DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Modeling Interfacial Glass-Water Reactions: Recent Advances and Current Limitations

Abstract

Describing the reactions that occur at the glass-water interface and control the development of the altered layer constitutes one of the main scientific challenges impeding existing models from providing accurate radionuclide release estimates. Radionuclide release estimates are a critical component of the safety basis for geologic repositories. The altered layer (i.e., amorphous hydrated surface layer and crystalline reaction products) represents a complex region, both physically and chemically, sandwiched between two distinct boundaries pristine glass surface at the inner most interface and aqueous solution at the outer most interface. Computational models, spanning different length and time-scales, are currently being developed to improve our understanding of this complex and dynamic process with the goal of accurately describing the pore-scale changes that occur as the system evolves. These modeling approaches include geochemical simulations [i.e., classical reaction path simulations and glass reactivity in allowance for alteration layer (GRAAL) simulations], Monte Carlo simulations, and Molecular Dynamics methods. Finally, in this manuscript, we discuss the advances and limitations of each modeling approach placed in the context of the glass-water reaction and how collectively these approaches provide insights into the mechanisms that control the formation and evolution of altered layers.

Authors:
 [1];  [2];  [3];  [3];  [4]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Environmental Sciences Division
  2. Alternative Energies and Atomic Energy Commission (CEA), Bagnols-sur-Ceze (France). Marcoule DEN Lab. of Long Term Behavioral Study
  3. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Dept. of Geochemistry
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical Sciences Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE); USDOE Office of Environmental Management (EM); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1185436
Grant/Contract Number:  
AC05-00OR22725; AC05-76RL01830; AC04-94AL85000
Resource Type:
Accepted Manuscript
Journal Name:
International Journal of Applied Glass Science
Additional Journal Information:
Journal Volume: 5; Journal Issue: 4; Journal ID: ISSN 2041-1286
Publisher:
American Ceramic Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 97 MATHEMATICS AND COMPUTING; alteration layer; secondary phase formation; nuclear waste glass; GRAAL; geochemical reaction path modeling; glass corrosion; Molecular Dynamic simulations; and Monte Carlo simulations

Citation Formats

Pierce, Eric M., Frugier, Pierre, Criscenti, Louise J., Kwon, Kideok D., and Kerisit, Sebastien N.. Modeling Interfacial Glass-Water Reactions: Recent Advances and Current Limitations. United States: N. p., 2014. Web. doi:10.1111/ijag.12077.
Pierce, Eric M., Frugier, Pierre, Criscenti, Louise J., Kwon, Kideok D., & Kerisit, Sebastien N.. Modeling Interfacial Glass-Water Reactions: Recent Advances and Current Limitations. United States. https://doi.org/10.1111/ijag.12077
Pierce, Eric M., Frugier, Pierre, Criscenti, Louise J., Kwon, Kideok D., and Kerisit, Sebastien N.. Sat . "Modeling Interfacial Glass-Water Reactions: Recent Advances and Current Limitations". United States. https://doi.org/10.1111/ijag.12077. https://www.osti.gov/servlets/purl/1185436.
@article{osti_1185436,
title = {Modeling Interfacial Glass-Water Reactions: Recent Advances and Current Limitations},
author = {Pierce, Eric M. and Frugier, Pierre and Criscenti, Louise J. and Kwon, Kideok D. and Kerisit, Sebastien N.},
abstractNote = {Describing the reactions that occur at the glass-water interface and control the development of the altered layer constitutes one of the main scientific challenges impeding existing models from providing accurate radionuclide release estimates. Radionuclide release estimates are a critical component of the safety basis for geologic repositories. The altered layer (i.e., amorphous hydrated surface layer and crystalline reaction products) represents a complex region, both physically and chemically, sandwiched between two distinct boundaries pristine glass surface at the inner most interface and aqueous solution at the outer most interface. Computational models, spanning different length and time-scales, are currently being developed to improve our understanding of this complex and dynamic process with the goal of accurately describing the pore-scale changes that occur as the system evolves. These modeling approaches include geochemical simulations [i.e., classical reaction path simulations and glass reactivity in allowance for alteration layer (GRAAL) simulations], Monte Carlo simulations, and Molecular Dynamics methods. Finally, in this manuscript, we discuss the advances and limitations of each modeling approach placed in the context of the glass-water reaction and how collectively these approaches provide insights into the mechanisms that control the formation and evolution of altered layers.},
doi = {10.1111/ijag.12077},
journal = {International Journal of Applied Glass Science},
number = 4,
volume = 5,
place = {United States},
year = {Sat Jul 12 00:00:00 EDT 2014},
month = {Sat Jul 12 00:00:00 EDT 2014}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 24 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Numerical modelling of glass dissolution: gel layer morphology
journal, September 2001


