Exfoliated 2D Layered and Nonlayered Metal Phosphorous Trichalcogenides Nanosheets as Promising Electrocatalysts for CO<sub>2</sub> Reduction
Honglei Wang, Honglei Wang, Yunfei Jiao, Bing Wu, Dong Wang, Yueqi Hu, Fei Liang, Chen Shen, Andrea Knauer, Dan Ren, Hongguang Wang, Hongguang Wang, Peter A. van Aken, Hongbin Zhang, Zdeněk Sofer, Michaël Grätzel, Peter Schaaf
Abstract
Abstract Two‐dimensional (2D) materials catalysts provide an atomic‐scale view on a fascinating arena for understanding the mechanism of electrocatalytic carbon dioxide reduction (CO 2 ECR). Here, we successfully exfoliated both layered and nonlayered ultra‐thin metal phosphorous trichalcogenides (MPCh 3 ) nanosheets via wet grinding exfoliation (WGE), and systematically investigated the mechanism of MPCh 3 as catalysts for CO 2 ECR. Unlike the layered CoPS 3 and NiPS 3 nanosheets, the active Sn atoms tend to be exposed on the surfaces of nonlayered SnPS 3 nanosheets. Correspondingly, the nonlayered SnPS 3 nanosheets exhibit clearly improved catalytic activity, showing formic acid selectivity up to 31.6 % with −7.51 mA cm −2 at −0.65 V vs. RHE. The enhanced catalytic performance can be attributed to the formation of HCOO* via the first proton‐electron pair addition on the SnPS 3 surface. These results provide a new avenue to understand the novel CO 2 ECR mechanism of Sn‐based and MPCh 3 ‐based catalysts.