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

Abstract

We report a novel production method for uranium oxy uoride [(UO 2) 7F 14(H 2O) 7] 4H 2O, referred to as structure D. Structure D is produced as a product of hydrating anhydrous uranyl uoride, UO 2F 2, through the gas phase at ambient temperatures fol- lowed by desiccation by equilibration with a dry environment. We follow the structure of [(UO 2) 7F 14(H 2O) 7] 4H 2O 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).

Authors:
 [1];  [2];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1286878
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
Additional Journal Information:
Journal Volume: 119; Journal Issue: 49; Journal ID: ISSN 1089-5639
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY

Citation Formats

Miskowiec, Andrew J., Kirkegaard, Marie C., Huq, Ashfia, Mamontov, Eugene, Herwig, Kenneth W., Trowbridge, Lee D., Rondinone, Adam Justin, and Anderson, Brian B. Structural Phase Transitions and Water Dynamics in Uranyl Fluoride Hydrates. United States: N. p., 2015. Web. doi:10.1021/acs.jpca.5b09296.
Miskowiec, Andrew J., Kirkegaard, Marie C., Huq, Ashfia, Mamontov, Eugene, Herwig, Kenneth W., Trowbridge, Lee D., Rondinone, Adam Justin, & Anderson, Brian B. Structural Phase Transitions and Water Dynamics in Uranyl Fluoride Hydrates. United States. doi:10.1021/acs.jpca.5b09296.
Miskowiec, Andrew J., Kirkegaard, Marie C., Huq, Ashfia, Mamontov, Eugene, Herwig, Kenneth W., Trowbridge, Lee D., Rondinone, Adam Justin, and Anderson, Brian B. Tue . "Structural Phase Transitions and Water Dynamics in Uranyl Fluoride Hydrates". United States. doi:10.1021/acs.jpca.5b09296. https://www.osti.gov/servlets/purl/1286878.
@article{osti_1286878,
title = {Structural Phase Transitions and Water Dynamics in Uranyl Fluoride Hydrates},
author = {Miskowiec, Andrew J. and Kirkegaard, Marie C. and Huq, Ashfia and Mamontov, Eugene and Herwig, Kenneth W. and Trowbridge, Lee D. and Rondinone, Adam Justin and Anderson, Brian B.},
abstractNote = {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).},
doi = {10.1021/acs.jpca.5b09296},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 49,
volume = 119,
place = {United States},
year = {2015},
month = {11}
}

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