Steric Hindrance in Sulfur Vacancy of Monolayer MoS2 Boosts Electrochemical Reduction of Carbon Monoxide to Methane

Abstract The efficient generation of methane by total electroreduction of carbon monoxide (CO) could be of benefit for a more sustainable society. However, a highly efficient and selective catalyst for this process remains to be developed. In this study, density functional theory calculations indicate that steric hindrance in monolayer molybdenum sulfide with 2 S vacancies (DV‐MoS 2 ) can facilitate the conversion of CO into CH 4 with high activity and selectivity under electrochemical reduction at a low potential of −0.53 V vs. RHE and ambient conditions. The potential is a significant improvement on the state‐of‐the‐art Cu electrode (−0.74 V vs. RHE), with less electrical energy. Moreover, the results suggest that such steric hindrance effects are important for structure‐sensitive catalytic reactions.