Abstract
We have demonstrated the solid-state formation of a uranyl peroxide (UP) species from hydrated uranyl fluoride via a uranyl hydroxide intermediate, the first observation of a UP species formed in a solid-state reaction. Water vapor pressure is shown to be a driving factor of both the loss of fluorine and the subsequent formation of peroxo units. We have ruled out a photochemical mechanism for formation of the UP species by demonstrating that the same reaction occurs in the dark. A radiolytic mechanism is unlikely because of the low radioactivity of the sample material, suggesting the existence of a novel UP formation mechanism.
Original language | English |
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Pages (from-to) | 5711-5715 |
Number of pages | 5 |
Journal | Inorganic Chemistry |
Volume | 57 |
Issue number | 10 |
DOIs | |
State | Published - May 21 2018 |
Funding
The authors thank Lee Trowbridge, Darrell Simmons, Hal Jennings, Leigh Martin, and Ashley Shields in the Nuclear Security and Isotope Technology Division at Oak Ridge National Laboratory for source material production and helpful discussions. The SEM and EDS analyses were conducted at the Center for Nanophase Materials Sciences, which is a Department of Energy Office of Science User Facility. This manuscript has been authored by UT-Battelle, LLC, under Contract DE-AC05-00OR22725 with the U.S. Department of Energy (DOE). The U.S. government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. 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 U.S. government purposes. The 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). This material is based upon work supported by the U.S. Department of Homeland Security under Grant 2012-DN-130-NF0001. The views and conclusions contained in this document are those of the authors and should not be interpreted as representing the official policies, either expressed or implied, of the U.S. Department of Homeland Security.