Separation of long-lived radionuclides from high active nuclear waste

Charles Madic; Michaël Lecomte; Pascal Baron; Bernard Boullis

doi:10.1016/S1631-0705(02)01370-1

Du combustible nucléaire aux déchets : recherches actuelles/From nuclear fuels to waste: current research

Separation of long-lived radionuclides from high active nuclear waste
[Séparation de radionucléides à vie longue des déchets nucléaires de haute activité]

Charles Madic ¹ ; Michaël Lecomte ² ; Pascal Baron ² ; Bernard Boullis ²

¹ CEA, Direction de l'énergie nucléaire, bâtiment 523, CEA/Saclay, 91191 Gif-s-Yvette, France
² CEA, Direction de l'énergie nucléaire, bâtiment 222, CEA/VRH (Marcoule), BP 17171, 30207 Bagnols-s-Cèze, France

Comptes Rendus. Physique, Volume 3 (2002) no. 7-8, pp. 797-811.

Abstract (VO)
Résumé

The management of vitrified high activity waste issued from the reprocessing of spent nuclear fuel is often made questionable by the presence within this waste of long-lived radionuclides (LLRNs). New management scenarios of this waste are under study at the CEA since the beginning of the 1990s, involving the development of separation processes for some LLRNs. Six LLRNs are the targets of these studies; they are: (i) the minor actinides: neptunium, americium and curium; (ii) the fission products: technetium, iodine and caesium. The present paper highlights the main achievements of the research performed at the CEA in this field.

La gestion à très long terme des déchets de haute activité vitrifiés issus du retraitement des combustibles nucléaires usés est souvent mise en question par la présence dans ces déchets de radionucléides à vie longue (RNVL). De nouvelles méthodes de gestion de ces déchets sont à l'étude au CEA depuis le début des années 1990, qui ont conduit à la mise au point de procédés de séparation de certains RNVL. Six RNVL font l'objet de ces recherches, ce sont : (i) les actinides mineurs : neptunium, américium et curium, et (ii) les produits de fission : technétium, iode et césium. Cet article fait le point de l'état d'avancement des recherches menées au CEA dans ce domaine.

Reçu le : 2002-03-27
Accepté le : 2002-06-04
Publié le : 2002-07-16

DOI : 10.1016/S1631-0705(02)01370-1

Keywords: nuclear waste, reprocessing, partitioning, long-lived radionuclides, liquid–liquid extraction
Mots-clés : déchets nucléaires, retraitement poussé, radionucléides à vie longue, extraction liquide–liquide

Affiliations des auteurs :

Charles Madic ¹ ; Michaël Lecomte ² ; Pascal Baron ² ; Bernard Boullis ²

¹ CEA, Direction de l'énergie nucléaire, bâtiment 523, CEA/Saclay, 91191 Gif-s-Yvette, France
² CEA, Direction de l'énergie nucléaire, bâtiment 222, CEA/VRH (Marcoule), BP 17171, 30207 Bagnols-s-Cèze, France

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Charles Madic; Michaël Lecomte; Pascal Baron; Bernard Boullis. Separation of long-lived radionuclides from high active nuclear waste. Comptes Rendus. Physique, Volume 3 (2002) no. 7-8, pp. 797-811. doi : 10.1016/S1631-0705(02)01370-1. https://comptes-rendus.academie-sciences.fr/physique/articles/10.1016/S1631-0705(02)01370-1/

