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Crystallisation of a simulated borosilicate high-level waste glass produced on a full-scale vitrification line
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Rose, Peter B., Woodward, David I., Ojovan, Michael I., Hyatt, Neil C. and Lee, W. E. (2011) Crystallisation of a simulated borosilicate high-level waste glass produced on a full-scale vitrification line. Journal of Non-Crystalline Solids, Vol.357 (No.15). pp. 2989-3001. doi:10.1016/j.jnoncrysol.2011.04.003
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Official URL: http://dx.doi.org/10.1016/j.jnoncrysol.2011.04.003
Abstract
A simulated (inactive) borosilicate high-level waste (HLW) glass was produced on a full-scale vitrification line with composition simulating vitrified oxide fuel (UO(2)) reprocessing waste. As-cast samples were compositionally homogeneous (Type I microstructure) and/or compositionally inhomogeneous displaying compositional 'banding' and frequently containing 'reprecipitated calcine' (Type II microstructure). Crystal phases identified in as-cast samples were: tetragonal RuO(2), cubic Pd-Te alloy, cubic (Cr,Fe,Ni,Ru)(3)O(4), trigonal Na(3)Li(MoO(4))(2)center dot 6H(2)O, ostensibly cubic Zr(1-x-y)Ce(x)Gd(y)O(2-0.5y) and a lanthanoid (Nd,Gd,La,Ce) silicate. Zr(1-x-y)Ce(x)Gd(y)O(2-0.5y) and lanthanoid (Nd,Gd,La,Ce) silicate were found exclusively in the Type II microstructure as component crystal phases of 'reprecipitated calcine'. Heat treated samples (simulating the retarded cooling experienced by actual (active) borosilicate HLW glasses after pouring) displayed extensive crystallisation and cracking (Type A microstructure) and/or 'banded' crystallisation (Type B microstructure) depending on their parent (as-cast) microstructure (Type I and/or Type II respectively). Crystal phases identified in heat treated samples were: tetragonal SiO(2) (alpha-cristobalite), tetragonal (Na,Sr,Nd,La)MoO(4), cubic Ce(1-x-y)Zr(x)Gd(y)O(2-0.5y), a Ni-rich phase, a lanthanoid (Nd,Gd,La,Ce) silicate and orthorhombic LiNaZrSi(6)O(15) (zektzerite). alpha-cristobalite was found exclusively in the Type A microstructure, while lanthanoid (Nd,Gd, La,Ce) silicate and zektzerite were only found in the Type B microstructure. Potential host phases for HLW radionuclides are: Pd-Te alloy ((107)Pd and (79)Se), (Cr,Fe,Ni,Ru)(3)O(4) ((63)Ni), Zr(1-x-y)Ce(x)Gd(y)O(2-0.5y) ((93)Zr, Pu and U), both lanthanoid (Nd,Gd,La,Ce) silicates (Am and Cm), (Na,Sr,Nd,La)MoO(4) ((90)Sr, Am and Cm), Ce(1-x-y)Zr(x)Gd(y)O(2-0.5y) ((93)Zr, Pu and U), the Ni-rich phase ((63)Ni) and zektzerite ((93)Zr, (126)Sn and U). Cracking in samples was attributed to thermal expansion mismatch between the borosilicate HLW glass matrix and RuO(2), cristobalite (both a and beta), (Na,Sr,Nd,La)MoO(4) and zektzerite on cooling. There was also a contribution from the cristobalite alpha-beta phase transition.
| Item Type: | Journal Article | ||||
|---|---|---|---|---|---|
| Subjects: | Q Science > QC Physics Q Science > QD Chemistry |
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| Divisions: | Faculty of Science > Physics | ||||
| Library of Congress Subject Headings (LCSH): | Radioactive wastes -- Vitrification, Radioactive wastes -- Vitrification -- Simulation methods, Crystallization, Glass, Geochemistry | ||||
| Journal or Publication Title: | Journal of Non-Crystalline Solids | ||||
| Publisher: | Elsevier Science BV | ||||
| ISSN: | 00223093 | ||||
| Official Date: | 15 July 2011 | ||||
| Dates: |
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| Volume: | Vol.357 | ||||
| Number: | No.15 | ||||
| Page Range: | pp. 2989-3001 | ||||
| DOI: | 10.1016/j.jnoncrysol.2011.04.003 | ||||
| Status: | Peer Reviewed | ||||
| Publication Status: | Published | ||||
| Access rights to Published version: | Restricted or Subscription Access | ||||
| Funder: | Engineering and Physical Sciences Research Council (EPSRC), Nexia Solutions Limited, British Nuclear Fuels (Firm) (BNFL) | ||||
| Grant number: | 01300676 (EPSRC) |
Data sourced from Thomson Reuters' Web of Knowledge
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