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Molecular tuning boosts asymmetric C-C coupling for CO conversion to acetate

Author

Listed:
  • Jie Ding

    (City University of Hong Kong)

  • Fuhua Li

    (City University of Hong Kong)

  • Xinyi Ren

    (Dalian Institute of Chemical Physics, Chinese Academy of Sciences)

  • Yuhang Liu

    (Suzhou University of Science and Technology)

  • Yifan Li

    (Chinese Academy of Sciences)

  • Zheng Shen

    (Dalian Institute of Chemical Physics, Chinese Academy of Sciences)

  • Tian Wang

    (National University of Singapore)

  • Weijue Wang

    (Dalian Institute of Chemical Physics, Chinese Academy of Sciences)

  • Yang-Gang Wang

    (Southern University of Science and Technology)

  • Yi Cui

    (Chinese Academy of Sciences)

  • Hongbin Yang

    (Suzhou University of Science and Technology)

  • Tianyu Zhang

    (Beijing Forestry University)

  • Bin Liu

    (City University of Hong Kong
    City University of Hong Kong)

Abstract

Electrochemical carbon dioxide/carbon monoxide reduction reaction offers a promising route to synthesize fuels and value-added chemicals, unfortunately their activities and selectivities remain unsatisfactory. Here, we present a general surface molecular tuning strategy by modifying Cu2O with a molecular pyridine-derivative. The surface modified Cu2O nanocubes by 4-mercaptopyridine display a high Faradaic efficiency of greater than 60% in electrochemical carbon monoxide reduction reaction to acetate with a current density as large as 380 mA/cm2 in a liquid electrolyte flow cell. In-situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy reveals stronger *CO signal with bridge configuration and stronger *OCCHO signal over modified Cu2O nanocubes by 4-mercaptopyridine than unmodified Cu2O nanocubes during electrochemical CO reduction. Density function theory calculations disclose that local molecular tuning can effectively regulate the electronic structure of copper catalyst, enhancing *CO and *CHO intermediates adsorption by the stabilization effect through hydrogen bonding, which can greatly promote asymmetric *CO-*CHO coupling in electrochemical carbon monoxide reduction reaction.

Suggested Citation

  • Jie Ding & Fuhua Li & Xinyi Ren & Yuhang Liu & Yifan Li & Zheng Shen & Tian Wang & Weijue Wang & Yang-Gang Wang & Yi Cui & Hongbin Yang & Tianyu Zhang & Bin Liu, 2024. "Molecular tuning boosts asymmetric C-C coupling for CO conversion to acetate," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-47913-1
    DOI: 10.1038/s41467-024-47913-1
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    References listed on IDEAS

    as
    1. Xinyan Liu & Jianping Xiao & Hongjie Peng & Xin Hong & Karen Chan & Jens K. Nørskov, 2017. "Understanding trends in electrochemical carbon dioxide reduction rates," Nature Communications, Nature, vol. 8(1), pages 1-7, August.
    2. Hong Bin Yang & Sung-Fu Hung & Song Liu & Kaidi Yuan & Shu Miao & Liping Zhang & Xiang Huang & Hsin-Yi Wang & Weizheng Cai & Rong Chen & Jiajian Gao & Xiaofeng Yang & Wei Chen & Yanqiang Huang & Hao M, 2018. "Atomically dispersed Ni(i) as the active site for electrochemical CO2 reduction," Nature Energy, Nature, vol. 3(2), pages 140-147, February.
    3. Fengwang Li & Arnaud Thevenon & Alonso Rosas-Hernández & Ziyun Wang & Yilin Li & Christine M. Gabardo & Adnan Ozden & Cao Thang Dinh & Jun Li & Yuhang Wang & Jonathan P. Edwards & Yi Xu & Christopher , 2020. "Molecular tuning of CO2-to-ethylene conversion," Nature, Nature, vol. 577(7791), pages 509-513, January.
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