Abstract
Morphological analysis of uranium materials has proven to be a key signature for nuclear forensic purposes. This study examines the morphological changes to magnesium diuranate (MDU) and sodium diuranate (SDU) during reduction in a 10 % hydrogen atmosphere with and without steam present. Impurity concentrations of the materials were also examined pre and post reduction using energy dispersive X-ray spectroscopy combined with scanning electron microscopy (SEM-EDX). The structures of the MDU, SDU, and UO x samples were analyzed using powder X-ray diffraction (p-XRD). Using this method, UO x from MDU was found to be a mixture of UO2, U4O9, and MgU2O6 while UO x from SDU were combinations of UO2, U4O9, U3O8, and UO3. By SEM, the MDU and UO x from MDU had identical morphologies comprised of large agglomerates of rounded particles in an irregular pattern. SEM-EDX revealed pockets of high U and high Mg content distributed throughout the materials. The SDU and UO x from SDU had slightly different morphologies. The SDU consisted of massive agglomerates of platy sheets with rough surfaces. The UO x from SDU was comprised of massive agglomerates of acicular and sub-rounded particles that appeared slightly sintered. Backscatter images of SDU and related UO x materials showed sub-rounded dark spots indicating areas of high Na content, especially in UO x materials created in the presence of steam. SEM-EDX confirmed the presence of high sodium concentration spots in the SDU and UO x from SDU. Elemental compositions were found to not change between pre and post reduction of MDU and SDU indicating that reduction with or without steam does not affect Mg or Na concentrations. The identification of Mg and Na impurities using SEM analysis presents a readily accessible tool in nuclear material analysis with high Mg and Na impurities likely indicating processing via MDU or SDU, respectively. Machine learning using convolutional neural networks (CNNs) found that the MDU and SDU had unique morphologies compared to previous publications and that there are distinguishing features between materials created with and without steam.
Funding source: National Nuclear Security Administration
Award Identifier / Grant number: Unassigned
Funding source: Office of Defense Nuclear Nonproliferation
Award Identifier / Grant number: Unassigned
Funding source: National Technical Nuclear Forensics Center
Award Identifier / Grant number: Unassigned
Funding source: Department of Homeland Security
Award Identifier / Grant number: Unassigned
Acknowledgments
The MDU and SDU synthesis and characterization was supported by the Department of Homeland Security (DHS) under project 2016-DN-077-ARI102. The reduction of starting materials to UO x using dry and wet atmospheres and their subsequent characterization was funded by the Department of Energy’s National Nuclear Security Administration, Office of Defense Nuclear Nonproliferation Research and Development. SEM analysis at LANL was supported by the National Technical Nuclear Forensics Center (NTNFC) within Countering Weapons of Mass Destruction (CWMD), formerly the Domestic Nuclear Detection Office (DNDO), of the Department of Homeland Security. Through Los Alamos National Laboratory, this document is approved for unlimited release under LA-UR-23-26943. We would like to thank Thomas Blanton of the ICDD for supplying us with the pdf files of MgU2O6, MgUO4, and MgU3O10 for p-XRD analysis.
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Research ethics: All authors declare that the work presented in this manuscript is their own work and have not altered the data in any way.
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Author contributions: All the authors have accepted responsibility for the entire content of this submitted manuscript and approved submission.
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Competing interests: The authors declare no conflicts of interest regarding this article.
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Research funding: This work was supported by the Department of Homeland Security (DHS) under project 2016-DN-077-ARI102; Department of Energy’s National Nuclear Security Administration, Office of Defense Nuclear Nonproliferation Research and Development; Technical Nuclear Forensics Center (NTNFC) within Countering Weapons of Mass Destruction (CWMD), formerly the Domestic Nuclear Detection Office (DNDO), of the Department of Homeland Security.
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Data availability: All data presented in this manuscript is provided in the related supplemental information.
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Supplementary Material
This article contains supplementary material (https://doi.org/10.1515/ract-2023-0221).
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