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通过电芬顿法对抗菌剂环丙沙星进行氧化降解研究:动力学与氧化产物

Oxidative degradation study on antimicrobial agent ciprofloxacin by electro-Fenton process: kinetics and oxidation products.

作者信息

Yahya Muna Sh, Oturan Nihal, El Kacemi Kacem, El Karbane Miloud, Aravindakumar C T, Oturan Mehmet A

机构信息

Laboratoire d'Électrochimie et Chimie Analytique (LECA), Université Mohammed V - Agdal, Rabat, Morocco.

Université Paris-Est, Laboratoire Géomatériaux et Environnement (LGE), EA 4506, 5 Bd Descartes, 77454 Marne-la-Vallée, France.

出版信息

Chemosphere. 2014 Dec;117:447-54. doi: 10.1016/j.chemosphere.2014.08.016. Epub 2014 Sep 6.

Abstract

Oxidative degradation of the antimicrobial agent ciprofloxacin hydrochloride (CIP) has been investigated using electro-Fenton (EF) treatment with a constant current in the range 60-500 mA. The process generates highly oxidant species OH in situ via electrochemically monitored Fenton reaction. The EF experiments were performed using cells with a carbon felt cathode and Pt anode. Effect of applied current and catalyst concentration on the kinetics of oxidative degradation and mineralization efficiency have been investigated. Degradation of CIP followed pseudo-first order reaction kinetics. The rate constant of the oxidation of CIP by OH has been determined to be (1.01 ± 0.14) × 10(10) M(-1) s(-1) by using competitive kinetics method. An optimum current of 400 mA and a catalyst concentration of Fe(2+) at 0.1mM are found to be optimal for an effective degradation of CIP under our operating conditions. A remarkably high degree of mineralization (>94%) was obtained at 6h of treatment under these conditions. A number of stable intermediate products have been identified using HPLC and LC-MS/MS analyses. Based on the identified reaction intermediates, a plausible reaction pathway was proposed for the mineralization process. The high degree of mineralization obtained in this work highlights the potential application of EF process in the efficient removal of fluoroquinolone based drugs in aqueous medium.

摘要

采用恒电流在60 - 500 mA范围内的电芬顿(EF)处理方法,研究了抗菌剂盐酸环丙沙星(CIP)的氧化降解过程。该过程通过电化学监测的芬顿反应原位生成高氧化性物质·OH。EF实验在具有碳毡阴极和铂阳极的电解槽中进行。研究了施加电流和催化剂浓度对氧化降解动力学和矿化效率的影响。CIP的降解遵循准一级反应动力学。采用竞争动力学方法测定了·OH氧化CIP的速率常数为(1.01 ± 0.14) × 10(10) M(-1) s(-1)。发现在我们的操作条件下,400 mA的最佳电流和0.1 mM的Fe(2+)催化剂浓度对于有效降解CIP是最优的。在这些条件下处理6小时可获得高达94%以上的显著矿化度。使用高效液相色谱(HPLC)和液相色谱 - 串联质谱(LC-MS/MS)分析鉴定了许多稳定的中间产物。基于鉴定出的反应中间体,提出了矿化过程的合理反应途径。本研究中获得的高矿化度突出了EF工艺在高效去除水介质中氟喹诺酮类药物方面的潜在应用。

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