Hostname: page-component-848d4c4894-cjp7w Total loading time: 0 Render date: 2024-06-23T13:01:41.755Z Has data issue: false hasContentIssue false
  • English
  • Français

Chemistry of Glass Corrosion in High Saline Brines

Published online by Cambridge University Press:  21 February 2011

B. Grambow  and
R. Müller
B. Grambow
Affiliation:
Hahn–Meitner–Institut Berlin, Glienicker Str. 100, D–1000 Berlin 39, FRG
R. Müller
Affiliation:
Hahn–Meitner–Institut Berlin, Glienicker Str. 100, D–1000 Berlin 39, FRG
Get access

Abstract

Experimental data were obtained for conventional pH values corrected for liquid junction, amorphous silica solubility and glass corrosion in concentrated salt brines. The data were interpreted with a geochemical model. The brine chemistry was described with the Pitzer formalism [1] using a data base which allows calculation of brine compositions in equilibrium with salt minerals at temperatures up to 200°C.

In MgCl2 dominated brines Mg silicates form and due to the consumption of Mg the pH decreases with proceeding reaction. A constant pH (about 4) and composition of alteration products is achieved, when the alkali release from the glass balances the Mg consumption. The low pH results in high release of rare earth elements REE and U from the glass. In the NaCl dominated brine MgCl2 becomes exhausted by Mg silicate formation. As long as there is still Mg left in solution the pH decreases. After exhaustion of Mg the pH rises with the alkali release from the glass and analcime is formed.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 176: Symposium U – Scientific Basis for Nuclear Waste Management XIII , 1989 , 229
Copyright
Copyright © Materials Research Society 1990

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] Pitzer, K.S., J.Phys.Chem. 77, 268–277 (1973)Google Scholar
[2] “JSS-Project Phase IV: Final Report - Experimental and Modeling Studies of HLW-Glass Dissolution in Repository Environments”, JSS-Report 87-01, SKB, Stockholm (1987)Google Scholar
[3] Grambow, B., “Nuclear Waste Glass Dissolution: Mechanism, Model and Application”, JSS-Project Report 87–02, (1987)Google Scholar
[4] Lutze, W., Müller, R. and Montserrat, W., Mat. Res. Soc. Symp. Proc. Vol. 112, Materials Research Society, Pittsburgh PA (1988)Google Scholar
[5] Lutze, W., Müller, R. and Montserrat, W., Mat. Res. Soc. Symp. Proc. Vol. 127, Materials Research Society, Pittsburgh PA, pp. 81–89 (1989)Google Scholar
[6] Harvie, C.E., Müller, N., and Weare, J., Geochim. Cos-mochim. Acta 48, 1203–1618 (1984)Google Scholar
[7] Harvie, C.E. and Weare, J., Geochim. Cosmochim. Acta 44, 981–997 (1980)Google Scholar
[8] Gueddari, M., Monnin, C., Perret, D., Fritz, B., Tardy, Y., Chem. Geol. 39, 165–178 (1983)Google Scholar
[9] Marshall, W.L., Geochim.Cosmochim. Acta 44, 907–913 (1980)Google Scholar
[10] Wolery, T.J., “EQ3NR, A Computer Program for Geochemical Aqueous Speciation-Solubility Calculations”, Lawrence Li-vermore Natl. Lab., UCRL-53414, Livermore CA. USA (1983)Google Scholar
[11] Wolery, T.J., “EQ3/6 Modifications for Geochemical Modeling of Brines”, Lawrence Livermore National Laboratory Report, Livermore, CA. USA (1983)Google Scholar
[12] Pabalan, R.T. and Pitzer, K.S., Geochim. Cosmochim. Acta 51, 2429–2443 (1987)Google Scholar
[13] Møller, N., Geochim. Cosmochim. Acta 52, 821–837 (1988)Google Scholar
[14] Greenberg, J.P. und Møller, N., Geochim. Cosmochim. Acta 52, 2503–2518 (1989)Google Scholar
[15] Marshall, W.L. and Chent, C.A., Geochim. Cosmochim. Acta 46, 289–291 (1982)Google Scholar
[16] Chen, C.A. and Marshall, W.L., Geochim. Cosmochim. Acta 46, 279–287 (1982)Google Scholar
[17] Pitzer, K.S., CRC Press. Inc. Boca Raton, Fl., USA (1979)Google Scholar
[18] Reardon, E. J., J. Phys. Chem. 92. (1988) pp. 6426–6431 Google Scholar
[19] Gmelins Handbuch der Anorganischen Chemie, Kalium, An-hangband, Ergänzungsband, (1970)Google Scholar
[20] D'Ans, J., “Die L6sungsgleichgewichte der Systeme der Salze ozeanischer Salzablagerungen” Verlagsgesellschaft für Ackerbau, Berlin (1933)Google Scholar
[21] Knauss, K.G., Wolery, T. and Jackson, K.J., ‘A New Approach to Measure pH in Concentration Electrolytes’ GSA meeting, 1989 Google Scholar
[22] Grambow, B., Müller, R., Rother, A. and Lutze, W., “Radionuclide Release in Low pH High Saline Brines Resulting From Glass Corrosion” to be published in Radiochimica Acta Google Scholar