Strain-Induced Self-Assembly at Interface of Two-Dimensional Heterostructures Boosts CO2 Reduction to Methanol by H2O

CO2 conversion with pure H2O into CH3OH and O2 driven by solar energy can supply fuels and life-essential substances for extraterrestrial exploration. However, the effective production of CH3OH is significantly challenging. Here we report an organozinc complex/MoS2 heterostructure linked by well-defined zinc–sulfur covalent bonds derived by the structural deformation and intensive coupling of dx2 – y2(Zn)-p(S) orbitals at the interface, resulting in distinctive charge transfer behaviors and excellent redox capabilities as revealed by experimental characterizations and first-principle calculations. The synthesis strategy is further generalized to more organometallic compounds, achieving various heterostructures for CO2 photoreduction. The optimal catalyst delivers a promising CH3OH yield of 2.57 mmol gcat–1 h–1 and selectivity of more than 99.5%. The reverse water gas shift mechanism is identified for methanol formation. Meanwhile, energy-unfavorable adsorption of methanol on MoS2, where the photogenerated holes accumulate, ensures the selective oxidation of water over methanol.