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Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction

Author

Listed:
  • Yuehan Cao

    (Southwest Petroleum University
    Southwest Petroleum University)

  • Lan Guo

    (Southwest Petroleum University)

  • Meng Dan

    (Southwest Petroleum University
    Lund University)

  • Dmitry E. Doronkin

    (Institute for Chemical Technology and Polymer Chemistry and Institute of Catalysis Research and Technology, Karlsruhe Institute of Technology)

  • Chunqiu Han

    (Southwest Petroleum University)

  • Zhiqiang Rao

    (Southwest Petroleum University)

  • Yang Liu

    (Southwest Petroleum University
    Lund University)

  • Jie Meng

    (Lund University
    Technical University of Denmark)

  • Zeai Huang

    (Southwest Petroleum University)

  • Kaibo Zheng

    (Lund University
    Technical University of Denmark)

  • Peng Chen

    (Southwest Petroleum University
    University of Electronic Science and Technology of China)

  • Fan Dong

    (University of Electronic Science and Technology of China)

  • Ying Zhou

    (Southwest Petroleum University
    Southwest Petroleum University)

Abstract

The surface electron density significantly affects the photocatalytic efficiency, especially the photocatalytic CO2 reduction reaction, which involves multi-electron participation in the conversion process. Herein, we propose a conceptually different mechanism for surface electron density modulation based on the model of Au anchored CdS. We firstly manipulate the direction of electron transfer by regulating the vacancy types of CdS. When electrons accumulate on vacancies instead of single Au atoms, the adsorption types of CO2 change from physical adsorption to chemical adsorption. More importantly, the surface electron density is manipulated by controlling the size of Au nanostructures. When Au nanoclusters downsize to single Au atoms, the strong hybridization of Au 5d and S 2p orbits accelerates the photo-electrons transfer onto the surface, resulting in more electrons available for CO2 reduction. As a result, the product generation rate of AuSA/Cd1−xS manifests a remarkable at least 113-fold enhancement compared with pristine Cd1−xS.

Suggested Citation

  • Yuehan Cao & Lan Guo & Meng Dan & Dmitry E. Doronkin & Chunqiu Han & Zhiqiang Rao & Yang Liu & Jie Meng & Zeai Huang & Kaibo Zheng & Peng Chen & Fan Dong & Ying Zhou, 2021. "Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-21925-7
    DOI: 10.1038/s41467-021-21925-7
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    Cited by:

    1. Chen, Zhangsen & Zhang, Gaixia & Chen, Hangrong & Prakash, Jai & Zheng, Yi & Sun, Shuhui, 2022. "Multi-metallic catalysts for the electroreduction of carbon dioxide: Recent advances and perspectives," Renewable and Sustainable Energy Reviews, Elsevier, vol. 155(C).
    2. 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.
    3. Xinfeng Chen & Chengdong Peng & Wenyan Dan & Long Yu & Yinan Wu & Honghan Fei, 2022. "Bromo- and iodo-bridged building units in metal-organic frameworks for enhanced carrier transport and CO2 photoreduction by water vapor," Nature Communications, Nature, vol. 13(1), pages 1-14, December.
    4. Yao Chai & Yuehua Kong & Min Lin & Wei Lin & Jinni Shen & Jinlin Long & Rusheng Yuan & Wenxin Dai & Xuxu Wang & Zizhong Zhang, 2023. "Metal to non-metal sites of metallic sulfides switching products from CO to CH4 for photocatalytic CO2 reduction," Nature Communications, Nature, vol. 14(1), pages 1-11, December.

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