Progress in Catalyst Deactivation: Proceedings of the NATO Advanced Study Institute on Catalyst Deactivation, Algarve, Portugal, May 18–29, 1981 PDF
Preview Progress in Catalyst Deactivation: Proceedings of the NATO Advanced Study Institute on Catalyst Deactivation, Algarve, Portugal, May 18–29, 1981
PROGRESS IN CATALYST DEACTIVATION NATO ADVANCED STUDY INSTITUTES SERIES Proceedings of the Advanced Study Institute Programme, which aims at the dissemination of advanced knowledge and the formation of contacts among scientists from different countries. The series is published by an international board of publishers in conjunction with NATO Scientific Affairs Division A Life Sciences Plenum Publishing Corporation B Physics London and New York C Mathematical and D. Reidel Publishing Company Physical Sciences Dordrecht and Boston D Behavioural and Martinus Nijhoff Publishers Social Sciences The Hague, Boston and London E Applied Sciences Series E: Applied Sciences - No. 54 PROGRESS IN CATALYST DEACTIVATION Proceedings of the NATO Advanced Study Institute on Catalyst Deactivation, Algarve, Portugal, May 18-29, 1981 edited by Jose Luis Figueiredo Professor of Chemical Engineering University of Porto, Portugal 'Mil . ;D~ !! ~ ~ .·.a~1 1982 Martinus Nijhoff Publishers The Hague! Boston! London Distributors: for the United States and Canada Kluwer Boston, Inc. 190 Old Derby Street Hingham, MA 02043 USA for all other countries Kluwer Academic Publishers Group Distribution Center P.O.Box 322 3300 AH Dordrecht The Netherlands Library of Congress Cataloging in Publication Data NATO Advanced Study Institute on Catalyst Deactivation (1981 : Algarve. Portugal) Progress in catalyst deactivation. (NATO advanced study institutes. Series E. Applied sciences ; v. 54) 1. Catalyst poisoning--Congresses. 1. Figueiredo, Jose Luis. II. Title. III. Series. TP156.C35N37 1981 660.2'995 82-7886 ISBN-U 978-94-009-7599-6 AACR2 ISBN-13: 978-94-009-7599-6 e-ISBN-13: 978-94-009-7599-6 001: 10.1007/978-94-009-7599-6 Copyright © 1982 by Martinus Nijhoff Publishers, The Hague. Softcover reprint of the hardcover 15t edition 1982 All rights reserved. No part of this publication may be reproduced, stored in a retrieval system, or transmitted, in any form or by any means, mechanical, photocopying, recording, or otherwise, without the prior written permission of the publishers, Martinus Nijhoff Publishers, P.O. Box 566,2501 CN The Hague, The Netherlands. v PREFACE Most catalysts used in the chemical and petrochemical indus tries are strongly affected by one or another form of deactivation, leading to poor performances and reduced life. The increasing num ber of scientific communications devoted to the subject in recent years, and culminating with an International Symposium held in Antwerp in October 1980, is a measure of the interest it arouses in both the industrial and academic communities. A stage has been reached whereby it was thought that a NATO Advanced Study Institute on "Catalyst Deactivation" might be fruit ful in establishing the state of the art and in stimulating a more systematic research on the phenomenon. Such a meeting was held ~n Lagos, Portugal, from 18 to 29 May 1981. The purpose of the Institute was to present and discuss in a didatic and systematic way the various processes that lead to cata lyst deactivation, namely coking, poisoning and solid state trans formations, and at the same time to promote the exchange of ideas and experiences among the participants, drawn from industry and uni versity. The lectures presented at the Institute are collected in this volume with the exception of Dr. L.L.Hegedus "Catalyst Poisoning", which has been previously published (Catalysis Reviews, Science md Engineering, 23, 377-476, 1981). The material is arranged in five sections. The introduction contains an overview together with a summary of experimental tests used to assess catalyst deactivation. The next three sections treat in turn catalyst deactivation by coking, poisoning and solid state transformations. For each of these topics, the presentation ranges from the fundamental aspects to their practical consequences. The VI deactivation and regeneration of reforming catalysts was chosen for the final section as an example of the interaction of various de activation processes, and emphasizes the links between fundamental research and industrial practice. All the lectures are to be thanked for their clear presenta tions and written contributions. I am particularly indebted to Pro fessors G.F.Froment and D.L.Trimm, whose advice was invaluable in establishing the scientific contents of the course, and to Profes sor B.Delmon, who coordinated the section on solid state transfor mations. I am also most grateful for the advice of my colleague Prof. A.E.Rodrigues, for the collaboration of Dr. C.A.Bernardo and Mrs. M.C.A.Ferraz at various stages in the organization and, in particu lar,for the dedication of the Institute's secretary Maria Idalina~ The financial support of the NATO Advanced Study Institutes Programme made this course possible. The participants made it all worthwhile. VII NATO ADVANCED STUDY INSTITUTE "CATALYST DEACTIVATION" Organizing Committee Director: J.L.Figueiredo Scientific Advisors: G.F.Froment, D.L.Trimm Local Committee: C.A.Bernardo, M.C.A.Ferraz, F.Freire Secretary: Maria Idalina Lecturers Prof. J.B.Butt, Northwestern University, USA Prof. B.Delmon, Universite Catholique de Louvain, Belgium Prof. D.A.Dowden, Imperial College, London, UK Prof. J.L.Figueiredo, Universidade do Porto, Portugal Dr. J.-P.Franck, Institut Fran~ais du Petrole, France Prof. G.F.Froment, Rijksuniversiteit, Gent, Belgium Dr. L.L.Hegedus, W.R.Grace & Co., USA Dr. L.D.Rollmann, Mobil Research & Development Corporation, USA Dr. J.R.Rostrup-Nielsen, Haldor Tops~e A/S, Denmark Prof. D.L.Trimm, University of New South Wales, Australia Prof. S.E.Wanke, University of Alberta, Canada IX TABLE OF CONTENTS Part I. Introduction D.L. Trimm Introduction to catalyst deactivation 3 D.L. Trimm Experimental assessment of catalyst deactivation 23 Part II. Coking D.L. Trimm Coke formation in the gas phase and on surfaces 31 J.L. Figueiredo Carbon formation and gasification on nickel 45 D.L. Trimm Carbon formation on metals other than nickel and on alloys 65 L.D. Rollmann, D.E. Walsh Constraints on carbon formation in zeolite catalysts 81 J.G. Goodwin, Jr., D.G. Blackmond, J.E. Lester Application of Fourier transform infrared spectroscopy to studies of coke formation on cracking catalysts 93 G.F. Froment A rigorous formulation of the effect of coke formation on catalyst activity 103 J.R. Rostrup-Nielsen Criteria for carbon formation (steam reforming and methanationl 127 Part III. Poisoning J.B. Butt Catalyst poisoning and chemical process dynamics 153 J.R. Rostrup-Nielsen Sulfur poisoning (steam reforming and methanationl 209 x Part IV. Solid state transformations B. Delmon, P. Grange The role of chemical transformations of solids in ageing and deactivation of catalysts 231 D.A. Dowden The catalytic effects of water and halogens on the alteration of catalyst surfaces 281 S.E. Wanke Sintering of commercial supported platinum group metal catalysts 315 S.E. Wanke, C. Bolivar Sintering studies using model supported metal catalysts 329 S.E. Wanke Models for the sintering of supported metal catalysts 341 Part V. Industrial example J.-P. Franck, G. Martino Deactivation and regeneration of catalytic-reforming catalysts 355 List of participants and lecturers 399 Part I INTRODUCTION
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