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Engineering Unsymmetrically Coordinated Fe Sites via Heteroatom Pairs Synergetic Contribution for Efficient Oxygen Reduction.

Authors
  • An, Qizheng1
  • Zhang, Xu2
  • Yang, Chenyu1
  • Su, Hui3
  • Zhou, Wanlin1
  • Liu, Meihuan1
  • Zhang, Xiuxiu1
  • Sun, Xuan1
  • Bo, Shuowen1
  • Yu, Feifan1, 4
  • Jiang, Jingjing1
  • Zheng, Kun2
  • Liu, Qinghua1
  • 1 National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui, 230029, P. R. China. , (China)
  • 2 Beijing Key Lab of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100124, P. R. China. , (China)
  • 3 Key Laboratory of Light Energy Conversion Materials of Hunan Province College, College of Chemistry and Chemical Engineering, Hunan Normal University, Changsha, Hunan, 410081, P. R. China. , (China)
  • 4 School of Chemistry and Chemical Engineering, Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan, Shihezi University, Shihezi, 832003, P. R. China. , (China)
Type
Published Article
Journal
Small
Publisher
Wiley (John Wiley & Sons)
Publication Date
Dec 01, 2023
Volume
19
Issue
49
Identifiers
DOI: 10.1002/smll.202304303
PMID: 37566779
Source
Medline
Keywords
Language
English
License
Unknown

Abstract

Single-atom Fe catalysts are considered as the promising catalysts for oxygen reduction reaction (ORR). However, the high electronegativity of the symmetrical coordination N atoms around Fe site generally results in too strong adsorption of *OOH intermediates on the active site, severely limiting the catalytic performance. Herein, a "heteroatom pair synergetic modulation" strategy is proposed to tailor the coordination environment and spin state of Fe sites, enabling breaking the shackles of unsuitable adsorption of intermediate products on the active centers toward a more efficient ORR pathway. The unsymmetrically Co and B heteroatomic coordinated Fe single sites supported on an N-doped carbon (Fe─B─Co/NC) catalyst perform excellent ORR activity with high half-wave potential (E1/2 ) of 0.891 V and a large kinetic current density (Jk ) of 60.6 mA cm-2 , which is several times better than those of commercial Pt/C catalysts. By virtue of in situ electrochemical impedance and synchrotron infrared spectroscopy, it is observed that the optimized Fe sites can effectively accelerate the evolution of O2 into the *O intermediate, overcoming the sluggish O─O bond cleavage of the *OOH intermediate, which is responsible for fast four-electron reaction kinetics. © 2023 Wiley-VCH GmbH.

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