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 CO2 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 MoS2 antisite defect (Co‐MoS2) is designed from both the activity and selectivity aspects. By virtue of i) moderately electron‐deficient state (Coδ+) ensuring efficient CO2 activation and HER suppression; ii) the strong adsorption capability for intermediate enhancing selectivity; iii) the single atomic active site avoiding the formation of C2 products, Co‐MoS2 could selectively convert CO2 to CH4 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.