Hostname: page-component-78c5997874-g7gxr Total loading time: 0 Render date: 2024-11-17T16:11:19.564Z Has data issue: false hasContentIssue false
  • English
  • Français

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
Get access

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

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

1. Thomas, L.E. and Einziger, R.E., Mater. Charact. 28, 149 (1992).Google Scholar
2. Einziger, R.E., Thomas, L.E., Buchanan, H.C. and Stout, R.B., presented at 3rd Int. HLRWM Conference, Las Vegas, NV, 1992.Google Scholar
3. Eringen, A.C., Mechanics of Continua, (John Wiley & Sons, New York, 1967).Google Scholar
4. Sedov, L.I., Continuum Mechanics (Wolters and Noordnoft, Netherlands, 1972).Google Scholar
5. Wagner, C. and Schottky, W., Z. Physik Chemie 11, 163 (1930).Google Scholar
6. Smoluckowski, R., in Phase Transformation in Solids, edited by Smoluckowski, R., Mayer, J.E. and Weyl, W.A., (John Wiley & Sons, New York, 1951) p. 149;Google Scholar
Buerger, M.J., in Phase Transformation in Solids, edited by Smoluckowski, R., Mayer, J.E. and Weyl, W.A., (John Wiley & Sons, New York, 1951, p. 183;Google Scholar
Geisler, A.H., in Phase Transformation in Solids, edited by Smoluckowski, R., Mayer, J.E. and Weyl, W.A., (John Wiley & Sons, New York, 1951, p. 387;Google Scholar
Cohen, M., in Phase Transformation in Solids, edited by Smoluckowski, R., Mayer, J.E. and Weyl, W.A., (John Wiley & Sons, New York, 1951, p. 588.Google Scholar
7. Rees, A.L.G., Chemistry of the Defect Solid State, (Methuens Monographs, London, 1954).Google Scholar
8. Wojciechowski, K.F., Physics 27, 509 (1961).Google Scholar
9. Li, J.C.M., Oriani, R.A. and Darken, L.S., Z. Physik Chemie NF 49, 271 (1966).Google Scholar
10. Anderson, J.S. in Problems of Non-stoichiometry, edited by Rabenau, A., (North Holland & Elsevier, 1970), p. 1;Google Scholar
Jeannin, Y.P., in Problems of Non-stoichiometry, edited by Rabenau, A., (North Holland & Elsevier, 1970), p. 77;Google Scholar
Jagodzinski, H., in Problems of Non-stoichiometry, edited by Rabenau, A., (North Holland & Elsevier, 1970), p. 131.Google Scholar
11. Gibbs, J.W., The Scientific Papers of J. Willard Gibbs (Dover, Inc., New York, 1961).Google Scholar
12. Boltzmann, L., Lectures on Gas Theory, translation by Brush, Stephen G., (Univ. of California Press, Berkeley, CA, 1964).Google Scholar
13. Onsager, L., Physics Rev. 37, 405 (1931); and 38, 2265 (1931).Google Scholar
14. Stout, R.B., Crystal Lattice Defects 9, 65 (1981).Google Scholar
15. Stout, R.B., in Wave Propagation in Granular Media, edited by Karamonlidis, D. and Stout, R. B. (AMD 101, ASME, New York, 1989) p. 51.Google Scholar