Cu‒S Covalent Bonds Enable the Anchoring of Single-atom Cu on Layered MoS(2) for Highly Selective and Active Photothermal Catalytic Conversion of CO(2)-H(2)O to Ethanol

Cu‒S共价键能够将单原子Cu锚定在层状MoS(2)上,从而实现CO(2)-H(2)O高选择性、高活性的光热催化转化制乙醇

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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.

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