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Pyridinium Functionalized Ionic Metal-Organic Frameworks Designed as Bifunctional Catalysts for CO2 Fixation into Cyclic Carbonates.

Ionic metal-organic frameworks (MOFs) offer a new platform to design and construct complete heterogeneous bifunctional catalytic systems for the chemical fixation of CO2 with epoxides. Herein, we developed a series of bifunctional pyridinium ionic MOF heterogeneous catalysts (66Pym-RXs and 67BPym-MeI) by the post-synthetic N-alkylation of non-coordinated pyridine sites in porous MOFs. The synergetic catalytic effect of acidic sites with nucleophilic anions in the ionic MOF significantly enhanced the catalytic activity towards the cycloaddition of CO2 with epoxides to produce cyclic carbonates under a cocatalyst-free and solvent-free mild condition. The catalytic activity of ionic MOFs is easily tuned by the introduction of different alkyl groups into pyridinium cations and halide ions. The 66Pym-iPrI catalyst displayed the highest catalytic performance in terms of the turnover number (TON) value for the synthesis of cyclic carbonate. The proposed alternative method provides the means of developing functional N-heterocyclic groups for the new design of bifunctional ionic MOFs as potential heterogeneous catalysts for CO2 fixation applications.