摘要本论文基于天然卟啉的模型,如P450, VB12,通过修饰改性合成氯化血红素双丙酸羧基,合成了一系列锰金属次卟啉衍生物,并将其作为催化剂应用于苯乙烯的催化氧化中,考察其催化性能。论文包括以下几个方面主要内容:1. 绪论部分主要介绍了血红素的研究历史,综合阐述了细胞色素P450酶的研究现状和作用机理,并简单总结了模拟P450金属卟啉的催化研究和金属卟啉的催化应用领域,最后综述了苯乙烯催化氧化的工艺进展。
2. 实验部分主要介绍了本论文前期所合成的一系列化合物的合成方法和表征结果。本论文是以氯化血红素为原料,首先合成了次卟啉,然后在次卟啉13, 17-位双丙酸基上进行改性修饰,合成了一系列化合物,将合成的这些次卟啉衍生物配体与金属锰离子络合,并将次卟啉衍生物锰金属络合物用于催化空气氧化苯乙烯的反应。
3. 第三部分为结论部分。该部分总结了合成中出现的问题和反应条件优化结果以及实验后处理方法。10253
关键词: 氯化血红素,次卟啉,氧化苯乙烯,金属卟啉
毕业设计说明书(论文)外文摘要
Title Synthesis and design of intramolecular six-coordinate manganese deuteroporphyrins: study of their catalytic activities in oxidation of styrene
Abstract
The thesis based on the model of the natural porphyrins,such as P450, VB12, a series of Mn-deteroporphyrin derivatives introduced in the heme-propionate side chains have been synthesized, and they’ve been employed into the oxidation of styrene as catalyst, which showed different catalytic activity.
The contents of this thesis are presented as follows:
1. The first chapter mainly introduced the history of heme, and elaborated the current situation and mechanism of cytochrome P450 comprehensively. Research on the catalytic oxidation to mimic cytochrome P450 and the catalytic applications of the metalporphyrin has also been carried out. Meanwhile, the technological progress of the catalytic oxidation of styrene has been summarized.
2. The second chapter is the section of experiment. In this chapter, a series of Mn-deuteroporphyrin derivatives have been synthesized and their constructures were proved by MS, 1H NMR, IR and UV-Vis, respectively. In this paper, deuteroporphyrin was synthesized from hemin, and modified the propionate side chains at 13, 17-sites of deuteroporphyrin synthesizing a series of compound, then, these deuteroporphyrin derivatives complexed with manganese ion. At last, these Mn-deuteroporphyrin were used to the process of the oxidation reaction of styrene.
3. The third chapter is the conclusion section. This chapter mainly discussed troubles emeraged in the experiment, optimization of reaction conditions and aftertreatment of the reactions.
Keywords: Hemin, Deuteroporphyrin, oxidation of styrene, metalloporphyrin
目 录
1 引言 1
1.1 细胞色素P450 1
1.2 血红素的概况 2
1.3 烟酸及其化合物性质 4
1.4 金属卟啉绿色催化领域的应用 4
1.5 本课题研究的目的和意义 6
1.6 本课题研究的内容 7
2 实验部分 9
2.1 主要仪器与试剂 9
2.2 合成部分 10
3 催化氧化 18
3.1 催化甲苯氧化反应工艺流程 18
3.2 金属次卟啉衍生物催化空气氧化苯乙烯反应 18
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