Highly radioactive 238Pu-doped and non-radioactive samples of borosilicate glass with chemical compositions and synthesis routine similar to SON68 glass were studied under static saturated leaching conditions in distilled water at 90 °C. Dramatic differences in behavior of the radioactive and model glasses were observed. On time scale of 4 months the radioactive glass is fully covered by mechanically unstable alteration layer, possibly consisting of aluminum hydroxides with small fraction of a separate secondary Pu bearing phase. The model glass remains virtually pristine. Addition of Eu3+ into the glass allowed examination of the glass radio- and photoluminescence and to assess changes or REE3+ impurity local environment during self-irradiation and leaching. Photoluminescence spectra suggest more ordered local environment of europium ions in the alteration “gel” than in the bulk glass. Peculiar behavior of the photoluminescence spectra excited at different laser power is observed for the alteration layer and is ascribed to optical bleaching of color centers.

Samples of Chernobyl fuel debris, including massive corium and “lava” were collected inside the Chernobyl “Sarcophagus” or “Shelter” in 1990, transported to Leningrad (St. Petersburg) and stored under laboratory conditions for many years. In 2011 aged samples were visually re-examined and it was confirmed that most of them remained intact, although some evidence of self-destruction and chemical alteration were clearly observed. Selected samples of corium and “lava” were affected by static leaching at temperatures of 25, 90 and 150 °C in distilled water. A normalized Pu mass loss (NLPu) from corium samples after 140 days was noted to be 0.5 g/m2 at 25 °C and 1.1 g/m2 at 90 °C. For “lava” samples NLPu was 2.2–2.3 g/m2 at 90 °C for 140 days. The formation of secondary uranyl phases on the surface of corium and “lava” samples altered at 150 °C was confirmed. The results obtained are considered as an important basis for the simulation of fuel debris aging at Fukushima Daiichi nuclear power plant (NPP).

No abstract

We examined the degradation of nuclear waste borosilicate and phosphate glasses containing strong alpha-emitter 238Pu at a specific activity of 6.33 × 105 MBq/g in comparison with similar non-radioactive, non-radioactive irradiated and radioactive samples containing beta- and gamma-emitters, namely radionuclides 134Cs and 137Cs. For irradiation and leaching experiments, we used borosilicate and phosphate glasses, which are well-known and currently used to immobilize high-level radioactive waste. The main focus was the observation of the surface of altered glasses. Comparative analysis of hydrolytic surface alteration of borosilicate and phosphate nuclear waste glasses reveals that the behavior of radioactive samples differs significantly from that of non-radioactive glasses.