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Hydrogel 3D network derived and in-situ magnetized Fe@C for activation of peroxymonosulfate to degrade ciprofloxacin

Journal 2022 · IF 9.136 · 发表于 2022 年 7 月 19 日
作者: Mingzhe Li,Wenli Yao,Min Yu,Changduo Sun,Xinquan Deng,Fengjuan Chen,Lei Zhou,Yian Zheng
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摘要

Hydrogels possess 3D network with abundant reactive groups, and can bind with active metal ions within their confined 3D structure for fabricating functional materials . In this study, a chitosan grafted polyacrylic acid (CTS-g-PAA) hydrogel was prepared for loading Fe 2+ , which was then converted into magnetic Fe@C via subsequent pyrolysis process . In Fe@C activated peroxymonosulfate (PMS) (Fe@C/PMS) system, the degradation behaviors of ciprofloxacin (CIP) were systematically investigated, including influencing parameters, reactive oxygen species (ROSs), degradation mechanism and potential eco-toxicity of degradation intermediates. The results showed that CTS-g-PAA supported, in-situ derived magnetic Fe@C had not only stable catalytic ability at pH 3.0–9.0, but also high degradation efficiency in the presence of inorganic Cl − and HCO 3 − (5–20 mM) as well as organic humid acid (10 and 20 mg/L). Under the optimized conditions, the degradation efficiency of CIP could reach to 96.84 % within 1 h. In Fe@C/PMS system, the main ROSs involved free radicals SO 4 •− , •OH, O 2 •− and non-free radical 1 O 2 . Through free radical quantitative experiments, the concentration of SO 4 •− and •OH at 60 min was determined respectively to be 11.84 µM and 0.14 µM, proving the dominant role of SO 4 •− . By HPLC-MS analysis, the degradation products were proposed via four degradation pathways, including hydroxylation, defluorination and decarboxylation, as well as the ring opening of quinolone and piperazine. Finally, the potential eco-toxicity of CIP and its degradation intermediates was evaluated by using ECOSAR method based on quantitative structure–activity relationships analysis.

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