The Dissolution Behavior of Borosilicate Glasses in Far-From Equilibrium Conditions
Abstract
An area of agreement in the waste glass corrosion community is that, at far-from-equilibrium conditions, the dissolution of borosilicate glasses used to immobilize nuclear waste is known to be a function of both temperature and pH. The aim of this work is to study the effects of temperature and pH on the dissolution rate of three model nuclear waste glasses (SON68, ISG, AFCI). The dissolution rate data are then used to parameterize a kinetic rate model based on Transition State Theory that has been developed to model glass corrosion behavior in dilute conditions. To do this, experiments were conducted at temperatures of 23, 40, 70, and 90 °C and pH(22 °C) values of 9, 10, 11, and 12 with the single-pass flow-through (SPFT) test method. Both the absolute dissolution rates and the rate model parameters are compared with previous results. Rate model parameters for the three glasses studied here are nearly equivalent within error and in relative agreement with previous studies though quantifiable differences exist. The glass dissolution rates were analyzed with a linear multivariate regression (LMR) and a nonlinear multivariate regression performed with the use of the Glass Corrosion Modeling Tool (GCMT), with which a robust uncertainty analysis ismore »
- Authors:
-
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1420433
- Report Number(s):
- PNNL-SA-126627
Journal ID: ISSN 0016-7037; PII: S001670371830070X; TRN: US1801494
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Geochimica et Cosmochimica Acta
- Additional Journal Information:
- Journal Volume: 226; Journal ID: ISSN 0016-7037
- Publisher:
- The Geochemical Society; The Meteoritical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES
Citation Formats
Neeway, James J., Rieke, Peter C., Parruzot, Benjamin P., Ryan, Joseph V., and Asmussen, R. Matthew. The Dissolution Behavior of Borosilicate Glasses in Far-From Equilibrium Conditions. United States: N. p., 2018.
Web. doi:10.1016/j.gca.2018.02.001.
Neeway, James J., Rieke, Peter C., Parruzot, Benjamin P., Ryan, Joseph V., & Asmussen, R. Matthew. The Dissolution Behavior of Borosilicate Glasses in Far-From Equilibrium Conditions. United States. https://doi.org/10.1016/j.gca.2018.02.001
Neeway, James J., Rieke, Peter C., Parruzot, Benjamin P., Ryan, Joseph V., and Asmussen, R. Matthew. Sat .
"The Dissolution Behavior of Borosilicate Glasses in Far-From Equilibrium Conditions". United States. https://doi.org/10.1016/j.gca.2018.02.001. https://www.osti.gov/servlets/purl/1420433.
@article{osti_1420433,
title = {The Dissolution Behavior of Borosilicate Glasses in Far-From Equilibrium Conditions},
author = {Neeway, James J. and Rieke, Peter C. and Parruzot, Benjamin P. and Ryan, Joseph V. and Asmussen, R. Matthew},
abstractNote = {An area of agreement in the waste glass corrosion community is that, at far-from-equilibrium conditions, the dissolution of borosilicate glasses used to immobilize nuclear waste is known to be a function of both temperature and pH. The aim of this work is to study the effects of temperature and pH on the dissolution rate of three model nuclear waste glasses (SON68, ISG, AFCI). The dissolution rate data are then used to parameterize a kinetic rate model based on Transition State Theory that has been developed to model glass corrosion behavior in dilute conditions. To do this, experiments were conducted at temperatures of 23, 40, 70, and 90 °C and pH(22 °C) values of 9, 10, 11, and 12 with the single-pass flow-through (SPFT) test method. Both the absolute dissolution rates and the rate model parameters are compared with previous results. Rate model parameters for the three glasses studied here are nearly equivalent within error and in relative agreement with previous studies though quantifiable differences exist. The glass dissolution rates were analyzed with a linear multivariate regression (LMR) and a nonlinear multivariate regression performed with the use of the Glass Corrosion Modeling Tool (GCMT), with which a robust uncertainty analysis is performed. This robust analysis highlights the high degree of correlation of various parameters in the kinetic rate model. As more data are obtained on borosilicate glasses with varying compositions, a mathematical description of the effect of glass composition on the rate parameter values should be possible. This would allow for the possibility of calculating the forward dissolution rate of glass based solely on composition. In addition, the method of determination of parameter uncertainty and correlation provides a framework for other rate models that describe the dissolution rates of other amorphous and crystalline materials in a wide range of chemical conditions. As a result, the higher level of uncertainty analysis would provide a basis for comparison of different rate models and allow for a better means of quantifiably comparing the various models.},
doi = {10.1016/j.gca.2018.02.001},
journal = {Geochimica et Cosmochimica Acta},
number = ,
volume = 226,
place = {United States},
year = {2018},
month = {2}
}
Web of Science
Figures / Tables:

Works referenced in this record:
Thermodynamic and kinetic constraints on reaction rates among minerals and aqueous solutions; I, Theoretical considerations
journal, March 1982
- Aagaard, P.; Helgeson, H. C.
