Pyrochemical Separations : Workshop Proceedings -- Avignon, France -- 14-16 March 2000.

336 Pages·2001·6.75 MB·English

by  OECD

Nuclear Science
P
yrochemical Separations
Workshop Proceedings
Avignon, France
14-16 March 2000
N U C L E A R • E N E R G Y • A G E N C Y
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OECD PROCEEDINGS
Proceedings of the Workshop on
P
YROCHEMICAL
S
EPARATIONS
Co-organised by the
European Commission
Hosted by
Commissariat à l’Énergie Atomique Valrhô
Avignon, France
14-16 March 2000
NUCLEAR ENERGY AGENCY
ORGANISATION FOR ECONOMIC CO-OPERATION AND DEVELOPMENT
ORGANISATION FOR ECONOMIC CO-OPERATION AND DEVELOPMENT
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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
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FOREWORD
In the future, nuclear fuel will reach high burn-up, and recycling of spent fuel will possibly have
to be performed after shorter cooling times to be economically and ecologically attractive. Dry
reprocessing using pyrochemical methods has received the attention of some research institutes due to
its potential advantages of compactness in the plant design, criticality safety considerations as well as
stability against high radiation dose.
Recently, partitioning and transmutation (P&T) of long-lived fission products and minor actinides
has been considered as one of the future options of waste management. In order to achieve effective
transmutation, multi-recycling of fuel with much higher burn-up and shorter cooling time will be
required. Therefore, the role of pyrochemical reprocessing becomes more important for the
implementation of the P&T option.
The proposed processes are complex and necessitate the use of highly controlled atmospheres to
avoid hydrolysis and precipitation reactions. Except for the pilot-scale demonstration of the
pyro-electrolysis at Argonne National Laboratory (Idaho) and the Russian Institute of Atomic
Reactors, all other studies are at the laboratory scale. Much R&D work is required in order to upgrade
the pyrochemical separation process to the current level of industrial aqueous reprocessing.
For this reason, the OECD/NEA Nuclear Science Committee decided to organise a workshop to
exchange information about recent activities on pyrochemical separations and to make a
recommendation about the future activities of the OECD/NEA in the field.
The Workshop on Pyrochemical Separations, co-organised by the European Commission and
hosted by CEA Valrho, was successfully held in Avignon, France, on 14-15 March 2000, with more
than 70 participants from 14 countries and 3 international organisations. There were 21 oral
presentations and 8 posters on the following topics:
• National and international R&D programmes on pyrochemical separations.
• Role and requirements of pyrochemical reprocessing in future fuel cycles.
• Recent progress in research activities, including:
− Basic data (thermodynamics, reaction mechanisms, reaction kinetics, molecular modelling).
− Results and experiences from process experiments.
− Process simulation and process design.
It was recommended that an expert group be set up to prepare a state-of-the-art report on
pyrochemical separations. The report, furnishing timely and coherent coverage of situations in each
country and providing a common scientific base on pyrochemical separations, will be very useful for
promoting efficient international collaboration.
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TABLE OF CONTENTS
FOREWORD.................................................................................................................................... 3
EXECUTIVE SUMMARY.............................................................................................................. 9
OPENING SESSION....................................................................................................................... 11
C. Madic
Welcome Address..................................................................................................... 13
Ph. Savelli
Opening Address...................................................................................................... 15
SESSION I National and International R&D Programmes on Pyrochemical
Separations.............................................................................................................. 17
Chair: G. Choppin, B. Boullis
M. Hugon
Research Work on Radionuclide Partitioning from Nuclear Waste
Co-Financed by the European Commission............................................................. 19
J.T. Laidler
Pyrochemical Separations Technologies Envisioned for the US
Accelerator Transmutation of Waste System........................................................... 25
A.V. Bychkov, O.V. Skiba, S.K. Vavilov, M.V. Kormilitzyn, A.G. Osipenco
Overview of RIAR Activity on Pyroprocess Development and Application
to Oxide Fuel and Plans in the Coming Decade....................................................... 37
R. Thied, D. Hebditch, P. Parkes, R. Taylor, B. Hanson, P. Wilson
BNFL’s Molten Salts Programme: Industrialising Processes for
Irradiated Fuel........................................................................................................... 47
B. Boullis, Ph. Brossard
Assessment of Pyrochemical Processes for Separation/Transmutation
Strategies: Proposed Areas of Research................................................................... 59
SESSION II Role and Requirements of Pyrochemical Separations in the Future
Fuel Cycles............................................................................................................... 61
Chairs: P. Wilson, M. Hugon
L. Koch
Role of Pyrochemistry in Advanced Nuclear Energy Generating System............... 63
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J. Uhlir
