Applied Catalysis2022，Vol.30511.DOI:10.1016/j.apcatb.2021.121035

Clarifying the critical roles of iron in boosting oxygen reduction: Single Fe atoms anchored on carbon vacancies as efficient active sites

Tan F. Li W. Wang J. Shi Q. Yang X. Min C. Zhou L. Li Z. Zhang B. Zheng X. Li L. Zhang L.
Applied Catalysis2022，Vol.30511.DOI:10.1016/j.apcatb.2021.121035
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  • NSTL
  • Elsevier

Clarifying the critical roles of iron in boosting oxygen reduction: Single Fe atoms anchored on carbon vacancies as efficient active sites

Tan F. 1Li W. 1Wang J. 1Shi Q. 1Yang X. 1Min C. 2Zhou L. 2Li Z. 3Zhang B. 4Zheng X. 5Li L. 6Zhang L.7
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作者信息

  • 1. Faculty of Materials Science and Engineering Kunming University of Science and Technology
  • 2. Research Center for Analysis and Measurement Kunming University of Science and Technology
  • 3. Analysis Center Tsinghua University Tsinghua University
  • 4. Shenyang National Laboratory for Materials Science Institute of Metal Research Chinese Academy of Sciences
  • 5. National Synchrotron Radiation Laboratory (NSRL) University of Science and Technology of China
  • 6. Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied Physics Chinese Academy of Sciences
  • 7. Faculty of Materials Science and Engineering Yunnan University
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Abstract

? 2022 Elsevier B.V.Due to highly heterogeneity of pyrolyzed transition metal-nitrogen-carbon (M-N-C) catalyst, elucidating mechanisms of roles of metal in enhancing oxygen reduction reaction (ORR) is challenging. Here, we design a surface structurally-defined precursor with Fe-N coordination to atomically disperse iron (Fe) on N-doped carbon hollow microspheres surface (NHMs@Fe) by pyrolysis of the precursor. The obtained NHMs@Fe catalyst exhibits a high ORR activity comparable to commercial Pt/C catalyst. The detailed analyses confirmed that (i) Fe atoms are uniformly distributed on N-poor carbon surface, and (ii) the designed Fe-Nx coordination are destroyed and don't convert into Fe-Nx active sites after thermal activation. We find that single Fe atoms produced by carbothermal reduction are directly trapped into adjacent carbon vacancies generated by the removal of N to create active sites for ORR. This work not only reveals the origin of activity of Fe-N-C catalyst but also opens an avenue for preparation of high-performance M-N-C catalysts.

Key words

Carbon vacancy/Catalytic active site/Oxygen reduction reaction/Single iron atom/Structurally-defined precursor

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出版年

2022
Applied Catalysis

Applied Catalysis

ISSN：0926-3373
被引量18
参考文献量50
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