Non-Aqueous Electrochemical Fluorination of Used Nuclear Fuel as an Advanced Separation Process
Abstract
Development of efficient and environmentally benign methods to reprocess used nuclear fuel (UNF) will enable technologies for a nuclear renaissance. Electrochemical and fluorination methods for reprocessing UNF have been proposed, but combinations of electrochemical and fluorination methods have not been investigated. Electrochemical fluorination may reduce waste volumes compared to the main large-scale aqueous methods for processing used nuclear fuel. A non-aqueous electrochemical fluorination reprocessing method has been developed and demonstrated that enables gas phase uranium recovery while allowing for potential control of the reaction using a single process. Thermodynamic modeling showed a galvanic reaction between UNF and a fluorinating agent, such as NF3, in a molten fluoride electrolyte was possible and could selectively fluorinate U to UF6. To verify the model results, a reactor system for electrochemical fluorination was constructed along with vessels for product collection and analysis. Initial trials of the electrochemical reaction were performed and characterized by several electrochemical methods. The electrochemical oxidation of U using NF3 as an oxidizing agent was demonstrated and UF6 as a reaction product was detected.
- Authors:
-
[1];
[1]
- Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
- Publication Date:
- Research Org.:
- Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
- Sponsoring Org.:
- USDOE; SRNL Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1512421
- Report Number(s):
- SRNL-STI-2019-00219
Journal ID: ISSN 0013-4651
- Grant/Contract Number:
- AC09-08SR22470
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the Electrochemical Society
- Additional Journal Information:
- Journal Volume: 166; Journal Issue: 8; Journal ID: ISSN 0013-4651
- Publisher:
- The Electrochemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; electrochemical engineering; molten salts; FLiNaK; galvanic cell; uranium hexafluoride
Citation Formats
Martínez-Rodríguez, Michael J., Olson, Luke C., Gray, Joshua R., and García-Díaz, Brenda L. Non-Aqueous Electrochemical Fluorination of Used Nuclear Fuel as an Advanced Separation Process. United States: N. p., 2019.
Web. doi:10.1149/2.0261908jes.
Martínez-Rodríguez, Michael J., Olson, Luke C., Gray, Joshua R., & García-Díaz, Brenda L. Non-Aqueous Electrochemical Fluorination of Used Nuclear Fuel as an Advanced Separation Process. United States. https://doi.org/10.1149/2.0261908jes
Martínez-Rodríguez, Michael J., Olson, Luke C., Gray, Joshua R., and García-Díaz, Brenda L. Mon .
"Non-Aqueous Electrochemical Fluorination of Used Nuclear Fuel as an Advanced Separation Process". United States. https://doi.org/10.1149/2.0261908jes. https://www.osti.gov/servlets/purl/1512421.
@article{osti_1512421,
title = {Non-Aqueous Electrochemical Fluorination of Used Nuclear Fuel as an Advanced Separation Process},
author = {Martínez-Rodríguez, Michael J. and Olson, Luke C. and Gray, Joshua R. and García-Díaz, Brenda L.},
abstractNote = {Development of efficient and environmentally benign methods to reprocess used nuclear fuel (UNF) will enable technologies for a nuclear renaissance. Electrochemical and fluorination methods for reprocessing UNF have been proposed, but combinations of electrochemical and fluorination methods have not been investigated. Electrochemical fluorination may reduce waste volumes compared to the main large-scale aqueous methods for processing used nuclear fuel. A non-aqueous electrochemical fluorination reprocessing method has been developed and demonstrated that enables gas phase uranium recovery while allowing for potential control of the reaction using a single process. Thermodynamic modeling showed a galvanic reaction between UNF and a fluorinating agent, such as NF3, in a molten fluoride electrolyte was possible and could selectively fluorinate U to UF6. To verify the model results, a reactor system for electrochemical fluorination was constructed along with vessels for product collection and analysis. Initial trials of the electrochemical reaction were performed and characterized by several electrochemical methods. The electrochemical oxidation of U using NF3 as an oxidizing agent was demonstrated and UF6 as a reaction product was detected.},
doi = {10.1149/2.0261908jes},
journal = {Journal of the Electrochemical Society},
number = 8,
volume = 166,
place = {United States},
year = {Mon Apr 29 00:00:00 EDT 2019},
month = {Mon Apr 29 00:00:00 EDT 2019}
}
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