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Michael J. Hudson; Laurence M. Harwood; Dominic M. Laventine; Frank W. Lewis Use of Soft Heterocyclic N-Donor Ligands To Separate Actinides and Lanthanides, Inorganic Chemistry, Volume 52 (2013) no. 7, p. 3414 | DOI:10.1021/ic3008848
Emma Aneheim; Christian Ekberg; Alexander Littley; Elin Löfström-Engdahl; Gunnar Skarnemark Technetium chemistry in a novel group actinide extraction process, Journal of Radioanalytical and Nuclear Chemistry, Volume 296 (2013) no. 2, p. 743 | DOI:10.1007/s10967-012-1928-2
Nuclear Energy, Nuclear Reactors, Nuclear Fuel, and Fuel Cycles, Nuclear and Radiochemistry (2013), p. 507 | DOI:10.1002/9783527653331.ch15
P. Deepika; K. N. Sabharwal; T. G. Srinivasan; P. R. Vasudeva Rao Studies on Bis Annulated Triazinyl Pyridine (BATP) using Extraction Chromatography, Separation Science and Technology, Volume 48 (2013) no. 13, p. 2020 | DOI:10.1080/01496395.2013.788519
Daniel Magnusson; Andreas Geist; Andreas Wilden; Giuseppe Modolo Direct Selective Extraction of Actinides(III) from PUREX Raffinate Using a Mixture of CyMe4-BTBP and TODGA as 1-cycle SANEX Solvent PART II: Flow-sheet Design for a Counter-Current Centrifugal Contactor Demonstration Process, Solvent Extraction and Ion Exchange, Volume 31 (2013) no. 1, p. 1 | DOI:10.1080/07366299.2012.700596
R. J. Taylor; C. R. Gregson; M. J. Carrott; C. Mason; M. J. Sarsfield Progress towards the Full Recovery of Neptunium in an Advanced PUREX Process, Solvent Extraction and Ion Exchange, Volume 31 (2013) no. 4, p. 442 | DOI:10.1080/07366299.2013.800438
G. Benay; G. Wipff Liquid–Liquid Extraction of Uranyl by an Amide Ligand: Interfacial Features Studied by MD and PMF Simulations, The Journal of Physical Chemistry B, Volume 117 (2013) no. 24, p. 7399 | DOI:10.1021/jp4028386
G. Benay; G. Wipff Oil-Soluble and Water-Soluble BTPhens and Their Europium Complexes in Octanol/Water Solutions: Interface Crossing Studied by MD and PMF Simulations, The Journal of Physical Chemistry B, Volume 117 (2013) no. 4, p. 1110 | DOI:10.1021/jp3103707
Sylvie L. Pailloux; Daniel Rosario‐Amorin; Manab Chakravarty; Jean‐Michel Camus; Karen Ann Smith; Eileen N. Duesler; Diane A. Dickie; Robert T. Paine; Kevin K. Klausmeyer; Daniel A. Padron; Benjamin P. Hay; Laetitia H. Delmau Synthesis and Properties of New (Phosphinoylmethyl)Pyridine N‐Oxides, Zeitschrift für anorganische und allgemeine Chemie, Volume 639 (2013) no. 7, p. 1101 | DOI:10.1002/zaac.201300099
Ruiqin Liu; Yuezhou Wei; Yuanlai Xu; Shigekazu Usuda; Seongyun Kim; Hiromichi Yamazaki; Keizo Ishii Evaluation study on properties of isohexyl-BTP/SiO2-P resin for direct separation of trivalent minor actinides from HLLW, Journal of Radioanalytical and Nuclear Chemistry, Volume 292 (2012) no. 2, p. 537 | DOI:10.1007/s10967-012-1631-3
Jessie L. Brown; Skye Fortier; Richard A. Lewis; Guang Wu; Trevor W. Hayton A Complete Family of Terminal Uranium Chalcogenides, [U(E)(NSiMe32)3]− (E = O, S, Se, Te), Journal of the American Chemical Society, Volume 134 (2012) no. 37, p. 15468 | DOI:10.1021/ja305712m
