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Speciation, Techniques and Facilities for Radioactive Materials at Synchrotron Light Sources

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Speciation, Techniques and Facilities for Radioactive Materials at Synchrotron Light Sources Proceedings of the Workshop on SPECIATION, TECHNIQUES AND FACILITIES FOR RADIOACTIVE MATERIALS AT SYNCHROTRON LIGHT SOURCES 4-6 October 1998 Grenoble, France co-sponsored by European Commission Forschungszentrum Rossendorf European Synchrotron Radiation Facility Commissariat à l’Énergie Atomique US Department of Energy 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 Member countries, while maintaining financial stability, and thus to contribute to the development of the world economy; − to contribute to sound economic expansion in Member as well as non-member countries in the process of economic development; and − to contribute to the expansion of world trade on a multilateral, non-discriminatory basis in accordance with international obligations. The original Member countries of the OECD are Austria, Belgium, Canada, Denmark, France, Germany, Greece, Iceland, Ireland, Italy, Luxembourg, the Netherlands, Norway, Portugal, Spain, Sweden, Switzerland, Turkey, the United Kingdom and the United States. The following countries became Members subsequently through accession at the dates indicated hereafter; Japan (28th April 1964), Finland (28th January 1969), Australia (7th June 1971), New Zealand (29th May 1973), Mexico (18th May 1994), the Czech Republic (21st December 1995), Hungary (7th May 1996), Poland (22nd November 1996) and the Republic of Korea (12th December 1996). 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 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 all OECD Member countries, except New Zealand and Poland. The Commission of the European Communities takes part in the work of the Agency. The primary objective of the NEA is to promote co-operation among the governments of its participating countries in furthering the development of nuclear power as a safe, environmentally acceptable and economic energy source. This is achieved by: − encouraging harmonization of national regulatory policies and practices, with particular reference to the safety of nuclear installations, protection of man against ionising radiation and preservation of the environment, radioactive waste management, and nuclear third party liability and insurance; − assessing the contribution of nuclear power to the overall energy supply by keeping under review the technical and economic aspects of nuclear power growth and forecasting demand and supply for the different phases of the nuclear fuel cycle; − developing exchanges of scientific and technical information particularly through participation in common services; − setting up international research and development programmes and joint undertakings. In these and related tasks, the NEA works in close collaboration with the International Atomic Energy Agency in Vienna, with which it has concluded a Co-operation Agreement, as well as with other international organisations in the nuclear field. © OECD 1999 Permission to reproduce a portion of this work for non-commercial purposes or classroom use should be obtained through the Centre français d’exploitation du droit de copie (CCF), 20, rue des Grands-Augustins, 75006 Paris, France, Tel. (33-1) 44 07 47 70, Fax (33-1) 46 34 67 19, for every country except the United States. In the United States permission should be obtained through the Copyright Clearance Center, Customer Service, (508)750-8400, 222 Rosewood Drive, Danvers, MA 01923, USA, or CCC Online: http://www.copyright.com/. All other applications for permission to reproduce or translate all or part of this book should be made to OECD Publications, 2, rue André-Pascal, 75775 Paris Cedex 16, France. FOREWORD X-ray spectroscopic and scattering techniques are powerful tools for providing molecular scale information on radionuclides in solution, and in crystalline and amorphous solids. They permit the characterisation of species that are important for chemical processing, waste management and materials identification and are a key link to laboratory-based techniques. Intense monochromatic X-ray photons, which are necessary for such experiments, are available only at synchrotron light sources. In order to study processes utilising radioactive materials with modern X-ray techniques, special procedures and facilities are necessary. At present a few synchrotron laboratories and users have set up procedures