- American Journal of Science, Vol. 282, Issue 3
The kinetics and mechanisms of simulated British Magnox waste glass dissolution as a function of pH, silicic acid activity and time in low temperature aqueous systems
journal, October 2000
- Abraitis, P. K.; Livens, F. R.; Monteith, J. E.
- Applied Geochemistry, Vol. 15, Issue 9
Hydrolysis of R7T7 Nuclear Waste Glass in Dilute Media: Mechanisms and Rate as a function of Ph
journal, January 1990
- Advocat, T.; Crovisier, J. L.; Vernaz, E.
- MRS Proceedings, Vol. 212
Influence of zirconium on the structure of pristine and leached soda-lime borosilicate glasses: Towards a quantitative approach by 17O MQMAS NMR
journal, August 2008
- Angeli, Frédéric; Charpentier, Thibault; Gaillard, Marina
- Journal of Non-Crystalline Solids, Vol. 354, Issue 31
First investigations of the influence of IVB elements (Ti, Zr, and Hf) on the chemical durability of soda-lime borosilicate glasses
journal, October 2010
- Bergeron, Boris; Galoisy, Laurence; Jollivet, Patrick
- Journal of Non-Crystalline Solids, Vol. 356, Issue 44-49
Geologic Disposal of High-Level Radioactive Waste: Status, Key Issues, and Trends
journal, November 2012
- Birkholzer, Jens; Houseworth, James; Tsang, Chin-Fu
- Annual Review of Environment and Resources, Vol. 37, Issue 1
A Kinetic Model for Borosilicate Glass Dissolution Based on the Dissolution Affinity of a Surface Alteration Layer
journal, January 1989
- Bourcier, William L.; Peiffer, Dennis W.; Knauss, Kevin G.
- MRS Proceedings, Vol. 176
Kinetics of Mineral Dissolution
book, January 2008
- Brantley, Susan L.; Brantley, Susan L.; Kubicki, James D.
- Kinetics of Water-Rock Interaction, p 151-210
Principal component analysis
journal, January 2014
- Bro, Rasmus; Smilde, Age K.
- Anal. Methods, Vol. 6, Issue 9
Insight into silicate-glass corrosion mechanisms
journal, October 2008
- Cailleteau, Céline; Angeli, Frédéric; Devreux, François
- Nature Materials, Vol. 7, Issue 12
Single-pass flow-through test elucidation of weathering behavior and evaluation of contaminant release models for Hanford tank residual radioactive waste
journal, January 2013
- Cantrell, Kirk J.; Carroll, Kenneth C.; Buck, Edgar C.
- Applied Geochemistry, Vol. 28
The initial dissolution rates of simulated UK Magnox–ThORP blend nuclear waste glass as a function of pH, temperature and waste loading
journal, November 2015
- Cassingham, N.; Corkhill, C. L.; Backhouse, D. J.
- Mineralogical Magazine, Vol. 79, Issue 6
Modules based on the geochemical model PHREEQC for use in scripting and programming languages
journal, October 2011
- Charlton, Scott R.; Parkhurst, David L.
- Computers & Geosciences, Vol. 37, Issue 10
Silicate Glass and Mineral Dissolution: Calculated Reaction Paths and Activation Energies for Hydrolysis of a Q 3 Si by H 3 O + Using Ab Initio Methods
journal, January 2006
- Criscenti, Louise J.; Kubicki, James D.; Brantley, Susan L.
- The Journal of Physical Chemistry A, Vol. 110, Issue 1
Hafnium in peralkaline and peraluminous boro-aluminosilicate glass and glass sub-components: a solubility study
journal, October 2003
- Davis, L. L.; Darab, J. G.; Qian, M.
- Journal of Non-Crystalline Solids, Vol. 328, Issue 1-3
R7T7 Glass Initial Dissolution Rate Measurements Using a High-Temperature Soxhlet Device
journal, January 1990
- Delage, Fabienne; Dussossoy, J. L.
- MRS Proceedings, Vol. 212
Kinetics of quartz dissolution in electrolyte solutions using a hydrothermal mixed flow reactor
journal, April 1990
- Dove, Patricia M.; Crerar, David A.
