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FeS/SiO 微球作为非均相 Fenton 催化剂增强环丙沙星的催化降解:动力学、反应途径与机制。

Enhanced catalytic degradation of ciprofloxacin with FeS/SiO microspheres as heterogeneous Fenton catalyst: Kinetics, reaction pathways and mechanism.

机构信息

Key Laboratory of Tropical Marine Bio-resources and Ecology, Guangdong Provincial Key Laboratory of Applied Marine Biology, South China Sea Institute of Oceanology, Chinese Academy of Sciences, Guangzhou 510301, China.

Key Laboratory of Tropical Marine Bio-resources and Ecology, Guangdong Provincial Key Laboratory of Applied Marine Biology, South China Sea Institute of Oceanology, Chinese Academy of Sciences, Guangzhou 510301, China.

出版信息

J Hazard Mater. 2017 Apr 5;327:108-115. doi: 10.1016/j.jhazmat.2016.12.045. Epub 2016 Dec 27.

DOI:10.1016/j.jhazmat.2016.12.045
PMID:28049066
Abstract

In this study, the application of FeS/SiO microspheres as a catalyst to activate HO for the degradation of ciprofloxacin (CIP) was systematically investigated. Results demonstrated that the presence of SiO microspheres on the surface of FeS could effectively make the reaction of aqueous Fe and HO smoothly continuous by controlling the release of aqueous Fe from FeS. Nearly 100% of CIP was degraded after 60min under the optimum conditions. A superior performance on the CIP degradation and high reusability of the catalyst was obtained in FeS/SiO microspheres activated HO system. A low concentration of ethylene diamine tetraacetie acid (EDTA) did positively affect the degradation rate of CIP. A synergetic effect between adsorption and oxidation processes contributed to the significant enhancement of CIP degradation. Seven oxidation intermediates were identified during the CIP degradation process, and the direct HO oxidation proved to be a main CIP degradation pathway. For degradation pathway of CIP, oxidation of piperazine ring would be its first step, followed by cleavage of the heterocyclic ring. Subsequently, the substitution, hydroxylation and decarboxylation processes occurred. This is the first report on the feasibility of FeS/SiO microspheres activated HO system for the enhanced degradation of CIP.

摘要

在这项研究中,系统地研究了 FeS/SiO 微球作为催化剂来激活 HO 以降解环丙沙星(CIP)的应用。结果表明,SiO 微球存在于 FeS 表面可以通过控制 FeS 中水溶液 Fe 的释放,有效地使水溶液 Fe 和 HO 的反应顺利连续进行。在最佳条件下,经过 60min,几乎 100%的 CIP 被降解。在 FeS/SiO 微球激活 HO 体系中,催化剂对 CIP 的降解具有优异的性能和高的可重复使用性。低浓度的乙二胺四乙酸(EDTA)对 CIP 的降解速率有积极的影响。吸附和氧化过程之间的协同作用导致 CIP 降解的显著增强。在 CIP 降解过程中鉴定出了 7 种氧化中间产物,直接 HO 氧化被证明是 CIP 降解的主要途径。对于 CIP 的降解途径,哌嗪环的氧化将是其第一步,随后是杂环的断裂。随后,发生取代、羟化和脱羧反应。这是首次报道 FeS/SiO 微球激活 HO 系统在增强 CIP 降解方面的可行性。

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