Constructing tunable coordinatively unsaturated sites in Fe-based metal-organic framework for effective degradation...

Micropollutants are ubiquitously detected in the aqueous environment, which needs to be removed by novel materials effectively. Herein, we synthesized a photo-Fenton catalyst based on MIL-53 (Fe) to effectively degrade sulfadimidine, one of the micropollutants in water. Abundant Lewis acid active sites (54.26 μmol/g) were successfully constructed within the metal cluster using FeCl₃·6H₂O, 1,4-benzene dicarboxylate, and modulators. This study reports a strategy by effectively constructing tunable Lewis acid active sites within the cavities in MIL-53 (Fe) via a facile solvothermal reaction for sixteen micropollutants removal. The photo-Fenton degradation of sulfamethazine was completely removed (∼99%) within only 1 min with a small amount of hydrogen peroxide added. Both theoretical calculation and the experiment results prove that introducing the unsaturated coordinated/lewis acid sites can remarkably reduce the band gap energy and increase the charge-separation efficiency by changing the electron configuration with more distribution asymmetry of structures. The effective degradation of structurally diverse pharmaceuticals with environmentally relevant concentrations was studied by immobilizing MOF-catalyst into a PVDF support. This work advanced the development of effective approaches for emergency contaminants control.