07 Fakultät Konstruktions-, Produktions- und Fahrzeugtechnik

Permanent URI for this collectionhttps://elib.uni-stuttgart.de/handle/11682/8

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1974 - 19786

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Start date: 1974End date: 1979

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    Kinetic instabilities in heterogeneously catalyzed reactions. Pt. 1, Rate multiplicity with Langmuir-type kinetics
    (1978) Eigenberger, Gerhart
    This paper is concerned with the occurrence of rate multiplicities (ignition-extinction phenomena). It is shown that rate multiplicity can be caused by the competing chemisorption of A and B upon the same active sites of the catalyst. Rate multiplicity can occur if at least one of the chemisorption or reaction steps is of second order. No rate multiplicity can be expected, if either A or B reacts via an Eley-Rideal type mechanism.
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    Mechanismen und Auswirkungen kinetischer Instabilitäten bei heterogen-katalytischen Reaktionen
    (1976) Eigenberger, Gerhart
    Die gewonnenen Ergebnisse lassen den Schluß zu, daß kinetische Instabilitäten bei heterogen-katalytischen Reaktionen mit formalkinetischen Ansätzen vom Langmuir-Typ sinnvoll beschrieben werden können. Die gelegentlich geäußerte Hoffnung, daß aus einer solchen modellmäßigen Beschreibung der Reaktion im Instabilitätsbereich Schlüsse auf die tatsächlich wirksamen Mechanismen (Mikrokinetik) der Reaktion gezogen werden können, wird allerdings selten erfüllt sein. Wie bei der Aufstellung von Langmuir-Hinshelwood-Ansätzen für eine Oberflächenreaktion ergibt sich auch hier eine beinahe unbeschränkte Mannigfaltigkeit bei der Postulation möglicher Mechanismen. Hier wie dort wird es das Ziel der reaktionstechnischen Betrachtung sein, einen möglichst einfachen Mechanismus mit einem möglichst großen Gültigkeitsbereich zu finden. Für den Fall der CO-Oxydation an Platin sollte diese Arbeit einige Hinweise dazu liefern.
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    Influence of the wall on the dynamic behavior of homogeneous tubular reactors with a highly exothermic reaction
    (1974) Eigenberger, Gerhart
    The influence of the tube wall on the behavior of tubular reactors with a highly exothermic reaction was studied. The effect of heat accumulation in the wall has a considerable influence upon the transient behavior of the reactor. Because of this influence excess temperatures can occur if the feed temperature is lowered or the flow velocity is raised. For a gas phase reaction the transient behavior is determined almost completely by the heat capacity of the wall. An example of multiple steady states caused by axial heat conduction in the wall is given, and the influence of heat conduction in the wall is compared with that in the reaction mixture.
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    Kinetic instabilities in catalytic reactions : a modelling approach
    (1976) Eigenberger, Gerhart
    It is the purpose of this contribution to show under which conditions relatively simple Langmuir-type rate mechanisms exhibit steady state multiplicity as well as periodic instabilities and may serve as models for experimentally observed phenomena.
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    A modified Crank-Nicolson technique with non-equidistant space steps
    (1976) Eigenberger, Gerhart; Butt, John B.
    A finite difference method with non-equidistant space steps, based upon the Crank-Nicolson technique is presented. Its prime feature is the automatic positioning of axial grid points at required positions. Thus reducing considerably the total number of grid points and hence the amount of computer time. The method is demonstrated for a number of examples of tubular reactor calculations. It proves to be well suited for the solution of all kinds of diffusion type models, especially if steep gradients or moving profiles occur, and can be used even on moderate size process computers.
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    Kinetic instabilities in heterogeneously catalyzed reactions. Pt. 2, Oscillatory instabilities with Langmuir type reactions
    (1978) Eigenberger, Gerhart
    An analysis of the kinetic model studied in Part I of this contribution gave no indication for the occurrance of periodic solutions. However if an additional slow chemisorption ("buffer") step is added to the model, relaxation oscillations can develop in regions where the original model exhibited multiple solutions. The behaviour of the extended model is analysed via the singular perturbation approach and by simulation. It is shown that a broad variety of slow chemisorption steps can serve as buffer with the restriction that the buffer step should not, or at least only slightly, contribute to the surface reaction.