质子交换膜燃料电池阴极非贵金属M-Nx/C型氧还原催化剂研究进展

doi:10.3866/PKU.WHXB202210036

物理化学学报 >> 2023, Vol. 39 >> Issue (8): 2210036.doi: 10.3866/PKU.WHXB202210036

所属专题：能源电催化

质子交换膜燃料电池阴极非贵金属M-N_x/C型氧还原催化剂研究进展

兰畅¹^,², 楚宇逸¹^,², 王烁¹^,², 刘长鹏¹, 葛君杰¹^,*(), 邢巍¹^,*()

¹ 中国科学院长春应用化学研究所, 长春 130022
² 中国科学技术大学应用化学与工程学院, 合肥 230026

收稿日期:2022-10-26 录用日期:2022-12-05 发布日期:2022-12-09
通讯作者: 葛君杰,邢巍 E-mail:gejj@ciac.ac.cn;xingwei@ciac.ac.cn
作者简介:第一联系人：
^†These authors contributed equally to this work.
基金资助:
国家科技重大专项(2018YFB1502700);国家自然科学基金(21633008);国家自然科学基金(21875243);国家自然科学基金(U1601211);吉林省科技发展计划(20200201001JC);吉林省科技发展计划(20190201270JC);吉林省科技发展计划(20180101030JC)

Research Progress of Proton-Exchange Membrane Fuel Cell Cathode Nonnoble Metal M-N_x/C-Type Oxygen Reduction Catalysts

Chang Lan¹^,², Yuyi Chu¹^,², Shuo Wang¹^,², Changpeng Liu¹, Junjie Ge¹^,*(), Wei Xing¹^,*()

¹ Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China
² School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, China

Received:2022-10-26 Accepted:2022-12-05 Published:2022-12-09
Contact: Junjie Ge, Wei Xing E-mail:gejj@ciac.ac.cn;xingwei@ciac.ac.cn
Supported by:
the National Science and Technology Major Project(2018YFB1502700);the National Natural Science Foundation of China(21633008);the National Natural Science Foundation of China(21875243);the National Natural Science Foundation of China(U1601211);the Jilin Province Science and Technology Development Program(20200201001JC);the Jilin Province Science and Technology Development Program(20190201270JC);the Jilin Province Science and Technology Development Program(20180101030JC)

摘要/Abstract

摘要：

氧还原反应(ORR)是燃料电池能量转换的关键步骤，开发高性能低成本的催化剂以替代铂族贵金属是推动燃料电池商业化的重要途径。本文综述了质子交换膜燃料电池非贵金属M-N_x/C型催化剂的最新研究进展，概括了氧还原反应的基础理论，系统展示了先进表征技术对活性位点鉴定和反应机理研究的作用，总结了M-N_x/C型催化剂近年来的代表工作和活性突破，阐述了稳定性问题的根源及对应的方案策略，我们认为M-N_x/C型催化剂未来的发展方向是理性设计具高位点密度和高稳定性的催化剂。

关键词: 质子交换膜燃料电池, 氧还原反应, 非贵金属催化剂, 稳定性, 电催化

Abstract:

Proton-exchange membrane fuel cells (PEMFCs) are an efficient and clean energy conversion technology with the advantage of zero pollution for transportation applications. The oxygen reduction reaction (ORR) is the key step in the energy conversion at the cathode, but the slow kinetics requires a high content of expensive platinum-group-metal (PGM) catalysts. Therefore, research on high-performance and inexpensive catalysts to replace PGM-based catalysts are essential to promote the commercialization of fuel cells. Single-atom catalysts (SACs) with highly active sites that are atomically dispersed on substrates exhibit unique advantages, such as maximum atomic utilization, abundant chemical structures, and extraordinary catalytic performances for multiple important reactions. Inspired by macrocyclic compounds with MN₄ active centers, the application of pyrolyzed M-N_x/C type SACs (M = Fe, Co, Mn, Ru, Cr, Zn, etc.) in the ORR has significantly progressed within the last ten years. Particularly, single-atom Fe-N-C catalysts have been extensively investigated, demonstrating high ORR activity, which indicates that the initial electrochemistry and fuel cell performance are similar to that of conventional Pt/C catalysts. However, in the oxidizing and acidic PEMFC cathode, Fe-N-C catalysts are degraded rapidly, which hinders the application of these nonprecious metal M-N_x/C-type catalysts. Several degradation mechanisms have been proposed over the past few years, such as carbon oxidation, demetallation, and waterflooding. However, the degradation mechanisms remain unknown and require further investigation of the underlying causes of the mechanism, degradation process, and coping strategies. To achieve the future commercialization of high-performance M-N_x/C catalysts, several key challenges are summarized with potential research guidelines proposed to overcome bottlenecks. This review summarizes the development history and state-of-the-art research progress on nonprecious metal M-N_x/C-type catalysts in PEMFCs. First, we introduce the basic theory of the ORR and the methods of advanced characterization techniques for active site identification and reaction mechanism analysis to gain a comprehensive understanding of the structure–performance relationship. Subsequently, the representative studies and recent advancements in M-N_x/C-type catalysts by experimental and theoretical calculations are presented. Additionally, we analyze the root cause of the stability problems and propose the corresponding solution strategies to promote the intrinsic electrocatalytic ORR activity and durability, including regulating the electronic structure and coordination environment, as well as altering the central metal atoms and guest groups. Finally, we propose that the future direction of M-N_x/C-type catalysts is the rational design of catalysts with a high site density and high stability. Moreover, improving the lifetime of nonprecious metal catalysts remains essential for feasible applications in the future.

