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Speciation, Techniques and Facilities for Radioactive Materials at Synchrotron Light Sources Nuclear Science NEA/NSC/DOC(2009)15 Speciation, techniques and facilities for radioactive materials at synchrotron light sources Actinide XAS 2008 Proceedings of the 5th workshop Saint-Aubin, France 15-17 July 2008 © OECD 2009 NUCLEAR ENERGY AGENCY Organisation for Economic Co-operation and Development ORGANISATION FOR ECONOMIC CO-OPERATION AND DEVELOPMENT The OECD is a unique forum where the governments of 30 democracies work together to address the economic, social and environmental challenges of globalisation. The OECD is also at the forefront of efforts to understand and to help governments respond to new developments and concerns, such as corporate governance, the information economy and the challenges of an ageing population. The Organisation provides a setting where governments can compare policy experiences, seek answers to common problems, identify good practice and work to co-ordinate domestic and international policies. The OECD member countries are: Australia, Austria, Belgium, Canada, the Czech Republic, Denmark, Finland, France, Germany, Greece, Hungary, Iceland, Ireland, Italy, Japan, Korea, Luxembourg, Mexico, the Netherlands, New Zealand, Norway, Poland, Portugal, the Slovak Republic, Spain, Sweden, Switzerland, Turkey, the United Kingdom and the United States. The Commission of the European Communities takes part in the work of the OECD. OECD Publishing disseminates widely the results of the Organisation’s statistics gathering and research on economic, social and environmental issues, as well as the conventions, guidelines and standards agreed by its members. This work is published on the responsibility of the Secretary-General of the OECD. The opinions expressed and arguments employed herein do not necessarily reflect the official views of the Organisation or of the governments of its member countries. 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, 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. Corrigenda to OECD publications may be found on line at: www.oecd.org/publishing/corrigenda. © OECD 2009 You can copy, download or print OECD content for your own use, and you can include excerpts from OECD publications, databases and multimedia products in your own documents, presentations, blogs, websites and teaching materials, provided that suitable acknowledgment of OECD as source and copyright owner is given. All requests for public or commercial use and translation rights should be submitted to [email protected]. Requests for permission to photocopy portions of this material for public or commercial use shall be addressed directly to the Copyright Clearance Center (CCC) at [email protected] or the Centre français d'exploitation du droit de copie (CFC) [email protected]. FOREWORD Foreword “Actinide-XAS” is a series of workshops on Speciation, Techniques and Facilities for Radioactive Materials at Synchrotron Light sources, which provides every two or three years a unique opportunity for scientists involved in the field as well as newcomers, to present, discuss and exchange on the applications and results from synchrotron-based techniques in radionuclide/actinide sciences. Previous editions of the workshop were held in Grenoble, France (1998 and 2000), in Berkeley, USA (2004) and in Karlsruhe, Germany (2006). Ten years after the inaugural conference, “Actinide-XAS-2008”, the 5th edition in the series, was successfully held in Saint-Aubin (near Paris) from 15-17 July 2008 at Synchrotron SOLEIL, where MARS, the new French hard X-ray beamline dedicated to the study of radioactive matter, will be opening to users in 2009. The workshop was co-organised by SOLEIL, the Comissariat à l’Energie Atomique (CEA) and the Centre National de la Recherche Scientifique (CNRS), and was financially supported by SOLEIL, CEA, the interdisciplinary programme PACEN of the CNRS, the region Ile-de France, OECD’s Nuclear Energy Agency (NEA) for the proceedings publication, and the European Network of Excellence for Actinide Sciences (ACTINET) for the payment of the participation of students and post-docs. Also, for the first time, the workshop was organised as a satellite meeting of the 5th edition of the international topical conference on plutonium and actinides, Plutonium Futures –The Science 2008 (held in Dijon). More than one hundred people registered for the conference and 83 were effectively present. The audience was composed of 61 scientists or staff members, 15 post-doctoral students and 7 PhD students originating from laboratories belonging to 10 different countries, including the United States, Japan and Russia. SPECIATION, TECHNIQUES AND FACILITIES FOR RADIOACTIVE MATERIALS AT SYNCHROTRON LIGHT SOURCES – © OECD/NEA 2009 3 TABLE OF CONTENTS Table of contents Foreword.......................................................................................................................................................... 3 Executive summary ....................................................................................................................................... 9 Session I Solution and co-ordination chemistry of the radionuclides ........................................... 11 Chair: T. Reich S. Suzuki, T. Yaita, Y. Okamoto, H. Shiwaku EXAFS investigation of uranium(VI)-N,N-dialkylamide complexes .................................. 13 H. Matsuura, A. Nezu, H. Akatsuka, T. Nagai, A. Uehara, T. Fujii, O. Shirai, H. Yamana, M. Myochin, Y. Okamoto XAFS analysis on the molten chlorides containing uranyl ions ....................................... 19 L. Giachini, M. Meyer, L-V. Nguyen, R. Guilard, S. Faure, B. Batifol, H. Chollet, A.C. Scheinost, C. Hennig X-ray absorption studies of the interaction between uranium(VI) and silica-gel-bound tetraazamacrocycles .................................................................................. 27 Abstracts* O.P. Lam, M. Denecke, S. Conradson, K. Meyer Systematic XAS studies on uranium co-ordination complexes featuring the U3+ to U6+ series ................................................................................................................. 37 C.A. Sharrad, H. Kinoshita, I. May, I.B. Polovov, V.A. Volkovich, J.M. Charnock, B. Kralj, R.G. Lewin Understanding actinide behaviour in high temperature molten salts ............................. 39 C. Hennig, K. Servaes, P. Nockemann, R. Van Deun Combining EXAFS, UV-Vis and XRD to extract uranyl chloride speciation and co-ordination in solution ................................................................................................ 41 Session II Radionuclides in environmental and life sciences ........................................................... 43 Chair: M.A. Denecke O.N. Batuk, S.N. Kalmykov, E.V. Zakharova, M. Klimenkov, V.V. Kriventsov Uranium dioxide behaviour in hydrothermal oxidising conditions ................................. 45 Abstracts R. Dähn, M. Vespa, D.K. Shuh, T. Tyliszczak, E. Wieland Soft X-ray scanning transmission spectromicroscopy of metal uptake by nuclear waste repository materials.................................................................................. 55 S. Selenska-Pobell The impact of micro-organisms on the behaviour of actinides in natural environments ............................................................................................................. 57 H. Moll, M. Glorius, A. Roßberg, G. Bernhard Uranium(VI) complexation with pyoverdins and related model compounds studied by EXAFS ..................................................................................................................... 59 * The full papers being unavailable at the time of publication, only the abstracts are included. SPECIATION, TECHNIQUES AND FACILITIES FOR RADIOACTIVE MATERIALS AT SYNCHROTRON LIGHT SOURCES – © OECD/NEA 2009 5 TABLE
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