Elementary Reaction Steps in Heterogeneous Catalysis
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1 Elementary Reaction Steps in Heterogeneous Catalysis
2 NATO ASI Series Advanced Science Institutes Series A Series presenting the results of activities sponsored by the NA TO Science Committee, which aims at the dissemination of advanced scientific and technological knowledge, with a view to strengthening links between scientific communities. The Series is published by an intemational board of publishers in conjunction with the NATO Scientific Affairs Division A Life Sciences B Physics C Mathematical and Physical Sciences D Behavioural and Social Sciences E Applied Sciences F Computer and Systems Sciences G Ecological Sciences H Cell Biology I Global Environmental Change Plenum Publishing Corporation London and New York Kluwer Academic Publishers Dordrecht, Boston and London Springer-Verlag Berlin, Heidelberg, New York, London, Paris and Tokyo NATO-PCO-DATA BASE The electronic index to the NATO ASI Series provides full bibliographical references (with keywords and/or abstracts) to more than contributions from international scientists published in all sections of the NATO ASI Series. Access to the NATO-PCO-DATA BASE is possible in two ways: - via online FILE 128 (NATO-PCO-DATA BASE) hosted by ESRIN, Via Galileo Galilei, Frascati, Italy. - via CD-ROM "NATO-PCO-DAT A BASE" with user-friendly retrieval software in English, French and German ( WTV GmbH and DATAWARE Technologies Inc. 1989). The CD-ROM can be ordered through any member of the Board of Publishers or through NATO-PCO, Overijse, Belgium. Series C: Mathematical and Physical Sciences - Vol. 398
3 Elementary Reaction Steps in Heterogeneous Catalysis edited by R. W. Joyner Leverhulme Centre for Innovative Catalysis, Department of Chemistry, University of Liverpool, Liverpool, United Kingdom and R. A. van Santen Schuit Institute of CatalYSiS, Eindhoven Technical University, Eindhoven, The Netherlands Springer Science + Business Media, B.V.
4 Proceedings of the NATO Advanced Research Workshop on Elementary Reaction Steps in Heterogeneous Catalysis Bedoin, Vaucluse, France November 1-7,1992 Library of Congress Cataloging-in-Publication Data NATO Advanced Research Workshop on Elementary Reaction Steps In Heterogeneous CatalysIs (1992 Bedoln, France) Elementary reaction steps In heterogeneous catalysis proceedings of the NATO Advanced Research Workshop on Elementary Reaction Steps In Heterogeneous CatalysIs, Bedoln, Vaucluse, France, November 1-7, 1992 I edited by R.W. Joyner and R.A. van Santen. p. cm. -- (NATO ASI series. Series C, Mathematical and physical sciences; no. 398) Inc 1 udes Index. ISBN ISBN (ebook) DOI / Heterogeneous catalysls--congresses. 2. Chemical reaction, Conditions and laws of--congresses. I. Joyner, R. W. II. Santen, R. A. van (Rutger A.) III. Title. IV. Series. Q0505.N ' 95--dc ISBN Printed on acid-free paper All Rights Reserved 1993 Springer Science+Business Media Dordrecht Originally published by Kluwer Academic Publishers in 1993 No part of the material protected by this copyright notice may be reproduced or utilized in any form or by any means, electronic or mechanical, including photo copying, recording or by any information storage and retrieval system, without written permission from the copyright owner.
