Sulfur vacancy-rich MoS2 as a catalyst for the hydrogenation of CO2 to methanol

The low-temperature hydrogenation of CO2 to methanol is of great significance for the recycling of this greenhouse gas to valuable products, however, it remains a great challenge due to the trade-off between catalytic activity and selectivity. Here, we report that CO2 can dissociate at sulfur vacancies in MoS2 nanosheets to yield surface-bound CO and Oat room temperature, thus enabling a highly efficient low-temperature hydrogenation of CO2 to methanol. Multiple in situ spectroscopic and microscopic characterizations combined with theoretical calculations demonstrated that in-plane sulfur vacancies drive the selective hydrogenation of CO2 to methanol by inhibiting deep hydrogenolysis to methane, whereas edge vacancies facilitate excessive hydrogenation to methane. At 180 degrees C, the catalyst achieved a 94.3% methanol selectivity at a CO2 conversion of 12.5% over the in-plane sulfur vacancy-rich MoS2 nanosheets, which notably surpasses those of previously reported catalysts. This catalyst exhibited high stability for over 3,000 hours without any deactivation, rendering it a promising candidate for industrial application.