Sodium ion migration mechanisms in silicate glasses probed by molecular dynamics simulations
journal, August 2003


Leaching of borosilicate glasses. II. Model and Monte-Carlo simulations
journal, September 2004


Molecular Dynamics Simulations of Water Structure and Diffusion in Silica Nanopores
journal, May 2012

  • Bourg, Ian C.; Steefel, Carl I.
  • The Journal of Physical Chemistry C, Vol. 116, Issue 21
  • DOI: 10.1021/jp301299a

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


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

Role and properties of the gel formed during nuclear glass alteration: importance of gel formation conditions
journal, September 2001


Deep-UV Raman spectroscopic analysis of structure and dissolution rates of silica-rich sodium borosilicate glasses
journal, May 2011


Aqueous alteration of five-oxide silicate glasses: Experimental approach and Monte Carlo modeling
journal, January 2008


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

Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995


Interdiffusion of hydrogen and alkali ions in a glass surface
journal, December 1975


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


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


Monte Carlo simulations of the dissolution of borosilicate glasses in near-equilibrium conditions
journal, May 2012


New techniques for modelling glass dissolution
journal, September 2001


Molecular dynamics computer simulations of silica surface structure and adsorption of water molecules
journal, April 1990


Solid-state NMR examination of alteration layers on nuclear waste glasses
journal, June 2013


A New Self-Consistent Empirical Interatomic Potential Model for Oxides, Silicates, and Silica-Based Glasses
journal, June 2006

  • Pedone, Alfonso; Malavasi, Gianluca; Menziani, M. Cristina
  • The Journal of Physical Chemistry B, Vol. 110, Issue 24
  • DOI: 10.1021/jp0611018

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


11B NMR studies and structural modeling of Na2OB2O3SiO2 glasses of high soda content
journal, October 1983


Monte Carlo simulations of the corrosion of aluminoborosilicate glasses
journal, October 2013


Development of empirical potentials for sodium borosilicate glass systems
journal, September 2011


Molecular dynamics simulation of a nuclear waste glass matrix
journal, February 1996


Nuclear magnetic resonance studies of the glasses in the system Na2OB2O3SiO2
journal, March 1978


Theoretical and 27Al CPMAS NMR investigation of aluminum coordination changes during aluminosilicate dissolution
journal, May 2005

  • Criscenti, Louise J.; Brantley, Susan L.; Mueller, Karl T.
  • Geochimica et Cosmochimica Acta, Vol. 69, Issue 9
  • DOI: 10.1016/j.gca.2004.10.020

Borosilicate glass alteration driven by magnesium carbonates
journal, January 2012


Thermodynamics of hydrothermal systems at elevated temperatures and pressures
journal, September 1969


Why Do Certain Glasses with a High Dissolution Rate Undergo a Low Degree of Corrosion?
journal, March 2011

  • Cailleteau, Céline; Devreux, François; Spalla, Olivier
  • The Journal of Physical Chemistry C, Vol. 115, Issue 13
  • DOI: 10.1021/jp111458f

