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Influence of Transition Metal Charge Compensation Species on Phase Assemblage in Zirconolite Ceramics for Pu Immobilisation

Published online by Cambridge University Press:  07 February 2020

L.R. Blackburn Open the ORCID record for L.R. Blackburn [Opens in a new window] ,
S.K. Sun ,
L.J. Gardner ,
E.R. Maddrell ,
M.C. Stennett Open the ORCID record for M.C. Stennett [Opens in a new window]  and
N.C. Hyatt
L.R. Blackburn
Affiliation:
Immobilisation Science Laboratory, University of Sheffield, Department of Materials Science and Engineering, Sir Robert Hadfield Building, Mappin Street, S13JD, UK
S.K. Sun
Affiliation:
Immobilisation Science Laboratory, University of Sheffield, Department of Materials Science and Engineering, Sir Robert Hadfield Building, Mappin Street, S13JD, UK
L.J. Gardner
Affiliation:
Immobilisation Science Laboratory, University of Sheffield, Department of Materials Science and Engineering, Sir Robert Hadfield Building, Mappin Street, S13JD, UK
E.R. Maddrell
Affiliation:
National Nuclear Laboratory, Workington, Cumbria, CA14 3YQ, UK
M.C. Stennett
Affiliation:
Immobilisation Science Laboratory, University of Sheffield, Department of Materials Science and Engineering, Sir Robert Hadfield Building, Mappin Street, S13JD, UK
N.C. Hyatt*
Affiliation:
Immobilisation Science Laboratory, University of Sheffield, Department of Materials Science and Engineering, Sir Robert Hadfield Building, Mappin Street, S13JD, UK
*
*(Email: [email protected])
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Abstract

Immobilisation of Pu in a zirconolite matrix (CaZrTi2O7) is a viable pathway to disposition. A-site substitution, in which Pu4+ is accommodated into the Ca2+ site in zirconolite, coupled with sufficient trivalent M3+/Ti4+ substitution (where M3+ = Fe, Al, Cr), has been systematically evaluated using Ce4+ as a structural analogue for Pu4+. A broadly similar phase assemblage of zirconolite-2M and minor perovskite was observed when targeting low levels of Ce incorporation. As the targeted Ce fraction was elevated, secondary phase formation was influenced by choice of M3+ species. Co-incorporation of Ce/Fe resulted in the stabilisation of a minor Ce-containing perovskite phase at high wasteloading, whereas considerable phase segregation was observed for Cr3+ incorporation. The most favourable substitution approach appeared to be achieved with the use of Al3+, as no perovskite or free CeO2 was observed. However, high temperature treatments of Al containing specimens resulted in the formation of a secondary Ce-containing hibonite phase.

Keywords

ceramicwaste management
Type
Articles
Information
MRS Advances , Volume 5 , Issue 1-2: Scientific Basis for Nuclear Waste Management XLIII , 2020 , pp. 93 - 101
Copyright
Copyright © Materials Research Society 2020

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