Behavior of fission gases in nuclear fuel: XAS characterization of Kr in UO2
Résumé
X-ray Absorption Spectroscopy (XAS) was used to study the behavior of krypton as a function of its concentration in UO2 samples implanted with Kr ions. For a 0.5 at.% krypton local concentration, by combining XAS results and DFT + U calculations, we show that without any thermal treatment Kr atoms are mainly incorporated in the UO2 lattice as single atoms inside a neutral bound Schottky defect with O vacancies aligned along the (100) direction (BSD1). A thermal treatment at 1273 K induces the precipitation of dense Kr nano-aggregates, most probably solid at room temperature. In addition, 26 ± 2% of the Kr atoms remain inside BSD1 showing that Kr-BSD1 complex is stable up to this temperature. Consequently, the (in-)solubility of krypton in UO2 has to be re-evaluated. For high Kr concentration (8 at.%), XAS signals show that Kr atoms have precipitated in nanometer-sized aggregates with internal densities ranging between 4.15(7) g cm−3 and 3.98(5) g cm−3 even after annealing at 873 K. By neglecting the effect due to the UO2 matrix, the corresponding krypton pressures at 300 K were equal to 2.6(3) GPa and 2.0(2) GPa, respectively. After annealing at 1673 K, regardless of the initial Kr concentration, a bi-modal distribution is observed with solid nano-aggregates even at room temperature and larger cavities only partially filled with Kr. These results are very close to those observed in UO2 fuel irradiated in reactor. In this study we show that a rare gas can be used as a probe to investigate the defect creation and their stability in UO2.