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CHEMICAL THERMODYNAMICS

OF URANIUM

Ingmar GRENTHE (Chairman)

Royal Institute of Technology

Stockholm (Sweden)

Jean FUGER

Commission of the European Communities, JRC

European Institute for Transuranium Elements

Karlsruhe (Federal Republic of Germany)

Rudy J.M. KONINGS

Netherlands Energy Research Foundation ECN

Petten (The Netherlands)

Robert J. LEMIRE

AECL Research, Whiteshell Laboratories

Pinawa, Manitoba (Canada)

Anthony B. MULLER

Science Applications International Corporation

McLean, Virginia (USA)

Chinh NGUYEN-TRUNG

CREGU

Vandœuvre-l`es-Nancy (France)

Hans WANNER

OECD Nuclear Energy Agency, Data Bank

Issy-les-Moulineaux (France)

Edited by

Hans WANNER and Isabelle FOREST

OECD Nuclear Energy Agency, Data Bank

Issy-les-Moulineaux (France)

NUCLEAR ENERGY AGENCY

ORGANISATION FOR ECONOMIC CO-OPERATION AND DEVELOPMENT ORGANISATION FOR ECONOMIC CO-OPERATION AND DEVELOPMENT

Pursuant to Article 1 of the Convention signed in Paris on 14th December 1960, and which came into force

on 30th September 1961, the Organisation for Economic Co-operation and Development (OECD) shall promote

policies designed:

to achieve the highest sustainable economic growth and employment and a rising standard of living in

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Zealand (29th May 1973), Mexico (18th May 1994), the Czech Republic (21st December 1995), Hungary (7th May

1996), Poland (22nd November 1996), Korea (12th December 1996) and the Slovak Republic (14 December 2000).

The Commission of the European Communities takes part in the work of the OECD (Article 13 of the OECD

Convention).

NUCLEAR ENERGY AGENCY

The OECD Nuclear Energy Agency (NEA) was established on 1st February 1958 under the name of the

OEEC European Nuclear Energy Agency. It received its present designation on 20th April 1972, when Japan became

its first non-European full member. NEA membership today consists of 28 OECD member countries: Australia,

Austria, Belgium, Canada, the Czech Republic, Denmark, Finland, France, Germany, Greece, Hungary, Iceland,

Ireland, Italy, Japan, Luxembourg, Mexico, the Netherlands, Norway, Portugal, the Republic of Korea, the Slovak

Republic, Spain, Sweden, Switzerland, Turkey, the United Kingdom and the United States. The Commission of the

European Communities also takes part in the work of the Agency.

The mission of the NEA is:

to assist its member countries in maintaining and further developing, through international co-

operation, the scientific, technological and legal bases required for a safe, environmentally friendly and

economical use of nuclear energy for peaceful purposes, as well as to provide authoritative assessments and to forge common understandings on key issues, as input to government decisions on nuclear energy policy and to broader OECD policy analyses in areas such as energy and sustainable development.

Specific areas of competence of the NEA include safety and regulation of nuclear activities, radioactive

waste management, radiological protection, nuclear science, economic and technical analyses of the nuclear fuel cycle,

nuclear law and liability, and public information. The NEA Data Bank provides nuclear data and computer program

services for participating countries.

In these and related tasks, the NEA works in close collaboration with the International Atomic Energy

Agency in Vienna, with which it has a Co-operation Agreement, as well as with other international organisations in the

nuclear field.

OECD 2004

Permission to reproduce a portion of this work for non-commercial purposes or classroom use should be obtained through the Centre

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OECD Publications, 2, rue André-Pascal, 75775 Paris Cedex 16, France. iii

