Please use this identifier to cite or link to this item: https://apo.ansto.gov.au/dspace/handle/10238/9774
Title: Partitioning of Ce, as a simulant for Pu, in a multiphase ceramic nuclear waste form
Authors: Zhang, Z
Spiers, KM
Vance, ER
Davis, J
Keywords: Pyrochlore
Ceramics
Cerium
Rare earths
Plutonium
Perovskite
Sintering
Fluorescence
Ceramics
Issue Date: 28-May-2020
Publisher: The American Ceramic Society
Citation: Zhang, Z., Spiers, K. M., Vance, E. R., & Davis, J. (2020). Partitioning of Ce, as a simulant for Pu, in a multiphase ceramic nuclear waste form. Journal of the American Chemical Society, 103(10), 5515-5524. doi:10.1111/jace.17277
Abstract: A pyrochlore‐rich multiphase ceramic waste form was prepared by the alkoxide‐route and consolidated by sintering in air. Cerium (Ce) was used as a surrogate for plutonium (Pu), which was found in both the major pyrochlore and minor perovskite phases, but not the minor rutile phase. A synchrotron‐based fluorescence X‐ray absorption near‐edge spectroscopy (XANES) imaging technique was employed to determine the Ce oxidation state in each of the two Ce‐containing phases. It was shown that the major pyrochlore phase contains only tetravalent Ce, whereas the minor perovskite phase incorporates exclusively trivalent Ce. The effect of sintering atmosphere was also investigated, which revealed a very different phase assemblage when sintered in argon (Ar). A major perovskite phase was produced under Ar with a minor zirconolite‐4M phase, both containing trivalent Ce. The composition of the minor rutile phase remained the same whether it was sintered in air or Ar. The results demonstrate the importance of controlling the oxidation state of multivalent waste ions in the design of ceramic waste forms. © 2020 The American Ceramic Society,
URI: https://doi.org/10.1111/jace.17277
https://apo.ansto.gov.au/dspace/handle/10238/9774
ISSN: 1551-2916
Appears in Collections:Journal Articles

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