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Article Abstract
Selective C-H activation is the most important step for organic molecule transformation. Photocatalytic radicals driven C-H activation is considered a promising route but suffers from simultaneously utilizing electron/hole pairs which are limited to broad-band gap semiconductors. Herein, a half-photocathodic reaction strategy is demonstrated to activate and oxygenate C(sp)-H bonds of toluene toward selective benzaldehyde production using a narrow-bandgap CuBiO (CBO) porous photocathode. The intrinsic Cu/Cu redox of porous CBO photocathode catalyzes the photocathodic oxygen reductive HO to generate ·OH capable of oxidation which activates the C(sp)-H bond that is further oxygenated via ·O formed of the photocathodic oxygen reduction. As a result, the benzaldehyde selectivity is up to 90%. Impressively, the narrow-band gap of CBO enables record-high light-driven benzaldehyde yields of 111.93 mmol m h with stability of over 20 h. This work opens a green and efficient light-driven C(sp)-H bond oxidation strategy by using a narrow-bandgap photocathode.
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