Efficient customization of multi-target molecularly imprinted MOFs for degradation of refractory organic pollutants: Theoretical design and selective degradation mechanism

This study proposes a novel theoretical molecular design strategy for the customization of multi-target molecularly imprinted metal-organic framework (MOF) catalysts. Based on the theoretical calculation, high-performance imprinted catalysts (MIP-DVB) were successfully synthesized. The results demonstrated that molecular imprinting significantly enhanced the selective adsorption capacities of MIP-DVB toward sulfonamides (SAs). Its adsorption capacities for sulfamethoxazole (SMX), sulfamethazine (SDM), and sulfacetamide (SCT) were 4.25, 4.02, and 3.18 times that of Fe₃O₄@MOFs, respectively. Under the synergistic effect of adsorption and catalysis, the total removal amount of SAs by the catalyst exceeded 25 mg/g. In the mixed system, the catalyst exhibited excellent selectivity recognition ability, with an imprinting factor of 2.06. Electrostatic potential analysis indicates that the common imprinted recognition site of -SO₂NH- is the key to multi-targeted imprinting. The complex hydrogen bond effect on the sulfonamide group plays an important role in the targeted adsorption process. Additionally, the degradation mechanism of SAs was also explored, and possible degradation pathways were proposed based on the identification of intermediates. This study provides important theoretical guidance for the efficient synthesis of multi-targeted imprinted catalysts and significantly advances the industrial application of imprinted MOFs for the removal of refractory organic pollutants from water.