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High Durability of Fe–N–C Single‐Atom Catalysts with Carbon Vacancies toward the Oxygen Reduction Reaction in Alkaline Media

Hao TianCentre for Clean Energy Technology School of Mathematical and Physical Sciences Faculty of Science University of Technology Sydney Broadway NSW 2007 AustraliaAiling SongHebei Key Laboratory of Applied Chemistry College of Environmental and Chemical Engineering Yanshan University Qinhuangdao 066004 ChinaPeng ZhangKey Laboratory for Water Quality and Conservation of the Pearl River Delta Ministry of Education Institute of Environmental Research at Greater Bay Guangzhou University Guangzhou 510006 ChinaKaian SunDepartment of Chemistry Tsinghua University Beijing 100084 ChinaJingjing WangNorthwest Institute of Eco‐Environment and Resources Chinese Academy of Sciences Lanzhou 730000 ChinaBing SunCentre for Clean Energy Technology School of Mathematical and Physical Sciences Faculty of Science University of Technology Sydney Broadway NSW 2007 AustraliaQiaohui FanNorthwest Institute of Eco‐Environment and Resources Chinese Academy of Sciences Lanzhou 730000 ChinaGuangjie ShaoHebei Key Laboratory of Applied Chemistry College of Environmental and Chemical Engineering Yanshan University Qinhuangdao 066004 ChinaChen ChenDepartment of Chemistry Tsinghua University Beijing 100084 ChinaHao LiuCentre for Clean Energy Technology School of Mathematical and Physical Sciences Faculty of Science University of Technology Sydney Broadway NSW 2007 AustraliaYadong LiDepartment of Chemistry Tsinghua University Beijing 100084 ChinaGuoxiu WangCentre for Clean Energy Technology School of Mathematical and Physical Sciences Faculty of Science University of Technology Sydney Broadway NSW 2007 Australia

2023en

ABI

Annotatsiya

Abstract Single‐atom catalysts (SACs) have attracted extensive interest to catalyze the oxygen reduction reaction (ORR) in fuel cells and metal–air batteries. However, the development of SACs with high selectivity and long‐term stability is a great challenge. In this work, carbon vacancy modified Fe–N–C SACs (Fe H –N–C) are practically designed and synthesized through microenvironment modulation, achieving high‐efficient utilization of active sites and optimization of electronic structures. The Fe H –N–C catalyst exhibits a half‐wave potential ( E 1/2 ) of 0.91 V and sufficient durability of 100 000 voltage cycles with 29 mV E 1/2 loss. Density functional theory (DFT) calculations confirm that the vacancies around metal–N 4 sites can reduce the adsorption free energy of OH*, and hinder the dissolution of metal center, significantly enhancing the ORR kinetics and stability. Accordingly, Fe H –N–C SACs presented a high‐power density and long‐term stability over 1200 h in rechargeable zinc–air batteries (ZABs). This work will not only guide for developing highly active and stable SACs through rational modulation of metal–N 4 sites, but also provide an insight into the optimization of the electronic structure to boost electrocatalytical performances.

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Identifikatorlar

DOI: 10.1002/adma.202210714

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