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Title: Crystal chemistry and structures of (Ca,U) titanate pyrochlores
Authors: James, M
Carter, ML
Zhang, Z
Zhang, Y
Wallwork, KS
Avdeev, M
Vance, ER
Keywords: Titanates
Electron microscopy
X-ray diffraction
Crystal structure
Issue Date: 1-Oct-2010
Publisher: Wiley-Blackwell
Citation: James, M., Carter, M. L., Zhang, Z., Zhang, Y., Wallwork, K. S., Avdeev, M., & Vance, E. R. (2010). Crystal chemistry and structures of (Ca,U) titanate pyrochlores. Journal of the American Ceramic Society, 93(10), 3464-3473. doi:10.1111/j.1551-2916.2010.03871.x
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.
Gov't Doc #: 2943
ISSN: 0002-7820
Appears in Collections:Journal Articles

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