Structural features of early fuel cycle taggant incorporation for intentional nuclear forensics

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Abstract

To develop strategies for incorporating transition metal taggants (Fe, Cr, and Ni) into oxide fuels and to understand how these taggant candidates persist through early fuel cycle processes, synthetic procedures are modified from established production routes to yield intentionally tagged early fuel cycle intermediates including uranyl nitrate hexahydrate (UNH, UO2(NO3)2·6H2O), uranyl peroxide tetrahydrate (studtite, UO2O2·4H2O), and uranyl peroxide dihydrate (metastudtite, UO2O2·2H2O). First, Fe, Cr, and Ni nitrate solutions are introduced to an aqueous solution of UNH followed by precipitation to produce tagged UNH. Then, studtite is precipitated from UNH followed by dehydration to metastudtite. Structural influences of taggant incorporation within all synthesized phases are investigated using powder X-ray diffraction (PXRD) and Raman spectroscopy to provide insight into crystallographic modifications resulting from the addition of tags to these early fuel cycle materials and elucidate the chemical form of taggants introduced at these stages. The possibility of segregation of taggant species into discrete phases within U matrices was examined using scanning electron microscopy with energy dispersive X-ray spectroscopy. Taggant concentrations in solid-phase materials were determined using inductively coupled plasma-optical emission spectroscopy. Observations from Raman spectroscopy and PXRD indicate that introducing transition metal tags during uranyl nitrate precipitation results in potential impurity phase segregation in UNH, but transition metal incorporation is suggested by results for tagged uranyl peroxide materials. Results from this study will inform strategies for optimizing taggant incorporation in UO2.

Original languageEnglish
Article number154787
JournalJournal of Nuclear Materials
Volume588
DOIs
StatePublished - Jan 2024

Funding

The authors thank Ali Moore, Tara Rose, JJ Quinn, and Keith Gilbert for their support. Our work was greatly improved by fruitful discussions and feedback from Drs. Connor Parker and Luke Sadergaski, and from the helpful suggestions provided by two anonymous reviewers. This work was funded by the United States Department of Energy National Nuclear Security Administration (NNSA) Office of Defense Nuclear Nonproliferation (DNN) Research and Development Forensics program . Notice: This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05–00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ).

Keywords

  • Metastudtite
  • Nuclear forensics
  • Raman spectroscopy
  • Studtite
  • Uranyl nitrate
  • Uranyl peroxide

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