Studies on Microporous Materials towards Green Chemical Catalysis

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We studied on the synthesis and tuning of preparation of new type of zeolites and functionalization of mesoporous materials in order to find microporous materials as catalysts for green chemical processes. Principal results in this work are as follows :1) New type of BEA zeolite containing lanthana and ceria (La-BEA and Ce-BEA) were synthesized and applied for the hydrocarbon conversion. The decrease in coke-formation by using these zeolites as catalysts resulted in the low deactivation during their catalysis.2) The synthesis of nano-sized BEA was synthesized by using TEAOH and cetyltrimethylammonium chloride as dual temperate in order to enhance the availability of channels of zeolites with particle size of 30-50 nm.3) Three dimensional MCM-68 zeolite with 12-10-10-MR channel system was synthesized and applied for the isopropylation of biphenyl (BP), resulting in the selective formation of 4,4'-diisopropylbiphenyl (4,4'-DIPB). This is due to the discrimination of 4,4'-DIPB from its other DIPB isomers by the restriction in channels.4) Multi-valent metal salts, such as FeCI_3 6H_2O, AICI_3 6H_2O, ZrOCl_2 6H_2O, were active for the esterification of fatty acid with fatty alcohol. The catalytic species are bore on the cationic cluster formed by the hydrolysis of multi-valent metal salt. The catalytic activity as improved by the loading of cluster cation on mesoporous silica. Multi-valent metal salts were also active for the esterification of lauric acid with glycerin. Monolaurin and dilaurin were obtained in presence of excess glycerin by using these salts.5) The t-butylation of phenol was examined over H-Y zeolite and Sc(OTf)_3 in supercritical CO_2 medium, resulting in the high yield of 2,4-di-t-butylphenol over H-Y zeolite and 2,4,6-tri-t-butylphenol over Sc(OTf)_3 supported on mesoporous silica. These high yields compared to those in vapor and liquid phases are due to low coke-formation in supercritical CO_2 medium.