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Durability of Zirconolite in Hydrothermal Fluids: Implications for Nuclear Waste Disposal

Published online by Cambridge University Press:  21 March 2011

R. Gieré ,
J. Malmström ,
E. Reusser ,
G.R. Lumpkin ,
M. Düggelin ,
D. Mathys ,
R. Guggenheim  and
D. Günther
R. Gieré
Affiliation:
Earth & Atmospheric Sciences, Purdue University, West Lafayette, IN 47907-1397, USA; Email: giere@purdue.edu
J. Malmström
Affiliation:
Institute of Mineralogy and Petrography, ETH-Zentrum, 8092 Zürich, Switzerland
E. Reusser
Affiliation:
Institute of Mineralogy and Petrography, ETH-Zentrum, 8092 Zürich, Switzerland
G.R. Lumpkin
Affiliation:
Australian Nuclear Science & Technology Organisation, Menai, NSW 2234, Australia
M. Düggelin
Affiliation:
SEM-Laboratory, University of Basel, Klingelbergstrasse 50, 4056 Basel, Switzerland
D. Mathys
Affiliation:
SEM-Laboratory, University of Basel, Klingelbergstrasse 50, 4056 Basel, Switzerland
R. Guggenheim
Affiliation:
SEM-Laboratory, University of Basel, Klingelbergstrasse 50, 4056 Basel, Switzerland
D. Günther
Affiliation:
Institute of Inorganic Chemistry, ETH-Zentrum, 8092 Zürich, Switzerland
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Abstract

Synthetic zirconolite (CaZrTi2O7) doped with rare earth elements (REEs) and Hf has been subjected to corrosion tests in a closed system at elevated temperature and pressure in fluids with various compositions. Together with previous studies, the results indicate only a very weak corrosion below 250°C at a pressure of 50 MPa. Above that temperature and up to 500°C zirconolite suffers from relatively rapid corrosion and, depending on the fluid composition, it may be covered by various secondary phases. Above 500°C in Na-rich fluids, zirconolite is replaced by perovskiteand calzirtite (nominally CaTiO3 and Ca2r5Ti2O16, respectively), but theREEs and Hf (acting as actinide analogues and/or neutron absorbers) are almost quantitatively incorporated into the secondary phases. The breakdown of zirconolite and its replacement by other phases in the laboratory tests are comparable to reactions observed in natural systems. Additional experiments with U-doped zirconolite revealed differences in the behavior of the used actinide analogues (Nd, Ce, Gd)and U during corrosion. The results of this study, together with observations on natural samples, strongly support the use of zirconolite-based ceramic waste forms for actinide-rich wastes.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 663: Symposium – Scientific Basis for Nuclear Waste management XXIV , 2000 , 267
Copyright
Copyright © Materials Research Society 2001

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References

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