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The Study on Application of Metal-organic Frameworks MOF-5、MIL-120 and NCU-3 in Hydrogenation and Hydroxylation Reactions

Author: JianLiJuan
Tutor: ZhangNing；ChenChao
School: Nanchang University
Course: Industrial Catalysis
Keywords: Metal organic framework compounds Thermal stability Coordinatively unsaturated Cu (Ⅱ) Benzene hydrogenation Phenol hydroxylation Catalytic
CLC: O643.32
Type: Master's thesis
Year: 2011
Downloads: 444
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Abstract


MOFs compound (Metal-organic frameworks, MOFs) are a class of metal ions and organic ligand is formed by self-assembly process with a certain periodicity porous network structure of the new functional materials. Because in the gas storage, catalysis, sensing, and separation and purification of the potential application of great interest due to the researchers. Particularly its specific pore structure and large specific surface area, while introduced in the design functionalized produce metal ion and the ligand catalytic sites and other properties, making it the application of the catalyst are of great concern. Contents of this thesis is the choice of a certain thermal stability and hydrogen adsorption capacity of the metal organic framework compound MOF-5, MIL-120 used as a carrier gas-solid phase reaction of benzene hydrogenation will also contain unsaturated ligand metal ions metal organic framework compounds NCU-3 for liquid phenol hydroxylation reaction, investigated the catalytic effect. 1 The first part of the selection of two thermal stability with a metal-organic framework compound MOF-5, MIL-120 for the Ni-based catalyst carrier prepared by impregnation Ni catalyst, for the hydrogenation of benzene, the investigated its hydrogenation catalytic activity. The experimental results showed that: two novel catalyst activity are better than Ni/Al2O3 catalysts by XRD, H2-TPR, H2-TPD characterization methods such as catalytic activity explores the reasons for differences. (2) The second part describes a layered structure having a 2D MOFs compound [Cu2 (BPTC) (Im) 4 (H2O) (DMF)] n (H4BPTC = 3,3 ', 4,4' - biphenyl tetracarboxylic acid, Im = imidazole) (NCU-3) activation and its phenol hydroxylation reaction in the catalytic performance. Since NCU-3 unsaturated ligand Cu ions, with an acceptable guest molecules reactive sites can be applied to the catalytic hydroxylation of phenol. During the experiment, we investigated the solvent, temperature, amount of catalyst, time and other factors on the catalytic performance. Experimental results show that, NCU-3 catalytic phenol hydroxylation optimal reaction conditions: ethanol and water (4:1) mixture as the solvent system, the reaction temperature is 40 ℃, 4h, two phenol yield and selectivity the highest, where a yield of 13% of catechol, hydroquinone, a yield of 11%. And Cu (Ⅱ) ((Cu (OAc) 2) to make the catalytic activity as compared, NCU-3 showed a better selectivity diphenols (94%). Therefore, it can be inferred NCU-3 with the unsaturated Bit of Cu (Ⅱ) coordination environment and the catalytic hydroxylation of phenol has played a positive role, combined with the experimental data and the literature, we give the general process of the reaction.

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CLC: > Mathematical sciences and chemical > Chemistry > Physical Chemistry ( theoretical chemistry ),chemical physics > Chemical kinetics,catalysis > Catalytic > Catalytic reaction
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