超疏水性有机无机杂化层状钛硅亚微球的合成及其催化烯烃环氧化反应性能研究

项目名称： 超疏水性有机无机杂化层状钛硅亚微球的合成及其催化烯烃环氧化反应性能研究

项目编号： No.21271153

项目类型： 面上项目

立项/批准年度： 2013

项目学科： 数理科学和化学

项目作者： 肖丽萍

作者单位： 浙江大学

项目金额： 78万元

中文摘要： 钛硅分子筛类材料是一类以过氧化氢为氧化剂的有机物选择性氧化反应的有效催化剂，独立分散的四配位钛和高疏水性的微观环境是获得高效催化活性的关键。本项目提出合成一种超疏水性、高比表面积且催化活性中心高度分散的有机无机杂化的层状钛硅亚微球材料。以有机硅氧烷基和钛的醇盐为共同前驱体，采用气溶胶辅助自组装的方法（Arosol-Assisted Self-Assembly, AASA）使有机、无机分子在三维限制空间内自组装成超疏水性钛硅亚微球结构，通过控制溶胶-凝胶过程和挥发诱导自组装的方式来调控材料的结构、形貌以及疏水性能；重点研究超疏水层状钛硅亚微球的形成过程；研究超疏水层状钛硅材料室温下对环己烯环氧化的催化活性和催化机理，探究超疏水材料的结构与催化活性的构效关系；在此基础上针对烯烃环氧化反应设计合成出低能耗、高效率、高稳定性的选择性氧化催化剂，为拓展超疏水材料在催化领域的应用提供可行的途径。

中文关键词： 有机无机杂化；钛硅材料；超疏水性；烯烃环氧化；

英文摘要： Titanium-containing zeolites and related materials have been found to be effective for the selective oxidation of organic compounds with aqueous hydrogen peroxide. Isolated tetrahedrally-coordinated Ti4+ and its location in a hydrophobic environment is the key for high catalytic activity. In this project, we propose to synthesize an organic-inorganic hybrid layered titanosilicate submicrosphere with superhydrophobicity, high surface area and well dispersed catalytic active center. The strategy of synthesis of this superhydrophobic layered titanosilicate sub-sphere is based on an arosol-assisted self-assemble (AASA) process by using alkytriethoxysilanes and alkyl orthotitanates as precursors without adding any organic template. The structure, morphology and hydrophobicity of the synthesized materials will be tuned by controlling the sol-gel process and evaporation-induced assembly procedure. This project will focus on the self-assemble mechanism of superhydrophobic layered titanosilicate. Furthermore, the catalytic activity of the resultant materials will be assayed in olefins epoxidation at room temperature. After establishing the structure-activity relationships, the catalytic mechanism of spuerhydrophobic titanosilicate materials in olefins epoxidation will be further investigated. This superhydrophobic organi

英文关键词： organo-inorgano hybrid；titanosilicates；super-hydrophobicity；epoxidation of olefins；