Published online by Cambridge University Press: 17 March 2011
polycrystalline sample of Ti-pyrochlore, (Ca,Gd,Hf,U,Pu)2Ti2O7, doped with approximately 8.7 wt.% 238Pu and 20.0 wt.% 238U, has been studied at different cumulative doses of alpha induced radiation damage using scanning electron microscopy (SEM) and quantitative electron probe microanalysis (EMPA). All analyses of 238Pu-doped Ti-pyrochlore were done for comparison with 239Pu-doped pyrochlore synthesized under similar conditions. Our results suggest that accelerated alpha-induced radiation damage affects not only the crystalline structure of 238Pu-doped pyrochlore, but also causes changes in the chemical composition of the pyrochlore, and as proposed, destruction of pyrochlore-U-Pu solid solution. Numerous inclusions of a separate U-oxide phase were found in the 238Pu-doped pyrochlore crystalline matrix. The inclusions were observed visually using SEM and increased as a function of the cumulative dose. Also, after a cumulative dose of 1.1 × 1025 alpha decays/m3 the pyrochlore became nearly amorphous and inclusions of Hf-Ti-Ca-O phase were found in the crystalline matrix. In all cases separate phases of U-oxide and Hf-Ti-Ca-O were localized in chemically inhomogeneous areas. The results obtained allow us to assume that under self-irradiation the amorphization of Ti-pyrochlore might be accompanied with destruction of single solid solution, (Ca,Gd,Hf,U,Pu)2Ti2O7, into several pyrochlore phases of different chemical composition and precipitation of some amount of Pu and U into separate oxide phases.