咪唑类离子液体与二噁英类物质相互作用的多尺度理论研究

Dioxins, known as "centurial poison", are the most poisonous materials in persistent organic pollutants (POPs). The prevention and reduction of the dioxin contamination is one of the important environmental topics in the world. Ionic liquids, as a kind of new medium and functional materials, have many unique physicochemical properties and are expected to be potential absorption of dioxins. This proposal aims to explore the mechanism of the interaction between imidazolium ionic liquids and dioxins, and to reveal the microscopic nature of the interaction between the two molecules at the molecular level using quantum chemical calculations and molecular dynamics simulations. .Our main aims include: understanding the composite system containing ionic liquids and dioxin, and elucidating the microscopic essence of the recognition between ionic liquids and dioxins. The capture capacity of ionic liquids to dioxins will be analyzed and improved. We will also investigate the effects of ionic liquids on the structure and spectrum character of dioxins to explore the effective imidazolium-based ionic liquids for the enrichment and detection of dioxins. The routine spectrum methods of detecting dioxins will be also discussing.All of those works will provide theoretical guidance for relevant experimental detection and analysis techniques, as well as new insights and clues for pollution control of dioxins.

二噁英是毒性最强的一类持久性有机污染物，有“世纪之毒”之称。二噁英污染防治是当今国际社会共同关注的重大环境问题之一。离子液体作为一种新型介质和复合功能材料具有许多优良物理化学性能，被期望是捕获二噁英类物质的潜在载体。本项目拟用多尺度理论化学方法研究咪唑类离子液体与二噁英类物质相互作用的分子机理，探讨二噁英富集与检测方面的一些基础科学问题，通过量子化学计算和分子动力学模拟等手段系统研究离子液体与二噁英组成的二元复合体系，从分子水平上揭示二者相互识别的微观本质，分析离子液体阴阳离子在捕获二噁英过程中所扮演的角色，掌握改进其捕获能力的有效手段，分析离子液体对二噁英结构与谱学性质的影响，筛选富集、检测二噁英的有效离子液体，探讨检测二噁英的常规谱学方法，以期为相关的实验研究提供一定的理论指导，为发展相关的检测分析技术奠定一定的理论基础。

二噁英是毒性最强的一类持久性有机污染物，有“世纪之毒”之称。二噁英污染防治是当今国际社会共同关注的重大环境问题之一。离子液体作为一种新型介质和复合功能材料具有许多优良物理化学性能，被期望是捕获二噁英类物质的潜在载体。通过收集了210种二噁英的实验资料，完成对其红外和拉曼光谱计算，建立了数据库并实现程序化。结果表明：甲醛能够有效阻止木质素结构单元间发生聚合反应，使木质素单体产率接近理论值。通过密度泛函理论计算揭示了甲醛分子高效阻止木质素聚合反应的内在本质。通过DFT计算研究了二氯化锰（MnCl2）和1-甲基-3-(3-磺酸丁基)咪唑甲基磺酸离子液体([C4SO3HMIM][CH3SO3])在1-丁基-3-甲基咪唑氯离子液体([BMIM]Cl)中催化葡萄糖异构化为果糖，异构化反应涉及葡糖糖开环、质子转移、1,2-H迁移、闭环等过程，其中1,2-H迁移为整个反应的决速步骤，其能垒为33.0 kcal/mol。计算结果改进了人们对金属氯化物和功能性离子液体协同催化葡萄糖转化为果糖机理的认识，为相关的催化剂设计提供了一定的理论指导。