Grenzen konventioneller Ansätze zur Beschreibung der effektiven Kinetik dreiphasiger heterogen-katalysierter Reaktionen - Untersuchungen am Modellsystem der Ni-katalysierten Hydrierung von 1-Hexen

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Fortschritt-Berichte VDI

Dipl.-Ing. Stefan Fritz, Bayreuth

Nr. 943

Verfahrenstechnik

Reihe 3

Grenzen konventioneller Ansätze zur Beschrei-

bung der effektiven Kinetik dreiphasiger

heterogen-katalysierter Reaktionen

Untersuchungen am Modellsystem

der Ni-katalysierten Hydrierung

von 1-Hexen

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ZĞĂŬƚŝŽŶĞŶ Ͳ

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ƌƐƚŐƵƚĂĐŚƚĞƌ͗ WƌŽĨ͘ƌ͘Ͳ/ŶŐ͘ŶĚƌĞĂƐ:ĞƐƐ

ǁĞŝƚŐƵƚĂĐŚƚĞƌ͗ WƌŽĨ͘ƌ͘ƌĞƌ͘ŶĂƚ͘WĞƚĞƌtĂƐƐĞƌƐĐŚĞŝĚ dĂŐĚĞƌŵƺŶĚůŝĐŚĞŶWƌƺĨƵŶŐ͗ Ϯϯ͘:ƵůŝϮϬϭϰ

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Black L_143694_Pflichtexemplare.pdf

Oktober 22, 2014 | 09:13:38 1

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Reihe 3

Fortschritt-Berichte VDI

Grenzen konventioneller Ansätze zur Beschrei- bung der effektiven Kinetik dreiphasiger

heterogen-katalysierter Reaktionen

Untersuchungen am Modellsystem der Ni-katalysierten Hydrierung von 1-Hexen

Dipl.-Ing. Stefan Fritz, Bayreuth

Verfahrenstechnik

Nr. 943

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Alle Rechte, auch das des auszugsweisen Nachdruckes, der auszugsweisen oder vollständigen Wiedergabe (Fotokopie, Mikrokopie), der Speicherung in Datenverarbeitungsanlagen, im Internet und das der Übersetzung, vorbehalten.

Als Manuskript gedruckt. Printed in Germany.

ISSN 0178-9503

dreiphasiger heterogen-katalysierter Reaktionen

Untersuchungen am Modellsystem der Ni-katalysierten Hydrierung von 1-Hexen

Fortschr.-Ber. VDI Reihe 3 Nr. 943. Düsseldorf: VDI Verlag 2014.

178 Seiten, 95 Bilder, 16 Tabellen.

ISBN 978-3-18-394303-6, ISSN 0178-9503,

¤ 67,00/VDI-Mitgliederpreis ¤ 60,30.

Für die Dokumentation: Dreiphasige heterogene Katalyse – Hydrierung – Gas- und Dampf- blasenbildung – Effektive Reaktionskinetik – Wärmetransport – Stofftransport – Empirische Korrelationen – Thiele-/Zeldovich-Modell – Oszillationstheorie

Hinsichtlich der ökonomischen Effizienz und Aspekten der Sicherheit ist die Vorhersage des Prozessverhaltens dreiphasiger heterogen-katalysierter Reaktionen bei der Auslegung von Reak- toren erforderlich und die Kenntnis des externen als auch internen Wärme- und Stofftransports somit von großer Bedeutung. Unter bestimmten Prozessbedingungen kommt es aufgrund einer oszillierenden Gas- und/oder Dampfblasenbildung zu einem konvektiven Stoff- und Wärme- strom; dieser wirkt sich erheblich auf die Hydrodynamik sowohl im Katalysatorpartikel als auch in der umgebenden Flüssigphase aus. Im Zuge konventioneller Korrelationen und Modell- ansätze wird dieser konvektive Beitrag nicht berücksichtigt. Mit Hilfe der Oszillationstheorie kann der enorme Einfluss der Blasenbildung hingegen erklärt und die experimentellen Befunde interpretiert werden. Die unterschiedlichen Mechanismen des Stoff- und Wärmetransports und verschiedene Konzepte zur Beschreibung entsprechender Reaktionen bei unterschiedlichen Prozessbedingungen werden im Detail diskutiert.

Bibliographische Information der Deutschen Bibliothek

Die Deutsche Bibliothek verzeichnet diese Publikation in der Deutschen Nationalbibliographie;

detaillierte bibliographische Daten sind im Internet unter http://dnb.ddb.de abrufbar.

Bibliographic information published by the Deutsche Bibliothek (German National Library)

The Deutsche Bibliothek lists this publication in the Deutsche Nationalbibliographie (German National Bibliography); detailed bibliographic data is available via Internet at http://dnb.ddb.de.

