Low‐Coordination Single Au Atoms on Ultrathin ZnIn<sub>2</sub>S<sub>4</sub>Nanosheets for Selective Photocatalytic CO<sub>2</sub>Reduction towards CH<sub>4</sub>
Shenghe Si, Hongwei Shou, Yuyin Mao, Xiaolei Bao, Guangyao Zhai, Kepeng Song, Zeyan Wang, Peng Wang, Yuanyuan Liu, Zhaoke Zheng, Ying Dai, Li Song, Baibiao Huang, Hefeng Cheng
Abstract
Abstract Selective CO 2 photoreduction to hydrocarbon fuels such as CH 4 is promising and sustainable for carbon‐neutral future. However, lack of proper binding strengths with reaction intermediates makes it still a challenge for photocatalytic CO 2 methanation with both high activity and selectivity. Here, low‐coordination single Au atoms (Au 1 ‐S 2 ) on ultrathin ZnIn 2 S 4 nanosheets was synthesized by a complex‐exchange route, enabling exceptional photocatalytic CO 2 reduction performance. Under visible light irradiation, Au 1 /ZnIn 2 S 4 catalyst exhibits a CH 4 yield of 275 μmol g −1 h −1 with a selectivity as high as 77 %. As revealed by detailed characterizations and density functional theory calculations, Au 1 /ZnIn 2 S 4 with Au 1 ‐S 2 structure 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 *CH 3 intermediate, thereby leading to the selective CH 4 generation from CO 2 photoreduction.