Immobilisation of Simulated Plutonium-Contaminated Material in Phosphate Glass: An Initial Scoping Study

Abstract

ABSTRACTVitrification is a potential route for the immobilisation of Plutonium Contaminated Material (PCM). This is an Intermediate Level Waste (ILW) arising from operations in which there is contact with Pu isotopes. PCM consists of low levels of Pu combined with metals, masonry, glass, ceramics, polymers and other carbonaceous materials. Simulated PCM containing CeO2 as a PuO2 surrogate was mixed with a phosphate precursor and vitrified. Pre-oxidation of PCM simulant prior to vitrification minimised the violence of batch reactions. No pre-oxidation produced inhomogeneous slag-like materials with high residual metals and particulates. Pre-oxidation at 600°C in air and at 1200°C in an O2-rich atmosphere produced more favourable results, with increasingly vitreous products resulting from more oxidised PCM simulant. The most oxidised PCM simulant produced phosphate glasses with low levels of particulate inclusions, as confirmed by x-ray diffraction and scanning electron microscopy. Particulates included iron-rich metallics and aluminous oxides. Increased melting times and temperatures may have reduced the number of inclusions slightly, but O2 bubbling during melting resulted in little additional benefit. Waste loading equivalent to ∼60 weight % of untreated waste may be possible. There was little evidence of Ce partitioning, indicating that it was immobilised within the glass matrix and had little preference for metallic or crystalline phases. These results demonstrate the potential feasibility for vitrification of PCM in phosphate glass, justifying further investigation into this potentially novel solution.