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Development of Zirconolite-based Glass-Ceramics for the Conditioning of Actinides

Published online by Cambridge University Press:  21 March 2011

P. Loiseau ,
D. Caurant ,
N. Baffier ,
L. Mazerolles  and
C. Fillet
P. Loiseau
Affiliation:
de Chimie Appliquée de l'Etat Solide (UMR CNRS 7574), ENSCP, 11 rue P. et M. Curie, 75231 Paris Cedex 05, France
D. Caurant
Affiliation:
de Chimie Appliquée de l'Etat Solide (UMR CNRS 7574), ENSCP, 11 rue P. et M. Curie, 75231 Paris Cedex 05, France
N. Baffier
Affiliation:
de Chimie Appliquée de l'Etat Solide (UMR CNRS 7574), ENSCP, 11 rue P. et M. Curie, 75231 Paris Cedex 05, France
L. Mazerolles
Affiliation:
Centre d'Etudes de Chimie Métallurgique (CECM, UPR CNRS 2801), 15 rue Georges Urbain, 94407 Vitry-sur-Seine Cedex, France
C. Fillet
Affiliation:
Commissariat à l'Energie Atomique (CEA), Centre d'Etudes de la Vallée du Rhône, DCC/DRRV/SCD/LEBM, BP 171, 30207 Bagnols-sur-Céze, France
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Abstract

Zirconolite (CaZrTi2O7) based glass-ceramics designed for the specific immobilization of plutonium wastes or minor actinides (Np, Am, Cm) from high level radioactive wastes were investigated. To reach an efficient double containment, actinides must be preferentially located in the crystalline phase, which is homogeneously dispersed in a calcium aluminosilicate residual glass. Several heat treatments (between 950° and 1350°C) of a parent glass belonging to the SiO2-Al2O3-CaO system and containing TiO2 and ZrO2 were performed to prepare glass-ceramics. Trivalent minor actinides were simulated introducing Nd2O3 in the glass composition. Electron microscopy, X-ray diffraction (XRD) and thermal analysis have shown that devitrification processes in the bulk and on glass surface are different. They lead to the crystallization of zirconolite in the bulk and to a mixture of titanite (CaTiSiO5) and anorthite (CaAl2Si2O8) near the surface. For heat treatment temperatures greater than or equal to 1250°C, baddeleyite (m-ZrO2) crystals form at the expense of zirconolite in the bulk of glass-ceramics. XRD indicates that the order in zirconolite Ca/Zr planes increases with heating temperature. At the same time, extended defects density decreases.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 663: Symposium – Scientific Basis for Nuclear Waste management XXIV , 2000 , 179
Copyright
Copyright © Materials Research Society 2001

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