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Synthesis And Catalytic Performance Of Rare Earth Metal-Organic Framework And PCN-224

Posted on:2021-04-05Degree:MasterType:Thesis
Country:ChinaCandidate:B H WuFull Text:PDF
GTID:2381330611953069Subject:Inorganic Chemistry
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Metal-organic framework materials?MOFs?are a type of network porous crystalline materials composed of metal ions and organic ligands.By virtue of its diversity of structure composition,MOFs can also predict the structure,control its own growth,and post synthetic modification,which has occupied a position in the field of chemistry and material chemistry.Due to its large surface area and adjustable pore size,MOFs have developed rapidly in the field of catalysis,and have been widely used in photocatalysis,electrocatalysis,and many heterogeneous catalysis directions.The one-pot tandem reaction and the CO2 coupling catalytic reaction at room temperature and pressure are both low-consumption and energy-saving reactions.It accords with contemporary chemistry research concept and has high research value and significance.This paper mainly explores the application of MOFs in different catalytic fields.It is divided into four chapters:Chapter 1:Firstly,the research background and development status of MOFs are discussed.It mainly introduces the tandem catalysis reaction and the carbon dioxide cycloaddition catalysis.Chapter 2:Three six-core rare earth cluster MOFs materials,Y-MOF-NH2,Dy-MOF-NH2,and Er-MOF-NH2 were synthesized and applied to the one-pot tandem reaction of catalytic Deacetalization--Knoevenagle.This type of complex is synthesized by solvothermal reaction of organic linear ligands with-NH2 and rare earth metal salts,and has high density Lewis acidic sites and Br?nsted basic sites and get good catalytic effect.Chapter 3:Investigated the cycloaddition reaction between propylene oxide and carbon dioxide catalyzed by PCN-224?Cu?,PCN-224?Zn?and PCN-224?Cu?Zn?at room temperature and 1 atm.This kind of complexes are introduced into the porphyrin ligands by post-synthesis with the introduction of a single metal Cu,a single metal Zn and a mixture of the both.In the catalytic cycloaddition reaction,the catalytic effect of PCN-224?Zn?was better than that of PCN-224?Cu?and PCN-224?Cu?Zn?.Chapter 4:Summarize the content of this article.In this paper,the organic ligands for the synthesis of MOFs are 2?-amino-1,1?:4?,1??-terphenyl-4,4??-dicarboxylic acid and tetrakis?4-carboxybenzene?porphyrin.The former formed six-core rare earth cluster MOFs with rare earth metals and used as a one-pot tandem Deacetalization-Knoevenagle reaction.Among them,the catalytic effect of Y-MOF-NH2 is particularly prominent,with the yield of the end product reaching 99.23%,and the catalytic yield can still be maintained at a high level after 5 cycle experiments.The latter is an experimental study on the effect of different doped metals on the carbon dioxide cycloaddition reaction.The order of catalytic yield was PCN-224?Zn?>PCN-224?Cu,Zn?>PCN-224?Cu?.The mixed metal MOF did not exhibit better catalytic performance than the single metal.
Keywords/Search Tags:Metal-Organic Frameworks, Porous-Organic Frameworks, tandem reaction, catalyst, one-pot, mixed metal
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