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Oxygen-tolerant CO2 electroreduction over covalent organic frameworks via photoswitching control oxygen passivation strategy

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  • Hong-Jing Zhu

    (Chinese Academy of Sciences
    Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China
    University of Chinese Academy of Science)

  • Duan-Hui Si

    (Chinese Academy of Sciences
    Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China
    University of Chinese Academy of Science)

  • Hui Guo

    (Chinese Academy of Sciences
    Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China
    University of Chinese Academy of Science)

  • Ziao Chen

    (Chinese Academy of Sciences
    Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China
    University of Chinese Academy of Science)

  • Rong Cao

    (Chinese Academy of Sciences
    Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China
    University of Chinese Academy of Science)

  • Yuan-Biao Huang

    (Chinese Academy of Sciences
    Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China
    University of Chinese Academy of Science)

Abstract

The direct use of flue gas for the electrochemical CO2 reduction reaction is desirable but severely limited by the thermodynamically favorable oxygen reduction reaction. Herein, a photonicswitching unit 1,2-Bis(5’-formyl-2’-methylthien-3’-yl)cyclopentene (DAE) is integrated into a cobalt porphyrin-based covalent organic framework for highly efficient CO2 electrocatalysis under aerobic environment. The DAE moiety in the material can reversibly modulate the O2 activation capacity and electronic conductivity by the framework ring-closing/opening reactions under UV/Vis irradiation. The DAE-based covalent organic framework with ring-closing type shows a high CO Faradaic efficiency of 90.5% with CO partial current density of −20.1 mA cm−2 at −1.0 V vs. reversible hydrogen electrode by co-feeding CO2 and 5% O2. This work presents an oxygen passivation strategy to realize efficient CO2 electroreduction performance by co-feeding of CO2 and O2, which would inspire to design electrocatalysts for the practical CO2 source such as flue gas from power plants or air.

Suggested Citation

  • Hong-Jing Zhu & Duan-Hui Si & Hui Guo & Ziao Chen & Rong Cao & Yuan-Biao Huang, 2024. "Oxygen-tolerant CO2 electroreduction over covalent organic frameworks via photoswitching control oxygen passivation strategy," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-45959-9
    DOI: 10.1038/s41467-024-45959-9
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