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The Construction Of High-performance Metal Catalytic Materials And Their Environment-friendly Catalytic Performance

Posted on:2011-06-07Degree:MasterType:Thesis
Country:ChinaCandidate:Z H ZhuFull Text:PDF
GTID:2191360302492132Subject:Physical chemistry
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At present, the energy economy has become one of the points in the global development strategy. In the chemical industry whether or not has the ability to achieve this strategy is the most important among. In the chemical industry process, an important step is the catalyst, which a large extent determine the level of production technology and the feasibility of the value. At the same time, the catalyst does not minimize the weight of itself in the course of the reaction, which has the ability to improve the rate of chemical reaction and create the higher social worth. Recently, catalysts have been developed to a nano-level, its unique structure has aroused wide interest researches. The use of nano-structured catalyst, consider from the synthetic, as well as the energy economy. On the on hand, solving the problem of resource waste and pollution which made in the process of synthesized catalysts; on the other hand, solving the defeat of traditional way. In a word, the aim is to enhance the utilization of resource and improve the catalytic activities.In this paper, the energy economy is the center principle. Using the MIL-101as the carrier which has the order microporous-mesoporous and the larger surface area, then composed the Pd/MIL-101catalyst, in order to improve dispersedly of activity centre Pd. Afterward, applied catalysts to Sonogashira reaction,Heck reaction and synthesized the indoles; meanwhile, according to the vesicle-assisted template and chemical reduction method, synthesized the hollow structure Pd/M(M=Co, Fe, Ni, Cu, Zn) catalyst, especially, Pd/Co, Pd/Fe, their activity were measured by the coupling and hydrogen reaction; at the same tome, prepared the uniform size of Co-B and hollow Ni/Co-B amorphouse alloy catalyst, which was applied to the n-butyraldehyde (EHA)and octenal(2-EHA) hydrogen reaction in liquid-phase. Moreover, the character of catalysts were analyzed by XRD, BET, FESEM, TEM, H2-TPD, DSC, ICP and so on.1. Catalyst preparation1) Synthesized of Pd/MIL-101 catalyst: using H2 reduce the Pd(acac)2 was in the MIL-101, and check its character in load weight as well as the carrier. 2) Synthesized of hollow Pd/M (M=Co, Fe, Ni, Cu, Zn) catalysts: with the [PdX4]2- becoming to the vesicle framework, and participated into the other metals M, in end, the hollow Pd/M were prepared by the chemical reduction of NaBH4.3) Synthesized of the uniform size Co-B and hollow Ni/Co-B catalysts: placing the CoCl2 solution into the Bu4PBr solution, and KCl was not added until the solution was in super-saturation, the KBH4 reduced the saturation solution.2. Activity testAccording to the coupling reaction ,such as Sonogashira,Heck,Ullmann reaction and so on, and the n-butyraldehyde (EHA)and octenal(2-EHA) liquid hydrogenation, estimated the activities of catalysts. In coupling reaction, in a certain amount of round-botton, joined the solvent, substrate, catalyst and others; in the hydrogenation, in an autoclave, joined the solvent ethanol, reagent, catalyst and with the 1.0MPa of hydrogen pressure。The result was checked by the GC-MS,HNMR,GC and others. The result displayed as followed: 1) In Sonogashira coupling reaction, the material MIL-101 showed the higher activity and selectivity than Si material of MCM-41, SBA-15 and carbon; 2) With the vesicle-assistant template and chemical reduction, synthesized the hollow Pd/Co, Pd/Fe catalysts, which had much better reaction activity and yield than regular and the single hollow Pd catalyst; 3) Preparation of the uniform size Co-B and hollow Ni/Co-B amorphouse alloy catalysts, in the n-butyraldehyde (EHA)and octenal(2-EHA) liquid hydrogenation, they all appeared better result than regular Co-B,Ni/Co-B, which also proved that amorphouse alloy catalyst of special morphology structure is more promising in future.
Keywords/Search Tags:catalyst, MIL-101, Pd/M, Co-B, Sonogashira reaction, Heck reaction, indols, n-butyraldehyde (EHA), octenal(2-EHA), hydrogenation
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