Insight Understanding of Ultrathin Carbon-Deficient Molybdenum Carbide Catalytic Activity for CO2 Conversion into Hydrocarbon Fuels

The catalytic reduction of carbon dioxide (CO2) to produce methane (CH4) as a hydrocarbon fuel has attracted extensive attention for renewable energy. In this study, we investigate ultrathin carbon-deficient molybdenum carbide (MoC0.66) as a catalyst for CO2 capture and conversion. Our findings indicate that MoC0.66 possesses remarkable catalytic activity for CO2 hydrogenation to CH4. Interestingly, unlike conventional catalysts, the limiting step of the MoC0.66 catalyst is determined by the release of *OH species during the CO2 reduction reaction (CO2RR). Increasing the temperature can improve the release of H2O and CH4 as well as the selectivity of the CO2RR. Moreover, the increase of temperature promotes the CO2RR on MoC0.66 by increasing the reaction rate, as evidenced by both simulation and experimental results. These results provide a way for the understanding of insight mechanisms for the CO2RR to energy-rich fuels at the atomic level and guide experimental applications of carbon-neutral reactions.