固载型杂多酸-离子液体的设计及其原位一步合成

项目名称： 固载型杂多酸-离子液体的设计及其原位一步合成

项目编号： No.21203060

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： 赵海红

作者单位： 湖南师范大学

项目金额： 24万元

中文摘要： 本项目针对目前固载型杂多酸催化剂在液相氧化反应中活性组分易溶脱，高负载量催化剂制备过程中杂多阴离子易崩解、对载体破坏严重等问题，利用咪唑离子液体结构对催化活性中心的稳定作用，通过设计含离子液体单元的有机-无机杂化介孔材料，并在其中构建稳定且微观化学环境均一的杂多酸催化活性中心，一步法原位合成固载型杂多酸-离子液体催化剂。考察离子液体功能化有机硅前驱体和有机-无机杂化介孔材料的合成方法、载体织构性质、载体表面亲/疏水性与酸/碱性等表面性质、离子液体与杂多酸的结合方法等对催化剂活性中心结构的影响。以苯甲醇水相氧化反应为探针反应，研究不同的杂多酸组成及载体织构性质等对催化活性中心结构和催化氧化反应中活性及选择性的影响规律,以期在固载型杂多酸催化剂的分子设计等基础研究和醇类绿色氧化等应用研究方面取得创新性研究成果。

中文关键词： 杂多酸；离子液体；固载；有机-无机杂化介孔材料；催化氧化

英文摘要： The use of supported heteropoly acid catalysts in liquid phase oxidation offers several advantages over homogeneous ones, including ease of recovery and recycling, atom utility, and enhanced stability. However, it also has some disadvantages, such as leaching of active species into the reaction medium, destruction of heteropolyanion and supports due to much heteropoly acid contents.In order to overcome the above-mentioned problems, attempts have been, in this project, made to combine mesoporous silicas having tunable nano-channel and rather high surface area with heteropoly acids-based imidazolium ionic liquids, aiming to fabricate the task-specific active sites of heteropoly acid on pore surface and/or in framework of mesostructure. As such, this project has focused on the in-situ one-pot synthesis of heteropoly acids-based supported ionic liquids. And the catalytic activities of the synthesised materials have been tested in the heterogeneous oxidation of alcohols using H2O2 as an oxidizing agent. The effects of the ionic liquid and heteropoly acid contents on mesostructure and relative catalytic performance of the obtained catalyst were investigated.We hope to bring forth new achievements in supported heteropoly acid catalysts and the green oxidation of alcohols.

英文关键词： heteropoly acid；ionic liquid；supported；organic-inorganic hybrid mesoporous materials；catalytic oxidation