and facilities for the use of radioactive materials. Other synchrotron laboratories and user groups are constructing or planning such facilities. For this reason, the first Euroconference and NEA Workshop on Speciation, Techniques and Facilities for Radioactive Materials at Synchrotron Light Sources, Actinide-XAS-98, was held from 4-6 October 1998 in Grenoble, France, with close to 100 participants from 15 countries (see Annex 1). It was hosted by the European Synchrotron Radiation Facility (ESRF), and organised mainly by the Forschungszentrum Rossendorf, Germany. The European Commission, the CEA (France) and the US DOE co-sponsored the meeting. There were 31 oral presentations and 22 posters covering: 1. Introduction to synchrotron radiation techniques, such as X-ray absorption spectroscopy, X-ray scattering, and X-ray imaging. 2. Results in the field of radionuclide/actinide chemistry and physics obtained by synchrotron radiation: • Radionuclides in the environment. • Nuclear waste management. • Separation technology. • General actinide chemistry. • Radiopharmaceutical chemistry. • Electronic and magnetic properties. 3. Status reports on current and future actinide experimental stations at synchrotron light sources. These proceedings contain the abstracts and some of the full papers presented at the meeting. The editors, Dr. Edelstein, Dr. Nitsche and Dr. Reich, and other anonymous referees reviewed the full papers. The organising committee (see Annex 2) wishes to acknowledge and thank these reviewers. 3 TABLE OF CONTENTS FOREWORD.................................................................................................................................... 3 EXECUTIVE SUMMARY.............................................................................................................. 11 Session I: INTRODUCTION TO SYNCHROTRON RADIATION TECHNIQUES ............ 13 Chairs: N.M. Edelstein, C. Madic, S. Tachimori, D.C. Koningsberger H. Nitsche, T. Reich, C. Hennig, A. Roßberg, G. Geipel, M.A. Denecke L. Baraniak, P. Panak, A. Abraham, B. Mack, S. Selenska-Pobell, G. Bernhard Application of Synchrotron Radiation Techniques to Radionuclide Studies................. 15 D.C. Koningsberger XAFS Spectroscopy: A Powerful Tool to Investigate Local Structure and Electronic Properties...................................................................................................... 29 J. Goulon Experimental Aspects of X-Ray Absorption Spectroscopy........................................... 31 A. Filipponi Theoretical Framework for Data and Error Analysis as Applied to X-Ray Absorption Spectroscopy............................................................................................... 33 V.I. Nefedov Introduction to X-Ray Photoelectron Spectroscopy: A Complementary Technique to X-Ray Absorption Spectroscopy ............................................................. 35 D.K. Shuh Introduction to Actinide Investigations with X-Ray Techniques Below 2 keV ............ 37 W. Matz Introduction to X-Ray Diffraction at Synchrotron Light Sources ................................. 39 G.H. Lander X-Ray Scattering Applied to Magnetism of the Actinides ............................................ 51 U. Wahlgren, B. Schimmelpfennig, L. Maron, V. Vallet, I. Grenthe, O. Gropen Molecular Modelling of Actinide Complexes ............................................................... 53 Session II: APPLICATIONS OF SYNCHROTRON TECHNIQUES....................................... 67 Chairs: P.G. Allen, F.R. Livens, A.M. Scheidegger, N. Baclet, D.K. Smith C. Madic, C. Den Auwer, R. Guillaumont Application of X-Ray Absorption Spectroscopy (XAS) to Actinide Solution Chemistry.......................................................................................................................69 5 P.M. Bertsch, D.B. Hunter, M. Duff Micro/Spatially Resolved XRF and XAFS for the In Situ Interrogation of Radionuclide Distribution and Speciation in Environmental Samples.......................... 81 T. Reich, H. Moll, M.A. Denecke, C. Hennig, G. Geipel, G. Bernhard, H. Nitsche, P.G. Allen, J.J. Bucher, N.M. Edelstein, D.K. Shuh EXAFS Studies of Uranium(VI) Sorption on Mineral Surfaces.................................... 83 D.K. Veirs X-Ray Absorption Spectroscopy Studies of Plutonium Nitrate Species in Solution and on Ion Exchange Resins ....................................................................... 93 F. David, B. Fourest, S. Hubert, J.F. Le Du, R. Revel, C. Den Auwer, C. Madic, L.R. Morss, G. Ionova, V.
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