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.

The catalytic conversion of CO2 into high-value C2+ 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/MoS2 photothermal catalyst is synthesized via a two-step hydrothermal method, anchoring single-atom Cu on layered MoS2 for CO2 and H2O reduction into C2 products (ethanol, acetylene, and ethane). Under optimal conditions (250 °C, 903 mW·cm-2, 320-780 nm), the Cu5%-MoS2 catalyst achieves an ethanol yield of 3.1 mmol·g-1·h-1, 4.6 times higher than blank MoS2. Mechanistic studies reveal that Cu improves light absorption and enhances CO2 adsorption and *COOH accumulation at MoS2 edge S sites, as confirmed by density functional theory (DFT) calculations. Mo-Cu dual sites stabilize *CHO intermediates, boosting C2 product selectivity. The synergistic photothermal effect accelerates charge migration and surface reactions. This work provides cost-effective insights into photothermal CO2 conversion for fuel production.