Targeted degradation of refractory organic pollutants in wastewater based on molecularly imprinted catalytic materials: Adsorption process and degradation mechanism

摘要

In this study, the role of weak interactions in the targeted adsorption of refractory organic pollutants by imprinted catalysts (MIL100@MIP) was elucidated. Through the imprinting technique, the targeted adsorption capacity for sulfamethoxazole (SMX) was increased by 3 times. With the synergy of adsorption and degradation, the removal of SMX reached 49.03 mg/g in MIL100@MIP/PS system. Methacrylic acid (MAA), acrylamide (AM), and 4-vinyl pyridine (4-VP) were used to construct different imprinting recognition sites. UV-vis spectral analysis indicated that MIL100@MIP adsorbed SMX through weak interactions. Dynamic experiments showed that MIL100@MIP-4-VP exhibited the best adsorption performance. Density functional theory (DFT) calculations and wave function analysis indicated that 7L-7L stacking played a dominant role in the SMX adsorption process. The solvent effect was investigated by dynamics simulation. Finally, three possible SMX degradation pathways and the catalytic mechanism of MIL100@MIP were proposed based on the EPR and intermediate product analysis. This study has valuable guidance for improving the targeted degradation performance of imprinted catalytic materials.

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