Investigation of UO2 doped with Fe2O3 sintered under a reducing atmosphere

Abstract

Nuclear fuel produced with trace amounts of transition metal additives is of potential interest for introducing intentional signatures for accelerating nuclear forensics. In this work, we investigate the effects on microstructure, grain size, crystal structure, and stoichiometry when trace amounts of Fe in the form of Fe₂O₃ are added to UO₂. Sintering of compacts with different concentrations, from 250 to 3000 ppmw, was performed under a reducing atmosphere at 1773 K. The persistence of the taggant during the fuel fabrication process as well as its impact on grain size, crystal lattice, and first-neighbor chemistry was evaluated using inductively coupled plasma–optical emission spectroscopy, powder X-ray diffraction (pXRD), Raman spectroscopy, scanning electron microscopy–backscatter electron spectroscopy, energy dispersive spectroscopy, and thermogravimetric analysis. We observed that a negligible amount of Fe was lost during sintering. Our results indicate that the feedstock, Fe₂O₃ transforms into Fe and FeO under the test sintering conditions. For all compositions, metallic Fe precipitate was found in grain boundaries as a secondary phase. The potential incorporation of ionic Fe into the UO₂ unit cell was determined by pXRD and Raman spectra.