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81 Springer Series in Chemical Physics Springer Springer Series in Chemical Physics 81 Edited by J. P. Toennies Springer Berlin Heidelberg New York Barcelona Budapest Hong Kong London Milan Paris Santa Clara Singapore Tokyo Springer Series in Chemical Physics Editors: Vitalii I. Goldanskii Fritz P. Schafer J. Peter Toennies Managing Editor: H. K. V. Lotsch 40 High-Resolution Spectroscopy of 52 Multiple-Photon Laser Chemistry Transient Molecules By. R.V. Ambartzumian, C.D. Cantrell, By E. Hirota and A. Puretzky 41 High Resolution Spectral Atlas of 53 Ultrafast Phenomena VII Nitrogen Dioxide 559-597 nm Editors: C. B. Harris, E. P. Ippen, By K. Uehara and H. Sasada G.A. Mourou, and A.H. Zewail 42 Antennas and Reaction Centers of 54 Physics of Ion Impact Phenomena Photosynthetic Bacteria Editor: D. Mathur Structure, Interactions, and Dynamics 55 Ultrafast Phenomena VIII Editor: M.E. Michel-Beyerle Editors: J.-L. Martin, A. Migus, 43 The Atom-Atom Potential Method G. A. Mourou, and A. H. Zewail Applications to Organic Molecular 56 Clusters of Atoms and Molecules Solids Salvation and Chemistry of Free By A.J. Pertsin and A.I. Kitaigorodsky Clusters, and Embedded, Supported and 44 Secondary Ion Mass Spectrometry Compressed Clusters SIMS V Editor: H. Haberland Editors: A. Benninghoven, R. J. Colton, 57 Radiationless Transitions in Poly- D.S. Simons, and H.W. Werner atomic Molecules 45 Thermotropic Liquid Crystals, By E. S. Medvedev and V. I. Osherov Fundamentals 58 Positron Annihilation in Chemistry By G. Vertogen and W.H. de Jeu By O. E. Mogensen 46 Ultrafast Phenomena V 59 Soot Formation in Combustion Editors: G.R. Fleming and Mechanisms and Models A.E. Siegman Editor: H. Bockhorn 47 Complex Chemical Reaction Systems 60 Ultrafast Phenomena IX Mathematical Modelling Editors: P. F. Barbara, W. H. Knox, and Simulation G. A. Mourou, and A. H. Zewail Editors: J. Warnatz and W. Jager 61 Gas Phase Chemical Reaction Systems 48 Ultrafast Phenomena VI Experiments and Models 100 Years Editors: T. Yajima, K. Yoshihara, After Max Bodenstein C. B. Harris, and S. Shionoya Editors: J. Wolfrum, H.-R. Volpp, 49 Vibronic Interactions in Molecules R. Rannacher, and J. Warnatz and Crystals 62 Ultrafast Phenomena X By B. Bersuker and V. Z. Polinger I. Editors: P. F. Barbara, J. G. Fujimoto, 50 Molecular and Laser Spectroscopy W. H. Knox, and W. Zinth By Zu-Geng Wang and Hui-Rong Xia 51 Space-Time Organization in Macro- molecular Fluids Editors: F. Tanaka, M. Doi, and T.Ohta Volumes 1-39 are listed at the end of the book 1. Wolfrum· H.-R. Volpp R. Rannacher . 1. Warnatz (Eds.) Gas Phase Chemical Reaction Systems Experiments and Models 100 Years After Max Bodenstein Proceedings of an International Symposion, held at the "Internationales Wissenschaftsforum Heidelberg", Heidelberg, Germany, July 25-28, 1995 With 148 Figures Springer Professor Dr. J. Wolfrum Professor Dr. J. Warnatz Dr. H.-R. Volpp Interdisziplinlires Zentrum Physikalisch-Chemisches Institut flir WissenschaftIiches Rechnen Universitiit Heidelberg Universitiit Heidelberg 1m Neuenheimer Feld 253 1m Neuenheimer Feld 368 D-69120 Heidelberg, Germany D-69120 Heidelberg, Germany Professor Dr. R. Rannacher Institut flir Angewandte Mathematik Universitat Heidelberg 1m Neuenheimer Feld 293 D-69120 Heidelberg, Germany Series Editors Professor Dr. Fritz Peter Schafer Max-Planck- Institut flir Biophysikalische Chemie D-37077 Gottingen-Nikolausberg, Germany Professor Vitalii I. Goldanskii Professor Dr. J. Peter Toennies Institute of Chemical Physics Max-Planck- Institut Academy of Sciences flir Stromungsforschung Ulitsa Kossigyna 4 B unsenstrasse 10 Moscow, 117334, Russia D-37073 Gottingen, Germany Managing Editor: Dr. Helmut K.Y. Lotsch Springer-Verlag, Tiergartenstrasse 17, D-69121 Heidelberg, Germany Cataloging-in-Publication Data applied for Die Deutsche Bibliothek - CIP-Einheitsaufnahme Gas pbase cbemical raction systems: experiments and models 100 years after Max Bodenstein ; proceedings of an international symposion, held at the Internationales Wissenschaftsforum Heidelberg, Heidelberg, Germany, July 25 - 28, 19951 J. Wolfrum ... (ed.). - Berlin; Heidelberg; New York; Barcelona; Budapest; Hong Kong; London; Mil&..il ; Paris; Santa Clara; Singapore; Tokyo: Springer, 1996 (Springer series in chemical physics ; Vol. 61) ISBN 3-540-61662-4 NE: Wolfrum, Jiirgen [Hrsg.]; Intemationales Wissenschaftsforum <Heidelberg>; GT ISSN 0172-6218 ISBN-13: 978-3-642-80301-7 e-ISBN-13: 978-3-642-80299-7 001: 10.1007/978-3-642-80299-7 This work is subject to copyright. All rights are reserved, whether the whole or part of the material is concerned, specifically the rights of translation, reprinting, reuse of illustrations, recitation, broadcasting, reproduction on microfilms or in any other way, and storage in data banks. Duplication