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 pH^{90 °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:

Gin, Stéphane  ^[1];

• Search DOE PAGES for author "Gin, Stéphane"
• Search DOE PAGES for ORCID "0000-0002-1950-9195"

Wang, Mengyi ^[2]; Bisbrouck, Nicolas ^[1]; Taron, Mélanie ^[1]; Lu, Xiaonan ^[3]; Deng, Lu ^[3]; Angeli, Frédéric ^[1]; Charpentier, Thibault  ^[4];

• Search DOE PAGES for author "Charpentier, Thibault"
• Search DOE PAGES for ORCID "0000-0002-3034-1389"

Delaye, Jean-Marc ^[1]; Du, Jincheng  ^[3];

• Search DOE PAGES for author "Du, Jincheng"
• Search DOE PAGES for ORCID "0000-0003-4805-7498"

Bauchy, Mathieu  ^[5]

• Search DOE PAGES for author "Bauchy, Mathieu"
• Search DOE PAGES for ORCID "0000-0003-4600-0631"

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+ Show Author Affiliations

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:

Mon Mar 16 00:00:00 EDT 2020

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