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 Cu_5%–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.