Comptes Rendus
no. 7-8
Du combustible nucléaire aux déchets : recherches actuelles/From nuclear fuels to waste: current research
New conditionings for separated long-lived radionuclides
[Nouvelles matrices pour le conditionnement des radioéléments à vie longue]
Christophe Guy1  ; Fabienne Audubert1 ; Jean-Eric Lartigue1 ; Christelle Latrille1 ; Thierry Advocat2 ; Catherine Fillet2
1 CEA Cadarache, BP 108, 13108 St Paul-Lez-Durance, France
2 CEA Marcoule, BP 171, 30207 Bagnols-sur-Céze, France
Comptes Rendus. Physique, Volume 3 (2002) no. 7-8, pp. 827-837.

Les radioéléments à vie longue (Iode129, césium135 et actinides mineures) peuvent être incorporés dans des structures cristallines de matériaux spécifiques à haute durabilité chimique. Les apatites, la zirconolite, les monazites, le phosphate-diphosphate de thorium et la hollandite sont étudiés au CEA et dans le cadre d'un groupement de recherche (NOMADE). Une première étape est consacrée à la faisabilité scientifique visant à élaborer et caractériser les matériaux et à étudier leur durabilité chimique et leur comportement sous irradiation. Au stade actuel des recherches, le développement des apatites pour l'iode et les actinides, de la zirconolite, des monazites et du phosphate–diphosphate de thorium pour les actinides a atteint cette étape. Le conditionnement du césium dans la hollandite ou les minéraux phosphatés nécessite des développements supplémentaires.

Long-lived radionuclides such as I129, Cs135 and minor actinides can be incorporated in crystalline structures of several specific materials with high chemical durability. Apatites, zirconolite, monazites, thorium phosphate-diphosphate and hollandite are being studied at the CEA and among a scientific research group called NOMADE. A first step is devoted to the scientific feasibility dealing with elaboration and characterization of non-radioactive materials and studies of their chemical durability and radiation stability. Development of apatite for iodine and minor actinides, zirconolite for minor actinides, monazite for trivalent actinides and thorium phosphate–diphosphate for tetravalent actinides has reached the scientific feasibility. Cs conditioning in hollandite and phosphate minerals needs further studies.

Reçu le :
Révisé le :
Publié le :
DOI : 10.1016/S1631-0705(02)01377-4
Keywords: high level waste, conditioning, ceramic matrices
Mots-clés : déchets de haute activité, conditionnement, céramiques matrices

Christophe Guy 1 ; Fabienne Audubert 1 ; Jean-Eric Lartigue 1 ; Christelle Latrille 1 ; Thierry Advocat 2 ; Catherine Fillet 2

1 CEA Cadarache, BP 108, 13108 St Paul-Lez-Durance, France
2 CEA Marcoule, BP 171, 30207 Bagnols-sur-Céze, France 
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Christophe Guy; Fabienne Audubert; Jean-Eric Lartigue; Christelle Latrille; Thierry Advocat; Catherine Fillet. New conditionings for separated long-lived radionuclides. Comptes Rendus. Physique, Volume 3 (2002) no. 7-8, pp. 827-837. doi : 10.1016/S1631-0705(02)01377-4. https://comptes-rendus.academie-sciences.fr/physique/articles/10.1016/S1631-0705(02)01377-4/

