Cu‒S Covalent Bonds Enable the Anchoring of Single-atom Cu on Layered MoS for Highly Selective and Active Photothermal Catalytic Conversion of CO-HO to Ethanol.

The catalytic conversion of CO into high-value C 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 photothermal catalyst is synthesized via a two-step hydrothermal method, anchoring single-atom Cu on layered MoS for CO and HO reduction into C products (ethanol, acetylene, and ethane). Under optimal conditions (250 °C, 903 mW·cm, 320-780 nm), the Cu-MoS catalyst achieves an ethanol yield of 3.1 mmol·g·h, 4.6 times higher than blank MoS. Mechanistic studies reveal that Cu improves light absorption and enhances CO adsorption and *COOH accumulation at MoS edge S sites, as confirmed by density functional theory (DFT) calculations. Mo-Cu dual sites stabilize *CHO intermediates, boosting C product selectivity. The synergistic photothermal effect accelerates charge migration and surface reactions. This work provides cost-effective insights into photothermal CO conversion for fuel production.