A general mechanism for gel layer formation on borosilicate glass under aqueous corrosion

Gin, Stephane; Mir, Anamul Haq; Jan, Amreen; Delaye, Jean-Marc; Chauvet, Elodie; de Puydt, Yves; Gourgiotis, Alkiviadis; Kerisit, Sebastien N.

doi:10.1021/acs.jpcc.9b10491

A general mechanism for gel layer formation on borosilicate glass under aqueous corrosion

Journal Article · Thu Mar 05 04:00:00 EST 2020 · Journal of Physical Chemistry C

DOI:https://doi.org/10.1021/acs.jpcc.9b10491· OSTI ID:1605359

Gin, Stephane ^[1]; Mir, Anamul Haq ^[2]; Jan, Amreen ^[3]; Delaye, Jean-Marc ^[4]; Chauvet, Elodie ^[5]; de Puydt, Yves ^[5]; Gourgiotis, Alkiviadis ^[6]; Kerisit, Sebastien N. ^[7]

CEA Marcoule
University of Huddersfield
UNIVERSITY PROGRAMS
CEA
Tescan Analytics
Institut de Radioprotection et de Sûreté Nucléaire
BATTELLE (PACIFIC NW LAB)

Mineral and glass dissolution is a scientific topic deeply investigated but incompletely understood and of a great interest for the geochemical and materials science communities. If the interfacial dissolution/reprecipitation mechanism seems to be applicable to most of silicate minerals, the debate remains open concerning glass. Here we studied two model glasses, a ternary borosilicate (CJ1) and the same glass doped with 4.1 mol% of Al2O3 (CJ2). The two glasses were altered at 90°C, pH 9, and in conditions far and close to saturation with respect to amorphous silica, to determine the initial and residual rates. Moreover, a specific experiment was conducted for a short duration with a solution highly enriched with 18O and 29Si isotopes to understand how passivating gels form. SEM, TEM and ToF-SIMS characterization, along with Monte Carlo simulations were used to understand the rate limiting reactions at play and infer the role of Al. We show that Al yields a slower matrix dissolution in dilute conditions. However, it slows down he formation and the maturation of the passivating gel and favors alteration by partial hydrolysis of Si and Al entities followed by in-situ reorganization/relaxation into a porous network. Unexpectedly, CJ1 experienced both interfacial dissolution/reprecipitation and partial hydrolysis followed by in situ reorganization of the silicate network during the course of a single experiment. This study offers a unified concept that can pave the way for the future development of a predictive kinetic model based on a detailed description of bond breaking and bond forming as a function of glass composition and alteration conditions.

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Performance and Design of Nuclear Waste Forms and Containers (WastePD); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1605359

Report Number(s):: PNNL-SA-149447

Journal Information:: Journal of Physical Chemistry C, Journal Name: Journal of Physical Chemistry C Journal Issue: 9 Vol. 124

Country of Publication:: United States

Language:: English

References (47)

