项目名称： 羟基自由基引发多溴联苯醚替代品的大气转化机制及动力学

项目编号： No.21477015

项目类型： 面上项目

立项/批准年度： 2015

项目学科： 环境科学、安全科学

项目作者： 谢宏彬

作者单位： 大连理工大学

项目金额： 50万元

中文摘要： 多溴联苯醚替代品(新型溴代阻燃剂和有机磷阻燃剂)在大气环境中已被频繁检出，特别是在极地地区，其检出浓度已超过被广泛研究的多溴联苯醚，成为一种具有潜在环境风险的污染物。根据有机污染物大气转化的一般规律及这些替代品的分子结构特征，它们与OH自由基反应将是其大气转化的重要途径。因此，从污染物环境生态风险评价角度来看，揭示OH自由基引发这些替代品的大气化学具有重要意义。本项目拟采用量子化学计算和微观动力学模拟相结合的方法，研究OH自由基与代表性替代品的反应机制、动力学及其生成产物在大气环境中(O2/NO)的进一步转化机制、动力学，以确定替代品的大气寿命及产物分布；研究大气中的水对代表性替代品大气转化的影响机制，以更好地理解它们在实际大气中的转化。研究结果对于多溴联苯醚替代品的环境风险评价及增强水对大气污染物转化影响的理解具有重要意义。

中文关键词： 替代阻燃剂；羟基自由基；反应机理；动力学；计算模拟

英文摘要： Emerging brominated flame retardants and organophosphorus flame retardants as the alternatives of polybrominated diphenyl ethers (PBDEs) have been frequently detected in the atmosphere. Especially in the polar region, their detected concentration was even higher than that of widely concerned PBDEs. Now, the alternatives of PBDEs have become the pollutants with potential environmental risk. According to the general knowledge on transformation of organic pollutants in the atmosphere and the structural feature of the alternatives of PBDEs, the reactions of the alternatives of PBDEs with ?OH should be their important removal way. Therefore, in the view of the environmental risk evaluation on the pollutants, it is essential to reveal the atmospheric chemistry of alternatives of polybrominated diphenyl ethers initiated by ?OH. In this project, the quantum chemical calculation and kinetic modeling are used to 1) investigate the reaction mechanism and kinetics of the representative alternatives of PBDEs with ?OH and ensuing reactions of the produced active radicals including isomerization, dissociation, and bimolecular reaction with O2/NO, to predict their atmospheric lifetime and product distribution; 2)explore the influence of water, which is an important component in the atmosphere, on the above reaction process to b

英文关键词： AFRs；？OH；Mechanism；kinetics；Computational study