卤代芳烃化学发光的结构效应、分子机制及其应用

发布时间：2018-02-04 16:48

本文关键词： 卤代芳烃高级氧化化学发光羟基自由基卤代醌中间体半醌自由基结构-效应关系　出处：《化学进展》2017年09期 　论文类型：期刊论文

【摘要】：卤代芳烃是一类在环境中广泛存在的化合物,因其可能导致人体及生态系统的潜在环境风险而被公众日益关注。最近,高级氧化过程作为一种"环境绿色友好"的技术被用于处理和降解这类难降解持久性有机污染物。我们先前意外发现,卤代醌的典型代表物四氯苯醌与过氧化氢反应不仅会生成·OH,还会产生专一依赖于·OH的两次化学发光。进一步研究发现,对产生·OH的高级氧化体系而言,不仅四氯苯醌的前体五氯酚和其他卤代酚能产生化学发光,其余所有经测试的卤代芳烃也能产生化学发光。在此基础上,对19种氯酚同系物产生化学发光的结构-效应关系进行了系统研究,结果发现:氯原子取代数目越多化学发光越强。有趣的是,氯酚的化学发光还与生成的氯代醌中间体以及半醌自由基呈良好相关性。基于上述结果,我们认为反应生成了某种醌中间体以及激发态多羰基产物,正是它们导致了化学发光。进而开发出一种快速灵敏的化学发光分析手段,不仅可检测和定量痕量的卤代芳烃,还可为预测其毒性以及实时监测降解动力学提供有用信息。
[Abstract]:Halogenated aromatics are a class of compounds widely existing in the environment. Recently, halogenated aromatic hydrocarbons have attracted increasing public concern for their potential environmental risks to human bodies and ecosystems. Advanced oxidation processes are used as an "environmentally green" technology to treat and degrade such refractory persistent organic pollutants. The reaction of tetrachlorobenzoquinone with hydrogen peroxide, a typical haloquinone, not only produces 路OH, but also produces two chemiluminescence dependent on 路OH. For advanced oxidation systems producing 路OH, not only pentachlorophenol and other halogenated phenols, precursors of tetrachlorobenzoquinone, can produce chemiluminescence, but all other halogenated aromatics tested can also produce chemiluminescence. The structure-effect relationship of chemiluminescence produced by 19 chlorophenol congeners was systematically studied. It was found that the more the number of substituted chlorine atoms, the stronger the chemiluminescence. The chemiluminescence of chlorophenol also has a good correlation with the intermediate of chloroquinone and the free radical of semi-quinone. Based on the above results, we believe that some quinone intermediates and excited polycarbonyl products were formed. It is they that lead to chemiluminescence, and a rapid and sensitive method for chemiluminescence analysis is developed, which not only detects and quantifies trace halogenated aromatics. It can also provide useful information for predicting its toxicity and monitoring degradation kinetics in real time.
【作者单位】：中国科学院生态环境研究中心环境化学与生态毒理学国家重点实验室;中国科学院大学;
【基金】：中国科学院战略性先导科技专项(B类)(No.XDB01020300) 国家自然科学基金项目(No.21321004,21477139,21577149)资助~~
【分类号】：X592
【正文快照】： during·OH-dependent PCP degradation4 The structure-activity relationship study on the CLemission from the degradation of chlorinatedphenols4.1 Chlorinated phenols could generate CL duringthe·OH-generating AOPs4.2 A good correlation between CL emission

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