“金属有机大环-多酸”主客体自组装体系的建立与催化应用

项目名称： “金属有机大环-多酸”主客体自组装体系的建立与催化应用

项目编号： No.21271025

项目类型： 面上项目

立项/批准年度： 2013

项目学科： 数理科学和化学

项目作者： 许颜清

作者单位： 北京理工大学

项目金额： 80万元

中文摘要： 本项目主要利用配位化学和超分子自组装方法，构建新型的金属有机大环(Metal Organic Macrocycle, MOMC)包裹多酸簇(Polyoxometalate, POM)的主客体自组装体系，即"MOMC-POM"。在该体系中，MOMC带高的正电荷，POM则带多个负电荷，两者间会产生强的静电吸引作用；同时，MOMC内部孔道与目标POM在尺寸和形状上的匹配也会带来有利的热力学能。因此，这种MOMC嵌套POM的主客体微观结构，可以为多酸组分引入金属有机外壳的保护，实现多酸组分在分子水平上的分散和固定，为其在催化领域的应用中多相化难题的解决方案提供新思路。我们拟围绕过渡金属取代的Keggin、Dawson及夹心型杂多酸，通过设计合成与组装得到相应的MOMC-POM产品，用于催化CO2和环氧化合物生成环状碳酸酯的体系，希望在保证良好催化性能同时实现催化剂的回收及多次循环利用。

中文关键词： 过渡金属取代的多酸；金属有机大环；固载；催化；

英文摘要： This project aims at the foundation of novel host-guest self-assembly system of "Metal Organic Macrocle-Polyoxometalate" ("MOMC-POM") by the methods of coordination chemistry and supramolecular self-assemble. The MOMC possesses high positive charges and the POM belongs to polyanions with multi-negative charges. So there would exist strong electrostatic interactions between the two compositions. With such electric field together with the shape-match fator, it is possible to give rise to a self-assembly system that the POMs are encapsuled or wrapped in the interior hollow of the MOMC, which would afford a metal-organic shell for the POM. As a result, it would bring a brand new way to solve the heterogeneous catalysis problem on POM. Moreover, we will choose the transitional-meatal-substituted Keggin, Dawson and Sandwich-type heteropolyoxoanions to assemble with appropriate MOMC, and then we will further investigate on their catalytic property of turning carbon dioxide into cyclic carbonate. We hope we would fulfill the good catalytic result and the recycle preperty of the catalysis, which finally contribute on the pratical usage of the POM with experimental and theoretical support.

英文关键词： PW11M；Organometallic macrocyclic compounds；load；catalysis；