Engineering the surface delocalized electrons facilitates the ring-opening for deep toluene oxidation

Abstract

The stable conjugated structure of benzene-ring poses the persistent challenge for deep oxidation of toluene. In this study, the electronic structure of benzene-ring-containing reactants is tailored by engineering the interlayer hydrogenation in layered Bi2O2CO3, where charge separation and migration capabilities are improved and the confined charge in the interlayer and intralayer could transfer to catalyst surface and serve as delocalized electrons. The ring-opening site, the C = C bond, is activated by delocalized electrons. Consequently, the conjugated structure of the benzene-ring turns into a state with uneven charge distribution, resulting in weakened stability. With the attack of photo-generated radicals, the destabilized benzene-ring structure can be destroyed with direct ring-opening of toluene and achieves deep oxidation of toluene. Therefore, the degradation and mineralization of photocatalytic toluene are improved with great stability and humidity adaptability. This concept of promoting ring-opening with delocalized electrons provides a new strategy for the development of high-performance photocatalyst.