Complexity of Uranyl Peroxide Cluster Speciation from Alkali-Directed Oxidative Dissolution of Uranium Dioxide

Inorganic Chemistry
Sarah HickamPeter C Burns

Abstract

Solid UO2 dissolution and uranium speciation in aqueous solutions that promote formation of uranyl peroxide macroanions was examined, with a focus on the role of alkali metals. UO2 powders were dissolved in solutions containing XOH (X = Li, Na, K) and 30% H2O2. Inductively coupled plasma optical emission spectrometry (ICP-OES) measurements of solutions revealed linear trends of uranium versus alkali concentration in solutions resulting from oxidative dissolution of UO2, with X:U molar ratios of 1.0, showing that alkali availability determines the U concentrations in solution. The maximum U concentration in solution was 4.20 × 105 parts per million (ppm), which is comparable to concentrations attained by dissolving UO2 in boiling nitric acid, and was achieved by lithium hydroxide promoted dissolution. Raman spectroscopy and electrospray ionization mass spectrometry (ESI-MS) of solutions indicate that dissolution is accompanied by the formation of various uranyl peroxide cluster species, the identity of which is alkali concentration dependent, revealing remarkably complex speciation at high concentrations of base.

References

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Dec 3, 2010·Journal of the American Chemical Society·Pere MiróCarles Bo
May 26, 2011·Journal of the American Chemical Society·Ginger E Sigmon, Peter C Burns
Jul 12, 2011·Dalton Transactions : an International Journal of Inorganic Chemistry·S MecaJ de Pablo
Oct 5, 2011·Dalton Transactions : an International Journal of Inorganic Chemistry·Pier Luigi ZanonatoIngmar Grenthe
Jun 15, 2012·Chemical Society Reviews·May Nyman, Peter C Burns
Aug 4, 2012·Chemical Society Reviews·Haralampos N MirasLeroy Cronin
Oct 26, 2012·Chemical Reviews·Jie Qiu, Peter C Burns
Nov 16, 2012·The Journal of Physical Chemistry. a·Valérie ValletIngmar Grenthe
Nov 22, 2012·Journal of the American Chemical Society·May Nyman, Todd M Alam
Jan 16, 2014·Inorganic Chemistry·Brendan T McGrailPeter C Burns
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Aug 20, 2016·Chemistry : a European Journal·Clément Falaise, May Nyman
Mar 22, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Peter C Burns, May Nyman

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Citations

Mar 7, 2019·Chemistry : a European Journal·Ana ArteagaMay Nyman
May 9, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Haylie L LobeckPeter C Burns
Oct 13, 2019·Angewandte Chemie·Dmytro V Kravchuk, Tori Z Forbes

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