生物质平台化合物定向转化催化剂的构效关系研究

项目名称： 生物质平台化合物定向转化催化剂的构效关系研究

项目编号： No.21473155

项目类型： 面上项目

立项/批准年度： 2015

项目学科： 数理科学和化学

项目作者： 侯昭胤

作者单位： 浙江大学

项目金额： 92万元

中文摘要： 生物质平台化合物的高效转化具有重要的意义，但是在液相反应介质中适合于平台化合物转化的固体催化剂的构效关系与传统的气-固相催化反应过程有明显的差别、研究基础相对薄弱；本项目拟以生物质平台化合物（如乙醇、甘油和葡萄糖）的液相转化为目标，设计和制备系列亲疏水性可调、酸碱性可调、吸附性能可控、水热稳定性良好的多功能固体催化剂，希望通过对催化剂的分散性能、吸附性能、水热稳定性以及反应前后结构与性能的变化规律研究,深入揭示平台化合物转化反应中催化剂的构效关系规律,详细研究反应介质（溶剂等）对平台化合物转化途径和机理的影响、对催化剂结构和性能的影响等，寻找催化剂+溶剂的协同作用规律，为生物质平台化合物的高效转化提供理论支持、为液-固相反应中催化剂构效关系规律提供实验依据。这些研究不仅对生物质平台化合物的高效转化具有重要的意义，同时对传统催化理论的发展也具有重要的意义。

中文关键词： 平台化合物；多相催化剂；构效关系；选择氧化；反应机理

英文摘要： Catalytic transformation of biobased chemicals to valuable products is of great importance for the development of biore?nery. Most reported catalytic transformation processes were performed in liquid phase because of the higher boiling points, good solubility (in water) of these biobased chemicals. As the field of chemistry continues to encourage the development of sustainable chemical processes utilizing environmentally benign reaction conditions, the use of water as a green solvent becomes an attractive choice. However, the structure-activity relationships of heterogeneous catalysts that scientists have developed over the last century in the gas-solid phase petrochemical industry have not been optimized for use of biobased chemicals in aqueous media. On the base of the active role of water in selective oxidation of glycerol and ethanol, additional research is needed to understand how solvent affects other catalytic transformations on traditional transition metal catalysts. The aim of this suggested project is to disclose the structure-activity relationships of solid catalysts in catalytic oxidation of ethanol, glycerol and glucose in liquid phase. And we will focus our study on the role of solvents as well as the structure of catalysts in these oxidation reactions. A series of solid materials with optimized hydrophility/hydrophobility, acidity/basicity, selective adsorption of biobased chemicals, good hydrothermal stability will be synthesized, and used as the supports for transition metals, alloys, and/or oxides. These catalysts will be tested in the selective oxidation of ethanol, glycerol and glucose in liquid phase. The structure and surface properties of these catalysts in both static state and in-situ state will be characterized in detail, and these properties will be discussed with their activity and selectivity. The role of solvent (water) on reaction mechanism, and on the structure of solid catalysts will be screened, and we will try our best to find the synergistic effect of catalyst + solvent in the transformation of biobased chemicals.The structure-activity relationships of solid catalysts in selective oxidation in liquid phase will be proposed on the base of these research works. During the research process, we will discuss our results and suggestions with those famous scientists in this area through manuscript submission, international congress and lectures. Several young scientists will grow up during this research process. We think that this project will contribute to the development of heterogeneous catalysis, especially in the area of selective oxidation of biobased chemicals in liquid phase.

英文关键词： Biobased chemicals;Solid catalysts;Structure-activity relationships;Selective oxidation;Reaction mechanism