Preface to the 2004 reprint

Chemical Thermodynamics of Uranium is the first book in a series of monographs providing a critical review of the thermodynamic properties of the actinide elements and their compounds; it was followed by monographs on neptunium, plutonium, americium and technetium and their compounds. Other monographs dealing with selenium, nickel and actinide complexes with organic ligands are in preparation. Chemical Thermodynamics of Uranium was published in 1992 and an update that also contains new thermodynamic data for neptunium, plutonium and americium is due to be published in 2003. The characteristic feature of this series is the extensive discussions of experimental data obtained from the original publications and reports. In some cases the review teams have reinterpreted the original data, which have also been recalculated to zero ionic strength using the specific ion interaction method. The methodology used for activity factor corrections and statistical analysis is described in the appendices. The detailed discussion of the experimental data allows the user to follow the reasoning behind the selection and thus agree or disagree with the thermodynamic values selected. Why the need for a reprint of the first volume? The answer is simple - the first edition is sold out. However, there are other reasons, too. The most important is that the 2003 Update only contains discussions of the thermodynamic data that has been published since the cut-off date for the original 1992 edition. When the new literature has not led to an update of the selected values, the 1992 edition still provides the detailed discussions leading to the retained selections. This volume is an identical reprint of the first edition. It contains some errors and other mistakes that have been corrected in the 2003 Update. I was gratified, as were the other members of the first uranium team, that the new experimental data reported in the 2003 Update have resulted in few major changes in the thermodynamic data and in the chemical models used to describe the complex formation with different ligands. Our quantitative understanding of the chemistry of uranium in the form of thermodynamic data is with some exceptions good, and should provide a sound basis for applications. However, there are still some areas where additional experimental data are needed as discussed in the 2003 Update. On behalf of the review team I would like to thank the readers that have pointed out errors in the first edition. These have been corrected in the 2003 Update, but not in this reprint.

Ingmar Grenthe

Stockholm, 5 May 2003

iv

Editor"s note to the 2004 reprint

The present volume is a reprint of the 1992 edition of Chemical Thermodynamics of Uranium by Ingmar Grenthe, Jean Fuger, Rudy J. M. Konings, Robert J. Lemire, Anthony B. Muller, Chinh Nguyen-Trung and Hans Wanner. The book was edited at the NEA Data Bank by Hans Wanner and Isabelle Forest and published by Elsevier under the North-Holland imprint. As part of Phase II of the NEA Thermochemical Database Project (TDB), a new publication entitled Update on the Chemical Thermodynamics of Uranium, Neptunium, Plutonium, Americium and Technetium and authored by Robert A. Palmer and Malcolm H. Rand, was published by Elsevier in 2003. For uranium, this Update contains a review of the literature published since the cut-off date for the literature reviewed in the 1992 edition cited above. As a consequence of this new TDB Review, some of the values selected in the earlier publication have been superseded while others have retained their validity. The 2003 Update is self- contained with respect to any new data selections but the discussions leading to the retained selections can in most cases only be found in the 1992 publication. Since the latter is no longer available from its original publisher, the NEA is making the present reprint available to the scientific community. Consequently, it is important to note that the Tables of Selected Values contained in this reprint ARE OUTDATED AND

SHOULD NOT

())*Update. This reprint has been prepared at the NEA Data Bank by Federico Mompean, Myriam Illemassene and Jane Perrone by reprocessing the files employed in the production of the 1992 edition. Every effort has been made to preserve the original layout and page numbering. We are grateful to the many readers who have provided feedback and pointed out errors in the 1992 book. In particular, Dr. Lionel Bion and Dr. Pierre Vitorge from the Commissariat à l"Énergie Atomique (France) identified an error in Figure V.19, page 325, due to the interchange of the labels for the species U(OH) 4 (aq) and UO 2 CO 3 (aq). In an attempt to make this reprint as close a reproduction of the original publication as possible, we have not implemented any corrections. v

Preface

This is the first volume in a series of critical reviews of the chemical thermodynam- ics of those elements that are of particular importance in the safety assessment of radioactive waste disposal systems. The NEA Thermochemical Data Base (TDB) project was begun seven years ago by the OECD Nuclear Energy Agency (NEA) as a result of discussions that had taken place during radioactive waste management conferences held in the United States and France. Anthony Muller initiated the project and, at first, he coordinated it at the NEA; in 1986 he was succeeded by

Hans Wanner.