of this publication or parts thereof is permitted only under the provisions of the German Copyright Law of September 9, 1965, in its current version, and permission for use must always be obtained from Springer-Verlag. Violations are liable for prosecution under the German Copyright Law. © Springer-Verlag Berlin Heidelberg 1996 Softcover reprint of the hardcover I st edition 1996 The use of general descriptive names, registered names, trademarks, etc. in this publication does not imply, even in the absence of a specific statement, that such names are exempt from the relevant protective laws and regulations and therefore free for general use. SPIN: 10545060 54/3144 3 2 10- Printed on acid-free paper Preface This volume consists of edited papers presented at the International Symposion Gas Phase Chemical Reaction Systems: Experiments and Models 100 Years After Max Bodenslein, held at the Internationales Wissenschaftsforum Heidelberg (IWH) in Heidelberg during July 25-28, 1995. The intention of this symposion was to bring together leading researchers from the fields of reaction dynamics, kinetics, catalysis and reactive flow model­ ling to discuss and review the advances in the understanding of chemical kinetics about 100 years after Max Bodenstein's pioneering work on the "hydrogen iodine reaction", which he carried out at the Chemistry Institute of the University of Heidelberg. The idea to focus in his doctoral thesis [1] on this reaction was brought up by his supervisor Victor Meyer (successor of Robert Bunsen at the Chemistry Institute of the University of Heidelberg) and originated from the non­ reproducible behaviour found by Bunsen and Roscoe in their early photochemical investigations of the H2/Cl2 system [2] and by van't Hoff [3], and V. Meyer and co-workers [4] in their experiments on the slow combustion of H2/02 mixtures. Whereas earlier work by Hautefeuille [5] and Lemoine [6] on the "behavi­ our of hydrogen iodine gas in the heat" and the "photosensitivity of hydrogen iodine" was more of a qualitative character, it was Bodenstein's systematic studies on the thennal [7] and light-induced [8] decomposition of hydrogen iodine, where he combined experimental reaction kinetics studies with mathematical analysis and modelling, that paved the way for modem quantitative treatment of chemical systems of practical interest. Chemical processes occurring in industrial applica­ tions, such as in engine combustion or the chemical vapour deposition of diamond, usually consist of a large number of elementary chemical reactions coupled with transport and diffusion phenomena and very often involve heterogeneous reaction steps. Therefore, the development of reliable computational methods for numerical modelling and simulation of such processes necessitates a close and well-coordi­ nated interaction across the disciplinary boundaries of mathematics, physics, chemistry, and engineering. In the past, two workshops held here in Heidelberg [9,10] paid tribute to this multidisciplinary challenge, which was also recognized by the foundation of the Interdiszipliniires Zentrumfiir Wissenschaftliches Rechnen (IWR) in 1987 and the subsequent establishment of the Sondeiforschungbereich (SFB) 359: Reaktive Stromungen, Diffusion und Transport at the University of Heidelberg in 1993. It was the encouraging experience and enthusiasm within the research work of the SFB 359 that led to the idea of this symposion, which we hope has achieved its aims, both to remember the historical impact Max Bodenstein had on the develop­ ment of chemical kinetics and to allow for intense discussions between scientists who actively work on different aspects of the quantitative investigation and model­ ling of chemical reaction systems. Overall about 100 scientists from 10 countries (England, France, Gennany, Hungary, India, Israel, Italy, Sweden, Taiwan, and the U.S.A.) participated, pre­ senting and discussing a total of 23 papers and 21 posters and making this sympo­ sion a very stimulating one. We hope that this book will transfer a flavour of this stimulating atmosphere to a wider audience. The "Bodenstein family tree" depicted in Fig. I was created - with the enthusiastic help of the participants - during the symposion in order to illustrate v the scientific connections (rather than strict teacher-student relationships) originat­ ing from Max Bodenstein's pioneering work. We by no means intend this tree to be an exhaustive representation of the kinetics community. In addition, for those readers who are interested in more historical details of Max Bodenstein's life we would like to recommend the beautiful article by Erika Cremer [11], in which she describes his scientific life which led him from Heidel­ berg (where he received his doctoral degree in 1893), via Berlin,
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