Hostname: page-component-78c5997874-mlc7c Total loading time: 0 Render date: 2024-11-08T05:01:07.570Z Has data issue: false hasContentIssue false

Control of R7T7 Nuclear Glass Alteration Kinetics Under Saturation Conditions

Published online by Cambridge University Press:  15 February 2011

S. Gin*
Affiliation:
Commissariat à l'Energie Atomique (CEA), Rhône Valley Research Center, DCC/DRDD/SCD, BP 171, 30207 Bagnols-sur-Cèze, France
Get access

Abstract

The hypothesis of French nuclear waste glass disposal in a geological repository implies a comprehensive assessment of all the glass elements liable to participate in controlling the material alteration kinetics. The hypothetical existence of kinetically limiting elements other than silica could account for the observed R7T7 glass behavior in the presence of certain clays, and notably the continued high alteration rates observed even after silica saturation occurs. Flowing experiments with solutions near silica saturation but highly subsaturated with respect to aluminum hydroxide were defined to investigate the possible limiting role of aluminum. Experiments were conducted at different flow rates with the same constant steady-state H4 SiO4 activity for all the tests. The glass dissolution rate was observed to depend on the solution flow rate, indicating that under these conditions the kinetics are not controlled by dissolved silica alone. An additional experiment, in which only the Al(OH)4 activity in solution was allowed to vary, demonstrated the critical role of this element. Several interpretations are discussed.

Type
Research Article
Copyright
Copyright © Materials Research Society 1996

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

1. Grambow, B. (1985), “A General Rate Equation for Nuclear Waste Glass Corrosion”, in Scientific Basis for Nuclear Waste Management VIII, edited by Jantzen, C., Syone, J. and Ewing, R., Mater. Res. Soc. Symp. Proc. vol.44, pp. 15–21.Google Scholar
2. Advocat, T. (1991), Les mécanismes de corrosion en phase aqueuse du verre nucléaire R7T7. Approche expérimentale: Essai de modélisation thermodynamique and cinétique, PhD thesis, Université Louis Pasteur, Strasbourg, France.Google Scholar
3. Bourcier, W.L., Weed, H.C., Nguyen, S.N., Nielsen, J.K., Morgan, L., Newton, L. and Knauss, K.G. (1992), “Solution Compositional Effects on the Dissolution Kinetics of Borosilicate Glass”, Water-Rock Interaction, Kharaka, & Mest, (eds.), Balkema, Rotterdam.Google Scholar
4. NoguèS, J.L., Vernaz, E. and Jacquet-Francillon, N. (1985), “Alterability of the French LWR Solution Reference Glass Repository Conditions”, in Scientific Basis for Nuclear Waste Management VIII, eds. Jantzen, C., Syone, J. and Ewing, R., Mater. Res. Soc. Symp. Proc. vol.44,pp. 195–204.Google Scholar
5. Gin, S. (1994), Etude expérimentale de l'influence d'espèces aqueuses sur la cinétique de dissolution du verre nucléaire R7T7, PhD thesis, Université de Poitiers, France.Google Scholar
6. Vernaz, E., Advocat, T. and Dussosso, Y J.L. (1989), “Effects of the SAN Ratio on the Long Term Corrosion Kinetics of R7T7 Glass”, in Ceramic Transactions, vol. 9. Nuclear Waste Management, Mellinger ed., pp. 175185.Google Scholar
7. Grambow, B. and Strachan, D.M. (1988), A Comparison of the Performance of Nuclear Waste Glass by Modeling, PNL 6698. Pacific Northwest Laboratory, Richland, WA.Google Scholar
8. Caurel, J. (1990), Altération hydrothermale du verre R7T7: Cinétiques de dissolution du verre à 150°C et 250°C, rôle des phases néoformées, PhD thesis, Université de Poitiers, France.Google Scholar