Diamide-linked imidazolyl Poly(dicationic ionic liquid)s for the conversion of CO₂ to cyclic carbonates under ambient...

The ionic active centers and hydrogen-bond donors (HBDs) in heterogeneous catalytic materials are highly beneficial for enhancing the interaction between solid-liquid-gas three-phase interfaces and promoting effective fixation of carbon dioxide (CO₂). Diamide-linked imidazolyl poly(dicationic ionic liquid)s catalysts PIMDILs (PMAIL-x and PBAIL-2) were synthesized through the copolymerization of diamide-linked imidazolyl dicationic ionic liquids (IMDILs) with divinylbenzene (DVB), which successfully enable the simultaneous construction of high-density and uniformly distributed ionic active centers (2.014-4.883 mmol g^-1) and hydrogen-bond donors (HBDs). The as-synthesized PIMDILs present excellent catalytic activity in promoting the cycloaddition of CO₂ with epoxides. PMAIL-2 could convert epichlorohydrin (ECH) with a quantitative conversion of 99.8 % (selectivity > 99 %) under ambient pressure. Furthermore, only a decrease in activity of 5 % was observed even after six cycles of recycling. The excellent conversions (>97.3 %) were achieved for various terminal substituted epoxides. The experimental and characterization results reveal that the high-density ionic active centers and amide HBDs can effectively activate the reaction substrates, their synergistic effect plays a crucial role at the catalyst interface. This work is expected to provide some useful insights for the rational construction of heterogeneous catalysts for CO₂ conversion.