Electrochemical Deposition with Redox Replacement of Lanthanum with Uranium in Molten LiCl-KCl

Eakin, Jeffrey Allen; Molina, Daniel E.; Guo, Xiaofeng; Beyenal, Haluk; Ivory, Cornelius F.

doi:10.1149/1945-7111/acc09c

Electrochemical Deposition with Redox Replacement of Lanthanum with Uranium in Molten LiCl-KCl

Journal Article · Thu Mar 09 23:00:00 EST 2023 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/1945-7111/acc09c· OSTI ID:1960013

^[1]; ^[2]; Guo, Xiaofeng ^[2]; ^[2]; Ivory, Cornelius F. ^[2]

Washington State Univ., Pullman, WA (United States); University of Notre Dame
Washington State Univ., Pullman, WA (United States)

Electrochemical recovery of dilute concentrations of actinides from spent nuclear fuel would reduce the longevity of storing high-level nuclear waste. Electrochemical deposition with redox replacement (EDRR) is used in a molten salt medium for the selective electrochemical recovery of uranium in the presence of excess concentrations of lanthanum. In each EDRR cycle, after a short electrodeposition pulse, the deposited lanthanum is spontaneously replaced by uranium at open circuit. After repeated cycles, uranium metal was obtained on a tungsten electrode immersed in LiCl-KCl melt that contained 1 wt.% lanthanum chloride – 0.15 wt.% uranium⁴⁺ chloride. Here, scanning electron microscopy and energy dispersive X-ray spectroscopy analysis revealed uranium particles approximately 0.5 - 1 μm with well-defined rectangular shapes; and with 20 – 60 times more uranium recovered on the surface of the electrode than lanthanum.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Notre Dame, IN (United States)

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

Grant/Contract Number:: NA0003763

OSTI ID:: 1960013

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 3 Vol. 170; ISSN 0013-4651

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

References (43)

