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; Fritzsche, Moritz B. K.

doi:10.1038/s41563-019-0293-8

Cited by 81 publications

(114 citation statements)

References 49 publications

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“…There are two dominant theories: ion exchange followed by structural reorganization versus stoichiometric dissolution followed by in situ reprecipitation [154,155,156]. Both theories have ample experimental and theoretical support [1,154,155,156,157,158,159,160]. A major consequence of the different formation mechanisms is that the resulting alteration layers may have different properties and can be amorphous or crystalline, dense or porous [161], and passivating or not.…”

Section: Incongruent Dissolution and Surface Alteration Layer Of Multmentioning

confidence: 99%

Thermodynamic equilibrium and kinetic fundamentals of oxide dissolution in aqueous solution

Wang

2020

J. Mater. Res.

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Section: Incongruent Dissolution and Surface Alteration Layer Of Multmentioning

confidence: 99%

Thermodynamic equilibrium and kinetic fundamentals of oxide dissolution in aqueous solution

Wang

2020

J. Mater. Res.

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“…In a later stage, it is probable that the capillary condensation of water in the nanoporosity opened by network depolymerization and departure of alkali and alkaline-earth ions changes this situation, with the apparition of a true liquid phase and local pH conditions as put forward in ref. 27 for instance.…”

Section: Discussionmentioning

confidence: 99%

Evidence for different behaviors of atmospheric glass alteration as a function of glass composition

et al. 2020

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The glass composition is a determining parameter that influences the glass chemical durability, particularly in atmospheric conditions (defined by the relative humidity, RH, < 100%). This is obvious in the field of the cultural heritage (CH), where some glass compositions qualified as unstable show advanced signs of degradation under atmosphere, while others seem, on the contrary, stable. This study investigates the differences between stable and unstable glass compositions regarding the phenomenology of the atmospheric glass alteration, by means of accelerated ageing of three glass replicas followed by the characterization of their alteration layers at different scales. Over the same ageing period and experimental conditions, the two glass compositions qualified as unstable develop thick hydrated layers and a thin top layer of carbonate precipitates. Their hydrated layers are depolymerized, and they remarkably retain alkalis and non-bridging oxygens in a dense network of hydrogen bonds, as demonstrated by 29Si and 1H MAS NMR. On the contrary, the stable glass composition shows a considerably thinner hydrated layer and, relatively, a higher amount of carbonates on the surface. In unstable glasses, the retention of a significant proportion of alkalis and NBOs, probably by maintaining a basic character to the hydrated layer, seems comparatively a destabilizing factor sustaining hydration by fast network hydrolysis.

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“…According to the first model [1][2][3] , selective ion exchange of alkali with H + /H 3 O + (interdiffusion) and subsequent structural reorganisation of the hydrated glass leads to the formation of a silica-rich surface alteration layer (SAL) that tends to slow down the rate of glass corrosion. The second model [4][5][6] proposes that the SAL is formed as a result of simultaneous glass dissolution and silica precipitation from a thin layer of supersaturated water present at the glass-water interface. Evidence in favour of both of these models 3,[6][7][8][9] shows that they are non-universal in nature, and attempts of developing unifying models have been made 10 .…”

Section: Introductionmentioning

confidence: 99%

“…The second model [4][5][6] proposes that the SAL is formed as a result of simultaneous glass dissolution and silica precipitation from a thin layer of supersaturated water present at the glass-water interface. Evidence in favour of both of these models 3,[6][7][8][9] shows that they are non-universal in nature, and attempts of developing unifying models have been made 10 . Nevertheless, none of these models directly take into account the effect of glass composition 11 and leaching conditions on the microstructure of the leached glass and the impact of this microstructure on mass transport.…”

Section: Introductionmentioning

confidence: 99%

Effect of decades of corrosion on the microstructure of altered glasses and their radiation stability

et al. 2020

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Understanding the microstructural evolution of glasses during their interaction with water and radiation is of fundamental importance in addressing the corrosion of nuclear waste forms under geological disposal conditions. Here we report the results of more than 21 years of corrosion of two borosilicate glasses showing the formation of mesoporous C-S-H gels in Ca-bearing glasses and a mainly microporous microstructure in Al-bearing glasses. These porous corroded glasses were then irradiated with heavy ions to simulate the effects of recoil nucleus damage and monitored in real time using transmission electron microscopy with in situ ion irradiation. The ballistic collisions remarkably healed the porous corroded glasses to a pore-free homogeneous microstructure. Besides providing new insights and predictions about how doped glasses and actual waste forms may evolve under corrosion and irradiation, the results highlight the non-universal nature of the existing corrosion models and the important role that the glass composition and radiation damage play in the evolution of the microstructure during corrosion.npj Materials Degradation (2020) 4:11 ; https://doi.

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Real-time in situ observations of reaction and transport phenomena during silicate glass corrosion by fluid-cell Raman spectroscopy

Cited by 81 publications

References 49 publications

Thermodynamic equilibrium and kinetic fundamentals of oxide dissolution in aqueous solution

Thermodynamic equilibrium and kinetic fundamentals of oxide dissolution in aqueous solution

Evidence for different behaviors of atmospheric glass alteration as a function of glass composition

Effect of decades of corrosion on the microstructure of altered glasses and their radiation stability

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