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Activity Coefficients

in

Electrolyte Solutions

2nd Edition

Editor

Kenneth S. Pitzer, Ph.D.

Professor

nesEyileri vo Sueltfiy2 drtKeyfti2 vo SEhtovyrtE .eyPehe2z SEhtovyrtES,S Cyeff .vDE ,Eivr Rrr RyFvy .vfivr Nvrcvr

PREFACE

The progress toward a second edition of "Activity Coefficients in Electrolyte Solutions" was well advanced by Dr. R. M. Pytkowicz, the editor of the first edition, when he resigned

in early 1989 for health reasons. After a substantial hiatus, I was asked to take over the

editorship. Most of the chapters and authors remain as were planned by Dr. Pytkowicz, but a few changes in authorship or coauthorship were necessary and one new chapter (8) was added. 1 am responsible for the present organization of the book but am happy to acknowledge

the role of Dr. Pytkowicz.L2 eKEhMEitvr DvrDeyrtrk iue kereyEh fiEie vo PrvHhecke tr iutf otehc Erc iue vssvyT

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Activity Coefficients

in

Electrolyte Solutions

2nd Edition

Editor

Kenneth S. Pitzer, Ph.D.

Professor

nesEyileri vo Sueltfiy2 drtKeyfti2 vo SEhtovyrtE .eyPehe2z SEhtovyrtE

INTRODU CTIO N

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1979. Clegg and Whitfield discuss both the history and current status of these methods in

Section II of Chapter 6. While the title of Chapter 6 is "Activity Coefficients in Natural

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vkyEsu2 tf DheEy oyvl iue yefMhif syeferiec in various chapters, especially in Chapters 6 and

7, The application to aerosols which comprise aqueous electrolytes is less obvious but

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ion that is related to a biological function in many cases.' 16 The ionic strength is rather

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REFERENCES

1 Robinson. R. A. and Stokes. R. H-, Electrolyte Solutions, revised, Butterworths, London. Isled., 1955;

2nd ed.. revised 1965.Om Harned, H. S. and Owen. B. B., The Physical Chemistry of Electrolyte Solutions, Reinhold Publishing.

New York. 1958.(m Milner, S. R., The vtrial of a mixture of ions. Phil Mag., 23. 551, 1912; 25. 742. 1913,)m Debye, P. and Huckel, E., Zur theorie der electrolyte, I and II. Phys. Z . 24. 185 and 305. 1923.I Plummer, L. N., Parkhurst, D. L., Fleming, G. W., and Dunkle, S. A., A computer program incor

porating Pilzer's equations for calculation of geochemical reactions in brines. U S, Geological Survey,

Water-Resources Investigations Report 88-4153, Reston. VA. 1988. Also, see Chapters 3. 6, and 7.6. Barrie, C. E. and Weare, J. H., The predication of mineral solubilities in natural waters: the Na-K-Mg-

Ca-CKS0,-M.,0 system from zero to high concentration at 25°C. Geochim. Cosmochim. Acta. 44. 981,W6J8m

Um Filippov, V. K., Dmitriev, G. V., and Yakovleva, S. 1.. Use of the Purer method for calculating the

activity of componcnls in mixed solutions of electrolytes according to data on solubility, Doki Akad Nuuk.

SSSR, Ft:. Khim.. 252. 156. 1980; Engl, transl.. 252. 359, 1980; and subsequent papers.J Mu. C. and Lindsay, W, T., Jr., Thermodynamics of sodium chloride solutions at high temperatures. J

Solution Chem.. 1,45. 1972.6m Albert}1, R. A., Standard Gibbs free energy, enthalpy, and entropy changes as a function of pH and pMg

for several reactions involving adenosine phosphates. J. BioI Chem . 244 . 3290. 1969.W8m Phillips, R. C., George. P., and Rutman, R. J., Thermodynamic data for the hydrolysis of adenosine

triphosphate as a TuncUon of pH. Mg-' ion concentration, and ionic strength. J Biol Oirm.. 244, 3330.

1969.11 Goldberg. R. N. and Tewari, Y. B., Thermodynamics of the disproportionation of adenosine 5'-dtphos-

phate to adenosine 5'-tnphosphatc and adenosine 5'-monophosphate. Biophys. Chem., 40. 241, 1991.WO Guyrin, R. W., Gelberg, H. J., and Veech, R. L" Equilibrium constants of the malalc dehydrogenase,

citrate synthase, citrate lyase, and acetyl coenzymc A hydrolysis reactions under physiological conditions.