Bridging oxygen as a site for proton adsorption on the vitreous silica surface
journal, August 2009

  • Lockwood, Glenn K.; Garofalini, Stephen H.
  • The Journal of Chemical Physics, Vol. 131, Issue 7
  • DOI: 10.1063/1.3205946

First-order dissolution rate law and the role of surface layers in glass performance assessment
journal, September 2001


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

A computer simulation study of natural silicate melts. Part I: Low pressure properties
journal, March 2007


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


Shell-model molecular dynamics calculations of modified silicate glasses
journal, March 2006


Aqueous corrosion of borosilicate glass under acidic conditions: A new corrosion mechanism
journal, June 2010


Monte Carlo simulations of borosilicate glass corrosion: predictions for morphology and kinetics
journal, October 2004


Alkali ion migration mechanisms in silicate glasses probed by molecular dynamics simulations
journal, June 2002

  • Cormack, A. N.; Du, J.; Zeitler, T. R.
  • Physical Chemistry Chemical Physics, Vol. 4, Issue 14
  • DOI: 10.1039/b201721k

Modeling the Water−Bioglass Interface by Ab Initio Molecular Dynamics Simulations
journal, May 2009

  • Tilocca, Antonio; Cormack, Alastair N.
  • ACS Applied Materials & Interfaces, Vol. 1, Issue 6
  • DOI: 10.1021/am900198t

Composition effects on synthetic glass alteration mechanisms: Part 1. Experiments
journal, December 2010


Application of the GRAAL model to leaching experiments with SON68 nuclear glass in initially pure water
journal, August 2009


ReaxFF SiO Reactive Force Field for Silicon and Silicon Oxide Systems
journal, May 2003

  • van Duin, Adri C. T.; Strachan, Alejandro; Stewman, Shannon
  • The Journal of Physical Chemistry A, Vol. 107, Issue 19
  • DOI: 10.1021/jp0276303

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


Module-oriented modeling of reactive transport with HYTEC
journal, April 2003


Investigation of gel porosity clogging during glass leaching
journal, November 2008


Ab Initio Investigation of Dissolution Mechanisms in Aluminosilicate Minerals
journal, February 2009

  • Morrow, Christin P.; Nangia, Shikha; Garrison, Barbara J.
  • The Journal of Physical Chemistry A, Vol. 113, Issue 7
  • DOI: 10.1021/jp8079099

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

On the effect of glass composition in the dissolution of glasses by water
journal, January 2008


Kinetics of leaching near the percolation threshold
journal, December 1998


Effect of clayey groundwater on the dissolution rate of the simulated nuclear waste glass SON68
journal, January 2012


Monte Carlo simulations of the dissolution of borosilicate and aluminoborosilicate glasses in dilute aqueous solutions
journal, September 2011


Monte Carlo Modelling of Glass Dissolution: Comparison with Experiments
journal, January 2000


HLW glass dissolution in the presence of magnesium carbonate: Diffusion cell experiment and coupled modeling of diffusion and geochemical interactions
journal, November 2013


The Structure of Bioactive Silicate Glasses:  New Insight from Molecular Dynamics Simulations
journal, January 2007

  • Tilocca, Antonio; Cormack, Alastair N.; de Leeuw, Nora H.
  • Chemistry of Materials, Vol. 19, Issue 1
  • DOI: 10.1021/cm061631g

Modelling Glass Dissolution with a Monte Carlo Technique
journal, January 1995


Glass–water interphase reactivity with calcium rich solutions
journal, August 2011


Theoretical consideration on the application of the Aagaard–Helgeson rate law to the dissolution of silicate minerals and glasses
journal, September 2008


A molecular dynamic calculation of the structure of sodium silicate glasses
journal, December 1979

  • Soules, T. F.
  • The Journal of Chemical Physics, Vol. 71, Issue 11
  • DOI: 10.1063/1.438210