Direct Electrodeposition of UO2 from Uranyl Bis(trifluoromethanesulfonyl)imide Dissolved in 1-Ethyl-3-methylimidazolium Bis(trifluoromethanesulfonyl)imide Room Temperature Ionic Liquid System

John W. Freiderich; Eranda Wanigasekara; Xiao Guang Sun; Roberta A. Meisner; Harry M. Meyer; Huimin Luo; Lætitia H. Delmau; Sheng Dai; Bruce A. Moyer

doi:10.1016/j.electacta.2013.10.187

Direct Electrodeposition of UO₂ from Uranyl Bis(trifluoromethanesulfonyl)imide Dissolved in 1-Ethyl-3-methylimidazolium Bis(trifluoromethanesulfonyl)imide Room Temperature Ionic Liquid System

John W. Freiderich, Eranda Wanigasekara, Xiao Guang Sun, Roberta A. Meisner, Harry M. Meyer, Huimin Luo, Lætitia H. Delmau, Sheng Dai, Bruce A. Moyer

Research output: Contribution to journal › Article › peer-review

21 Scopus citations

Abstract

This study demonstrates a direct electrodeposition of UO₂ at a Pt cathode from a solution of uranyl bis(trifluoromethanesulfonyl)imide [UO ₂(NTf₂)₂)] in a bulk room-temperature ionic liquid (RTIL), 1-ethyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide (EMIM⁺NTf₂^-). Cyclic voltammetry (CV) studies revealed two reduction waves corresponding to the conversion of uranium(VI) to uranium(IV), and a mechanism for the overall electroreduction is proposed. A controlled-potential experiment was performed, holding the reduction potential at-1.0 V for 24 h to obtain a brown-black deposit of UO₂ on the Pt cathode. The Faradaic efficiency of the reduction process was determined to be >80%. The UO₂ deposit was characterized by powder X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS).

Original language	English
Pages (from-to)	630-638
Number of pages	9
Journal	Electrochimica Acta
Volume	115
DOIs	https://doi.org/10.1016/j.electacta.2013.10.187
State	Published - Jan 1 2014

Funding

This research was supported by the Fuel Cycle Research and Development Program, Office of Nuclear Energy, U.S. Department of Energy. Authors thank Dr. Gilbert Brown (CSD), Dr. Claudia Rawn (MST), and Shawn Reeves (MST) at ORNL for useful discussions regarding electrochemistry, XRD, and SEM. Authors also gratefully acknowledge the use of ORNL's ShaRE User Facility, which is sponsored by the Office of Basic Energy Sciences, U.S. Department of Energy.

Keywords

Electrodeposition
Ionic Liquids
Uranium Dioxide

Access to Document

10.1016/j.electacta.2013.10.187

Cite this

Freiderich, J. W., Wanigasekara, E., Sun, X. G., Meisner, R. A., Meyer, H. M., Luo, H., Delmau, L. H., Dai, S., & Moyer, B. A. (2014). Direct Electrodeposition of UO₂ from Uranyl Bis(trifluoromethanesulfonyl)imide Dissolved in 1-Ethyl-3-methylimidazolium Bis(trifluoromethanesulfonyl)imide Room Temperature Ionic Liquid System. Electrochimica Acta, 115, 630-638. https://doi.org/10.1016/j.electacta.2013.10.187

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title = "Direct Electrodeposition of UO2 from Uranyl Bis(trifluoromethanesulfonyl)imide Dissolved in 1-Ethyl-3-methylimidazolium Bis(trifluoromethanesulfonyl)imide Room Temperature Ionic Liquid System",

abstract = "This study demonstrates a direct electrodeposition of UO2 at a Pt cathode from a solution of uranyl bis(trifluoromethanesulfonyl)imide [UO 2(NTf2)2)] in a bulk room-temperature ionic liquid (RTIL), 1-ethyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide (EMIM+NTf2-). Cyclic voltammetry (CV) studies revealed two reduction waves corresponding to the conversion of uranium(VI) to uranium(IV), and a mechanism for the overall electroreduction is proposed. A controlled-potential experiment was performed, holding the reduction potential at-1.0 V for 24 h to obtain a brown-black deposit of UO2 on the Pt cathode. The Faradaic efficiency of the reduction process was determined to be >80%. The UO2 deposit was characterized by powder X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS).",

