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

SEPARATION AND PURIFICATION TECHNOLOGY(2022)

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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 Fe2+, 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 spe-cies (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 HCO3- (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 SO4 center dot-, center dot OH, O-2(center dot-) and non-free radical O-1(2). Through free radical quantitative experiments, the concentration of SO4 center dot- and (OH)-O-center dot at 60 min was determined respectively to be 11.84 mu M and 0.14 mu M, proving the dominant role of SO4 center dot- . 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 structur-e-activity relationships analysis.
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Key words
Hydrogel,Peroxymonosulfate,Ciprofloxacin,Degradation,Toxicity
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