文章简介
晶态多孔材料CPF-5-Mn后合成修饰及其催化应用研究
  

摘要:通过溶剂热方法合成的晶态多孔材料催化剂CPF-5-Mn具有稳定性高、活性高、可回收再利用等优势。利用多孔材料后合成修饰的方法将其活性位金属Mn进行离子交换,成功获得CPF-5-Mn的结构类似物CPF-5-FeCPF-5-CuCPF-5-Co。此方法弥补了采用相应的金属前驱体直接溶剂热合成法无法合成的不足。将CPF-5-Mn的系列催化剂应用于催化含杂原子底物碳氢键活化中,直接活化杂原子邻位C-H键,以中等产率得到了目标杂原子邻位胺化产物,具有较高的化学选择性,这拓展了CPF-5系列催化剂在碳氢键活化尤其是碳氢键胺化中的应用,对生物活性分子后修饰、医药中间体合成中非均相催化剂的选用提供了新思路。

关键词:晶态多孔材料;后合成修饰;非均相催化剂;C-H键胺化

AbstractThe crystal porous material catalyst CPF-5-Mn synthesized by solvothermal method has the advantages of high stability, high activity and recycling. By using the method of postsynthetic modification of porous material, the active sites of CPF-5-Mn were modified by ion exchange to the structure analogs CPF-5-Fe, CPF-5-Cu, CPF-5-Co. This method makes up for the deficiency of direct solvothermal synthesis of corresponding metal precursor. The series catalysts of CPF-5-Mn were applied to catalyze the C-H bond activation of hetero-atomic substrates, directly activating the ortho C-H bond of hetero-atom, and the target amination product was obtained with medium yield and high chemical selectivity, which expanded the application of CPF-5-Mn series catalysts in C-H bond activation, especially in selective amination. It provides a new idea for the selection of heterogeneous catalysts for post-modification of bioactive molecules and synthesis of pharmaceutical intermediates.

Key wordsCrystalline porous materials; postsynthetic modification; Heterogeneous Catalyst; C-H amination




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