文档介绍:华中科技大学
硕士学位论文
金属配位天然高分子催化剂的合成与性能研究
姓名:王欣
申请学位级别:硕士
专业:高分子化学与物理
指导教师:杨济活
20040511
摘要
本论文主要研究了天然生物高分子络合物催化剂的合成表征及其在氢化反
应中的催化性能我们选择了多种天然生物高分子如甲壳质甲壳胺羊毛羧
甲基纤维素等作为配体与金属 Pt, Pd 等金属离子络合制备了一系列的高分子
催化剂并通过 XPS, IR 对催化剂进行了表征
首先在 SiO 2-CMC-Pt 催化性能研究中以苯甲苯硝基苯等单取代苯环化
合物均以 100%的产率获得目标产物以双取代的甲苯胺为重点研究对象研究不
同反应条件对催化性能的影响结果显示催化剂催化活性很高该催化剂用于苯乙
胺的不对称加氢也获得 %的产率和 %的光学收率其次我们又合成了
SiO 2-CMC-Pd 催化剂研究了它在硝基苯苯甲醛的催化加氢的性能最后我们
还研究了以羊毛为配体的 Wool-Pd 催化剂在催化加氢上的催化活性结果也证明羊
毛是一种优良的配体催化剂的催化性能好另外本论文还对双酚 F 的加氢作了
研究发现 SiO 2-CMC-Pt 催化剂对此有一定的效果
研究表明天然生物高分子与金属络合后有着优异的催化性能而且所需的反
应条件温和同其它催化剂相比天然生物高分子金属络合物催化剂具有制备简单
催化活性高选择性好稳定性好可以重复使用等优点对于这类催化剂的研究
具有应用价值和广阔前景
关键词天然高分子催化加氢苯甲醛硝基苯甲苯胺苯乙胺
I
Abstract
The synthesis, characterization and catalytic properties in hydrogenation of some
natural polymer-supported plexes were mainly investigated. Some natural
bio-polymer (such as wool, chitosan, chitin and carboxymethylcellulose) were chosen as
ligands. And the coordination with metal or metal ion of Pt, Pd were prepared. The
investigation of some the structure of catalyst were carried out with XPS and IR.
Firstly, we researched the catalytic activity of SiO 2-CMC-Pt on the benzene, toluene,
nitrobenzene et al that is one-substituted aromatics. Then, we used the catalyst to catalyze
hydrogenation of m-toluidine, o-toluidine and p-toluidine to 3-methylcyclohexylamine, 2-
methylcyclohexylamine and 4-methylcyclohexylamine respectively at room temperature
under 1 atm H2, when optimum Pt content in SiO 2-CMC-plex, reaction temperature
and solvent are selected. And we have also found that SiO 2-CMC-Pt could catalyze the
asymmetric hydrogenation of ( )-1-phenylethylamine to (s)-(+)-1-cyclohexylethylamine
in % product yield and % optical yield respectively. And we have researched the
hydrogenation of the bisphenol F by using SiO 2-CMC-Pt catalyst, the results are well.
Secondly, the hydrogenation nitrobenzene and benzaldehyde with SiO 2-CMC-Pd