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CoOx clusters-decorated IrO2 electrocatalyst activates NO3- mediator for benzylic C-H activation

Author

Listed:
  • Ziyu Mi

    (Nanyang Technological University
    Technology and Research (A*STAR); 1 Pesek Road Jurong Island)

  • Yuke Li

    (#16-16 Connexis)

  • Chao Wu

    (Technology and Research (A*STAR); 1 Pesek Road Jurong Island)

  • Mingsheng Zhang

    (#08-03 Innovis)

  • Xun Cao

    (Technology and Research (A*STAR); 1 Pesek Road Jurong Island)

  • Shibo Xi

    (Technology and Research (A*STAR); 1 Pesek Road Jurong Island)

  • Jia Zhang

    (#16-16 Connexis)

  • Wan Ru Leow

    (Nanyang Technological University
    Technology and Research (A*STAR); 1 Pesek Road Jurong Island)

Abstract

Electrochemical conversion of petrochemical-derived hydrocarbons to high-value oxygenates can utilize renewable energy and reduce carbon emissions. However, this involves the challenging activation of inert C(sp3)-H bonds at room temperature. Here, we introduce an electrocatalyst:mediator assembly in which CoOx clusters-decorated IrO2 electrocatalyst activates NO3- mediator to a highly reactive radical capable of abstracting a hydrogen atom from benzylic C-H. The interface between CoOx and IrO2 promotes NO3- activation by facilitating the desorption of NO3● radical for subsequent reaction. Our strategy is demonstrated through the selective oxidation of toluene to benzaldehyde with high Faradaic efficiency of 86( ±1)% at 25 mA/cm2, a factor of >3 times higher than the bare electrocatalyst. The electrocatalyst:mediator assembly is operated stably for 100 h, with minimal decline in performance. When translated into a flow system, a Faradaic efficiency of 60( ±4)% at 200 mA/cm2 was achieved.

Suggested Citation

  • Ziyu Mi & Yuke Li & Chao Wu & Mingsheng Zhang & Xun Cao & Shibo Xi & Jia Zhang & Wan Ru Leow, 2025. "CoOx clusters-decorated IrO2 electrocatalyst activates NO3- mediator for benzylic C-H activation," Nature Communications, Nature, vol. 16(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-58733-2
    DOI: 10.1038/s41467-025-58733-2
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