One-pot non-covalent heterogenization and aromatization of poly(ionic liquids) for metal-/cocatalyst-free and atmospheric CO₂ conversion

The intensification of Lewis acidity/basicity of a given heterogeneous catalyst at a molecular level is an advanced approach for boosting CO2 activation and conversion under extremely mild conditions, which, yet remains a great challenge. This work proposes a one-pot strategy for heterogenization and aromatization of homopolymerized ionic liquids (HpolyILs) through dynamic imine assembly with aromatic spacers for boosting CO2 conversion into cyclic carbonates. The aromatization of HpolyILs can be controllably achieved at room temperature, and has been proven to enhance the Lewis acidity of C-2 proton on imidazolium IL for promoting ring-opening of epoxides and facilitate CO2 bending synchronously. The resultant dynamic covalent polyILs exhibit superior catalytic activity and outstanding recyclability for a variety of epoxides under extremely mild conditions (1 atm, 50-90 degrees C) without metal/co-catalyst consumption. This work offers a feasible to scale-up approach for tailor-made designing high-efficiency heterogeneous catalysts for CO2 utilization, guiding the precise regulation of acid-base catalysis.