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Enhancement of Borosilicate Glass Dissolution by Silica Sorption and Diffusion in Compacted Bentonite: A Model Study.

Published online by Cambridge University Press:  28 February 2011

Enzo Curti
Affiliation:
Paul Scherrer Institut, Würenlingen and Villigen, CH-5232 Villigen PSI, Switzerland
P. A. Smith
Affiliation:
Paul Scherrer Institut, Würenlingen and Villigen, CH-5232 Villigen PSI, Switzerland
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Abstract

Experimental evidence indicates that glass corrosion rates decrease proportionally with the increase of silicic acid concentration in the solution contacting the glass surface. A minimum corrosion rate (Rsat) is reached when the solution becomes saturated with respect to an unidentified amorphous siliceous compound. In a repository where the vitrified waste form is surrounded by compacted bentonite, the silica dissolved from the glass will diffuse into the pore solution and concentration gradients will be established throughout the backfill material. The silicic acid concentration at the glass-bentonite interface, and thus the glass corrosion rate, will then be diffusion controlled. Moreover, experimental work suggests that significant sorption of silica by clay minerals in bentonite may accelerate glass corrosion.

A model describing glass corrosion coupled with diffusive transport and sorption of silica in bentonite has been developed and incorporated in a FORTRAN computer code (GLADIS). The model assumes: (a) a linear isotherm for the sorption of silica (KD), (b) time and space invariant pH, temperature and ionic strength, (c) proportionality between the quantity of silica precipitated and the amount of glass dissolved and (d) cylindrical geometry. Preliminary calculations with a particular parameter set at 90°C, assuming no silica sorption on the bentonite, indicate for an unfractured glass block that a stationary state is rapidly reached in which the silica concentration at the glass-bentonite interface is lower than the saturation concentration. This implies that the glass corrodes at a more rapid rate than Rsat (RsS ∼ 8 Rsat) If moderate silica sorption is assumed (KD = 0.5 m3 kg−1), the attainment of stationary conditions is delayed by the removal of silicic acid from solution, and the average corrosion rate is further increased by a factor ∼ 2.

Type
Research Article
Copyright
Copyright © Materials Research Society 1991

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References

REFERENCES

[1] Grambow, B., Hermannson, H.P., Björner, I.K. and Werme, L. in Scientific Basic for Nuclear Waste Management IX, edited by Werme, L.O., (Mater. Res. Soc. Proc., 50, Pittsburgh PA 1985), pp. 187194.Google Scholar
[2] Björner, I.K. et al., JSS Project Phase V: Final Repor (88–02), SKB report, Stockholm, 1988.Google Scholar
[3] Nagra, Projekt Gewähr Report NGB 85–09, Baden (Switzerland), 1985.Google Scholar
[4] Lanza, F. and Ronsecco, C. in Scientific Basis for Nuclear Waste Management V, edited by Lutze, W., (Elsevier Science Publisher, New York, 1982), pp. 125133.Google Scholar
[5] Godon, N., Effet de matériaux d’environnement sur l’altération du verre nucléaire R7T7 - influence des argiles, phD Thesis, Université d’Orldans, 1988.Google Scholar
[6] Tan, K.H., The effect of interaction and adsorption of silica on structural changes in clay minerals, Soil Science, 134. pp. 300307.Google Scholar
[7] Nordstrom, D.K. and Munoz, J.L., Geochemical Thermodynamics, Benjamin Cummings Publisher, Menlo Park CA 1985.Google Scholar
[8] IMSL, Inc. Math/Library–Fortran subroutines for mathematical applications, version 1.0, 1987.Google Scholar