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以铁/铜氧化物作为过一硫酸盐的非均相活化剂对四环素的降解机制

[Degradation Mechanism of Tetracycline Using Fe/Cu Oxides as Heterogeneous Activators of Peroxymonosulfate].

作者信息

Li Jing, Bao Jian-Guo, Du Jiang-Kun, Leng Yi-Fei, Kong Shu-Qiong

机构信息

School of Environmental Studies, China University of Geosciences, Wuhan 430074, China.

出版信息

Huan Jing Ke Xue. 2018 Jul 8;39(7):3203-3211. doi: 10.13227/j.hjkx.201709227.

Abstract

A green, highly efficient, and porous copper-ferrite heterogeneous catalyst (Fe-Cu-400) with good magnetism was synthesized via a coprecipitation method. The catalysts were characterized using XRD, BET, FESEM, and EDS. The performance of Fe-Cu-400 as a catalyst was evaluated by activating peroxymonosulfate (PMS) for degradation of tetracycline (TC) in aqueous solution and investigating the influence of several water parameters. The Fe-Cu-400/PMS system showed a greater TC degradation ability, and the degradation rate of TC was enhanced with an increase in the PMS concentration and the initial pH of the coupled Fe-Cu-400/PMS system. Anions including HPO, HCO, and Cl promoted TC degradation, whereas NO showed a low inhibitory influence. In addition, Fe-Cu-400 exhibited excellent reusability towards activating PMS for TC degradation after five runs of tests. Possible mechanisms of the activation of PMS by Fe-Cu-400 and the main reactive species were proposed based on radical identification tests and XPS analysis. Furthermore, a potential degradation pathway was proposed that included hydrolysis and sequential removal of -methyl, hydroxyl, and amine functional groups according to the results of LC-MS and TOC detections.

摘要

通过共沉淀法合成了一种具有良好磁性的绿色、高效、多孔铜铁氧体多相催化剂(Fe-Cu-400)。采用X射线衍射(XRD)、比表面积分析(BET)、场发射扫描电子显微镜(FESEM)和能谱分析(EDS)对催化剂进行了表征。通过活化过一硫酸盐(PMS)降解水溶液中的四环素(TC)并研究几个水质参数的影响,评估了Fe-Cu-400作为催化剂的性能。Fe-Cu-400/PMS体系表现出更强的TC降解能力,随着PMS浓度的增加以及Fe-Cu-400/PMS耦合体系初始pH值的升高,TC的降解率提高。包括HPO、HCO和Cl在内的阴离子促进了TC的降解,而NO表现出较低的抑制作用。此外,经过五次测试后,Fe-Cu-400在活化PMS降解TC方面表现出优异的可重复使用性。基于自由基鉴定试验和X射线光电子能谱(XPS)分析,提出了Fe-Cu-400活化PMS的可能机制以及主要活性物种。此外,根据液相色谱-质谱联用(LC-MS)和总有机碳(TOC)检测结果,提出了一条潜在的降解途径,包括水解以及依次去除甲基、羟基和胺官能团。

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