The Physics and Chemistry of Aqueous Ionic Solutions

NATO ASI Series Advanced Science Institutes Series

A series presenting the results of activities sponsored by the NATO Science Committee, which aims at the dissemination of advanced scientific and technological knowledge, witha view to strengthening links between scientific communities.

The series is published by an international board of publishers in conjunction with the NATO Scientific Affairs Division

A Life Sciences Plenum Publishing Corporation B Physics London and New York

C Mathematical D. Reidel Publishing Company and Physical Sciences Dordrecht, Boston, Lancaster and Tokyo

D Behavioural and Social Sciences Martinus Nijhoff Publishers E Engineering and Dordrecht, Boston and Lancaster

Materials Sciences

F Computer and Systems Sciences Springer-Verlag G Ecological Sciences Berlin, Heidelberg, New York, London, H Cell Biology Paris, and Tokyo

Series C: Mathematical and Physical Sciences Vol. 205

NATO ASI Series Advanced Science Institutes Series

A series presenting the results of activities sponsored by the NATO Science Committee, which aims at the dissemination of advanced scientific and technological knowledge, witha view to strengthening links between scientific communities.

The series is published by an international board of publishers in conjunction with the NATO Scientific Affairs Division

A Life Sciences Plenum Publishing Corporation B Physics London and New York

C Mathematical D. Reidel Publishing Company and Physical Sciences Dordrecht, Boston, Lancaster and Tokyo

D Behavioural and Social Sciences Martinus Nijhoff Publishers E Engineering and Dordrecht, Boston and Lancaster

Materials Sciences

F Computer and Systems Sciences Springer-Verlag G Ecological Sciences Berlin, Heidelberg, New York, London, H Cell Biology Paris, and Tokyo

Series C: Mathematical and Physical Sciences Vol. 205

The Physics and Chemistry of Aqueous Ionic Solutions

edited by

M.-C. Bellissent-Funel Laboratoire Leon Brillouin (CEA-CNRS), Centre d'Etudes Nucleaires de Saclay, France

and

G. W. Neilson H. H. Witts Physics Laboratory, University of Bristol, U.K.

D. Reidel Publishing Company

Dordrecht / Boston / Lancaster / Tokyo

Published in cooperation with NATO Scientific Affairs Division

Proceedings of the NATO Advanced Study Institute on The Physics and Chemistry of Aqueous Ionic Solutions Cargese, Corsica (France) June 22-July 5, 1986

Library of Congress Cataloging in Publication Data NATO Advanced Study Institute on the Physics and Chemistry of Aqueous Ionic Solutions

(1986: Cargese, Corsica) The physics and chemistry of aqueous ionic solutions.

(NATO ASI series. Series C, Mathematical and physical sciences; vol. 205) "Proceedings of the NATO Advanced Study Institute on the Physics and Chemistry of

Aqueous Ionic Solutions, Cargese, Corsica (France), June 22-July 5, 1986"- CIP t.p. verso. 1. Ionic solutions-Congresses. I. Bellissent-Funel, M.-C. (Marie-Claire), 1943-

II. Neilson, G. W. III. North Atlantic Treaty Organization. Scientific Affairs Division. IV. Title. V. Series: NATO ASI series. Series C, Mathematical and physical sciences; vol. 205. QD543:N38 1986 541.3'422 87-12722 ISBN-13: 978-94-010-8236-5 e-ISBN-13: 978-94-009-3911-0

001: 10.1007/978-94-009-3911-0

Published by D. Reidel Publishing Company p.o. Box 17, 3300 AA Dordrecht. Holland

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In all other countries, sold and distributed by Kluwer Academic Publishers Group, P.O. Box 322, 3300 AH Dordrecht, Holland

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All Rights Reserved © 1987 by D. Reidel Publishing Company, Dordrecht, Holland.

Softcover reprint of the hardcover 1 st edition 1987 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 photocopying, recording or by any information storage and retrieval system, without written permission from the copyright owner.

