Electrochemistry of soluble UO22+ from the direct dissolution of UO2CO3 in acidic ionic liquid containing water

Pemberton, Wendy J.; Droessler, Janelle E.; Kinyanjui, John M.; Czerwinski, Kenneth R.; Hatchett, David W.

doi:10.1016/j.electacta.2013.01.044

Title: Electrochemistry of soluble UO₂²⁺ from the direct dissolution of UO₂CO₃ in acidic ionic liquid containing water

Journal Article · Tue Jan 29 00:00:00 EST 2013 · Electrochimica Acta

DOI:https://doi.org/10.1016/j.electacta.2013.01.044· OSTI ID:1454616

Pemberton, Wendy J. ^[1]; Droessler, Janelle E. ^[1]; Kinyanjui, John M. ^[1]; Czerwinski, Kenneth R. ^[1]; Hatchett, David W. ^[1]

Univ. of Nevada, Las Vegas, NV (United States)

The direct dissolution of UO₂CO₃ in neat and “wet” ionic liquid (IL) trimethyl-n-butylammonium bis(trifluoromethansulfonyl)imide [Me₃NⁿBu][TFSI] is examined. The ionic liquid serves as both the solvent for the direct dissolution of UO₂CO₃(s) and the electrolyte solution for the electrochemical analysis of the soluble uranyl species. The solubility data indicate that displacement of the CO₃^2- occurs slowly due to the low concentration of protons available from residual water in the pristine IL. Enhanced dissolution of UO₂CO₃ through the formation of carbonic acid H₂CO₃ is achieved after the addition of acid, bis(trifluoromethanesulfonyl)amide (HTFSI) and water. The soluble uranyl cation can then coordinate with the TFSI anion in place of the displaced CO₃^2- anion following the decomposition of carbonic acid and purging of CO₂(g) and water from the IL. The solubility of UO₂CO₃ was examined using liquid scintillation counting of ²³³U for the pristine ionic liquid. The “wet” ionic liquid containing HTFSI and soluble UO₂CO₃ was evaluated using UV/vis spectroscopy before and after dissolution. The electrochemical deposition of uranium species from ionic liquid was evaluated using cyclic voltammetry. The potential mediated deposition of uranium species was achieved and verified using scanning electron microscopy (SEM) and the solid uranium deposits were evaluated using energy dispersive X-ray emission spectroscopy (EDX).

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States). Nuclear Science and Security Consortium

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

DOE Contract Number:: Na0000979

OSTI ID:: 1454616

Journal Information:: Electrochimica Acta, Vol. 93, Issue C; ISSN 0013-4686

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

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Title: Electrochemistry of soluble UO₂²⁺ from the direct dissolution of UO₂CO₃ in acidic ionic liquid containing water