Benefits of using multiple Raman laser wavelengths for characterizing defects in a UO ₂ matrix Karcher, Samuel; Mohun, Ritesh; Olds, Travis Journal of Raman Spectroscopy, Vol. 53, Issue 5 https://doi.org/10.1002/jrs.6321	journal	February 2022
Chlorine corrosion of graphites and technical carbons - I. Reaction with gaseous chlorine at elevated temperatures Wendt, H.; Dermeik, S.; Ziogas, A. Materials and Corrosion/Werkstoffe und Korrosion, Vol. 41, Issue 8 https://doi.org/10.1002/maco.19900410803	journal	August 1990
Exhaustive electrolysis for recovery of actinides from molten LiCl–KCl using solid aluminium cathodes Souček, P.; Malmbeck, R.; Mendes, E. Journal of Radioanalytical and Nuclear Chemistry, Vol. 286, Issue 3 https://doi.org/10.1007/s10967-010-0739-6	journal	August 2010
Electrochemical separation of uranium and cerium in molten LiCl–KCl Wang, C. S.; Liu, Y.; He, H. Journal of Radioanalytical and Nuclear Chemistry, Vol. 298, Issue 1 https://doi.org/10.1007/s10967-013-2506-y	journal	April 2013
Pyrochemical extraction analysis of an immiscible molten LiCl–KCl/Cd system Kim, K. R.; Ahn, D. H.; Shim, J. B. Journal of Radioanalytical and Nuclear Chemistry, Vol. 304, Issue 1 https://doi.org/10.1007/s10967-014-3824-4	journal	November 2014
Electrochemical behavior and electrowinning of uranium(IV) from FLiNaK molten salt Jiang, Feng; Huang, Wei; Zheng, Haiyang Journal of Radioanalytical and Nuclear Chemistry, Vol. 311, Issue 3 https://doi.org/10.1007/s10967-016-5160-3	journal	January 2017
Pyrolytic boron nitride coated graphite as a container of reference electrodes for molten fluorides Kontoyannis, Christos G. Electrochimica Acta, Vol. 40, Issue 15 https://doi.org/10.1016/0013-4686(94)00364-7	journal	October 1995
Evaluation of stainless steel–zirconium alloys as high-level nuclear waste forms McDeavitt, S. M.; Abraham, D. P.; Park, J. Y. Journal of Nuclear Materials, Vol. 257, Issue 1 https://doi.org/10.1016/S0022-3115(98)00433-4	journal	September 1998
Vaporization study on lanthanum–uranium and cerium–uranium alloys by mass-spectrometric method Shoji, Yoshiyuki; Matsui, Tsuneo; Nakamura, Kinya Journal of Nuclear Materials, Vol. 265, Issue 1-2 https://doi.org/10.1016/S0022-3115(98)00511-X	journal	February 1999
Pyrochemical Reprocessing of Spent Fuel by Electrochemical Techniques Using Solid Aluminium Cathodes Souček, P.; Malmbeck, R.; Nourry, C. Energy Procedia, Vol. 7 https://doi.org/10.1016/j.egypro.2011.06.052	journal	January 2011
Electrochemical behaviour of LaCl3 at tungsten and aluminium cathodes in LiCl–KCl eutectic melt Vandarkuzhali, S.; Gogoi, Nibedita; Ghosh, Suddhasattwa Electrochimica Acta, Vol. 59 https://doi.org/10.1016/j.electacta.2011.10.062	journal	January 2012
Electrochemical separation of Th from ThO2 and Eu2O3 assisted by AlCl3 in molten LiCl–KCl Liu, Ya-Lan; Yan, Yong-De; Han, Wei Electrochimica Acta, Vol. 114 https://doi.org/10.1016/j.electacta.2013.09.154	journal	December 2013
Thermodynamics of separation of uranium from neodymium between the gallium-indium liquid alloy and the LiCl-KCl molten salt phases Smolenski, V.; Novoselova, A.; Osipenko, A. Electrochimica Acta, Vol. 133 https://doi.org/10.1016/j.electacta.2014.04.042	journal	July 2014
Investigation on the electrochemical behavior of neodymium chloride at W, Al and Cd electrodes in molten LiCl-KCl eutectic Vandarkuzhali, S.; Chandra, Manish; Ghosh, Suddhasattwa Electrochimica Acta, Vol. 145 https://doi.org/10.1016/j.electacta.2014.08.069	journal	November 2014
Investigation of the effects of uranium(III)-chloride concentration on voltammetry in molten LiCl-KCl eutectic with a glass sealed tungsten electrode Rappleye, Devin; Teaford, Kevin; Simpson, Michael F. Electrochimica Acta, Vol. 219 https://doi.org/10.1016/j.electacta.2016.10.075	journal	November 2016
