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Zirconolite-based glass-ceramics for actinides immobilization: Effects of glass composition and of actinides simulant nature

Published online by Cambridge University Press:  11 February 2011

Pascal Loiseau
Affiliation:
LCAES (UMR 7574), ENSCP, 11 rue Pierre et Marie Curie 75231 Paris Cedex 05, FRANCE
Daniel Caurant
Affiliation:
LCAES (UMR 7574), ENSCP, 11 rue Pierre et Marie Curie 75231 Paris Cedex 05, FRANCE
Isabelle Bardez
Affiliation:
LCAES (UMR 7574), ENSCP, 11 rue Pierre et Marie Curie 75231 Paris Cedex 05, FRANCE
Odile Majerus
Affiliation:
LCAES (UMR 7574), ENSCP, 11 rue Pierre et Marie Curie 75231 Paris Cedex 05, FRANCE
Noël Baffier
Affiliation:
LCAES (UMR 7574), ENSCP, 11 rue Pierre et Marie Curie 75231 Paris Cedex 05, FRANCE
Catherine Fillet
Affiliation:
CEA, DEN/DIEC/SCDV/LEBM, 30207 Bagnols-sur-Cèze, FRANCE
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Abstract

Zirconolite (CaZrTi2O7) based glass-ceramics, in which the crystalline phase (aimed at preferentially incorporating minor actinides or Pu) is embedded in a durable calcium aluminosilicate glassy matrix, can be envisaged as good waste form candidates. In this study, the effect of parent glass composition – and particularly of TiO2, ZrO2, CaO and Al2O3 amounts -on the microstructure and the structure of the glass-ceramics obtained after controlled devitrification (nucleation + crystal growth) is reported. It clearly appears that the volume percentage of zirconolite crystals and their nucleation rate in the bulk of the glass strongly depends both on (CaO + ZrO2 + TiO2) and Al2O3 amounts in parent glass. Neodymium is mainly used to simulate trivalent minor actinides whereas several samples were also prepared with other lanthanides (Ce, Eu, Gd, Yb) in order to investigate the effect of simulant field strength in glass on the nature and the composition of the crystals formed. The effect of partial or total molar substitution of ZrO2 by HfO2 in parent glass composition was also studied in order to prepare Ca(Zr1-xHfx)Ti2O7 (0 < × ≤ 1) based glass-ceramics which could be interesting in order to minimize criticality problems.

Type
Research Article
Copyright
Copyright © Materials Research Society 2003

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References

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