项目名称： 基于量子化学的稀土异戊橡胶催化剂结构-活性定量构效关系及优化设计研究

项目编号： No.21476119

项目类型： 面上项目

立项/批准年度： 2015

项目学科： 数理科学和化学

项目作者： 项曙光

作者单位： 青岛科技大学

项目金额： 89万元

中文摘要： 稀土异戊橡胶正成为世界异戊橡胶发展的方向，提高稀土催化剂中钕的利用率、降低生产成本和产品中的金属含量一直是理论和生产应用研究的热点与难点。项目采用量子化学计算与实验相结合的研究方法，对作为稀土异戊橡胶催化剂主要组分的钕配合物分子结构参数进行基于密度泛函（DFT）的量化计算，将该结构参数与由实验获得的异戊二烯配位聚合催化活性数据相关联，通过遗传算法（GA）建立催化剂结构-活性间的定量构效关系（QSAR）；并按照QSAR设计合成新型的钕配合物，实验测定其催化活性，对QSAR加以验证与反复优化修正。利用验证可靠的QSAR，从理论上解释异戊二烯配位聚合催化剂中钕有效利用率较低的原因，并对稀土异戊橡胶生产用催化剂进行优化设计，获得高活性的新型稀土催化剂，以提高钕的利用率、降低催化剂用量，达到降低异戊橡胶生产成本、提高产品性能的目的。该研究将填补国内外该领域的空白，具有重要的理论意义与实际应用价值。

中文关键词： 量子化学；定量构效关系；优化设计；稀土催化剂；异戊橡胶

英文摘要： Neodymium-catalized isoprene rubber(NdIR) is becoming the development trend of isoprene rubber(IR)in the world.It has long been the hot and difficult research subject both in theoretical and industrial fields to increase the effective percentage of neodymium in the rare earth catalyst to produce NdIR,and as a result to lower down the production cost and the metal content in the final product. A research method combining quantum chemical calculation and laboratry experiments is adopted to correlate the molecular structrual parameters of neodymium complexes obtained from quantum chemical calculation based on density functional theory(DFT)with their catalytic activity data for coordination polymerization of isoprene obtained from laboratry experiments,and therefore a qantitative structure-activity relationship(QSAR)of the neodymium complexes is constructed with an approach of genetic algorithm(GA).Furthermore, the project will go on to verify and optimize the QSAR obtained by designing and synthesizing new types of neodymium complexes according to the QSAR,and determining their catalytic activity through laboratry experiments.With the aid of the verified QSAR,we will try to answer the historical question that why the effective percentage of neodymum in the neodymium complex used as the catalyst for isoprene polymeriation is usually very low. We will then make optimal design to the polymerization catalyst used for NdIR production and obtain a new type of neodymium-based catalyst with high activity,so as to increase the effective percentage of neodymium and lower down the catalyst consumption,and as a result to lower down the production cost of NdIR and improve the product performance.This research project is going to fill the blank in this field at home and abroad with both theoretical significance and application value.

英文关键词： quantum chemistry;quantitative structure-activity relationship(QSAR);optimal design;neodymium-based catalyst;isoprene rubber(IR)