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Synthesis And Catalytic Properties Of Rare Earth Metal-Organic Frameworks

Posted on:2016-04-19Degree:MasterType:Thesis
Country:ChinaCandidate:Y X HuoFull Text:PDF
GTID:2191330473462392Subject:Chemical Engineering and Technology
Abstract/Summary:PDF Full Text Request
Metal organic skeleton materials (MOFs) is made by metal and organic ligand self-assemble to form a new type of material, with nanopores neat structure, larger specific surface area, entrance is larger, higher porosity and adjustable, and solid density is low and so on merits, in the field of gas separation and storage, catalysis, fluorescence field, magnetic field, sensors, liquid phase separation, drug delivery, membrane separation fields has been widely used. In particular, the using of MOFs as heterogeneous catalysts or as a carrier for the active catalytic species recently caused widespread concern, which has become a hot research question.The europium metal-organic framework (Eu-MOF) was synthesized using the rare earth metal yttrium as the metal ions and 1,3,5-trimesic acid (H3BTC) as organic ligand under hydrothermal conditions. The absorption desulphurization properties and the absorption desulphurization kinetics of Eu-MOF using the thiophene/n-octane as model oil were investigated. The adsorption desulphurization kinetics equation and the adsorption desulphurization isotherm of Eu-MOF were obtained. The results show that the Eu-MOF has excellent adsorption desulfurization ability under an optimum desulfurization conditions of the mmodel oil:madsorbent= 100:1 and 303K, The adsorption desulfurization rate and adsorption capacities reach 64.7% and 24.59 mgS/gEu-MOF after 4h, respectively. The adsorption process of thiophene was the quasi two level dynamic models.The yttrium metal-organic framework (Y-MOF) was synthesized using the rare earth metal yttrium as the metal ions and 1,3,5-trimesic acid (H3BTC) as organic ligand under hydrothermal conditions. The absorption desulphurization properties and the absorption desulphurization kinetics of Y-MOF using the thiophene/n-octane as model oil were investigated. The adsorption desulphurization kinetics equation and the adsorption desulphurization isotherm of Y-MOF were obtained. The results show that the Y-MOF has excellent adsorption desulfurization ability under an optimum desulfurization conditions of the mmodel oil:madsorbent= 100:1 and 303K. The adsorption desulfurization rate and adsorption capacities reach 80.7% and 30.7 mgS/gY-MOF, respectively. The adsorption process of thiophene was the quasi two level dynamic models. The adsorption kinetics equation was dqjdt= 0.007 (31.97-qt)2. When the liquid space velocity was from the range of 1.0 h-1 to 1.8 h-1, the capacity of adsorption removal thiophene was from 2.21% to 1.80%.Michael addition reaction of amines with a,β-unsaturated compounds was employed as a model reaction to test the catalytic activity of the MOFs. Experiment systematically investigated the reaction time, reaction temperature, amount of catalyst and the molar ratio of the substrate and the repeated use of the catalyst of the reaction, the results showed that the optimal reaction conditions, the reaction time is 4 h, reaction temperature is 80℃, two reactant content quality ratio of n (methyl acrylate):n (aniline)= 1:2, dosage of catalyst Y-MOF and the ratio of the reactant dosage of aniline for 1:10. aniline and methyl acrylate can be 88% high yield synthesis of β-amino ester. Y-MOF catalyst through the catalyst regeneration can be reused at least five times.
Keywords/Search Tags:metal-organic frameworks materials, rare earth metal, adsorption desulfurization, kinetics, thermodynamics, catalyst, Aza-Michael
PDF Full Text Request
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