Dual-Doping Promotes the Carbon Dioxide Electroreduction Activity of MoS₂ Nanosheet Array

Electrocatalytic reduction of CO2 (ECR) to valuable fuels and chemicals using spare renewable energy offers a promising strategy to realize the artificial carbon cycle. Significant advances in ECR have been achieved, but challenges remain, such as accelerating the rate-limiting CO desorption step required for MoS2. Here, a N,P-codoped MoS2 nanosheet array was synthesized via a hydrothermal method, followed by an NH3-etching treatment. It can effectively catalyze CO2 reduction to CO with the highest faradaic efficiency of 91.5% at −0.9 V vs RHE in an ionic liquid electroyte. Meanwhile, the catalyst can maintain the ECR activity for 30 h with negligible decay. The theoretical calculations indicate that the dopants synergistically promote the desorption of the *CO moiety, thus resulting in an enhanced ECR activity. This work opens a new avenue for designing MoS2-based materials for the electroreduction of CO2 to CO.