Tandem dissolution of UO3 in amide-based acidic ionic liquid and in situ electrodeposition of UO2 with regeneration of the ionic liquid: a closed cycle
Abstract
A closed cycle is demonstrated for the tandem dissolution and electroreduction of UO3 to UO2 with regeneration of the acidic ionic liquid. The dissolution is achieved by use of the acidic ionic liquid N,N-dimethylacetimidium bis(trifluoromethanesulfonimide) in 1-ethyl-3-methylimidazolium bis(trifluoromethanesulfonimide) serving as the diluent. Bulk electrolysis performed at 1.0 V vs. Ag reference yields a dark brown-black uranium deposit (UO2) on the cathode. Anodic oxidation of water in the presence of dimethylacetamide regenerates the acidic ionic liquid. We have demonstrated the individual steps in the cycle together with a sequential dissolution, electroreduction, and regeneration cycle.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Energy and Transportation Science Division
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies (NE-5); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1286700
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Dalton Transactions
- Additional Journal Information:
- Journal Volume: 45; Journal Issue: 25; Journal ID: ISSN 1477-9226
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Acidic ionic liquids; Uranium Dioxide; Dissolution; electrodeposition
Citation Formats
Wanigasekara, Eranda, Freiderich, John W., Sun, Xiao-Guang, Meisner, Roberta A., Luo, Huimin, Delmau, Lætitia H., Dai, Sheng, and Moyer, Bruce A. Tandem dissolution of UO3 in amide-based acidic ionic liquid and in situ electrodeposition of UO2 with regeneration of the ionic liquid: a closed cycle. United States: N. p., 2016.
Web. doi:10.1039/C6DT00873A.
Wanigasekara, Eranda, Freiderich, John W., Sun, Xiao-Guang, Meisner, Roberta A., Luo, Huimin, Delmau, Lætitia H., Dai, Sheng, & Moyer, Bruce A. Tandem dissolution of UO3 in amide-based acidic ionic liquid and in situ electrodeposition of UO2 with regeneration of the ionic liquid: a closed cycle. United States. https://doi.org/10.1039/C6DT00873A
Wanigasekara, Eranda, Freiderich, John W., Sun, Xiao-Guang, Meisner, Roberta A., Luo, Huimin, Delmau, Lætitia H., Dai, Sheng, and Moyer, Bruce A. Thu .
"Tandem dissolution of UO3 in amide-based acidic ionic liquid and in situ electrodeposition of UO2 with regeneration of the ionic liquid: a closed cycle". United States. https://doi.org/10.1039/C6DT00873A. https://www.osti.gov/servlets/purl/1286700.
@article{osti_1286700,
title = {Tandem dissolution of UO3 in amide-based acidic ionic liquid and in situ electrodeposition of UO2 with regeneration of the ionic liquid: a closed cycle},
author = {Wanigasekara, Eranda and Freiderich, John W. and Sun, Xiao-Guang and Meisner, Roberta A. and Luo, Huimin and Delmau, Lætitia H. and Dai, Sheng and Moyer, Bruce A.},
abstractNote = {A closed cycle is demonstrated for the tandem dissolution and electroreduction of UO3 to UO2 with regeneration of the acidic ionic liquid. The dissolution is achieved by use of the acidic ionic liquid N,N-dimethylacetimidium bis(trifluoromethanesulfonimide) in 1-ethyl-3-methylimidazolium bis(trifluoromethanesulfonimide) serving as the diluent. Bulk electrolysis performed at 1.0 V vs. Ag reference yields a dark brown-black uranium deposit (UO2) on the cathode. Anodic oxidation of water in the presence of dimethylacetamide regenerates the acidic ionic liquid. We have demonstrated the individual steps in the cycle together with a sequential dissolution, electroreduction, and regeneration cycle.},
doi = {10.1039/C6DT00873A},
journal = {Dalton Transactions},
number = 25,
volume = 45,
place = {United States},
year = {Thu May 19 00:00:00 EDT 2016},
month = {Thu May 19 00:00:00 EDT 2016}
}
Web of Science
Works referenced in this record:
Room-temperature ionic liquids: new solvents for f -element separations and associated solution chemistry
journal, February 2003
- Visser, Ann E.; Rogers, Robin D.
- Journal of Solid State Chemistry, Vol. 171, Issue 1-2
Mechanisms of Metal Ion Transfer into Room-Temperature Ionic Liquids: The Role of Anion Exchange
journal, December 2003
- Jensen, Mark P.; Neuefeind, Jörg; Beitz, James V.
- Journal of the American Chemical Society, Vol. 125, Issue 50
Lanthanides and Actinides in Ionic Liquids
journal, June 2007
- Binnemans, Koen
- Chemical Reviews, Vol. 107, Issue 6
Electrodeposition of Nanocrystalline Metals and Alloys from Ionic Liquids
journal, July 2003
- Endres, Frank; Bukowski, Mirko; Hempelmann, Rolf
- Angewandte Chemie International Edition, Vol. 42, Issue 29
The Electrochemistry of Copper in a Room Temperature Acidic Chloroaluminate Melt
journal, June 1979
- Hussey, C. L.; King, L. A.; Carpio, R. A.
- Journal of The Electrochemical Society, Vol. 126, Issue 6
Reprocessing of spent nuclear waste using ionic liquids
journal, September 2010
- Ha, Sung Ho; Menchavez, Russel Navarro; Koo, Yoon-Mo
- Korean Journal of Chemical Engineering, Vol. 27, Issue 5
Effect of Process Variables During the Head-End Treatment of Spent Oxide Fuel
journal, May 2008
- Westphal, B. R.; Bateman, K. J.; Morgan, C. D.