TABLE OF CONTENTS

List of participants ••••••••••••••••••••••••••••••••••••••••••••• vii

Photograph ••••••••••••••••••••••••••••••••••••••••••••••••••••••• xi i

Preface and Acknowledgements .....................................• xv

J.P. Hansen Basic Statistical Theory of Liquids .•............................... l

H.L. Friedman Theory af Ionic Solutions at Equilibrium .........•................. 61

J.B. Hubbard Non-Equilibrium Theories of Electrolyte Solutions .................. 95

J.E. Enderby Diffraction Studies of Aqueous Ionic Solutions ................•... 129

A.J. Dianoux Neutron and NMR Spectroscopy of Aqueous Ionic Solutions ...•....... 147

P.A. Madden Light Scattering and Related Topics ...............•............... 18l

P. Bopp Molecular Dynamics Simulations of Aqueous Ionic Solutions •........ 2l7

M.P. Tosi, P. Ballone and G. Pastore Structural Models of the Electrode/Electrolyte Interface .......... 245

R. Parsons Electrode/Electrolyte Interfaces Experimental Results ........... 255

J.-M. Victor Basic Theory of Polyelectrolytes •.......•.......•.........•....... 29l

G. Jannink Experiments on Polyelectrolyte Solutions •......................•.. 3ll

E.U. Franck Supercritical Studies ......••................••.....•............. 337

VI TABLE OF CONTENTS

P. Chieux The Study of Aqueous Ionic Glasses ......... , ...................... 359

G. ~lichard Natural Aqueous Solutions in the Earth ............................ 379

D. Levesque Theoretical Calculations of Ionic Solutions ....................... 399

P. Turq Computer Simulation of Electrolyte Solutions ...................... 409

D. Ande1man, F. Brochard and J.F. Joanny Structured Monolayers of Charged and Polar Molecules at the Liquid/Air Interface ..............•......................•.•...... 417

C. Monnin and J. Schott Chemical Equilibrium Between Minerals and Natural Waters .......... 429

J.Klinger Solid Aqueous Solutions ........................................... 441

J. Dupuy, A. E1arby-Aouizerat, P. Claudy, J.-F. Jal, J.M. Letoffe and P. Chieux Vitrification and Crystallization of Water ....................... 447

Posters ............. ......................•.......•....•.••.•..• .. 453 Postscript and Summary ............................•..•.........••• 457 Sub ject Index .....................•............•..•....••..•...... 461 Formula and Compound Index .....••••.••..••••.•....•........•...•.. 47l

LIST OF PARTICIPANTS

BELLISSENT-FUNEL Marie-Claire Laboratoire Leon Bri lIouin, C EN-Saclay 91191 Gif-sur-Yvette Cedex, France

NEILSON George W. H.H. Wills Physics Lab. Univ. of Bristol Tyndall Avenue, BS8 lTL Bristol, U.K.

AKDENIZ Zehra I.T.U. Fen-Edebiyat FakUltesi Maslak-Istanbul, Turkey

AOUIZERAT-ELARBY Anna Dept. Physique des Materiaux, Univ. C laude Bernard, 43 bd du 11 Novembre 1918 69622 Villeurbanne Cedex, France

ANDELMAN David Exxon Research and Eng. Rte 22 East Annandale NJ 08801, U.S.A.

ASHDOWN Steven Dept. of Physical Chemistry, Univ. of Bristol, Cantock's C lose, Bristol, U.K.

AUTHIER Isabelle Lab. Physique Thermique, ESPC I 10 rue Vauquelin, 75231 Paris Cedex 05 France

BARAN Y AI Andras Theoretical Chemistry Lab. Lorand Eotvos, Univ. Muzeum Krt. 6-8, H 1088 Budapest, Hungary

BELLON I Luc Dept. de Physico-Chimie, C EN-Saclay 91191 Gif-sur-Yvette Cedex, France

vii

BENMOUNA Mustapha IN ES Sciences Exactes, Dept. de Physique Tlemcen BP. 119, Algerie

BOPP Philippe Institut fUr Physikalische Chemie, Techn. Hoch., Petersenstrasse 20, D-6100 Darmstadt, F. R.G.

BORG IS Daniel Lab. de Physique Theorique des Liquides, Univ. P. & M. Curie, 4 place Jussieu 75230 Paris Cedex OS, France

BROSETA Daniel Lab. Physico-Chimie Macromoleculaire (CNRS), ESPCI, 10 rue Vauquelin 75231 Paris Cedex OS, France

BULONE Donatella Istituto per Ie Applicazioni Interdisci­plinari della Fisica (C N R), Via Archirafi 36, 90123 Palermo, Italy

C ABAC 0 Maria Isabel Centro Fisica Materia Condensada, 2 avo Prof. Gama Pinto, 1699 Lisboa Codex, Portugal

C AILL OL Jean-Michel Lab. Physique Theorique & Hautes Energies, Bat. 210, Univ. Paris Sud, 91405 Orsay Cedex, France

CAPONETTI Eugenio Istituto Chimica Fisica, Via Archirafi 26,90144 Palermo, Italy

viii

CAUC HETEUX Isabelle College de France, Physique de la Matiere Condensee, 11 place Marcelin­Berthelot, 75231 Paris Cedex 05, France

CHIEUX Pierre Institut Laue-Langevin, 156 X 38042 Grenoble Cedex, France

COLLINS John College of Natural and Agricultural Sci., Univ. of California, Riverside CA 92521-0424, U.S.A.

