高铁酸盐氧化水中双氯芬酸污染物的反应机制和毒性评价
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- 英文论文题名：Oxidative Removal of Diclofenac by Ferrate(Ⅵ) in Aqueous Media:Reaction Mechanism and Toxicity Evaluation
- 论文作者：汪应灵 ; 袁建梅 ; 谢友海 ; 刘国光
- 英文论文作者：Yingling Wang ; Jianmei Yuan ; Youhai Xie ; Guoguang Liu ; Key Laboratory of Medical Molecular Probes ; School of Basic Medical Sciences ; Xinxiang Medical University ; School of Environment ; Henan Normal University ; Key Laboratory for Yellow River and Huaihe River Water Environment and Pollution Control ; Ministry of Education
- 年：2016
- 作者机构：新乡医学院基础医学院医用分子探针重点实验室;河南师范大学环境学院黄淮水环境污染与防治教育部省部共建重点实验室;
- 论文关键词：双氯芬酸 ; 高铁酸盐 ; 反应机理 ; 生物毒性
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第二十六分会：环境化学
- 语种：中文
- 分类号：X52
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第二十六分会 ; 环境化学
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：117k
- 原文格式：D
- 会议级别：全国
摘要
双氯芬酸作为新兴污染物经常在水源水,甚至饮用水中被检测到,且含量较高[1-2]。本文研究了Fe(Ⅵ)氧化双氯芬酸的反应机理、毒性变化及TOC去除效果。根据UPLC-MS质谱图,结合双氯芬酸的结构特点和Fe(Ⅵ)的反应特性,推测出5种初级产物,反应由Fe(Ⅵ)直接亲电氧化为主导,·OH自由基贡献不大,主要反应途径包括母体物质及其产物的羟基取代反应和中间体自由基的偶联反应,生成的副产物主要有氯代酚类、醌类及其它二聚体形态[3]。随着反应时间的延长,反应液的矿化程度逐渐提升,而毒性在反应初期稍有下降,然后随着双氯芬酸不断降解,毒性开始增大而后又缓慢减小,在双氯芬酸刚刚消失以后达到最大,说明双氯芬酸的初级降解产物氯代酚类衍生物对毒性贡献小,而中间体自由基形成的醌类二聚体的毒性最大。
Diclofenac(DCF) is one of the most commonly used non-steroidal anti-inflammatory drugs and emerging micro-organic contaminants,which has been frequently detected with high levels in the aquatic environment.The reaction mechanism,toxicity variation and TOC removal efficiency were explored during the ferrate(Ⅵ) oxidation process.Five primary products were identified by UPLC-MS combined with the structure characteristic of DCF and reactivity properties of Fe(Ⅵ).Fe(Ⅵ) rather than ·OH radical plays a dominant role during the oxidation process.The reaction mechanism was proposed to be hydroxylation of DCF and degradation products and coupling reaction of organic radical intermidates.DCF oxidation occurred at the phenol moiety and yielded chlorophenol,quinine intermediates and other organic dimmers.As the reaction time was prolonged,the mineralization of solution was gradually improved,while there was a slight decrease of inhibition rate during the initial reaction period.Subsequently,the overall toxicity began to increase rapidly and then decreased slowly,reaching a maximum value when DCF had just completely disappeared.These results suggested that higher concentrations of chlorophenol derivatives did not yield appreciable effect on the overall toxicity,relative to quinine dimmer.
Diclofenac(DCF) is one of the most commonly used non-steroidal anti-inflammatory drugs and emerging micro-organic contaminants,which has been frequently detected with high levels in the aquatic environment.The reaction mechanism,toxicity variation and TOC removal efficiency were explored during the ferrate(Ⅵ) oxidation process.Five primary products were identified by UPLC-MS combined with the structure characteristic of DCF and reactivity properties of Fe(Ⅵ).Fe(Ⅵ) rather than ·OH radical plays a dominant role during the oxidation process.The reaction mechanism was proposed to be hydroxylation of DCF and degradation products and coupling reaction of organic radical intermidates.DCF oxidation occurred at the phenol moiety and yielded chlorophenol,quinine intermediates and other organic dimmers.As the reaction time was prolonged,the mineralization of solution was gradually improved,while there was a slight decrease of inhibition rate during the initial reaction period.Subsequently,the overall toxicity began to increase rapidly and then decreased slowly,reaching a maximum value when DCF had just completely disappeared.These results suggested that higher concentrations of chlorophenol derivatives did not yield appreciable effect on the overall toxicity,relative to quinine dimmer.
引文
[1]Souza B M,Dezotti M W C,Boaventura R A R,et al.Chemical Engineering Journal,2014,256:448-457.
[2]Michael I,Achilleos A,Lambropoulou D,et al.Applied Catalysis B:Environmental,2014,147:1015-1027
[3]Souza B M,Dezotti M W C,Boaventura R A R,et al.Chemical Engineering Journal,2014,256:448-457
[2]Michael I,Achilleos A,Lambropoulou D,et al.Applied Catalysis B:Environmental,2014,147:1015-1027
[3]Souza B M,Dezotti M W C,Boaventura R A R,et al.Chemical Engineering Journal,2014,256:448-457