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Alteration of a Zirconolite Glass-Ceramic Matrix under Hydrothermal Conditions

Published online by Cambridge University Press:  21 March 2011

Christelle Martin
Commissariat à l'énergie Atomique (CEA), Valrhû–Marcoule BP 17171, 30207 Bagnols-sur-Cèze Cedex, France
Isabelle Ribet
Commissariat à l'énergie Atomique (CEA), Valrhû–Marcoule BP 17171, 30207 Bagnols-sur-Cèze Cedex, France
Thierry Advocat
Commissariat à l'énergie Atomique (CEA), Valrhû–Marcoule BP 17171, 30207 Bagnols-sur-Cèze Cedex, France
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Glass-ceramic matrices based on zirconolite (CaZrTi2O7) are being considered for specific conditioning of plutonium or the minor actinides. The actinides are distributed throughout the zirconolite crystals and the residual glass phase. Since zirconolite alteration is extremely limited, however, actinide release from the glass-ceramic material is mainly attributable to alteration of the residual glass. Zirconolite glass-ceramic specimens and specimens corresponding to the residual glass phase alone were therefore altered under hydrothermal conditions (150°C) and under initial rate conditions (100°C) to compare their kinetic behavior and estimate the effect of the crystals on material alteration. Under hydrothermal conditions, alteration occurred during the first few days: SEM observations showed greater alteration of the glass-ceramic material due to a phenomenon of preferential glass alteration around the zirconolite crystals; after three days the alteration rate had considerably diminished and both specimens exhibited similar behavior. Under initial rate conditions the initial rates differed due to a variation in the reactive surface area of the glass-ceramic.

Research Article
Copyright © Materials Research Society 2002

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