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| Title: | Crystal chemistry and structures of (Ca,U) titanate pyrochlores. |
| Authors: | James, M Carter, ML Zhang, ZM Zhang, YJ Wallwork, KS Avdeev, M Vance, ER |
| Keywords: | Titanates Pyrochlore Electron Microscopy X-Ray Diffraction Crystal Structure Argon |
| Issue Date: | 1-Oct-2010 |
| Publisher: | Wiley-Blackwell |
| Citation: | James, M., Carter, M. L., Zhang, Z. M., Zhang, Y. J., Wallwork, K. S., Avdeev, M., et al. (2010). Crystal chemistry and structures of (Ca,U) titanate pyrochlores. Journal of the American Ceramic Society, 93(10), 3464-3473. |
| Abstract: | Analysis of multiphase (Ca,U) titanate pyrochlore samples produced under argon or in air, using laboratory X-ray powder diffraction (XRD) and electron microscopy revealed discrete pyrochlore phase compositions, together with either perovskite or rutile impurities. Investigations of these samples using diffuse reflectance and X-ray photoelectron spectroscopies revealed mixed U4+/U5+ oxidation states for argon-annealed samples and U5+/U6+ oxidation states for air-annealed samples. Single-phase (Ca1.25U4+0.25U5+0.50)Ti2O7 (argon) and (Ca1.40U5+0.60)(Ti1.90U6+0.10)O7 (air) compositions were synthesized and characterized using a combination of synchrotron X-ray and neutron powder diffraction. Severe intensity reduction of hkl odd XRD peaks from the sample produced in air was found to be the result of U6+ sharing the Ti site. The refined crystal structures for both single-phase samples were found to be consistent with the compositions and mixed oxidation states observed by the above spectroscopic measurements. Although the normalized uranium leach rate of the argon-annealed sample was found to be approximately twice that of the air-annealed sample, in 7-day Product Consistency Test the durability of both compounds with respect to leaching by water was found to be excellent. Ca releases were in the range of 0.01–0.03 g/L and U releases were <3 × 10−5 g/L. © 2010, Wiley-Blackwell. The definitive version is available at www3.interscience.wiley.com |
| URI: | http://dx.doi.org/10.1111/j.1551-2916.2010.03871.x http://apo.ansto.gov.au/dspace/handle/10238/2763 |
| ISSN: | 0002-7820 |
| Appears in Collections: | Journal Articles
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