Energy & Environmental Materials >

2024 , Vol. 7 >Issue 2: 12560

DOI: https://doi.org/10.1002/eem2.12560

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

  • Shidong Li 1 ,
  • Lixue Xia 1 ,
  • Jiantao Li 4 ,
  • Zhuo Chen 1 ,
  • Wei Zhang 1 ,
  • Jiexin Zhu 1 ,
  • Ruohan Yu 5 ,
  • Fang Liu 5 ,
  • Sungsik Lee 6 ,
  • Yan Zhao , 7,8 ,
  • Liang Zhou , 1,2,3 ,
  • Liqiang Mai , 1,2,3
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  • 1. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
  • 2. Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory, Foshan 528200, China
  • 3. Hubei Longzhong Laboratory, Xiangyang 441000, China
  • 4. Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, IL 60439, USA
  • 5. NRC (Nanostructure Research Centre), Wuhan University of Technology, Wuhan 430070, China
  • 6. X-ray Science Division, Advanced Photon Sources, Argonne National Laboratory, 9700 South Cass, Avenue, Lemont, IL 60439, USA
  • 7. State Key Laboratory of Silicate Materials for Architectures, International School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, China
  • 8. The Institute of Technological Sciences, Wuhan University, Wuhan 430072, China
yan2000@whut.edu.cn
liangzhou@whut.edu.cn
mlq518@whut.edu.cn

Received date: 06 Oct 2022

Revised date: 08 Nov 2022

Copyright

2022 2022 The Authors. Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.
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Abstract

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.

Key words： coordination structure; electronic configuration; FeN4 moiety; oxygen reduction reaction; sulfur doping

Cite this article

Shidong Li , Lixue Xia , Jiantao Li , Zhuo Chen , Wei Zhang , Jiexin Zhu , Ruohan Yu , Fang Liu , Sungsik Lee , Yan Zhao , Liang Zhou , Liqiang Mai . Tuning Structural and Electronic Configuration of FeN4 via External S for Enhanced Oxygen Reduction Reaction[J]. Energy & Environmental Materials, 2024 , 7(2) : 12560 . DOI: 10.1002/eem2.12560

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