Structural Phase Transitions and Water Dynamics in Uranyl Fluoride Hydrates

Miskowiec, Andrew J.; Kirkegaard, Marie C.; Huq, Ashfia; Mamontov, Eugene; Herwig, Kenneth W.; Trowbridge, Lee D.; Rondinone, Adam Justin; Anderson, Brian B.

doi:10.1021/acs.jpca.5b09296

Title: Structural Phase Transitions and Water Dynamics in Uranyl Fluoride Hydrates

Journal Article · Tue Nov 17 00:00:00 EST 2015 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI:https://doi.org/10.1021/acs.jpca.5b09296· OSTI ID:1286878

Miskowiec, Andrew J. ^[1]; Kirkegaard, Marie C. ^[2]; Huq, Ashfia ^[1]; Mamontov, Eugene ^[1]; Herwig, Kenneth W. ^[1]; Trowbridge, Lee D. ^[1]; Rondinone, Adam Justin ^[1]; Anderson, Brian B. ^[1]

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

We report a novel production method for uranium oxy uoride [(UO₂)₇F₁₄(H₂O)₇] 4H₂O, referred to as structure D. Structure D is produced as a product of hydrating anhydrous uranyl uoride, UO₂F₂, through the gas phase at ambient temperatures fol- lowed by desiccation by equilibration with a dry environment. We follow the structure of [(UO₂)₇F₁₄(H₂O)₇] 4H₂O through an intermediate, liquid-like phase, wherein the coordination number of the uranyl ion is reduced to 5 (from 6 in the anhydrous struc- ture), and a water molecule binds as an equatorial ligand to the uranyl ion. Quasielas- tic neutron scattering results compare well with previous measurements of mineral hydrates. The two groups of structurally distinct water molecules in D perform re- stricted motion on a length scale commensurate with the O{H bond (r = 0.92 A). The more tightly bound equatorial ligand waters rotate slower (Dr = 2.2 ps^-1) than their hydrogen-bonded partners (Dr = 28.7 ps^-1).

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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:: 1286878

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Vol. 119, Issue 49; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 9 works

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Analysis of Water Coupling in Inelastic Neutron Spectra of Uranyl Fluoride Miskowiec, Andrew; Niedziela, J. L.; Kirkegaard, Marie C. Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-019-46675-x	journal	July 2019
A NanoSIMS 50 L Investigation into Improving the Precision and Accuracy of the 235U/238U Ratio Determination by Using the Molecular 235U16O and 238U16O Secondary Ions Zirakparvar, N.; Hexel, Cole; Miskowiec, Andrew Minerals, Vol. 9, Issue 5 https://doi.org/10.3390/min9050307	journal	May 2019

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