CUNNINGHAM Daniel Dept. of Chemistry, Univ. of Southampton, Southampton S09 5N H, U.K.

DANG Xuan Dept. of Chemistry, Univ. of Houston, Central Campus, Houston TX 77004, U.S.A.

DELAPLANE Robert Oniversity of Uppsala, Box 531, S-751 21 Uppsala, Sweden

DEL VALLE GONZALES Alejandro Dept. Cristalografia e Mineralogia Univ. de Valladolid, 47011 Valladolid, Spain

DIANOUX Albert Institut Laue-Langevin, 156 X 38042 Grenoble Cedex, France

DUBESSY Jean C REGU, B.P. 23 54501 Vandoeuvre les Nancy Cedex, France

DUPUY Josette Dept. Physique, des Materiaux, Univ. Claude Bernard, 43 bd du 11 Nov. 1918 69622 Villeurbanne Cedex, France

ENDERBY John Institut Laue-Langevin, 156 X 38042 Grenoble Cedex, France

LIST OF PARTICIPANTS

ERIKSSON Anders Uppsala University, Inst. of Chemistry Box 531, S-751 21 Uppsala, Sweden

FINNEY John Birkbeck College, Univ. of London Malet Street, London WC1E 7HX, U.K.

FRANCK Ernst Institute of Physical Chemistry, Univ. of Karlsruhe, 12 Kaiser St. D-7500 Karlsruhe, F.R.G.

FRIEDMAN Harold Chemistry Dept. State Univ. of New York, Stony Brook, New York 11794, U.S.A.

GAILLARD Jean-Fran~ois Lab. de Geochimie des Eaux, Univ. Paris VII, 2 place Jussieu, 75251 Paris Cedex 05, France

GOLDMAN Saul Dept. of Chemistry and Biochemistry, Univ. of Guelph, Guelph, Ontario N1G 2W1, Canada

GOMEZ-ESTEVEZ Juan Dept. de Termologia, Fac. de Fisica, Univ. de Barcelona, Diagonal 645, 08028 Barcelona, Spain

GORDON Heather Dept. of Chemistry and Biochemistry Univ. of Guelph, Guelph, Ontario N1G 2W1, Canada

GULLIDGE Philip H.H. Wills Physics Lab., Univ. of Bristol Tyndall Avenue, Bristol BS8 1 TL, U.K.

HANSEN Jean-Pierre Lab. de Physique Theorique des Liquides Univ. Paris VI, 4 place Jussieu 75230 Paris Cedex 05, France

HERDMAN John H.H. Wills Physics Lab., Univ. of Bristol Tyndall Avenue, Bristol BS8 1 TL, U.K.

LIST OF PARTICIPANTS

HERNING Thierry Societe Rousselot, 8 rue Christophe Colomb, 75008 Paris, France

HOLMBERG Sven Dept. of Physics, Uppsala Univ., Box 530 S-75121 Uppsala, Sweden

HUBBARD Joseph Thermophysics Division, Bldg 221, Rm A311, US Dept. of Commerce, NBS Gaithersburg MD 20899, U.S.A.

JANNINK Gerard Laboratoire Leon Bri 1I0uin, C EN-Sa clay 91191 Gif-sur-Yvette Cedex, France

KJELLANDER Roland Dept. of Applied Mathematics, Research School of Physical Sciences, Australian National Univ., Canberra ACT 260, Australia

KLINGER JUrgen Lab. de Glaciologie & de Geophysique de I'Environnement du C N RS, B.P. 96 38402 St-Martin-d'Heres Cedex, France

K ORKMAZ Mustafa Hacetteppe Univ., Fac. of Engineering, Dept. of Physics Engineering, Beytepe, Ankara, Turkey

K RISTIANSSON Olof Institut de Chimie, Univ. d'Uppsala Box 531, S-75121 Uppsala, Sweden

LEVESQUE Dominique Lab. de Physique Theorique & Hautes Energies, Bat. 210, Univ. Paris Sud 91405 Orsay Cedex, France

MADDEN Paul Dept. of Physical Chemistry, South Park Road, Oxford OX1 3Q2, U.K.

