Tuning Structural and Electronic Configuration of FeN4 via External S for Enhanced Oxygen Reduction Reaction

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外文摘要：The Fe-N-C material represents an attractive oxygen reduction reaction electrocatalyst,and the FeN4 moiety has been identified as a very competitive catalytic active site.Fine tuning of the coordination structure of FeN4 has an essential impact on the catalytic performance.Herein,we construct a sulfur-modified Fe-N-C catalyst with controllable local coordination environment,where the Fe is coordinated with four in-plane N and an axial external S.The external S atom affects not only the electron distribution but also the spin state of Fe in the FeN4 active site.The appearance of higher valence states and spin states for Fe demonstrates the increase in unpaired electrons.With the above characteristics,the adsorption and desorption of the reactants at FeN4 active sites are optimized,thus promoting the oxygen reduction reaction activity.This work explores the key point in electronic configuration and coordination environment tuning of FeN4 through S doping and provides new insight into the construction of M-N-C-based oxygen reduction reaction catalysts.

外文关键词：

coordination structureelectronic configurationFeN4 moietyoxygen reduction reactionsulfur doping

作者：

Shidong Li、Lixue Xia、Jiantao Li、Zhuo Chen、Wei Zhang、Jiexin Zhu、Ruohan Yu、Fang Liu、Sungsik Lee、Yan Zhao、Liang Zhou、Liqiang Mai

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作者单位：

State Key Laboratory of Advanced Technology for Materials Synthesis and Processing,Wuhan University of Technology,Wuhan 430070,China

Chemical Sciences and Engineering Division,Argonne National Laboratory,9700 South Cass Avenue,Lemont,IL 60439,USA

NRC(Nanostructure Research Centre),Wuhan University of Technology,Wuhan 430070,China

X-ray Science Division,Advanced Photon Sources,Argonne National Laboratory,9700 South Cass,Avenue,Lemont,IL 60439,USA

State Key Laboratory of Silicate Materials for Architectures,International School of Materials Science and Engineering,Wuhan University of Technology,Wuhan 430070,China

The Institute of Technological Sciences,Wuhan University,Wuhan 430072,China

Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory,Foshan 528200,China

Hubei Longzhong Laboratory,Xiangyang 441000,China

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基金：

National Key Research and Development Program of ChinaNational Natural Science Foundation of ChinaU.S.Department of Energy(DOE)Office of Energy Efficiency and Renewable Energy,Vehicle Technologies OfficeArgonne National Laboratory is operated for the DOE Office of Science by UChicago Argonne LLCU.S.Department of Energy(DOE)Office of Science User Facility,operated for the DOE Office of Science by Argonne National Laborato

项目编号：

2020YFA071500052127816DE-AC02-06CH11357DE-AC02-06CH11357

出版年：

2024

DOI：

10.1002/eem2.12560

能源与环境材料(英文)

ISSN：

年,卷(期)：2024.7(2)