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Title: Monte Carlo simulation of borosilicate glass dissolution using molecular dynamics-generated glass structures

Abstract

Atomic-scale insights into borosilicate glass dissolution are vital to the development of waste form corrosion models. While Monte Carlo (MC) simulations have been instrumental in advancing the state of knowledge, all simulations to date have relied on lattices to represent the glass structure, potentially introducing artifacts. A new approach (amorphous MC approach) was developed whereby glass structures generated from molecular dynamics simulations were used as starting points for MC simulations. Correlations between dissolution rate and structural features were revealed in MC simulations of sodium borosilicate glasses that covered a wide compositional range. Notably, the lattice MC approach predicted the fraction of tetrahedral boron to have a lesser influence on the dissolution rate than computed with the amorphous MC approach. The lattice MC simulations further overestimated the dissolution rate for a given glass composition. These findings illustrate the importance of using truly amorphous structures in MC simulations of glass corrosion.

Authors:
ORCiD logo [1]; ORCiD logo [2]
+ Show Author Affiliations
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Univ. of North Texas, Denton, TX (United States)
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); Univ. of North Texas, Denton, TX (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE); USDOE Office of Electricity (OE), Advanced Grid Research & Development. Power Systems Engineering Research; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
OSTI Identifier:
1600992
Alternate Identifier(s):
OSTI ID: 1691660
Grant/Contract Number:  
SC0016584; AC05-76RL01830; DESC0016584
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Non-Crystalline Solids
Additional Journal Information:
Journal Volume: 522; Journal Issue: C; Journal ID: ISSN 0022-3093
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Monte Carlo; Glass dissolution; Molecular dynamics; Dissolution mechanisms

Citation Formats

Kerisit, Sebastien, and Du, Jincheng. Monte Carlo simulation of borosilicate glass dissolution using molecular dynamics-generated glass structures. United States: N. p., 2019. Web. doi:10.1016/j.jnoncrysol.2019.119601.
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Kerisit, Sebastien, & Du, Jincheng. Monte Carlo simulation of borosilicate glass dissolution using molecular dynamics-generated glass structures. United States. https://doi.org/10.1016/j.jnoncrysol.2019.119601
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Kerisit, Sebastien, and Du, Jincheng. Mon . "Monte Carlo simulation of borosilicate glass dissolution using molecular dynamics-generated glass structures". United States. https://doi.org/10.1016/j.jnoncrysol.2019.119601. https://www.osti.gov/servlets/purl/1600992.
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@article{osti_1600992,
title = {Monte Carlo simulation of borosilicate glass dissolution using molecular dynamics-generated glass structures},
author = {Kerisit, Sebastien and Du, Jincheng},
abstractNote = {Atomic-scale insights into borosilicate glass dissolution are vital to the development of waste form corrosion models. While Monte Carlo (MC) simulations have been instrumental in advancing the state of knowledge, all simulations to date have relied on lattices to represent the glass structure, potentially introducing artifacts. A new approach (amorphous MC approach) was developed whereby glass structures generated from molecular dynamics simulations were used as starting points for MC simulations. Correlations between dissolution rate and structural features were revealed in MC simulations of sodium borosilicate glasses that covered a wide compositional range. Notably, the lattice MC approach predicted the fraction of tetrahedral boron to have a lesser influence on the dissolution rate than computed with the amorphous MC approach. The lattice MC simulations further overestimated the dissolution rate for a given glass composition. These findings illustrate the importance of using truly amorphous structures in MC simulations of glass corrosion.},
doi = {10.1016/j.jnoncrysol.2019.119601},
journal = {Journal of Non-Crystalline Solids},
number = C,
volume = 522,
place = {United States},
year = {Mon Aug 12 00:00:00 EDT 2019},
month = {Mon Aug 12 00:00:00 EDT 2019}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1016/j.jnoncrysol.2019.119601
Copyright Statement
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Cited by: 8 works
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Figures / Tables:

Figure 1 Figure 1: Example of an amorphous MC simulation of the dissolution of a glass with composition 42.9 mol% SiO2 14.3 mol% B2O3 42.9 mol% Na2O (K3R3 glass). (A) Instantaneous values of the number of dissolved network former sites, Si/B ratio, fraction of sites dissolved as clusters, and interfacial roughness. (B)more » MD-generated glass structure used as repeat unit in the MC simulation. Si, B, Na, and O atoms are shown in red, green, yellow, and blue, respectively. Polyhedron representation is used for the network formers. (C) Snapshots of the MC simulation (from left to right: initial configuration and interfacial region after 1000 and 5000 computer steps). Si, B, and water sites are shown in red, green, and blue, respectively.« less
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      Figures / Tables found in this record:

      Figure 1 (p. 11)figure
      Figure 2 (p. 13)figure
      Table 1 (p. 14)table
      Figure 3 (p. 16)figure
      Figure 4 (p. 18)figure
      Figure 5 (p. 19)figure
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