Direct separation of uranium from lanthanides (La, Nd, Ce, Sm) in oxide mixture in LiCl-KCl eutectic melt Liu, Yalan; Liu, Kui; Luo, Lixia Electrochimica Acta, Vol. 275 https://doi.org/10.1016/j.electacta.2018.04.140	journal	June 2018
Electrochemical recovery of minor concentrations of gold from cyanide-free cupric chloride leaching solutions Korolev, Ivan; Altınkaya, Pelin; Halli, Petteri Journal of Cleaner Production, Vol. 186 https://doi.org/10.1016/j.jclepro.2018.03.177	journal	June 2018
A direct synthesis of platinum/nickel co-catalysts on titanium dioxide nanotube surface from hydrometallurgical-type process streams Yliniemi, Kirsi; Nguyen, Nhat Truong; Mohajernia, Shiva Journal of Cleaner Production, Vol. 201 https://doi.org/10.1016/j.jclepro.2018.08.022	journal	November 2018
Separation of actinides from irradiated An–Zr based fuel by electrorefining on solid aluminium cathodes in molten LiCl–KCl Souček, P.; Murakami, T.; Claux, B. Journal of Nuclear Materials, Vol. 459 https://doi.org/10.1016/j.jnucmat.2014.12.103	journal	April 2015
Actinides recovery from irradiated metallic fuel in LiCl–KCl melts Murakami, T.; Rodrigues, A.; Ougier, M. Journal of Nuclear Materials, Vol. 466 https://doi.org/10.1016/j.jnucmat.2015.08.045	journal	November 2015
Transient modeling of spent nuclear fuel electrorefining with liquid metal electrode Seo, Seungjin; Choi, Sungyeol; Park, Byung Gi Journal of Nuclear Materials, Vol. 491 https://doi.org/10.1016/j.jnucmat.2017.04.053	journal	August 2017
Galvanic reduction of uranium(III) chloride from LiCl-KCl eutectic salt using gadolinium metal Bagri, Prashant; Zhang, Chao; Simpson, Michael F. Journal of Nuclear Materials, Vol. 493 https://doi.org/10.1016/j.jnucmat.2017.06.007	journal	September 2017
Relative impact of H2O and O2 in the oxidation of UO2 powders from 50 to 300 °C Donald, Scott B.; Davisson, M. Lee; Dai, Zurong Journal of Nuclear Materials, Vol. 496 https://doi.org/10.1016/j.jnucmat.2017.10.014	journal	December 2017
Optimization of UCl 3 and MgCl 2 separation from molten LiCl-KCl eutectic salt via galvanic drawdown with sacrificial Gd anode Bagri, Prashant; Ong, Joshua; Zhang, Chao Journal of Nuclear Materials, Vol. 505 https://doi.org/10.1016/j.jnucmat.2018.04.011	journal	July 2018
Oxidation and anion lattice defect signatures of hypostoichiometric lanthanide-doped UO2 Olds, Travis A.; Karcher, Samuel E.; Kriegsman, Kyle W. Journal of Nuclear Materials, Vol. 530 https://doi.org/10.1016/j.jnucmat.2019.151959	journal	March 2020
Effect of added gadolinium oxide on the thermal air oxidation of uranium dioxide Scheele, Randall D.; Hanson, Brady D.; Casella, Andrew M. Journal of Nuclear Materials, Vol. 552 https://doi.org/10.1016/j.jnucmat.2021.153008	journal	August 2021
Separation of uranium from lanthanides (La, Sm) with sacrificial Li anode in LiCl-KCl eutectic salt Wang, Dong-Dong; Liu, Ya-Lan; Yang, Da-Wei Separation and Purification Technology, Vol. 292 https://doi.org/10.1016/j.seppur.2022.121025	journal	July 2022
Targeted surface modification of Cu/Zn/Ag coatings and Ag/Cu particles based on sacrificial element selection by electrodeposition and redox replacement Wang, Zulin; Yliniemi, Kirsi; Wilson, Benjamin P. Surface and Coatings Technology, Vol. 441 https://doi.org/10.1016/j.surfcoat.2022.128531	journal	July 2022
Leakless, Bipolar Reference Electrodes: Fabrication, Performance, and Miniaturization Walker, Nicole L.; Dick, Jeffrey E. Analytical Chemistry, Vol. 93, Issue 29 https://doi.org/10.1021/acs.analchem.1c00675	journal	July 2021
Platinum Recovery from Industrial Process Solutions by Electrodeposition–Redox Replacement Halli, Petteri; Heikkinen, Joonas J.; Elomaa, Heini ACS Sustainable Chemistry & Engineering, Vol. 6, Issue 11 https://doi.org/10.1021/acssuschemeng.8b03224	journal	September 2018
