Complexity of Uranyl Peroxide Cluster Speciation from Alkali-Directed Oxidative Dissolution of Uranium Dioxide
- Univ. of Notre Dame, IN (United States). Dept. of Civil and Environmental Engineering and Earth Sciences
- Univ. of Notre Dame, IN (United States). Dept. of Chemistry and Biochemistry
- Univ. of Notre Dame, IN (United States). Dept. of Civil and Environmental Engineering and Earth Sciences, and Dept. of Chemistry and Biochemistry
Solid UO2 dissolution and uranium speciation in aqueous solutions that promote formation of uranyl peroxide macroanions was examined, focusing on the role of alkali metals. UO2 powders were dissolved in solutions containing XOH (X = Li, Na, or K) and 30% H2O2. Inductively coupled plasma optical emission spectroscopy (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 4.36 x 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. Lastly, Raman spectroscopy and electrospray ionization mass spectrometry (ESI-MS) of solutions indicate that dissolution is accompanied by formation of various uranyl peroxide cluster species, the identity of which is alkali concentration-dependent, revealing remarkably complex speciation at high concentrations of base.
- Research Organization:
- Energy Frontier Research Centers (EFRC) (United States). Materials Science of Actinides (MSA); University of Notre Dame, IN (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)
- Grant/Contract Number:
- NA0003763; SC0001089
- OSTI ID:
- 1460947
- Journal Information:
- Inorganic Chemistry, Vol. 57, Issue 15; ISSN 0020-1669
- Publisher:
- American Chemical Society (ACS)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
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