Positron annihilation spectroscopy study of lattice defects in non-irradiated doped and un-doped fuels

Abstract

Fission gas behavior within the fuel structure plays a major role for the safety of nuclear fuels during operation in the nuclear power plant. Fission gas distribution and retention is determined by both, micro- and lattice-structure of the fuel matrix. The ADOPT (Advanced Doped Pellet Technology) fuel, containing chromium and aluminum additives, shows larger grain sizes than standard (undoped) UO2 fuel, enhancing the fission gas retention properties of the matrix. However, the additions of such trivalent cations shall also induce defects in the lattice. In this study, we investigated the microstructure of such doped fuels as well as a reference standard UO2 by positron annihilation spectroscopy (PAS). Although this technique is particularly sensitive to lattice point defects in materials, a wider application in the UO2 research is still missing. The PAS-lifetime components were measured in the hotlab facility of PSI using a 22 Na source sandwiched between two 500-μ m-thin sample discs. The values of lifetime at the center and the rim of both samples, examined to check at the radial homogeneity of the pellets, are not significantly different. The mean lifetimes were found to be longer in the ADOPT material, 220 ps, than in standard UO2 , 190 ps, which indicates a larger presence of additional defects, presumably generated by the dopants. While two-component decomposition (bulk + one defect component) could be performed for the standard material, only one lifetime component was found in the doped material. The absence of the bulk component in the ADOPT sample refers to a saturated positron trapping (i.e., all positrons are trapped at defects). In order to associate a type of lattice defect to each PAS component, interpretation of the PAS experimental observations was conducted with respect to existing experimental and modeling studies. This work has shown the efficiency of PAS to detect lattice point defects in UO2 produced by Cr and Al oxides. These additives create lattice irregularities, which are acting as sinks for fission products on one hand and trapping positrons on the other hand. Fitting of the obtained experimental data with a suitable theoretical model can provide a valuable qualitative assessment of these defects. At this stage of the research, some of the existing models were used for this purpose.