Impact of aqueous solution pH on network structure of corrosion–induced surface layers of boroaluminosilicate glass

Kaya, Huseyin; Gin, Stephane; Vogt, Bryan D.; Kim, Seong H.

doi:10.1111/jace.18606

Impact of aqueous solution pH on network structure of corrosion–induced surface layers of boroaluminosilicate glass

Journal Article · Sun Jun 19 00:00:00 EDT 2022 · Journal of the American Ceramic Society

DOI:https://doi.org/10.1111/jace.18606· OSTI ID:1879852

Kaya, Huseyin ^[1]; ^[2]; Vogt, Bryan D. ^[3]; ^[3]

Pennsylvania State Univ., University Park, PA (United States); Pennsylvania State University
Univ. of Montpellier, Bagnols sur Cèze (France)
Pennsylvania State Univ., University Park, PA (United States)

Understanding of the long-term stability of vitrified nuclear waste glass is critical to its safe storage, but knowledge gaps remain regarding the corrosion mechanism, especially with respect to surface alteration layers whose presence changes the observed corrosion rates. Here, we report the aqueous corrosion of a model boroaluminosilicate glass at ground water relevant pHs as investigated by vibrational spectroscopy to understand the network structure of the alteration layer that we hypothesize controls the corrosion rates. Both specular reflection infrared spectroscopy and infrared variable angle spectroscopic ellipsometry were used to elucidate details of the structure of the alteration layers formed at pH 7 and pH 9. After 2312 days, the thickness of the alteration layer is found to be ~2000 nm for corrosion at pH 7 and ~300 nm for corrosion at pH 9. Here, the interpretation of the vibrational spectra suggests that alteration layers formed at pH 7 and pH 9 both exhibit a porous network with "silica-like" structures, but with differences in the bond lengths and bond angles in the glass network. Moreover, the relative abundance of the hydrous species within the porous network appears to be dependent on pH. Additionally, the spectroscopic data suggest that the B and Ca trapped in the alteration layer during the secondary corrosion of the pH 9 pre-corroded sample in pH 3 solution are hydrated within the nano-porous layer and not bound to the silicate network. However, the precise chemical form remains to be determined. Based on these findings, we propose that the combination of the network structure of the alteration layer and the relative abundance of hydrous species within the alteration layer act to control the transport of ionic species dissolved from the reaction front to the aqueous solution outside the glass.

View Accepted Manuscript (DOE)

Research Organization:: Pennsylvania State Univ., University Park, PA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0016584

OSTI ID:: 1879852

Journal Information:: Journal of the American Ceramic Society, Journal Name: Journal of the American Ceramic Society Journal Issue: 11 Vol. 105; ISSN 0002-7820

Publisher:: American Ceramic SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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