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 d_{x² - 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 g_cat^-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.