Light-Driven Reconstruction of MoS2 Nanosheets Boosts Photothermal Reverse Water Gas Shift Reaction with Near-Unity Selectivity

In-depth understanding of the reconstruction behaviors during photothermal reactions is of paramount importance for the design of highly efficient photothermal catalysts. Here, we demonstrate the photothermal effect-induced reconstruction of MoS2 nanosheets during the photothermal reverse water gas shift (RWGS) reaction. Specifically, under the operating photothermal reaction conditions, the MoS2 nanosheet catalyst undergoes rapid surface temperature increase up to around 380 °C, which can react with the H2 gas to produce in-plane S vacancies, thereby leading to the reconstruction of MoS2 nanosheets for enhanced RWGS reaction activity. An approximately 7.8 mmol g–1 h–1 evolution rate with a near-unity selectivity of CO (>99%) is achieved over MoS2 nanosheets during 100 h stability testing under flow-bed reaction and atmospheric pressure. Detailed structural characterizations combined with density functional theory simulations unravel that the photothermal effect-induced reconstruction of MoS2 can facilitate the charge separation and adsorption of reactants, lower the energy barrier of the *COOH intermediate, and meanwhile, improve the H2 dissociation ability for promoting the RWGS reaction.