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HSO3-强化Fe3+/S2O82-降解水中双氯芬酸
引用本文:冯姝,王鸿斌,刘义青,付永胜.HSO3-强化Fe3+/S2O82-降解水中双氯芬酸[J].中国环境科学,2021,41(6):2677-2684.
作者姓名:冯姝  王鸿斌  刘义青  付永胜
作者单位:1. 西南交通大学地球科学与环境工程学院, 四川 成都 611756;2. 成都大学建筑与土木工程学院, 四川 成都 610106
基金项目:四川省科技厅重大专项(2018SZDZX0026);中央高校基本科研业务费科技创新项目(2682018CX32)
摘    要:采用HSO3-强化Fe3+/S2O82-降解水中双氯芬酸(DCF),考察了溶液初始pH值,Fe3+、HSO3-和S2O82-用量,溶解氧对HSO3-/Fe3+/S2O82-体系降解DCF的影响;通过自由基淬灭实验,识别了体系中主要的活性物种;最后,探讨了DCF在该体系中的降解产物和转化路径.结果表明:HSO3-可以明显促进Fe3+/S2O82-对DCF的降解,初始pH 4.0时,DCF降解效果最佳.DCF的降解速率随Fe3+或S2O82-浓度的增大而增大;适量增加HSO3-浓度可提高DCF的降解,而过量的HSO3-对DCF降解有一定抑制作用.在通入氮气条件下,DCF去除率仅下降10.4%,无明显的抑制作用.自由基抑制实验表明,该体系含有SO4·-、HO·和SO5·-3种活性自由基,其对DCF降解的贡献率分别为83.0%、12.8%和4.3%.在HSO3-/Fe3+/S2O82-降解DCF的反应中共检测出4种产物,据此提出DCF可能的转化路径为:羟基化、脱羧基、脱水和甲酰化反应.

关 键 词:双氯芬酸  亚硫酸氢盐  过硫酸盐  铁离子  硫酸根自由基  
收稿时间:2020-11-04

Bisulfite enhanced degradation of diclofenac in Fe3+/persulfate system
FENG Shu,WANG Hong-Bin,LIU Yi-Qing,FU Yong-Sheng.Bisulfite enhanced degradation of diclofenac in Fe3+/persulfate system[J].China Environmental Science,2021,41(6):2677-2684.
Authors:FENG Shu  WANG Hong-Bin  LIU Yi-Qing  FU Yong-Sheng
Institution:1. Faculty of Geosciences and Environmental Engineering, Southwest Jiaotong University, Chengdu 611756, China;2. School of Architecture and Civil Engineering, Chengdu University, Chengdu 610106, China
Abstract:The degradation of diclofenac (DCF) by bisulfite enhanced Fe3+/persulfate system was investigated. The influence of pH, Fe3+ dosage, HSO3- dosage, persulfate (PS) dosage and dissolved oxygen on DCF degradation in HSO3-/Fe3+/S2O82-system was explored. The main reactive radical species for DCF removal in this system was also identified by scavenging experiments. Finally, The degradation products and transformation mechanism of DCF by HSO3-/Fe3+/S2O82- were evaluated. DCF could be effectively degraded by the introduction of HSO3- in Fe3+/PS process, and the optimal pH was 4.0. The increased initial Fe3+, HSO3-or PS concentration promoted DCF degradation while excessive HSO3- could inhibit its degradation by acting as a SO4·- scavenger. The degradation rate of DCF was only reduced by 10.4% with bubbling nitrogen, and there was no obvious inhibitory effect in this system. According to the radical scavenging experiments, the contribution of SO4·-, HO· and SO5·- to DCF degradation in HSO3-/Fe3+/S2O82- system were calculated to be 83.0%, 12.8% and 4.3%, respectively. Four transformation products were detected using UPLC-Q-TOF-MS. The potential degradation mechanism of DCF was thus proposed showing four reaction pathways including hydroxylation, decarboxylation, dehydration and formylation.
Keywords:diclofenac  bisulfite  persulfate  ferric ion  sulfate radical  
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