Highly active single-layer 2H-MoS2 for CO2 hydrogenation to methanol

Few-layer MoS2 were recently discovered as promising catalyst for CO2 hydrogenation to methanol, despite extreme conditions proposed for its synthesis. Herein, we developed an exceptionally facile, safe, and scalable strategy to prepare single-layer MoS2 (s-MoS2) at ambient pressure using instantaneous self-assembled micelles of didodecyldimethylammonium (DA)-MoS4 complexes as precursor. During the pyrolysis, the presence and subsequent decomposition of coordinated DA inhibited the growth and sheet-stacking of MoS2 in c-direction, resulting in discrete s-MoS2 molecular sheets which maximize the exposure of in-plane S vacancies (Sv). Remarkably, s-MoS2 displayed 77% methanol selectivity and methanol space time yield of 1.54 g center dot g(MoS2)(-1)center dot h(-1), representing the top levels among reported MoS2 catalysts under similar conditions. Density functional theory (DFT) simulations attribute high activity of s-MoS2 to its ability to stabilize in-plane low-coordinated Mo atoms in the vicinity of Sv on both sides of monolayer. The superior performance of s-MoS2 creates new prospects for technological applications beyond CO2 hydrogenation.