CHEMICAL THERMODYNAMICS OF COMPOUNDS AND COMPLEXES OF U, Np, Pu, Am, Tc, Se, Ni AND Zr WITH SELECTED ORGANIC LIGANDS CHEMICAL THERMODYNAMICS Vol. 1. Chemical Thermodynamics of Uranium (H. Wanner and I. Forest, eds.) Vol. 2. Chemical Thermodynamics of Americium (R.J. Silva etal.) Vol. 3. Chemical Thermodynamics of Technetium (M.C.A. Sandino and E. Östhols, eds.) Vol. 4. Chemical Thermodynamics of Neptunium and Plutonium (OECD Nuclear Energy Agency, ed.) Vol. 5. Update on the Chemical Thermodynamics of Uranium, Neptunium, Plutonium, Americium and Technetium (OECD Nuclear Energy Agency, ed.) Vol. 6. Chemical Thermodynamics of Nickel (OECD Nuclear Energy Agency, ed.) Vol. 7. Chemical Thermodynamics of Selenium (OECD Nuclear Energy Agency, ed.) Vol. 8. Chemical Thermodynamics of Zirconium (OECD Nuclear Energy Agency, ed.) Vol. 9. Chemical Thermodynamics of Compounds and Complexes of U, Np, Pu, Am, Tc, Se, Ni and Zr with Selected Organic Ligands (OECD Nuclear Energy Agency, ed.) CHEMICAL THERMODYNAMICS 9 Chemical Thermodynamics of Compounds and Complexes of U, Np, Pu, Am, Tc, Se, Ni and Zr with Selected Organic Ligands Wolfgang Hummel (Chairman) Laboratory for Waste Management Paul Scherrer Institut Villigen (Switzerland) Giorgio Anderegg Linfeng Rao Swiss Federal Institute of Technology Glenn T. Seaborg Center (ETH) Chemical Sciences Division Zürich (Switzerland) Lawrence Berkeley National Laboratory Berkeley (California, USA) Ignasi Puigdomènech Osamu Tochiyama Swedish Nuclear Fuel and Institute of Multidisciplinary Research Waste Management Co. (SKB) for Advanced Materials (IMRAM) Stockholm (Sweden) Tohoku University Sendai (Japan) Edited by FedericoJ. MOMPEAN (Series Editor and Project Co-ordinator) Myriam ILLEMASSÈNE (Volume Editor) and Jane PERRONE OECD Nuclear Energy Agency, Data Bank Issy-les-Moulineaux (France) 2005 ELSEVIER AMSTERDAM (cid:129) BOSTON (cid:129) HEIDELBERG (cid:129) LONDON (cid:129) NEW YORK (cid:129) OXFORD PARIS (cid:129) SAN DIEGO (cid:129) SAN FRANCISCO (cid:129) SINGAPORE (cid:129) SYDNEY (cid:129) TOKYO Published by ELSEVIERB.V. Radarweg 29 P.O. Box 211, 1000 AE Amsterdam, The Netherlands ISBN-13: 978-0-444-51402-8 ISBN-10: 0-444-51402-3 ISBN: 0-444-52124-0 (CD-ROM) Copyright © Organisation for Economic Co-Operation and Development, 2005. All rights reserved. No reproduction, copy, transmission or translation of this publication may be made without written permission. Applications should be sent to OECD Publishing: [email protected] or by fax (33 1) 45 24 13 91. Special regulations for readers in the U.S.A. - This publication has been registered with the Copyright Clearance Center Inc. 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Printed in The Netherlands Preface This book is the ninth of the series "Chemical Thermodynamics" edited by the OECD Nuclear Energy Agency (NEA), and it is the first review in this series focused on or- ganic ligands. This Organics Review was initiated by the Management Board of the NEA Thermochemical Database Project Phase II (NEA TDB II). Originally Wolfgang Hummel (PSI, Switzerland), Giorgio Anderegg (ETH Zurich, Switzerland), Ignasi Puigdomenech (SKB, Sweden), Osamu Tochiyama (Tohoku University, Sendai, Japan), Josef Havel and Pfemek Lubal (Masaryk University, Brno, Czech Republic) partici- pated in the Organics Review. In August 2003 time constraints and the pressure of other commitments forced Josef Havel and Pfemek Lubal to resign from the Review Team. In December 2003 Linfeng Rao (LBNL, Berkeley, USA) joined the Review Team. The first meeting of the Organics Review Group was held in August 1998 at the NEA Headquarters at Issy-les-Moulineaux (France) and six plenary meetings fol- lowed in October 1999 (Brno, Czech Republic), April 2000 (Sendai, Japan), November 2000 (PSI, Switzerland), September 2001 (Bregenz, Austria), October 2002 (PSI, Swit- zerland) and January 2004 (OECD, Paris, France). The Executive Group of the Man- agement Board provided scientific assistance and Hans Wanner, as the designated member of the Executive Group, participated in some of the Review Group meetings and maintained close contact with the chairman of the Organics Review Team. At the NEA Data Bank the responsibility for the overall co-ordination of the Project was placed with Eric Osthols (from its initiation in 1998 to February 2000), with Stina Lundberg (from March 2000 to September 2000) and with Federico Mompean (since September 2000). Federico Mompean was in charge of the preparation of the successive drafts, updating the NEA thermodynamic database and editing the book to its present final form, with assistance from Myriam Illemassene and Jane Perrone. All the members of the Review Team contributed fully to the main text and the discussions, and the excellent internal communication of the team has to be noted here. However, the workload was distributed according to the expertise of each member. Wolfgang Hummel was the principal author of the sections about oxalic acid, protonation and Na and K interactions of oxalate, while Josef Havel and Pfemek Lubal were initially involved in reviewing the compounds and complexes of oxalate. Ignasi Puigdomenech reviewed citric acid and ethylenediaminetetraacetic acid, as well as protonation and Na and K interactions of citrate and edta. Osamu Tochiyama was the principal author of all sections concerning metal citrate complexes, whereas Giorgio Anderegg carried out the review of edta complexes with the editorial help of Wolfgang VI PREFACE Hummel. After the resignation of Josef Havel and Pfemek Lubal their remaining tasks were reassigned: Linfeng Rao reviewed