Hydroconversion of methylcyclohexane on TEOS-modified H-ZSM-5 zeolite catalysts: Production of a high-quality synthetic steamcracker feedstock

With the advent of the European Auto Oil Programme and comparable legislation in other parts of the world, the aromatics content of gasoline has to be reduced considerably. Therefore, new outlets for surplus aromatics have to be found. Mixed n-alkanes with two and more carbon atoms (C 2+- n-alkanes)...

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Veröffentlicht in:	Microporous and mesoporous materials Jg. 59; H. 1; S. 1 - 12
Hauptverfasser:	Berger, Christine, Raichle, Andreas, Rakoczy, Rainer A, Traa, Yvonne, Weitkamp, Jens
Format:	Journal Article
Sprache:	Englisch
Veröffentlicht:	Amsterdam Elsevier Inc 18.04.2003 Elsevier
Schlagworte:	Catalysis Catalytic reactions Chemical liquid deposition (CLD) Chemistry Exact sciences and technology General and physical chemistry Ring opening of cycloalkanes Steamcracker feed (synthetic) Tetraethoxysilane (TEOS) Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry Zeolite H-ZSM-5 Chemical liquid deposition (CLD) Zeolite H-ZSM-5 Ring opening of cycloalkanes Steamcracker feed (synthetic) Tetraethoxysilane (TEOS) Catalytic reaction Cyclohexane derivatives Hydrocarbon Steam cracking Acidic site Organic silane Zeolite Cycloalkane Experimental study Ring cleavage Molecular sieve Heterogeneous catalysis Brönsted acid Preparation Modified material
ISSN:	1387-1811, 1873-3093
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Abstract	With the advent of the European Auto Oil Programme and comparable legislation in other parts of the world, the aromatics content of gasoline has to be reduced considerably. Therefore, new outlets for surplus aromatics have to be found. Mixed n-alkanes with two and more carbon atoms (C 2+- n-alkanes) represent a high-quality synthetic feedstock for steamcrackers. Thus, the hydrogenation of aromatics to cycloalkanes followed by their hydroconversion into C 2+- n-alkanes (predominantly ethane, propane and n-butane) could become a useful process option for converting surplus aromatics into a synthetic steamcracker feed. During hydroconversion of methylcyclohexane to C 2+- n-alkanes, the catalytic properties of acidic zeolite H-ZSM-5 can be remarkably improved by chemical liquid deposition of tetraethoxysilane. Thereby, the yield of the desired C 2+- n-alkanes at, e.g., 400 °C can be enhanced from around 77% to nearly 82%. Simultaneously, a drastic diminution of the concentration of external Brønsted acid sites and a significant decrease of the total concentration of Brønsted acid sites were observed by adsorption of, respectively, collidine and pyridine monitored by FTIR spectroscopy. Nitrogen adsorption experiments revealed a slight decrease of the micropore volume. These data are consistent with an extensive deactivation of the active sites on the external surface and in close proximity to the pore openings, the latter leading to pore mouth narrowing or, more likely, to partial pore mouth plugging.
AbstractList	With the advent of the European Auto Oil Programme and comparable legislation in other parts of the world, the aromatics content of gasoline has to be reduced considerably. Therefore, new outlets for surplus aromatics have to be found. Mixed n-alkanes with two and more carbon atoms (C 2+- n-alkanes) represent a high-quality synthetic feedstock for steamcrackers. Thus, the hydrogenation of aromatics to cycloalkanes followed by their hydroconversion into C 2+- n-alkanes (predominantly ethane, propane and n-butane) could become a useful process option for converting surplus aromatics into a synthetic steamcracker feed. During hydroconversion of methylcyclohexane to C 2+- n-alkanes, the catalytic properties of acidic zeolite H-ZSM-5 can be remarkably improved by chemical liquid deposition of tetraethoxysilane. Thereby, the yield of the desired C 2+- n-alkanes at, e.g., 400 °C can be enhanced from around 77% to nearly 82%. Simultaneously, a drastic diminution of the concentration of external Brønsted acid sites and a significant decrease of the total concentration of Brønsted acid sites were observed by adsorption of, respectively, collidine and pyridine monitored by FTIR spectroscopy. Nitrogen adsorption experiments revealed a slight decrease of the micropore volume. These data are consistent with an extensive deactivation of the active sites on the external surface and in close proximity to the pore openings, the latter leading to pore mouth narrowing or, more likely, to partial pore mouth plugging.
Author	Raichle, Andreas Weitkamp, Jens Rakoczy, Rainer A Traa, Yvonne Berger, Christine
Author_xml	– sequence: 1 givenname: Christine surname: Berger fullname: Berger, Christine – sequence: 2 givenname: Andreas surname: Raichle fullname: Raichle, Andreas – sequence: 3 givenname: Rainer A surname: Rakoczy fullname: Rakoczy, Rainer A – sequence: 4 givenname: Yvonne surname: Traa fullname: Traa, Yvonne – sequence: 5 givenname: Jens surname: Weitkamp fullname: Weitkamp, Jens email: jens.weitkamp@po.uni-stuttgart.de
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Keywords	Chemical liquid deposition (CLD) Zeolite H-ZSM-5 Ring opening of cycloalkanes Steamcracker feed (synthetic) Tetraethoxysilane (TEOS) Catalytic reaction Cyclohexane derivatives Hydrocarbon Steam cracking Acidic site Organic silane Zeolite Cycloalkane Experimental study Ring cleavage Molecular sieve Heterogeneous catalysis Brönsted acid Preparation Modified material
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SubjectTerms	Catalysis Catalytic reactions Chemical liquid deposition (CLD) Chemistry Exact sciences and technology General and physical chemistry Ring opening of cycloalkanes Steamcracker feed (synthetic) Tetraethoxysilane (TEOS) Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry Zeolite H-ZSM-5
Title	Hydroconversion of methylcyclohexane on TEOS-modified H-ZSM-5 zeolite catalysts: Production of a high-quality synthetic steamcracker feedstock
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