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Title: Tomographic mapping of the nanoscale water-filled pore structure in corroded borosilicate glass

Abstract

Cryo-based atom probe tomography has been applied to directly reveal the water-solid interface and hydrated corrosion layers making up the nanoscale porous structure of a corroded borosilicate glass in its native aqueous environment. The analysis includes morphology and compositional mapping of the inner gel/glass interface, isolation of a tomographic sub-volume of the tortuous water-filled gel, and comparison of the gel structure with simulations. The nanoscale porous structure is qualitatively consistent with that of the molecular dynamics simulation, enabling in greater confidence in both interrogations. Comparison of the gel/glass interface between desiccated and cryogenically preserved samples reveals consistently abrupt B dissolution behavior and quantitative differences in the apparent H ingress into the glass. These comparisons give some guidance to future experimental approaches to understanding glass corrosion behavior. More broadly, the cryogenic preservation and 3D visualization of the native water/solid structure in 3D at the nanoscale has direct relevance to a wide range of materials systems beyond glass science.

Authors:
ORCiD logo; ORCiD logo; ; ; ; ; ORCiD logo;
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Performance and Design of Nuclear Waste Forms and Containers (WastePD); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1619776
Alternate Identifier(s):
OSTI ID: 1650564; OSTI ID: 1667369
Report Number(s):
PNNL-SA-155600
Journal ID: ISSN 2397-2106; 8; PII: 110
Grant/Contract Number:  
AC05-76RL01830; SC0016584
Resource Type:
Published Article
Journal Name:
npj Materials Degradation
Additional Journal Information:
Journal Name: npj Materials Degradation Journal Volume: 4 Journal Issue: 1; Journal ID: ISSN 2397-2106
Publisher:
Springer
Country of Publication:
United Kingdom
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Perea, Daniel E., Schreiber, Daniel K., Ryan, Joseph V., Wirth, Mark G., Deng, Lu, Lu, Xiaonan, Du, Jincheng, and Vienna, John D.. Tomographic mapping of the nanoscale water-filled pore structure in corroded borosilicate glass. United Kingdom: N. p., 2020. Web. https://doi.org/10.1038/s41529-020-0110-5.
Perea, Daniel E., Schreiber, Daniel K., Ryan, Joseph V., Wirth, Mark G., Deng, Lu, Lu, Xiaonan, Du, Jincheng, & Vienna, John D.. Tomographic mapping of the nanoscale water-filled pore structure in corroded borosilicate glass. United Kingdom. https://doi.org/10.1038/s41529-020-0110-5
Perea, Daniel E., Schreiber, Daniel K., Ryan, Joseph V., Wirth, Mark G., Deng, Lu, Lu, Xiaonan, Du, Jincheng, and Vienna, John D.. Wed . "Tomographic mapping of the nanoscale water-filled pore structure in corroded borosilicate glass". United Kingdom. https://doi.org/10.1038/s41529-020-0110-5.
@article{osti_1619776,
title = {Tomographic mapping of the nanoscale water-filled pore structure in corroded borosilicate glass},
author = {Perea, Daniel E. and Schreiber, Daniel K. and Ryan, Joseph V. and Wirth, Mark G. and Deng, Lu and Lu, Xiaonan and Du, Jincheng and Vienna, John D.},
abstractNote = {Cryo-based atom probe tomography has been applied to directly reveal the water-solid interface and hydrated corrosion layers making up the nanoscale porous structure of a corroded borosilicate glass in its native aqueous environment. The analysis includes morphology and compositional mapping of the inner gel/glass interface, isolation of a tomographic sub-volume of the tortuous water-filled gel, and comparison of the gel structure with simulations. The nanoscale porous structure is qualitatively consistent with that of the molecular dynamics simulation, enabling in greater confidence in both interrogations. Comparison of the gel/glass interface between desiccated and cryogenically preserved samples reveals consistently abrupt B dissolution behavior and quantitative differences in the apparent H ingress into the glass. These comparisons give some guidance to future experimental approaches to understanding glass corrosion behavior. More broadly, the cryogenic preservation and 3D visualization of the native water/solid structure in 3D at the nanoscale has direct relevance to a wide range of materials systems beyond glass science.},
doi = {10.1038/s41529-020-0110-5},
journal = {npj Materials Degradation},
number = 1,
volume = 4,
place = {United Kingdom},
year = {2020},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41529-020-0110-5

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