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Influence of oxygen partial pressure on defect concentrations and on oxygen diffusion in UO2+x

Abstract : The hyperstoichiometric uranium dioxide (UO2+x) is stable over a wide range of temperature and compositions. Such variations of composition and the eventual presence of doping elements or impurities lead to a variation of anionic and electronic defect concentrations. Moreover, many properties of this material are affected by its composition modifications, in particular their atomic transport properties. Firstly we developed a point defect model to evaluate the dependence of the electronic and oxygen defect concentrations upon temperature, equilibrium oxygen partial pressure and impurity content. The physical constants of the model, in particular the equilibrium constants of the defect formation reactions were determined from deviation from stoichiometry and electrical conductivity measurements of literature. This work enabled us to interpret our measures of conductivity, oxygen chemical and self- diffusion coefficients. From a quantitative standpoint, the analysis of our experimental results allows to evaluate the oxygen interstitial diffusion coefficient but also its formation energy. Moreover, an estimate of oxygen di-interstitial formation energy is also provided. Presence of oxygen clusters leads oxygen self- and chemical diffusion to decrease. X-ray Absorption Spectroscopy characterization shows the presence of the same defect in the entire deviation from stoichiometry studied, confirming the approach used to develop the model.
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Elisabetta Pizzi. Influence of oxygen partial pressure on defect concentrations and on oxygen diffusion in UO2+x. Other. Ecole Centrale Paris, 2013. English. ⟨NNT : 2013ECAP0059⟩. ⟨tel-00969106⟩

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