铂合金氧还原催化剂:合成、结构和性能

doi:10.1016/S1872-2067(19)63407-8

催化学报 ›› 2020, Vol. 41 ›› Issue (5): 739-755.DOI: 10.1016/S1872-2067(19)63407-8

铂合金氧还原催化剂:合成、结构和性能

王晓霞^a,b, Joshua Sokolowski^b, 刘辉^c, 武刚^b

a 华东理工大学机械与动力工程学院, 上海 200237, 中国;
b 纽约州立大学布法罗分校化学与生物工程学院, 纽约 14260, 美国;
c 上海动力储能电池系统工程技术有限公司, 上海 200241, 中国

收稿日期:2019-05-10 修回日期:2019-07-10 出版日期:2020-05-18 发布日期:2019-12-31
通讯作者: 武刚
基金资助:
国家自然科学基金（21805089）；上海市自然科学基金（16ZR1408600）；中央高校基本科研业务费（222201814024）.

Pt alloy oxygen-reduction electrocatalysts: Synthesis, structure, and property

Xiao Xia Wang^a,b, Joshua Sokolowski^b, Hui Liu^c, Gang Wu^b

a School of Mechanical and Power Engineering, East China University of Science and Technology, Shanghai 200237, China;
b Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York Buffalo, NY 14260, USA;
c Shanghai Power & Energy Storage Battery System Engineering Tech. Co. Ltd., Shanghai 200241, China

Received:2019-05-10 Revised:2019-07-10 Online:2020-05-18 Published:2019-12-31
Contact: S1872-2067(19)63407-8
Supported by:
This work was supported by the National Natural Science Foundation of China (21805089), Shanghai Natural Science Foundation of China (16ZR1408600), and the Fundamental Research Funds for the Central Universities (222201814024), and the financial support from U.S. Department of Energy, Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office.

摘要/Abstract

摘要： 质子交换膜燃料电池是一种将燃料中的化学能直接转化为电能的装置，它具有转化效率高、能量密度高、低温启动、易于操作等优点，因而被认为是最具发展前景的新能源利用方式，在电动汽车、便携电源及分散式电站有着广泛应用.但是，目前质子交换膜燃料电池技术的发展面临着巨大挑战，主要问题包括高成本、低功率密度和低寿命.众所周知，质子交换膜燃料电池中的阴极氧还原反应在酸性条件下是一个复杂的四电子过程，动力学速度缓慢，限制了电池的最终性能.目前大量使用的阴极氧还原催化剂是细小的铂或铂合金纳米颗粒负载在碳载体上，其成本占燃料电池总成本的比例最大.制约燃料电池商业化发展的另一个重要问题是电池寿命低，其中氧还原催化剂的稳定性是决定电池寿命的主要因素.在这样的研究背景下，如何降低催化剂中铂的用量、提高催化剂活性和稳定性显得尤为重要，这也是近年来国内外学者研究的热点.
在铂基合金催化剂中，通常采用过渡金属元素作为掺杂元素，由于原子半径不匹配（几何效应）以及电子结构不同（电子效应），合金催化剂表现出优于纯铂催化剂的催化性能.近几年，对于铂基合金催化剂的研究已取得重大进展，以合金组成和结构研究为基础，通过精确控制原子结构、调控表面电子状态以及制备工艺，获得了各种特殊形貌的催化剂，大大提高了催化活性.本文深入综述了近年来铂基合金氧还原催化剂制备、形貌和性能，特别关注了催化剂形貌和催化活性之间的关系.值得注意的是，具有有序原子排列的铂合金催化剂不仅在半电池中表现出优异活性，在实际质子交换膜燃料电池中也显示了很好的活性和稳定性.另一方面，碳载体的形貌及微观结构也对提高催化活性和稳定性起到决定性作用，通过化学手段加强金属纳米颗粒与碳载体之间的相互作用也是提高催化剂稳定性的重要途径.
尽管铂基氧还原催化剂在近几年取得了重要进展，但在实际商业化过程中还存在诸多挑战，本文在综述进展的基础上，对铂基催化剂的发展提出了展望.首先，对于氧还原反应机理仍需要深入研究，采用更加精确的理论模型模拟氧还原动力学过程，以获得影响催化活性的关键因素.其次，提高催化剂在膜电极中的催化活性和利用率.目前，氧还原催化剂在半电池测试中性能优异，但是实际燃料电池操作条件下其性能远不能达到要求，这与膜电极、催化剂层及扩散层结构相关.因此，基于不同铂基催化剂的特性，合理设计膜电极组件的结构是将催化剂进行实际应用的基础.最后，催化剂的稳定性仍需进一步提高，尽管目前大部分催化剂在实验室半电池研究中表现了很好的稳定性，但在实际燃料电池中的稳定性研究还不足，而且对催化剂在膜电极中性能衰退机理的研究也非常有限.因此，对于铂基氧还原催化剂的研发仍需要国内外科研工作者不懈的努力.

关键词: 质子交换膜燃料电池, 氧还原反应, 低铂催化剂, 催化活性, 稳定性

Abstract: Proton exchange membrane fuel cells (PEMFCs) are considered a promising power source for electric vehicles and stationary residential applications. However, current PEMFCs have several problems that require solutions, including high cost, insufficient power density, and limited performance durability. A kinetically sluggish oxygen reduction reaction (ORR) is primarily responsible for these issues. The development of advanced Pt-based catalysts is crucial for solving these problems if the large-scale application of PEMFCs is to be realized. In this review, we summarize the recent progress in the development of PtM alloy (M=Fe, Co, Ni, etc.) catalysts with an emphasis on ordered PtM intermetallic catalysts, which exhibit significantly enhanced activity and stability. In addition to exploring the intrinsic catalytic performance in traditional aqueous electrolytes via engineering nanostructures, morphologies, and crystallinity of PtM particles, we highlight recent efforts to study catalysts under real fuel cell environments by the membrane electrode assembly (MEA).

Key words: Proton exchange membrane fuel cell, Oxygen reduction reaction, Low Pt catalyst, Catalytic activity, Stability

王晓霞, Joshua Sokolowski, 刘辉, 武刚. 铂合金氧还原催化剂:合成、结构和性能[J]. 催化学报, 2020, 41(5): 739-755.

Xiao Xia Wang, Joshua Sokolowski, Hui Liu, Gang Wu. Pt alloy oxygen-reduction electrocatalysts: Synthesis, structure, and property[J]. Chinese Journal of Catalysis, 2020, 41(5): 739-755.

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铂合金氧还原催化剂:合成、结构和性能

Pt alloy oxygen-reduction electrocatalysts: Synthesis, structure, and property

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