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作 者:兰畅 楚宇逸 王烁 刘长鹏[1] 葛君杰[1] 邢巍[1] Chang Lan;Yuyi Chu;Shuo Wang;Changpeng Liu;Junjie Ge;Wei Xing(Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,China;School of Applied Chemistry and Engineering,University of Science and Technology of China,Hefei 230026,China)
机构地区:[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
出 处:《物理化学学报》2023年第8期19-38,共20页Acta Physico-Chimica Sinica
基 金:国家科技重大专项(2018YFB1502700);国家自然科学基金(21633008,21875243,U1601211);吉林省科技发展计划(20200201001JC,20190201270JC,20180101030JC)资助项目。
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。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-groupmetal(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 an
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