Hostname: page-component-586b7cd67f-2brh9 Total loading time: 0 Render date: 2024-11-25T17:42:18.675Z Has data issue: false hasContentIssue false
  • English
  • Français

Testing the Grambow Glass Dissolution Model by Comparing it With Monte Carlo Simulation Results

Published online by Cambridge University Press:  10 February 2011

Marc Aertsens
Marc Aertsens*
Affiliation:
SCK·CEN, Boeretang 200, B-2400 Mol, Belgium.
Get access

Abstract

We have developed a Monte Carlo (simulation) model to describe glass dissolution. This model uses similar parameters to those used in the Grambow model, which has been the main glass dissolution model during the last decade. While the Grambow model is macroscopic, ours is microscopic. This assures that the value of our parameters is time independent and allows changes in the gel structure (not just concentrations) to be described.

We relate our parameters to those of the Grambow model and test whether the basic assumptions of the Grambow model are consistent with our simulation results. In these simulations, as the solution evolves towards silica saturation, the silica concentration in solution can become higher than the (final) silica saturation concentration. A possible explanation for this behavior, which is observed experimentally as well, is that the silica saturation concentration is not constant as a function of time. Initially, the silica saturation concentration is the glass saturation concentration. The glass saturation concentration is higher than the final silica saturation concentration, which corresponds to saturation of the gel. In the Grambow model, the initial dissolution rate (at the gel/water interface) and the diffusion coefficient of silica in the gel are not constant either. The existence of a final dissolution rate depends on the silica content of the glass and on the protection provided by the gel layer. In the simulations, a protective gel is mainly formed by the adsorption (precipitation) of dissolved silica particles from the solution in contact with the gel. This makes us expect that (1) the gel would be non protective for dynamic tests (with a low silica content in solution) and (2) the gel would be very protective in static tests with high surface to volume ratios.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 556: Symposium QQ – Scientific Basis for Nuclear Waste Management XXII , 1999 , 409
Copyright
Copyright © Materials Research Society 1999

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

1. Aagaard, P. and Helgeson, H.., Am. J. of Science 282, p. 237 (1982).Google Scholar
2. Grambow, B., Nuclear waste glass dissolution. mechanism, model and application, (Report to the JSS-project 87-02, phase IV, 1987).Google Scholar
3. Advocat, T., Couchan, J. L., Crovisier, J. L., Guy, C., Daux, V., Jégou, C., Gin, S. and Vernaz, E. in Scientific Basis for Nuclear Waste Management XXI, edited by Kinley, I. Mc, McCombie, C. (Mat. Res. Soc. Symp. Proc. 506, 1998) pp. 63–70.Google Scholar
4. Kuhn, W. and Bunnell, L., Results of testing the Grambow rate law for use in HWVP glass durability correlations, (Report PNNL-1 1070 UC-810, Richland, Washington, USA, 1996).Google Scholar
5. Jdgou, C., Gin, S., Vernaz, E. and Larché, F. in Proc. of XVlll Int. Congr. on Glass, edited by. Choudhary, M.., Huff, N. and Drummond, C. (Am. Ceram. Soc., San Francisco, USA, 1998).Google Scholar
6. Gin, S., Jégou, C., Vernaz, E., and Larché, F. in Proc. of XVIII Int. Congr. on Glass, edited by. Choudhary, M., Huff, N. and Drummond, C. (Am. Ceram. Soc., San Francisco, USA, 1998).Google Scholar
7. Lasaga, A. in Kinetics o/geochemical processes, edited by Lasaga, A. and Kirkpatrick, R. (Rev. Mineralogy 8, 1981), p. 1.Google Scholar
8. Böhm, T. and Chudek, J., Fundamentals of Glass Science and Technology (Glafo, Växjö, Sweden, 1997), p. 476.Google Scholar
9. Aertsens, M. and Iseghem, P. Van in Scientific Basis for Nuclear Waste Management XX, edited by Murphy, W. and Knecht, D. (Mat. Res. Soc. Symp. Proc. 412, 1996) pp. 271–277.Google Scholar
10. Aertsens, M. in Glass, scientifc research for high performance containment (CEA/Vairh6, Summer Session Proc., 1998), p. 343.Google Scholar
11. Aertsens, M. in Proc. of XVIIl Int. Congr. on Glass, edited by. Choudhary, M., Huff, N., and Drummond, C. (Am. Ceram. Soc.,San Francisco, USA, 1998).Google Scholar
12. Dove, P. and Crerar, C., Geochim. Cosmochim. Acta 54, p. 955 (1990).Google Scholar
13. Vernaz, E. and Dussossoy, J., Applied Geochem., Suppl. Issue no 1, p. 13 (1992).Google Scholar
14. Jantzen, C., in Corrosion of Glass, Ceramics and Ceramic Conductors-Principles, edited by Clark, D. and Zoitos, B.. (Noyes Publications, Park Ridge, New Jersey,1992), p. 153.Google Scholar
15. Delage, F., Larche, F. and Vernaz, E. in Scientific Basis for Nuclear Waste Management XVI, edited by Interrante, C. and Pabalan, R. Mc (Mat. Res. Soc. Symp. Proc. 294, 1993) pp. 171–176.Google Scholar
16. Lodding, A. and Iseghem, P. Van in Scientific Basis for Nuclear Waste Management XX, edited by Murphy, W. and Knech, D. (Mat. Res. Soc. Symp. Proc. 412, 1996) pp. 229–238.Google Scholar
17. Bunker, B., Tallant, D., Headley, T., Turner, G. and Kirkpatrick, R., Phys. Chem. Glasses 29, p. 106 (1988).Google Scholar
18. Vernaz, E., Grambow, B., Lutze, W., Lemmens, K., and Iseghem, P. Van in Proc. Fourth Conf European Comm. on management and disposal of radioactive waste, edited by McMenamin, T. (EUR 17543 EN, 1996), pp. 239–253.Google Scholar
19. Xing, S., Buechele, A. and Pegg, I. in Scientific Basis for Nuclear Waste Management XVIL, edited by Barkatt, A. and Konynenbur, R. Van, (Mat. Res. Soc. Symp. Proc. 333, 1994) pp. 541–548.Google Scholar
20. Perera, G., Doremus, R. and Lanford, W.., J. Am. Ceram. Soc. 74, p. 1269 (1991).Google Scholar
21. Deruelle, O., Barboux, P., Spalla, O., Ricol, S., Lambard, J. and Vernaz, E.. in Glass, scientific research for high performance containment (CEA/Valrh6, Summer Session Proc., 1998), p. 435.Google Scholar
22. Helebrant, A., Silikaty 41 (4), p. 147 (1997).Google Scholar
23. Lee, T. and Clark, D., Adv. Ceram. 20, p. 505 (1986).Google Scholar
24. Chick, L. and Pederson, L., in Scientific Basis for Nuclear Waste Management VII, edited by Vay, G. Mc (Mat. Res. Soc. Symp. Proc. 26, 1984) pp. 635–642.Google Scholar
25. Xiao, Y. and Lasaga, A., Geochim. Cosmochim. Acta 60, p. 2283 (1996).Google Scholar