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Title: Monte Carlo Simulation of the Corrosion of Irradiated Simplified Nuclear Waste Glasses

Abstract

Ballistic effects due to recoil nuclei will be the predominant mode of long-term radiation damage of nuclear waste glass in disposal facilities. While these ballistic effects are known to modify the glass structure in ways that have been quantified using molecular dynamics (MD) simulations, the effect of irradiation-induced structural changes on glass corrosion is not understood. Monte Carlo (MC) simulations were therefore performed to quantify the effects of structural changes determined from MD simulations on the corrosion of simplified nuclear waste glasses, namely sodium borosilicate and sodium alumino-borosilicate glasses. MC simulations were first performed to determine separately the effects of irradiation-induced changes in boron coordination, the number and nature of Qn species, and the angular distribution of Si-O-Si linkages, that is, changes to the short-range order of the glass. Generally, the MC simulations showed the resulting effects on the kinetics (B release rate) and extent (B leached thickness) of corrosion were correlated to the extent of depolymerization of the glass network introduced by these local structural changes. The combined effects of these structural changes, as parameterized using the results of MD simulations, were then determined using a glass composition for which relevant experimental data were available for comparison. Here, themore » combined effect of local changes was lower than the increase in alteration depth observed upon irradiation. This insight from the MC simulations highlighted the need to consider changes in the medium-range order to completely account for experimental observations.« less

Authors:
 [1];  [2];  [3];  [4]
  1. UNIVERSITY PROGRAMS
  2. CEA
  3. CEA Marcoule
  4. BATTELLE (PACIFIC NW LAB)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Performance and Design of Nuclear Waste Forms and Containers (WastePD); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1582587
Report Number(s):
PNNL-SA-140805
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of Non-crystalline Solids
Additional Journal Information:
Journal Volume: 519
Country of Publication:
United States
Language:
English

Citation Formats

Jan, Amreen, Delaye, Jean-Marc, Gin, Stephane, and Kerisit, Sebastien N. Monte Carlo Simulation of the Corrosion of Irradiated Simplified Nuclear Waste Glasses. United States: N. p., 2019. Web. doi:10.1016/j.jnoncrysol.2019.05.025.
Jan, Amreen, Delaye, Jean-Marc, Gin, Stephane, & Kerisit, Sebastien N. Monte Carlo Simulation of the Corrosion of Irradiated Simplified Nuclear Waste Glasses. United States. https://doi.org/10.1016/j.jnoncrysol.2019.05.025
Jan, Amreen, Delaye, Jean-Marc, Gin, Stephane, and Kerisit, Sebastien N. 2019. "Monte Carlo Simulation of the Corrosion of Irradiated Simplified Nuclear Waste Glasses". United States. https://doi.org/10.1016/j.jnoncrysol.2019.05.025.
@article{osti_1582587,
title = {Monte Carlo Simulation of the Corrosion of Irradiated Simplified Nuclear Waste Glasses},
author = {Jan, Amreen and Delaye, Jean-Marc and Gin, Stephane and Kerisit, Sebastien N.},
abstractNote = {Ballistic effects due to recoil nuclei will be the predominant mode of long-term radiation damage of nuclear waste glass in disposal facilities. While these ballistic effects are known to modify the glass structure in ways that have been quantified using molecular dynamics (MD) simulations, the effect of irradiation-induced structural changes on glass corrosion is not understood. Monte Carlo (MC) simulations were therefore performed to quantify the effects of structural changes determined from MD simulations on the corrosion of simplified nuclear waste glasses, namely sodium borosilicate and sodium alumino-borosilicate glasses. MC simulations were first performed to determine separately the effects of irradiation-induced changes in boron coordination, the number and nature of Qn species, and the angular distribution of Si-O-Si linkages, that is, changes to the short-range order of the glass. Generally, the MC simulations showed the resulting effects on the kinetics (B release rate) and extent (B leached thickness) of corrosion were correlated to the extent of depolymerization of the glass network introduced by these local structural changes. The combined effects of these structural changes, as parameterized using the results of MD simulations, were then determined using a glass composition for which relevant experimental data were available for comparison. Here, the combined effect of local changes was lower than the increase in alteration depth observed upon irradiation. This insight from the MC simulations highlighted the need to consider changes in the medium-range order to completely account for experimental observations.},
doi = {10.1016/j.jnoncrysol.2019.05.025},
url = {https://www.osti.gov/biblio/1582587}, journal = {Journal of Non-crystalline Solids},
number = ,
volume = 519,
place = {United States},
year = {2019},
month = {9}
}

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