具有金属活性位点的多酸基MOFs材料设计合成及协同催化研究

项目名称： 具有金属活性位点的多酸基MOFs材料设计合成及协同催化研究

项目编号： No.21301010

项目类型： 青年科学基金项目

立项/批准年度： 2014

项目学科： 数理科学和化学

项目作者： 马凤吉

作者单位： 安阳师范学院

项目金额： 25万元

中文摘要： 金属有机骨架（MOFs）作为一类新兴材料已成为横跨多个学科的研究热点之一。其中，具有金属活性位点的MOFs材料因其独特的结构和优异的性质，备受催化领域的关注。然而，稳定性较差、金属位点催化活性较低等因素一定程度上限制了其作为非均相催化剂的应用。针对此问题，本项目拟选用第一过渡系金属或稀土金属与刚性羧酸类配体或含氮配体配位，并在水（溶剂）热合成过程中引入具有催化活性的多酸（POMs），设计合成具有金属活性位点的多酸基MOFs材料，在保持材料多孔性的同时提高稳定性和催化活性。在对所合成材料进行结构分析和物理性质表征的基础上，揭示材料结构与性质之间的关系。并进一步通过酯化反应作为模型反应评价材料的催化性能，探讨多酸与MOFs金属活性中心的协同催化作用，总结反应温度、时间及催化剂用量等因素对催化剂活性的影响规律，阐明协同催化机理，为设计开发新型催化剂提供实验和理论依据。

中文关键词： 多酸；金属-有机骨架；催化反应；协同作用；

英文摘要： Metal-Organic Frameworks (MOFs) as a kind of promising material has been one of the research focuses in number of disciplines. In particular, MOFs with metal active sites have attracted increasing attention in the field of catalysis due to their unique structures and remarkable properties. However, their application as heterogeneous catalyst is limited to an extent because of the poor stabilities and low catalytic activities of some metal sites. In this project, we will choose rigid carboxylate or nitrogenous organic ligands, and introduce polyoxometalates (POMs) with catalytic activity into MOFs during the process of hydrothermal synthesis, geting POM-based MOFs with metal active sites. The permanent porosity of the materials will be retained with the improving of the stability and the catalytic activity. In addition to the structural analysis and property characterizations, the relation between structure and properties will be investigated. Furthermore, the synergistic catalytic effect is going to be evaluated by esterification reaction. The influence rules between the reaction temperature,time, catalyst dosage and catalyst activity will be summarized. And the mechanism catalyzed by POMs and metal active sites will be clarified. It will provide the experimental and theoretical basis for the design and develop

英文关键词： polyoxometalate；metal-organic framework；catalysis；synergistic effect；