P. Deepika; K. N. Sabharwal; T. G. Srinivasan; P. R. Vasudeva Rao Studies on Separation of Minor Actinides from Lanthanides from High Level Waste by Extraction Chromatography Using 2,6-Bistriazinyl Pyridine, Nuclear Technology, Volume 179 (2012) no. 3, p. 407 | DOI:10.13182/nt12-a14172
Bohumír Grüner; Petr Švec; Pavel Selucký; Mária Bubeníková Halogen protected cobalt bis(dicarbollide) ions with covalently bonded CMPO functions as anionic extractants for trivalent lanthanide/actinide partitioning, Polyhedron, Volume 38 (2012) no. 1, p. 103 | DOI:10.1016/j.poly.2012.02.029
K. Bell; A. Geist; F. McLachlan; G. Modolo; R. Taylor; A. Wilden Nitric Acid Extraction into TODGA, Procedia Chemistry, Volume 7 (2012), p. 152 | DOI:10.1016/j.proche.2012.10.026
Daniel Magnusson; Andreas Geist; Rikard Malmbeck; Giuseppe Modolo; Andreas Wilden Flow-Sheet Design for an Innovative SANEX Process Using TODGA and SO3-Ph-BTP, Procedia Chemistry, Volume 7 (2012), p. 245 | DOI:10.1016/j.proche.2012.10.040
Christine Rostaing; Christophe Poinssot; Dominique Warin; Pascal Baron; Brigitte Lorraina Development and Validation of the EXAm Separation Process for Single Am Recycling, Procedia Chemistry, Volume 7 (2012), p. 367 | DOI:10.1016/j.proche.2012.10.057
K. Bell; C. Carpentier; M. Carrott; A. Geist; C. Gregson; X. Hérès; D. Magnusson; R. Malmbeck; F. McLachlan; G. Modolo; U. Müllich; M. Sypula; R. Taylor; A. Wilden Progress Towards the Development of a New GANEX Process, Procedia Chemistry, Volume 7 (2012), p. 392 | DOI:10.1016/j.proche.2012.10.061
Jamie Brown; Fiona McLachlan; Mark Sarsfield; Robin Taylor; Giuseppe Modolo; Andreas Wilden Plutonium Loading of Prospective Grouped Actinide Extraction (GANEX) Solvent Systems based on Diglycolamide Extractants, Solvent Extraction and Ion Exchange, Volume 30 (2012) no. 2, p. 127 | DOI:10.1080/07366299.2011.609378
Hitos Galán; María Teresa Murillo; Rosa Sedano; Ana Núñez; Javier de Mendoza; Amparo González‐Espartero; Pilar Prados Hydrolysis and Radiation Stability of m‐Xylylene Bis‐diglycolamide: Synthesis and Quantitative Study of Degradation Products by HPLC–APCI+, European Journal of Organic Chemistry, Volume 2011 (2011) no. 20-21, p. 3959 | DOI:10.1002/ejoc.201100443
G. Benay; R. Schurhammer; G. Wipff Basicity, complexation ability and interfacial behavior of BTBPs: a simulation study, Phys. Chem. Chem. Phys., Volume 13 (2011) no. 7, p. 2922 | DOI:10.1039/c0cp01975e
P. Deepika; N. Sivaraman; K. N. Sabharwal; T. G. Srinivasan; P. R. Vasudeva Rao Separation of lanthanides and actinides on a bistriazinyl pyridine coated reverse phase column, Radiochimica Acta, Volume 99 (2011) no. 6, p. 325 | DOI:10.1524/ract.2011.1819
Thomas Fanghänel; Jean-Paul Glatz; Rudy J. M. Konings; Vincenzo V. Rondinella; Joe Somers Transuranium Elements in the Nuclear Fuel Cycle, Handbook of Nuclear Engineering (2010), p. 2935 | DOI:10.1007/978-0-387-98149-9_26
