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Phase evolution from Ln2Ti2O7 (Ln=Y and Gd) pyrochlores to brannerites in glass with uranium incorporation
Authors:Yingjie Zhang  Linggen Kong  Robert D Aughterson  Inna Karatchevtseva  Rongkun Zheng
Affiliation:1. Nuclear Fuel Cycle Research Theme, Australian Nuclear Science and Technology Organisation, Kirrawee DC, New South Wales, Australia;2. School of Physics and Advanced Materials, University of Sydney, Ultimo, New South Wales, Australia
Abstract:Ln2Ti2O7 (Ln=Y and Gd) pyrochlore glass‐ceramics have been fabricated successfully via internal crystallization. Subsequently, the phase evolution from Ln2Ti2O7 pyrochlores to Ln0.5U0.5Ti2O6 brannerites in glass with uranium (U) substitutions on the Ln‐site of Ln2Ti2O7 has been investigated using X‐ray diffraction, scanning electron microscope‐electron dispersive spectroscopy, transmission electron microscopy, Raman and diffuse reflectance spectroscopy. Combined characterization by XRD, SEM‐EDS and TEM SAED confirms the structures and phase evolution while Raman spectroscopy reveals characteristic vibration modes for both pyrochlore and brannerite. In addition, DRS of the U5+ ion has been used to probe the phase evolution, with the corresponding ff transition band of 2F7/2 energy level significantly shifting to longer wavenumbers due to the local coordination environment changing from eightfold coordination in pyrochlore to sixfold coordination in brannerite.
Keywords:glass‐ceramics  pyrochlore  titanates  uranium/uranium compounds
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