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ϱ͘ϴ͘Ϯ͘ϭ ŝŶĨůƵƐƐĞŝŶĞƐŝŶĞƌƚĞŶ&ƌĞŵĚŐĂƐĞƐĂƵĨĚŝĞĞĨĨĞŬƚŝǀĞZĞĂŬƚŝŽŶƐͲ

ŐĞƐĐŚǁŝŶĚŝŐŬĞŝƚ͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘ϭϯϭ ϱ͘ϴ͘Ϯ͘Ϯ ŝŶĨůƵƐƐĚĞƐ&ƌĞŵĚŐĂƐĞƐĂƵĨĚĞŶćƵƘĞƌĞŶtćƌŵĞƚƌĂŶƐƉŽƌƚ͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘ϭϯϮ ϱ͘ϴ͘ϯ ŝŶĨůƵƐƐĞŝŶĞƌŬŽŶŝƐĐŚĞŶDĂŬƌŽƉŽƌĞ͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘ϭϯϯ

ϲ ƵƐĂŵŵĞŶĨĂƐƐƵŶŐ͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘ϭϯϱ ϳ ^ƵŵŵĂƌǇ͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘ϭϰϭ ϴ ŶŚĂŶŐ͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘ϭϰϳ ϴ͘ϭ ŶŚĂŶŐ͗,ĞƌůĞŝƚƵŶŐĞŶǁŝĐŚƚŝŐĞƌ'ůĞŝĐŚƵŶŐĞŶ͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘ϭϰϳ ϴ͘ϭ͘ϭ ^ƚŽĨĨďŝůĂŶǌƵŶƚĞƌĚĞƌŶŶĂŚŵĞĞŝŶĞƌĞďĞŶĞŶWůĂƚƚĞ͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘ϭϰϳ ϴ͘ϭ͘Ϯ mďĞƌƐĐŚƵƐƐŬƌŝƚĞƌŝƵŵʗ_ŝŶƚŝŵ/ŶŶĞƌĞŶĚĞƐWĂƌƚŝŬĞůƐ͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘ϭϰϴ ϴ͘ϭ͘ϯ WŽƌĞŶŶƵƚǌƵŶŐƐŐƌĂĚƵŶĚŵŽĚŝĨŝǌŝĞƌƚĞƌdŚŝĞůĞͲDŽĚƵů͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘ϭϰϵ ϴ͘Ϯ ŶŚĂŶŐ͗dĂďĞůůĂƌŝƐĐŚĞDĞƐƐĞƌŐĞďŶŝƐƐĞƵŶĚďĞƌĞĐŚŶĞƚĞtĞƌƚĞĚĞƌZŝŶŐƐƉĂůƚͲ

ǀĞƌƐƵĐŚĞ͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘ϭϱϭ ϴ͘ϯ ŶŚĂŶŐ͗WŚǇƐŝŬĂůŝƐĐŚĞ^ƚŽĨĨŐƌƂƘĞŶ͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘ϭϱϯ ϵ >ŝƚĞƌĂƚƵƌǀĞƌǌĞŝĐŚŶŝƐ͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘ϭϱϴ sĞƌƂĨĨĞŶƚůŝĐŚƵŶŐĞŶ͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘͘ϭϲϯ

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ѐǀ, sĞƌĚĂŵƉĨƵŶŐƐĞŶƚŚĂůƉŝĞ :ͬŵŽů

KďĞƌĨůćĐŚĞ ŵϸ

Ă dĞŵƉĞƌĂƚƵƌůĞŝƚĨćŚŝŐŬĞŝƚ ŵϸͬƐ

Ă <ŽŚćƐŝŽŶƐĚƌƵĐŬ WĂͼŵ^ϲͬŵŽůϸ

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_Ɖ ćƵƘĞƌĞWĂƌƚŝŬĞůŽďĞƌĨůćĐŚĞ ŵϸ

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ď <ŽǀŽůƵŵĞŶ ŵϹͬŵŽů

Đ <ŽŶǌĞŶƚƌĂƚŝŽŶ ŵŽůͬŵϹ

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ŝĨĨƵƐŝŽŶƐŬŽĞĨĨŝǌŝĞŶƚ ŵϸͬƐ

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_ϲ,ϭϮ ŝĨĨƵƐŝŽŶƐŬŽĞĨĨŝǌŝĞŶƚǀŽŶϭͲ,ĞǆĞŶŝŶϭͲ,ĞǆĞŶ ŵϸͬƐ _,Ϯ ŝĨĨƵƐŝŽŶƐŬŽĞĨĨŝǌŝĞŶƚǀŽŶtĂƐƐĞƌƐƚŽĨĨŝŶϭͲ,ĞǆĞŶ ŵϸͬƐ

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ĨŽƌŵĂůĞŝĨĨƵƐŝŽŶƐĞŶĞƌŐŝĞ :ͬŵŽů

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Ő ƌĚďĞƐĐŚůĞƵŶŝŐƵŶŐ ŵϸͬƐ

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Z ƵŶŝǀĞƌƐĞůůĞ'ĂƐŬŽŶƐƚĂŶƚĞ :ͬ;ŵŽůͼ<Ϳ

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