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Title: Can a simple topological-constraints-based model predict the initial dissolution rate of borosilicate and aluminosilicate glasses?

Abstract

Tuning glass composition to obtain targeted properties generally relies on empirical approaches. However, a deep understanding of the physical and chemical mechanisms linking glass composition to its structure and properties would enable developing reliable predictive models. Indeed, although empirical models are usually able to interpolate composition–property relationships within a given compositional envelope, they often fail at extrapolating predictions far from their training domain. Here, as an alternative route to empirical models, we show that a structural descriptor based on the number of topological constraints per atom can be used to predict the initial dissolution rate of aluminosilicate and borosilicate glasses after being parameterized on different families of glasses (specific series of borosilicate glasses). Sixteen glasses belonging to these families were studied and their initial dissolution rates were determined at 90 °C and pH90 °C = 9, covering rates spanning over 5 orders of magnitude. The model based on topological constraints was trained based on seven select borosilicate glasses (R2 = 0.997) and used to predict the dissolution rate of nine additional borosilicate and aluminosilicate glasses. We show that, provided that corrections are made for high alkali content glasses that dissolve incongruently (preferential release of Na), the model gives reasonable predictions,more » even far from its training domain.« less

Authors:
ORCiD logo [1];  [2];  [1];  [1];  [3];  [3];  [1]; ORCiD logo [4];  [1]; ORCiD logo [3]; ORCiD logo [5]
  1. Univ. of Montpellier, Marcoule (France)
  2. Univ. of California, Los Angeles, CA (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  3. Univ. of North Texas, Denton, TX (United States)
  4. Univ. of Paris-Saclay, Gif Sur Yvette (France)
  5. Univ. of California, Los Angeles, CA (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); Alternative Energies and Atomic Energy Commission (CEA), Cadarache (France)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1667367
Grant/Contract Number:  
SC0016584; 1562066
Resource Type:
Accepted Manuscript
Journal Name:
npj Materials Degradation
Additional Journal Information:
Journal Volume: 4; Journal Issue: 1; Journal ID: ISSN 2397-2106
Publisher:
Springer
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; atomistic models; reaction kinetics and dynamics

Citation Formats

Gin, Stéphane, Wang, Mengyi, Bisbrouck, Nicolas, Taron, Mélanie, Lu, Xiaonan, Deng, Lu, Angeli, Frédéric, Charpentier, Thibault, Delaye, Jean-Marc, Du, Jincheng, and Bauchy, Mathieu. Can a simple topological-constraints-based model predict the initial dissolution rate of borosilicate and aluminosilicate glasses?. United States: N. p., 2020. Web. https://doi.org/10.1038/s41529-020-0111-4.
Gin, Stéphane, Wang, Mengyi, Bisbrouck, Nicolas, Taron, Mélanie, Lu, Xiaonan, Deng, Lu, Angeli, Frédéric, Charpentier, Thibault, Delaye, Jean-Marc, Du, Jincheng, & Bauchy, Mathieu. Can a simple topological-constraints-based model predict the initial dissolution rate of borosilicate and aluminosilicate glasses?. United States. https://doi.org/10.1038/s41529-020-0111-4
Gin, Stéphane, Wang, Mengyi, Bisbrouck, Nicolas, Taron, Mélanie, Lu, Xiaonan, Deng, Lu, Angeli, Frédéric, Charpentier, Thibault, Delaye, Jean-Marc, Du, Jincheng, and Bauchy, Mathieu. Mon . "Can a simple topological-constraints-based model predict the initial dissolution rate of borosilicate and aluminosilicate glasses?". United States. https://doi.org/10.1038/s41529-020-0111-4. https://www.osti.gov/servlets/purl/1667367.
@article{osti_1667367,
title = {Can a simple topological-constraints-based model predict the initial dissolution rate of borosilicate and aluminosilicate glasses?},
author = {Gin, Stéphane and Wang, Mengyi and Bisbrouck, Nicolas and Taron, Mélanie and Lu, Xiaonan and Deng, Lu and Angeli, Frédéric and Charpentier, Thibault and Delaye, Jean-Marc and Du, Jincheng and Bauchy, Mathieu},
abstractNote = {Tuning glass composition to obtain targeted properties generally relies on empirical approaches. However, a deep understanding of the physical and chemical mechanisms linking glass composition to its structure and properties would enable developing reliable predictive models. Indeed, although empirical models are usually able to interpolate composition–property relationships within a given compositional envelope, they often fail at extrapolating predictions far from their training domain. Here, as an alternative route to empirical models, we show that a structural descriptor based on the number of topological constraints per atom can be used to predict the initial dissolution rate of aluminosilicate and borosilicate glasses after being parameterized on different families of glasses (specific series of borosilicate glasses). Sixteen glasses belonging to these families were studied and their initial dissolution rates were determined at 90 °C and pH90 °C = 9, covering rates spanning over 5 orders of magnitude. The model based on topological constraints was trained based on seven select borosilicate glasses (R2 = 0.997) and used to predict the dissolution rate of nine additional borosilicate and aluminosilicate glasses. We show that, provided that corrections are made for high alkali content glasses that dissolve incongruently (preferential release of Na), the model gives reasonable predictions, even far from its training domain.},
doi = {10.1038/s41529-020-0111-4},
journal = {npj Materials Degradation},
number = 1,
volume = 4,
place = {United States},
year = {2020},
month = {3}
}

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