Strain-Induced Self-Assembly at Interface of Two-Dimensional Heterostructures Boosts CO<sub>2</sub> Reduction to Methanol by H<sub>2</sub>O
Ming Cheng, Ning Cao, Zhi Wang, Ke Wang, Tiancheng Pu, Yukun Li, Tulai Sun, Xuanyu Yue, Wenkang Ni, Wenxin Dai, Yi He, Yao Shi, Peng Zhang, Yihan Zhu, Pengfei Xie
Abstract
CO 2 conversion with pure H 2 O into CH 3 OH and O 2 driven by solar energy can supply fuels and life-essential substances for extraterrestrial exploration. However, the effective production of CH 3 OH is significantly challenging. Here we report an organozinc complex/MoS 2 heterostructure linked by well-defined zinc–sulfur covalent bonds derived by the structural deformation and intensive coupling of d x 2 – y 2 (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 CO 2 photoreduction. The optimal catalyst delivers a promising CH 3 OH 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 MoS 2, where the photogenerated holes accumulate, ensures the selective oxidation of water over methanol.