The mechanism of borosilicate glass corrosion revisited Geisler, Thorsten; Nagel, Thorsten; Kilburn, Matt R. Geochimica et Cosmochimica Acta, Vol. 158 https://doi.org/10.1016/j.gca.2015.02.039	journal	June 2015
Dissolution of nepheline, jadeite and albite glasses: toward better models for aluminosilicate dissolution Hamilton, James P.; Brantley, Susan L.; Pantano, Carlo G. Geochimica et Cosmochimica Acta, Vol. 65, Issue 21 https://doi.org/10.1016/S0016-7037(01)00724-4	journal	November 2001
A comparative review of the aqueous corrosion of glasses, crystalline ceramics, and metals Frankel, Gerald S.; Vienna, John D.; Lian, Jie npj Materials Degradation, Vol. 2, Issue 1 https://doi.org/10.1038/s41529-018-0037-2	journal	May 2018
Contribution of Monte Carlo Modeling to Understanding the Alteration of Nuclear Glasses by Water Ledieu, Aurélien; Devreux, François; Barboux, Philippe Nuclear Science and Engineering, Vol. 153, Issue 3 https://doi.org/10.13182/NSE06-A2614	journal	July 2006
The structure of Na2O–Al2O3–SiO2 glass: impact on sodium ion exchange in H2O and D2O McGrail, B. P.; Icenhower, J. P.; Shuh, D. K. Journal of Non-Crystalline Solids, Vol. 296, Issue 1-2 https://doi.org/10.1016/S0022-3093(01)00890-0	journal	December 2001
Dissolution of silica component of glass network at early stage of corrosion in initially silica‐saturated solution Ngo, Dien; Liu, Hongshen; Kaya, Huseyin Journal of the American Ceramic Society, Vol. 102, Issue 11 https://doi.org/10.1111/jace.16550	journal	May 2019
Origin and consequences of silicate glass passivation by surface layers Gin, Stéphane; Jollivet, Patrick; Fournier, Maxime Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms7360	journal	February 2015
New Insight into the Residual Rate of Borosilicate Glasses: Effect of S/V and Glass Composition Gin, Stéphane; Frugier, Pierre; Jollivet, Patrick International Journal of Applied Glass Science, Vol. 4, Issue 4 https://doi.org/10.1111/ijag.12048	journal	October 2013
A simplified model for glass dissolution in water Devreux, F.; Barboux, Ph.; Filoche, M. Journal of Materials Science, Vol. 36, Issue 6, p. 1331-1341 https://doi.org/10.1023/A:1017591100985	journal	January 2001
Insight into silicate-glass corrosion mechanisms Cailleteau, Céline; Angeli, Frédéric; Devreux, François Nature Materials, Vol. 7, Issue 12 https://doi.org/10.1038/nmat2301	journal	October 2008
Monte Carlo simulations of borosilicate glass corrosion: predictions for morphology and kinetics Ledieu, A.; Devreux, F.; Barboux, P. Journal of Non-Crystalline Solids, Vol. 345-346 https://doi.org/10.1016/j.jnoncrysol.2004.08.152	journal	October 2004
Leaching of borosilicate glasses. I. Experiments Ledieu, A.; Devreux, F.; Barboux, P. Journal of Non-Crystalline Solids, Vol. 343, Issue 1-3 https://doi.org/10.1016/j.jnoncrysol.2004.06.006	journal	September 2004
Dynamics of self-reorganization explains passivation of silicate glasses Gin, Stéphane; Collin, Marie; Jollivet, Patrick Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-04511-2	journal	June 2018
Leaching of borosilicate glasses. II. Model and Monte-Carlo simulations Devreux, F.; Ledieu, A.; Barboux, P. Journal of Non-Crystalline Solids, Vol. 343, Issue 1-3 https://doi.org/10.1016/j.jnoncrysol.2004.06.007	journal	September 2004
How hexagonal mesoporous silica evolves in water on short and long term: Role of pore size and silica wall porosity Gouze, B.; Cambedouzou, J.; Parrès-Maynadié, S. Microporous and Mesoporous Materials, Vol. 183 https://doi.org/10.1016/j.micromeso.2013.08.041	journal	January 2014
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
Morphological evolution of alteration layers formed during nuclear glass alteration: new evidence of a gel as a diffusive barrier Rebiscoul, Diane; Van der Lee, Arie; Rieutord, Francois Journal of Nuclear Materials, Vol. 326, Issue 1 https://doi.org/10.1016/j.jnucmat.2003.10.015	journal	March 2004
