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The Diffusion of Radionuclides through Waste Encapsulation Grouts

  • Adam V. Chambers (a1), Andrew Green (a1), Andrew W. Harris (a2), Timothy G. Heath (a1), Fiona M.I. Hunter (a1), Michelle C. Manning (a1) and Stephen J. Williams (a1)...

Abstract

United Kingdom Nirex Limited develops and advises on safe, environmentally sound and publicly acceptable options for the long-term management of radioactive waste. One option Nirex has developed is a phased geological repository concept for intermediate level waste and some low level wastes that makes use of a combination of engineered and natural barriers. Physical containment of radionuclides would be achieved by immobilisation and packaging of wastes (mostly) in stainless steel containers.

Existing models of the migration of dissolved radionuclides from packaged wastes suggest that radionuclide release is determined largely by the rate of diffusion through the encapsulation grout used to immobilise the waste. The use of such models requires diffusion coefficient data for radionuclides in waste encapsulation grouts. This paper describes a programme of through-diffusion experiments, and modelling interpretation, aimed at deriving diffusion coefficients for some radionuclides in two types of encapsulation grout.

An intrinsic diffusion coefficient of HTO of around 1×10−13 to 2×10−13 m2s−1 was determined for a 3:1 mix of blast furnace slag to ordinary Portland cement, compared to around 4×10−13 to 5×10−13 m2s−1 for a 3:1 mix of pulverised fuel ash to ordinary Portland cement. These values are lower than that assumed for a non-sorbing radionuclide in an earlier modelling exercise. Porosity values around 0.3 were obtained in each case. For 36Cl as chloride, the experiments showed no significant breakthrough over the experimental timescale of about one year, suggesting an intrinsic diffusion coefficient below 5×10−13 m2s−1. One possibility is that chlorine-containing solids are precipitating in the cement. An intrinsic diffusion coefficient for 137Cs in the 3:1 mix of pulverised fuel ash to ordinary Portland cement of 4×10−15 m2s−1 was estimated, significantly lower than that determined for HTO.

The results from three of the sixteen experiments could not be fitted with a simple diffusion model, and for a further five experiments there was some doubt as to whether simple diffusion behaviour had been observed. It is suggested that this may have been due to cracks in the grouts that were sufficiently large to affect the diffusion properties of the grouts, although none was visible to the naked eye. Cracking of the waste encapsulation grouts could provide a mechanism for enhanced migration of radionuclides from waste packages, compared with diffusion in a homogeneous porous medium alone.

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References

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1 United Kingdom Nirex Limited, Generic Repository Studies: The Nirex Phased Disposal Concept, Nirex Report N/074, (2003).
2. Askarieh, M.M., Chambers, A.V. and Gould, L.J., in Scientific Basis for Nuclear Waste Management XXIII, edited by Smith, R.W. and Shoesmith, D.W., (Mater. Res. Soc. Proc. 608, Pittsburg, PA, USA, 2000) pp.243248.
3. Bourke, P.J., Gilling, D., Jefferies, N.L., D.A. Lever and Lineham, T.R., Nirex Report NSS/R135 (1988).
4. A. Haworth, A.C. Smith and Thompson, A.M., Nirex Report NSS/R366 (2001).
5. Chambers, A.V., Green, A., Harris, A.W., Hunter, F.M.I., Manning, M.C. and Williams, S.J., Serco Assurance Report SA/ENV-0646 (2005) draft.
6. Harris, A.W. and Nickerson, A.K., Nirex Report NSS/R309 (1995).
7. Harris, A.W. and Nickerson, A.K., Nirex Report NSS/R335 (1997).
8. Tits, J., Jakob, A., Wieland, E. and Spieler, P., J. Contaminant Hydrology 61, 4562 (2001).

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