The inertisation of the zeolites ZSM-5, mordenite and beta by chemical vapour deposition using tetraethoxysilane

dc.contributor.advisorO'Connor, Cyril
dc.contributor.advisorMöller, Klaus
dc.contributor.authorWeber, Reinier Willem
dc.contributor.authorWeber, Reinier Willem
dc.date.accessioned2017-01-30T08:00:42Z
dc.date.available2017-01-30T08:00:42Z
dc.date.issued1998
dc.date.updated2016-12-06T09:04:29Z
dc.description.abstractThe structural characteristic of greatest interest for catalysis in zeolites is the channel system, because these catalysts may display shape selective properties if the reactions take place within the channel system. However, the external surface of zeolites is accessible to all molecules and behaves in a non-shape selective manner. Coke formation on the external surface of zeolites may prevent access to the channel system of the zeolite due to pore blocking. It would thus be of great benefit to study the effects of inertising the external acidity of zeolites, thereby enhancing the shape selective properties of these catalysts, and possibly also to reduce coke formation at the entrances to the pores. Given the industrial importance of ZSM-5, this is a particularly good zeolite to study in this regard. Chemical vapour deposition (CVD) and chemical liquid deposition (CLD) methods have shown great promise in inertising the external surface acidity of zeolites and thus increasing their selectivity for various reactions. The external surface acidity can be inertised by a thin layer of silica coating the external surfaces of the zeolites. The silica layer can also narrow the pore openings uniformly, thus increasing the shape selective properties of the zeolites even more. By implication, coating ZSM-5 in a shell of iso-structural Silicalite-1 may provide an inert layer around the ZSM-5 crystals, without necessarily altering the pore opening size. In this study, the following methods have been used to inertise the external surface acidity of ZSM-5, Mordenite and Beta: (i) Chemical vapour deposition - Tetraethoxysilane (TEOS) was contacted with the catalyst using a vapour phase flow system and static vacuum system. The effects of deposition temperature and time were varied in order to vary the amount of TEOS deposited on the samples. The effect of the decomposition species formed during TEOS deposition on the complete inertisation of the external surface acidity was investigated. (ii) Chemical liquid deposition Pure tetraethoxysilane (TEOS) or tetraethoxysilane diluted in water, ethanol or n-hexane was contacted with the catalyst at ambient temperatures. The effect on the inertisation of the external surface acidity in the presence of diluents, similar in nature to typical decomposition products formed at certain different temperatures, was studied. (iii) Coating with Silicalite shells - Parent ZSM-5 seed crystals were immersed into a Silicalite-1 synthesis mixture in order to obtain an iso-structural coating. The seed crystals used for modification were (a) the assynthesized material, (b) detemplated but not ion-exchanged parent crystals (Na-form), and (c) detemplated and ion-exchanged parent crystals (NH4-form). The primary objective of these studies was to determine how. complete inertisation of the external surface acidity could be achieved. By modifying samples under different conditions as outlined above, information was obtained on the uniformity of the coating of samples modified in each of the different systems. ZSM-5, Mordenite and Beta samples modified using similar CVD and CLD modification conditions were compared. Post-modification treatment was employed to determine whether the silica layer deposited during CVD treatment was irreversibly attached to the external surface of the samples.
dc.identifier.apacitationWeber, R. W., & Weber, R. W. (1998). <i>The inertisation of the zeolites ZSM-5, mordenite and beta by chemical vapour deposition using tetraethoxysilane</i>. (Thesis). University of Cape Town ,Faculty of Engineering & the Built Environment ,Department of Chemical Engineering. Retrieved from http://hdl.handle.net/11427/23695en_ZA
dc.identifier.chicagocitationWeber, Reinier Willem, and Reinier Willem Weber. <i>"The inertisation of the zeolites ZSM-5, mordenite and beta by chemical vapour deposition using tetraethoxysilane."</i> Thesis., University of Cape Town ,Faculty of Engineering & the Built Environment ,Department of Chemical Engineering, 1998. http://hdl.handle.net/11427/23695en_ZA
dc.identifier.citationWeber, R., Weber, R. 1998. The inertisation of the zeolites ZSM-5, mordenite and beta by chemical vapour deposition using tetraethoxysilane. University of Cape Town.en_ZA
dc.identifier.ris TY - Thesis / Dissertation AU - Weber, Reinier Willem AU - Weber, Reinier Willem AB - The structural characteristic of greatest interest for catalysis in zeolites is the channel system, because these catalysts may display shape selective properties if the reactions take place within the channel system. However, the external surface of zeolites is accessible to all molecules and behaves in a non-shape selective manner. Coke formation on the external surface of zeolites may prevent access to the channel system of the zeolite due to pore blocking. It would thus be of great benefit to study the effects of inertising the external acidity of zeolites, thereby enhancing the shape selective properties of these catalysts, and possibly also to reduce coke formation at the entrances to the pores. Given the industrial importance of ZSM-5, this is a particularly good zeolite to study in this regard. Chemical vapour deposition (CVD) and chemical liquid deposition (CLD) methods have shown great promise in inertising the external surface acidity of zeolites and thus increasing their selectivity for various reactions. The external surface acidity can be inertised by a thin layer of silica coating the external surfaces of the zeolites. The silica layer can also narrow the pore openings uniformly, thus increasing the shape selective properties of the zeolites even more. By implication, coating ZSM-5 in a shell of iso-structural Silicalite-1 may provide an inert layer around the ZSM-5 crystals, without necessarily altering the pore opening size. In this study, the following methods have been used to inertise the external surface acidity of ZSM-5, Mordenite and Beta: (i) Chemical vapour deposition - Tetraethoxysilane (TEOS) was contacted with the catalyst using a vapour phase flow system and static vacuum system. The effects of deposition temperature and time were varied in order to vary the amount of TEOS deposited on the samples. The effect of the decomposition species formed during TEOS deposition on the complete inertisation of the external surface acidity was investigated. (ii) Chemical liquid deposition Pure tetraethoxysilane (TEOS) or tetraethoxysilane diluted in water, ethanol or n-hexane was contacted with the catalyst at ambient temperatures. The effect on the inertisation of the external surface acidity in the presence of diluents, similar in nature to typical decomposition products formed at certain different temperatures, was studied. (iii) Coating with Silicalite shells - Parent ZSM-5 seed crystals were immersed into a Silicalite-1 synthesis mixture in order to obtain an iso-structural coating. The seed crystals used for modification were (a) the assynthesized material, (b) detemplated but not ion-exchanged parent crystals (Na-form), and (c) detemplated and ion-exchanged parent crystals (NH4-form). The primary objective of these studies was to determine how. complete inertisation of the external surface acidity could be achieved. By modifying samples under different conditions as outlined above, information was obtained on the uniformity of the coating of samples modified in each of the different systems. ZSM-5, Mordenite and Beta samples modified using similar CVD and CLD modification conditions were compared. Post-modification treatment was employed to determine whether the silica layer deposited during CVD treatment was irreversibly attached to the external surface of the samples. DA - 1998 DB - OpenUCT DP - University of Cape Town LK - https://open.uct.ac.za PB - University of Cape Town PY - 1998 T1 - The inertisation of the zeolites ZSM-5, mordenite and beta by chemical vapour deposition using tetraethoxysilane TI - The inertisation of the zeolites ZSM-5, mordenite and beta by chemical vapour deposition using tetraethoxysilane UR - http://hdl.handle.net/11427/23695 ER - en_ZA
dc.identifier.urihttp://hdl.handle.net/11427/23695
dc.identifier.vancouvercitationWeber RW, Weber RW. The inertisation of the zeolites ZSM-5, mordenite and beta by chemical vapour deposition using tetraethoxysilane. [Thesis]. University of Cape Town ,Faculty of Engineering & the Built Environment ,Department of Chemical Engineering, 1998 [cited yyyy month dd]. Available from: http://hdl.handle.net/11427/23695en_ZA
dc.language.isoeng
dc.language.isoeng
dc.publisher.departmentDepartment of Chemical Engineeringen_ZA
dc.publisher.facultyFaculty of Engineering and the Built Environment
dc.publisher.institutionUniversity of Cape Town
dc.publisher.institutionUniversity of Cape Town
dc.subject.otherChemical Engineering
dc.titleThe inertisation of the zeolites ZSM-5, mordenite and beta by chemical vapour deposition using tetraethoxysilane
dc.titleThe inertisation of the zeolites ZSM-5, mordenite and beta by chemical vapour deposition using tetraethoxysilane
dc.typeDoctoral Thesis
dc.type.qualificationlevelDoctoral
dc.type.qualificationnamePhD
uct.type.filetype
uct.type.filetypeText
uct.type.filetypeImage
uct.type.publicationResearch
uct.type.resourceThesis
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