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Melted Synthetic Zirconolite-Based Matrices: Effect of Cooling Rate and Heat Treatment on Ceramic Microstructure and Chemical Durability

Published online by Cambridge University Press:  21 March 2011

T. Advocat ,
P.J. McGlinn ,
C Fillet ,
G. Leturcq ,
S. Schuller ,
A. Bonnetier  and
K. Hart
T. Advocat
Affiliation:
CEA/SCD-Marcoule, BP 171 30207 Bagnols-sur-Cèze Cedex, France
P.J. McGlinn
Affiliation:
ANSTO, New Illawarra Road, Menai PMB1, NSW2234, Australia
C Fillet
Affiliation:
CEA/SCD-Marcoule, BP 171 30207 Bagnols-sur-Cèze Cedex, France
G. Leturcq
Affiliation:
ANSTO, New Illawarra Road, Menai PMB1, NSW2234, Australia
S. Schuller
Affiliation:
CEA/SCD-Marcoule, BP 171 30207 Bagnols-sur-Cèze Cedex, France
A. Bonnetier
Affiliation:
CEA/SCD-Marcoule, BP 171 30207 Bagnols-sur-Cèze Cedex, France
K. Hart
Affiliation:
ANSTO, New Illawarra Road, Menai PMB1, NSW2234, Australia
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Abstract

The heat treatment conditions are a key factor in fabricating zirconolite ceramics and glass-ceramics following high-temperature melting. An oxide mixture melted at 1450°C and subsequently heat-treated at 1200°C yielded a glass-ceramic containing crystallized zirconolite–2M. The silica-enriched residual glass represented about 60-70 vol% of the total; the actinide surrogates (Nd, Ce)were equally distributed between the residual glass and the zirconolite crystals. Zirconolite ceramics obtained after melting an oxide mixture at 1600–1700°C consisted of zirconolite, perovskite and rutile. Rapid cooling rates (> 100°#x00B0;··min-1) were obtained by pouring the melt into ingot molds; the resulting zirconolite ceramics were characterized by crystals of zirconolite-2M ranging from 1 to no more than 20 μm. Slow cooling (< 25°C#x00B0;··min-1 produced ceramics with crystals several hundred micrometers long. Despite the microstructural differences, the chemical durability of the zirconolite ceramics was identical. The initial alteration rates r 0 were about two orders of magnitude lower than those measured for the residual aluminosilicate glass of the zirconolite glass-ceramics. Moreover, during long-term leach tests at high S/V ratios to obtain advanced degrees of reaction progress, the alteration rates of all the materials diminished by over 3 to 4 orders of magnitude below r 0.

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Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 663: Symposium – Scientific Basis for Nuclear Waste management XXIV , 2000 , 277
Copyright
Copyright © Materials Research Society 2001

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References

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