uranium oxalate compounds and complexes, Wolfgang Hummel Ca and Mg oxalates, Osamu Tochiyama Zr and Am oxalates and Ignasi Puigdomenech Ni, Tc, Se, Np and Pu oxalates. The chapter on iso-saccharinic acid and compounds and complexes of isa is a joint review of Linfeng Rao and Wolfgang Hummel. Villigen, Switzerland, March 2005 Wolfgang Hummel, Chairman Acknowledgements For the preparation of this book, the authors have received financial support from the NEA TDB Phase II Project. The following organisations take part in the Project: ANSTO, Australia ONDRAF/NIRAS, Belgium RAWRA, Czech Republic POSIVA, Finland ANDRA, France IPSN (now IRSN), France FZK, Germany JNC, Japan ENRESA, Spain SKB, Sweden SKI, Sweden HSK, Switzerland NAGRA, Switzerland PSI, Switzerland BNFL, UK NIREX, UK DoE, USA The authors would like to express their gratitude to Richard M. Kettler (De- partment of Geology, University of Nebraska, Lincoln, Nebraska, USA), Ranko P. Bontchev (Sandia National Laboratories, Albuquerque, New Mexico, USA) and Marian Borkowski (Los Alamos National Laboratory, Los Alamos, NM, USA) for providing unpublished data, to Martin A. Glaus and Jan Tits (both from the Laboratory for Waste Management, Paul Scherrer Institut, Villigen, Switzerland) for providing preprints of their most recent publications and to Pavel Samoylov from the Nikolaev Institute of Inorganic Chemistry (RAS) for providing access to a monograph by N. M. Nikolaeva. VII Vlll ACKNOWLEDGEMENTS The authors would like to acknowledge the contributions of Prof. Josef Havel and Dr. Pfemek Lubal (both from the Department of Analytical Chemistry, Masaryk University, Brno, Czech Republic) to the section of oxalate compounds and complexes, mainly for nickel and neptunium, during the early stages of the review process. At the NEA Data Bank, Pierre Nagel and Eric Lacroix have provided excellent software and advice, which have eased the editorial and database work. Cynthia Picot, Solange Quarmeau and Amanda Costa from NEA Publications have provided consider- able help in editing the present series. Their contributions and the support of many NEA staff members are highly appreciated. Jan Rosdahl (Inorganic Chemistry, Royal Institute of Technology, Stockholm, Sweden) helped through literature searches in preparing several figures showing mo- lecular structures of complexes. His contribution is gratefully recognized. Ingmar Grenthe (Inorganic Chemistry, Royal Institute of Technology, Stock- holm, Sweden) reviewed early versions of Chapters VII and VIII. His contributions are gratefully acknowledged. The entire manuscript of this book has undergone a peer review by an inde- pendent international group of reviewers, according to the procedures in the TDB-6 Guideline, available from the NEA. The peer reviewers have seen and approved the modifications made by the authors in response to their comments. The peer review comment records may be obtained on request from the OECD Nuclear Energy Agency. The peer reviewers were: Prof. Gregory R. Choppin, Florida State University, Tallahassee, Florida, USA Prof. Pier G. Daniele, University of Turin, Turin, Italy Prof. Alfredo Mederos, University of La Laguna, Tenerife, Spain Their contributions are gratefully acknowledged. Note from the Chairman of the NEA TDB Project Phase II The need to make available a comprehensive, internationally recognised and quality- assured chemical thermodynamic database that meets the modelling requirements for the safety assessment of radioactive waste disposal systems prompted the Radioactive Waste Management Committee (RWMC) of the OECD Nuclear Energy Agency (NEA) to launch in 1984 the Thermochemical Database Project (NEA TDB) and to foster its continuation as a semi-autonomous project known as NEA TDB Phase II in 1998. The RWMC assigned a high priority to the critical review of relevant chemical thermodynamic data of inorganic species and compounds of the actinides uranium, neptunium, plutonium and americium, as well as the fission product technetium. The first four books in this series on the chemical thermodynamics of uranium, americium, neptunium and plutonium, and technetium originated from this initiative. The organisation of Phase II of the TDB Project reflects the interest in many OECD/NEA member countries for a timely compilation of the thermochemical data that would meet the specific requirements of their developing national waste disposal pro- grammes. The NEA TDB Phase II Review Teams, comprising internationally recognised experts in the field of chemical thermodynamics, exercise their scientific judgement in an independent way during the preparation of the review reports. The work of these Review Teams has also been subjected to further independent peer review. Phase II of the TDB Project consisted of: (i) updating the existing, CODATA- compatible database for inorganic species and compounds of uranium, neptunium, plu- tonium, americium and technetium, (ii) extending it to include selected data on inor- ganic species and compounds of nickel, selenium and zirconium, (iii) and further adding data on organic complexes of citrate, oxalate, edta and iso-saccharinic acid (isa) with uranium, neptunium, plutonium, americium, technetium, nickel, selenium, zirconium and some other competing cations. The NEA TDB Phase II objectives were formulated by the 17 participating or- ganisations coming from the fields of radioactive waste management and nuclear regu- lation. The TDB Management Board is assisted for technical matters by an Executive Group of experts in chemical thermodynamics. In this second phase of the Project, the IX