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Preparation and Application of C-MCM-22 Composite Zeolites
Author: ShenWeiBin
Tutor: FangZuoWen
School: Shantou University
Course: Industrial Catalysis
Keywords: hard template zeolites MCM-22 composite zeolites
CLC: TB383.4
Type: Master's thesis
Year: 2010
Downloads: 58
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Abstract
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For hard templates have good stability and spatial confinement, the hard template method is a very important method for synthesizing composite materials and the zeolites with specific size and morphology.In this paper, firstly, SiO2 colloidal crystal and MCM-22 zeolites were synthesized. Secondly, macroporous carbon zeolites were prepared using SiO2 colloidal crystal as hard template. Thirdly, granular C-MCM-22 composite zeolites were prepared using carbon zeolites as hard template, and monodisperse C-MCM-22 composite zeolites were preapared using MCM-22 zeolites as hard template. All the materials were characterized by XRD、SEM, and so on. At last, composite catalysts were used in the synthesizing of dimethyl carbonate (DMC)by gas-phase oxidative carbonylation of co-feeding methanol with dimethyl ether. The results aresummarized as follows:1. Monodisperse SiO2 microspheres were prepared by sol-gel method. Then, SiO2 colloidal crystal was synthesized by solvent evaporation method. Finally, macroporous carbon zeolites were prepared using SiO2 colloidal crystal as hard template. The characterized results indicated that the monodispersed SiO2 microspheres with diameter about 200nm had regular spherical shape, and the SiO2 colloidal crystal was ordered. The macroporous carbon zeolites have copied the ordered structure of SiO2 colloidal crystal. Its bore diameter was as large as the bore diameter of SiO2 microspheres.2. Using hexamethyleneimine(HMI) as soft template, and the macroporous carbon zeolites as hard template, granular C-MCM-22 composite zeolites were prepared by static hydrothermal crystallization. The characterized results of SEM and XRD showed that the lamellar MCM-22 zeolite had grown inside the macroporous carbon zeolites. The shape of this MCM-22 zeolites were different from the common MCM-22 zeolites. Its diameter ranges from 50 nm to 200 nm.3. Monodisperse MCM-22 zeolites were prepared by static hydrothermal crystallization method. Then, the monodisperse C-MCM-22 composite zeolites were prepared by static hydrothermal crystallization method, using sucrose as carbon source and MCM-22 zeolites as hard template. The characterized results proved that the MCM-22 zeolites was thin pancake-shaped, and the monodisperse C-MCM-22 composite zeolites, wrapped by a layer of carbon, was thin pancake-shaped too. After the MCM-22 zeolites were moved away from C-MCM-22 by HF, the zeolites are pancake-shaped with hollow.4. The space time yield of DMC over the mixed catalysts of Cu-Pd-TBAB/AC and Cu-Pd/MCM-22 could be improved effectively after the dimethyl ether was introduced to the gas-phase oxidative carbonylation of methanol. However, the catalytic performance in the co-feeding system over the bi-functional catalysts, which were prepared by using the monodisperse C-MCM-22 composite zeolites or granular C-MCM-22 composite zeolites as support, was decreased.
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