Hierarchically Porous Metal–Organic Framework/MoS₂ Interface for Selective Photocatalytic Conversion of CO₂ with H₂O into CH₃COOH

Abstract Metal–organic frameworks (MOFs) provide a platform to design new heterogeneous catalysts for catalytic CO 2 reduction, but selective formation of C2 valuable liquid fuel products remains a challenge. Herein, we propose a strategy to synthesize composites by integrating MoS 2 nanosheets into hierarchically porous defective UiO‐66 ( d ‐UiO‐66) to form Mo‐O‐Zr bimetallic sites on the interfaces between UiO‐66 and MoS 2 . The active interfaces are favorable for the efficient transfer of photo‐generated charge carriers and for promoting the activity, whereas, the synergy of the components at the interfaces achieves selectivity for C2 production. The d ‐UiO‐66/MoS 2 composite facilitates the photo‐catalytic conversion of gas phase CO 2 and H 2 O to CH 3 COOH under visible light irradiation without any other adducts. The evolution rate and selectivity of CH 3 COOH reached 39.0 μmol g −1 h −1 and 94 %, respectively, without any C1 products, suggesting a new approach for the design of highly efficient photocatalysts of CO 2 for C2 production. Theoretical calculations demonstrate the charge‐polarized Zr‐O‐Mo aided the C−C coupling process with the largely reduced energy barrier.

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