Characterizing the degradation of [(UO2F2)(H2O)]7 4H2O under humid conditions

Kirkegaard, Marie C.; Ambrogio, Michael W.; Miskowiec, Andrew J.; Shields, Ashley E.; Niedziela, Jennifer L.; Spano, Tyler L.; Anderson, Brian B.

doi:10.1016/j.jnucmat.2019.151889

Title: Characterizing the degradation of [(UO₂F₂)(H₂O)]₇ 4H₂O under humid conditions

Journal Article · 17 November 2019 · Journal of Nuclear Materials

DOI: https://doi.org/10.1016/j.jnucmat.2019.151889 · OSTI ID:1607037

Kirkegaard, Marie C. ^[1];

^[2];

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Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Under humid conditions, uranyl fluoride ([(UO₂F₂)(H₂O)]₇·4H₂O) undergoes a loss of fluorine to form a uranyl hydroxide species, which can be further hydrated to form a uranyl peroxide species. X-ray diffraction data of the uranyl peroxide product is presented for the first time. In addition, the temperature and humidity conditions under which these reactions occur have been clarified by a 220-day experiment using microRaman spectroscopy to track chemical changes in individual particles of uranyl fluoride. At 25 and 35^°C, uranyl fluoride is found to be stable at 32% relative humidity but not stable at and above 59% relative humidity. We show that water vapor pressure is the driving factor in formation of both the hydroxide and peroxide products. The kinetics of the transformation from uranyl fluoride into uranyl hydroxide is consistent with a denucleation reaction following the absorption of water molecules.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1607037

Journal Information:: Journal of Nuclear Materials, Journal Name: Journal of Nuclear Materials Journal Issue: C Vol. 529; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
degradation
raman spectroscopy
relative humidity
uranium
uranyl flouride
uranyl hydroxide
uranyl peroxide
x-ray diffraction

Title: Characterizing the degradation of [(UO2F2)(H2O)]7 4H2O under humid conditions

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Title: Characterizing the degradation of [(UO₂F₂)(H₂O)]₇ 4H₂O under humid conditions