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Study on Cr-based Catalysts for Vapor-phase Fluorination to Synthesis CF4 and Preparation of β-AlF3 with High Surface Area

Author: JiaWenZhi
Tutor: LuoMengFei
School: Zhejiang Normal University
Course: Physical and chemical
Keywords: Cl / F exchange reaction Cr- based catalysts CF4 Lewis acid Carbon hard template A high specific surface area of the β-AlF3
CLC: O643.32
Type: Master's thesis
Year: 2011
Downloads: 33
Quote: 0
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Abstract


Due to the serious damage to the atmospheric ozone layer, chlorofluorocarbons (CFCs), international environmental organizations to develop Montreal Protocol to limit the use of ozone-depleting substances (ODS), chlorofluorocarbons (CFCs). CFCs elimination technology CFCs conversion and utilization or development of CFCs alternatives is a very meaningful work. CCl2F (CFC-12) has been widely used in household and industrial propellants, refrigerants, is destroying the ozone layer. How can tetrafluoromethane (CF4) transformed into a high value-added CCl2F2 one of the objectives of this study. C1 / F exchange reaction CCl2F2 transformed CF4 gas phase in the Cr-based catalyst CCl2F2 fluoride reaction to synthetic. The goal of our research is carried out a detailed study of Cr-based catalysts, catalyst phase structure and surface chromium species were characterized using a variety of characterization techniques. Catalytic C1 / F exchange reaction catalyst used in Cr/AlF3 A1F3 carrier has a great influence on the performance of the Cr-based catalyst; the A1F3 carrier wherein the high specific surface area is possible to improve the performance of the Cr-based catalyst; paper uses a novel carbon hard template prepared by a high specific surface area A1F3 A1F3 has more number of Lewis acid sites, the C1 / F exchange reaction has a strong catalytic activity; related to the characterization and materials prepared. The papers on the following three aspects to a series of work: 1, using deposition precipitation prepared a series of different calcination temperature CrOx-Y2O3 catalyst for the gas-phase the fluoride CCl2F2 synthesis CF4. Fluorination reaction CCl2F2 and CClF3 as the raw materials to participate comparative study, the researchers found that the process CCl2F2 two-step continuous fluoride from CCl2F2 into CClF3 occur relatively fast, however from CClF3 transformed for CF4 is the rate-determining step. Calcined at 600 ℃ CrOx-Y2O3 catalyst after the fluorination catalyst has a very good activity, the tetrafluoromethane the yield in the reaction is maintained at about 95% within 10 hours. Characterization results and found that the activity of the catalyst and catalyst Cr species and the Lewis acid sites related. 2, deposition of Cr2O3-AlF3 catalysts were prepared by different content of Cr203, used for the gas fluoride CCl2F2 synthesis of CF4 reaction. The experiment found that the activity of the catalyst The a Cr203 content was 61.2% Cr2O3-AlF3 best, 94% of the yield of CF4 at 400 ℃. Characterized by XRD and Raman spectroscopy showed that the presence of crystalline phases Cr203 and a-AlF3 catalyst. NH3-temperature programmed desorption and adsorption of pyridine infrared spectroscopy characterization of the catalyst surface and the presence of strong Lewis acidity. Cr2O3-AlF3 catalyst of Cr species and Lewis acids, respectively, as the active centers of the catalytic CC12F2 hydrofluorination reaction (reaction with HF) and disproportionation reactions. This shows that the Cr2O3-AlF3 catalyst is a dual-function catalyst of the fluorination and the disproportionation reaction. 3, through a novel carbonaceous hard template SYSTEM prepared by a high specific surface area of ??the β-AlF3-. Pores of carbon charged into the porous type of γ-A1203, and then formed by vapor-phase fluorination of carbon-containing AlF3-carbon templating agent is removed by burning method, to obtain a specific surface area of ??114 m2g-1 of β-AlF3-. Fluoride and carbon combustion temperature on the phase state of the sample preparation and the specific surface area of. A high specific surface area of ??the B-AIF3 for CCl2F2 Cl / F exchange reaction, and exhibits a high activity, which is attributed to a number of more Lewis acid centers.

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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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