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

SEPARATION AND PURIFICATION TECHNOLOGY [2022]
Mingzhe Li, Wenli Yao, Min Yu, Changduo Sun, Xinquan Deng, Fengjuan Chen, Lei Zhou, Yian Zheng
ABSTRACT

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.

MATERIALS

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