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Developing methodologies for source attribution: glass phase separation in Trinitite using NF3

  • Elizabeth C. Koeman EMAIL logo , Bruce K. McNamara , Frances N. Smith , Antonio Simonetti and Peter C. Burns
Published/Copyright: December 19, 2016
Radiochimica Acta
From the journal Radiochimica Acta Volume 105 Issue 5

Abstract

This study details thermal reactions between glasses, common minerals, and Trinitite post-detonation material with the fluorinating agent nitrogen trifluoride (NF3). The ultimate goal of our investigation is to develop a relatively rapid method for the effective separation of bomb components from complex matrices resulting from a nuclear explosion. Trinitite samples, silicate minerals (quartz; plagioclase and microcline), amorphous SiO2, calcite, a natural glass (obsidian), and two synthetic glasses were characterized extensively before and after the fluorination to fully understand the effects of the NF3 thermal treatment. Samples were reacted with NF3 using a combined thermogravimetric (TG) differential thermal analysis (DTA) unit, as well as in a stainless steel bomb reactor connected to a fluorination line. Subsequent to the NF3 treatment, samples were imaged by scanning electron microscopy in order to document changes in grain size and morphology. Energy dispersive spectroscopy was performed to determine changes in major element abundances. Results demonstrate that rates of reaction are dependent on grain size, temperature, pressure, and time of fluorination. All mineral samples experienced mass loss during fluorination. Specifically, amorphous SiO2 (~90% mass loss) experienced the most while calcite experienced the least (~18%). Major element analysis reveals that mass loss is attributable to the volatilization of silica (SiO2) in Si-bearing phases, or sample decomposition in calcite due to fluorination. Results for fluorinated samples of Trinitite demonstrate that mass loss occurs at different rates for each sample, but each sample experienced an expected large decrease in Si content (resulting from volatilization of SiF4). Hence, the concentration of metals in the residual material increased due to the volatilization of Si. These results validate that this thermal-fluorination technique allows the separation of silica from minerals (i.e. naturally occurring crystalline materials) and glasses (i.e. amorphous materials), leaving behind non-volatile fluorinated species and refractory phases. The results from our investigation clearly indicate that the NF3 treatment of nuclear materials is a technique that provides effective separation of bomb components from complex matrices (e.g. post-detonation samples), which will aid with rapid and accurate source attribution.

Keywords: Nuclear forensics; Trinitite; nitrogen trifluoride; fluorination; glass separation

Acknowledgements

This work is funded by DOE/NNSA Grant PDP11-40/DE-NA0001112. We thank Dr. I. Steele and PNNL staff, S. M. Goodwin, B. J. Garcia, and A. D. Eckberg, for their guidance with electron microprobe analysis. We also thank J. Szymanowski for her guidance and training on PXRD analyses. Finally, we thank M. Schweiger and the staff at PNNL’s Advanced Process Engineering Laboratory (APEL) for providing glass samples and sample preparation support.

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Supplemental Material:

The online version of this article (DOI: 10.1515/ract-2016-2641) offers supplementary material, available to authorized users.

Received: 2016-6-8
Accepted: 2016-10-12
Published Online: 2016-12-19
Published in Print: 2017-5-1

©2017 Walter de Gruyter GmbH, Berlin/Boston

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https://doi.org/10.1515/ract-2016-2641
Keywords for this article
Nuclear forensics; Trinitite; nitrogen trifluoride; fluorination; glass separation

Articles in the same Issue

  1. Frontmatter
  2. Neutron capture cross section measurements and theoretical calculation for the 186W(n,γ)187W reaction
  3. Adsorption of U(VI) ions from aqueous solutions by activated carbon prepared from Antep pistachio (Pistacia vera L.) shells
  4. Radiolytic syntheses of hollow UO2 nanospheres in Triton X-100-based lyotropic liquid crystals
  5. Hafnium(IV) complexation with oxalate at variable temperatures
  6. Radioiodinated famotidine as a new highly selective radiotracer for peptic ulcer disorder detection, diagnostic nuclear imaging and biodistribution
  7. Optimized production, quality control, biological evaluation and PET/CT imaging of 68Ga-PSMA-617 in breast adenocarcinoma model
  8. Pilot-scale study of the radiation-induced silica removal from underground brackish water in Saudi Arabia
  9. Developing methodologies for source attribution: glass phase separation in Trinitite using NF3
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