Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: 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 » 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.« less

Authors:
 [1];  [1];  [1];  [1];  [1]
+ Show Author Affiliations
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (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.
Copy to clipboard
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
Copy to clipboard
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.
Copy to clipboard
@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}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1016/j.gca.2018.02.001
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 32 works
Citation information provided by
Web of Science

Figures / Tables:

Table 1 Table 1: List of glass compositions in mass%, mol%, normalization factor for Si, Na, and B (unitless), and density (10-3 kg cm-3).
All figures and tables (14 total)
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Thermodynamic and kinetic constraints on reaction rates among minerals and aqueous solutions; I, Theoretical considerations
journal, March 1982

Hydrolysis of R7T7 Nuclear Waste Glass in Dilute Media: Mechanisms and Rate as a function of Ph
journal, January 1990

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

First investigations of the influence of IVB elements (Ti, Zr, and Hf) on the chemical durability of soda-lime borosilicate glasses
journal, October 2010

Geologic Disposal of High-Level Radioactive Waste: Status, Key Issues, and Trends
journal, November 2012

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
  • DOI: 10.1557/PROC-176-209

Kinetics of Mineral Dissolution
book, January 2008

  • Brantley, Susan L.; Brantley, Susan L.; Kubicki, James D.
  • Kinetics of Water-Rock Interaction, p 151-210
  • DOI: 10.1007/978-0-387-73563-4_5

Principal component analysis
journal, January 2014

Insight into silicate-glass corrosion mechanisms
journal, October 2008

  • Cailleteau, Céline; Angeli, Frédéric; Devreux, François
  • Nature Materials, Vol. 7, Issue 12
  • DOI: 10.1038/nmat2301

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

Modules based on the geochemical model PHREEQC for use in scripting and programming languages
journal, October 2011

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
  • DOI: 10.1021/jp044360a

Hafnium in peralkaline and peraluminous boro-aluminosilicate glass and glass sub-components: a solubility study
journal, October 2003

R7T7 Glass Initial Dissolution Rate Measurements Using a High-Temperature Soxhlet Device
journal, January 1990

Kinetics of quartz dissolution in electrolyte solutions using a hydrothermal mixed flow reactor
journal, April 1990

The dissolution kinetics of quartz in aqueous mixed cation solutions
journal, November 1999

The Activated Complex in Chemical Reactions
journal, February 1935

  • Eyring, Henry
  • The Journal of Chemical Physics, Vol. 3, Issue 2
  • DOI: 10.1063/1.1749604

Resumption of nuclear glass alteration: State of the art
journal, May 2014

Glass dissolution rate measurement and calculation revisited
journal, August 2016

SON68 nuclear glass dissolution kinetics: Current state of knowledge and basis of the new GRAAL model
journal, October 2008

The mechanism of borosilicate glass corrosion revisited
journal, June 2015

  • Geisler, Thorsten; Nagel, Thorsten; Kilburn, Matt R.
  • Geochimica et Cosmochimica Acta, Vol. 158
  • DOI: 10.1016/j.gca.2015.02.039

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
  • DOI: 10.1021/jp205477q

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

An international initiative on long-term behavior of high-level nuclear waste glass
journal, June 2013

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
  • DOI: 10.1038/ncomms7360

The controversial role of inter-diffusion in glass alteration
journal, November 2016

A General Rate Equation for Nuclear Waste Glass Corrosion
journal, January 1984

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
  • DOI: 10.1016/j.gca.2014.04.028

In-situ Raman and Brillouin light scattering study of the international simple glass in response to temperature and pressure
journal, March 2015

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
  • DOI: 10.1016/S0016-7037(00)00388-4

Glass–water interaction: Effect of high-valence cations on glass structure and chemical durability
journal, May 2016

The dissolution kinetics of amorphous silica into sodium chloride solutions: effects of temperature and ionic strength
journal, December 2000

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
  • DOI: 10.1016/j.gca.2008.02.026

Experimentally determined dissolution kinetics of SON68 glass at 90°C over a silica saturation interval: Evidence against a linear rate law
journal, August 2013

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
  • DOI: 10.1080/00223131.2012.669246

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
  • DOI: 10.1111/ijag.12043

Forward dissolution rate of silicate glasses of nuclear interest in clay-equilibrated groundwater
journal, November 2012

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

Chemical kinetics of water-rock interactions
journal, June 1984

Measurement of kinetic rate law parameters on a NaCaAl borosilicate glass for low-activity waste
journal, October 1997

Near-field performance assessment for a low-activity waste glass disposal system: laboratory testing to modeling results
journal, September 2001

The structure of Na2O–Al2O3–SiO2 glass: impact on sodium ion exchange in H2O and D2O
journal, December 2001

Dissolution mechanism of the SON68 reference nuclear waste glass: New data in dynamic system in silica saturation conditions
journal, August 2011

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
  • DOI: 10.1016/j.gca.2008.01.040

The ion exchange phase in corrosion of nuclear waste glasses
journal, November 2006

Reaction of soda lime silicate glass in isotopically labelled water
journal, October 1986

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

Experimental determination of the effect of the ratio of B/Al on glass dissolution along the nepheline (NaAlSiO4)–malinkoite (NaBSiO4) join
journal, May 2010

Rate equations for modeling carbon dioxide sequestration in basalt
journal, June 2017

The kinetics of silica-water reactions
journal, November 1980

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
  • DOI: 10.1063/1.1432119

Compositional effects on long-term dissolution of borosilicate glass
journal, July 2000

Glass dissolution: testing and modeling for long-term behavior
journal, September 2001

Effects of alteration product precipitation on glass dissolution
journal, June 2014

Glass dissolution as a function of pH and its implications for understanding mechanisms and future experiments
journal, December 2017

Impact of boron complexation by Tris buffer on the initial dissolution rate of borosilicate glasses
journal, June 2013

The Long-Term Corrosion and Modelling of Two Simulated Belgian Reference High-Level Waste Glasses
journal, January 1987

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
  • DOI: 10.1016/j.gca.2004.05.027

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
  • DOI: 10.1111/ijag.12052
    Sort by:
    [ × clear filter / sort ]

    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
    • DOI: 10.3390/ma12091462

    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
    • DOI: 10.1557/adv.2020.39

    A comparative review of the aqueous corrosion of glasses, crystalline ceramics, and metals
    journal, May 2018

    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
    • DOI: 10.1038/s41529-019-0069-2

    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
    • DOI: 10.1111/jace.16411

    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
    • DOI: 10.1038/s41529-018-0050-5

    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
    • DOI: 10.3390/ma12091462
      Sort by:
      [ × clear filter / sort ]

      Figures / Tables found in this record:

      Table 1 (p. 8)table
      Figure 1 (p. 9)figure
      Table 2 (p. 10)table
      Figure 2 (p. 13)figure
      Figure 3 (p. 15)figure
      Table 3: Part 1 (p. 16)table
      Table 3: Part 2 (p. 17)table
      Table 4: Part 1 (p. 18)table
      Table 4: Part 2 (p. 19)table
      Table 5 (p. 20)table
      Table 6 (p. 21)table
      Figure 4 (p. 22)figure
      Figure 5 (p. 23)figure
      Figure 6 (p. 29)figure
        [ × clear filter / sort ]
        Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

        Similar Records in DOE PAGES and OSTI.GOV collections: