Glass dissolution rate measurement and calculation revisited

Fournier, Maxime; Ull, Aurélien; Nicoleau, Elodie; Inagaki, Yoshiyuki; Odorico, Michaël; Frugier, Pierre; Gin, Stéṕhane

doi:10.1016/j.jnucmat.2016.04.028

Cited by 77 publications

(68 citation statements)

References 55 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…1a, good agreement was found between the data collected in this study and that of Neeway et al 16 and the combined data sets were used to obtain the rate parameters in Table 1. Figure 1c shows that the silicon foward rates (R Si ), obtained at different pH and T are smaller by factors varying between 2 and 7 than those obtained by Inagaki et al 21 using the micro-channel-flow through (MCFT) methodology (depending on specific pH and temperature, Supplementary 21 contained KCl and HCl and that utilised by Fournier et al 22 contained KOH; it is possible that K participated in ion-exchange reactions with alkali elements (i.e., Na) in the glass, enhancing the dissolution rate. 23 Alternatively alkali and alkaline earth salts have also been shown to increase the dissolution rate of both amorphous silica 24 and crystalline quartz.…”

Section: Discussionmentioning

confidence: 84%

Corrosion of the International Simple Glass under acidic to hyperalkaline conditions

et al. 2018

View full text Add to dashboard Cite

Assessment of glass dissolution kinetics, under disposal relevant temperature and pH environments, is required to credibly estimate radionuclide release rates from vitrified radioactive waste. Leaching of the International Simple Glass (ISG) under acidic to hyperalkaline conditions was examined. Forward rate measurements have been obtained using the dynamic leaching SPFT protocol and rate parameters for B, Na and Si in the basic regime; errors in rates predicted using these parameters at high pH and temperature are significant because the fitting uses logarithmic data. Longer term behaviour under hyperalkaline conditions, representative of some disposal environments, was investigated using the PCT and MCC-1 static leaching protocols with Ca(OH)2 solutions for up to 120 days (PCT) and 720 days (MCC-1). In hyperalkaline conditions dissolution was incongruent for all elements and the presence of alternating zirconia-rich and zirconia-poor alteration layers was observed on all leached monoliths, indicating the occurrence of a self-organisation phenomenon during leaching.

show abstract

Section: Discussionmentioning

confidence: 84%

Corrosion of the International Simple Glass under acidic to hyperalkaline conditions

et al. 2018

View full text Add to dashboard Cite

show abstract

“…Tests were conducted in dilute conditions, i.e., far from equilibrium, to avoid any effect of dissolved gel species on the Gibbs free energy of reaction (supplementary material Table S6 d). Despite the fact that r 0 does not appear to be very sensitive to variation of the gels composition and structure, and that the uncertainty is approximately 25%, 36 a lower r 0 is measured for the Cs-rich gel than for the other gels. This indicates that Cs improves both the passivation properties and the resistance of the gel towards hydrolysis.…”

Section: Discussionmentioning

confidence: 88%

“…The Si concentration was monitored over time by spectrophotometry and ICP-AES. For more extensive details on the procedure, please refer to Fournier, et al 36 …”

Section: Leaching Experimentsmentioning

confidence: 99%

Impact of alkali on the passivation of silicate glass

et al. 2018

Self Cite

View full text Add to dashboard Cite

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.

show abstract

“…The uncertainty in r 0 was estimated to be about 10%, taking into account errors in the measured surface area of the glass, in the silicon concentration, and the repeatability of the measurements. 20 The residual rates (r r ) were calculated from the normalized boron and sodium mass losses between 72 and 224 days. The associated uncertainty was also 10%.…”

Section: Glass Alteration Experimentsmentioning

confidence: 99%

“…The residual alteration rate, reflecting its long-term behavior, was obtained in initially silicon-saturated media (avoiding hydrolysis mechanisms 19 ). Fibers ensured that the samples used in the dissolution experiments all had the same surface state, thus limiting surface-related uncertainties 20 in the measured rates.…”

Section: Introductionmentioning

confidence: 99%

Effect of thermally induced structural disorder on the chemical durability of International Simple Glass

et al. 2018

Self Cite

View full text Add to dashboard Cite

While the influence of silicate oxide glass composition on its chemical durability is increasingly known, the contribution of structure only is less well understood, yet is crucial for an accurate description of aqueous alteration mechanisms. The effect of structural disorder can be investigated by varying the thermal history of the glass. Furthermore, the structural changes generated by selfirradiation in nuclear glasses can be compared with those induced by fast quenching. In the context of deep geological disposal of vitreous matrices, it is then challenging to address the structural impact on glass durability. Here, a borosilicate glass, the International Simple Glass, was fiberized to obtain a rapidly quenched sample. The quenching rate and fictive temperature were evaluated from in situ Raman and Brillouin spectroscopies. Multinuclear nuclear magnetic resonance was used to obtain insight into the effect of quenching on the pristine and altered glass structure. Higher bond angle distribution and lower mixing of alkalis were observed in the fast quenched glass. Some of AlO 4 groups are then Ca-compensated, while a part of BO 4 is transformed into BO 3 units. The structural modifications increase the hydrolysis of the silicate network occurring in the forward rate regime at 90°C by a factor of 1.4-1.8 depending on the pH value. Residual rate regime is similarly affected, more significantly at the beginning of the experiments conducted in silica saturated solutions. These findings prove that the reactivity of glass remains controlled by its structure under the various alteration regimes.

show abstract

Glass dissolution rate measurement and calculation revisited

Cited by 77 publications

References 55 publications

Corrosion of the International Simple Glass under acidic to hyperalkaline conditions

Corrosion of the International Simple Glass under acidic to hyperalkaline conditions

Impact of alkali on the passivation of silicate glass

Effect of thermally induced structural disorder on the chemical durability of International Simple Glass

Contact Info

Product

Resources

About