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Inter-site structural heterogeneity induction of single atom Fe catalysts for robust oxygen reduction

Author

Listed:
  • Peng Zhang

    (China University of Petroleum (East China))

  • Hsiao-Chien Chen

    (Chang Gung University
    Chang Gung Memorial Hospital)

  • Houyu Zhu

    (China University of Petroleum (East China))

  • Kuo Chen

    (China University of Petroleum (East China))

  • Tuya Li

    (China University of Petroleum (East China))

  • Yilin Zhao

    (China University of Petroleum (East China))

  • Jiaye Li

    (China University of Petroleum (East China))

  • Ruanbo Hu

    (Beijing University of Chemical Technology)

  • Siying Huang

    (China University of Petroleum (East China))

  • Wei Zhu

    (Beijing University of Chemical Technology)

  • Yunqi Liu

    (China University of Petroleum (East China))

  • Yuan Pan

    (China University of Petroleum (East China))

Abstract

Metal-nitrogen-carbon catalysts with hierarchically dispersed porosity are deemed as efficient geometry for oxygen reduction reaction (ORR). However, catalytic performance determined by individual and interacting sites originating from structural heterogeneity is particularly elusive and yet remains to be understood. Here, an efficient hierarchically porous Fe single atom catalyst (Fe SAs-HP) is prepared with Fe atoms densely resided at micropores and mesopores. Fe SAs-HP exhibits robust ORR performance with half-wave potential of 0.94 V and turnover frequency of 5.99 e−1s−1site−1 at 0.80 V. Theoretical simulations unravel a structural heterogeneity induced optimization, where mesoporous Fe-N4 acts as real active centers as a result of long-range electron regulation by adjacent microporous sites, facilitating O2 activation and desorption of key intermediate *OH. Multilevel operando characterization results identify active Fe sites undergo a dynamic evolution from basic Fe-N4 to active Fe-N3 under working conditions. Our findings reveal the structural origin of enhanced intrinsic activity for hierarchically porous Fe-N4 sites.

Suggested Citation

  • Peng Zhang & Hsiao-Chien Chen & Houyu Zhu & Kuo Chen & Tuya Li & Yilin Zhao & Jiaye Li & Ruanbo Hu & Siying Huang & Wei Zhu & Yunqi Liu & Yuan Pan, 2024. "Inter-site structural heterogeneity induction of single atom Fe catalysts for robust oxygen reduction," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-46389-3
    DOI: 10.1038/s41467-024-46389-3
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    References listed on IDEAS

    as
    1. Jiantao Fan & Ming Chen & Zhiliang Zhao & Zhen Zhang & Siyu Ye & Shaoyi Xu & Haijiang Wang & Hui Li, 2021. "Bridging the gap between highly active oxygen reduction reaction catalysts and effective catalyst layers for proton exchange membrane fuel cells," Nature Energy, Nature, vol. 6(5), pages 475-486, May.
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    3. Wanlin Zhou & Hui Su & Weiren Cheng & Yuanli Li & Jingjing Jiang & Meihuan Liu & Feifan Yu & Wei Wang & Shiqiang Wei & Qinghua Liu, 2022. "Regulating the scaling relationship for high catalytic kinetics and selectivity of the oxygen reduction reaction," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    4. Yazhou Zhou & Xiafang Tao & Guangbo Chen & Ruihu Lu & Ding Wang & Ming-Xi Chen & Enquan Jin & Juan Yang & Hai-Wei Liang & Yan Zhao & Xinliang Feng & Akimitsu Narita & Klaus Müllen, 2020. "Multilayer stabilization for fabricating high-loading single-atom catalysts," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
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