Low‐Coordination Single Au Atoms on Ultrathin ZnIn2S4Nanosheets for Selective Photocatalytic CO2Reduction towards CH4

Abstract

AbstractSelective CO2photoreduction to hydrocarbon fuels such as CH4is promising and sustainable for carbon‐neutral future. However, lack of proper binding strengths with reaction intermediates makes it still a challenge for photocatalytic CO2methanation with both high activity and selectivity. Here, low‐coordination single Au atoms (Au1‐S2) on ultrathin ZnIn2S4nanosheets was synthesized by a complex‐exchange route, enabling exceptional photocatalytic CO2reduction performance. Under visible light irradiation, Au1/ZnIn2S4catalyst exhibits a CH4yield of 275 μmol g−1 h−1with a selectivity as high as 77 %. As revealed by detailed characterizations and density functional theory calculations, Au1/ZnIn2S4with Au1‐S2structure not only display fast carrier transfer to underpin its superior activity, but also greatly reduce the energy barrier for protonation of *CO and stabilize the *CH3intermediate, thereby leading to the selective CH4generation from CO2photoreduction.