Three‐in‐One Oxygen Vacancies: Whole Visible‐Spectrum Absorption, Efficient Charge Separation, and Surface Site Activation for Robust CO2 Photoreduction

Abstract A facile and controllable in situ reduction strategy is used to create surface oxygen vacancies (OVs) on Aurivillius‐phase Sr 2 Bi 2 Nb 2 TiO 12 nanosheets, which were prepared by a mineralizer‐assisted soft‐chemical method. Introduction of OVs on the surface of Sr 2 Bi 2 Nb 2 TiO 12 extends photoresponse to cover the whole visible region and also tremendously promotes separation of photoinduced charge carriers. Adsorption and activation of CO 2 molecules on the surface of the catalyst are greatly enhanced. In the gas‐solid reaction system without co‐catalysts or sacrificial agents, OVs‐abundant Sr 2 Bi 2 Nb 2 TiO 12 nanosheets show outstanding CO 2 photoreduction activity, producing CO with a rate of 17.11 μmol g −1 h −1 , about 58 times higher than that of the bulk counterpart, surpassing most previously reported state‐of‐the‐art photocatalysts. Our study provides a three‐in‐one integrated solution to advance the performance of photocatalysts for solar‐energy conversion and generation of renewable energy.