Hostname: page-component-848d4c4894-xfwgj Total loading time: 0 Render date: 2024-06-27T07:57:21.587Z Has data issue: false hasContentIssue false

Glass Degradation in Performance Assessment Models1

Published online by Cambridge University Press:  08 April 2015

William L. Ebert*
Affiliation:
Argonne National Laboratory, Argonne, IL, U.S.A
Get access

Abstract

The interface with reactive transport models used in performance assessment calculations is described to identify aspects of the glass waste form degradation model important to long-term predictions. These are primarily the conditions that trigger the change from the residual rate to the Stage 3 rate and the values of those rates. Although the processes triggering the change and controlling the Stage 3 rate are not yet understood mechanistically, neither appears related to an intrinsic property of the glass. The sudden and usually significant increase in the glass dissolution rate suggests the processes that trigger the increase are different than the processes controlling glass dissolution prior to that change. Application of a simple expression that was derived for mineral transformation to represent the kinetics of coupled glass dissolution and secondary phase precipitation reactions is shown to be consistent with experimental observations of Stage 3 and useful for modeling long-term glass dissolution in a complex disposal environment.

Type
Articles
Copyright
Copyright © Materials Research Society 2015 

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

Fournier, M., Frugier, P., and Gin, S. (2014). “Resumption of nuclear glass alteration : State of the art.” Journal of Nuclear Materials, 448, 348363.CrossRefGoogle Scholar
Jantzen, C.M. (2013). Letter Report on SRNL Modeling Accelerated Leach Testing of Glass (ALTGLASS). SRNL-L3100-2013-00177; FCRD-SWF-2013-000339, Rev. 0.Google Scholar
Gin, S. et al. . (2013). “An international initiative on long-term behavior of high-level nuclear waste glass.” Materials Today 16(6).CrossRefGoogle Scholar
Aagaard, P. and Helgeson, H.C. (1982). “Thermodynamics and Kinetic Constraints on Reaction Rates among Minerals and Aqueous Solutions. I. Theoretical Considerations,” American Journal of Science, 282, 237285.CrossRefGoogle Scholar
Grambow, B. (1987). Nuclear waste glass dissolution: Mechanism, Model, and Application. Swedish Nuclear Fuel and Waste Management report JSS-TR-87-02.Google Scholar
Lasaga, A.C. (1981). “Rate Laws of Chemical Reactions,” in Reviews in Mineralogy, Vol. 8: Kinetics of Geochemical Processes, ed. Lasaga, A.C. and Kirkpatrick, R.J., pp. 168.Google Scholar
Burch, T.E., Nagy, K.L., and Lasaga, A.C. (1993). “Free Energy Dependence of albite dissolution kinetics at 80 °C and pH 8.8.” Chemical Geology, 105, 137162.CrossRefGoogle Scholar
Maher, K., Steefel, C.I., White, A.F., and Stonestrom, D.A. (2009). “The role of reaction affinity and secondary minerals in regulating chemical weathering rates at the Santa Cruz Soil Chronosequence, California.” Geochimica et Cosmochimica Acta, 73, 28042831.CrossRefGoogle Scholar
Grambow, B, and Strachan, D.M. (1988). A comparison of the performance of nuclear waste glasses by modeling. Pacific Northwest National Laboratory report PNL-6698.CrossRefGoogle Scholar
Van Iseghem, P. and Grambow, B. (1988). “The Long-Term Corrosion and Modeling of Two Simulated Belgian Reference High-Level Waste Glasses.” Scientific Basis for Nuclear Waste Management XI. Material Research Society Symposium Proceedings, 112, 631639.Google Scholar
Strachan, D.M. and Croak, T.L. (2000). “Compositional effects on long-term dissolution of borosilicate glass.” Journal of Non-Crystalline Solids, 272, 2233.CrossRefGoogle Scholar
Grambow, B. and Műller, R. (2001). “First-order dissolution rate law and the role of surface layers in glass performance assessment.” Journal of Nuclear Materials, 298, 112124.CrossRefGoogle Scholar
Strachan, D.M. and Neeway, J. (2014). “Effects of alteration product precipitation on glass dissolution.” Applied Geochemistry 45, 144157.CrossRefGoogle Scholar
Helgeson, H.C. (1968). “Evaluation of irreversible reactions in geochemical processes involving minerals and aqueous solution—I. Thermodynamic relations.” Geochimica et Cosmochimica Acta 32, 853877.CrossRefGoogle Scholar
Helgeson, H. C. (1979). “Mass transfer among minerals and hydrothermal solutions.” In Geochemistry of Hydrothermal Ore Deposits (ed. Barnes, H. L.). John Wiley & Sons, New York, pp. 568610.Google Scholar
Zhu, C. and Lu, P. (2009). “Alkali feldspar dissolution and secondary mineral precipitation in batch systems: 2. Saturation states of product minerals and reaction paths.” Geochimica et Cosmochimica Acta, 73, 31713200.CrossRefGoogle Scholar
Zhu, C. (2009). “Geochemical modeling of reaction paths and geochemical reaction networks.” in Reviews in Mineralogy & Geochemistry, Vol. 70, pp. 533569.CrossRefGoogle Scholar
Lasaga, A. (1998). Kinetic Theory in the Earth Sciences, Princeton University Press, Princeton, NJ. (See section 1.12)CrossRefGoogle Scholar
Nagy, K.L., Blum, A.E., and Lasaga, A.C. (1991). “Dissolution and precipitation kinetics of kaolinite at 90 °C and pH 3: The dependence on solution saturation state.” American Journal of Science, 291, 649686.CrossRefGoogle Scholar
Zhu, C., Lu, P., Zheng, Z., and Ganor, J. (2010). “Coupled alkali feldspar dissolution and secondary mineral precipitation in batch systems: 4. Numerical modeling of kinetic reaction paths.” Geochimica et Cosmochimica Acta, 74, 39633983.CrossRefGoogle Scholar