Current Understanding and Remaining Challenges in Modeling Long-Term Degradation of Borosilicate Nuclear Waste Glasses Vienna, John D.; Ryan, Joseph V.; Gin, Stéphane International Journal of Applied Glass Science, Vol. 4, Issue 4 https://doi.org/10.1111/ijag.12050	journal	November 2013
Monte Carlo simulations of the corrosion of aluminoborosilicate glasses Kerisit, Sebastien; Ryan, Joseph V.; Pierce, Eric M. Journal of Non-Crystalline Solids, Vol. 378 https://doi.org/10.1016/j.jnoncrysol.2013.07.014	journal	October 2013
Monte Carlo simulations of the dissolution of borosilicate glasses in near-equilibrium conditions Kerisit, Sebastien; Pierce, Eric M. Journal of Non-Crystalline Solids, Vol. 358, Issue 10 https://doi.org/10.1016/j.jnoncrysol.2012.03.003	journal	May 2012
Effect of composition on the short-term and long-term dissolution rates of ten borosilicate glasses of increasing complexity from 3 to 30 oxides Gin, Stéphane; Beaudoux, Xavier; Angéli, Frédéric Journal of Non-Crystalline Solids, Vol. 358, Issue 18-19 https://doi.org/10.1016/j.jnoncrysol.2012.05.024	journal	September 2012
An international initiative on long-term behavior of high-level nuclear waste glass Gin, S.; Abdelouas, A.; Criscenti, L. J. Materials Today, Vol. 16, Issue 6 https://doi.org/10.1016/j.mattod.2013.06.008	journal	June 2013
Effect of pH on the stability of passivating gel layers formed on International Simple Glass Fournier, Maxime; Ducasse, Thomas; Pérez, Anne Journal of Nuclear Materials, Vol. 524 https://doi.org/10.1016/j.jnucmat.2019.06.029	journal	October 2019
Present understanding of R7T7 glass alteration kinetics and their impact on long-term behavior modeling Vernaz, E.; Gin, S.; Jégou, C. Journal of Nuclear Materials, Vol. 298, Issue 1-2 https://doi.org/10.1016/S0022-3115(01)00643-2	journal	September 2001
The fate of silicon during glass corrosion under alkaline conditions: A mechanistic and kinetic study with the International Simple Glass Gin, Stéphane; Jollivet, Patrick; Fournier, Maxime Geochimica et Cosmochimica Acta, Vol. 151 https://doi.org/10.1016/j.gca.2014.12.009	journal	February 2015
Spectroscopic ellipsometry study of thickness and porosity of the alteration layer formed on international simple glass surface in aqueous corrosion conditions Ngo, Dien; Liu, Hongshen; Sheth, Nisha npj Materials Degradation, Vol. 2, Issue 1 https://doi.org/10.1038/s41529-018-0040-7	journal	July 2018
Atom-Probe Tomography, TEM and ToF-SIMS study of borosilicate glass alteration rim: A multiscale approach to investigating rate-limiting mechanisms Gin, S.; Jollivet, P.; Barba Rossa, G. Geochimica et Cosmochimica Acta, Vol. 202 https://doi.org/10.1016/j.gca.2016.12.029	journal	April 2017
Modeling Interfacial Glass-Water Reactions: Recent Advances and Current Limitations Pierce, Eric M.; Frugier, Pierre; Criscenti, Louise J. International Journal of Applied Glass Science, Vol. 5, Issue 4 https://doi.org/10.1111/ijag.12077	journal	July 2014
The effect of composition on the leaching of three nuclear waste glasses: R7T7, AVM and VRZ Frugier, Pierre; Martin, Christelle; Ribet, Isabelle Journal of Nuclear Materials, Vol. 346, Issue 2-3 https://doi.org/10.1016/j.jnucmat.2005.06.023	journal	November 2005
Nanometre-scale evidence for interfacial dissolution–reprecipitation control of silicate glass corrosion Hellmann, Roland; Cotte, Stéphane; Cadel, Emmanuel Nature Materials, Vol. 14, Issue 3 https://doi.org/10.1038/nmat4172	journal	January 2015
Glass dissolution rate measurement and calculation revisited Fournier, Maxime; Ull, Aurélien; Nicoleau, Elodie Journal of Nuclear Materials, Vol. 476 https://doi.org/10.1016/j.jnucmat.2016.04.028	journal	August 2016
Experimentally determined dissolution kinetics of SON68 glass at 90°C over a silica saturation interval: Evidence against a linear rate law Icenhower, Jonathan P.; Steefel, Carl I. Journal of Nuclear Materials, Vol. 439, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2013.04.008	journal	August 2013
