Diffusion of Zr, Ru, Ce, Y, La, Sr and Ba fission products in UO 2

Perriot, R.; Liu, X. -Y.; Stanek, C. R.; Andersson, D. A.

doi:10.1016/j.jnucmat.2015.01.001

Title: Diffusion of Zr, Ru, Ce, Y, La, Sr and Ba fission products in UO ₂

Journal Article · Thu Jan 08 00:00:00 EST 2015 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2015.01.001· OSTI ID:1402584

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Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

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.

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Research Organization:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1402584

Alternate ID(s):: OSTI ID: 1246599

Report Number(s):: LA-UR-14-28421; TRN: US1703113

Journal Information:: Journal of Nuclear Materials, Vol. 459, Issue C; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 15 works

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Title: Diffusion of Zr, Ru, Ce, Y, La, Sr and Ba fission products in UO ₂