3d双金属掺杂MCM-41催化氧化合成医药中间体及其机理研究

Mesoporous silica materials MCM-41 doped with bimetallic elements which are cobalt or vanadium combination with other 3d metal elements will be synthesized. The materials will be characterized by different methods. The effect of synthesis condition will be studied on the structure. The synthesized mesoporous materials will be used to catalytic oxidation of tetralin and bromotoluene to synthesize pharmaceutical intermediates such as tetralone and bromobenzaldehyde with air, oxygen or hydrogen peroxide as oxidant; and the effect of reaction solvent, reaction time, temperature， the amount of catalyst and oxidant on the efficiency of catalysis will be studied. And we will investigate the relationship between the structure of the different catalysts, the double hetero-atom interaction and the catalytic oxidation activity, and reveal the nature of the catalyst structure and catalytic activity, and thus guide us to prepare related catalyst and study the corresponding catalytic oxidation。. If the project will be put into practice, it can promote the development of synthesis technology of pharmaceutical intermediates, and promote the application of mesoporous molecular sieves in the synthesis of pharmaceutical intermediates, and thus to provide the experimental basis for design of more efficient and green catalyst.

四氢萘酮、溴代苯甲醛、溴代苯甲酸等重要医药中间体的传统合成成本高、污染大，相关绿色合成急需高选择性氧化催化剂。将钴或钒与其它3d金属元素组合，对介孔硅材料MCM-41进行双金属元素改性合成，通过相关表征获得催化剂结构、表面性质以及活性中心的相关信息，研究不同合成条件对分子筛结构的影响，并用相应材料催化空气、氧气及双氧水氧化四氢萘合成四氢萘酮，氧化溴代甲苯合成溴代苯甲醛等医药中间体，研究反应溶剂、时间、温度及催化剂用量等对催化效率的影响；探讨不同催化剂结构、双杂原子间的相互作用与催化氧化活性间相互关系，揭示催化剂结构和催化氧化活性之间的本质，进而指导相关催化剂制备以及相应催化氧化的实验研究。 项目的实施，可促进医药中间体合成技术的发展，推动介孔分子筛在医药中间体合成中的应用，为设计更高效和绿色的催化剂提供实验依据。

本项目通过钴或钒与3d常见金属共掺杂、铜离子、碘化亚铜等改性MCM-41、硅胶等介孔硅材料催化氧化四氢萘合成医药中间体α-四氢萘酮，获得了较好的催化效果。研究高效催化材料的构筑，发展了多种新催化材料，开展了介孔材料的制备、表征及催化氧化性能的研究，探索了制备条件对催化剂催化性能的影响，探讨了反应溶剂、反应时间、温度、催化剂用量等对催化性能的影响，并通过自由基捕捉实验推测了相关反应机理，实现了α-四氢萘酮的高选择性转化。工作为α-四氢萘酮的高效转化奠定了科学基础，促进了介孔材料在医药中间体合成方面的应用，为设计更高效和绿色的催化剂提供了实验依据。

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