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摘 要：目前，环境问题已成为国际社会关注的焦点之一。因此，相关的绿色化学应运而生，与此相关的各种绿色化学合成方法、工艺倍受人们的关注。碳氢化合物的氧化是有机合成和工业使用的重要方法，氧化过程百分之九十是催化氧化过程。目前使用的催化体系主要有两种：一种是传统的化学催化，一种是自然界酶催化。化学催化与酶催化相比，不仅反应条件剧烈，而且有很多副反应，从而使产物的产率和选择性比较低，同时造成很高的能源消耗和资源浪费，还存在对生产设备的腐蚀和环境污染等问题。
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氧化反应是精细化学品生产中最主要的反应之一，烯烃的氧化反应产物是很多有机合成的中间体。氧化烯烃所使用的氧化剂主要有双氧水、叔丁基过氧化氢、间氯过苯甲酸等，这些氧化剂或多或少存在一定的弊端。目前的研究主要集中在新的绿色催化氧化体系的探索。4214
本论文探讨新型仿生水溶性催化剂制备及其在烯烃的环氧化和烯丙位氧化反应的应用。以氧气为氧化剂探索合理的催化氧化反应条件。
关键词：酞菁；烯烃；烯丙位氧化；环氧化
The Research on the Preparation, Characterization and Catalytic Properties of Tetracarboxylic Phthalocyanine
Abstract：At present, environmental problems have become the focus of attention of the international community one. Therefore, related to the green chemistry arises at the historic moment, and the related all sorts of green chemical synthesis method; process much the attention of people. The oxidation of hydrocarbons is organic synthesis and industrial use of important method, oxidation process ninety percent is catalytic oxidation process currently used catalytic system mainly has two kinds: one kind is the traditional chemical catalysis, enzyme catalysis is a kind of nature. Compared with the chemical catalytic enzyme catalysis, not only reaction conditions severe, and there are many side effects, so that the product yield and selectivity is lower, at the same time cause high energy consumption and large waste of resources, but also the existence of production equipment corrosion and environment pollution.
Oxidation reaction is one of the main reactions in fine chemicals production, the product of oxidation of olefins reaction is intermediates in a lot of organic synthesis. Oxidants are mainly used by oxidation of olefins, tertiary butyl peroxide hydrogen peroxide, and chlorine between benzoic acid and so on, these antioxidants are more or less having certain drawbacks. The current research mainly focuse on the exploration of new green catalytic oxidation system.
This paper explores new bionic water-soluble catalyst preparation and applications in the olefin epoxidation and allylic oxidation reaction. We explore reasonable catalytic oxidation reaction condition with oxygen as oxidant.
Key Words: phthalocyanine; olefin; allylic oxidation; epoxidation
目录
1 课题背景..1
2 文献综述..3
2.1 仿生催化研究概况3
2.2 细胞色素P-450催化底物机理..4
2.3 酞菁研究的基本现状.6
2.4 酞菁的基本结构与基本性质.6
2.5 酞菁的种类7
2.6 酞菁的合成8
2.6.1 单核酞菁的合成.8
2.6.2 两性酞菁的合成.8
2.6.3 直接取代法..9
2.6.4 插入配位法..9
2.7 烯烃环氧化反应研究进展9
2.7.1 卤醇法..10
2.7.2 双氧水氧化.10
2.7.3 过酸氧化11
2.7.4 氧气氧化12
3 金属酞菁合成以及对烯烃催化氧化反应研究.13
3.1 实验试剂及仪器.13
3.2 2,9,16,23-四取代酞菁钴催化剂的制备..14
3.2.1 2,9,16,23-四酰胺基酞菁钴催化剂的制备14
3.2.2 2,9,16,23-四羧基酞菁钴催化剂的制备..14
3.2.3 2,9,16,23-四取代酞菁钴催化剂的表征..14
3.3 2,9,16,23-四羧基酞菁钴对烯烃环氧化的研究..15