| 吉非罗齐在热活化过硫酸盐体系中的降解机制研究 |
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| 引用本文： | 马京帅,吕文英,刘国光,陈平,李富华,王枫亮,陆一达,姚琨. 吉非罗齐在热活化过硫酸盐体系中的降解机制研究[J]. 环境科学学报, 2016, 36(10): 3774-3783 |
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| 作者姓名： | 马京帅 吕文英 刘国光 陈平 李富华 王枫亮 陆一达 姚琨 |
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| 作者单位： | 广东工业大学环境科学与工程学院, 广州 510006,广东工业大学环境科学与工程学院, 广州 510006,广东工业大学环境科学与工程学院, 广州 510006,广东工业大学环境科学与工程学院, 广州 510006,广东工业大学环境科学与工程学院, 广州 510006,广东工业大学环境科学与工程学院, 广州 510006,广东工业大学环境科学与工程学院, 广州 510006,广东工业大学环境科学与工程学院, 广州 510006 |
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| 基金项目： | 国家自然科学基金（No.21377031）；广东省科技项目（No.2013B020800009） |
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| 摘 要： | 以降血脂药物吉非罗齐(GEM)为目标污染物,研究其在热活化过硫酸盐体系中的降解机制.结果表明,GEM的降解过程符合准一级反应动力学规律,增加过硫酸盐初始浓度或升高反应溶液温度都可以显著提高GEM的降解速率常数(kobs),其反应的表观活化能Ea为133.14k J·mol~(-1).酸性和中性条件下GEM的降解效果要好于碱性条件.自然水体中的腐植酸(HA)和HCO_3~-对GEM的降解有明显的抑制作用.自由基清除实验表明,在酸性和中性条件下,SO_4~(·-)对GEM的降解起主导作用,而在碱性条件下,HO·成为体系主要的氧化物种.利用HPLC-MS/MS技术共检测到11种中间产物,推测GEM的降解路径涉及苯环的羟基化和醛基化反应、苯环侧链的环化作用和脱羧反应以及醚支链的断裂.
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| 关 键 词： | 吉非罗齐 过硫酸盐 热活化 动力学 降解机制 路径 |
| 收稿时间： | 2016-01-12 |
| 修稿时间： | 2016-02-11 |
Degradation mechanism of gemfibrozil in heat-activated persulfate oxidation process |
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| MA Jingshuai,L,#; Wenying,LIU Guoguang,CHEN Ping,LI Fuhu,WANG Fengliang,LU Yida and YAO Kun. Degradation mechanism of gemfibrozil in heat-activated persulfate oxidation process[J]. Acta Scientiae Circumstantiae, 2016, 36(10): 3774-3783 |
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| Authors: | MA Jingshuai,L&# Wenying,LIU Guoguang,CHEN Ping,LI Fuhu,WANG Fengliang,LU Yida YAO Kun |
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| Affiliation: | School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006,School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006,School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006,School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006,School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006,School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006,School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006 and School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006 |
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| Abstract: | The degradation mechanism of lipid-lowering drug gemfibrozil (GEM) in heat-activated persulfate oxidation process was investigated. The experimental results show that the degradation of GEM followed pseudo-first-order kinetics. The pseudo-first-order kinetic rate constant (kobs) increased markedly with increasing initial persulfate concentration and temperature, and the activation energy (Ea) was calculated to be 133.14 kJ·mol-1. Acidic and neutral conditions were more beneficial for the degradation of GEM than basic condition. Humic acid (HA) and HCO3- in natural water had strong inhibitory effects on the degradation of GEM. Radical scavenging test revealed that SO4·- played a critical role under acidic and neutral conditions, while HO· was predominant oxidizing species at basic condition. Eleven intermediates were identified by applying HPLC-MS/MS techniques, and it is speculated that the degradation pathways of GEM involved hydroxylation and aldehydes reactions of benzene ring, the cyclization and decarboxylation reaction of branched chain, as well as the cleavage of ether side chain. |
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| Keywords: | gemfibrozil persulfate heat-activated kinetics degradation mechanism pathways |
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