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

CO is a key intermediate during electrochemical CO₂ 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 3d-transition metal atoms supported by monolayered MoS₂ with S vacancy as efficient electrocatalyst for CO electroreduction to CH₄ . The screening result indicates that Cr doped defective MoS₂ (labeled as Cr/S_v -MoS₂ ) is beneficial to electroreduction of CO to CH₄ , 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.