J Biol. Chem.. 248. 6957, 1973.13 Cohen. C. J., Fozzard, H. A., and Sheu, S.-S., Increase in intracellular sodium ion activity during

stimulation in mammalian cardiac muscle. Circ, Bex , 50, 651. 1982.W) Shorofsky, S. R., Field, M., and Fozzard, H. A" Mechanism of Cl secretion in canine trachea; changes

in intracellular chloride activity with secretion, J Membrane Biol., 81,1. 1984.WI Biber, T. U. I... Drewnowska, K., Baumgarten. C. M.. and Fisher, R. S" Intracellular Cl activity

changes of frog skin. Am. J Physiol., 249. F432. 1985.W;m Gambalc. F., Menini, A., and Rauch, G " Effects of calcium on the gramicidin A single channel in

phosphatidvlserine membranes. Eur. Biophys. J , 14. 369. 1987.17 Kitic, D., Pallia. M. L" Favetto, G. J., and Oiirife, J., Mixed saturated salt solutions as standards for

w ater activity measurements in the microbiological growth range. J. FaodSci.. 53, 578. 1988, and preceding

articles there citedWJ .EMlkEyierz Sm Lmz R syvkyEl ovy DEhDMhEitvr vo EDitKti2 DveootDterif Ei feheDiec DvrDeriyEitvrf Erc

ielseyEiMyefz Comput. Biol. Med., II. 189, 1981.

THE EDITOR

Kenneth S. Pitzer was bom in Pomona, California in 1914. He received his B.S. degree from the California Institute of Technology in 1935, his Ph.D. from the University of California, Berkeley in 1937, a D.Sc. from Wesleyan University in 1962, and an LL.D. from the University of California in 1963 and from Mills College in 1969. He was a member of the faculty at Berkeley from 1937 to 1960, serving also as Dean of the College of Chemistry from 1951 to 1960. On leave from the University of California, he was Technical Director of the Maryland Research Laboratory, a World War II entity from 1943 to 1944, and was Director of Research for the U.S. Atomic Energy Commission from 1949 to 1951. In 1961, he became President and Professor of Chemistry at Rice University, serving until 1968 when he became President of Stanford University until 1970. In 1971 he returned to the University of California, Berkeley, as Professor until 1984 and thereafter as Professor Emeritus but

was recalled for continued service.His advisory committee and other part-time service included the General Advisory

Committee to the AEC, 1958 to 1965 (Chairman 1960 to 1962); President's Science Advisory Committee, 1965 to 1968; Commission on Chemical Thermodynamics of the International Union of Pure and Applied Chemistry, 1953 to 1961; NASA Science and Technology Advisory Committee, 1964 to 1965; Trustee, Harvey Mudd College, 1956 to 1961, Mills College, 1958 to 1961, Pitzer College 1966 to the present, Rand Corporation, 1962 to 1972; Member of the Board of Directors, Owens Illinois, Inc., 1967 to 1986; Federal Reserve Bank of Dallas, 1965 to 1968, the American Council on Education, 1967 to 1971; and Member of the Council of the National Academy of Sciences, 1964 to 1967 and 1973 to

1976.His research has extended through many areas of physical chemistry and into topics of

importance including inorganic and organic chemistry, chemical engineering, and geochem istry. In addition to work on aqueous electrolytes reflected in this volume, his research has included quantum theory and statistical mechanics as applied to chemical problems ranging from the potential restricting rotation about single bonds, to the bonding in polyatomic carbon molecules, and to the effects of relativity on chemical bonds involving very heavy atoms. In addition to many journal articles and several book chapters, his books include Quantum Chemistry, 1953; Selected Values of Physical and Chemical Properties of Hydro carbons and Related Compounds, with F. D. Rossini and others, 1947, 2nd edition, 1953;

Thermodynamics, 2nd edition with L. Brewer, 1961, and a revision of the 1st edition ofG. N. Lewis and M. Randall.

His honors and awards include the National Medal of Science, 1975, the Robert A. Welch Award in Chemistry, 1984, the Alumnus of the Year Award, University of California, Berkeley, 1951, and the Alumni Distinguished Service Award, California Institute of Tech nology, 1966. From the American Chemical Society he received the Award in Pure Chem istry, 1943, in Petroleum Chemistry, 1949, the Gilbert Newton Lewis Medal, 1965, the Priestley Medal, 1969, and the Willard Gibbs Medal, 1976. Other recognitions include many special lectureships, a Guggenheim Fellowship, 1951, and election to the National Academy of Sciences in 1949.

CONTRIBUTORS

James N. Butler, Ph.D.

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TABLE OF CONTENTS

Chapter 1

Thermodynamics of Solutions............................................................................................ 1R. H. Stokes

Chapter 2

Introduction to the Statistical Mechanics of Solutions .......29Robert M. Mazo and Chung Yuan Moil

Chapter 3

Ion Interaction Approach: Theory and Data Correlation .............................75Kenneth S. Pitzer

Chapter 4

Experimental Methods: Potentiometric

.........................................................................155James N. Butler and Rabindra N. Roy

Chapter 5

Experimental Methods; Isopiestic........................................................................ ,209

Joseph A. Rard and Robert F. Platford

Chapter 6

Activity Coefficients in Natural Waters

quotesdbs_dbs48.pdfusesText_48

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