氮掺杂多孔碳负载钯纳米催化剂的制备及催化Suzuki偶联反应的研究

钯催化Suzuki偶联反应是构建联苯类化合物的重要方法之一，在天然产物和复杂药物的合成中发挥着重要的作用。本项目拟合成一系列氮杂环卡宾钯配位聚合物，以此为催化剂前体，通过高温碳化热解制备高效且可循环利用的环境友好型氮掺杂多孔碳负载钯纳米催化剂，并研究其在Suzuki偶联反应中的催化活性和循环使用性能。通过本课题的研究，揭示聚合物的热解机理和催化剂的形成机制，考察热解条件对催化剂微观形貌和孔隙结构的影响规律，阐明“N-杂环卡宾Pd配位聚合物的结构——氮掺杂碳负载Pd催化剂的结构——催化剂的活性”之间的关系，探索催化剂催化Suzuki偶联反应的机制，从而为更高层次上制备新型高效的Pd催化剂提供一定的理论基础。本项目的顺利实施为碳负载型Pd催化剂的制备提供一条崭新的途径，也为Suzuki偶联反应的工程应用提供一种新材料，同时也促进了化学、材料和环境等学科的交叉融合，有着重要的学术意义。

The Suzuki coupling reaction catalyzed by palladium catalysts is one of the most important methods for the fabrication of biphenyl compounds and is considered to be the most useful reaction in the synthesis of natural products and complicated pharmaceutical. In this project, the palladium nanoparticles catalyst supported on N-doped porous carbon with high activity and recyclability will be prepared by direct pyrolysis of a series of N-heterocyclic carbene palladium coordination polymers used as precursors, and their catalytic activity and reusability for Suzuki coupling reactions will be investigated. The pyrolysis mechanism of polymers and formation principle of catalysts will be revealed through the investigation of this project. The effects of the pyrolysis conditions on microcosmic morphology and pore structure of catalysts will be studied. The relationship between the structure of N-heterocyclic carbene palladium coordination polymers and framework of Pd nanoparticles catalysts supported on N-doped carbon and the catalytic ability of catalysts will be illustrated. The mechanism of catalysts for Suzuki coupling reactions will be explored in order to provide theory foundation for the synthesis of new and efficient palladium catalysts. The results obtained in this proposal will develop a new approach to prepare palladium nanoparticles-loaded carbon catalysts and supply a sort of new type material for engineering application of Suzuki coupling reactions, and promote the subject cross of chemistry, material and environment at the same time, which have significant academic meaning.