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Linking oxidative and reductive clusters to prepare crystalline porous catalysts for photocatalytic CO2 reduction with H2O

Author

Listed:
  • Jie Zhou

    (South China Normal University)

  • Jie Li

    (South China Normal University)

  • Liang Kan

    (South China Normal University)

  • Lei Zhang

    (South China Normal University)

  • Qing Huang

    (South China Normal University)

  • Yong Yan

    (South China Normal University)

  • Yifa Chen

    (South China Normal University)

  • Jiang Liu

    (South China Normal University)

  • Shun-Li Li

    (South China Normal University)

  • Ya-Qian Lan

    (South China Normal University)

Abstract

Mimicking natural photosynthesis to convert CO2 with H2O into value-added fuels achieving overall reaction is a promising way to reduce the atmospheric CO2 level. Casting the catalyst of two or more catalytic sites with rapid electron transfer and interaction may be an effective strategy for coupling photocatalytic CO2 reduction and H2O oxidation. Herein, based on the MOF ∪ COF collaboration, we have carefully designed and synthesized a crystalline hetero-metallic cluster catalyst denoted MCOF-Ti6Cu3 with spatial separation and functional cooperation between oxidative and reductive clusters. It utilizes dynamic covalent bonds between clusters to promote photo-induced charge separation and transfer efficiency, to drive both the photocatalytic oxidative and reductive reactions. MCOF-Ti6Cu3 exhibits fine activity in the conversion of CO2 with water into HCOOH (169.8 μmol g−1h−1). Remarkably, experiments and theoretical calculations reveal that photo-excited electrons are transferred from Ti to Cu, indicating that the Cu cluster is the catalytic reduction center.

Suggested Citation

  • Jie Zhou & Jie Li & Liang Kan & Lei Zhang & Qing Huang & Yong Yan & Yifa Chen & Jiang Liu & Shun-Li Li & Ya-Qian Lan, 2022. "Linking oxidative and reductive clusters to prepare crystalline porous catalysts for photocatalytic CO2 reduction with H2O," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-32449-z
    DOI: 10.1038/s41467-022-32449-z
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    1. Hong-Jing Zhu & Duan-Hui Si & Hui Guo & Ziao Chen & Rong Cao & Yuan-Biao Huang, 2024. "Oxygen-tolerant CO2 electroreduction over covalent organic frameworks via photoswitching control oxygen passivation strategy," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Zhongshan Chen & Jingyi Wang & Mengjie Hao & Yinghui Xie & Xiaolu Liu & Hui Yang & Geoffrey I. N. Waterhouse & Xiangke Wang & Shengqian Ma, 2023. "Tuning excited state electronic structure and charge transport in covalent organic frameworks for enhanced photocatalytic performance," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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