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

Ziyu Mi, Yuke Li, Chao Wu, Mingsheng Zhang, Xun Cao, Shibo Xi, Jia Zhang () and Wan Ru Leow ()
Additional contact information
Ziyu Mi: Nanyang Technological University
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

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-025-58733-2

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