MoS2 has been recognized as an effective catalyst for the hydrogenation of CO2 to methanol, where sulfur vacancies (Sv) serve as the active sites. However, its catalytic performance depends not only on the vacancy location (in-plane versus edge) but also on its precise configuration. In-plane adjacent double Sv function as the active sites for methanol formation, whereas in-plane separated single vacancies remain inactive due to the insufficient assembly of metal centers. In this study, we employed an etching-before-loading strategy to synthesize Fe/MoS2-e catalysts that build defect–metal interfaces between Fe clusters and the MoS2 basal plane, thereby activating basal-plane single Sv. Compared to Fe clusters supported on pristine MoS2, Fe clusters anchored at defect sites not only facilitated the generation of adjacent Sv during H2 pretreatment but also led to the formation of a distinct type of active site with single Sv. This architecture effectively activates CO2 into CO and modulates the adsorption strength of the key intermediate CO*, both of which contribute to a stable methanol yield of 170.8 mg·gcat.–1·h–1 and a high methanol selectivity (78.9%). This work provides a strategy for engineering defect-metal interfaces to enhance the catalytic performance in CO2 conversion and other thermochemical processes.
Yang et al. (2026) studied this question.