Aqueous corrosion of borosilicate glass under acidic conditions: A new corrosion mechanism

Geisler, Thorsten; Janssen, André; Scheiter, Daniel; Stephan, T.; Berndt, Jasper; Putnis, Andrew

doi:10.1016/j.jnoncrysol.2010.04.033

Cited by 199 publications

(187 citation statements)

References 34 publications

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“…However, these spots do not display 18 O enrichment, highlighting that in these zones there is no hydrolysis/condensation reactions yet. Indeed, if local hydrolysis/condensation reactions or interfacial dissolution/precipitation have occurred, 18 O would be included in the newly formed siloxane bonds, as it is observed and proposed by Geisler et al 10 In this study, the preliminary step in the formation of the alteration layer (that occurred during the experiment only in unsaturated conditions) seems to be only interdiffusion.…”

Section: Resultssupporting

confidence: 62%

“…2,8,9 In the second case, an interfacial dissolutionprecipitation process is proposed to explain the gel formation, notably on nuclear glass. [10][11][12] More consensually, the secondary phases are formed by the precipitation of dissolved elements of the glass and/or elements of the environment. These mechanisms are similar in saturated (liquid water) and unsaturated media (water vapor), but their relative contribution is different.…”

Section: +mentioning

confidence: 99%

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Long-term weathering rate of stained-glass windows using H and O isotopes

et al. 2018

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The understanding of glass alteration is a biogeochemical, industrial, societal (radioactive waste confinement), and cultural heritage issue. Studies have been mainly performed in aqueous conditions. However, glass reactivity under hydraulically unsaturated conditions may be more important than previously recognized. In this context, we evaluate here the role of the alteration layer formed on medieval stained-glass windows on the ongoing alteration in unsaturated conditions. H 2 O adsorption isotherms were measured to study the relation between the vapor sorption and the relative humidity inside the alteration layer. From it, the average pore radius was calculated, yielding a water vapor diffusion coefficient of 7.8 × 10 -7 m² s -1 inside the pore network. Experiments using doped water vapor (D 2 18 O) confirm the vapor transport up to the alteration front via fractures and pore network. They also demonstrate that the alteration mainly progresses via an interdiffusion mechanism. The calculated interdiffusion coefficients at 20°C are 3.6 × 10 -20 m 2 s -1 at 70% RH and 4.9 × 10 -20 m 2 s -1 at 90% RH, which is similar to the values measured on model stained-glass samples altered in short durations (1-4 years). Therefore, this study highlights that, given its morphology, the alteration layer is not protective against vapor transport and interdiffusion.

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Section: Resultssupporting

confidence: 62%

Section: +mentioning

confidence: 99%

Long-term weathering rate of stained-glass windows using H and O isotopes

et al. 2018

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“…[2][3][4][5] Glass alteration mechanisms are still heavily debated inside the scientific community, as no consensus has been reached yet for the way the passivation layer forms on the glass surface. [6][7][8][9] To better understand glass alteration at high reaction progress, Gin, et al 10 and Collin, et al 11 performed studies in Si-saturated conditions and slightly alkaline pH conditions, and characterized the passivating material. In these specific conditions, B, Na, and to a lesser extent Ca are leached out.…”

Section: Introductionmentioning

confidence: 99%

Impact of alkali on the passivation of silicate glass

et al. 2018

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Amorphous silica-rich surface layers, also called gels, can passivate silicate glass and minerals depending on environmental conditions. However, several uncertainties remain on the mechanisms controlling the formation of these layers. In this paper, the influence of exogenous ions supplied by solutions is studied, both on the formation and on the properties of the gel formed on international simple glass (ISG). ISG was altered at 90°C, pH 90°C 7, in silica-saturated solutions containing various alkaline cations separately (Li + , Na + , K + , and Cs + ). The alteration kinetics observed with Li and Na in the solution is similar to that observed with no ions, while K and Cs in the solution tend to decrease glass alteration. Furthermore, for K or Cs ions, the kinetics decreases as the ionic strength of the solution increases. The passivation layer formed in these solutions shows a selectivity toward cations following the series K > Cs > Na >> Li. These alkalis replace Ca from pristine glass in the altered structures, leading to differences in [AlO 4 ] − units charge compensation. Importantly, exchange between Ca and alkali also affects the total quantity of water inside each gel and this effect is well correlated with the observed drop in glass alteration.

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“…1. 7 A more accurate picture of the regions has been obtained by advanced characterization techniques such as atom probe tomography on corroded glasses 8,9 so that the nature of the alteration layer and related interface morphology can be more clearly understood.…”

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confidence: 99%

Atomistic computer simulations of water interactions and dissolution of inorganic glasses

Rimsza

2017

npj Mater Degrad

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Computer simulations at the atomistic scale play an increasing important role in understanding the structure features, and the structure-property relationships of glass and amorphous materials. In this paper, we reviewed atomistic simulation methods ranging from first principles calculations and ab initio molecular dynamics (AIMD) simulations, to classical molecular dynamics (MD), and meso-scale kinetic Monte Carlo (KMC) simulations and their applications to study the reactions and interactions of inorganic glasses with water and the dissolution behaviors of inorganic glasses. Particularly, the use of these simulation methods in understanding the reaction mechanisms of water with oxide glasses, water-glass interfaces, hydrated porous silica gels formation, the structure and properties of multicomponent glasses, and microstructure evolution are reviewed. The advantages and disadvantageous of these simulation methods are discussed and the current challenges and future direction of atomistic simulations in glass dissolution presented.npj Materials Degradation (2017) 1:16 ; doi:10.1038/s41529-017-0017-yThe corrosion or degradation of glasses in aqueous solutions are critical in a number of engineering and technological processes ranging from microelectronic packaging, glass reaction chambers, and the immobilization of nuclear waste materials, as well as in healthcare and biomedical fields such as dissolution of inhaled glass fibers and bioactive glasses for biomedical applications. In particular, immobilizing radioactive waste in borosilicate glasses is widely accepted as a preferred method to treat nuclear waste materials generated from civilian and military sources. This process, also known as vitrification, is a critical component of the cycle of nuclear energy to combat global environmental and energy challenges. Researchers from around the world have extensively invested in understanding glass corrosion in an effort to predict the long-term stability and release rate radionuclides to the environment during nuclear waste storage. 1,2Various mechanisms for glass corrosion have been proposed and despite intensive experimental investigations with advanced characterization techniques results are unclear. It is generally accepted that the corrosion of glass consists of a set of complex processes including hydration, hydrolysis, and ion-exchange that are coupled during glass dissolution. The initial stage is interdiffusion of proton or hydronium ions from the solution with sodium or other alkali ions in the glass.3 This is followed by the hydrophilic attack of water on the Si-O-Si or Si-O-Al linkages that lead to hydroxylation of the silicate glass network. The remaining hydrolyzed glass skeleton then undergoes condensation and repolymerization to form the hydrated nanoporous silica rich gel layer which can be protective, decreasing dissolution to a residual rate. [4][5][6] The morphology of the gel layer, such as thickness, pore structure, and chemical composition, depends on the original glass composition and the pH...

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Aqueous corrosion of borosilicate glass under acidic conditions: A new corrosion mechanism

Cited by 199 publications

References 34 publications

Long-term weathering rate of stained-glass windows using H and O isotopes

Long-term weathering rate of stained-glass windows using H and O isotopes

Impact of alkali on the passivation of silicate glass

Atomistic computer simulations of water interactions and dissolution of inorganic glasses

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