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Hexanuclear Rare-earth Cluster-organic Framework For The Catalytic CO2 Conveision

Posted on:2020-05-04Degree:MasterType:Thesis
Country:ChinaCandidate:Z Y ChenFull Text:PDF
GTID:2381330578950994Subject:Inorganic Chemistry
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Metal-organic framework materials?MOFs?are another important new type of porous materials in addition to zeolites and activated carbon.Due to its high porosity and low density,regular and adjustable pore size,even the diverse topologies,it is widely used in sensing,gas storage,adsorption separation,drug delivery and catalysis.MOFs have been widely used as heterogeneous catalysts in the field of catalysis in recent years.Among them,the rare-earth?cluster?MOFs?RE-MOFs?exhibit the certain Lewis acid sites.Therefore,it is gradually applied to the filed of catalysis.Chemically immobilized CO2 can be converted into chemicals or fuels,which is an effective and economical method that attracts more and more people's attention.This article is divided into four chapters:In the first chapter,we mainly introduces the research background,development of MOFs,and the application in the field of catalysis.Then we introduces the progress of RE-MOFs in catalysis,especially for the catalytic CO2 conveision.In the second chapter,three series of RE-MOFs incorporating and linear ligand2'-amino-1,1':4',1"-terphenyl-4,4"-dicarboxylic acid?H2tpdc-NH2?,were synthesized by traditional solvothermal:[?CH3?2NH2]2[Y6??3-OH?8?H2tpdc-NH2?6]·?solv?x?Y-MOF-NH2?[?CH3?2NH2]2[Dy6??3-OH?8?H2tpdc-NH2?6]·?solv?x?Dy-MOF-NH2?[?CH3?2NH2]2[Er6??3-OH?8?H2tpdc-NH2?6]·?solv?x?Er-MOF-NH2?These three complexes exhibited the three-dimensional?3 D?topology frameworks,characterized the structure and analyzed the properties of these complexes.Due to the presence of Lewis acidic sites,it was applied to the cycloaddition reaction of CO2 with epoxides under mild condition,and showed good catalytic effect.In the third chapter,we used 2'-methyl-1,1':4',1"-terphenyl-4,4"-dicarboxylic acid?H2tpdc-CH3?and 2',5'-dimethyl-1,1'4',1"-terphenyl-4,4"-dicarboxylic acid?H2tpdc-2?CH3??and Yttrium nitrate by solvothermal reactions to synthesize the two coordination polymer:[?CH3?2NH2]2[Y6??3-OH?8?H2tpdc-CH3?6]·?solv?x?Y-MOF-CH3?[?CH3?2NH2]2[Y6??3-OH?8(H2tpdc-2?CH3?6]·?solv?x?Y-MOF-2?CH3??The two complexes were characterized by a series of characterizations.Such as Powder X-Ray Diffraction?PXRD??Fourier Transform Infrared Spectrometry Spectroscopy?FT-IR??Thermal Gravimetric?TG?and Pyridine Adsorption Fourier-transform Infrared?Py-IR?.Because of the existence of Lewis and Br?nsted acid sites,they were used to catalyze the CO2 cycloaddition reaction under mild condition.In the fourth chapter,we have summarized the structure and properties of the five coordination polymers above.Due to the presence of acidic sites,these MOFs materials are used to catalyze the CO2 cycloaddition reaction under mild condition,and the catalytic effects were obviously.In addition,the influence to the structure of the MOFs on the catalytic effect also was discussed at last.
Keywords/Search Tags:Metal-organic frameworks, Rare earth clusters, Catalysis, mild condition, Cycloaddition of CO2 and epoxides
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