Periodate activation by MnFe2O4 spinel for sulfamethoxazole degradation: Iodate radical dominance, degradation pathway, DFT calculation and toxicity assessment
Separation and Purification Technology(2024)
摘要
This study synthesized spinel MnFe2O4 at different temperatures, which was applied to activate periodate (PI) for sulfamethoxazole (SMX) degradation. It was found that the 500-MFO (MnFe2O4 calcined at 500 ℃) demonstrated superior activity in PI activation, with notable sustainability but strong substrate selectivity. Furthermore, a comprehensive analysis, including quenching experiment, electron paramagnetic resonance (EPR) technique, X-ray photoelectron spectroscopy (XPS) analysis, metal ions leaching detection, homogeneous PI activation, and methyl phenyl sulfoxide (PMSO) probe test, revealed that homo- and heterogeneous pathways as well as free and non-free radical routes coexisted in the 500-MFO/PI system. Multiple active species, including iodate radical (IO3•), hydroxyl radical (•OH), superoxide radical (O2•-), singlet oxygen (1O2), and Mn(IV) were identified, with IO3• from heterogeneous activation being the primary species. When PMSO and SMX coexisted, PMSO could react with Mn(IV), promoting the regeneration of Mn reaction sites and the production of IO3•, thereby being beneficial for the degradation of SMX. The degradation pathways of SMX were elucidated through high-performance liquid chromatography-mass spectrometry (HPLC-MS) and density functional theory (DFT) calculation. The acute and chronic toxicity of thirteen by-products to aquatic organisms were predicted using the Ecological Structure Activity Relationships (ECOSAR) software, with the corresponding results revealing that although the toxicity of intermediates fluctuated, the final products were environmentally benign. Therefore, this investigation provides a viable method for SMX degradation in wastewater treatment.
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关键词
MnFe2O4,Periodate,Iodate radical,Degradation pathway,Toxicity assessment
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