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Title: Dynamics of self-reorganization explains passivation of silicate glasses

Understanding the dissolution of silicate glasses and minerals from atomic to macroscopic levels is a challenge with major implications in geoscience and industry. One of the main uncertainties limiting the development of predictive models lies in the formation of an amorphous surface layer––called gel––that can in some circumstances control the reactivity of the buried interface. Here, we report experimental and simulation results deciphering the mechanisms by which the gel becomes passivating. The study conducted on a six-oxide borosilicate glass shows that gel reorganization involving high exchange rate of oxygen and low exchange rate of silicon is the key mechanism accounting for extremely low apparent water diffusivity (~10 –21 m 2 s –1), which could be rate-limiting for the overall reaction. Furthermore, these findings could be used to improve kinetic models, and inspire the development of new molecular sieve materials with tailored properties as well as highly durable glass for application in extreme environments.
Authors:
 [1] ;  [1] ;  [1] ; ORCiD logo [1] ;  [1] ;  [2] ;  [3] ;  [4] ; ORCiD logo [3]
  1. CEA, DEN, DE2D, SEVT, Bagnols sur Ceze (France)
  2. Tescan Analytics, Fuveau (France)
  3. Univ. of North Texas, Denton, TX (United States)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Report Number(s):
PNNL-SA-133283
Journal ID: ISSN 2041-1723; PII: 4511
Grant/Contract Number:
AC05-76RL01830
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1457771

Gin, Stephane, Collin, Marie, Jollivet, Patrick, Fournier, Maxime, Minet, Yves, Dupuy, Laurent, Mahadevan, Thiruvilla, Kerisit, Sebastien, and Du, Jincheng. Dynamics of self-reorganization explains passivation of silicate glasses. United States: N. p., Web. doi:10.1038/s41467-018-04511-2.
Gin, Stephane, Collin, Marie, Jollivet, Patrick, Fournier, Maxime, Minet, Yves, Dupuy, Laurent, Mahadevan, Thiruvilla, Kerisit, Sebastien, & Du, Jincheng. Dynamics of self-reorganization explains passivation of silicate glasses. United States. doi:10.1038/s41467-018-04511-2.
Gin, Stephane, Collin, Marie, Jollivet, Patrick, Fournier, Maxime, Minet, Yves, Dupuy, Laurent, Mahadevan, Thiruvilla, Kerisit, Sebastien, and Du, Jincheng. 2018. "Dynamics of self-reorganization explains passivation of silicate glasses". United States. doi:10.1038/s41467-018-04511-2. https://www.osti.gov/servlets/purl/1457771.
@article{osti_1457771,
title = {Dynamics of self-reorganization explains passivation of silicate glasses},
author = {Gin, Stephane and Collin, Marie and Jollivet, Patrick and Fournier, Maxime and Minet, Yves and Dupuy, Laurent and Mahadevan, Thiruvilla and Kerisit, Sebastien and Du, Jincheng},
abstractNote = {Understanding the dissolution of silicate glasses and minerals from atomic to macroscopic levels is a challenge with major implications in geoscience and industry. One of the main uncertainties limiting the development of predictive models lies in the formation of an amorphous surface layer––called gel––that can in some circumstances control the reactivity of the buried interface. Here, we report experimental and simulation results deciphering the mechanisms by which the gel becomes passivating. The study conducted on a six-oxide borosilicate glass shows that gel reorganization involving high exchange rate of oxygen and low exchange rate of silicon is the key mechanism accounting for extremely low apparent water diffusivity (~10–21 m2 s–1), which could be rate-limiting for the overall reaction. Furthermore, these findings could be used to improve kinetic models, and inspire the development of new molecular sieve materials with tailored properties as well as highly durable glass for application in extreme environments.},
doi = {10.1038/s41467-018-04511-2},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {6}
}