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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:
Journal Article: 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. doi: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. doi: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}
}

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Free Publicly Available Full Text
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Cited by: 7works
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  • 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. The physico-chemical processes that control the development of this region have a significant impact on the long-term glass-water reaction. 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 Geochemicalmore » Reaction Path simulations, Glass Reactivity in Allowance for Alteration Layer simulations, Monte Carlo simulations, and Molecular Dynamics methods. Discussed in this manuscript are 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; thus providing the fundamental data needed to develop pore-scale equations that enable more accurate predictions of nuclear waste glass corrosion in a geologic repository.« less
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