Immobilization of tetravalent actinides in phosphate ceramics

Autor: Renaud Podor, Olivier Terra, Nicolas Dacheux, Fabienne Audubert
Přispěvatelé: Institut de Physique Nucléaire d'Orsay (IPNO), Université Paris-Sud - Paris 11 (UP11)-Institut National de Physique Nucléaire et de Physique des Particules du CNRS (IN2P3)-Centre National de la Recherche Scientifique (CNRS), Laboratoire des Technologies d'Elaboration des Combustibles (LTEC), Service Plutonium Uranium et Actinides mineurs (SPUA), Département d'Etudes des Combustibles (DEC), CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Département d'Etudes des Combustibles (DEC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Laboratoire de chimie du solide minéral (LCSM), Université Paul Verlaine - Metz (UPVM)-Université Henri Poincaré - Nancy 1 (UHP)-Centre National de la Recherche Scientifique (CNRS), C. Degueldre
Jazyk: angličtina
Rok vydání: 2005
Předmět:
Zdroj: Journal of Nuclear Materials
E-MRS 2005 Spring Meeting Symposium N on Nuclear Materials (including the 10th Inert Matrix Fuel Workshop)
E-MRS 2005 Spring Meeting Symposium N on Nuclear Materials (including the 10th Inert Matrix Fuel Workshop), May 2005, Strasbourg, France. pp.224-232, ⟨10.1016/j.jnucmat.2006.02.058⟩
ISSN: 0022-3115
DOI: 10.1016/j.jnucmat.2006.02.058⟩
Popis: Three phosphate-based ceramics were studied for the immobilization of tri- and tetravalent actinides: britholite Ca 9 Nd 1 - x An x IV ( PO 4 ) 5 - x ( SiO 4 ) 1 + x F 2 , monazite/brabantite Ln 1 - 2 x III Ca x An x IV PO 4 and thorium phosphate diphosphate β - Th 4 - x An x IV ( PO 4 ) 4 P 2 O 7 (β-TPD). For each material, the incorporation of thorium and uranium (IV) was examined through dry chemistry routes, using mechanical grinding of the initial mixtures then heating at high temperature (1373–1673 K). The quantitative incorporation of thorium in the britholite structure was obtained up to 20 wt% through the coupled substitution ( Nd 3 + , PO 4 3 - ) ⇔ ( Th 4 + , SiO 4 4 - ) . On the contrary, the incorporation of uranium was limited to 5–8 wt% and always led to a two-phase system composed by U-britholite and CaU2O5+y. The incorporation of Th and U(IV) was also examined in both matrices, β-TPD and monazite/brabantite solid solutions. Homogeneous and single phase samples of β-TUPD and (Th,U)-monazite/brabantite solid solutions were obtained using successive cycles of mechanical grinding/calcination. The three matrices were prepared in the pellet form then leached in 10−1 M or 10−4 M HNO3 at 363 K. The very low normalized dissolution rates confirmed the good resistance of the materials to aqueous alteration. Moreover, in over-saturation conditions, the formation of neoformed phases onto the surface of the pellets was evidenced for several sintered samples.
Databáze: OpenAIRE