In late 1986, two years after the preliminary talks, a meeting was held at which the first drafts of some of the sections in this volume were discussed. This resulted in some major revisions, updates, and also improved documentation of the evaluation and selection procedures. Since then the review team has met twice for extensive discussions. This volume is a collective effort: each participant contributed sections correspond- ing to his area of expertise. Robert Lemire has drafted the sections on the oxide and hydroxide compounds and complexes, the uranium nitrides, the solid uranium ni- trates and the arsenic-containing uranium compounds, and he has contributed to the sections on uranates in the final stage. He has also written Appendix D and established the procedures used for consistent estimation of entropies. The sections on gaseous and solid uranium halides were originally drafted by Anthony Muller, then commented upon by Jean Fuger, and finally thoroughly revised and extended by Rudy Konings, who joined the review team in 1990, and who has also drafted the section on gaseous uranium oxides and contributed to the sections on uranates in the final stage. Chinh Nguyen-Trung, who joined the review team in 1988, has con- tributed to the section on solid phosphorus-containing uranium compounds and the one on alkali metal uranates. Hans Wanner has developed the procedures, drafted the sections on uncertainties and on standards and conventions, and has verified and checked the consistency of data submitted by the project participants. My con- tribution consists of the sections on aqueous complexes (including Section V.2 but excluding the hydroxide complexes) and the parts of the sections on uranium miner- als that deal with solubility products. Hans Wanner and I drafted Appendix B on ionic strength corrections. Hans Wanner has been responsible for editing this volume. He was assisted by his colleagues from the NEA Data Bank: Isabelle Muller (formerly Poirot), succeeded by Isabelle Forest in 1989; Mikazu Yui, succeeded by Kaname Miyahara in 1990; and vi Pierre Nagel, who has developed the computerized data base system. I would also like to acknowledge contributions made by Donald Langmuir who participated in our first meeting. Unfortunately, because of insufficient funding, he was unable to take part in subsequent activities. The project has taken a long time to complete, partly because of lack of proper funding in its initial stages. I am grateful to the NEA Radioactive Waste Management Committee for its assistance in recent years in seeking this financial support. The efforts by Mr. Jean-Pierre Olivier, Head of the NEA Division for Radiation Protection and Radioactive Waste Management, to establish the TDB project at the NEA, are acknowledged. Dr. Kunihiko Uematsu, Director General of the NEA, has been instrumental in bringing this project to its successful conclusion. Mr. Johnny Ros´en, Head of the NEA Data Bank, has always been a source of support and encouragement. On behalf of the review team, I want to thank not only those named above, but also all the colleagues and co-workers who have helped us complete our task.

Stockholm, November 1991 Ingmar Grenthe, Chairman

vii

Acknowledgments

I. Grenthe thanks the Swedish Nuclear Fuel and Waste Management Company (SKB) for financial support. R.J. Lemire"s participation in this project was jointly funded by AECL Research and Ontario Hydro under the auspices of the CANDU Owners Group. He also wishes to express appreciation to P. Taylor and J. Paquette for helpful discussions, and to N.D. Haworth for assistance with the literature searches. C. Nguyen-Trung"s participation in this project was funded by CREGU. He wishes to thank R.E. Mesmer, D.A. Palmer and C.F. Baes, Jr., for helpful discussions and logistic support while he was at the Oak Ridge National Laboratory. H. Wanner wishes to thank Nathalie Cramer for entering thousands of data into the computerized data base, as well as S´everine Girod and Lionel Morel for their help in formatting and editing the text. The following eight independent experts have reviewed the contents of the present book according to the peer review procedures [90WAN2] prepared for this purpose in the framework of the NEA Thermochemical Data Base project. They have viewed and approved the modifications made by the authors according to their comments. The peer review comment records may be obtained on request from the OECD Nuclear

Energy Agency.

Prof. S. Ahrland University of Lund, Lund, Sweden

Dr. C.F. Baes, Jr. Oak Ridge National Laboratory, Oak Ridge,

Tennessee, USA (Retired)

Prof. L. Ciavatta University of Naples, Naples, Italy Prof. E.H.P. Cordfunke Netherlands Energy Research Foundation ECN,

Petten, The Netherlands

Prof. F.P. Glasser University of Aberdeen, Aberdeen, United Kingdom Prof. F. Grønvold University of Oslo, Oslo, Norway Dr. D.L. Hildenbrand SRI International, Menlo Park, California, USA Dr. F.J. Pearson, Jr. Ground-Water Geochemistry, Irving, Texas, USA We are grateful to I. Puigdomenech (Studsvik AB, Nykoeping, Sweden) for the production of the distribution and predominance diagrams,i.e., Figures V.4, V.5,

V.6, V.7, V.8, V.17, V.18, V.19, V.20.