MATHIEU Cecile Dept. Physique des Materiaux, Univ. C laude Bernard, 43 bd du 11 Nov. 1918 69622 Villeurbanne Cedex, France

MICHARD Gil Lab. de Geochimie des Eaux, Univ. Paris VII, 2 place Jussieu, 75251 Paris Cedex, OS, France

MIDDENDORF Dieter The Clarendon Lab., Univ. of Oxford, Parks Road, Oxford OX1 3PU, U.K.

MOBE RG Robert

IX

Dept. of Physics, Uppsala Univ., Box 530 S-75121 Uppsala, Sweden

MONNIN Christophe Lab. de Mineralogie & Cristallographie 38 rue des 36 Ponts, 31062 Toulouse, France

MONTAGUE Daniel Dept. of Physics, Willamette Univ. Salem, Oregon 97301, U.S.A.

OBERTHUR Radulf Institut Laue-Langevin, 156 X 38042 Grenoble Cedex, France

PARSONS Roger Dept. of Chemistry, Univ. of Bristol, Bristol BS8 lTS, U.K.

PENDER Celia Dept. of Chemistry, Univ. of Southampton, Southampton S09 5 N H, U.K.

PHILIPSE Albert Van't Hoff Lab., Padualaan 8, Utrecht, The Netherlands

PODGORNIK Rudi Institute Jozef Stefan, Jamova 39,

MAO Bingwei 61000 Ljubljana, Yugoslavia Dept. of Chemistry, Univ. of Southampton Southampton, S09 5NH, U.K. REMLER Dahlia

Physical Chemistry Lab., South Parks Road, Oxford OX1 3Q2, U.K.

x

RICHARDSON Charles Physics Dept. Univ. of Arkansas, Fayetteville AR 72701, U.S.A.

ROSI Barbara Dipartimento di Fisica, Univ. di Parma Via d'Azeglio 85, Italy

ROSINBERG Martin Groupe Froment, ESPC I, 10 rue Vauquelin, 75005 Paris, France

RUSSIER Vincent Physique des Liquides & Electrochimie, LP 15 C N RS, 4 place Jussieu 75230 Paris Cedex OS, France

SALMON Philip School of Mathematics & Physics, Univ. of East Anglia, Norwich, NR4 7T J, U.K.

SANDSTROM Magnus Dept. of Inorganic Chemistry, Royal Inst. of Technology, S-10044 Stockholm Sweden

SANTOS LOPES Maria Centro de Electroquimica e cinetica da Univ. de Lisboa, Fac. de Ciencias, rua da Escola Politecnica, 1200 Lisboa, Portugal

SC HAAF Pierre Institut Charles Sadron (C RM-EAHP) 6 rue Boussingault, 67083 Strasbourg France

SCHOSSELER Franc;ois Institut Charles Sadron (C RM-EAH P) 6 rue Boussingault, 67083 Strasbourg France

SIMONIN Jean-Pierre Lab. d'Electrochimie, Bat. F, Univ. P. & M. Curie, 8 rue Cuvier, 75005 Paris, France

SKIPPER Neal H.H. Wills Physics Lab., Univ. of Bristol Tyndall Avenue, Bristol BS8 lTL, U.K.

LIST OF PARTICIPANTS

SPOH REckhard Max Planck Institut fUr Chemie, Postfach 3060, D-6500 Mainz, F.R.G.

SVENSSON Bo Physical Chemistry II, Chemical Center POB 124, S-22100 Lund, Sweden

TANI Alessandro Dipartimento di Chimica, Univ. di Pisa, Via Risorgimento 85, 56100 Pisa, Italy

TIAN Zhong Dept. of Chemistry, Southampton Univ. Southampton S09 5NH, U.K.

TOSI Mario International Center for Theoretical Phys., Dipartimento di Fisica Teorica, Strada Costiera 11, 34100 Trieste, Italy

TUMEO Mark Dept. of Civil Engineering, Univ. of California, 206 Walker Hall, Davis CA 95616, U.S.A.

TURKMAN Aysen Dokuz Eyliil Univ. Muhendislik Mimarlic Fakultesi, Bornova Izmir, Turkey

TURNER Jacky Dept. of Cristallography, Birkbeck Coli. Univ. of London, Malet Street, London WC 1 E 7HX, U.K.

TURQ Pierre Proprietes Physico-Chimiques des Electrolytes Univ. Paris VI, 4 place Jussieu 75230 Paris Cedex OS, France

VAN AKEN George Van't Hoff Lab., Padualaan 8, POB 80051 35008 TB, Utrecht, The Netherlands

VAN DER MAAREL Johan Dept. of Physical and Macromolecular Chemistry, POB 9502, 2300 RA Leiden The Netherlands

LIST OF PARTICIPANTS

VIC TOR Jean-Marc Lab. Physique Theorique des Liquides, Univ. P. & M. Curie, 4 place Jussieu 75230 Paris Cedex OS, France

WALKER Patricia H.H. Wills Physics Lab., Univ. of Bristol Tyndall Avenue, Bristol BS8 1 TL, U.K.

