Abstract
The influence of increasing the waste loading of Ca- and Zn-containing MW high-level-waste glass, from 20 to 35 wt%, on the chemical durability was investigated using 112-day PCT-B tests at 90 °C in ultra-high-quality water. During the initial stage of dissolution, from 0 to 3 days, increased waste loadings corresponded to reduced boron dissolution rates. By 112 days, however, there was no difference in the normalised mass loss of boron as a function of waste loading, within experimental uncertainty. In comparison to literature values obtained for traditional MW high-level-waste glasses, containing no Ca and Zn, the boron dissolution rates of CaZn MW glasses in the residual stage of dissolution, > 28 days, were greater by at least an order of magnitude. Analysis of secondary phases, combined with geochemical modelling of the solutions, indicate that the dual formation of Mg- and Zn-smectite phyllosilicate clays, potentially saponite (Ca0.2Mg3(Si,Al)4O10(OH)2·4H2O) and sauconite (Na0.3Zn3(Si, Al)4O10(OH)2·nH2O), respectively, may be the cause of this enhanced dissolution.
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Acknowledgments
This work was funded, in part, by the EPSRC Next Generation Nuclear Centre for Doctoral Training Centre under Grant EP/L015390/1. Financial support for CLC from the EPSRC (ECR Fellowship; EP/N017374/1) is acknowledged. Input and interest from Radioactive Waste Management Limited (UK) was greatly appreciated. This research was performed at the MIDAS Facility, at the University of Sheffield, which was established with support from the UK Department of Energy and Climate Change 2015. Data are available upon request. Many thanks to the insightful anonymous reviewer.
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Fisher, A.J., Harrison, M.T., Hyatt, N.C. et al. The dissolution of simulant UK Ca/Zn-modified nuclear waste glass: the effect of increased waste loading. MRS Advances 6, 95–102 (2021). https://doi.org/10.1557/s43580-021-00025-0
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DOI: https://doi.org/10.1557/s43580-021-00025-0