Amino-functionalized organic polymer loaded with highly dispersed CuI for efficient catalytic conversion of CO2 with PA

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. [Display omitted] •A novel Cu@Co-PIL-N4 catalyst was prepared via ion-exchange deposition route.•Cu@Co-PIL-N4 integrates CO2 adsorption and capture into one catalytic system.•The novel catalysts exhibited high catalytic efficiency and diversity for CO2 conversion.•Cu@Co-PIL-N4 remained highly active for four successive reuses. Typically, the CO2 concentration in flue gas is very low (around 15%), thus capturing CO2 from flue gas requires high energy consumption and various purification processes [49,50]. Attributed to the excellent ability of Cu@Co-PIL-N4 catalyst for CO2 gas capture, it was applied for the carboxylative cyclization under dilute gas and achieved α-alkylidene cyclic carbonate yield of 68%. Therefore, attributed to these intriguing characteristics, this newly developed catalytic system provides a new strategy for CO2 capture and flue gas utilization in the field of CCUS (Fig. 5). α-hydroxy ketone is a very important and widely used compound [52,53] as biologically active natural product, pharmaceutical intermediate, and a photoinitiator in UV-curable coatings [54]. Therefore, the synthesis of α-hydroxy ketones via the triple component reaction of PA-CO2-H2O is a fascinating s