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

摘要

Metal-organic frameworks (MOFs) provide a platform to design new heterogeneous catalysts for catalytic CO2 reduction, but selective formation of C2 valuable liquid fuel products remains a challenge. Herein, we propose a strategy to synthesize composites by integrating MoS2 nanosheets into hierarchically porous defective UiO-66 (d-UiO-66) to form Mo-O-Zr bimetallic sites on the interfaces between UiO-66 and MoS2. 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/MoS2 composite facilitates the photo-catalytic conversion of gas phase CO2 and H2O to CH3COOH under visible light irradiation without any other adducts. The evolution rate and selectivity of CH3COOH reached 39.0 mu mol g(-1) h(-1) and 94 %, respectively, without any C1 products, suggesting a new approach for the design of highly efficient photocatalysts of CO2 for C2 production. Theoretical calculations demonstrate the charge-polarized Zr-O-Mo aided the C-C coupling process with the largely reduced energy barrier.