富亲核氧介孔复合氧化物上甲苯的高选择性催化氧化

项目名称： 富亲核氧介孔复合氧化物上甲苯的高选择性催化氧化

项目编号： No.21203093

项目类型： 青年科学基金项目

立项/批准年度： 2013

项目学科： 物理化学

项目作者： 王晓丽

作者单位： 南京工程学院

项目金额： 25万元

中文摘要： 耐高温介孔复合氧化物的制备和烷烃C-H键的选择性氧化是目前两大待解决的难题。本项目针对甲苯侧链C-H键氧化过程中目标产物苯甲醛选择性低的现状，首次提出利用模板剂-柱撑粒子法制备高温稳定的介孔复合氧化物，并在其上构建丰富的亲核氧活性中心，再负载贵金属或廉价过渡金属活性中心，为甲苯的选择性催化氧化制备出高选择性、高活性的催化剂。对催化剂的组成、结构、表面亲核氧的数量和分布进行充分表征，明确模板剂和柱撑粒子在介孔结构形成中的作用，认识亲核氧的产生机理，为耐高温的富亲核氧介孔复合氧化物的可控化制备提供理论依据。在釜式反应器中选择性催化氧化甲苯，重点研究亲核氧活性中心对苯甲醛选择性的影响、金属活性中心的对催化剂活性的影响，认识双中心协同催化作用，探讨催化剂的构效关系，揭示催化活性中心来源和反应机理，为甲苯乃至烷烃C-H的选择性催化氧化探索出新的催化体系。

中文关键词： 氧化；甲苯；苯甲醛；甘油；非均相

英文摘要： Nowadays, the two problems to be solved in academia are the preparation of mesoporous mixed oxides with high temperature stability and the selective oxidation of C-H bond in alkane. In the present investigation, we attempt to prepare highly efficient catalysts to improve the selectivity to benzaldehy in the selective oxidation of side chain in toluene. Firstly, the mesoporous mixed oxides with high temperature stability are prepared according to the method of template-pillared particles. Then, abundant nucleophilic oxygens are built, and noble or cheap transition metals are also supported on the surface of mixed oxides. In order to understand the effect of templates and pillared particles on the formation of mesoporous structure, and to clarify the generation mechanism of nucleophilic oxygen species, the composition, structure and the amount and distribution of surface nucleophilic oxygens in catalysts are fully characterized. All these studies will provied theoretical basis for the controllable preparation of mesoporous mixed oxides with high temperature stability. The catalytic performance of the obtained suportted mixed oxides is investigated in the selective oxidation of toluene. Our attention mainly focus on the role of nucleophilic oxygen species in benzaldehy selectivity, and the role of metal active cent

英文关键词： oxidation；toluene；benzaldehyde；glycerol；heterogeneous