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Radiation effects on the structure and alteration behavior of a SiO$_2$ ‐Al$_2$ O$_3$ ‐B$_2$ O$_3$ ‐Na$_2$ O glass

Amreen Jan 1 Jean‐marc Delaye 1, * Huseyin Kaya 2 Seong Kim 3 Anamul Haq Mir 4 Thibault Charpentier 5 Frédéric Angeli 1 Stephane Gin 1 
* Corresponding author
1 LDPV - Laboratoire de Développement des Procédés de Vitrification
DE2D - Département de recherche sur les technologies pour l'enrichissement, le démantèlement et les déchets : DES/ISEC/DE2D
5 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 : As borosilicate glasses are used in many countries to immobilize fission products and minor actinides after spent fuel reprocessing before storage in a deep geological repository, assessing their chemical durability is of paramount importance. Here pristine and pre-irradiated (952MeV, 136Xe) SiO2-B2O3-Al2O3-Na2O glasses with the same molar ratios as in the French SON68 and ISG glasses have been subjected to aqueous corrosion in deionized water and in silica saturated solution to measure the initial and longer-term alteration rates. Pristine and pre-irradiated glasses corrode following the same mechanisms but the pre-irradiation has a strong impact on the initial dissolution rate (increase by a factor of 5.6), and on the alteration layer depth in silica saturated conditions (by 2–3 folds). The later result is related to the formation of a more porous, less passivating gel on the pre-irradiated glass specimen. Using both experimental spectroscopies (NMR, IR, SFG) and classical molecular dynamics, the radiation effects on the glass structure and water diffusion have been assessed. After pre-irradiation, the density and the polymerization degree of the glass decrease while the topological disorder increases. In consequence, water diffusion accelerates. These observations allow to correlate the radiation impact on the alteration behavior to the structural changes.
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https://hal-cea.archives-ouvertes.fr/cea-03828008
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Submitted on : Tuesday, October 25, 2022 - 8:15:04 AM
Last modification on : Thursday, October 27, 2022 - 3:36:34 AM

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Amreen Jan, Jean‐marc Delaye, Huseyin Kaya, Seong Kim, Anamul Haq Mir, et al.. Radiation effects on the structure and alteration behavior of a SiO$_2$ ‐Al$_2$ O$_3$ ‐B$_2$ O$_3$ ‐Na$_2$ O glass. International Journal of Applied Glass Science, 2022, ⟨10.1111/ijag.16618⟩. ⟨cea-03828008⟩

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