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Coordination tailoring of Cu single sites on C3N4 realizes selective CO2 hydrogenation at low temperature

Author

Listed:
  • Tang Yang

    (Xiamen University)

  • Xinnan Mao

    (Soochow University
    Guangdong University of Technology)

  • Ying Zhang

    (Xiamen University)

  • Xiaoping Wu

    (Guangdong University of Technology)

  • Lu Wang

    (Soochow University)

  • Mingyu Chu

    (Soochow University
    Guangdong University of Technology)

  • Chih-Wen Pao

    (National Synchrotron Radiation Research Center)

  • Shize Yang

    (Arizona State University)

  • Yong Xu

    (Guangdong University of Technology)

  • Xiaoqing Huang

    (Xiamen University)

Abstract

CO2 hydrogenation has attracted great attention, yet the quest for highly-efficient catalysts is driven by the current disadvantages of poor activity, low selectivity, and ambiguous structure-performance relationship. We demonstrate here that C3N4-supported Cu single atom catalysts with tailored coordination structures, namely, Cu–N4 and Cu–N3, can serve as highly selective and active catalysts for CO2 hydrogenation at low temperature. The modulation of the coordination structure of Cu single atom is readily realized by simply altering the treatment parameters. Further investigations reveal that Cu–N4 favors CO2 hydrogenation to form CH3OH via the formate pathway, while Cu–N3 tends to catalyze CO2 hydrogenation to produce CO via the reverse water-gas-shift (RWGS) pathway. Significantly, the CH3OH productivity and selectivity reach 4.2 mmol g–1 h–1 and 95.5%, respectively, for Cu–N4 single atom catalyst. We anticipate this work will promote the fundamental researches on the structure-performance relationship of catalysts.

Suggested Citation

  • Tang Yang & Xinnan Mao & Ying Zhang & Xiaoping Wu & Lu Wang & Mingyu Chu & Chih-Wen Pao & Shize Yang & Yong Xu & Xiaoqing Huang, 2021. "Coordination tailoring of Cu single sites on C3N4 realizes selective CO2 hydrogenation at low temperature," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-26316-6
    DOI: 10.1038/s41467-021-26316-6
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    References listed on IDEAS

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    1. Alexander Schoedel & Zhe Ji & Omar M. Yaghi, 2016. "The role of metal–organic frameworks in a carbon-neutral energy cycle," Nature Energy, Nature, vol. 1(4), pages 1-13, April.
    2. Yizhen Chen & Hongliang Li & Wanghui Zhao & Wenbo Zhang & Jiawei Li & Wei Li & Xusheng Zheng & Wensheng Yan & Wenhua Zhang & Junfa Zhu & Rui Si & Jie Zeng, 2019. "Optimizing reaction paths for methanol synthesis from CO2 hydrogenation via metal-ligand cooperativity," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    3. Xiao Zhang & Xueqian Li & Du Zhang & Neil Qiang Su & Weitao Yang & Henry O. Everitt & Jie Liu, 2017. "Product selectivity in plasmonic photocatalysis for carbon dioxide hydrogenation," Nature Communications, Nature, vol. 8(1), pages 1-9, April.
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    Cited by:

    1. Yan, Xianyao & Duan, Chenyu & Yu, Shuihua & Dai, Bing & Sun, Chaoying & Chu, Huaqiang, 2024. "Recent advances on CO2 reduction reactions using single-atom catalysts," Renewable and Sustainable Energy Reviews, Elsevier, vol. 190(PB).

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