Daniel Caurant; Pascal Loiseau; Isabelle Bardez Structural characterization of Nd-doped Hf-zirconolite Ca1−xNdxHfTi2−xAlxO7 ceramics, Journal of Nuclear Materials, Volume 407 (2010) no. 2, p. 88 | DOI:10.1016/j.jnucmat.2010.09.033
B. Grüner; M. Kvíčalová; P. Selucký; M. Lučaníková Anionic alkyl diglycoldiamides with covalently bonded cobalt bis(dicarbollide)(1−) ions for lanthanide and actinide extractions, Journal of Organometallic Chemistry, Volume 695 (2010) no. 9, p. 1261 | DOI:10.1016/j.jorganchem.2010.02.014
Claire Mantel; Pierre‐Alain Bayle; Sabine Hediger; Claude Berthon; Michel Bardet Study of liquid–liquid interfaces by an easily implemented localized NMR sequence, Magnetic Resonance in Chemistry, Volume 48 (2010) no. 8, p. 600 | DOI:10.1002/mrc.2628
Giuseppe Modolo Actinide(III) Recovery from High Active Waste Solutions Using Innovative Partitioning Processes, Nuclear Energy and the Environment, Volume 1046 (2010), p. 89 | DOI:10.1021/bk-2010-1046.ch008
G. Benay; R. Schurhammer; G. Wipff BTP-based ligands and their complexes with Eu3+ at “oil”/water interfaces. A molecular dynamics study, Physical Chemistry Chemical Physics, Volume 12 (2010) no. 36, p. 11089 | DOI:10.1039/c000772b
T. Kobayashi; T. Yaita; S. Suzuki; H. Shiwaku; Y. Okamoto; K. Akutsu; Y. Nakano; Y. Fujii Effect of the Introduction of Amide Oxygen into 1,10-Phenanthroline on the Extraction and Complexation of Trivalent Lanthanide in Acidic Condition, Separation Science and Technology, Volume 45 (2010) no. 16, p. 2431 | DOI:10.1080/01496395.2010.510094
P. Deepika; K. N. Sabharwal; T. G. Srinivasan; P. R. Vasudeva Rao Studies on the Use ofN,N,N´,N´-Tetra(2-ethylhexyl) Diglycolamide (TEHDGA) for Actinide Partitioning. I: Investigation on Third-Phase Formation and Extraction Behavior, Solvent Extraction and Ion Exchange, Volume 28 (2010) no. 2, p. 184 | DOI:10.1080/07366290903565885
Michael F. Schettini; Guang Wu; Trevor W. Hayton Coordination of N-Donor Ligands to a Uranyl(V) β-Diketiminate Complex, Inorganic Chemistry, Volume 48 (2009) no. 24, p. 11799 | DOI:10.1021/ic9018508
Skye Fortier; Guang Wu; Trevor W. Hayton Synthesis and Redox Chemistry of High-Valent Uranium Aryloxides, Inorganic Chemistry, Volume 48 (2009) no. 7, p. 3000 | DOI:10.1021/ic802266y
Bohumír Grüner; Magdaléna Kvíčalová; Jaromír Plešek; Václav Šícha; Ivana Císařová; Mária Lučaníková; Pavel Selucký Cobalt bis(dicarbollide) ions functionalized by CMPO-like groups attached to boron by short bonds; efficient extraction agents for separation of trivalent f-block elements from highly acidic nuclear waste, Journal of Organometallic Chemistry, Volume 694 (2009) no. 11, p. 1678 | DOI:10.1016/j.jorganchem.2008.11.056
María Teresa Murillo; Amparo G. Espartero; Jorge Sánchez‐Quesada; Javier de Mendoza; Pilar Prados Synthesis of Pre‐Organized Bisdiglycolamides (BisDGA) and Study of their Extraction Properties for Actinides(III) and Lanthanides(III), Solvent Extraction and Ion Exchange, Volume 27 (2009) no. 2, p. 107 | DOI:10.1080/07366290802672212
