Synthesis and characterisation of HIP Ca0.80Ce0.20ZrTi1.60Cr0.40O7 zirconolite and observations of the ceramic–canister interface

Lewis R. Blackburn; Max R. Cole; Laura J. Gardner; Daniel J. Bailey; Merve Kuman; Amber R. Mason; Shi Kuan Sun; Ewan R. Maddrell; Martin C. Stennett; Claire L. Corkhill; Neil C. Hyatt

doi:10.1557/s43580-021-00055-8

Synthesis and characterisation of HIP Ca_0.80Ce_0.20ZrTi_1.60Cr_0.40O₇ zirconolite and observations of the ceramic–canister interface

Lewis R. Blackburn^*, Max R. Cole, Laura J. Gardner, Daniel J. Bailey, Merve Kuman, Amber R. Mason, Shi Kuan Sun, Ewan R. Maddrell, Martin C. Stennett, Claire L. Corkhill, Neil C. Hyatt^*

^*Corresponding author for this work

Research output: Contribution to journal › Article (Academic Journal) › peer-review

4 Citations (Scopus)

Abstract

A sample of zirconolite with nominal composition Ca_0.80Ce_0.20ZrTi_1.60Cr_0.40O₇ was processed via Hot Isostatic Pressing (HIP), with a dwell temperature and pressure of 1320 °C/100 MPa maintained for 4 h. The produced wasteform was characterised by powder XRD, SEM–EDS, Ce L₃ and Cr K-edge XANES. A significant portion of the Ce inventory did not fully partition within the zirconolite phase, instead remaining as CeO₂ within the microstructure. Inspection of the stainless steel–ceramic interface detailed the presence of an interaction region dominated by a Cr-rich oxide layer. No significant Cr or Fe migration was observed, although a greater concentration of perovskite was observed at the periphery, relative to the bulk ceramic matrix. The X-ray absorption features of Cr remained analogous with Cr³⁺ accommodation within TiO₆ octahedra in the zirconolite matrix. The absorption edge of Ce was comprised of contributions from zirconolite-2M and unincorporated CeO₂, with an average oxidation state of Ce^3.9+. As zirconolite-2M accounted for > 92 wt% of the overall phase assemblage, it is clear that the dominant oxidation state of Ce in this phase was Ce⁴⁺.

Original language	English
Pages (from-to)	112-118
Number of pages	7
Journal	MRS Advances
Volume	6
Issue number	4-5
DOIs	https://doi.org/10.1557/s43580-021-00055-8
Publication status	Published - 16 Apr 2021

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Blackburn, L. R., Cole, M. R., Gardner, L. J., Bailey, D. J., Kuman, M., Mason, A. R., Sun, S. K., Maddrell, E. R., Stennett, M. C., Corkhill, C. L., & Hyatt, N. C. (2021). Synthesis and characterisation of HIP Ca_0.80Ce_0.20ZrTi_1.60Cr_0.40O₇ zirconolite and observations of the ceramic–canister interface. MRS Advances, 6(4-5), 112-118. https://doi.org/10.1557/s43580-021-00055-8

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title = "Synthesis and characterisation of HIP Ca0.80Ce0.20ZrTi1.60Cr0.40O7 zirconolite and observations of the ceramic–canister interface",

abstract = "A sample of zirconolite with nominal composition Ca0.80Ce0.20ZrTi1.60Cr0.40O7 was processed via Hot Isostatic Pressing (HIP), with a dwell temperature and pressure of 1320 °C/100 MPa maintained for 4 h. The produced wasteform was characterised by powder XRD, SEM–EDS, Ce L3 and Cr K-edge XANES. A significant portion of the Ce inventory did not fully partition within the zirconolite phase, instead remaining as CeO2 within the microstructure. Inspection of the stainless steel–ceramic interface detailed the presence of an interaction region dominated by a Cr-rich oxide layer. No significant Cr or Fe migration was observed, although a greater concentration of perovskite was observed at the periphery, relative to the bulk ceramic matrix. The X-ray absorption features of Cr remained analogous with Cr3+ accommodation within TiO6 octahedra in the zirconolite matrix. The absorption edge of Ce was comprised of contributions from zirconolite-2M and unincorporated CeO2, with an average oxidation state of Ce3.9+. As zirconolite-2M accounted for > 92 wt% of the overall phase assemblage, it is clear that the dominant oxidation state of Ce in this phase was Ce4+. ",

author = "Blackburn, {Lewis R.} and Cole, {Max R.} and Gardner, {Laura J.} and Bailey, {Daniel J.} and Merve Kuman and Mason, {Amber R.} and Sun, {Shi Kuan} and Maddrell, {Ewan R.} and Stennett, {Martin C.} and Corkhill, {Claire L.} and Hyatt, {Neil C.}",

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T1 - Synthesis and characterisation of HIP Ca0.80Ce0.20ZrTi1.60Cr0.40O7 zirconolite and observations of the ceramic–canister interface

AU - Blackburn, Lewis R.

AU - Cole, Max R.

AU - Gardner, Laura J.

AU - Bailey, Daniel J.

AU - Kuman, Merve

AU - Mason, Amber R.

AU - Sun, Shi Kuan

AU - Maddrell, Ewan R.

AU - Stennett, Martin C.

AU - Corkhill, Claire L.

AU - Hyatt, Neil C.

PY - 2021/4/16

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N2 - A sample of zirconolite with nominal composition Ca0.80Ce0.20ZrTi1.60Cr0.40O7 was processed via Hot Isostatic Pressing (HIP), with a dwell temperature and pressure of 1320 °C/100 MPa maintained for 4 h. The produced wasteform was characterised by powder XRD, SEM–EDS, Ce L3 and Cr K-edge XANES. A significant portion of the Ce inventory did not fully partition within the zirconolite phase, instead remaining as CeO2 within the microstructure. Inspection of the stainless steel–ceramic interface detailed the presence of an interaction region dominated by a Cr-rich oxide layer. No significant Cr or Fe migration was observed, although a greater concentration of perovskite was observed at the periphery, relative to the bulk ceramic matrix. The X-ray absorption features of Cr remained analogous with Cr3+ accommodation within TiO6 octahedra in the zirconolite matrix. The absorption edge of Ce was comprised of contributions from zirconolite-2M and unincorporated CeO2, with an average oxidation state of Ce3.9+. As zirconolite-2M accounted for > 92 wt% of the overall phase assemblage, it is clear that the dominant oxidation state of Ce in this phase was Ce4+.

AB - A sample of zirconolite with nominal composition Ca0.80Ce0.20ZrTi1.60Cr0.40O7 was processed via Hot Isostatic Pressing (HIP), with a dwell temperature and pressure of 1320 °C/100 MPa maintained for 4 h. The produced wasteform was characterised by powder XRD, SEM–EDS, Ce L3 and Cr K-edge XANES. A significant portion of the Ce inventory did not fully partition within the zirconolite phase, instead remaining as CeO2 within the microstructure. Inspection of the stainless steel–ceramic interface detailed the presence of an interaction region dominated by a Cr-rich oxide layer. No significant Cr or Fe migration was observed, although a greater concentration of perovskite was observed at the periphery, relative to the bulk ceramic matrix. The X-ray absorption features of Cr remained analogous with Cr3+ accommodation within TiO6 octahedra in the zirconolite matrix. The absorption edge of Ce was comprised of contributions from zirconolite-2M and unincorporated CeO2, with an average oxidation state of Ce3.9+. As zirconolite-2M accounted for > 92 wt% of the overall phase assemblage, it is clear that the dominant oxidation state of Ce in this phase was Ce4+.

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