Theoretical Screening of Transition Metal Doped Defective MoS2 as Efficient Electrocatalyst for CO Conversion to CH4

Abstract CO is a key intermediate during electrochemical CO 2 conversion. The deep reduction of CO to value‐added chemical products is a crucial strategy for effective carbon utilization. Single transition metal atoms supported by two‐dimensional material present a novel paragon for various catalytic reactions. Herein, we employ first principle theory to study a series of single 3 d ‐transition metal atoms supported by monolayered MoS 2 with S vacancy as efficient electrocatalyst for CO electroreduction to CH 4 . The screening result indicates that Cr doped defective MoS 2 (labeled as Cr/S v ‐MoS 2 ) is beneficial to electroreduction of CO to CH 4 , with even less negative limiting potential (−0.32 V) than Cu that has been widely studied as the most promising electrocatalyst in experiment. The outstanding activity is derived from the regulation of the d‐ band‐center of doped Cr and Mo atoms exposed on the surface. This discovery provides a theoretical basis for the preparation of future electrocatalysts for CORR.