Aurélien Pitois; Laura Aldave de Las Heras; Maria Betti Determination of fission products in nuclear samples by capillary electrophoresis-inductively coupled plasma mass spectrometry (CE-ICP-MS), International Journal of Mass Spectrometry, Volume 270 (2008) no. 3, p. 118 | DOI:10.1016/j.ijms.2007.11.012
Jerzy Narbutt; Jadwiga Krejzler Neutral bidentate N-heterocyclic ligands – phase transfer reagents improving the kinetics of solvent extraction of Am(III) and Eu(III) ions with tetradentate 6,6′-bis-(diethyl-1,2,4-triazin-3-yl)-2,2′-bipyridine, Radiochimica Acta, Volume 96 (2008) no. 4-5, p. 219 | DOI:10.1524/ract.2008.1482
N. Nguyen; A. Ducouret; F. Studer; V. Aubin; D. Caurant; D. Gourier; J -M. Costantini Defects induced by electron irradiation in hollandite ceramics, specific radioactive cesium-host wasteforms: a 57Fe Mössbauer study, ICAME 2005 (2007), p. 489 | DOI:10.1007/978-3-540-49850-6_76
N. Dacheux; S. Grandjean; J. Rousselle; N. Clavier Hydrothermal Method of Preparation of Actinide(IV) Phosphate Hydrogenphosphate Hydrates and Study of Their Conversion into Actinide(IV) Phosphate Diphosphate Solid Solutions, Inorganic Chemistry, Volume 46 (2007) no. 24, p. 10390 | DOI:10.1021/ic701297v
Daniel Caurant; Pascal Loiseau; Isabelle Bardez; Christel Gervais Effect of Al2O3 concentration on zirconolite (Ca(Zr,Hf)Ti2O7) crystallization in (TiO2,ZrO2,HfO2)-rich SiO2–Al2O3–CaO–Na2O glasses, Journal of Materials Science, Volume 42 (2007) no. 20, p. 8558 | DOI:10.1007/s10853-007-1810-8
Daniel Caurant; Isabelle Bardez; Pascal Loiseau Crystallization of CaHf1−xZrxTi2O7 (0 ≤ x ≤ 1) zirconolite in SiO2–Al2O3–CaO–Na2O–TiO2–HfO2–ZrO2–Nd2O3 glasses, Journal of Materials Science, Volume 42 (2007) no. 24, p. 10203 | DOI:10.1007/s10853-007-1979-x
G. Bilancia; D. Arginelli; G. Brunnetti; S. Sabbinoneda Determination of plutonium and 90Sr in air particulate samples, Journal of Radioanalytical and Nuclear Chemistry, Volume 271 (2007) no. 2, p. 475 | DOI:10.1007/s10967-007-0233-y
G. Chevrot; R. Schurhammer; G. Wipff Synergistic effect of dicarbollide anions in liquid–liquid extraction: a molecular dynamics study at the octanol–water interface, Phys. Chem. Chem. Phys., Volume 9 (2007) no. 16, p. 1991 | DOI:10.1039/b616753e
E. A. Mowafy Application of N,N′‐Dimethyl‐N,N′‐Di(4‐Chlorophenyl)Tetradecyl Malonamide for the Selective Recovery of Iron(III) from Concentrated Chloride Solutions, Solvent Extraction and Ion Exchange, Volume 25 (2007) no. 6, p. 791 | DOI:10.1080/07366290701634321
N. Nguyen; A. Ducouret; F. Studer; V. Aubin; D. Caurant; D. Gourier; J.-M. Costantini Defects induced by electron irradiation in hollandite ceramics, specific radioactive cesium-host wasteforms: a 57Fe Mössbauer study, Hyperfine Interactions, Volume 166 (2006) no. 1-4, p. 489 | DOI:10.1007/s10751-006-9313-6
J. Warchoł; P. Misaelides; R. Petrus; D. Zamboulis Preparation and application of organo-modified zeolitic material in the removal of chromates and iodides, Journal of Hazardous Materials, Volume 137 (2006) no. 3, p. 1410 | DOI:10.1016/j.jhazmat.2006.04.028
