Zhong, M.-X., Walkley, B. orcid.org/0000-0003-1069-1362, Bailey, D.J. orcid.org/0000-0002-0313-8748 et al. (9 more authors) (2021) Synthesis of Ca1-xCexZrTi2-2xAl2xO7 zirconolite ceramics for plutonium disposition. Journal of Nuclear Materials, 556. 153198. ISSN 0022-3115
Abstract
A series of zirconolite ceramics with stoichiometry Ca1-xCexZrTi2-2xAl2xO7 (x = 0–0.35), considered as a host phase for the immobilisation of separated plutonium, were prepared from a mixture of oxide precursors by sintering in air at 1450 °C. Ce was utilised as a structural surrogate for Pu, with Al added to provide charge compensation. XRD and electron diffraction analyses indicated crystallisation of the zirconolite-2M polytype for all compositions, accompanied by various secondary phases contingent on the doping level, consistent with microstructure observation. The relative yield of zirconolite phases remained above 94 wt.% for 0.05 < x < 0.20. It was determined that Ce was partially reduced to the Ce3+ oxidation state and Al occupied mainly octahedral Ti sites. The incorporation rate of CeO2 was calculated to be 9.27 wt.% in Ca0.80Ce0.20ZrTi1.60Al0.40O7 with a comparatively high yield of 94.7 wt.%, which is representative of a PuO2 incorporation rate of 14.86 wt.%.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Copyright, Publisher and Additional Information: | © 2021 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/). |
Keywords: | Plutonium immobilisation; Ceramic wasteforms; Zirconolite; Waste loading; Local environment |
Dates: |
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Institution: | The University of Sheffield |
Academic Units: | The University of Sheffield > Faculty of Engineering (Sheffield) > Department of Chemical and Biological Engineering (Sheffield) The University of Sheffield > Faculty of Engineering (Sheffield) > Department of Materials Science and Engineering (Sheffield) |
Funding Information: | Funder Grant number Engineering and Physical Sciences Research Council EP/L014041/1; EP/M026566/1; EP/N017374/1 Engineering and Physical Sciences Research Council EP/S01019X/1; EP/S011935/1 |
Depositing User: | Symplectic Sheffield |
Date Deposited: | 15 Oct 2021 06:24 |
Last Modified: | 15 Oct 2021 06:24 |
Status: | Published |
Publisher: | Elsevier BV |
Refereed: | Yes |
Identification Number: | 10.1016/j.jnucmat.2021.153198 |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:179258 |