- Geochimica et Cosmochimica Acta, Vol. 54, Issue 4
The dissolution kinetics of quartz in aqueous mixed cation solutions
journal, November 1999
- Dove, Patricia M.
- Geochimica et Cosmochimica Acta, Vol. 63, Issue 22
The Activated Complex in Chemical Reactions
journal, February 1935
- Eyring, Henry
- The Journal of Chemical Physics, Vol. 3, Issue 2
Resumption of nuclear glass alteration: State of the art
journal, May 2014
- Fournier, Maxime; Gin, Stéphane; Frugier, Pierre
- Journal of Nuclear Materials, Vol. 448, Issue 1-3
Glass dissolution rate measurement and calculation revisited
journal, August 2016
- Fournier, Maxime; Ull, Aurélien; Nicoleau, Elodie
- Journal of Nuclear Materials, Vol. 476
SON68 nuclear glass dissolution kinetics: Current state of knowledge and basis of the new GRAAL model
journal, October 2008
- Frugier, P.; Gin, S.; Minet, Y.
- Journal of Nuclear Materials, Vol. 380, Issue 1-3
The mechanism of borosilicate glass corrosion revisited
journal, June 2015
- Geisler, Thorsten; Nagel, Thorsten; Kilburn, Matt R.
- Geochimica et Cosmochimica Acta, Vol. 158
Nuclear Glass Durability: New Insight into Alteration Layer Properties
journal, August 2011
- Gin, Stéphane; Guittonneau, Claire; Godon, Nicole
- The Journal of Physical Chemistry C, Vol. 115, Issue 38
Effect of composition on the short-term and long-term dissolution rates of ten borosilicate glasses of increasing complexity from 3 to 30 oxides
journal, September 2012
- Gin, Stéphane; Beaudoux, Xavier; Angéli, Frédéric
- Journal of Non-Crystalline Solids, Vol. 358, Issue 18-19
An international initiative on long-term behavior of high-level nuclear waste glass
journal, June 2013
- Gin, S.; Abdelouas, A.; Criscenti, L. J.
- Materials Today, Vol. 16, Issue 6
Origin and consequences of silicate glass passivation by surface layers
journal, February 2015
- Gin, Stéphane; Jollivet, Patrick; Fournier, Maxime
- Nature Communications, Vol. 6, Issue 1
The controversial role of inter-diffusion in glass alteration
journal, November 2016
- Gin, S.; Neill, L.; Fournier, M.
- Chemical Geology, Vol. 440
A General Rate Equation for Nuclear Waste Glass Corrosion
journal, January 1984
- Grambow, B.
- MRS Proceedings, Vol. 44
Experimental determination of plagioclase dissolution rates as a function of its composition and pH at 22°C
journal, August 2014
- Gudbrandsson, Snorri; Wolff-Boenisch, Domenik; Gislason, Sigurdur R.
- Geochimica et Cosmochimica Acta, Vol. 139
In-situ Raman and Brillouin light scattering study of the international simple glass in response to temperature and pressure
journal, March 2015
- Guerette, Michael; Huang, Liping
- Journal of Non-Crystalline Solids, Vol. 411
Dissolution of albite glass and crystal
journal, August 2000
- Hamilton, James P.; Pantano, Carlo G.; Brantley, Susan L.
- Geochimica et Cosmochimica Acta, Vol. 64, Issue 15
Glass–water interaction: Effect of high-valence cations on glass structure and chemical durability
journal, May 2016
- Hopf, J.; Kerisit, S. N.; Angeli, F.
- Geochimica et Cosmochimica Acta, Vol. 181
The dissolution kinetics of amorphous silica into sodium chloride solutions: effects of temperature and ionic strength
journal, December 2000
- Icenhower, Jonathan P.; Dove, Patricia M.
- Geochimica et Cosmochimica Acta, Vol. 64, Issue 24
Experimentally determined dissolution kinetics of Na-rich borosilicate glass at far from equilibrium conditions: Implications for Transition State Theory
journal, June 2008
- Icenhower, Jonathan P.; McGrail, B. Peter; Shaw, Wendy J.
- Geochimica et Cosmochimica Acta, Vol. 72, Issue 12
Experimentally determined dissolution kinetics of SON68 glass at 90°C over a silica saturation interval: Evidence against a linear rate law
journal, August 2013
- Icenhower, Jonathan P.; Steefel, Carl I.
- Journal of Nuclear Materials, Vol. 439, Issue 1-3
Dissolution rate of borosilicate glass SON68: A method of quantification based upon interferometry and implications for experimental and natural weathering rates of glass
journal, May 2015
- Icenhower, Jonathan P.; Steefel, Carl I.
