Cu‒S Covalent Bonds Enable the Anchoring of Single‐atom Cu on Layered MoS2 for Highly Selective and Active Photothermal Catalytic Conversion of CO2−H2O to Ethanol

Abstract The catalytic conversion of CO 2 into high‐value C 2+ products offers a sustainable path toward carbon neutrality. However, traditional photocatalytic and thermal catalytic methods face challenges like low selectivity and yields. Herein, a novel Cu/MoS 2 photothermal catalyst is synthesized via a two‐step hydrothermal method, anchoring single‐atom Cu on layered MoS 2 for CO 2 and H 2 O reduction into C 2 products (ethanol, acetylene, and ethane). Under optimal conditions (250 °C, 903 mW·cm −2 , 320–780 nm), the Cu 5% –MoS 2 catalyst achieves an ethanol yield of 3.1 mmol·g −1 ·h −1 , 4.6 times higher than blank MoS 2 . Mechanistic studies reveal that Cu improves light absorption and enhances CO 2 adsorption and *COOH accumulation at MoS 2 edge S sites, as confirmed by density functional theory (DFT) calculations. Mo–Cu dual sites stabilize *CHO intermediates, boosting C 2 product selectivity. The synergistic photothermal effect accelerates charge migration and surface reactions. This work provides cost‐effective insights into photothermal CO 2 conversion for fuel production.