Efficient periodate activation by chalcopyrite for levofloxacin hydrochloride degradation: Effects of sulfur species and dominant pathways of reactive oxygen species

SEPARATION AND PURIFICATION TECHNOLOGY(2024)

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摘要
In this study, chalcopyrite (CuFeS2) was synthesized, characterized, and used to activate periodate (PI), and the mechanism of levofloxacin hydrochloride (LVF) removal at a neutral pH was elucidated. LVF removal was directly related to its concentration and that of PI, CuFeS2 dosage, and pH. More than 90 % of 10 mu M LVF was removed within 30 min using the CuFeS2/PI system, and the apparent rate constant (kobs) was 7.85-fold higher than that of an FeS/PI system. Electron paramagnetic resonance spectroscopy, quenching studies, and quantitative analysis revealed the roles of different reactive oxygen species in LVF removal and their dominant pathways. O-2(center dot-) was generated during the cycling of metal species and played a major role in LVF degradation, as the pollutant structure contains N-based heterocycles, F and carboxyl groups, etc. The surface-bound Fe(II) represented the dominant active sites for PI activation, and the reductive S species and Cu(I)-Fe(III) interaction could enhance the regeneration of the Fe(II) active sites. Based on the results of ultra-high-performance liquid chromatography-mass spectrometry and density functional theory calculations, the intermediates of LVF were identified, and possible pathways were proposed. In addition, IO4- was transformed into IO3- without the generation of undesired iodine species (HOI, I-2(,) and I-3(-)). Therefore, this study could provide an effective method based on the CuFeS2/PI system for use in fluoroquinolone antibiotic removal.
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关键词
Fluoroquinolones,Cu-Fe bimetallic sulfide,Sulfur species,Advanced oxidation processes,Wastewater treatment
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