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

Published online by Cambridge University Press:  09 December 2019

Amber R. Mason ,
Stephanie M. Thornber ,
Martin C. Stennett Open the ORCID record for Martin C. Stennett [Opens in a new window] ,
Laura J. Gardner ,
Dirk Lützenkirchen-Hecht  and
Neil C. Hyatt
Amber R. Mason
Affiliation:
Immobilisation Science Laboratory, Department of Materials Science and Engineering, The University of Sheffield, Mappin Street, Sheffield, S1 3JD, UK
Stephanie M. Thornber
Affiliation:
Immobilisation Science Laboratory, Department of Materials Science and Engineering, The University of Sheffield, Mappin Street, Sheffield, S1 3JD, UK
Martin C. Stennett
Affiliation:
Immobilisation Science Laboratory, Department of Materials Science and Engineering, The University of Sheffield, Mappin Street, Sheffield, S1 3JD, UK
Laura J. Gardner
Affiliation:
Immobilisation Science Laboratory, Department of Materials Science and Engineering, The University of Sheffield, Mappin Street, Sheffield, S1 3JD, UK
Dirk Lützenkirchen-Hecht
Affiliation:
Fakultät 4 - Physik, Bergische Universität Wuppertal, Gaußstraße 20, 42097 Wuppertal, Germany
Neil C. Hyatt*
Affiliation:
Immobilisation Science Laboratory, Department of Materials Science and Engineering, The University of Sheffield, Mappin Street, Sheffield, S1 3JD, UK
*
*(Email: [email protected])
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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.

Keywords

actinideglassceramic
Type
Articles
Information
MRS Advances , Volume 5 , Issue 1-2: Scientific Basis for Nuclear Waste Management XLIII , 2020 , pp. 37 - 43
Copyright
Copyright © Materials Research Society 2019

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