Crystal chemical design principles were applied to synthesise novel U dominant and titanium excess betafite phases CaUZrTiO and CaUZrTiO, in high yield (85-95 wt%), and ceramic density reaching 99% of theoretical. Substitution of Ti on the A-site of the pyrochlore structure, in excess of full B-site occupancy, enabled the radius ratio (r/r = 1.69) to be tuned into the pyrochlore stability field, approximately 1.48 ≲ r/r ≲ 1.78, in contrast to the archetype composition CaUTiO (r/r = 1.75). U L-edge XANES and U 4f and U 4f XPS data evidenced U as the dominant speciation, consistent with the determined chemical compositions. The new betafite phases, and further analysis reported herein, point to a wider family of actinide betafite pyrochlores that could be stabilised by application of the underlying crystal chemical principle applied here.
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| http://dx.doi.org/10.1038/s41598-023-36571-w | DOI Listing |
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