Novel neutral and ionic metal-organic frameworks for sustainable catalytic processes

Abstract

This thesis explores new strategies for designing and enhancing the chemical reactivity of metal-organic frameworks (MOFs) to convert waste into valuable chemical products. MOFs were synthesized in combination with 3D-printed polymers and ionic liquids, forming composite materials with improved catalytic performance due to the high dispersion of active sites. Functionalization was achieved by anchoring amino acids to the MOFs, creating multifunctional materials under mild, environmentally friendly conditions using non-toxic, abundant metals and bio-based ligands. Various synthesis methods based on classical, solvent-assisted, and rapid green, onepot approaches were used to develop and characterize these materials. The resulting MOFs were effective in reactions relevant to waste valorization, such as CO₂ fixation and carbonyl activation, operating under mild conditions without additives. The materials demonstrated superior activity, stability, and reusability, aligning with principles of green and circular chemistry, and contributing to the development of advanced heterogeneous catalysts for sustainable chemical processes.