Influence of ionic liquid anions on electrochemical CO2 reduction to higher hydrocarbons on sulfur-vacant MoS2

Molybdenum disulfide (MoS 2 ) has emerged as a promising electrocatalyst for the electrochemical reduction of CO 2 , primarily yielding carbon monoxide. However, product selectivity is known to be highly sensitive to structural features such as edge termination and defect density. In this work, we report the formation of higher hydrocarbons (C 2 + products) enabled by the presence of inherent sulfur vacancies in MoS 2 when combined with various ionic liquids as co-catalysts. While MoS 2 has traditionally shown limited hydrocarbon output, our findings demonstrate for the first time that native defect sites, interacting synergistically with the electrolyte environment, can facilitate the production of significant amounts of C 2 + species. These results provide new insights into defect-mediated catalytic pathways and highlight the importance of electrolyte design in tuning product distribution during CO 2 electroreduction. • First observation of C 2 + hydrocarbon formation on sulfur-vacant MoS 2 . • Imidazolium-based ionic liquids modulate CO 2 RR selectivity on MoS 2 . • Anion identity of ionic liquid governs surface binding and deactivation in CO 2 RR.