5 CONTENTS Preface ix Introduction: Elementary Reaction Steps in Heterogeneous Catalysis.... R.W. Joyner and R.A. van Santen Session 1: Catalytic Reactivity Surface Science as a Basis for Understanding Heterogeneous Catalysis... 3 G.A. Somorjai Organometallic Chemistry as a Basis for Understanding Heterogeneous Catalysis J.M. Basset, S.L. Scott, A. Choplin, M. Leconte, F. Quignard, C. Santini and A. Theolier The Organic Chemical Approach to Heterogeneous Catalysis J.J. Rooney Electrochemical Activation of Catalysed Reactions C.G. Vayenas Selective Oxidation Pathways at Oxide Surfaces: The Transformation of Alkanes on Vanadyl Pyrophosphate G. Centi Theory of Bronsted Acidity in Zeolites R.A. van Santen, G.J. Kramer and W.P.J.H. Jacobs Discussion Summary: Session Rapporteur P.B. Wells Session 2: Swface Science Studies in Catalysis Surface Reactivity of Oxides E. Bordes Adsorption and Reactions of CO, NO, H2 and Oz on Group VIII Metal Surfaces B.E. Nieuwenhuys
6 vi Model Catalyst Studies of Titania Supported Rhodium J. Evans, B.E. Hayden, J.F.W. Mosselmans and AJ. Murray The Dynamics of Alkane Adsorption on Metals G.W. Coulston and G.L. Haller The Study of Dynamics at Catalytic Surfaces with Nuclear Magnetic Resonance Spectroscopy T.M. Duncan Discussion Summary: Session Rapporteur H.P.C.E. Kuipers Session 3: In-situ Methods in Catalysis Applications of Synchrotron Radiation in Catalysis R.W. Joyner Infrared Spectroscopy as a Probe of Surface Acidity H. Knozinger The Effects of Coadsorbates on the Behaviour of Surface Species and Sites in Catalysis by Means of EXAFS and FTIR Y.Iwasawa How Can Scanning Tunneling Microscopy, Coupled with Theory, Help Us Understand Some Elementary Steps in Catalysis P. Sautet, J.C. Dunphy and M.B. Salmeron Discussion Summary: Session Rapporteur V. Ponec Session 4: The Contribution of Theory to Catalytic Understanding Quantum Chemistry of Chemisorption at Metal and Oxide Surfaces: A Cluster Model Approach G. Pacchioni and P.S. Bagus Reaction Dynamics at Surfaces S. Holloway Chemical Reactivity as a Function of Coverage V.P. Zhdanov Solvent Effects on the Diels-Alder Reaction of Methyl Vinyl Ketone and Cyclopentadiene from Computer Simulations W.L. Jorgensen, D. Lim and J.F. Blake
7 Molecular Modeling and Molecular Graphics of Sorbates in Molecular Sieves D.P. Vercauteren, L. Leherte, DJ. Vanderveken, I.A. Horsley, C.M. Freeman and E.G. Derouane Discussion Summary: Session Rapporteur E. Shustorovich Session 5: Chemical Kinetics alld Chemical Engineering Reaction Modelling on the Basis of the Published Potential Energy Diagram K.C. Waugh Transient Kinetics in Catalysis by Metals A. Frennet Reaction Kinetics and Industrial Catalysis I. Rostrup-Nielsen Discussion Summary: Session Rapporteur I.C. Vedrine Summary Lectures Toward Next Century's Industrial Catalysis J.J. Lerou and L.E. Manzer Elementary Reaction Steps in Heterogeneous Catalysis: A Workshop Overview G.L. Haller and G.W. Coulston List of Contributors Index vii
8 Preface This book comprises the proceedings of a NATO sponsored Advanced Research Workshop held from 1st November to 6th November 1992 in the delightful Chateau de Florans, Bedoin, Vaucluse, France and entitled 'Elementary Reaction Steps in Heterogeneous Catalysis.' The organisers are grateful to the Science Committee of NATO for their support of this meeting. This is believed to be the first wide ranging NATO ARW in the field of heterogeneous catalysis for 20 years, following a previous venture organised in Sardinia by Basolo and Burwell, of Northwestern University, Illinois, USA [1]. This volume collects the lecture presentations and reports on the lively Panel discussions. The idea for the meeting evolved from a series of International Symposia on Quantum Chemistry and Mechanism in Heterogeneous Catalysis. The first of these was held in Lyon, France in 1986, the second in Krakow, Poland in 1988 and the third in Berkeley, California in The organising committee of the present meeting was Bernard Bigot, France, Tony Farragher, Netherlands, Richard Joyner, UK, Mme. Danielle Olivier, France, and Rutger van Santen, Netherlands, (Chairman). We wish to thank all members of the committee but in particular Bernard Bigot, who undertook the very extensive work involved in the local organisation with consummate skill and made our stay in Provence a great pleasure. Bernard Bigot's secretary, Mme. Marie-Noelle Coscat and Richard Joyner's secretary, Mrs. Pat Gibbs, also deserve our considerable thanks. There were fifty-four participants from eleven countries. About two thirds of these came from academic laboratories and the rest from the European and American chemical and oil industry. The backgrounds of the participants varied from chemical engineering to theoretical physics and surface physics to organic chemistry. We would like to thank all those who took part. Richard Joyner Liverpool Rutger van Santen Eindhoven 1) Basolo, F. and Burwell, R.L Jr., Eds., (1973) 'Catalysis, Progress in Research,' Plenum New York. ix
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