聚合物催化伯醇类化合物的绿色氧化研究.doc

毕业设计说明书中文摘要

伯醇类化合物的选择性氧化反应是有机化工领域中不可或缺的一部分，伴随着绿色氧化技术的发展，对于清洁而廉价的催化剂的研究显得尤为重要。在本论文中，我们采用氧气/过氧化氢作为氧化剂，制备了两种新型环保可回收的催化剂，来实现醇的绿色高效选择性催化氧化。

制备Au纳米颗粒负载的金属有机配位聚合物MOCP-Au。用苯甲醇作为底物，以氧气为氧化剂，可以在不添加有机溶剂的条件下进行醇的选择性氧化反应，整个反应过程符合节能环保的要求。形态统一、大小相仿的Au纳米颗粒在MOCP-Au中表现出高度的分散性，且具备优异的催化能力。在该体系中，苯甲醇的转化率约为54%，反应的选择性高达99%。

制备了一系列金属有机配位聚合物（MOCP）负载的杂多酸（POM）催化剂MOCP-POMs。高度一致的大小和形态使得催化剂与底物之间的接触变得容易，同时，MOCP确保了POM能被良好的包覆，而不会聚集成团。以苯甲醇作为反应底物，将MOCP-PW应用于十六烷基三甲基溴化铵胶束溶液中的醇类选择性氧化反应，反应3小时，反应转化率可达98%。

关键词  金属有机配位聚合物  伯醇  催化氧化  绿色

毕业设计说明书外文摘要

Title    Research on Green Selective Oxidation of Alcohol Catalyzed 

          by Polymer                                         

Abstract

As one of the most important reactions in the field of organic synthesis, selective oxidation of alcohols plays an irreplaceable role in many industrial processes. Due to the development of green chemistry, it is so urgent to research on relatively cleaner and more inexpensive catalysts. In this thesis, two types of new eco-friendly recyclable catalysts, respectively with O2 and H2O2 as oxidant, were designed to realize efficient green selective oxidation of alcohol.

A metal-organic coordination polymer encapsulated gold nanoparticles noted as MOCP-Au was developed. In order to simplify processes and avoid pollution, the reactions were carried out in solvent–free condition, using benzyl alcohol as substrate and O2 as oxidant. The entire reaction process was green and eco-friendly. In these experiments, it was observed that the catalysts with uniform gold nanoparticles were easy to disperse; meanwhile, they also reflected fine activity. In this catalytic system, the conversion reached 33% and the selectivity was 98%.

A series of polyoxometalate (POM)-based metal-organic coordination polymers (MOCP) were synthesized and used in selective oxidation of alcohols. The catalysts with uniform size and morphology were easy accessed between substrates and catalysts. At the same time, MOCP ensured that POM was encapsulated, which could dramatically prevent the assembly of catalysts. Under CTAB aqueous solution as solvent, MOCP-PW as model catalyst, the conversion of benzyl alcohol achieved 98% after 3 hours.

Keywords  Metal-Organic Coordination Polymers，Alcohol，Catalytic Oxidation，Green

 

目   次

1  绪论 1

1.1  绿色氧化反应 1

1.2  金属有机配位聚合物 2

1.3  本文的选题意义及研究内容 4

2  MOCP-Au催化伯醇类化合物的氧化反应研究 6

2.1  引言 6

2.2  实验部分 6

2.3  实验结果与讨论 8

2.4  本章小结 15

3  MOCP-POMs催化伯醇类化合物的氧化反应研究 17

3.1  引言 17

3.2  实验部分 17

3.3  实验结果与讨论 19

3.4  本章小结 26

结论 28

致谢 30

参考文献 31