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The Use of Laser Microprobe-ICP-MS in the Examination of Nuclear Waste Glasses

Published online by Cambridge University Press:  03 September 2012

S. Shuttleworth
Affiliation:
Department of Earth and Planetary Sciences, Washington University, 1 Brookings Drive, Campus Box 1169, St Louis, MO 63130, USA
J. E. Monteith
Affiliation:
Research and Technology, BNFL, Sellafield, Seascale, Cumbria, CA20 1PG, UK
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Abstract

Vitrification is the most developed method for the immobilisation of highly radioactive waste obtained from reprocessing irradiated nuclear fuel. Highly active wastes continue to be vitrified at Sellafield in the Waste Vitrification Plant (WVP) and the product glass has previously been subjected to rigorous characterisation in order to ensure waste form integrity and stability during interim storage. However, the vitrified waste may eventually be placed in an underground repository and so further studies may be needed to confirm the chemical stability of vitrified wastes in different disposal scenarios. One area of uncertainty is in knowing how the alteration products and surface layers on a corroded glass effect the dissolution process and the solution concentrations of long-lived radionuclides. This study shows how the technique of laser microprobe inductively coupled plasma mass spectrometry (LM-ICP-MS) can be used to provide a direct chemical analysis of vitrified samples, both in their as-cast state and after leach testing. LM-ICP-MS, solutions' nebulisation ICP-MS (to provide chemical analyses of the leachants), light microscopy, scanning electron microscopy and confocal laser microscopy were used to examine the effect of leaching on the surfaces of vitrified samples. Data were obtained for a number of simulated WVP-type product glasses that were subjected to soxhlet leach testing for varying lengths of time. The LM-ICP-MS data clearly show that the technique offers a rapid and relatively accurate method for detecting and monitoring minute changes in the surface layers of glass and in the build-up of alteration products. Hence, LM-ICP-MS could be used to obtain valuable mechanistic information on the degradation of glass by examining radionuclide behaviour in the surface layers of glass as it corrodes over extended time periods.

Type
Research Article
Copyright
Copyright © Materials Research Society 1997

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References

REFERENCES

1. Shuttleworth, S. and Monteith, J. E., JAAS. In preparation.Google Scholar
2. Gray, A. L., Analyst, 110, p. 551556 (1985).Google Scholar
3. Arrowsmith, P., Anal. Chem., 59, p. 14371444 (1987).10.1021/ac00137a014Google Scholar
4. Abell, I., Gregson, D. and Shuttleworth, S., Laser Ablation ICP-MS Analysis of Ceramic Materials, The Physics and Chemistry of Carbides, Nitrides and Borides. NATO ASI Series. Series E: Applied Sciences (1990), 185, p. 121130.Google Scholar
5. Fryer, B. J., Jackson, S. E. and Longerich, H. P., The Canadian Mineralogist, 33, p. 303312(1995).Google Scholar
6. Longerich, H. P., Jackson, S. E., Fryer, B. J. and Strong, D. F., Geosci. Can., 20, p. 2127(1993).Google Scholar
7. Norman, M. D., Pearson, N. J., Sharma, A. and Griffin, W. L.. Geostandards Newsletter, 20 (2), p. 247261 (1996).Google Scholar
8. Chapman, N. A. and McKinley, I. G., The Geological Disposal of Nuclear Waste. John Wiley & Sons, Chichester, 1987, p. 8184.Google Scholar
9. Lutze, W. in Radioactive Waste Forms for the Future, edited by Lutze, W. and Ewing, R. C, North-Holland Physics Publishing, The Netherlands, 1988, p. 93115.Google Scholar
10. Werme, L., Bjorner, I. K., Bart, G., Zwicky, H. U., Grambow, B., Lutze, W., Ewing, R. C. and Magrabi, C., J. Mater. Res., 5 (5), p. 11301146 (1990) and references cited therein.10.1557/JMR.1990.1130Google Scholar
11. Hall, A.R., Hough, A. and Marples, J. A. C. in Scientific Basis for Nuclear Waste Management. (Mater. Res. Soc. Sypm. Proc), 1982, 5, p. 8392.Google Scholar