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Unique hole-accepting carbon-dots promoting selective carbon dioxide reduction nearly 100% to methanol by pure water

Author

Listed:
  • Yiou Wang

    (University College London
    Ludwig-Maximilians-Universität München)

  • Xu Liu

    (University College London)

  • Xiaoyu Han

    (University College London
    The University of Manchester)

  • Robert Godin

    (Imperial College London
    The University of British Columbia)

  • Jialu Chen

    (University of St. Andrews)

  • Wuzong Zhou

    (University of St. Andrews)

  • Chaoran Jiang

    (University College London)

  • Jamie F. Thompson

    (Imperial College London)

  • K. Bayazit Mustafa

    (University College London
    Sabancı University)

  • Stephen A. Shevlin

    (University College London)

  • James R. Durrant

    (Imperial College London)

  • Zhengxiao Guo

    (University College London
    The University of Hong Kong
    The University of Hong Kong
    The University of Hong Kong)

  • Junwang Tang

    (University College London)

Abstract

Solar-driven CO2 reduction by abundant water to alcohols can supply sustainable liquid fuels and alleviate global warming. However, the sluggish water oxidation reaction has been hardly reported to be efficient and selective in CO2 conversion due to fast charge recombination. Here, using transient absorption spectroscopy, we demonstrate that microwave-synthesised carbon-dots (mCD) possess unique hole-accepting nature, prolonging the electron lifetime (t50%) of carbon nitride (CN) by six folds, favouring a six-electron product. mCD-decorated CN stably produces stoichiometric oxygen and methanol from water and CO2 with nearly 100% selectivity to methanol and internal quantum efficiency of 2.1% in the visible region, further confirmed by isotopic labelling. Such mCD rapidly extracts holes from CN and prevents the surface adsorption of methanol, favourably oxidising water over methanol and enhancing the selective CO2 reduction to alcohols. This work provides a unique strategy for efficient and highly selective CO2 reduction by water to high-value chemicals.

Suggested Citation

  • Yiou Wang & Xu Liu & Xiaoyu Han & Robert Godin & Jialu Chen & Wuzong Zhou & Chaoran Jiang & Jamie F. Thompson & K. Bayazit Mustafa & Stephen A. Shevlin & James R. Durrant & Zhengxiao Guo & Junwang Tan, 2020. "Unique hole-accepting carbon-dots promoting selective carbon dioxide reduction nearly 100% to methanol by pure water," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-16227-3
    DOI: 10.1038/s41467-020-16227-3
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    Cited by:

    1. Jijia Xie & Xiyi Li & Jian Guo & Lei Luo & Juan J. Delgado & Natalia Martsinovich & Junwang Tang, 2023. "Highly selective oxidation of benzene to phenol with air at room temperature promoted by water," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Zeshu Zhang & Chengliang Mao & Débora Motta Meira & Paul N. Duchesne & Athanasios A. Tountas & Zhao Li & Chenyue Qiu & Sanli Tang & Rui Song & Xue Ding & Junchuan Sun & Jiangfan Yu & Jane Y. Howe & We, 2022. "New black indium oxide—tandem photothermal CO2-H2 methanol selective catalyst," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    3. Lei Luo & Lei Fu & Huifen Liu & Youxun Xu & Jialiang Xing & Chun-Ran Chang & Dong-Yuan Yang & Junwang Tang, 2022. "Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    4. Xiaoqing Yan & Mengyang Xia & Hanxuan Liu & Bin Zhang & Chunran Chang & Lianzhou Wang & Guidong Yang, 2023. "An electron-hole rich dual-site nickel catalyst for efficient photocatalytic overall water splitting," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    5. Yang Liu & Jianhui Sun & Houhou Huang & Linlu Bai & Xiaomeng Zhao & Binhong Qu & Lunqiao Xiong & Fuquan Bai & Junwang Tang & Liqiang Jing, 2023. "Improving CO2 photoconversion with ionic liquid and Co single atoms," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    6. Lei Luo & Xiaoyu Han & Keran Wang & Youxun Xu & Lunqiao Xiong & Jiani Ma & Zhengxiao Guo & Junwang Tang, 2023. "Nearly 100% selective and visible-light-driven methane conversion to formaldehyde via. single-atom Cu and Wδ+," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    7. Yifan Gao & Shuai Liang & Biming Liu & Chengxu Jiang & Chenyang Xu & Xiaoyuan Zhang & Peng Liang & Menachem Elimelech & Xia Huang, 2023. "Subtle tuning of nanodefects actuates highly efficient electrocatalytic oxidation," Nature Communications, Nature, vol. 14(1), pages 1-13, December.

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