A systematic investigation of the phase assemblage and microstructure of the zirconolite CaZr1-xCexTi2O7 system

A series of zirconolite ceramics with nominal stoichiometry CaZr1-xCexTi2O7 (0.0 ≤ x ≤ 0.4) were synthesised under oxidizing, inert and reducing conditions, by a conventional solid-state cold press and sinter method. The evolution of phase assemblage and microstructure were characterized by XRD, SEM...

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Bibliographic Details
Published in:Journal of nuclear materials 2020-07, Vol.535, p.152137, Article 152137
Main Authors: Blackburn, Lewis R., Sun, Shikuan, Gardner, Laura J., Maddrell, Ewan R., Stennett, Martin C., Hyatt, Neil C.
Format: Article
Language:English
Subjects:
Ceramic
Cerium
Cold pressing
Immobilisation
Microstructure
Oxidation
Perovskites
Phase assemblages
Plutonium
Polytypes
Raman spectroscopy
Speciation
Stoichiometry
Surrogate
Wasteform
Zirconolite
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Summary:A series of zirconolite ceramics with nominal stoichiometry CaZr1-xCexTi2O7 (0.0 ≤ x ≤ 0.4) were synthesised under oxidizing, inert and reducing conditions, by a conventional solid-state cold press and sinter method. The evolution of phase assemblage and microstructure were characterized by XRD, SEM-EDS, Ce-L3 XANES and Raman spectroscopy techniques. It was determined that the relative yield of zirconolite-2M and zirconolite-4M polytypes, alongside secondary perovskite phases, was influenced by processing environment via the control of Ce3+/4+ speciation. Oxidizing conditions produced a mixture of zirconolite-2M and zirconolite-4M polytypes due to the formation of Ce4+. Inert and reducing conditions yielded predominantly zirconolite-2M and a Ce-bearing perovskite phase through favouring Ce3+ speciation.
ISSN:0022-3115
1873-4820
DOI:10.1016/j.jnucmat.2020.152137