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Recoverable operation strategy for selective and stable electrochemical carbon dioxide reduction to methane

Author

Listed:
  • Guorui Gao

    (Queen’s University, Department of Chemical Engineering)

  • Behnam Nourmohammadi Khiarak

    (Queen’s University, Department of Chemical Engineering)

  • Hengzhou Liu

    (Northwestern University, Department of Chemistry)

  • Thành Trần-Phú

    (Swinburne University of Technology, School of Science, Computing and Emerging Technologies)

  • Cornelius A. Obasanjo

    (Queen’s University, Department of Chemical Engineering)

  • Jackson Crane

    (Queen’s University, Department of Mechanical and Materials Engineering)

  • Hung D. T. Lai

    (Queen’s University, Department of Chemical Engineering)

  • Gelson T. S. T. da Silva

    (Queen’s University, Department of Chemical Engineering
    Federal University of Sao Carlos, Interdisciplinary Laboratory of Electrochemistry and Ceramics, Department of Chemistry)

  • Viktoria Golovanova

    (The Barcelona Institute of Science and Technology, ICFO–Institut de Ciències Fotòniques)

  • Jiantao Li

    (Northwestern University, Department of Chemistry)

  • Huajie Ze

    (Northwestern University, Department of Chemistry)

  • John Weiss

    (Northwestern University, Department of Chemistry)

  • Zedong Zhang

    (Northwestern University, Department of Chemistry)

  • Sungsik Lee

    (Argonne National Laboratory, X-ray Science Division)

  • Rosalie K. Hocking

    (Swinburne University of Technology, School of Science, Computing and Emerging Technologies)

  • F. Pelayo García de Arquer

    (The Barcelona Institute of Science and Technology, ICFO–Institut de Ciències Fotòniques)

  • Edward H. Sargent

    (Northwestern University, Department of Chemistry)

  • Cao-Thang Dinh

    (Queen’s University, Department of Chemical Engineering)

Abstract

In the carbon dioxide (CO2) electroreduction reaction, catalysts determine, to a large extent, the system’s product selectivity, energy efficiency and stability. Conventionally, catalysts are prepared and optimized ex situ before the reaction, but they often suffer from low stability due to intrinsic structural changes during the reaction. Here we demonstrate a recoverable operation strategy for selective and stable electroreduction of CO2 to methane. In this approach, active catalysts are formed and fully reset in situ during CO2 electroreduction reaction. By stabilizing catalyst precursors and controlling the formation and removal of the catalysts, we demonstrate an over 500-hour CO2-to-methane conversion with a Faradaic efficiency of over 60% at the reduction current density of above 0.2 A cm−2 and full-cell voltage of below 4.0 V. We further showcase benefits of the recoverable operation for potential integration with intermittent renewable power supply, contributing to more than 100 days with day-on and night-off operation.

Suggested Citation

  • Guorui Gao & Behnam Nourmohammadi Khiarak & Hengzhou Liu & Thành Trần-Phú & Cornelius A. Obasanjo & Jackson Crane & Hung D. T. Lai & Gelson T. S. T. da Silva & Viktoria Golovanova & Jiantao Li & Huaji, 2025. "Recoverable operation strategy for selective and stable electrochemical carbon dioxide reduction to methane," Nature Energy, Nature, vol. 10(11), pages 1360-1370, November.
    • Handle: RePEc:nat:natene:v:10:y:2025:i:11:d:10.1038_s41560-025-01883-w
    DOI: 10.1038/s41560-025-01883-w
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