Published online by Cambridge University Press: 03 September 2012
Vitrification is the most developed method for the immobilisation of highlyradioactive waste obtained from reprocessing irradiated nuclear fuel. Highlyactive wastes continue to be vitrified at Sellafield in the WasteVitrification Plant (WVP) and the product glass has previously beensubjected to rigorous characterisation in order to ensure waste formintegrity and stability during interim storage. However, the vitrified wastemay eventually be placed in an underground repository and so further studiesmay be needed to confirm the chemical stability of vitrified wastes indifferent disposal scenarios. One area of uncertainty is in knowing how thealteration products and surface layers on a corroded glass effect thedissolution process and the solution concentrations of long-livedradionuclides. This study shows how the technique of laser microprobeinductively coupled plasma mass spectrometry (LM-ICP-MS) can be used toprovide a direct chemical analysis of vitrified samples, both in theiras-cast state and after leach testing. LM-ICP-MS, solutions' nebulisationICP-MS (to provide chemical analyses of the leachants), light microscopy,scanning electron microscopy and confocal laser microscopy were used toexamine the effect of leaching on the surfaces of vitrified samples. Datawere obtained for a number of simulated WVP-type product glasses that weresubjected to soxhlet leach testing for varying lengths of time. TheLM-ICP-MS data clearly show that the technique offers a rapid and relativelyaccurate method for detecting and monitoring minute changes in the surfacelayers of glass and in the build-up of alteration products. Hence, LM-ICP-MScould be used to obtain valuable mechanistic information on the degradationof glass by examining radionuclide behaviour in the surface layers of glassas it corrodes over extended time periods.