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Morizet, Y., Soudani, S., Hamon, J., Paris, M., La, C. & Gautron, E. (2023) Iodine dissolution mechanisms in high-pressure aluminoborosilicate glasses and their relationship to oxygen speciation. J. Mater. Chem. A, 11 22891–22905.
Added by: Richard Baschera (2023-11-22 10:11:27) Last edited by: Richard Baschera (2023-11-22 10:14:26) |
| Type de référence: Article DOI: 10.1039/D3TA05344J Numéro d'identification (ISBN etc.): 2050-7496 Clé BibTeX: Morizet2023 Voir tous les détails bibliographiques  |
Catégories: IMN Créateurs: Gautron, Hamon, La, Morizet, Paris, Soudani Collection: J. Mater. Chem. A |
Consultations : 1/35
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| Liens URLs https://pubs.rsc.o ... 2023/ta/d3ta05344j |
| Résumé |
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Incorporation of iodine(I) into high-pressure vitrified glasses appears to be a potential solution for the immobilization of 129I radioisotopes. Under these conditions, I dissolution is strongly enhanced; however, the impact I dissolution has on the glass structure remains to be determined to assess the matrix durability. We have experimentally studied the change in I solubility and speciation in a series of sodium aluminoborosilicate glasses (Na2O ranging from 10 to 40 mol%) held at 0.25 and 1.0 GPa and 1250 °C. As expected, the I solubility increases with pressure and with increasing Na2O and is positively correlated with the glass optical basicity. The I speciation determined by XPS is changing with the initial loaded source of iodine (either I2 or I2O5) with a predominant iodide form (I−) in the glass structure. The investigation of the oxygen environment in the I-bearing glasses using O 1s XPS revealed that I dissolution induces an apparent oxygen loss within the glass structure. This result is consistent with our current view on I dissolution mechanisms. Furthermore, the subsequent simulations of the O 1s XPS spectra suggest that I dissolution consumes non-bridging oxygen to form bridging oxygen. This change in the oxygen speciation points toward an increase in the glass durability, which is an important aspect for nuclear waste immobilization.
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Publisher: The Royal Society of Chemistry
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