新型壳聚糖多孔微球负载过渡金属催化材料的构建及性能

项目名称： 新型壳聚糖多孔微球负载过渡金属催化材料的构建及性能

项目编号： No.21203123

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： 曾敏峰

作者单位： 绍兴文理学院

项目金额： 25万元

中文摘要： 本项目以生物可降解天然高分子壳聚糖为基体材料，以水溶性有机高分子或原位生成无机二氧化硅纳米粒子为模板致孔剂，设计制成具有大比表面积、高力学强度、高孔隙率的各种孔径尺寸的壳聚糖基多孔微球（微球直径1-2mm）。以此微球为载体，络合过渡金属（钯、镍、铜等）可制成壳聚糖多孔微球负载过渡金属催化材料，进一步高温碳化，得到具有超大比表面积、多级孔结构的多孔碳球负载过渡金属材料。重点考察这些新型非均相催化材料在各类有机偶联反应中的催化活性、稳定性和重复循环使用性，深入研究微观结构、过渡金属类型、反应类型、反应条件等对反应的影响，探索催化循环中各价态的过渡金属与载体孔道表面的大量氨基、羟基的作用机理，以期找到设计用于绿色催化偶联反应的新型壳聚糖基多孔微球负载过渡金属催化剂的普遍性规律，为实现复杂有机物分子的绿色、经济合成打下基础。

中文关键词： 壳聚糖；过渡金属；非均相催化；有机偶联反应；结构-性能关系

英文摘要： In this project, biodegradable nature polymer (chitosan) is used as an effective catalysts support material. Novel porous chitosan microspheres （diameter: 1-2 mm）with high specific areas, excellent mechanical properties,and high porous structure were prepared by a template extraction method. The used porogens are water soluble polar polymers or in-situ generated silica inorganic particles. Different transition metals (such as palladium,nickle or copper) were supported on such novel porous chitosan microspheres. The resultant porous chitosan supported transition metal catalyst can be further high-temperature carbonized to form high porous carbon miccrospheres supported transition metal catalysts. These heterogeneous catalysts were applied in catalyzing typical organic coupling reactions. The reactivity, stability and recyclability of this novel heterogeneous catalysts were thoroughly investigated.The influences of the microstructure of the catalysts, kinds of transition metals, reaction types, and reaction conditions on the reactions were also studied. Meanwhile, the valence state changes of the transition metals and the mechanism of their interaction with the polar groups (-OH and NH2) of chitosan were determined. The main purpose of this project is to develop a high effective chitosan supported transition metal

英文关键词： chitosan；transition metals；heterogeneous catalysis；organic coupling reactions；structure-property relations