Degradation of sulfamethoxazole by persulfate activated with heterogeneous catalyst MSBC-ZnFe2O4
摘要
This study addresses the challenge of refractory degradation of sulfonamide antibiotic sulfamethoxazole (SMX) in aquatic environments. A novel heterogeneous catalyst, comprising Fe3O4 and ZnFe2O4 supported on municipal sludge-derived biochar (SBC) (denoted as MSBC-ZnFe2O4), was constructed for the degradation of sulfamethoxazole via heterogeneous activation of persulfate (PDS). Unlike conventional magnetic biochar or ferrite catalysts that typically rely on a single-component active phase, the uniquely designed Fe3O4/ZnFe2O4 heterojunction in this system synergistically accelerates the Fe2+/Fe3+ redox cycle through directional interfacial electron transfer, which is the key factor accounting for the markedly enhanced PDS activation and SMX degradation efficiency. Material characterization revealed that the high specific surface area and abundant functional groups of SBC effectively inhibited metal particle agglomeration and maintained magnetic separation performance. Response surface methodology (RSM) optimization demonstrated that under the conditions of catalyst dosage 1.70 g/L, PDS concentration 6.70 mmol/L, pH 5.10, and solution temperature 30.5 °C, the SMX degradation rate reached 92.87%. The catalyst retained 84.51% of its initial activity after five consecutive cycles, with the homogeneous degradation rate due to leached ions was below 13.25%. Radical quenching experiments,electron paramagnetic resonance (EPR) analysis and electrochemical chronoamperometry experiments demonstrated that sulfate radicals (SO4⁻·) and hydroxyl radicals (·OH) served as the primary reactive oxygen species, while the non-radical pathway involving singlet oxygen (1O2) also contributed synergistically to the degradation process. This research overcomes the technical bottlenecks of easy agglomeration and difficult recovery common in iron-based catalysts through sludge resource utilization and heterojunction catalytic design, providing an efficient, stable, and environmentally friendly advanced oxidation technology solution for antibiotic pollution control.
Graphical abstract