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Fe2+和零价铁活化过一硫酸盐降解酸性橙7
引用本文:聂明华,徐文丽,张文静,吴乐良,董文博,晏彩霞.Fe2+和零价铁活化过一硫酸盐降解酸性橙7[J].环境科学学报,2018,38(10):3997-4005.
作者姓名:聂明华  徐文丽  张文静  吴乐良  董文博  晏彩霞
作者单位:江西师范大学地理与环境学院鄱阳湖湿地与流域研究教育部重点实验室;复旦大学环境科学与工程系上海市大气颗粒物污染与防治重点实验室
基金项目:国家自然科学基金(No.41601523,41601521);江西省自然科学基金(No.20161BAB213079,20161BAB213077);鄱阳湖湿地与流域研究教育部重点实验室开放基金(No.PK2016006);江西省教育厅科技计划项目(No.GJJ150307,GJJ160320);江西师范大学博士启动基金
摘    要:采用环境友好的Fe~(2+)和零价铁(ZVI)作活化剂,活化过一硫酸盐(PMS)来降解水中酸性橙7(AO7).结果表明,在Fe~(2+)-PMS体系中,AO7的降解效果不佳,但通过添加适量的络合剂,AO7的去除率会大幅提高.ZVI在PMS存在下被腐蚀,并能够缓慢、持续不断地释放Fe~(2+).ZVI-PMS体系可以在比较宽泛的pH范围(3~9)有效、快速地降解AO7,并且在酸性条件下降解速率较快.淬灭实验结果显示,硫酸根自由基(SO_4~(·-))对AO7的降解起主要作用.除了Cl~-和高浓度(50 mmol·L~(-1))的NO_3~-能够促进AO7的降解外,其他水中共存的阴离子对AO7在ZVI-PMS体系中的降解具有抑制作用,而腐殖酸(HA)则无明显影响.AO7在超纯水中的去除率高于其他实际水体,但反应90 min后,污水厂出水过滤水和胶体浓缩液中的AO7去除率也可高达98.6%和87.6%,说明ZVI-PMS可能可以有效地去除含有较高DOC含量的污水中的AO7.利用GC-MS检测到辐照后溶液中有3种中间产物,推测主要是通过AO7偶氮键断键后的中间产物进一步氧化形成.此外,TOC在一定程度上降低,说明部分AO7被矿化.

关 键 词:硫酸根自由基  共存物质  降解路径  过一硫酸盐  酸性橙7
收稿时间:2018/1/31 0:00:00
修稿时间:2018/3/4 0:00:00

Degradation of acid orange 7 by peroxymonosulfate activated by Fe2+ and zerovalent iron
NIE Minghu,XU Wenli,ZHANG Wenjing,WU Leliang,DONG Wenbo and YAN Caixia.Degradation of acid orange 7 by peroxymonosulfate activated by Fe2+ and zerovalent iron[J].Acta Scientiae Circumstantiae,2018,38(10):3997-4005.
Authors:NIE Minghu  XU Wenli  ZHANG Wenjing  WU Leliang  DONG Wenbo and YAN Caixia
Institution:Key Laboratory of Poyang Lake Wetland and Watershed Research, Ministry of Education, School of Geography and Environment, Jiangxi Normal University, Nanchang 330022,Key Laboratory of Poyang Lake Wetland and Watershed Research, Ministry of Education, School of Geography and Environment, Jiangxi Normal University, Nanchang 330022,Key Laboratory of Poyang Lake Wetland and Watershed Research, Ministry of Education, School of Geography and Environment, Jiangxi Normal University, Nanchang 330022,Key Laboratory of Poyang Lake Wetland and Watershed Research, Ministry of Education, School of Geography and Environment, Jiangxi Normal University, Nanchang 330022,Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Fudan University, Shanghai 200433 and Key Laboratory of Poyang Lake Wetland and Watershed Research, Ministry of Education, School of Geography and Environment, Jiangxi Normal University, Nanchang 330022
Abstract:This study evaluated the degradation of acid orange 7 (AO7) by peroxymonosulfate (PMS) activated by Fe2+ and zerovalent iron (ZVI). Results show that the Fe2+-PMS system ineffectively removed AO7. However, several chelating agents at an appropriate concentration could significantly improve the AO7 degradation. Comparing with Fe2+, ZVI served as an alternative iron source that could continuously release Fe2+ to activate PMS. The ZVI-PMS system was effective in a broader initial pH range from 3 to 9, and low pH promoted AO7 removal. In addition, the results of scavenging tests suggest that SO4·- radicals other than ·OH were the primary reactive oxygen species in the ZVI-PMS system. Cl- and NO3- (50 mmol·L-1) are found to accelerate AO7 decolourization rates while other anions retard AO7 degradation in the following sequence:NO2- > HPO42- > H2PO4- > HCO3-/CO32- > NO3-. In addition, no obvious impact was found by adding HA. The decolourization rate of AO7 in ultra-pure water was the highest among different water matrices. The removal efficiencies of AO7 from the filtrate and retentate phase of wastewater were up to 98.6% and 87.6% over 90 min, respectively. It is expected that the ZVI-PMS system could be applied for AO7 removal from wastewater containing a considerable organic carbon content. Based on the analysis of GC-MS and TOC, 3 major intermediate products were identified and the preliminary degradation pathways were proposed.
Keywords:sulfate radical  coexisting substances  degradation pathway  peroxymonosulfate  acid orange 7
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