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  • Regis Jardin; Claudiu C. Pavel; Philippe E. Raison; Daniel Bouëxière; Hernan Santa-Cruz; Rudy J.M. Konings; Karin Popa The high-temperature behaviour of PuPO4 monazite and some other related compounds, Journal of Nuclear Materials, Volume 378 (2008) no. 2, p. 167 | DOI:10.1016/j.jnucmat.2008.05.011
  • M. Tribet; N. Toulhoat; N. Moncoffre; Christophe Jegou; G. Leturcq; C. Corbel; P. Toulhoat Leaching of a zirconolite ceramic waste-form under proton and He2+ irradiation, Radiochimica Acta, Volume 96 (2008) no. 9-11, p. 619 | DOI:10.1524/ract.2008.1545
  • K. Rajesh; P. Shajesh; O. Seidel; P. Mukundan; K. G. K. Warrier A Facile Sol–Gel Strategy for the Synthesis of Rod‐Shaped Nanocrystalline High‐Surface‐Area Lanthanum Phosphate Powders and Nanocoatings, Advanced Functional Materials, Volume 17 (2007) no. 10, p. 1682 | DOI:10.1002/adfm.200600794
  • Claire Chaïrat; Eric H. Oelkers; Jacques Schott; Jean-Eric Lartigue Fluorapatite surface composition in aqueous solution deduced from potentiometric, electrokinetic, and solubility measurements, and spectroscopic observations, Geochimica et Cosmochimica Acta, Volume 71 (2007) no. 24, p. 5888 | DOI:10.1016/j.gca.2007.09.026
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  • 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
  • Jean-Marie Gras; Richard Do Quang; Hervé Masson; Thierry Lieven; Cécile Ferry; Christophe Poinssot; Michel Debes; Jean-Michel Delbecq Perspectives on the closed fuel cycle – Implications for high-level waste matrices, Journal of Nuclear Materials, Volume 362 (2007) no. 2-3, p. 383 | DOI:10.1016/j.jnucmat.2007.01.210
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  • Karin Popa; Damien Bregiroux; Rudy J.M. Konings; Thomas Gouder; Aurelian F. Popa; Thorsten Geisler; Philippe E. Raison The chemistry of the phosphates of barium and tetravalent cations in the 1:1 stoichiometry, Journal of Solid State Chemistry, Volume 180 (2007) no. 8, p. 2346 | DOI:10.1016/j.jssc.2007.06.006
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  • Ming Zhang; E.R. Maddrell; P.K. Abraitis; E.K.H. Salje Impact of leach on lead vanado-iodoapatite [Pb5(VO4)3I]: An infrared and Raman spectroscopic study, Materials Science and Engineering: B, Volume 137 (2007) no. 1-3, p. 149 | DOI:10.1016/j.mseb.2006.11.003
  • N. Kamel; H. Aït-Amar; A. Zahri The use of a soaking procedure combined with the sintering process to reach a high cerium content in a cerium-bearing Y-britholite, Progress in Nuclear Energy, Volume 49 (2007) no. 4, p. 351 | DOI:10.1016/j.pnucene.2007.03.002
  • O. Terra; N. Dacheux; F. Audubert; R. Podor Immobilization of tetravalent actinides in phosphate ceramics, Journal of Nuclear Materials, Volume 352 (2006) no. 1-3, p. 224 | DOI:10.1016/j.jnucmat.2006.02.058
  • Claire Chaïrat; Eric H. Oelkers; Jacques Schott; Jean-Eric Lartigue An experimental study of the dissolution rates of Nd-britholite, an apatite-structured actinide-bearing waste storage host analogue, Journal of Nuclear Materials, Volume 354 (2006) no. 1-3, p. 14 | DOI:10.1016/j.jnucmat.2006.01.022
  • 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
  • Olivier Terra; Fabienne Audubert; Nicolas Dacheux; Christophe Guy; Renaud Podor Synthesis and characterization of thorium-bearing britholites, Journal of Nuclear Materials, Volume 354 (2006) no. 1-3, p. 49 | DOI:10.1016/j.jnucmat.2006.02.094
  • D. Bregiroux; S. Lucas; E. Champion; F. Audubert; D. Bernache-Assollant Sintering and microstructure of rare earth phosphate ceramics REPO4 with RE=La, Ce or Y, Journal of the European Ceramic Society, Volume 26 (2006) no. 3, p. 279 | DOI:10.1016/j.jeurceramsoc.2004.11.004
  • Nelly Toulhoat; Nelly Toulhoat; Nathalie Moncoffre; Pierre Toulhoat; Christophe Jegou; Catherine Corbel; Isabelle Bardez; Gilles Leturcq Enhancement of Zirconolite Dissolution Due to Water Radiolysis, MRS Proceedings, Volume 985 (2006) | DOI:10.1557/proc-985-0985-nn09-04
  • M. Tribet; S. Gavarini; N. Toulhoat; N. Monocoffre; A. Chevarier; Christophe Jegou; G. Leturcq; C. Corbel; P. Toulhoat Leaching of zirconolite ceramics under H+ and He2+ irradiation, Radiochimica Acta, Volume 94 (2006) no. 9-11, p. 585 | DOI:10.1524/ract.2006.94.9-11.585
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  • E. R. Maddrell; P. K. Abraitis A Comparison of Wasteforms and Processes for the Immobilisation of Iodine-129, MRS Proceedings, Volume 807 (2003) | DOI:10.1557/proc-807-261
  • Damien Brégiroux; Fabienne Audubert; Eric Champion; Didier Bernache-Assollant Mechanical and thermal properties of hot pressed neodymium-substituted britholite Ca9Nd(PO4)5(SiO4)F2, Materials Letters, Volume 57 (2003) no. 22-23, p. 3526 | DOI:10.1016/s0167-577x(03)00120-4

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