Diffusion of Zr, Ru, Ce, Y, La, Sr and Ba fission products in UO 2
Abstract
The diffusivity of the solid fission products (FP) Zr (Zr4+), Ru (Ru4+, Ru3+), Ce (Ce4+), Y (Y3+), La (La3+), Sr (Sr2+) and Ba (Ba2+) by a vacancy mechanism has been calculated, using a combination of density functional theory (DFT) and empirical potential (EP) calculations. The activation energies for the solid fission products are compared to the activation energy for Xe fission gas atoms calculated previously. Apart from Ru, the solid fission products all exhibit higher activation energy than Xe. Furthermore, for all solid FPs except Y3+, the migration of the FP has lower barrier than the migration of a neighboring U atom, making the latter the rate limiting step for direct migration. An indirect mechanism, consisting of two successive migrations around the FP, is also investigated. The calculated diffusivities show that most solid fission products diffuse with rates similar to U self-diffusion. But, Ru, Ba and Sr exhibit faster diffusion than the other solid FPs, with Ru3+ and Ru4+ diffusing even faster than Xe for T < 1200 K. The diffusivities correlate with the observed fission product solubility in UO2, and the tendency to form metallic and oxide second phase inclusions.
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1402584
- Alternate Identifier(s):
- OSTI ID: 1246599
- Report Number(s):
- LA-UR-14-28421
Journal ID: ISSN 0022-3115; TRN: US1703113
- Grant/Contract Number:
- AC52-06NA25396
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Nuclear Materials
- Additional Journal Information:
- Journal Volume: 459; Journal Issue: C; Journal ID: ISSN 0022-3115
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 73 NUCLEAR PHYSICS AND RADIATION PHYSICS; 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS
Citation Formats
Perriot, R., Liu, X. -Y., Stanek, C. R., and Andersson, D. A. Diffusion of Zr, Ru, Ce, Y, La, Sr and Ba fission products in UO 2. United States: N. p., 2015.
Web. doi:10.1016/j.jnucmat.2015.01.001.
Perriot, R., Liu, X. -Y., Stanek, C. R., & Andersson, D. A. Diffusion of Zr, Ru, Ce, Y, La, Sr and Ba fission products in UO 2. United States. https://doi.org/10.1016/j.jnucmat.2015.01.001
Perriot, R., Liu, X. -Y., Stanek, C. R., and Andersson, D. A. Thu .
"Diffusion of Zr, Ru, Ce, Y, La, Sr and Ba fission products in UO 2". United States. https://doi.org/10.1016/j.jnucmat.2015.01.001. https://www.osti.gov/servlets/purl/1402584.
@article{osti_1402584,
title = {Diffusion of Zr, Ru, Ce, Y, La, Sr and Ba fission products in UO 2},
author = {Perriot, R. and Liu, X. -Y. and Stanek, C. R. and Andersson, D. A.},
abstractNote = {The diffusivity of the solid fission products (FP) Zr (Zr4+), Ru (Ru4+, Ru3+), Ce (Ce4+), Y (Y3+), La (La3+), Sr (Sr2+) and Ba (Ba2+) by a vacancy mechanism has been calculated, using a combination of density functional theory (DFT) and empirical potential (EP) calculations. The activation energies for the solid fission products are compared to the activation energy for Xe fission gas atoms calculated previously. Apart from Ru, the solid fission products all exhibit higher activation energy than Xe. Furthermore, for all solid FPs except Y3+, the migration of the FP has lower barrier than the migration of a neighboring U atom, making the latter the rate limiting step for direct migration. An indirect mechanism, consisting of two successive migrations around the FP, is also investigated. The calculated diffusivities show that most solid fission products diffuse with rates similar to U self-diffusion. But, Ru, Ba and Sr exhibit faster diffusion than the other solid FPs, with Ru3+ and Ru4+ diffusing even faster than Xe for T < 1200 K. The diffusivities correlate with the observed fission product solubility in UO2, and the tendency to form metallic and oxide second phase inclusions.},
doi = {10.1016/j.jnucmat.2015.01.001},
journal = {Journal of Nuclear Materials},
number = C,
volume = 459,
place = {United States},
year = {Thu Jan 08 00:00:00 EST 2015},
month = {Thu Jan 08 00:00:00 EST 2015}
}
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