High-efficiency photocatalytic CO2 reduction enabled by interfacial Ov and isolated Ti3+ of g-C3N4/TiO2 Z-scheme heterojunction.

ABSTRACT

Exploring the real force that drives the separation of Coulomb-bound electron-hole pairs in the interface of heterojunction photocatalysts can establish a clear mechanism for efficient solar energy conversion efficiency. Herein, the formation of oxygen vacancy (Ov) and isolated Ti3+ was precisely regulated at the interface of g-C3N4/TiO2 Z-scheme heterojunction (g-C3N4/Ov-Ti3+-TiO2) by optimizing the opening degree of the calcination system, showing excellent production rate of CO and CH4 from CO2 photoreduction under visible light. This photocatalytic system also exhibited prominent stability. Combining theoretical calculation and characterization, the introduction of Ov and isolated Ti3+ on the interface could construct a charge transfer channel to break the forbidden transition of n â†’ π*, improving the separation process of photoexcited electron-hole pairs. The photoexcited electrons weakened the covalent interaction of CO bonds to promote the activation of adsorbed inert CO2 molecules, significantly reducing the energy barrier of the rate-limiting step during CO2 reduction. This work demonstrates the great application potential of reasonably regulating heterojunction interface for efficient photocatalytic CO2 reduction.