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Preliminary investigation of chlorine speciation in zirconolite glass-ceramics for plutonium residues by analysis of Cl K-edge XANES

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Abstract

A zirconolite glass-ceramic material is a candidate wasteform for immobilisation of chlorine contaminated plutonium residues, in which plutonium and chlorine are partitioned to the zirconolite and aluminosilicate glass phase, respectively. A preliminary investigation of chlorine speciation was undertaken by analysis of Cl K-edge X-ray Absorption Near Edge Spectroscopy (XANES), to understand the incorporation mechanism. Cl was found to be speciated as the Cl- anion within the glass phase, according to the characteristic chemical shift of the X-ray absorption edge. By comparison with Cl K-edge XANES data acquired from reference compounds, the local environment of the Cl- anion is most closely approximated by the mineral marialite, in which Cl is co-ordinate to 4 x Na and/or Ca atoms.

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Authors and Affiliations

  1. Immobilisation Science Laboratory, Department of Materials Science and Engineering, The University of Sheffield, Mappin Street, Sheffield, S1 3JD, UK

    Amber R. Mason, Stephanie M. Thornber, Martin C. Stennett, Laura J. Gardner & Neil C. Hyatt

  2. Fakultät 4 — Physik, Bergische Universität Wuppertal, Gaußstraße 20, 42097, Wuppertal, Germany

    Dirk Lützenkirchen-Hecht

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  1. Amber R. Mason
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  2. Stephanie M. Thornber
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  3. Martin C. Stennett
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  4. Laura J. Gardner
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  5. Dirk Lützenkirchen-Hecht
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  6. Neil C. Hyatt
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Mason, A.R., Thornber, S.M., Stennett, M.C. et al. Preliminary investigation of chlorine speciation in zirconolite glass-ceramics for plutonium residues by analysis of Cl K-edge XANES. MRS Advances 5, 37–43 (2020). https://doi.org/10.1557/adv.2019.460

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