Core–shell NH2-UiO-66@iCOPs with built-in “adsorption engines” for improving CO2 adsorption and conversion

Integrating the advantages of metal–organic framework (MOFs) and ionic organic polymers (iCOPs), we fabricated a series of novel hybrid materials (core–shell M@iCOPs) by growing iCOP shell layers of varying thicknesses on the NH₂-UiO-66. These M@iCOP hybrids, with NH₂-UiO-66 serving as an embedded “adsorption engine,” exhibit richer pore channels, which combined with the nitrogen-rich structure and π-π stacking interactions in the shell layer of the iCOPs, which led to a significant enhancement of CO₂ adsorption with up to 3.33 mmol·g⁻¹ at 0 °C and 1 bar. Remarkably, M@iCOPs-400, which possesses abundant ionic and Lewis acid sites, demonstrates excellent performance in CO₂ conversion under milder conditions through interfacial synergistic effect, affording various cyclic carbonates in 90–99% yields. Overall, this research provides a straightforward and cost-effective approach for constructing core–shell M@iCOP materials.