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

Author:

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

Abstract

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+. Graphic abstract

Funder

Engineering and Physical Sciences Research Council

Publisher

Springer Science and Business Media LLC

Subject

Mechanical Engineering,Mechanics of Materials,Condensed Matter Physics,General Materials Science

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