MIL-101(Fe)-loaded mixed matrix membrane for H2O2 activation in fenton-like catalysis and enhanced degradation of ibuprofen

초록

Ibuprofen (IBP), a widely used nonsteroidal anti-inflammatory drug, is frequently identified in aquatic ecosystems and may pose long-term environmental risks. In this study, using the phase inversion method, mixed matrix membranes (MMMs) were synthesized with polyvinylidene fluoride (PVDF), polyvinylpyrrolidone, and a metal-organic framework (MIL-101(Fe)) for the degradation of IBP in water. The synthesized PVDF/MIL-101(Fe) MMMs (denoted as PM-x, x = 2, 4, 6, and 8 wt.%) were employed as adsorbents and catalysts for hydrogen peroxide (H2O2) activation. Among the fabricated membranes, PM-8 exhibited a 96.2% IBP removal efficiency under optimized catalytic conditions, determined through systematic investigation of key parameters. Additionally, PM-8 maintained a high degradation efficiency (over 84.7%) across a broad pH range (3-11) and showed excellent reusability, retaining over 90.0% removal efficiency after five reuse cycles. The removal mechanism involved various adsorption interactions, including pi-pi electron donor-acceptor interactions, surface complexation, and hydrogen bonding, along with catalytic oxidation driven by reactive oxygen species (center dot OH, O2 center dot-, and 1O2), generated through Fe(II)/Fe(III) redox cycling. UPLC-MS/MS analysis identified major intermediate products formed via hydroxylation, decarboxylation, and dehydrogenation pathways, outlining a plausible degradation route that ultimately leads to the mineralization of IBP. This study presents a promising strategy for IBP removal from aquatic environments, contributing to advancements in wastewater treatment technologies.

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