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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

Authors :
Jan, Amreen
Delaye, Jean‐marc
Kaya, Huseyin
Kim, Seong
Mir, Anamul Haq
Charpentier, Thibault
Angeli, Frédéric
Gin, Stephane
Laboratoire de Développement des Procédés de Vitrification (LDPV)
Département de recherche sur les Procédés et Matériaux pour les Environnements complexes (DPME)
CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN))
Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN))
Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)
Department of Materials Science and Engineering
Pennsylvania State University (Penn State)
Penn State System-Penn State System
Department of Chemical Engineering
University of Huddersfield
Laboratoire Structure et Dynamique par Résonance Magnétique (LCF) (LSDRM)
Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685)
Institut Rayonnement Matière de Saclay (IRAMIS)
Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (IRAMIS)
Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
the Center for Performance and Design of Nuclear Waste Forms and Containers, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC00165
the Engineering and Physical Sciences Research Council for funding under Early career Fellowship grant EP/ T012811/1.
Source :
International Journal of Applied Glass Science, International Journal of Applied Glass Science, 2022, ⟨10.1111/ijag.16618⟩
Publication Year :
2022
Publisher :
HAL CCSD, 2022.

Abstract

International audience; 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.

Details

Language :
English
ISSN :
20411286 and 20411294
Database :
OpenAIRE
Journal :
International Journal of Applied Glass Science, International Journal of Applied Glass Science, 2022, ⟨10.1111/ijag.16618⟩
Accession number :
edsair.od......3515..b1712235ff8e441f4f0baf99992983c8