期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 316, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2022.121631
关键词
Advanced oxidation process; Catalyst-free; Fluoroquinolones; Excited triplet state; Photoexcitation pathway
资金
- National Natural Science Foundation of China [4210071265, 52070133]
- Full-time Postdoctoral Research and Development Fund Project of Sichuan University [2020SCU12057]
- Applied Basic Research Project of Science and Technology Department of Sichuan Province [2021YJ0379]
This study reports the catalyst-free activation of peroxydisulfate (PDS) via visible light for the removal of fluoroquinolones (FQs). The mechanism of PDS activation by the excited triplet state of FQs ((3)FQs*) is proposed. Experimental results show that PDS can generate more ·OH in the presence of (3)FQs*. Both radical and non-radical oxidation reactions contribute to the degradation of FQs in the system. QTOF analysis and DFT calculations clarify the degradation pathways and reactive sites. The system exhibits excellent selective oxidation for FQs.
Recently, catalyst-free activation of peroxydisulfate (PDS) via visible light has been extensively investigated. However, the intrinsic relationship between the activation of PDS and the characteristics of pollutants has been largely ignored. This study reports that PDS activation by visible light without any artificial catalyst for the removal of fluoroquinolones (FQs), which reduced the adverse on ecological environment and human health concerns. Importantly, the mechanism of PDS activation by the excited triplet state of FQs ((3)FQs*) was proposed. Experimental results demonstrated PDS could generate more center dot OH with the existence of (3)FQs*. Meanwhile, the electron transfer pathways from FQs or (3)FQs* to PDS were studied. Both radical and non-radical oxidation reactions lead to the degradation of FQs in the Vis/PDS system. The degradation pathways and reactive sites were clarified by QTOF analysis and DFT calculations. Additionally, the degradation experiments of various contaminants demonstrated that the system showed excellent selective oxidation for FQs.
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