Convenient Synthesis, Structure, and Reactivity of (C ₅ Me ₅ )U(CH ₂ C ₆ H ₅ ) ₃ : A Simple Strategy for the Preparation of Monopentamethylcyclopentadienyl Uranium(IV) Complexes Kiplinger, Jaqueline L.; Morris, David E.; Scott, Brian L. Organometallics, Vol. 21, Issue 26 https://doi.org/10.1021/om0206610	journal	December 2002
Contributions to the Ohmic Drop in the Electrolysis of ZnCl₂in a Molten Chloride Electrolyte Lans, S. C.; Sandwijk, A. Van; Reuter, M. A. Journal of Applied Electrochemistry, Vol. 34, Issue 10 https://doi.org/10.1023/B:JACH.0000042678.49784.be	journal	October 2004
Ultrastructural Characterization of the Lower Motor System in a Mouse Model of Krabbe Disease Cappello, Valentina; Marchetti, Laura; Parlanti, Paola Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/s41598-016-0001-8	journal	December 2016
Progress in Electrometallurgical Treatment of Spent Nuclear Fuel Benedict, Robert; Goff, Michael; Teske, Gregory Journal of Nuclear Science and Technology, Vol. 39, Issue sup3 https://doi.org/10.1080/00223131.2002.10875575	journal	November 2002
Single-Stage Extraction Test with Continuous Flow of Molten LiCl-KCl Salt and Liquid Cd for Pyro-Reprocessing of Metal FBR Fuel Kinoshita, Kensuke; Tsukada, Takeshi; Ogata, Takanari Journal of Nuclear Science and Technology, Vol. 44, Issue 12 https://doi.org/10.1080/18811248.2007.9711406	journal	December 2007
Behavior of U-Zr Alloy Containing Simulated Fission Products during Anodic Dissolution in Molten Chloride Electrolyte Iizuka, Masatoshi; Omori, Takashi; Tsukada, Takeshi Journal of Nuclear Science and Technology, Vol. 47, Issue 3 https://doi.org/10.1080/18811248.2010.9711951	journal	March 2010
Electrochemical Behavior and Some Thermodynamic Properties of UCl[sub 4] and UCl[sub 3] Dissolved in a LiCl-KCl Eutectic Melt Kuznetsov, S. A.; Hayashi, H.; Minato, K. Journal of The Electrochemical Society, Vol. 152, Issue 4 https://doi.org/10.1149/1.1864532	journal	January 2005
Flow Injection Electrochemical Quartz Crystal Microbalance with ICP-OES Detection: Recovery of Silver by Electrodeposition with Redox Replacement in a Flow Cell Molina, Daniel E.; Wall, Nathalie; Beyenal, Haluk Journal of The Electrochemical Society, Vol. 168, Issue 5 https://doi.org/10.1149/1945-7111/abfcdd	journal	May 2021
Electrochemical Behavior of Sm(III) and Electrodeposition of Samarium from 1-Butyl-1-Methylpyrrolidinium Dicyanamide Ionic Liquid Andrew, Chrysanthus; Murugesan, Chandran; Jayakumar, Mani Journal of The Electrochemical Society, Vol. 169, Issue 2 https://doi.org/10.1149/1945-7111/ac4f76	journal	February 2022
Evaluation of the Electroextractions of Ce and Nd from LiCl-KCl Molten Salt Using Liquid Ga Electrode Liu, Kui; Liu, Ya-Lan; Chai, Zhi-Fang Journal of The Electrochemical Society, Vol. 164, Issue 4 https://doi.org/10.1149/2.0511704jes	journal	January 2017
The Future of Nuclear Energy: Electrochemical Reprocessing of Fuel Takes Center Stage Kersten, Bethany; Hawthorne, Krista; Williamson, Mark The Electrochemical Society Interface, Vol. 30, Issue 3 https://doi.org/10.1149/2.F06213F	journal	September 2021
A Description of the Ceramic Waste Form Production Process from the Demonstration Phase of the Electrometallurgical Treatment of EBR-II Spent Fuel Simpson, Michael F.; Goff, K. Michael; Johnson, Stephen G. Nuclear Technology, Vol. 134, Issue 3 https://doi.org/10.13182/NT01-A3200	journal	June 2001
SEPARATION OF CsCl FROM LiCl-CsCl MOLTEN SALT BY COLD FINGER MELT CRYSTALLIZATION Versey, Joshua R.; Phongikaroon, Supathorn; Simpson, Michael F. Nuclear Engineering and Technology, Vol. 46, Issue 3 https://doi.org/10.5516/NET.06.2013.082	journal	June 2014

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