Combination of Co Single Atom and MoS2 Antisite Defect for Efficient Electrocatalytic CO2 Methanation: A Rational Design at Electronic Scale

Abstract Methane, the simplest hydrocarbon, has a high energy density and is widely used as chemical feedstocks or fuels. Converting CO 2 to methane through electrochemical reduction offers a promising strategy for managing the global carbon balance, but is a challenge due to the lack of effective electrocatalysts. Herein, the Co single atom catalyst supported by MoS 2 antisite defect (Co‐Mo S2 ) is designed from both the activity and selectivity aspects. By virtue of i) moderately electron‐deficient state (Co δ+ ) ensuring efficient CO 2 activation and HER suppression; ii) the strong adsorption capability for intermediate enhancing selectivity; iii) the single atomic active site avoiding the formation of C 2 products, Co‐Mo S2 could selectively convert CO 2 to CH 4 with a limiting potential of −0.45 V vs . RHE, which outperforms most of the present catalysts, and is expected to be a promising substitution for Cu‐based catalysts.