Non-destructive characterization of corroded glass surfaces by spectroscopic ellipsometry

Kaspar, Tiffany C.; Reiser, Joelle T.; Ryan, Joseph V.; Wall, Nathalie A.

doi:10.1016/j.jnoncrysol.2017.10.054

Cited by 23 publications

(27 citation statements)

References 35 publications

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“…This will establish needed confidence to further mine the reconstructed gel structure for the tortuosity and interconnectedness that will inform models of transport behavior through these nanoscopic features. For now, we simply state that the general structure and porous volume are comparable and also consistent with expectations from the glass corrosion literature 32 .…”

Section: Cryo-fib Preparation and Apt Analysis Of Altered Glasssupporting

confidence: 84%

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

et al. 2020

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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.

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Section: Cryo-fib Preparation and Apt Analysis Of Altered Glasssupporting

confidence: 84%

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

et al. 2020

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“…2 and 3), which has not been taken into account in previous ICDP model. 12,14 Based on the new experimental results, we propose a unifying refined mechanistic glass corrosion model that in many aspects unifies all critical observations made on experimentally and naturally altered glass samples, such as an atomically sharp reaction interface, 13,14 interdiffusion profiles in the glass, 13,30 the formation of porosity, 7,12,30,36,37 as well as chemical and structural patterns in the SAL. 7,8,10,12 A schematic outline of the proposed mechanistic model is given in Fig.…”

Section: Discussionmentioning

confidence: 82%

Towards a unifying mechanistic model for silicate glass corrosion

et al. 2018

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Borosilicate glasses are currently used for the immobilization of highly radioactive waste and are materials of choice for many biomedical and research industries. They are metastable materials that corrode in aqueous solutions, reflected by the formation of silica-rich surface alteration layers (SAL). Until now, there is no consensus in the scientific community about the reaction and transport mechanism(s) and the rate-limiting steps involved in the formation of SALs. Here we report the results of multi-isotope tracer (2 H, 18 O, 10 B, 30 Si, 44 Ca) corrosion experiments that were performed with precorroded and pristine glass monoliths prepared from the six-component international simple glass and a quaternary aluminum borosilicate glass. Results of transmission electron microscopy and nanoscale analyses by secondary ion mass spectrometry reveal a nanometer-sharp interface between the SAL and the glass, where decoupling of isotope tracer occurs, while proton diffusion and ion exchange can be observed within the glass. We propose a unifying mechanistic model that accounts for all critical observations so far made on naturally and experimentally corroded glasses. It is based on an interface-coupled glass dissolution-silica precipitation reaction as the main SAL forming process. However, a diffusion-controlled ion exchange front may evolve in the glass ahead of the dissolution front if SAL formation at the reaction interface significantly slows down due to transport limitations.

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“…During glass corrosion at high S/V, mobile elements such as B, Na, and to a lesser extent Ca are dissolved into the solution, leaving behind a porous aluminosilicate gel layer 33 . The degree of corrosion is closely correlated to the thickness of the alteration layer 34 . Therefore, the corroded ISG samples were all sectioned to allow observation of the gel layer cross-sections in a scanning electron microscopy (SEM).…”

Section: Corrosion Of Isgmentioning

confidence: 99%

Near-field corrosion interactions between glass and corrosion resistant alloys

et al. 2020

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This study explores the corrosion interactions between model nuclear waste glass materials and corrosion resistant alloys, under accelerated conditions that simulate the near field of a nuclear waste repository. The interactions between the corrosion of stainless steel (SS) 316, alloy G30, or alloy 625, and international simple glass or soda-lime silica glass are systematically studied. The dissimilar materials were exposed in close proximity to each other in different electrolytes at 90°C. After exposure, the glass surface exposed near metals showed different regimes of corrosion, with distinct surface morphologies and chemistries that were likely affected by the local environment created by the localized corrosion of metals. Surface and solution analyses showed that the corrosion rate of glass was enhanced by the presence of metals. Infrared spectroscopy data suggested the local build-up of stresses in the contact area of glass, which may lead to the mechanical instability of the glass alteration layer. On the other hand, the effect of glass on metal corrosion is strongly dependent on the leaching solution. In electrolytes containing abundant aggressive anions such as Cl − , glass seems to suppress the localized corrosion of SS by the precipitation of a Si-rich surface film that protects the SS substrate from solutions. However, in less aggressive electrolytes, the corrosion rate of SS was increased by the presence of glass corrosion products. Overall, our study showed that the hidden and localized damage on glass in contact with metals may enhance the release rate of glass components compared to typical uniform glass corrosion.

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Non-destructive characterization of corroded glass surfaces by spectroscopic ellipsometry

Cited by 23 publications

References 35 publications

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

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

Towards a unifying mechanistic model for silicate glass corrosion

Near-field corrosion interactions between glass and corrosion resistant alloys

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