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

Frédéric Angeli 1 Thibault Charpentier 2 Patrick Jollivet 1 Dominique de Ligny 3 Michael Bergler 3 Alexander Veber 3 S. Gin 1 Hong Li 4 
1 LCLT - Laboratoire d'Etudes du Comportement à Long Terme des matériaux de conditionnement
DE2D - Département de recherche sur les technologies pour l'enrichissement, le démantèlement et les déchets : DEN/DE2D
2 LSDRM - Laboratoire Structure et Dynamique par Résonance Magnétique (LCF)
NIMBE UMR 3685 - Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M)
Abstract : 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 self-irradiation 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.
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Submitted on : Tuesday, September 11, 2018 - 5:25:01 PM
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Frédéric Angeli, Thibault Charpentier, Patrick Jollivet, Dominique de Ligny, Michael Bergler, et al.. Effect of thermally induced structural disorder on the chemical durability of International Simple Glass. npj Materials Degradation, 2018, 2 (1), pp.31. ⟨10.1038/s41529-018-0052-3⟩. ⟨cea-01872240⟩



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