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49,80 €ISBN 978-3-8440-5768-3Softcover204 pages94 figures302 g21 x 14,8 cmEnglishThesis
February 2018
Gregor Kiedorf
Mechanistic and kinetic analysis of homogeneously and heterogeneously catalyzed reactions
The experimental study of novel reactor concepts is financially expensive and time consuming. In order to optimize the reactor and process development, model based optimization strategies are becoming more popular. Basic requirement of these strategies are general reaction kinetics in a broad temperature and concentration range. Quite often simple empirical rate expressions, e.g. power laws, are in good agreement with available experimental data. However, there are several limits of such rate equations with respect to extrapolation. For this reason, the present work focuses on mechanistic reaction kinetic analysis and the corresponding parameter estimation in homogeneous and heterogeneous catalysis and their model application in innovative dynamic reactor concepts. The efficient and phase independent "General Catalytic Cycle Kinetics (GCCK)" approach (or Christiansen methodology) is used to derive mechanistic kinetic rate approaches based on catalytic cycles. Due to high number of unknown kinetic parameters included in the mechanistically based GCCK approach, suitable model reduction techniques, such as the subset selection method or additional independent specific dynamic experimental data, support parameter estimation. Sensitive parameters can be identified and determined for the reduced kinetic models. In the presented case studies, the GCCK approach is successfully applied for the homogeneously catalyzed hydroformylation and the heterogeneously catalyzed total oxidation.
Keywords: kinetic analysis; parameter estimation; homogeneous and heterogeneous catalysis; loop reactor
Forschungsberichte aus dem Max-Planck-Institut für Dynamik komplexer technischer Systeme
Edited by Prof. Dr. Peter Benner, Prof. Dr.-Ing. Udo Reichl, Prof. Dr.-Ing. Andreas Seidel-Morgenstern and Prof. Dr.-Ing. Kai Sundmacher, Magdeburg
Volume 49
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