Key words: Proton exchange membrane fuel cell, Oxygen reduction reaction, Non-precious metal catalyst, Stability, Electrocatalysis

兰畅, 楚宇逸, 王烁, 刘长鹏, 葛君杰, 邢巍. 质子交换膜燃料电池阴极非贵金属M-N_x/C型氧还原催化剂研究进展[J]. 物理化学学报, 2023, 39(8), 2210036. doi: 10.3866/PKU.WHXB202210036

Chang Lan, Yuyi Chu, Shuo Wang, Changpeng Liu, Junjie Ge, Wei Xing. Research Progress of Proton-Exchange Membrane Fuel Cell Cathode Nonnoble Metal M-N_x/C-Type Oxygen Reduction Catalysts[J]. Acta Phys. -Chim. Sin. 2023, 39(8), 2210036. doi: 10.3866/PKU.WHXB202210036

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202210036

https://www.whxb.pku.edu.cn/CN/Y2023/V39/I8/2210036

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Catalyst	Active site	Electrolyte	Halfwave potential/V (vs. RHE)	Maximum Power
TPI@Z8(SiO₂)-650-Z ⁵⁴	FeN₄	0.5 mol∙L⁻¹ H₂SO₄	0.823	H₂/2.5 bar O₂: 1.18 W∙cm⁻²
Cr/N/C-950 ²²	CrN₄	0.1 mol∙L⁻¹ HClO₄	0.773	–
Ru-SSC ²³	RuN₄	0.1 mol∙L⁻¹ HClO₄	0.824	H₂/1.5 bar O₂: 0.64 W∙cm⁻²
Ir-SAC ⁵⁵	IrN₄	0.1 mol∙L⁻¹ HClO₄	0.864	H₂/O₂: 0.932 W∙cm⁻²
FeCoN_x/C ²⁴	FeCoN₅-OH	0.1 mol∙L⁻¹ HClO₄	0.860	H₂/O₂: 0.819 W∙cm⁻²
Fe-N-C-YZ ⁵³	FeN₄	0.5 mol∙L⁻¹ H₂SO₄	0.916	H₂/air 300/1000 sccm: 0.558 W∙cm^–2
Mn(acac)₃@ZIF-NC ⁵⁷	MnN₄	0.5 mol∙L⁻¹ H₂SO₄	0.872	50%RH H₂/air 250 kPa: 0.674 W∙cm⁻²
Fe/NC-NaCl ⁵⁸	FeN₄	0.1 mol∙L⁻¹ HClO₄	0.832	H₂/O₂: 0.89 W∙cm⁻²
Cu-SAs/N-C ⁵⁹	CuN₄	0.1 mol∙L⁻¹ HClO₄ 0.1 mol∙L⁻¹ KOH	0.730 0.895	–
Ce-SAS/HPNC ⁶⁰	Ce-N₄/O₆	0.1 mol∙L⁻¹ HClO₄	0.862	H₂/2 bar O₂: 0.525 W∙cm^–2
Zn-N-C ⁶¹	ZnN₄	0.1 mol∙L⁻¹ HClO₄ 0.1 mol∙L⁻¹ KOH	0.746 0.873	–
Co-N-C ⁶²	CoN₄	0.5 mol∙L⁻¹ H₂SO₄	0.820	H₂/O₂: 0.64 W∙cm^–2

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质子交换膜燃料电池阴极非贵金属M-N_x/C型氧还原催化剂研究进展

Research Progress of Proton-Exchange Membrane Fuel Cell Cathode Nonnoble Metal M-N_x/C-Type Oxygen Reduction Catalysts

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质子交换膜燃料电池阴极非贵金属M-Nx/C型氧还原催化剂研究进展

Research Progress of Proton-Exchange Membrane Fuel Cell Cathode Nonnoble Metal M-Nx/C-Type Oxygen Reduction Catalysts

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质子交换膜燃料电池阴极非贵金属M-N_x/C型氧还原催化剂研究进展

Research Progress of Proton-Exchange Membrane Fuel Cell Cathode Nonnoble Metal M-N_x/C-Type Oxygen Reduction Catalysts