畢業(yè)設(shè)計(jì)說明書中文摘要

伯醇類化合物的選擇性氧化反應(yīng)是有機(jī)化工領(lǐng)域中不可或缺的一部分，伴隨著綠色氧化技術(shù)的發(fā)展，對(duì)于清潔而廉價(jià)的催化劑的研究顯得尤為重要。在本論文中，我們采用氧氣/過氧化氫作為氧化劑，制備了兩種新型環(huán)?？苫厥盏拇呋瘎?，來實(shí)現(xiàn)醇的綠色高效選擇性催化氧化。

制備Au納米顆粒負(fù)載的金屬有機(jī)配位聚合物MOCP-Au。用苯甲醇作為底物，以氧氣為氧化劑，可以在不添加有機(jī)溶劑的條件下進(jìn)行醇的選擇性氧化反應(yīng)，整個(gè)反應(yīng)過程符合節(jié)能環(huán)保的要求。形態(tài)統(tǒng)一、大小相仿的Au納米顆粒在MOCP-Au中表現(xiàn)出高度的分散性，且具備優(yōu)異的催化能力。在該體系中，苯甲醇的轉(zhuǎn)化率約為54%，反應(yīng)的選擇性高達(dá)99%。

制備了一系列金屬有機(jī)配位聚合物（MOCP）負(fù)載的雜多酸（POM）催化劑MOCP-POMs。高度一致的大小和形態(tài)使得催化劑與底物之間的接觸變得容易，同時(shí)，MOCP確保了POM能被良好的包覆，而不會(huì)聚集成團(tuán)。以苯甲醇作為反應(yīng)底物，將MOCP-PW應(yīng)用于十六烷基三甲基溴化銨膠束溶液中的醇類選擇性氧化反應(yīng)，反應(yīng)3小時(shí)，反應(yīng)轉(zhuǎn)化率可達(dá)98%。

關(guān)鍵詞  金屬有機(jī)配位聚合物  伯醇  催化氧化  綠色

畢業(yè)設(shè)計(jì)說明書外文摘要

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  緒論 1

1.1  綠色氧化反應(yīng) 1

1.2  金屬有機(jī)配位聚合物 2

1.3  本文的選題意義及研究?jī)?nèi)容 4

2  MOCP-Au催化伯醇類化合物的氧化反應(yīng)研究 6

2.1  引言 6

2.2  實(shí)驗(yàn)部分 6

2.3  實(shí)驗(yàn)結(jié)果與討論 8

2.4  本章小結(jié) 15

3  MOCP-POMs催化伯醇類化合物的氧化反應(yīng)研究 17

3.1  引言 17

3.2  實(shí)驗(yàn)部分 17

3.3  實(shí)驗(yàn)結(jié)果與討論 19

3.4  本章小結(jié) 26

結(jié)論 28

致謝 30

參考文獻(xiàn) 31