In addition, we thank the following for their technical comments and suggestions in the course of the project: P.L. Brown, Australian Nuclear Science and Technology viii Organization, Lucas Heights, New South Wales, Australia; M.W. Chase, National In- stitute of Standards and Technology, Gaithersburg, Maryland, USA; K. Czyscinski, Roy F. Weston Inc., Washington, D.C., USA; D. Garvin, National Institute of Stan- dards and Technology, Gaithersburg, Maryland, USA; I. Khodakovsky, Vernadsky Institute, USSR Academy of Sciences, Moscow, USSR; O. Kubaschewski, Aachen, Germany; L. Maya, Oak Ridge National Laboratory, Oak Ridge, Tennessee, USA; L.R. Morss, Argonne National Laboratory, Argonne, Illinois, USA; T.W. Newton, Los Alamos National Laboratory, Los Alamos, New Mexico, USA; D.K. Nordstrom, US Geological Survey, Menlo Park, California, USA; V.B. Parker, National Institute of Standards and Technology, Gaithersburg, Maryland, USA; S.L. Phillips, Lawrence Berkeley Laboratory, Berkeley, California, USA; M.H. Rand, Harwell Laboratory, Didcot, United Kingdom; J.A. Rard, Lawrence Livermore National Laboratory, Liv- ermore, California, USA; W.J. Ullman, University of Delaware, Lewes, Delaware, USA; P. Vitorge, Commissariat `a l"Energie Atomique, Fontenay-aux-Roses, France; E.F. Westrum, Jr., University of Michigan, Ann Arbor, Michigan, USA; We are indebted to the following for permission to reproduce copyright material: American Institute of Physics and the authors for Figure II.1 (from D.D. Wagman et al. [82WAG/EVA]), and John Wiley & Sons, Inc., for Table II.5 (from C.J. Baes,

Jr., and R.E. Mesmer [76BAE/MES]).

Paris, January 1992 The Editors

ix

Foreword

The present volume starts a series of detailed expert reviews of the chemical ther- modynamics of key elements in nuclear technology and waste management. Volumes on americium, technetium, neptunium and plutonium are currently in progress. The recommended thermodynamic data are the result of a critical assessment of published information. The data network developed at the Data Bank of the OECD Nuclear Energy Agency (NEA),cf. Section I.4, ensures consistency not only within the rec- ommended data set on uranium but also among all the data sets to be published in the series. The NEA Data Bank provides a number of services that may be useful to the reader of this book. •The recommended data can be obtained on eletronic media (PC diskettes, mag- netic tape, or via computer networks) directly from the NEA Data Bank. The special formatting of the data allows easy conversion to any specific formats convenient to the user. •The NEA Data Bank maintains a library of tested computer programs in various areas. This includes geochemical codes such as PHREEQE, EQ3/6, MINEQL, MINTEQ, PHRQPITZ,etc., in which chemical thermodynamic data like those presented in this book are required as the basic input data. These computer codes can be obtained on request from the NEA Data Bank. •Short courses on the use of geochemical codes and thermodynamic data have been organized at the NEA Data Bank since 1985, tought by the authors of the codes PHREEQE, MINEQL and EQ3/6. It is planned to give further courses on the codes mentioned above or on new ones, corresponding to the interest expressed by the user"s community. Persons interested in further courses are advised to contact the NEA Data Bank. For requests of data, computer programs, on-line access, and for further informa- tion, please write to:

OECD Nuclear Energy Agency

Data Bank

Le Seine St. Germain

2-12, Rue Jean-Pierre Timbaud

F-92130 Issy-les-Moulineaux

France

xi

Contents

IIntroduction1

I.1 Background......................................................................................................1

I.2 Focus on the review..........................................................................................2

I.3 Review Procedure and results...........................................................................3

I.4 The NEA-TBD system......................................................................................4

I.5 Presentation of the selected data......................................................................6

IIStandards and Conventions9

II.1 Symbols, terminology and nomenclature...........................................................9

II.1.1 Abbreviations........................................................................................9

II.1.2 Symbols and terminology.......................................................................9

II.1.3 Chemical formulae and nomenclature...................................................9

II.1.4 Phase designators................................................................................13

II.1.5 Processes.............................................................................................14

II.1.6 Equilibrium constants.........................................................................14

II.1.7Order of formulae................................................................................20

II.1.8 Reference codes...................................................................................20

II.2 Units and conversion factors...........................................................................22

II.3 Standard and reference conditions..................................................................24

II.3.1 Standard state.....................................................................................24

II.3.2 Standard state pressure......................................................................24

II.3.3 Reference temperature........................................................................28

II.4 Fundamental physical constants.....................................................................28

IIISelected uranium data29

IVSelected auxiliary data63

VDiscussion of data selection85

V.1 Elemental uranium........................................................................................85

V.1.1 Uranium metal....................................................................................85

V.1.2 Uranium gas.......................................................................................86

V.2 Simple uranium aqua ions..............................................................................86

V.2.1 UO

V.2.2 UO

V.2.3 U

4+

V.2.4 U

3+

V.2.5 U

2+ V.3 Oxygen and hydrogen compounds and complexes............................................97 V.3.1Gaseous uranium oxides......................................................................97 V.3.2 Aqueous uranium hydroxide complexes...............................................98 V.3.3 Crystaline and amorphous uranium oxides and hydroxides...............131

