Dependence of UO${}_2$ surface morphology on processing history within a single synthetic route

This study aims to determine forensic signatures for processing history of UO${}_2$ based on modifications in intermediate materials within the uranyl peroxide route. Uranyl peroxide was calcined to multiple intermediate U-oxides including Am-UO${}_3$, α-UO${}_3$, and α-U${}_3$O${}_8$ during the production of UO${}_2$. The intermediate U-oxides were then reduced to α-UO${}_2$ via hydrogen reduction under identical conditions. Powder X-ray diffractometry (p-XRD) and X-ray photoelectron spectroscopy (XPS) were used to analyze powders of the intermediate U-oxides and resulting UO${}_2$ to evaluate the phase and purity of the freshly synthesized materials. All U-oxides were also analyzed via scanning electron microscopy (SEM) to determine the morphology of the freshly prepared powders. The microscopy images were subsequently analyzed using the Morphological Analysis for Materials (MAMA) version 2.1 software to quantitatively compare differences in the morphology of UO${}_2$ from each intermediate U-oxide. In addition, the microscopy images were analyzed using a machine learning model which was trained based on a VGG 16 architecture. Results show no differences in the XRD or XPS spectra of the UO${}_2$ produced from each intermediate. However, results from both the segmentation and machine learning proved that the morphology was quantifiably different. In addition, the morphology of UO${}_2$ was very similar, if not identical, to the intermediate material from which it was prepared, thus making quantitative morphological analysis a reliable forensic signature of processing history.