基于量子化学的有机磷农药光催化降解机理研究

项目名称： 基于量子化学的有机磷农药光催化降解机理研究

项目编号： No.21307035

项目类型： 青年科学基金项目

立项/批准年度： 2014

项目学科： 环境科学、安全科学

项目作者： 戴珂

作者单位： 华中农业大学

项目金额： 26万元

中文摘要： 有机磷农药是我国使用量最大的农药品种，残存于水和土壤中的有机磷农药及其初级代谢产物已经造成了严重的环境污染。利用光催化氧化技术降解有机磷农药是环境污染治理的一项重要研究课题，但有机磷农药的光催化降解中间产物和降解机理仍不十分清楚。 本项目拟采用光谱、色谱和色谱－质谱联用等仪器分析技术研究有机磷农药光催化降解的动力学、中间/矿化产物和降解历程，考察反应条件对光催化降解动力学和中间产物的影响。在实验研究的基础上，借助量子化学从头算方法(密度泛函理论)计算研究有机磷农药的降解过程，获得有机磷农药分子、产物自由基及过渡态的分子构型、轨道能量、电子云密度等信息，计算降解反应的活化能和反应速率常数。采用理论计算结合实验研究的方法，阐明有机磷农药的光催化降解机理以及反应条件对降解机理的影响机制，揭示有机磷农药在光催化反应中的转化规律，为绿色高效去除有机污染物提供科学依据和技术支持。

中文关键词： 有机磷农药；光催化降解；中间产物；量子化学计算；

英文摘要： Organophosphorus pesticide, one of the most used pesticides in China, has caused severe envioronmental problems due to its residuel and prelimary metabolic intermediates in soil and water. Therefore, photocatalytic degradation of organophosphorus pesticide by photocatalytic oxidation is an important research topic of the environmental pollution control. However, the photocatalytic degradation intermediates and mechanism of organophosphorus pesticide is still beyond our knowledge. This project aimed to study the degradation pathway, degradation intermediates, mineralized products and degradation process by a variety of means of instrumental analysis (spectrometry, chromatography and chromatography-mass spectra), to study the molecular structure, orbital energy, electron density and degradation process of organophosphorus pesticide and its reactive/transition state intermediates by using quantum chemical method (density functional theory). Based on the combination of experimental and theoretical results, uncover the photocatalytic degradation mechanism and its influencing mechanism by reaction conditions. The outputs of this project would promote our understanding on the basic discipline for the metabolic regularity of organophosphorus pesticide in photocatalytic degradation and facilitate the utilization of photo

英文关键词： organophosphorus pesticide；photocatalytic degradation；intermediates；quantum chemical calculation；