State Key Laboratory of Fine Chemicals & Laboratory of Advanced Materials and Catalytic Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
With the advantages of low raw material cost and 100% atom utilization, the synthesis of high value-added chemical product cyclic carbonates by the cycloaddition of CO2 to epoxides has become one of the most prospective approaches to achieve the industrial utilization of CO2. In the reported catalytic systems, the complexity of the catalyst synthesis process, high cost, separation difficulties, and low CO2 capture limit the catalytic efficiency and its large-scale application. In this paper, Ag nanoparticles loaded on polyethyleneimine (PEI)-modified UiO-66-NH2 (Ag/PEI@UiO-66-NH2) are successfully synthesized by in situ immersion reduction. The Ag nanoparticles and the amino groups on the surfaces of PEI@UiO-66-NH2 contribute to the adsorption of CO2 and polarization of C–O bonds in epoxides, thereby boosting the conversion capability for the CO2 cycloaddition reaction. At the amount of propylene oxide of 0.25 mol and the catalyst dosage of 1% of the substrate, the yield and selectivity of propylene carbonate are up to 99%. In addition, the stability and recyclability of Ag/PEI@UiO-66-NH2 catalyst are attained. The Ag/PEI@UiO-66-NH2 catalyst also demonstrates a wide range of activity and distinctive selectivity toward cyclo-carbonates in the cycloaddition of CO2 to epoxides. This work provides a guide to designing a highly efficient catalyst for in situ capture and high-value utilization of CO2 in industrial applications.
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