Structure and Reactivity of X-ray Amorphous Uranyl Peroxide, U2O7

Samuel O. Odoh, Jacob Shamblin, Christopher A. Colla, Sarah Hickam, Haylie L. Lobeck, Rachel A K Lopez, Travis Olds, Jennifer E S Szymanowski, Ginger E. Sigmon, Joerg Neuefeind, William H. Casey, Maik Lang, Laura Gagliardi, Peter C. Burns

Research output: Contribution to journalArticle

28 Scopus citations

Abstract

Recent accidents resulting in worker injury and radioactive contamination occurred due to pressurization of uranium yellowcake drums produced in the western U.S.A. The drums contained an X-ray amorphous reactive form of uranium oxide that may have contributed to the pressurization. Heating hydrated uranyl peroxides produced during in situ mining can produce an amorphous compound, as shown by X-ray powder diffraction of material from impacted drums. Subsequently, studtite, [(UO2)(O2)(H2O)2](H2O)2, was heated in the laboratory. Its thermal decomposition produced a hygroscopic anhydrous uranyl peroxide that reacts with water to release O2 gas and form metaschoepite, a uranyl-oxide hydrate. Quantum chemical calculations indicate that the most stable U2O7 conformer consists of two bent (UO2)2+ uranyl ions bridged by a peroxide group bidentate and parallel to each uranyl ion, and a μ2-O atom, resulting in charge neutrality. A pair distribution function from neutron total scattering supports this structural model, as do 1H- and 17O-nuclear magnetic resonance spectra. The reactivity of U2O7 in water and with water in air is higher than that of other uranium oxides, and this can be both hazardous and potentially advantageous in the nuclear fuel cycle.

Original languageEnglish (US)
Pages (from-to)3541-3546
Number of pages6
JournalInorganic chemistry
Volume55
Issue number7
DOIs
StatePublished - Apr 18 2016

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    Odoh, S. O., Shamblin, J., Colla, C. A., Hickam, S., Lobeck, H. L., Lopez, R. A. K., Olds, T., Szymanowski, J. E. S., Sigmon, G. E., Neuefeind, J., Casey, W. H., Lang, M., Gagliardi, L., & Burns, P. C. (2016). Structure and Reactivity of X-ray Amorphous Uranyl Peroxide, U2O7. Inorganic chemistry, 55(7), 3541-3546. https://doi.org/10.1021/acs.inorgchem.6b00017