- Nuclear Technology, Vol. 162, Issue 2
Fundamental Studies on Electrochemical Deposition of Lead from Lead Oxide in 2:1 Urea/Choline Chloride Ionic Liquids
journal, January 2014
- Yang, Haoxing; Reddy, Ramana G.
- Journal of The Electrochemical Society, Vol. 161, Issue 10
Task-Specific Ionic Liquid for Solubilizing Metal Oxides
journal, October 2006
- Nockemann, Peter; Thijs, Ben; Pittois, Stijn
- The Journal of Physical Chemistry B, Vol. 110, Issue 42
Zinc Electrodeposition from a Deep Eutectic System Containing Choline Chloride and Ethylene Glycol
journal, January 2010
- Whitehead, Adam H.; Pölzler, Matthias; Gollas, Bernhard
- Journal of The Electrochemical Society, Vol. 157, Issue 6
Dissolution of zinc oxide in a protic ionic liquid with the 1-methylimidazolium cation and electrodeposition of zinc from ZnO/ionic liquid and ZnO/ionic liquid–water mixtures
journal, September 2015
- Liu, Zhen; El Abedin, Sherif Zein; Endres, Frank
- Electrochemistry Communications, Vol. 58
Solvent Extraction of Sr 2+ and Cs + using Protic Amide-Based Ionic Liquids
journal, July 2010
- Luo, Huimin; Huang, Jing-Fang; Dai, Sheng
- Separation Science and Technology, Vol. 45, Issue 12-13
Physical Properties of Ionic Liquids: Database and Evaluation
journal, December 2006
- Zhang, Suojiang; Sun, Ning; He, Xuezhong
- Journal of Physical and Chemical Reference Data, Vol. 35, Issue 4, p. 1475-1517
Direct Electrodeposition of UO2 from Uranyl Bis(trifluoromethanesulfonyl)imide Dissolved in 1-Ethyl-3-methylimidazolium Bis(trifluoromethanesulfonyl)imide Room Temperature Ionic Liquid System
journal, January 2014
- Freiderich, John W.; Wanigasekara, Eranda; Sun, Xiao-Guang
- Electrochimica Acta, Vol. 115
Extraction of uranium (VI) by 1.1M tri-n-butylphosphate/ionic liquid and the feasibility of recovery by direct electrodeposition from organic phase
journal, January 2008
- Giridhar, P.; Venkatesan, K. A.; Subramaniam, S.
- Journal of Alloys and Compounds, Vol. 448, Issue 1-2
Electrodeposition of metallic uranium at near ambient conditions from room temperature ionic liquid
journal, January 2011
- Jagadeeswara Rao, Ch.; Venkatesan, K. A.; Nagarajan, K.
- Journal of Nuclear Materials, Vol. 408, Issue 1
Determination of Successive Complexation Constants in an Ionic Liquid: Complexation of UO 2 2+ with NO 3 − in C 4 -mimTf 2 N Studied by UV−Vis Spectroscopy
journal, April 2010
- Georg, Sylvia; Billard, Isabelle; Ouadi, Ali
- The Journal of Physical Chemistry B, Vol. 114, Issue 12
Dissolution of UO2, UO3 and of some lanthanide oxides in BumimTf2N: effect of acid and water and formation of UO2(NO3)3–
journal, January 2007
- Billard, Isabelle; Gaillard, Clotilde; Hennig, Christoph
- Dalton Transactions, Issue 37
Electrochemistry of soluble UO22+ from the direct dissolution of UO2CO3 in acidic ionic liquid containing water
journal, March 2013
- Pemberton, Wendy J.; Droessler, Janelle E.; Kinyanjui, John M.
- Electrochimica Acta, Vol. 93, p. 264-271
Electrochemical behavior of uranyl in ionic liquid 1-butyl-3-methylimidazolium chloride mixture with water
journal, May 2014
- Tan, Xu-Feng; Yuan, Li-Yong; Nie, Chang-Ming
- Journal of Radioanalytical and Nuclear Chemistry, Vol. 302, Issue 1
Effect of alkyl chain length of tri- n -alkyl phosphate extractants on the electrochemical behaviour of U(VI) in ionic liquid medium
journal, June 2016
- Rama, R.; Rout, Alok; Venkatesan, K. A.
- Journal of Electroanalytical Chemistry, Vol. 771
Electrochemical Studies on [UO 2 (DMF) 5 ](CIO 4 ) 2 , UO 2 (acac) 2 DMF, and UO 2 (salen)DMF (DMF= N , N -dimethylformamide, acac=acetylacetonate, salen= N , N′-disalicylideneethylenediaminate) Complexes in DMF
journal, February 2002
- Kim, Seong-Yun; Tomiyasu, Hiroshi; Ikeda, Yasuhisa
- Journal of Nuclear Science and Technology, Vol. 39, Issue 2
Influence du solvant sur la reduction electrochimique du nitrate et de l'acetate d'uranyle
journal, January 1988
- Marouani, S.; Louati, A.; Gross, M.
- Electrochimica Acta, Vol. 33, Issue 1
Works referencing / citing this record:
Synthesis and Dissolution of Metal Oxides in Ionic Liquids and Deep Eutectic Solvents
journal, December 2019
- Richter, Janine; Ruck, Michael
- Molecules, Vol. 25, Issue 1