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Validation of glass dissolution and Si diffusion parameters with a combined glass dissolution-diffusion experiment in Boom Clay

Published online by Cambridge University Press:  21 March 2011

Karel Lemmens
Affiliation:
Waste and Disposal Department SCKCCEN (Belgian Nuclear Research Centre), Boeretang 200, B-2400 Mol, Belgium, klemmens@sckcen.be
Marc Aertsens
Affiliation:
Waste and Disposal Department SCKCCEN (Belgian Nuclear Research Centre), Boeretang 200, B-2400 Mol, Belgium, maertsen@sckcen.be
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Abstract

Existing knowledge on glass dissolution and silica diffusion in Boom Clay is validated by experiments where both phenomena could be studied simultaneously. SON68 glass coupons, doped with radioactive 32Si, were sandwiched between two cores of fresh humid Boom Clay and heated to 30°C. At the end of the experiment, the system was dismantled, the mass loss of the glass coupon was measured, and the clay core was sliced to determine the diffusion profile of the 32Si dissolved from the glass. These data were completed with analyses of the clay water and surface analyses for analogous tests with undoped glass. The results are interpreted by assuming congruent glass dissolution at a constant rate, with a glass silica saturation concentration between 14 and 20 mg/l, a forward glass dissolution rate (at zero silica concentration) of 0.028 g.m−2day−1, an apparent silica diffusion coefficient in the clay of 1.4 10−12 m2sec−1, and a distribution coefficient for silica on Boom Clay between 0.010 and 0.075 m3kg−1. These parameter values are close to the range found in literature. It was not necessary to consider diffusion through the gel, precipitation or detailed geochemical reactions. The modeling exercise shows that the existing knowledge about the subsystems glass and clay can succesfully be integrated to describe the coupled processes in the whole system.

Type
Research Article
Copyright
Copyright © Materials Research Society 2006

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References

REFERENCES

1. Ribet, I., Gin, S., Godon, N., Jollivet, P., Minet, Y., Grambow, B., Abdelouas, A., Ferrand, K., Lemmens, K., Aertsens, M., Pirlet, V., Jacques, D., Crovisier, J.L., Aouad, G., Arth, A., Clément, A., Fritz, B., Morvan, G., Munier, I., Nero, M. Del, Ozgümüs, A., Curti, E., Luckscheiter, B., Schwyn, B., in Final Technical Report for GLASTAB, contract N° FIKW-CT-2000-00007 with the European Commission (2004)Google Scholar
2. Gin, S., Jollivet, P., Mestre, J.P., Jullien, M., Pozo, C., ‘French SON 68 nuclear glass alteration mechanisms on contact with clay media’, Applied Geochemistry 16, 861881 (2001)Google Scholar
3. Craen, M. De, Geet, M. Van, Wang, L., Put, M., ‘High sulphate concentrations in squeezed Boom Clay pore water: evidence of oxidation of clay cores, Physics and Chemistry of the Earth 29, 91–003 (2004)Google Scholar
4. Aertsens, M., Cannière, P. De, Moors, H., ‘Modelling of silica diffusion experiments with 32Si in Boom Clay’, Journal of Contaminant Hydrology 61, 117129 (2003)Google Scholar
5. Lemmens, K., ‘The effect of clay on the dissolution of nuclear waste glass’, Journal of Nuclear Materials 298, 1118 (2001)Google Scholar
6. Godon, N. et al. , Dossier de reference sur le comportement à long terme des verres nucléaires, RT DTCD 2004/06 (2004)Google Scholar
7. Crank, J., The mathematics of diffusion, 2nd ed., Clarendon Press, Oxford, 1975 Google Scholar