Impact of Hydrogen on the Intermediate Oxygen Clusters and Diffusion in Fluorite Structured UO 2+x

Joseph Flitcroft, Adam Symington, Marco Molinari, Nicholas A. Brincat, Nicholas R. Williams, Stephen C. Parker

Research output: Contribution to journalArticle

Abstract

Uranium dioxide is the most prevalent nuclear fuel. Defect clusters are known to be present in significant concentrations in hyperstoichoimetric uranium oxide, UO2+x, and have a significant impact on the corrosion of the material. A detailed understanding of the defect clusters that form is required for accurate diffusion models in UO2+x. Using ab initio
calculations, we show that at low excess oxygen concentration, where defects are mostly isolated oxygen interstitials, hydrogen stabilizes the initial clustering. The simplest cluster at this low excess oxygen stoichiometry consists of a pair of oxygen ions bound to an oxygen vacancy, namely the split mono-interstital, which resembles larger split interstitials clusters in UO2+x. Our data shows that, depending on local hydrogen concertation, the presence of hydrogen stabilizes this cluster over isolated oxygen interstitials.
Original languageEnglish
Pages (from-to)3774-3779
Number of pages6
JournalInorganic Chemistry
Volume58
Issue number6
Early online date5 Mar 2019
DOIs
Publication statusPublished - 2019

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Fluorspar
fluorite
Hydrogen
Oxygen
oxygen
hydrogen
interstitials
Defects
defects
uranium oxides
nuclear fuels
Nuclear fuels
Oxygen vacancies
oxygen ions
dioxides
Stoichiometry
uranium
stoichiometry
corrosion
Ions

Cite this

Flitcroft, Joseph ; Symington, Adam ; Molinari, Marco ; Brincat, Nicholas A. ; Williams, Nicholas R. ; Parker, Stephen C. / Impact of Hydrogen on the Intermediate Oxygen Clusters and Diffusion in Fluorite Structured UO 2+x. In: Inorganic Chemistry. 2019 ; Vol. 58, No. 6. pp. 3774-3779.
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Impact of Hydrogen on the Intermediate Oxygen Clusters and Diffusion in Fluorite Structured UO 2+x. / Flitcroft, Joseph; Symington, Adam ; Molinari, Marco; Brincat, Nicholas A.; Williams, Nicholas R.; Parker, Stephen C.

In: Inorganic Chemistry, Vol. 58, No. 6, 2019, p. 3774-3779.

Research output: Contribution to journalArticle

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AU - Molinari, Marco

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