D. Caurant; O. Majerus; P. Loiseau; I. Bardez; N. Baffier; J.L. Dussossoy Crystallization of neodymium-rich phases in silicate glasses developed for nuclear waste immobilization, Journal of Nuclear Materials, Volume 354 (2006) no. 1-3, p. 143 | DOI:10.1016/j.jnucmat.2006.03.014
V Aubin-Chevaldonnet; D Gourier; D Caurant; S Esnouf; T Charpentier; J M Costantini Paramagnetic defects induced by electron irradiation in barium hollandite ceramics for caesium storage, Journal of Physics: Condensed Matter, Volume 18 (2006) no. 16, p. 4007 | DOI:10.1088/0953-8984/18/16/009
A.P. Paiva; M.C. Costa Application of N,N′-tetrasubstituted malonamides to the recovery of iron(III) from chloride solutions, Hydrometallurgy, Volume 77 (2005) no. 1-2, p. 103 | DOI:10.1016/j.hydromet.2004.10.014
F. Goubard; P. Griesmar; A. Tabuteau Alpha self-irradiation effects in ternary oxides of actinides elements: The zircon-like phases AmIIIVO4 and AIINpIV(VO4)2 (A=Sr, Pb), Journal of Solid State Chemistry, Volume 178 (2005) no. 6, p. 1898 | DOI:10.1016/j.jssc.2005.03.039
Jennifer L. Ladd-Lively; Barry B. Spencer; Robert M. Counce Separation of Cesium and Strontium from Residues Arising from Fluoride Volatility Processing of Spent Nuclear Fuel, Separation Science and Technology, Volume 40 (2005) no. 1-3, p. 17 | DOI:10.1081/ss-200041756
G. Bilancia; A. Facchini; M. Ferrando; M. Giola; F. Maluta; M. Mariani; M. Mazzuccato; C. Madic; S. Sabbioneda Selective Actinide Extraction with a Tri‐Synergistic Mixture Using a Centrifugal Contactor Battery, Solvent Extraction and Ion Exchange, Volume 23 (2005) no. 6, p. 773 | DOI:10.1080/07366290500294905
P. Loiseau; D. Caurant; N. Baffier; L. Mazerolles; C. Fillet Glass–ceramic nuclear waste forms obtained from SiO2–Al2O3–CaO–ZrO2–TiO2 glasses containing lanthanides (Ce, Nd, Eu, Gd, Yb) and actinides (Th): study of internal crystallization, Journal of Nuclear Materials, Volume 335 (2004) no. 1, p. 14 | DOI:10.1016/j.jnucmat.2004.05.020
Jean-Paul Grouiller; Sylvie Pillon; Cyrille de Saint Jean; Frederic Varaine; Lydie Leyval; Guy Vambenepe; Bertrand Carlier Minor actinides transmutation scenario studies with PWRs, FRs and moderated targets, Journal of Nuclear Materials, Volume 320 (2003) no. 1-2, p. 163 | DOI:10.1016/s0022-3115(03)00184-3
V. Aubin; D. Caurant; D. Gourier; N. Baffier; S. Esnouf; T. Advocat Radiation Effects on Hollandite Ceramics developed for Radioactive Cesium Immobilization, MRS Proceedings, Volume 792 (2003) | DOI:10.1557/proc-792-r2.3
T. Advocat; F. Jorion; T. Marcillat; G. Leturcq; X. Deschanels; J. M. Boubals; L. Bojat; P. Nivet; S. Peuget Fabrication of 239/238Pu-Zirconolite Ceramic Pellets by Natural Sintering, MRS Proceedings, Volume 807 (2003) | DOI:10.1557/proc-807-267
Gérard Cote The supramolecular speciation: a key for improved understanding and modelling of chemical reactivity in complex systems, Radiochimica Acta, Volume 91 (2003) no. 11, p. 639 | DOI:10.1524/ract.91.11.639.23471

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