keywords = "Electrodeposition, Ionic Liquids, Uranium Dioxide",

author = "Freiderich, {John W.} and Eranda Wanigasekara and Sun, {Xiao Guang} and Meisner, {Roberta A.} and Meyer, {Harry M.} and Huimin Luo and Delmau, {L{\ae}titia H.} and Sheng Dai and Moyer, {Bruce A.}",

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doi = "10.1016/j.electacta.2013.10.187",

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Freiderich, JW, Wanigasekara, E, Sun, XG, Meisner, RA, Meyer, HM , Luo, H , Delmau, LH , Dai, S & Moyer, BA 2014, 'Direct Electrodeposition of UO₂ from Uranyl Bis(trifluoromethanesulfonyl)imide Dissolved in 1-Ethyl-3-methylimidazolium Bis(trifluoromethanesulfonyl)imide Room Temperature Ionic Liquid System', Electrochimica Acta, vol. 115, pp. 630-638. https://doi.org/10.1016/j.electacta.2013.10.187

Direct Electrodeposition of UO₂ from Uranyl Bis(trifluoromethanesulfonyl)imide Dissolved in 1-Ethyl-3-methylimidazolium Bis(trifluoromethanesulfonyl)imide Room Temperature Ionic Liquid System. / Freiderich, John W.; Wanigasekara, Eranda; Sun, Xiao Guang et al.
In: Electrochimica Acta, Vol. 115, 01.01.2014, p. 630-638.

Research output: Contribution to journal › Article › peer-review

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T1 - Direct Electrodeposition of UO2 from Uranyl Bis(trifluoromethanesulfonyl)imide Dissolved in 1-Ethyl-3-methylimidazolium Bis(trifluoromethanesulfonyl)imide Room Temperature Ionic Liquid System

AU - Freiderich, John W.

AU - Wanigasekara, Eranda

AU - Sun, Xiao Guang

AU - Meisner, Roberta A.

AU - Meyer, Harry M.

AU - Luo, Huimin

AU - Delmau, Lætitia H.

AU - Dai, Sheng

AU - Moyer, Bruce A.

PY - 2014/1/1

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N2 - This study demonstrates a direct electrodeposition of UO2 at a Pt cathode from a solution of uranyl bis(trifluoromethanesulfonyl)imide [UO 2(NTf2)2)] in a bulk room-temperature ionic liquid (RTIL), 1-ethyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide (EMIM+NTf2-). Cyclic voltammetry (CV) studies revealed two reduction waves corresponding to the conversion of uranium(VI) to uranium(IV), and a mechanism for the overall electroreduction is proposed. A controlled-potential experiment was performed, holding the reduction potential at-1.0 V for 24 h to obtain a brown-black deposit of UO2 on the Pt cathode. The Faradaic efficiency of the reduction process was determined to be >80%. The UO2 deposit was characterized by powder X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS).

AB - This study demonstrates a direct electrodeposition of UO2 at a Pt cathode from a solution of uranyl bis(trifluoromethanesulfonyl)imide [UO 2(NTf2)2)] in a bulk room-temperature ionic liquid (RTIL), 1-ethyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide (EMIM+NTf2-). Cyclic voltammetry (CV) studies revealed two reduction waves corresponding to the conversion of uranium(VI) to uranium(IV), and a mechanism for the overall electroreduction is proposed. A controlled-potential experiment was performed, holding the reduction potential at-1.0 V for 24 h to obtain a brown-black deposit of UO2 on the Pt cathode. The Faradaic efficiency of the reduction process was determined to be >80%. The UO2 deposit was characterized by powder X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS).

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JF - Electrochimica Acta

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