Experimental measurements of Xe and Kr releases from UO2 and determination of their migration mechanisms - Release rate data.

We present the raw data obtained from release rate at 1300°C of Xe and Kr implanted in UO2, related to [1]. We performed different sample preparation (polishing treatment) on polycrystalline and monocrystalline UO2. Ion implantation were performed at various fluences between 9.5 × 1010 to 5 × 1014 i/cm2 in UO2 samples. Release rate of Xe and Kr are obtained at 1300°C under vacuum from desorption experiments performed on the PIAGARA plateform at the CENBG (Centre d'Etudes Nucléaires de Bordeaux-Gradignan). Since we made a variety of samples depending on multiple parameters (sample type, sample preparation, ion implantation type and fluence), these data represent a serious amount of work that could be saved for the scientific community that might use them for other purposes such as burst modelling.

Dissolution of cerium(IV)-lanthanide(III) oxides: comparative effect of chemical composition, temperature, and acidity.

The dissolution of Ce(1-x)Ln(x)O(2-x/2) solid solutions was undertaken in various acid media in order to evaluate the effects of several physicochemical parameters such as chemical composition, temperature, and acidity on the reaction kinetics. The normalized dissolution rates (R(L,0)) were found to be strongly modified by the trivalent lanthanide incorporation rate, due to the presence of oxygen vacancies decreasing the samples cohesion. Conversely, the nature of the trivalent cation considered only weakly impacted the R(L,0) values. The dependence of the normalized dissolution rates on the temperature then appeared to be of the same order of magnitude than that of chemical composition. Moreover, it allowed determining the corresponding activation energy (E(A) ≈ 60-85 kJ·mol(-1)) which accounts for a dissolution driven by surface-controlled reactions. A similar conclusion was made regarding the acidity of the solution: the partial order related to (H(3)O(+)) reaching about 0.7. Finally, the prevailing effect of the incorporation of aliovalent cations in the fluorite-type CeO(2) matrix on the dissolution kinetics precluded the observation of slight effects such as those linked to the complexing agents or to the crystal structure of the samples.

Stability and structural evolution of Ce(IV)(1-x)Ln(III)(x)O(2-x/2) solid solutions: a coupled µ-Raman/XRD approach.

Several CeO(2)-based mixed oxides with general composition Ce(1-x)Ln(x)O(2-x/2) (for 0 ≤ x ≤ 1 and Ln = La, Nd, Sm, Eu, Gd, Dy, Er, or Yb) were prepared using an initial oxalic precipitation leading to a homogeneous distribution of cations in the oxides. After characterization of the Ce/Nd oxalate precursors and then thermal conversion to oxides at T = 1000 °C, investigation of the crystalline structure of these oxides was carried out by XRD and µ-Raman spectroscopy. Typical fluorite Fm ̅3m structure was obtained for relatively low Ln(III) contents, while a cubic Ia ̅3̅ superstructure was evidenced above x ≈ 0.4. Moreover, since Nd(2)O(3) does not crystallize with the Ia ̅3̅-type structure, two-phase systems composed with additional hexagonal Nd(2)O(3) were obtained for x(Nd) ≥ 0.73 in the Ce(1-x)Nd(x)O(2-x/2) series. The effect of heat treatment temperature on these limits was explored through µ-Raman spectroscopy, which allowed determining the presence of small amounts of the different crystal structures observed. In addition, the variation of the Ce(1-x)Ln(x)O(2-x/2) unit cell parameter was found to follow a quadratic relation as a result of the combination between increasing cationic radius, modifications of cation coordination, and decreasing O-O repulsion caused by oxygen vacancies.