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Room‐temperature diffusion coefficients for oxygen and water in UO 2 matrices: a SIMS study
Author(s) -
Marchetti I.,
Carbol P.,
Himbert J.,
Belloni F.,
Fanghänel T.
Publication year - 2013
Publication title -
surface and interface analysis
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.52
H-Index - 90
eISSN - 1096-9918
pISSN - 0142-2421
DOI - 10.1002/sia.5028
Subject(s) - grain boundary , grain boundary diffusion coefficient , arrhenius equation , chemistry , crystallite , analytical chemistry (journal) , secondary ion mass spectrometry , oxygen , thermal diffusivity , diffusion , uranium dioxide , atmospheric temperature range , effective diffusion coefficient , self diffusion , mineralogy , thermodynamics , materials science , activation energy , uranium , metallurgy , crystallography , mass spectrometry , microstructure , environmental chemistry , magnetic resonance imaging , chromatography , radiology , medicine , physics , organic chemistry , self service , business , marketing
To understand the mechanism of fuel oxidation, in the event of exposure of spent nuclear fuel to groundwater in a final repository, the key parameters are the diffusion coefficients for oxygen and water in UO 2 . In the temperature range relevant for geological disposal (20–100 °C), we conducted static corrosion experiments, for 3–6 months, with 18 O‐labelled water on different UO 2 matrices (single‐crystal, polycrystalline UO 2 , SIMFUEL) so that we could evaluate the penetration of the 18 O‐tracer by means of secondary ion mass spectrometry depth profiling, measuring the 18 O/ 16 O ratio. Fick's second law was applied to fit the diffusion profiles in the single crystal and to determine the chemical diffusion coefficient of oxygen, which was found to be in good agreement with the Arrhenius plot extrapolation from high‐temperature literature data. Profiles of polycrystalline UO 2 could be fitted with the Levine–MacCallum model, showing that grain boundaries behave like high‐diffusivity paths. The presence of secondary phases precipitated along the grain boundaries, as in the case of SIMFUEL, showed a hindering effect for this grain‐boundary diffusion, reducing the measured penetration depth. Copyright © 2012 John Wiley & Sons, Ltd.