Regulating Asymmetric Charge Distribution in Cu ₂ MoS ₄ Nanosheets for Enhanced Photocatalytic CO ₂ Reduction

Abstract

Abstract Photocatalytic reduction of CO 2 to high‐value‐added chemicals represents a promising strategy for effective CO 2 utilization, and rationally regulating the electronic structure of the catalyst is the key to enhancing photocatalytic performance. Herein, it is demonstrated that in situ doping of atomic indium into the lattice of the Cu 2 MoS 4 catalyst results in remarkable enhancements in photocatalytic CO 2 reduction performance. A record gas product yield of 104.1 µmol·g −1 ·h −1 is achieved under visible light irradiation (>420 nm), accompanied by a generation rate of 35.3 µmol·g −1 ·h −1 for ethylene. Detailed experimental analyses and density functional theory (DFT) calculations reveal that the low electronegativity of indium atoms induces asymmetric charge redistribution near the doping sites. This effect facilitates the adsorption and dissociation of CO 2 molecules at the charge‐enriched Mo sites, as well as the subsequent generation of key intermediates ( * COCOH) toward ethylene formation. This work advances understanding of the potential mechanism between the electronic structure of the active site and photocatalytic performance, providing valuable insights into fabricating advanced materials for CO 2 conversion into solar fuels.