Abstract

Understanding the corrosion of nuclear waste glass is critical to predicting its safe disposal within a geological facility. The corrosion mechanisms and kinetics of the International Simple Glass, a simplified version of high-level nuclear waste glass, was shown to be significantly influenced by a high pH cement solution representative of disposal conditions. We provide the first microscopic characterisation of the porous, Zr-rich aluminoalkali-silica gel corrosion layer that was observed. Ca, Na and K from the cement solution were incorporated into the corrosion layer to charge compensate Si, Al and Zr species; the incorporation of Al was postulated to result in precipitation of an aluminosilicate-rich gel with large voids, facilitating rapid transport of species through the gel layer and significantly enhancing the corrosion rate. Precipitation of Al-containing zeolite and phyllosilicate phases was also observed, indicating that cementitious solutions may promote the detrimental ‘rate resumption’ stage of glass corrosion.

Highlights

  • It is the consensus of the regulatory agencies of a number of countries that vitrified nuclear waste should be disposed of within a deep geological disposal facility where it can safely undergo radioactive decay, isolated from the environment and future populations

  • The YCWCa solution maintained a high pH throughout the duration of the experiments; at 30 °C it was constant and remained at the value of the blank solution (pH(RT) 13.5), while at 70 °C a decline to pH(RT) 12 was observed (Supplementary Material Fig. S1)

  • The high pH and the composition of the cement leachate solution was found to exert a significant influence on the dissolution behaviour, as described below

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Summary

Introduction

It is the consensus of the regulatory agencies of a number of countries that vitrified nuclear waste should be disposed of within a deep geological disposal facility where it can safely undergo radioactive decay, isolated from the environment and future populations. It is postulated that such longer-term resumption may be related to the continual leaching of Ca during the degradation of cement by infiltrating groundwater.[23]

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