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Scalable synthesis of coordinatively unsaturated metal-nitrogen sites for large-scale CO2 electrolysis

Author

Listed:
  • Ji Wei Sun

    (East China University of Science and Technology)

  • Xuefeng Wu

    (East China University of Science and Technology)

  • Peng Fei Liu

    (East China University of Science and Technology)

  • Jiacheng Chen

    (East China University of Science and Technology)

  • Yuanwei Liu

    (East China University of Science and Technology)

  • Zhen Xin Lou

    (East China University of Science and Technology)

  • Jia Yue Zhao

    (East China University of Science and Technology)

  • Hai Yang Yuan

    (East China University of Science and Technology)

  • Aiping Chen

    (East China University of Science and Technology)

  • Xue Lu Wang

    (East China Normal University)

  • Minghui Zhu

    (East China University of Science and Technology)

  • Sheng Dai

    (East China University of Science and Technology)

  • Hua Gui Yang

    (East China University of Science and Technology)

Abstract

Practical electrochemical CO2-to-CO conversion requires a non-precious catalyst to react at high selectivity and high rate. Atomically dispersed, coordinatively unsaturated metal-nitrogen sites have shown great performance in CO2 electroreduction; however, their controllable and large-scale fabrication still remains a challenge. Herein, we report a general method to fabricate coordinatively unsaturated metal-nitrogen sites doped within carbon nanotubes, among which cobalt single-atom catalysts can mediate efficient CO2-to-CO formation in a membrane flow configuration, achieving a current density of 200 mA cm−2 with CO selectivity of 95.4% and high full-cell energy efficiency of 54.1%, outperforming most of CO2-to-CO conversion electrolyzers. By expanding the cell area to 100 cm2, this catalyst sustains a high-current electrolysis at 10 A with 86.8% CO selectivity and the single-pass conversion can reach 40.4% at a high CO2 flow rate of 150 sccm. This fabrication method can be scaled up with negligible decay in CO2-to-CO activity. In situ spectroscopy and theoretical results reveal the crucial role of coordinatively unsaturated metal-nitrogen sites, which facilitate CO2 adsorption and key *COOH intermediate formation.

Suggested Citation

  • Ji Wei Sun & Xuefeng Wu & Peng Fei Liu & Jiacheng Chen & Yuanwei Liu & Zhen Xin Lou & Jia Yue Zhao & Hai Yang Yuan & Aiping Chen & Xue Lu Wang & Minghui Zhu & Sheng Dai & Hua Gui Yang, 2023. "Scalable synthesis of coordinatively unsaturated metal-nitrogen sites for large-scale CO2 electrolysis," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-36688-6
    DOI: 10.1038/s41467-023-36688-6
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