Capture and in-situ conversion of low-concentration CO2 over robust poly(ionic liquid)@porous carbon nanocomposites under green, co-catalyst- and solvent-free conditions

Abstract

The development of advanced materials with dual functionalities for the capture of low-concentration CO2 and its in-situ conversion into value-added chemicals under mild and green conditions holds significant practical importance. In this study, we present a facile pyrolysis of fluid precursors followed by an in-situ polymerization strategy for preparing poly(ionic liquid)@porous carbon nanocomposites (PIL-Brx@Zn-CTM), which possess multiple active sites including Lewis acidic Zn2+, Lewis basic N, and nucleophilic Br– groups. Subsequently, we investigate their potential application in the efficient capture and conversion of low-concentration CO2 into cyclic carbonates. The influence of PIL-Brx@Zn-CTM structures and technological conditions on the cycloaddition reaction between low-concentration CO2 (15 % CO2 and 85 % N2) and epichlorohydrin was examined. The PIL-Br1.0@Zn-CTM nanocomposite was determined to be the most suitable catalyst, resulting in a 94 % yield of chloropropene carbonate with 99 % selectivity under mild, co-catalyst-, and solvent-free conditions. Furthermore, the reusability of PIL-Br1.0@Zn-CTM and its substrate scope were investigated. The PIL-Br1.0@Zn-CTM exhibited sustained high activity without a significant decrease after seven cycles of reuse, and it also demonstrated excellent catalytic activity for cycloaddition reactions involving low-concentration CO2 with various substituted epoxides. Finally, a mechanism for the cycloaddition reaction catalyzed by the PIL-Brx@Zn-CTM nanocomposite was proposed.