Engineering BiOBrx I1-x solid solutions with enhanced singlet oxygen production for photocatalytic benzylic C-H bond activation mediated by N-hydroxyl compounds

The aerobic, selective oxidation of hydrocarbons via C-H bond activation is still a challenge. This work shows the achievement of the room temperature visible light driven photocatalytic activation of benzylic C-H bonds with N-hydroxysuccinimide over BiOBrxI1-x (0 <= x <= 1) solid solutions, whose valance bands were engineered through varying the ratio of bromide to iodide. The optimal BiOBr0.85I0.15 catalyst exhibited over 98% conversion ratio of ethylbenzene, which was about 3.9 and 8.9 times that of pure BiOBr and BiOI, respectively. The excellent photocatalytic activity of BiOBr(0.85)I(0.15 )solid solution can be ascribed to the orbital hybridization of the valence band containing both Br 4p and I 5p orbitals, which could promote photo-induced charge carrier separation and improve the generation of singlet oxygen. This work shed some light on the rational design of photocatalysts for targeted organic transformation. (C) 2021 Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences. Published by Elsevier B.V. All rights reserved.

Automated summary

This study demonstrates the visible light-driven photocatalytic activation of benzylic C-H bonds using N-hydroxysuccinimide over BiOBrxI1-x solid solutions. The optimized BiOBr0.85I0.15 catalyst showed significantly higher conversion ratios compared to pure BiOBr and BiOI, attributed to orbital hybridization in the valence band and improved charge carrier separation and singlet oxygen generation. This work provides insights for the rational design of photocatalysts for targeted organic transformations.