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Kinematics and Thermodynamics of Non-Stoichiometric Oxidation Phase Transitions in Spent Fuel

Published online by Cambridge University Press:  01 January 1992

R. B. Stout ,
E.J. Kansa  and
A.M. Wijesinghe
R. B. Stout
Affiliation:
Univ. of Califomia/LLNL, P.O. Box 808, L-201, Livermore, CA 94551
E.J. Kansa
Affiliation:
Univ. of Califomia/LLNL, P.O. Box 808, L-201, Livermore, CA 94551
A.M. Wijesinghe
Affiliation:
Univ. of Califomia/LLNL, P.O. Box 808, L-201, Livermore, CA 94551
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Abstract

At low temperatures (<200°C), spent fuel from power reactors oxidizes from its UO2 lattice to a U4O9 lattice but with an oxygen-to-uranium (O/U) ratio of ∼2.4. Also, the weight gain time response has a plateau as the O/U approaches 2.4. Part of this response results from a geometrical dependency as a U4O9 oxidation front propagates into grain volumes of UO2. It may also be indicative of a metastable, non-stoichiometric U4O9 phase whose existence may inhibit the transition kinetics to the next expected phase of U3O8. To gain a mechanistic understanding and to plan future oxidation tests, lattice kinematic and thermodynamic models are developed for lattice deformations and energetics of lattice phase changes (UO2 → U4O9 → U3O7 → U3O8) that include zeroth order influences on oxidation kinetics due to interstitial oxygen atoms and vacancies plus interstitial and substitutional actinides and fission decay products in spent fuel.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 294: Symposium V – Scientific Basis for Nuclear Waste Management XVI , 1992 , 25
Copyright
Copyright © Materials Research Society 1993

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