Nonlinear dynamics and instability of aqueous dissolution of silicate glasses and minerals

Wang, Yifeng; Jove-Colon, Carlos F.; Kuhlman, Kristopher L.

doi:10.1038/srep30256

Nonlinear dynamics and instability of aqueous dissolution of silicate glasses and minerals

Journal Article · Fri Jul 22 00:00:00 EDT 2016 · Scientific Reports

DOI:https://doi.org/10.1038/srep30256· OSTI ID:1313074

Wang, Yifeng ^[1]; Jove-Colon, Carlos F. ^[1]; Kuhlman, Kristopher L. ^[1]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Aqueous dissolution of silicate glasses and minerals plays a critical role in global biogeochemical cycles and climate evolution. The reactivity of these materials is also important to numerous engineering applications including nuclear waste disposal. The dissolution process has long been considered to be controlled by a leached surface layer in which cations in the silicate framework are gradually leached out and replaced by protons from the solution. This view has recently been challenged by observations of extremely sharp corrosion fronts and oscillatory zonings in altered rims of the materials, suggesting that corrosion of these materials may proceed directly through congruent dissolution followed by secondary mineral precipitation. Here we show that complex silicate material dissolution behaviors can emerge from a simple positive feedback between dissolution-induced cation release and cation-enhanced dissolution kinetics. This self-accelerating mechanism enables a systematic prediction of the occurrence of sharp dissolution fronts (vs. leached surface layers), oscillatory dissolution behaviors and multiple stages of glass dissolution (in particular the alteration resumption at a late stage of a corrosion process). In conclusion, our work provides a new perspective for predicting long-term silicate weathering rates in actual geochemical systems and developing durable silicate materials for various engineering applications.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies (NE-5)

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1313074

Report Number(s):: SAND2016-4035J; 639042

Journal Information:: Scientific Reports, Journal Name: Scientific Reports Vol. 6; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Phosphatic alteration of lead-rich glazes during two centuries of burial: Bartlam, Bonnin & Morris, and Chelsea porcelain Owen, J. Victor; Hanley, Jacob J.; Petrus, Joeseph A. Archaeological and Anthropological Sciences, Vol. 11, Issue 12 https://doi.org/10.1007/s12520-019-00922-4	journal	August 2019
Morphological instability of aqueous dissolution of silicate glasses and minerals Wang, Yifeng; Jove-Colon, Carlos F.; Lenting, Christoph npj Materials Degradation, Vol. 2, Issue 1 https://doi.org/10.1038/s41529-018-0047-0	journal	September 2018
Corrosion of the International Simple Glass under acidic to hyperalkaline conditions Backhouse, Daniel J.; Fisher, Adam J.; Neeway, James J. npj Materials Degradation, Vol. 2, Issue 1 https://doi.org/10.1038/s41529-018-0050-5	journal	September 2018
Real-time in situ observations of reaction and transport phenomena during silicate glass corrosion by fluid-cell Raman spectroscopy Geisler, Thorsten; Dohmen, Lars; Lenting, Christoph Nature Materials, Vol. 18, Issue 4 https://doi.org/10.1038/s41563-019-0293-8	journal	February 2019
An insight into the corrosion of alkali aluminoborosilicate glasses in acidic environments Stone-Weiss, Nicholas; Youngman, Randall E.; Thorpe, Ryan Physical Chemistry Chemical Physics, Vol. 22, Issue 4 https://doi.org/10.1039/c9cp06064b	journal	January 2020
On Alteration Rate Renewal Stage of Nuclear Waste Glass Corrosion Ojovan, Michael I. MRS Advances, Vol. 5, Issue 3-4 https://doi.org/10.1557/adv.2020.36	journal	January 2020

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