Online monitoring the hydrolysis of uranium hexafluoride for intermediates by cryogenic layering and FTIR

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Abstract

Uranium hexafluoride (UF6) is a commonly utilized material feedstock in uranium enrichment processes due to its high vapor pressure and ease of sublimation. When exposed to air, UF6 undergoes spontaneous hydrolysis to form uranyl fluoride (UO2F2) particulates which are utilized for the detection of undeclared nuclear activities by nuclear safeguards organizations. The kinetics of the hydrolysis reaction and how they relate to particle morphology of the product are still debated in the literature. Here, we report the direct, in situ observation of UF6 reaction intermediates by cooling the reaction to cryogenic temperatures to significantly reduce the rate of hydrolysis. The reaction is then observable by Fourier transform infrared (FTIR) spectroscopy. The conversion of UF6 to UOF4 is observed as well as several other bands associated with possible long lived intermediate complexes. Chemometrics are used to further elucidate the reaction pathway from UF6 to UO2F2.

Original languageEnglish
Article number1300544
JournalFrontiers in Nuclear Engineering
Volume2
DOIs
StatePublished - 2023
Externally publishedYes

Funding

The author(s) declare financial support was received for the research, authorship, and/or publication of this article. Financial support for this work was provided by the National Nuclear Security Administration under Defense Nuclear Nonproliferation R&D. This work was produced by Battelle Savannah River Alliance, LLC under Contract No. 89303321CEM000080 with the US Department of Energy. Publisher acknowledges the US Government license to provide public access under the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). Assistance from Jason Richards at ORNL for UF expertise and samples is greatly appreciated. 6

Keywords

  • FTIR
  • cryogenic
  • hydrolysis
  • reaction kinetics
  • spectroscopy
  • uranium hexafluoride

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