Inorganic Chemistry · 2018 · 34 citations · 32 references
Natural SciencesChemistryMaterials ScienceAnalytical ChemistryInorganic ChemistryPhysical ChemistryAtomic SpectroscopyEnvironmental Analytical ChemistryInorganic SpectroscopyMass SpectrometryMetal OxidesMineral ChemistryAlkali Metal ChemistryElectrospray IonizationInductively Coupled Plasma Optical Emission SpectrometryInductively Coupled Plasma Optical Emission SpectroscopyInductively Coupled Plasma SpectrometryOxidative DissolutionUranium DioxideUranium Speciation
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.
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Peter C. Burns, Karrie‐Ann Kubatko, Ginger E. Sigmon et al. · Angewandte Chemie International Edition · 2005 · 277 citations · Full text