催化剂活性和稳定性的同时，开发出具有良好抗毒性的催化剂已成为研究人员的重点研究方向。

关键词: 燃料电池, 催化剂, 抗毒性, 氧还原

Abstract:

In proton exchange membrane fuel cell (PEMFC), for the sake of cost and practicality, the oxygen required for oxygen reduction reaction is basically from air. However, the pollutants in the air, such as SO₂ and NO₂, will lead to the poisoning of Pt catalyst. Therefore, improving the anti-toxicity of the catalyst has become one of the key issues to promote the large-scale application of PEMFC. The research progresses in the development of anti-toxicity catalysts for oxygen reduction reaction (ORR) and the anti-toxicity mechanism were introduced in this paper. At present, many ORR catalysts has been developed, mainly including platinum-based catalysts, non-noble metal catalysts and carbon-based catalysts. Their anti-toxicity could be improved mainly by inhibiting the electronic interaction between poisonous substance and catalyst, enhancing the spillover effects, reducing the oxidation potential of poisonous substance, introducing heteroatom (such as nitrogen, phosphorus), etc. At the same time, it is faced with some problems, such as the decrease of catalyst conductivity and activity and the complex preparation procedure. How to develop a catalyst with good anti-toxicity while maintaining its activity and stability has become a key research direction.

Key words: fuel cells, electrocatalyst, anti-toxicity, oxygen reduction reaction

中图分类号:

TK91

张启, 赵红, 荣峻峰. 质子交换膜燃料电池中氧还原反应抗毒性电催化剂研究进展[J]. 化工进展, 2023, 42(9): 4677-4691.

ZHANG Qi, ZHAO Hong, RONG Junfeng. Research progress of anti-toxicity electrocatalysts for oxygen reduction reaction in PEMFC[J]. Chemical Industry and Engineering Progress, 2023, 42(9): 4677-4691.

图/表 20

图1 质子交换膜燃料电池工作原理

表1 污染物浓度对电流的影响[14]

污染物	浓度/mg·m^-3	最大电流降/%	最小电流降/%	平均电流降/%
SO₂	0.286	6	0	2
	2.86	88	53	62
	11.44	95	67	85
NO₂	2.05	13	1	4
	20.50	91	31	66
	30.75	95	42	69
NO	1.34	63	11	33
	13.40	96	36	67
	20.10	97	43	72
NH₃	0.759	4	0	1
	2.28	34	0	9
	6.072	75	30	51

图2 在电池温度为70℃和电池电位为0.7V时，电流随毒化物浓度的变化曲线[14]

图3 氧还原活性作为氧结合能函数的趋势[39]

图4 催化剂中毒前后催化性能图[40][Pt担载量：JM Pt/C和Pt-MoO3/C分别为0.1353mg/cm2和0.08413mg/cm2]

表2 S和SO3在Pt(111)和PtMo(111)上的吸附能和距离[42]

结构	吸附能 /kJ·mol^-1	距离/nm
S/Pt(111)	-604.0	0.2310	0.2311	0.2312
S/PtMo(111)	-466.8	0.2353	0.2355	0.2354（S—Mo）
SO₃/Pt(111)	-282.8	0.2291	0.2153（O—Pt）	0.2160（O—Pt）
SO₃/PtMo(111)	-114.6	0.2222	0.2130（O—Pt）	0.1964（O—Mo）

图5 催化剂的TEM和循环伏安曲线[43]

图6 催化剂在毒化后进行5次连续循环伏安性能[44]

图7 在0.6V下Vulcan碳上的铂（Pt/C-MEA）和石墨烯上的铂（Pt/G-MEA）暴露于SO 2 的电流[47]

表3 Pt/C与质量分数5% WO x -Pt/C在经过一定浓度毒化物毒化后的SO x 初始覆盖率和损失程度[48]

毒化物浓度 /mol·L^-1	Pt/C		5% WO _x -Pt/C
毒化物浓度 /mol·L^-1	初始覆盖率	损失程度/%	初始覆盖率	损失程度/%
0.001	0.50±0.04	37±2	0.53±0.0.4	45±2
0.01	0.84±0.06	45±3	0.85±0.05	50±2
0.1	1.00±0.07	43±3	1.00±0.06	47±3

图8 WO x 促进碳载Pt催化剂上SO x 氧化的机理[48]

图9 催化剂毒化前后性能图和抗毒化作用原理[51]

图10 催化剂的电镜图像和稳定性测试结果[53]

表4 Fe-N4、Fe-N2C2和N掺杂石墨烯对O2、NO、NO2、CO和SO2的吸附能[54]

吸附物	吸附能/eV
吸附物	Fe-N₄	Fe-N₂C₂	N掺杂石墨烯
O₂	-1.01	-2.34	-0.15
SO₂	-0.81	-1.63	-0.17
NO	-1.97	-3.37	-0.09
NO₂	-1.45	-2.63	-0.43
CO	-1.61	-2.09	-0.01

图11 C-COP-P-M的合成及其结构示意图[55]

图12 T-FeN4、T-FeN3、G-FeN4和R-FeN2上吸附的CO和O 2 的优化结构[56][灰色、蓝色、紫色和红色表示C、N、Fe和O原子]

图13 CN x 和FeNC在经过CO毒化前后的极化曲线[59]

图14 H 2 S处理对Pt/Vulcan碳催化剂和CN x 催化剂氧还原活性的影响[60]

图15 催化剂催化ORR示意图和抗中毒性测试结果[63]

图16 PNC的ORR性能和抗中毒效果的图解 [64]

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