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Catalytic ozonation mechanism over M1-N3C1 active sites

Author

Listed:
  • Dingren Ma

    (Sun Yat-sen University)

  • Qiyu Lian

    (Sun Yat-sen University)

  • Yexing Zhang

    (Sun Yat-sen University)

  • Yajing Huang

    (Sun Yat-sen University)

  • Xinyi Guan

    (Sun Yat-sen University)

  • Qiwen Liang

    (Sun Yat-sen University)

  • Chun He

    (Sun Yat-sen University)

  • Dehua Xia

    (Sun Yat-sen University)

  • Shengwei Liu

    (Sun Yat-sen University)

  • Jiaguo Yu

    (China University of Geosciences)

Abstract

The structure-activity relationship in catalytic ozonation remains unclear, hindering the understanding of activity origins. Here, we report activity trends in catalytic ozonation using a series of single-atom catalysts with well-defined M1-N3C1 (M: manganese, ferrum, cobalt, and nickel) active sites. The M1-N3C1 units induce locally polarized M − C bonds to capture ozone molecules onto M atoms and serve as electron shuttles for catalytic ozonation, exhibiting excellent catalytic activities (at least 527 times higher than commercial manganese dioxide). The combined in situ characterization and theoretical calculations reveal single metal atom-dependent catalytic activity, with surface atomic oxygen reactivity identified as a descriptor for the structure-activity relationship in catalytic ozonation. Additionally, the dissociation barrier of surface peroxide species is proposed as a descriptor for the structure-activity relationship in ozone decomposition. These findings provide guidelines for designing high-performance catalytic ozonation catalysts and enhance the atomic-level mechanistic understanding of the integral control of ozone and methyl mercaptan.

Suggested Citation

  • Dingren Ma & Qiyu Lian & Yexing Zhang & Yajing Huang & Xinyi Guan & Qiwen Liang & Chun He & Dehua Xia & Shengwei Liu & Jiaguo Yu, 2023. "Catalytic ozonation mechanism over M1-N3C1 active sites," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-42853-8
    DOI: 10.1038/s41467-023-42853-8
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    References listed on IDEAS

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    1. Chen Dong & Jia-Jia Yang & Lin-Hua Xie & Ganglong Cui & Wei-Hai Fang & Jian-Rong Li, 2022. "Catalytic ozone decomposition and adsorptive VOCs removal in bimetallic metal-organic frameworks," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    2. Yanming Cai & Jiaju Fu & Yang Zhou & Yu-Chung Chang & Qianhao Min & Jun-Jie Zhu & Yuehe Lin & Wenlei Zhu, 2021. "Insights on forming N,O-coordinated Cu single-atom catalysts for electrochemical reduction CO2 to methane," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
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