Alteration kinetics of a simplified nuclear glass in an aqueous medium: effects of solution chemistry and of protective gel properties on diminishing the alteration rate Jégou, C.; Gin, S.; Larché, F. Journal of Nuclear Materials, Vol. 280, Issue 2 https://doi.org/10.1016/S0022-3115(00)00039-8	journal	July 2000
Why Do Certain Glasses with a High Dissolution Rate Undergo a Low Degree of Corrosion? Cailleteau, Céline; Devreux, François; Spalla, Olivier The Journal of Physical Chemistry C, Vol. 115, Issue 13 https://doi.org/10.1021/jp111458f	journal	March 2011
Monte Carlo simulations of the dissolution of borosilicate and aluminoborosilicate glasses in dilute aqueous solutions Kerisit, Sebastien; Pierce, Eric M. Geochimica et Cosmochimica Acta, Vol. 75, Issue 18 https://doi.org/10.1016/j.gca.2011.06.036	journal	September 2011
Fiji: an open-source platform for biological-image analysis Schindelin, Johannes; Arganda-Carreras, Ignacio; Frise, Erwin Nature Methods, Vol. 9, Issue 7 https://doi.org/10.1038/nmeth.2019	journal	June 2012
Monte Carlo simulations of coupled diffusion and surface reactions during the aqueous corrosion of borosilicate glasses Kerisit, Sebastien; Pierce, Eric M.; Ryan, Joseph V. Journal of Non-Crystalline Solids, Vol. 408 https://doi.org/10.1016/j.jnoncrysol.2014.07.020	journal	January 2015
First-order dissolution rate law and the role of surface layers in glass performance assessment Grambow, B.; Müller, R. Journal of Nuclear Materials, Vol. 298, Issue 1-2 https://doi.org/10.1016/S0022-3115(01)00619-5	journal	September 2001
ToF-SIMS depth profiling of altered glass Collin, Marie; Gin, Stéphane; Jollivet, Patrick npj Materials Degradation, Vol. 3, Issue 1 https://doi.org/10.1038/s41529-019-0076-3	journal	April 2019
Modeling glass corrosion with GRAAL Frugier, Pierre; Minet, Yves; Rajmohan, Natarajan npj Materials Degradation, Vol. 2, Issue 1 https://doi.org/10.1038/s41529-018-0056-z	journal	November 2018
SON68 nuclear glass dissolution kinetics: Current state of knowledge and basis of the new GRAAL model Frugier, P.; Gin, S.; Minet, Y. Journal of Nuclear Materials, Vol. 380, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2008.06.044	journal	October 2008
Molecular mechanisms for corrosion of silica and silicate glasses Bunker, B. C. Journal of Non-Crystalline Solids, Vol. 179 https://doi.org/10.1016/0022-3093(94)90708-0	journal	November 1994
Mineralogical evolution of Fe–Si-rich layers at the olivine-water interface during carbonation reactions Saldi, Giuseppe D.; Daval, Damien; Guo, Hua American Mineralogist, Vol. 100, Issue 11-12 https://doi.org/10.2138/am-2015-5340	journal	November 2015
Thermochemistry of nuclear waste glasses: application to weathering studies Linard, Yannick; Advocat, Thierry; Jégou, Christophe Journal of Non-Crystalline Solids, Vol. 289, Issue 1-3 https://doi.org/10.1016/S0022-3093(01)00714-1	journal	August 2001
Boron Speciation in Soda-Lime Borosilicate Glasses Containing Zirconium: Boron Speciation in Soda-Lime Borosilicate Glasses Angeli, Frédéric; Charpentier, Thibault; De Ligny, Dominique Journal of the American Ceramic Society, Vol. 93, Issue 9 https://doi.org/10.1111/j.1551-2916.2010.03771.x	journal	April 2010
Silicon isotope ratio measurements by inductively coupled plasma tandem mass spectrometry for alteration studies of nuclear waste glasses Gourgiotis, Alkiviadis; Ducasse, Thomas; Barker, Evelyne Analytica Chimica Acta, Vol. 954 https://doi.org/10.1016/j.aca.2016.11.063	journal	February 2017
Nuclear Waste Glasses - How Durable? Grambow, B. Elements, Vol. 2, Issue 6 https://doi.org/10.2113/gselements.2.6.357	journal	December 2006

Similar Records

A General Mechanism for Gel Layer Formation on Borosilicate Glass under Aqueous Corrosion

Journal Article · Thu Feb 06 23:00:00 EST 2020 · Journal of Physical Chemistry. C · OSTI ID:1600946

On the effect of Al on alumino-borosilicate glass chemical durability

Journal Article · Tue May 30 00:00:00 EDT 2023 · npj Materials Degradation · OSTI ID:2420564

A general mechanism for gel layer formation on borosilicate glass under aqueous corrosion

Citation Formats

References (47)

Similar Records

Related Subjects