CoO<sub>x</sub> clusters-decorated IrO<sub>2</sub> electrocatalyst activates NO<sub>3</sub><sup>-</sup> mediator for benzylic C-H activation.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 40210890.
- Also identified by DOI 10.1038/s41467-025-58733-2 and PMC identifier 11986119.
- Licence recorded as CC BY-NC-ND.
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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(sp<sup>3</sup>)-H bonds at room temperature. Here, we introduce an electrocatalyst:mediator assembly in which CoO<sub>x</sub> clusters-decorated IrO<sub>2</sub> electrocatalyst activates NO<sub>3</sub><sup>-</sup> mediator to a highly reactive radical capable of abstracting a hydrogen atom from benzylic C-H. The interface between CoO<sub>x</sub> and IrO<sub>2</sub> promotes NO<sub>3</sub><sup>-</sup> activation by facilitating the desorption of NO<sub>3</sub><sup>●</sup> 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/cm<sup>2</sup>, 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/cm<sup>2</sup> was achieved.