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XANES analysis of a Cm-doped borosilicate glass under \(\alpha \)-self-irradiation effects

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Abstract

Industrial borosilicate glasses containing fission products and minor actinides can be subjected to structural damage caused mainly by \(\alpha \)-self-irradiation effects. In this field of glasses under extreme conditions, we present an X-ray Absorption Near-Edge Structure investigation of two six-oxide borosilicate curium-doped glasses (based on the International Simplified Glass (ISG) composition). The first sample is an 8-year ISG damaged glass, which has already accumulated an \(\alpha \)-decay dose greater than 6.10\(^{18}\) \(\alpha \) g\(^{-1}\), a value corresponding to a damaged but stabilized structural state. The second sample results from annealing of the latter ISG damaged glass. Three species, Cm, Pu and Zr were probed at \(L_{3}\)-edge, \(L_{3}\)-edge and K-edge, respectively. From the experimental results, Cm and Pu species appear respectively in +3 and +4 oxidation states in both glasses. No Cm local environment changes are observed. In contrast, a small variation in Pu local environment appears between the damaged and annealed glasses, reflecting a possible coordination variation or Pu–Zr substitution. A more drastic effect appears for Zr local environment, where a sevenfold coordinated site grows over time under \(\alpha \)-self-irradiation effects, at the expense of the initial major sixfold site of symmetry. Moreover, annealing the damaged glass does not permit to retrieve a similar structural state to the one of a just melted curium-doped ISG.

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Acknowledgements

We would like to thank P. Martin, X. Deschanels, S. Peuget and J.-M. Delaye for valuable discussions, P. Jollivet for providing XAS crystalline references containing Zr, T. Dumas for providing sample holders, M. Bataille, P. Coste, C. Dubois, M. Desir, V. Broudic and P. Rigaux (all from CEA Marcoule) for technical and logistic support during the samples preparation, J. Rothe, M. Weigl (from Karlsruhe Institut für Technologie), C. Hennig (from Dresden Radiochemistry Institute) for providing Cm\(^{3+}\) aquo ion XANES spectra, and SOLEIL synchrotron for beamtime provision.

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Authors and Affiliations

  1. Commissariat à l’Energie Atomique, Direction de l’Energie Nucléaire, Laboratoire d’Etude des Matériaux Actifs, BP 17171, 30207, Bagnols sur Cèze, France

    O. Bouty

  2. Commissariat à l’Energie Atomique, Direction de l’Energie Nucléaire, Laboratoire des Combustibles, BP 17171, 30207, Bagnols sur Cèze, France

    L. Ramond

  3. Synchrotron SOLEIL, L’Orme des Merisiers, BP 48, 91192, Gif-sur-Yvette Cedex, Saint Aubin, France

    P. L. Solari & S. Cammelli

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  1. O. Bouty
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  2. L. Ramond
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  3. P. L. Solari
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  4. S. Cammelli
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Correspondence to O. Bouty.

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Bouty, O., Ramond, L., Solari, P.L. et al. XANES analysis of a Cm-doped borosilicate glass under \(\alpha \)-self-irradiation effects. J Mater Sci 51, 7918–7928 (2016). https://doi.org/10.1007/s10853-016-0058-6

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  • DOI: https://doi.org/10.1007/s10853-016-0058-6

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