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Title: Structural role of ZrO2 and its impact on properties of boroaluminosilicate nuclear waste glasses

Abstract

Addition of zirconia (ZrO2) to nuclear waste glasses, even in small amount, significantly affects physical properties such as chemical durability, density, viscosity, and glass transition temperature. Hence ZrO2 plays an important role in the development of nuclear waste glass compositions. It was found recently that addition of zirconia decreases the initial dissolution rate but increases long-term dissolution by changing the protective properties such as porosity of alteration layers. In this study, the International Simple Glass (ISG) with different amounts of ZrO2/SiO2 substitution was simulated using classical molecular dynamics (MD) simulations and recently developed composition-dependent potential sets. Local structural descriptors such as bond distances, bond angle distributions, and coordination numbers were systematically studied and compared with experimental values. Zr K-edge extended X-ray absorption fine structure spectra were also calculated and compared with experiment to resolve the local coordination environment around Zr. Medium-range structural information (e.g., Qn distribution, network connectivity, and ring-size distribution) showed that ZrO2/SiO2 substitution increases the overall network connectivity and the amount of smaller sized rings, which will decrease the initial dissolution rate by strengthening the glass network and limiting water diffusivity. Finally, diffusion and dynamic properties of the ions were studied and discussed to develop a better understandingmore » of the chemical durability of these glasses.« less

Authors:
 [1];  [1];  [2]; ORCiD logo [1]
  1. Univ. of North Texas, Denton, TX (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (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); Univ. of North Texas, Denton, TX (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1668035
Grant/Contract Number:  
SC0016584
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
npj Materials Degradation
Additional Journal Information:
Journal Volume: 2; Journal Issue: 1; Journal ID: ISSN 2397-2106
Publisher:
Springer
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Lu, Xiaonan, Deng, Lu, Kerisit, Sebastien, and Du, Jincheng. Structural role of ZrO2 and its impact on properties of boroaluminosilicate nuclear waste glasses. United States: N. p., 2018. Web. doi:10.1038/s41529-018-0041-6.
Lu, Xiaonan, Deng, Lu, Kerisit, Sebastien, & Du, Jincheng. Structural role of ZrO2 and its impact on properties of boroaluminosilicate nuclear waste glasses. United States. https://doi.org/10.1038/s41529-018-0041-6
Lu, Xiaonan, Deng, Lu, Kerisit, Sebastien, and Du, Jincheng. 2018. "Structural role of ZrO2 and its impact on properties of boroaluminosilicate nuclear waste glasses". United States. https://doi.org/10.1038/s41529-018-0041-6. https://www.osti.gov/servlets/purl/1668035.
@article{osti_1668035,
title = {Structural role of ZrO2 and its impact on properties of boroaluminosilicate nuclear waste glasses},
author = {Lu, Xiaonan and Deng, Lu and Kerisit, Sebastien and Du, Jincheng},
abstractNote = {Addition of zirconia (ZrO2) to nuclear waste glasses, even in small amount, significantly affects physical properties such as chemical durability, density, viscosity, and glass transition temperature. Hence ZrO2 plays an important role in the development of nuclear waste glass compositions. It was found recently that addition of zirconia decreases the initial dissolution rate but increases long-term dissolution by changing the protective properties such as porosity of alteration layers. In this study, the International Simple Glass (ISG) with different amounts of ZrO2/SiO2 substitution was simulated using classical molecular dynamics (MD) simulations and recently developed composition-dependent potential sets. Local structural descriptors such as bond distances, bond angle distributions, and coordination numbers were systematically studied and compared with experimental values. Zr K-edge extended X-ray absorption fine structure spectra were also calculated and compared with experiment to resolve the local coordination environment around Zr. Medium-range structural information (e.g., Qn distribution, network connectivity, and ring-size distribution) showed that ZrO2/SiO2 substitution increases the overall network connectivity and the amount of smaller sized rings, which will decrease the initial dissolution rate by strengthening the glass network and limiting water diffusivity. Finally, diffusion and dynamic properties of the ions were studied and discussed to develop a better understanding of the chemical durability of these glasses.},
doi = {10.1038/s41529-018-0041-6},
url = {https://www.osti.gov/biblio/1668035}, journal = {npj Materials Degradation},
issn = {2397-2106},
number = 1,
volume = 2,
place = {United States},
year = {2018},
month = {6}
}

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Works referencing / citing this record:

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