- Geochimica et Cosmochimica Acta, Vol. 157
Initial dissolution rate of a Japanese simulated high-level waste glass P0798 as a function of pH and temperature measured by using micro-channel flow-through test method
journal, April 2012
- Inagaki, Yaohiro; Makigaki, Hikaru; Idemitsu, Kazuya
- Journal of Nuclear Science and Technology, Vol. 49, Issue 4
Initial Dissolution Rate of the International Simple Glass as a Function of pH and Temperature Measured Using Microchannel Flow-Through Test Method
journal, October 2013
- Inagaki, Yaohiro; Kikunaga, Taiki; Idemitsu, Kazuya
- International Journal of Applied Glass Science, Vol. 4, Issue 4
Investigation of the maximum dissolution rates and temperature dependence of a simulated UK nuclear waste glass in circum-neutral media at 40 and 90°C in a dynamic system
journal, July 2017
- Iwalewa, Tajudeen M.; Qu, Tingyu; Farnan, Ian
- Applied Geochemistry, Vol. 82
Alteration kinetics of a simplified nuclear glass in an aqueous medium: effects of solution chemistry and of protective gel properties on diminishing the alteration rate
journal, July 2000
- Jégou, C.; Gin, S.; Larché, F.
- Journal of Nuclear Materials, Vol. 280, Issue 2
Forward dissolution rate of silicate glasses of nuclear interest in clay-equilibrated groundwater
journal, November 2012
- Jollivet, P.; Gin, S.; Schumacher, S.
- Chemical Geology, Vol. 330-331
An experimental study of illite dissolution kinetics as a function of ph from 1.4 to 12.4 and temperature from 5 to 50°C
journal, October 2003
- Köhler, Stephan J.; Dufaud, Fabien; Oelkers, Eric H.
- Geochimica et Cosmochimica Acta, Vol. 67, Issue 19
Chemical kinetics of water-rock interactions
journal, June 1984
- Lasaga, Antonio C.
- Journal of Geophysical Research: Solid Earth, Vol. 89, Issue B6
Measurement of kinetic rate law parameters on a NaCaAl borosilicate glass for low-activity waste
journal, October 1997
- McGrail, B. P.; Ebert, W. L.; Bakel, A. J.
- Journal of Nuclear Materials, Vol. 249, Issue 2-3
Near-field performance assessment for a low-activity waste glass disposal system: laboratory testing to modeling results
journal, September 2001
- McGrail, B. P.; Bacon, D. H.; Icenhower, J. P.
- Journal of Nuclear Materials, Vol. 298, Issue 1-2
The structure of Na2O–Al2O3–SiO2 glass: impact on sodium ion exchange in H2O and D2O
journal, December 2001
- McGrail, B. P.; Icenhower, J. P.; Shuh, D. K.
- Journal of Non-Crystalline Solids, Vol. 296, Issue 1-2
Dissolution mechanism of the SON68 reference nuclear waste glass: New data in dynamic system in silica saturation conditions
journal, August 2011
- Neeway, J.; Abdelouas, A.; Grambow, B.
- Journal of Nuclear Materials, Vol. 415, Issue 1
An experimental study of the dissolution mechanism and rates of muscovite
journal, October 2008
- Oelkers, Eric H.; Schott, Jacques; Gauthier, Jean-Marie
- Geochimica et Cosmochimica Acta, Vol. 72, Issue 20
The ion exchange phase in corrosion of nuclear waste glasses
journal, November 2006
- Ojovan, Michael I.; Pankov, Alexey; Lee, William E.
- Journal of Nuclear Materials, Vol. 358, Issue 1
Reaction of soda lime silicate glass in isotopically labelled water
journal, October 1986
- Pederson, L. R.; Baer, D. R.; McVay, G. L.
- Journal of Non-Crystalline Solids, Vol. 86, Issue 3
An experimental study of the dissolution rates of simulated aluminoborosilicate waste glasses as a function of pH and temperature under dilute conditions
journal, September 2008
- Pierce, Eric M.; Rodriguez, Elsa A.; Calligan, L. J.
- Applied Geochemistry, Vol. 23, Issue 9
Experimental determination of the effect of the ratio of B/Al on glass dissolution along the nepheline (NaAlSiO4)–malinkoite (NaBSiO4) join
journal, May 2010
- Pierce, E. M.; Reed, L. R.; Shaw, W. J.
