腐植酸对多溴联苯醚可见光光化学转化的影响及机理研究

项目名称： 腐植酸对多溴联苯醚可见光光化学转化的影响及机理研究

项目编号： No.21477080

项目类型： 面上项目

立项/批准年度： 2015

项目学科： 化学工业

项目作者： 孙春燕

作者单位： 绍兴文理学院

项目金额： 80万元

中文摘要： 作为持久性有机污染物，多溴联苯醚（PBDEs）的环境光化学行为及转化产物引起了高度关注，目前研究主要集中于PBDEs在环境中吸收紫外光的直接光解行为，而另一个重要的光化学转化途径--可见光间接光解却在极大程度上被大家忽视，这意味着PBDEs在环境中的一个新的转化途径。本项目研究环境中广泛存在的腐植酸（HA）及其组成、光学性能对PBDEs的可见光间接光解转化影响。结合HA中主要活性结构以苯甲酸和苯酚/苯醌为模型化合物，运用低温/瞬态电子顺磁技术、瞬态吸收光谱等手段以及动力学同位素效应等方法，揭示卤键络合物激发和HA敏化注入电子等不同的反应机理。 通过研究HA存在下PBDEs在液-液、固-液等不同环境界面的间接光解行为和产物分析，揭示平行脱溴vs逐级脱溴不同途径之间的制约关系, 为阐明PBDEs在自然界中光转化规律及减少转化产物的环境影响提供理论依据。

中文关键词： 多溴联苯醚；腐植酸；可见光；间接光解；环境转化

英文摘要： The transformation and products of polybrominated diphenyl ethers (PBDEs) by photochemistry in environment arouse high environmental concern because of their toxicity as persistent organic pollutants. The research on the photochemistry of PBDEs has mainly on the direct photolysis of PBDEs under UV light irradiation in the environment, while indirect photolysis of PBDEs by organic acid existed in the environment has been rarely reported. Indirect photolysis will extend to visible light. It will play the important role in the transformation of PBDEs by photochemistry in environment. We will research that PBDEs undergo indirect photolysis by humic acid abundant existed in the environment under visible light irradiation. The mechanism via the excitation of the halogen-binding-based complex between PBDEs and humic acid or the electron injection from sensitized humic acid will be researched by spin-trapping electron spin resonance (ESR) and so on used the benzoic acid and phenol/quinine as model compounds. The indirect photolysis of PBDEs and products will be further investigate under different reaction conditions to declare the rules on the parallel or step by step manners in the debromination of PBDEs. This study will help find the rules of photochemistry transformation of PBDEs in nature and reduce the effects of PBDEs on the environment.

英文关键词： Polybrominated diphenyl ethers;Humic acid;Visible light;Indirect photolysis;Environmental transformation