CONTENTSxii

V.3.4 Uranium hydrides.............................................................................148

V.4 Group 17 (halogen) compounds and complexes..............................................150 V.4.1 Fluorine compounds and complexes...................................................150 V.4.2 Chlorine compounds and complexes...................................................185 V.4.3 Bromine compounds and complexes...................................................213 V.4.4 Iodine compounds and complexes......................................................226 V.4.5 Mixed halogen compounds.................................................................232 V.5 Group 16 (chalcogen) compounds and complexes...........................................236 V.5.1 Sulphur compounds and complexes...................................................236 V.5.2 Selenium compounds and complexes.................................................256 V.5.3 Tellurium compounds........................................................................260 V.6 Group 15 compounds and complexes.............................................................261 V.6.1 Nitrogen compounds and complexes..................................................261 V.6.2 Phosphorus compounds and complexes..............................................279

V.6.3Arsenic compounds............................................................................301

V.6.4 Antimony compounds........................................................................304 V.7 Group 14 compounds and complexes.............................................................306 V.7.1 Carbon compounds and complexes.....................................................306 V.7.2 Silicon compounds and complexes......................................................334

V.7.3 Lead compounds................................................................................336

V.8 Actinide complexes.......................................................................................336

V.8.1 Actinide-actinide interactions............................................................336 V.8.2 Mixed U(VI), Np(VI) and Pu (VI) carbonate complexes......................337

V.9 Group 2 (alkaline earth) compounds.............................................................337

V.9.1 Beryllium compounds........................................................................337 V.9.2 Magnesium compounds.....................................................................338

V.9.3 Calcium compounds...........................................................................340

V.9.4 Strontium compounds........................................................................342

V.9.5 Barium compounds............................................................................345

V.10 Group 1 (alkali) compounds..........................................................................347

V.10.1 Lithium compounds...........................................................................347

V.10.2 Sodium compounds............................................................................349

V.10.3 Potassium compounds.......................................................................358 V.10.4 Rubidium compounds........................................................................359

V.10.5 Caesium compounds..........................................................................360

VIDiscussion of auxiliary data selection365

VI.1 Group 17 (halogen) auxiliary species.............................................................366

VI.1.1 Fluorine auxiliary species..................................................................366

VI.1.2 Chlorine auxiliary species..................................................................368

VI.1.3 Bromine auxiliary species..................................................................371

VI.1.4 Iodine auxiliary species.....................................................................373

VI.2 Group 16 (chalcogen) auxiliary species..........................................................374

VI.2.1 Sulphur auxiliary species..................................................................374

VI.2.2 Selenium auxiliary species................................................................380

VI.2.3 Tellurium..........................................................................................383

VI.3 Group15 auxiliary species.............................................................................384

VI.3.1 Nitrogen auxiliary species.................................................................384

VI.3.2 Phosphorus auxiliary species.............................................................386

VI.3.3 Arsenic auxiliary species...................................................................389

VI.3.4 Antimony..........................................................................................391

VI.4 Group 14 auxiliary species............................................................................392

VI.4.1 Carbon auxiliary species....................................................................392

VI.4.2 Silicon auxiliary species.....................................................................394

CONTENTSxiii

VI.5 Other auxiliary species.................................................................................400

VI.5.1Strontium auxiliary species...............................................................400

VI.5.2 Barium auxiliary species...................................................................400

VIIReference list403

VIIIAuthors list485

IXFormula list519

XAlphabetical name list549

XIAppendix A: Discussion of publications555

XIIAppendix B: Ionic strength corrections683

B.1 The specific ion interaction theory................................................................684

B.1.2 Estimation of ion interaction coefficients...........................................688 B.1.3 on the magnitude of in interaction coefficients...................................691 B.2 Ion interaction coefficients and equilibrium constants for ion pairs...............692

B.3 Tables of ion interaction coefficients.............................................................692

XIIIAppendix C: Assigned uncertainties699

C.1 One dource datum........................................................................................699

C.2 Two or more independent source data...........................................................700

C.3 Several data at different ionic strength.........................................................704

C.4 Procedures for data handling........................................................................708

C.4.1 Corrections to zero ionic strength......................................................708

C.4.2Propagation of errors.........................................................................709

C.4.3 Rounding...........................................................................................710

C.4.4Significant digits...............................................................................711

XIVAppendix D: The estimation of entropies713

xv

List of Tables

quotesdbs_dbs29.pdfusesText_35

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