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Identifying the active sites in unequal iron-nitrogen single-atom catalysts

Author

Listed:
  • Liang Huang

    (Chinese Academy of Sciences
    University of Science and Technology of China)

  • Qiong Liu

    (Chinese Academy of Sciences)

  • Weiwei Wu

    (Chinese Academy of Sciences
    University of Science and Technology of China)

  • Ge Gao

    (Chinese Academy of Sciences)

  • Xiliang Zheng

    (Chinese Academy of Sciences)

  • Jin Wang

    (University of Chinese Academy of Sciences
    State University of New York at Stony Brook)

  • Shaojun Dong

    (Chinese Academy of Sciences
    University of Science and Technology of China)

Abstract

Single-atom catalysts (SACs) have become one of the most attractive frontier research fields in catalysis and energy conversion. However, due to the atomic heterogeneity of SACs and limitations of ensemble-averaged measurements, the essential active sites responsible for governing specific catalytic properties and mechanisms remain largely concealed. In this study, we develop a quantitative method of single-atom catalysis–fluorescence correlation spectroscopy (SAC-FCS), leveraging the atomic structure-dependent catalysis kinetics and single-turnover resolution of single-molecule fluorescence microscopy. This method enables us to investigate the oxidase-like single-molecule catalysis on unidentical iron-nitrogen (Fe-N) coordinated SACs, quantifying the active sites and their kinetic parameters. The findings reveal the significant differences of single sites from the average behaviors and corroborate the oxidase-like catalytic mechanism of the Fe-N active sites. We anticipate that the method will give essential insights into the rational design and application of SACs.

Suggested Citation

  • Liang Huang & Qiong Liu & Weiwei Wu & Ge Gao & Xiliang Zheng & Jin Wang & Shaojun Dong, 2023. "Identifying the active sites in unequal iron-nitrogen single-atom catalysts," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-41311-9
    DOI: 10.1038/s41467-023-41311-9
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    References listed on IDEAS

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    1. Jinrun Dong & Yuxian Lu & Yang Xu & Fanfan Chen & Jinmei Yang & Yuang Chen & Jiandong Feng, 2021. "Direct imaging of single-molecule electrochemical reactions in solution," Nature, Nature, vol. 596(7871), pages 244-249, August.
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