WEIS Jean-Jacques Lab. de Physique Theorique & Hautes Energies, Bat. 210, Univ. Paris Sud, 91405 Orsay Cedex, France

WILGOCKI Michal Institute of Chemistry, Univ. of Wroclaw, F. Joliot Curie 14, 50-383 Wroclaw,Poland

WOODWARD Clifford Physical Chemistry II, Chemical Centre POB 124, S-221 00 Lund, Sweden

XIA Tai-he Institute of Biophysics, Academia Sinica, Beijing, China

XU Hong Service Chimie Physique II, CP 231 ULB Campus Plaine, 1050 Bruxelles Belgique

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PREFACE AND ACKNOWLEDGEMENTS

As stated in 1977 by Professor de Gennes in his closing address to the

participants of a previous NATO ASI on the Microscopic Structure and Dynamics

of Liquids: "my own dream for future ASPs is to see future summer schools

occurring as joint projects: liquid experts and solution chemists, liquid experts

and electron chemists, etc." Taking up this challenge, we organised at Gargese

(Corsica) an ASI in June 1986 which was composed of scientists whose interests

lay within the broad area of aqueous ionic solutions. The aims of the school

were to provide both new and established researchers from physics, chemistry,

biochemistry, electrochemistry and geochemistry with (j) a comprehensive

background to the theory of ionic solutions and (ij) a substantial account of

theoretical and experimental developments which have taken place in the

last decade.

This book contains a written record of the proceedings of our ASI on the

Physics and Chemistry of Aqueous Ionic Solutions. The Institute began with

a series of lectures on the basic statistical mechanical theory of liquids and

ionic solutions. These lectures were interspersed with presentations on the

new and powerful methods of neutron scattering, X-ray diffraction, light

scattering and n.m.r. The role which computer simulation plays in forging

a link between the formal theory and experimental results was discussed in

detail.

During the second half of the school special consideration was given to

how the subject might develop in the next decade. To achieve as broad a

perspective as possible lectures were given in a variety of areas including

ionic solutions under critical conditions, ionic glasses, polyelectrolytes,

electrochemistry, biochemistry and geochemistry. Lecturers were particularly

careful to point out where their work might be of technological significance.

The summer school also benefitted from several seminars on topics of current

interest, and these are presented towards the end of the book. Of particular xv

xvi PREFACE AND ACKNOWLEDGEMENTS

interest were the significant advances being made in the theoretical development

of solutions at interfaces, and dynamics of ions in the bulk.

A poster session was held with the main objective of encouraging younger

participants to present their results. A summary of the contents of this session

is given on page 453.

The ASI was brought to a close by Professors Friedman and Enderby who,

drawing on their wealth of experience, pointed out the many achievements

which have taken place in the past decade and how our view of Ionic Solutions

has been transformed by the combined efforts of theorists and experimentalists.

They invited us to contemplate, how much has still to be done, especially in

understanding complex ionic systems where our know lege of basic properties

is still sparse.

Given the scope of this school it is clear that it could not have been

undertaken without the help of many colleagues. Foremost among these is

Dr. Philip Bopp who greatly. assisted us before, during and after the ASI. His

organisation of the poster session was much appreciated by students and

lecturers alike. The assistance of Drs. Josette Dupuy and Jose Dianoux in helping

us set up the lecturing programme, and in organising an exciting and entertaining

social programme is gratefully acknowledged. •

We thank Mrs M-F. Hanseler and Mrs F. Cheriot for secretarial services

which ensured the smooth running of the school. We also are extremely grateful

to Mrs C. Pomeau for typing and arranging the final manuscript, and to Mrs

Pols-v.d. Heijden of Reidel , who has been instrumental in assembling this

final record of the ASI.

It is a pleasure to thank all lecturers and seminar speakers for presenting

a vivid and enthusiastic account of their work and thereby stimulating many

of us in our own endeavours in future.

Finally and most importantly we thank NATO and the other organisations

including C EA, C N RS, ILL, IC I, NSF (USA), IBM-Deutschland, WELLA-AG

for financial support which enabled us to provide funds for almost all

participants.

M.-C. Bellissent-Funel - Paris

G.W. Neilson - Bristol