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Application Of Functionalized Carbon Nanomaterials In The Catalytic Synthesis Of Propargylamines

Posted on:2015-03-29Degree:MasterType:Thesis
Country:ChinaCandidate:H X ChenFull Text:PDF
GTID:2181330422989621Subject:Chemistry
Abstract/Summary:PDF Full Text Request
Multi-component reactions have been one of the hot spots for researchers.However, how to complete the reaction efficiently is a key one. At presentpropargylamines compounds are a class of biologically active compounds and naturalproducts. Nowadays, synthesis of propargylamines compounds is mainly obtained bythe multi-component reaction. Yet so many problems still exists such as various kindsof raw materials, complexity of side reaction and low yield. In summary, contrasted tothe traditional methods, the paper made the following improvements to solve theseproblems: First, traditional method always involves homogeneous reaction in whichhomogeneous catalysts were difficult to separate with the product, and that led tosome residual metal ions in the product. So we designed green, efficient,environmentally friendly, recyclable heterogeneous catalysts, which not onlyovercome the drawbacks of homogeneous catalysts but also not reduce the reactivityof the catalyst. Second, conventional heating is employed in the traditional methods,which needed long reaction time, usually ranging from several hours to tens of hours.To solve this problem, microwave radiation is employed, which accelerated thereaction and greatly shorten the reaction time (usually tens of minutes). Third, organicsolvents are used in the traditional method frequently, which is not only a waste ofresources, but also not conducive to environmental protection. Our work introducedsolvent-free processing, which reduce not only costs but also pollution. Finally, thispaper is divided into the following chapters:The first chapter outlines the carbon nanomatierials, theirs functionalization, thedevelopment process of propargylamines compounds and synthetic methods, thecomparation between homogeneous and heterogeneous catalysts and their developments. Besides, common types of multi-component reactions, researchbackground and the main content are also introduced.The second chapter describes how to obtained GO-Cu(II). And it was characterizedby various means. Then series of A3-coupling reactions were carried out under thesolvent-free and microwave-assisted conditions and kinds of propargylamines wereobtained. Meanwhile reactions were amplified50times and the catalysts were after5recycles, the yield was still about80%.The third chapter introduces how to get magnetic metal complex and immobilizethe metal. And a variety of characterizations were conducted. Finally, series ofKA2-coupling reactions were carried out under the solvent-free andmicrowave-assisted conditions. Because the reaction was complex, it was recycledwhen it conducted4cycles with approaching80%yields.The fourth chapter describes that the polymer was obtained by nitroxide mediateradical polymerization, and then it conducted Diels-Alder reaction with carbonnanotubes. At last CuCl2salts were loaded on modified carbon nanotubes. It made aseries of corresponding characterization as well. Then series of three componentcoupling reactions were carried out under the solvent-free and microwave-assistedconditions. Meanwhile, reactions were also recycled, when it conducted6cycles withapproaching80%yields obtaining predetermined goal.The fifth chapter draws a conclusion for this research, and envisions the future ofthe work.
Keywords/Search Tags:functionalized graphene oxide, heterogeneous catalyst, propargylamines, carbon nanotubes, KA2-coupling reaction, A3-coupling reaction
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