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NMR Investigation of Cation Distribution in HLW Wasteform Glass

Published online by Cambridge University Press:  01 February 2011

Diane Holland ,
Ben G Parkinson ,
Moinul M Islam ,
Adam Duddridge ,
Jonathan M Roderick ,
Andy P Howes  and
Charlie R Scales
Diane Holland
Affiliation:
Department of Physics, University of Warwick, Coventry CV4 7AL, UK
Ben G Parkinson
Affiliation:
Department of Physics, University of Warwick, Coventry CV4 7AL, UK
Moinul M Islam
Affiliation:
Department of Physics, University of Warwick, Coventry CV4 7AL, UK
Adam Duddridge
Affiliation:
Department of Physics, University of Warwick, Coventry CV4 7AL, UK
Jonathan M Roderick
Affiliation:
Department of Physics, University of Warwick, Coventry CV4 7AL, UK
Andy P Howes
Affiliation:
Department of Physics, University of Warwick, Coventry CV4 7AL, UK
Charlie R Scales
Affiliation:
Nexia Solutions, Sellafield, Seascale, Cumbria, CA20 1PG, UK
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Abstract

Magic-angle-spinning NMR has been used to establish the structural roles of various cations added to the borosilicate glass which is used for the vitrification of high-level nuclear waste (HLW). Representative surrogate oxides with nominal valencies of +1, +2 and +3 have been studied which span the range of oxides from modifier to intermediate and conditional glassformer. NMR has been carried out on those nuclei which are accessible and the species observed have been correlated with the physical and chemical behaviour. The controlling factor is the manner in which the alkali cations partition between the various network groups, changing the distribution of silicon Qn species and the boron N4 ratio. Identifiable superstructural units are also present in these glasses. The aqueous corrosion rate increases with Q3 content, as does the weight loss due to evaporation from the melt. The activation energy for DC conduction scales with N4. Values of N4 obtained for these glasses deviate significantly from those predicted by the currently accepted model (Dell and Bray) and are strongly affected by the modifier or intermediate nature of the surrogate oxide and also by its effect on the distribution of nonbridging oxygens between the silicate and borate polyhedra.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 1107: Scientific Basis for Nuclear Waste Management XXXI , 2008 , 199
Copyright
Copyright © Materials Research Society 2008

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