新型多氮杂环席夫碱键合MCM-41对胺参与三组分反应的催化性能研究

发现和发展操作简单、资源利用率高、高原子经济性和生态好的反应模式是发展高效、高选择性有机合成反应的关键科学问题。本申请拟基于"多组分"反应策略，使用多氮杂环席夫碱键合MCM-41介孔材料作为非均相催化剂，胺类化合物作为一种氮源，直接参与三组分一步高效合成系列有机含氮化合物。从有机改性的介孔材料MCM-41入手，通过化学修饰将多氮杂环席夫碱经共价键键合到介孔材料的硅表面，合成系列多氮杂环席夫碱键合MCM-41介孔材料非均相催化剂，利用微量反应测试其催化性能，建立最优反应条件，并进行底物适应性考察。同时，探索催化剂结构特征与反应活性之间的关联，提出一个合理的反应机制。此反应催化剂和产物易于分离，可回收循环使用，符合绿色化学和原子经济原则。本项目的研究内容不仅可以丰富合成方法学，而且还可以探索将此类介孔材料应用于石油化工反应中，从而达到降低成本、减少能耗、保护环境的目的，具有十分重要的理论和现实

The reaction of simple operation, high resource utilization, high atom economy and pollution-free is a very important family in chemistry. Herein, we wish to study the highly selective synthesis of organic nitrogen compounds directly from amine promoted by multi-nitrogen heterocycle Schiff base supported MCM-41 catalyst using the three-component reactions methodology in this project. A series of multi-nitrogen heterocycle Schiff base supported MCM-41 catalysts, heterogeneous catalyst, will be synthesized by covalent bond bonding between organically modified MCM-41 and multi-nitrogen heterocycle aldehyde, and then investigated for the reaction. Under the optimized reaction conditions, the substrate scope is to be further examined. Meanwhile, the relationship between the catalyst structure and the reactivity, as well as the reaction mechanism will be further discussed. A possible catalytic cycle is to be proposed. Furthermore, the catalyst can be easily separated from the reaction mixture and reusable with high activity and selectivity. Hence, it is accord with the green chemistry and atom economy principle. This research will have important guiding significance for the further development of synthetic methodology, and also can further explore the mesoporous materials in petrochemical yield, and achieve lower costs, reduce energy consumption and protect the environment. There will be an important theoretical and practical significance to further study.