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Uranium oxide synthetic pathway discernment through thermal decomposition and morphological analysis

  • Ian J. Schwerdt , Casey G. Hawkins , Bryan Taylor , Alexandria Brenkmann , Sean Martinson und Luther W. McDonald IV EMAIL logo
Veröffentlicht/Copyright: 25. Oktober 2018
Radiochimica Acta
Aus der Zeitschrift Radiochimica Acta Band 107 Heft 3

Abstract

Many commercial processes exist for converting uranium from ore to the desired uranium compound for use in nuclear power or nuclear weapons. Accurately determining the processing history of the uranium ore concentrates (UOCs) and their calcination products, can greatly aid a nuclear forensics investigation of unknown or interdicted nuclear materials. In this study, two novel forensic signatures, based on nuclear materials synthesis, were pursued. Thermogravimetric analysis – mass spectrometry (TGA-MS) was utilized for its ability to discern UOCs based on mass changes and evolved gas species; while scanning electron microscopy (SEM), in conjunction with particle segmentation, was performed to identify microfeatures present in the calcination and reduction products (i.e. UO3, U3O8, and UO2) that are unique to the starting UOC. In total, five UOCs from common commercial processing routes including: ammonium diuranate (ADU), uranyl peroxide (UO4), sodium diuranate (SDU), uranyl hydroxide (UH), and ammonium uranyl carbonate (AUC), were synthesized from uranyl nitrate solutions. Samples of these materials were calcined in air at 400 °C and 800 °C. The 800 °C calcination product was subsequently reduced with hydrogen gas at 510 °C. The starting UOCs were investigated using TGA-MS; while SEM quantitative morphological analysis was used to identify signatures in the calcination products. Powder X-ray diffractometry (p-XRD) was used to identify the composition of each UOC and the subsequent calcination products. TGA-MS of the starting UOCs indicate temperature-dependent dehydration, volatilization, and reduction events that were unique to each material; thus making this a quantifiable signature of the initial material in the processing history. In addition, p-XRD, in conjunction with quantitative morphological analysis, was capable of discriminating calcination products of each processing history at the 99 % confidence level. Quantifying these nuclear material properties, enables nuclear forensics scientists to better identify the origin of unknown or interdicted nuclear materials.

Keywords: Nuclear forensics; uranium ore concentrates; scanning electron microscopy; thermogravimetric analysis; X-ray diffraction

Funding source: U.S. Department of Homeland Security

Award Identifier / Grant number: 2015-DN-077-ARI092

Funding source: Defense Threat Reduction Agency

Award Identifier / Grant number: HDTRA1-16-1-0026

Funding statement: This synthesis of the ADU, AUC, and their calcination products, along with their subsequent characterization by p-XRD, SEM, TGA-MS, and DSC were supported by the U.S. Department of Homeland Security, Domestic Nuclear Detection Office, under Grant Award no. 2015-DN-077-ARI092, Funder Id: http://dx.doi.org/10.13039/100000180. The synthesis of SDU, and UH along with their calcination products and subsequent characterization were supported by the Defense Threat Reduction Agency, under Grant Award no. HDTRA1-16-1-0026, Funder Id: http://dx.doi.org/10.13039/100000774. The U.S. Army Advanced Civil Schooling Program provided the funding for Major Bryan Taylor. The views and conclusions contained in this document are those of the authors and should not be interpreted as necessarily representing the official policies, either expressed or implied, of the U.S. Department of Homeland Security or Defense Threat Reduction Agency.

Acknowledgment

This work made use of University of Utah Shared facilities of the Surface Analysis and Nanoscale Imaging Group sponsored by the College of Engineering, Health Sciences Center, Office of the Vice President for Re-search, and the Utah Science Technology and Research (USTAR) Initiative of the State of Utah. This work made use of the Materials Characterization Lab at the University of Utah.

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Supplementary Material

The online version of this article offers supplementary material (https://doi.org/10.1515/ract-2018-3033).

Received: 2018-07-27
Accepted: 2018-10-01
Published Online: 2018-10-25
Published in Print: 2019-03-26

©2019 Walter de Gruyter GmbH, Berlin/Boston

Artikel in diesem Heft

  1. Frontmatter
  2. Uranium oxide synthetic pathway discernment through thermal decomposition and morphological analysis
  3. Applications of the uranium’s set of isotopes for nuclear dating: the Monte-Carlo method
  4. Quantification of trace level rare earth elements in Al matrices by ICP-MS
  5. Synergistic effect of vermiculite clay and ionizing irradiation on the physical and mechanical properties of polybutadiene rubber/ethylene propylene diene monomer nanocomposite
  6. Development of a novel 68Ga-dextran carboxylate derivative for blood pool imaging
  7. Distribution of naturally occurring radionuclides in soil around a coal-based power plant and their potential radiological risk assessment
  8. Investigation of γ ray shielding, structural and dissolution rate studies of alkali based bismuth borate glass systems with MoO3 added
  9. Novel radiochromic porphyrin-based film dosimeters for γ ray dosimetry: investigation on metal and ligand effects
https://doi.org/10.1515/ract-2018-3033
Schlagwörter für diesen Artikel
Nuclear forensics; uranium ore concentrates; scanning electron microscopy; thermogravimetric analysis; X-ray diffraction

Artikel in diesem Heft

  1. Frontmatter
  2. Uranium oxide synthetic pathway discernment through thermal decomposition and morphological analysis
  3. Applications of the uranium’s set of isotopes for nuclear dating: the Monte-Carlo method
  4. Quantification of trace level rare earth elements in Al matrices by ICP-MS
  5. Synergistic effect of vermiculite clay and ionizing irradiation on the physical and mechanical properties of polybutadiene rubber/ethylene propylene diene monomer nanocomposite
  6. Development of a novel 68Ga-dextran carboxylate derivative for blood pool imaging
  7. Distribution of naturally occurring radionuclides in soil around a coal-based power plant and their potential radiological risk assessment
  8. Investigation of γ ray shielding, structural and dissolution rate studies of alkali based bismuth borate glass systems with MoO3 added
  9. Novel radiochromic porphyrin-based film dosimeters for γ ray dosimetry: investigation on metal and ligand effects
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