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

Gin, Stéphane; Wang, Mengyi; Bisbrouck, Nicolas; Taron, Mélanie; Lu, Xiaonan; Deng, Lu; Angeli, Frédéric; Charpentier, Thibault; Delaye, Jean-Marc; Du, Jincheng; Bauchy, Mathieu

doi:10.1038/s41529-020-0111-4

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

Journal Article · Mon Mar 16 00:00:00 EDT 2020 · npj Materials Degradation

DOI:https://doi.org/10.1038/s41529-020-0111-4· OSTI ID:1667367

^[1]; Wang, Mengyi ^[2]; Bisbrouck, Nicolas ^[3]; Taron, Mélanie ^[3]; Lu, Xiaonan ^[4]; Deng, Lu ^[4]; Angeli, Frédéric ^[3]; ^[5]; Delaye, Jean-Marc ^[3]; ^[4]; ^[6]

Univ. of Montpellier, Marcoule (France); CEA, France
Univ. of California, Los Angeles, CA (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Univ. of Montpellier, Marcoule (France)
Univ. of North Texas, Denton, TX (United States)
Univ. of Paris-Saclay, Gif Sur Yvette (France)
Univ. of California, Los Angeles, CA (United States)

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, even far from its training domain.

View Accepted Manuscript (DOE)

Research Organization:: 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 Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0016584

OSTI ID:: 1667367

Journal Information:: npj Materials Degradation, Journal Name: npj Materials Degradation Journal Issue: 1 Vol. 4; ISSN 2397-2106

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

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