The mega-merger strategy: M@COF core-shell hybrid materials for facilitating CO2 capture and conversion to monocyclic and polycyclic carbonates

Metal-organic frameworks (MOFs) and covalent organic frameworks (COFs) have garnered significant attention for their potential in CO2 capture and conversion, owing to their unique properties. However, these materials suffer from inherent drawbacks such as poor stability and catalytic activity, leading to unsatisfactory utilization efficiency. In this work, we fabricated a series of novel M@COF hybrid materials by growing pyridine-based COFs with varying thicknesses on NH2-UiO-66 cores. These materials exhibited large specific surface areas and favorable chemical stability. The combination of the high specific surface area of MOF and the multiple interacting pi-pi stacking interactions of COF in these M@COF hybrid materials resulted in significantly enhanced CO2 adsorption performance, surpassing that of individual parent MOF or COF. In addition, an ion-functionalized M@COF-0.15-Br was fabricated through a simple post-synthesis modification. The presence of abundant ion active sites and interfacial synergistic effects in M@COF-0.15-Br effectively facilitated activation of reactants, enabling efficient catalytic conversion of CO2 to monocyclic and polycyclic carbonates. Consequently, the superior CO2 capture and conversion achieved using this M@COF core-shell hybrid material offers a new approach to design advanced functional materials with optimized structures for CO2 capture and conversion.