【作者】 王欣；

【导师】 杨济活；

【作者基本信息】 华中科技大学 ， 高分子化学与物理， 2004， 硕士

【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SiO2-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85.7%的产率和92.7%的光学收率。其次,我们又合成了SiO2-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SiO2-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。更多还原

【Abstract】 The synthesis, characterization and catalytic properties in hydrogenation of some natural polymer-supported metal complexes 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 SiO2-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 SiO2-CMC-Pt complex, reaction temperature and solvent are selected. And we have also found that SiO2-CMC-Pt could catalyze the asymmetric hydrogenation of (±)-1-phenylethylamine to (s)-(+)-1-cyclohexylethylamine in 85.7% product yield and 92.7% optical yield respectively. And we have researched the hydrogenation of the bisphenol F by using SiO2-CMC-Pt catalyst, the results are well.Secondly, the hydrogenation nitrobenzene and benzaldehyde with SiO2-CMC-Pd were investigated as well, and some satisfactory results were obtained.Finally, the catalytic activity of wool-Pd had also been researched. The results showed that the activity of catalyst was very good.From the above results, we found that the coordination of natural bio-polymer, especially carboxymethylcellulose, with Pt, Pd et al has satisfactory catalytic activity in the hydrogenation of aromatics. Compared with other catalyst, the preparation methods of natural bio-polymer-metal complex catalyst are more easier and it has higher selectivity, activity and stability. So, study of these catalysts is very valuable and we believe it will have a splendid future.更多还原