Selective Production of Intermediate Compounds of Reaction In Series by Use of Catalytic Zeolite Membrane Reactor

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Zeolites are crystalline alumino-silicate, and widely used as catalysts and adsorbents. MFI-type zeolite has fine pores within its crystals, the diameter of which is almost the same as the molecular size of benzene. Hence, the zeolite shows high molecular-sieving effect. When the zeolite is succeeded to be prepare in the shape of membrane, the membrane can enable to realize new separation and simultaneous reaction and separation with high performance. The main objective of this project is to development of MFI-type zeolite catalytic membrane, and to apply it to high separation and simultaneous reaction and separation processes. We obtained the following results through this research work :In fiscal year of 2001 :(1) MFI-type catalytic membrane was succeeded to prepared without any pin-holes by a new method, well-mixed hydrothermal synthesis.(2) Hydrophilic zeolite membrane with high acid-proof was successively prepared by the liquid phase oxidation method. This membrane allows the permeation for only water.(3) We developed a new method, called "Catalytic Cracking of Silane (CCS) method", for controlling the pore diameter and the location of acid sites distribution of zeolite. When diethoxymethyl-silane was employed for the CCS method, the effective pore diameter was decreased in pores. On the other hand, tri-phenyl silane was used, the effective pore diameter was decreased only at pore months.In fiscal year of 2002 :The CCS method with tri-phenyl sliane was applied to contorol the distribution of active sites (acid sites) on the zeolite membranes, to prepared the membrane with acid sites only within pores. When the reaction of methanol was conducted by use of this treated membrane, useful olefins were produced at selectivity above 85% under the conditions of the conversion of methanol of around 0 to 70% and zero pressure drop between the permeate and the feed sides.