【作者】 郑振华；

【导师】 万家义；

【作者基本信息】 四川大学 ， 物理化学， 2003， 硕士

【摘要】 随着催化剂生产工艺的迅猛发展，多相催化均相化及均相催化多相化的趋势日益明显。本文试图构造一种兼具两者优点的绿色催化体系，以期达到均相和多相催化剂协同作用、取长补短、对环境友好的目的。 制备了系列Cu-Ce/ZSM-5催化剂，进行了TPR、XRD及IR表征。考察了铈含量、不同硅铝比、不同铈源对催化剂还原性能的影响。 合成了系列过渡金属Schiff碱1：1及2：1型配合物，对其结构经摩尔电导、磁化率、DTA、SEM、UV、IR等确证。结果表明，制备方法的不同对配合物结构影响甚大；配合物中有水参与配位；配合物中有分子内氢键形成，这些均影响着配合物的生物活性。研究了在均相体系中，以所合成的Schiff碱Co(Ⅱ)配合物为模拟氧载体，考察了这一催化体系在以空气为氧源温和条件下催化异丙苯氧化反应。通过反应温度、催化剂浓度、搅拌速率、添加助剂、反应时间、不同催化剂等因素对氧化反应的影响，得到催化剂最佳工作条件。 研究了在水/有机两相催化剂体系中，引入相转移催化剂TBAB，与水溶性Schiff碱Co(Ⅱ)配合物共同作为异丙苯氧化反应的催化剂。考察了这一催化体系以空气为氧源温和条件下催化异丙苯氧化反应。结果表明，ω(CHP)可达26％，符合工业生产的要求。而且这一催化体系兼具均相催化和多相催化的优点，具有反应条件温和、反应速度快、催化剂易从产物中分离、易回收等优点，因而具有工业应用价值。更多还原

【Abstract】 With the rapid progress of catalysts preparation technology, the trends of the homogenization of heterogenous catalysis and the heterogenization of homogeneous catalysis have been obvious more and more. The writer tried to find a kind of green catalysis system ,which possesses the advantages both of them, to meet the demands of commercial application.A serious of catalysts Cu-Ce/ZSM-5 have been prepared and characterized by TPR, XRD and IR. The results show that the cerium content, the cerium source and the radio of silica to aluminum oxide of zeolite have influenced the reduction properties of catalysts.A serious of transition-metal complexes of Schiff base have been synthesized. The structures were characterized by DTA, SEM, UV, IR, molar conductances and magnetic moments. The results demonstrate that synthesis methods effect much on the structure of complexes; water is coordinated to metal; there the intramolecular hydrogen bond is formed, which have importance to the bioactivity. The catalytic properties of Schiff base cobalt(II) complexes in the oxidation of cumene in homogenous system have been studied and obtained the best reaction conditions.The phase transfer catalyst TBAB has been used in the water/organic biphase system. The oxidation of cumene catalyzed by the catalyst system with air as oxidant at amibient pressure and relatively lower temperature has been studied. The results show that (CHP) is 26%, which meets the demand of industrial application. The new system is characterized by wilder reaction, faster reactionspeed and the easy process of the separation of catalysts and feasibility of their reuse, which takes on the potential application in industry.更多还原