Abstract

The conversion of CO2 into high value-added chemicals through efficient catalysis is an ideal strategy to reduce atmospheric CO2 pollution and achieve carbon neutrality. Therefore, amino-functionalized organic polymer Cu@Co-PIL-N4 loaded with highly dispersed CuI as a novel catalyst was developed. The functionalization of the surface and the high dispersion of the active phase integrate CO2 capture and conversion into one catalytic system. The locally enriched CO2 is converted to the easily activated carbon-oxygen negative ion by the action of primary or secondary amines. Thus, it is easier to achieve efficient preparation of α-alkylidene cyclic carbonates (STY = 20.8 h−1) by CO2 carboxylative cyclization under mild conditions (25 °C, CO2 pressure of 1 bar). The addition of a small amount of water to the cyclization system boosted domino reaction to convert the α-alkylidene cyclic carbonates to α-hydroxy ketones. The domino reaction also exhibited efficient catalytic activity and outstanding regioselectivity. In addition, the Cu@Co-PIL-N4 catalyst exhibited excellent substrate expansion and cyclic regeneration for both reactions. This work promises great significance for further developing cost-effective and high-performance catalysts for the chemical conversion of CO2.

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