- Geochimica et Cosmochimica Acta, Vol. 74, Issue 9
Rate equations for modeling carbon dioxide sequestration in basalt
journal, June 2017
- Pollyea, Ryan M.; Rimstidt, J. Donald
- Applied Geochemistry, Vol. 81
The kinetics of silica-water reactions
journal, November 1980
- Rimstidt, J. D.; Barnes, H. L.
- Geochimica et Cosmochimica Acta, Vol. 44, Issue 11, p. 1683-1699
Dissolution of Columbia River Basalt under mildly acidic conditions as a function of temperature: Experimental results relevant to the geological sequestration of carbon dioxide
journal, May 2009
- Todd Schaef, H.; Peter McGrail, B.
- Applied Geochemistry, Vol. 24, Issue 5
High energy ion beam studies of ion exchange in a Na2O–Al2O3–SiO2 glass
journal, February 2002
- Shutthanandan, V.; Baer, D. R.; Thevuthasan, S.
- Journal of Applied Physics, Vol. 91, Issue 4
Compositional effects on long-term dissolution of borosilicate glass
journal, July 2000
- Strachan, Denis M.; Croak, Theresa L.
- Journal of Non-Crystalline Solids, Vol. 272, Issue 1
Glass dissolution: testing and modeling for long-term behavior
journal, September 2001
- Strachan, Denis M.
- Journal of Nuclear Materials, Vol. 298, Issue 1-2
Effects of alteration product precipitation on glass dissolution
journal, June 2014
- Strachan, Denis M.; Neeway, James J.
- Applied Geochemistry, Vol. 45
Glass dissolution as a function of pH and its implications for understanding mechanisms and future experiments
journal, December 2017
- Strachan, Denis
- Geochimica et Cosmochimica Acta, Vol. 219
Impact of boron complexation by Tris buffer on the initial dissolution rate of borosilicate glasses
journal, June 2013
- Tournié, A.; Majérus, O.; Lefèvre, G.
- Journal of Colloid and Interface Science, Vol. 400
The Long-Term Corrosion and Modelling of Two Simulated Belgian Reference High-Level Waste Glasses
journal, January 1987
- Van Iseghem, P.; Grambow, B.
- MRS Proceedings, Vol. 112
The dissolution rates of natural glasses as a function of their composition at pH 4 and 10.6, and temperatures from 25 to 74°C
journal, December 2004
- Wolff-Boenisch, Domenik; Gislason, Sigurdur R.; Oelkers, Eric H.
- Geochimica et Cosmochimica Acta, Vol. 68, Issue 23
First-Principles Study of Hydrolysis Reaction Barriers in a Sodium Borosilicate Glass
journal, November 2013
- Zapol, Peter; He, Haiying; Kwon, Kideok D.
- International Journal of Applied Glass Science, Vol. 4, Issue 4
Works referencing / citing this record:
An Assessment of Initial Leaching Characteristics of Alkali-Borosilicate Glasses for Nuclear Waste Immobilization
journal, May 2019
- Farid, Osama; Ojovan, Michael; Massoud, A.
- Materials, Vol. 12, Issue 9
Coupling Radioactive Waste Glass Dissolution Measurements in Generic Groundwaters With Reactive Transport Modeling of Repository Scenarios
journal, October 2019
- Iwalewa, T. M.; Farnan, I.
- Water Resources Research, Vol. 55, Issue 10
Evolution of cations speciation during the initial leaching stage of alkali-borosilicate-glasses
journal, January 2020
- Farid, Osama M.; Ojovan, M. I.; Rahman, R. O. Abdel
- MRS Advances, Vol. 5, Issue 3-4
A comparative review of the aqueous corrosion of glasses, crystalline ceramics, and metals
journal, May 2018
- Frankel, Gerald S.; Vienna, John D.; Lian, Jie
- npj Materials Degradation, Vol. 2, Issue 1
Physical and optical properties of the International Simple Glass
journal, April 2019
- Kaspar, Tiffany C.; Ryan, Joseph V.; Pantano, Carlo G.
- npj Materials Degradation, Vol. 3, Issue 1
Water diffusion in Zr‐containing fiberglass materials at room temperature
journal, March 2019
- Glazneva, Tatiana S.; Paukshtis, Evgeny A.; Sadovskaya, Ekaterina M.
- Journal of the American Ceramic Society, Vol. 102, Issue 9
Corrosion of the International Simple Glass under acidic to hyperalkaline conditions
journal, September 2018
- Backhouse, Daniel J.; Fisher, Adam J.; Neeway, James J.
- npj Materials Degradation, Vol. 2, Issue 1
Figures / Tables found in this record: