Tuning Structural and Electronic Configuration of FeN4 via External S for Enhanced Oxygen Reduction Reaction
作者机构：State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Chemical Sciences and Engineering Division Argonne National Laboratory NRC (Nanostructure Research Centre) Wuhan University of Technology X-ray Science Division Advanced Photon Sources Argonne National Laboratory State Key Laboratory of Silicate Materials for Architectures International School of Materials Science and Engineering Wuhan University of Technology The Institute of Technological Sciences Wuhan University Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Hubei Longzhong Laboratory
出 版 物：《Energy & Environmental Materials》 (能源与环境材料(英文))
年 卷 期：2024年第7卷第2期
页 面：97-105页
核心收录：
学科分类：0808[工学-电气工程] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 0805[工学-材料科学与工程（可授工学、理学学位）]
基 金：supported by the National Key Research and Development Program of China (Grant No.2020YFA0715000) the National Natural Science Foundation of China (Grant No.52127816) supported by the U.S.Department of Energy (DOE),Office of Energy Efficiency and Renewable Energy,Vehicle Technologies Office the DOE Office of Science by UChicago Argonne LLC under contract no.DE-AC02-06CH11357 the Advanced Photon Source (APS),a U.S.Department of Energy (DOE) Office of Science User Facility,operated for the DOE Office of Science by Argonne National Laboratory under Contract No.DE-AC02-06CH11357
主 题：coordination structure electronic configuration FeN4 moiety oxygen reduction reaction sulfur doping
摘 要：The Fe–N–C material represents an attractive oxygen reduction reaction electrocatalyst, and the FeN4moiety has been identified as a very competitive catalytic active site. Fine tuning of the coordination structure of FeN4has 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 FeN4active 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 FeN4active sites are optimized, thus promoting the oxygen reduction reaction activity. This work explores the key point in electronic configuration and coordination environment tuning of FeN4through S doping and provides new insight into the construction of M–N–C-based oxygen reduction reaction catalysts.
同方期刊数据库