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Structural and Crystallization Study of a Simplified Aluminoborosilicate Nuclear Glass Containing Rare-earths: Effect of ZrO2 Concentration

Published online by Cambridge University Press:  01 February 2011

Daniel Caurant ,
Arnaud Quintas ,
Odile Majerus ,
Pascal Loiseau ,
Thibault Charpentier ,
Philippe Vermaut  and
Jean-Luc Dussossoy
Daniel Caurant
Affiliation:
daniel-caurant@enscp.fr, CNRS, ENSCP LCMCP, PARIS, France
Arnaud Quintas
Affiliation:
arnaud.quintas@areva.com, CNRS, ENSCP LCMCP, PARIS, France
Odile Majerus
Affiliation:
odile-majerus@chimie-paristech.fr, CNRS, ENSCP LCMCP, PARIS, France
Pascal Loiseau
Affiliation:
pascal-loiseau@chimie-paristech.fr, CNRS, ENSCP LCMCP, PARIS, France
Thibault Charpentier
Affiliation:
thibault.charpentier@cea.fr, CEA, CEA CNRS UMR 3299, Gif-sur-Yvette, France
Philippe Vermaut
Affiliation:
philippe-vermaut@chimie-paristech.fr, ENSCP, CNRS UMR 7045, PARIS, France
Jean-Luc Dussossoy
Affiliation:
jean-luc.dussossoy@cea.fr, CEA, Department of Nuclear Energy, Bagnols-sur-Ceze, France
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Abstract

Zirconium is an abundant element in nuclear wastes. In this paper, we present structural and crystallization results for a simplified glass composition belonging to the SiO2-Al2O3-B2O3-Na2O-CaO-ZrO2-RE2O3 system (RE = Nd or La) developed to immobilize highly concentrated waste solutions. The effect of varying ZrO2 content on the structure and the crystallization tendency of this glass was studied using a multi-spectroscopic approach. Zr was shown to be located in six-fold coordinated sites whose charge compensation seems preferentially insured by Na+ cations. Whereas a significant decrease of the proportion of BO4 units was observed with ZrO2 content, no effect was detected on the environment of AlO4 units. However, a significant structural evolution of the silicate network occurred due to the formation of Si-O-Zr bonds. Whatever ZrO2 concentration, the crystallization of only a rare earth silicate apatite phase was observed during either slow cooling from the melt or isothermal heat treatment. Whereas nucleation mainly occurred from the surface of the glass without ZrO2, the introduction of zirconium induced apatite crystallization in the bulk. It is proposed that this nucleating effect of ZrO2 is mainly due to changes induced in the neighborhood of Nd3+ cations in glass structure.

Keywords

Zrwaste managementnuclear materials
Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 1265: Symposium AA – Scientific Basis for Nuclear Waste Management XXXIV , 2010 , 1265-AA03-02
Copyright
Copyright © Materials Research Society 2010

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References

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