Pyrochemical Reprocessing Technology and Molten Salt Transmutation
Reactor Systems........................................................................................................ 73
T. Inoue
Actinide Recycling by Pyroprocess for Future Nuclear Fuel Cycle System............ 79
S. Kitawaki, K. Kosugi, M. Fukushima, M. Myochin
Evaluation of Pyrochemical Reprocessing Technologies for Practical Use............. 87
SESSION III Part A: Basic Data (Thermodynamics, Reaction Mechanisms
Reaction Kinetics, Molecular Modelling, etc.)..................................................... 97
Chairs: L. Koch, T. Ogawa
M. Gaune-Escard, A.K. Adya, L. Rycerz
Molten Salt Data for Pyrochemistry: New Research Advances
and Development of Information System................................................................. 99
D. Lambertin, J. Lacquement, S. Sanchez, G. Picard
Electrochemical Properties of Plutonium in Molten CaCl -NaCl at 550°C............. 111
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F. Lantelme, T. Cartailler, P. Turq
Application of Electrochemical Techniques in Pyropartitioning Processes
and Reaction Modelling............................................................................................ 123
H. Yamana, J. Sheng, H. Moriyama
Thermodynamic Stabilities of Lanthanides and Actinides in Molten
Chloride and Liquid Metal........................................................................................ 135
Part B: Results and Experiences from Process Experiments............................. 145
Chairs: M. Gaune-Escard, T. Inoue
G.R. Choppin
Results of Demonstration Programme of Electrometallurgical Processing
of Breeder Reactor Fuel............................................................................................ 147
T. Ogawa, Y. Arai
Nitride/Pyroprocess for MA Transmutation and Fundamental Database................. 157
T. Usami, M. Kurata, T. Inoue, J. Jenkins, H. Sims, S. Beetham, D. Brown
Pyrometallurgical Reduction of Unirradiated TRU Oxides by Lithium
in a Lithium Chloride Medium................................................................................. 165
T. Koyama, K. Kinoshita, T. Inoue, M. Ougier, J.-P. Glatz, L. Koch
Small-Scale Demonstration of Pyrometallurgical Processing for Metal
Fuel and HLLW........................................................................................................ 177
T. Subramanian, B. Prabhakara Reddy, P. Venkatesh, R. Kandan,
T. Vandarkuzhali, K. Nagarajan, P.R. Vasudeva Rao
Studies on the Head-End Steps for Pyrochemical Reprocessing
of Oxide Fuels........................................................................................................... 187
6
Part C: Process Simulation and Process Design.................................................. 195
Chairs: J. Uhlir, H. Boussier
P. Hosnedl, O. Matal
Development of Structural Material and Equipment for Molten Salt
Technology............................................................................................................... 197
H. Moriyama, H. Yamana, K. Moritani
Kinetics of Pyrochemical Processing of Nuclear Materials Using Molten
Salt and Liquid Metal............................................................................................... 205
G. Picard, S. Sanchez, D. Lambertin, J. Lacquement
A Rational Approach to Pyrochemical Processes Via Thermodynamic
Analysis.................................................................................................................... 213
SESSION IV Open Discussion and Recommendations.............................................................. 227
Chair: C. Madic
POSTER SESSION.......................................................................................................................... 231
K. Guerman, T. Reich, C. Sergeant, R. Ortega, V. Tarasov, M. Simonoff
Technetium Metal and Pyrometallurgically Formed Sediments: Study
and Speciation by Tc NMR and EXAFS/XANES.................................................... 233
V.V. Ignatiev, R.Ya. Zakirov, K.F. Grebenkine
Molten Salt Burner Fuel Behaviour and Treatment.................................................. 243
C. Jouault, M. Allibert, R. Boen, X. Deschanels
Recovery of Noble Metals (Ru, Rh, Pd, Mo) and Tellurium from
Fission Products........................................................................................................ 255
S. Kitawaki, N. Kameshiro, M. Fukushima, M. Myochin
Study of Oxidising Uranium for Pyrochemical Reprocessing.................................. 265
C. Pernel, M. Ougier, J.-P. Glatz, L. Koch, T. Koyama
Partitioning of Americium Metal from Rare Earth Fission Products
by Electrorefining..................................................................................................... 275
W.A. Punjak, A.J. Vargas, Jr., G.D. Bird, E. Garcia
Americium Extraction Via In Situ Chlorination of Plutonium Metal....................... 285
G. Bourgès, A. Godot, C. Valot, D. Devillard
Pyro-Oxidation of Plutonium Spent Salts with Sodium Carbonate.......................... 287
S.A. Kuznetsov, M. Gaune-Escard
Electrochemical Studies of EuCl and EuCl in an Equimolar
3 2
NaCl-KCl Melt......................................................................................................... 295
V. Lelek, T. Marek
Generalised Perturbation Theory and Source of Information through
Chemical Measurements........................................................................................... 307
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Annex 1. LIST OF PARTICIPANTS.............................................................................................. 317
Annex 2. WORKSHOP ORGANISATION.................................................................................... 327
Annex 3. STATE-OF-THE-ART REPORT ON PYROCHEMICAL SEPARATIONS............ 329
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