Closing the Nuclear Fuel Cycle with a Simplified Minor Actinide Lanthanide Separation Process (ALSEP) and Additive Manufacturing
Abstract
Expanded low-carbon baseload power production through the use of nuclear fission can be enabled by recycling long-lived actinide isotopes within the nuclear fuel cycle. This approach provides the benefits of a) more complete utilization of the energy potential of mined uranium, b) reduced footprint of nuclear geological repositories, and c) reduction in the radiotoxicity decay time for the disposed waste from one hundred thousand years to a few hundred years. A key step in achieving this goal is the separation of long-lived isotopes of americium and curium for recycle into fast reactors. To achieve this goal, a novel process was successfully demonstrated on a lab scale using a bank of 1.25-cm centrifugal contactors, fabricated by additive manufacturing, and a simulant containing the major fission products. Am and Cm were separated from the lanthanides with over 99.9% completion. The sum of the impurities of the Am/Cm product stream was found to be 3.2.10-3 g/L. The process performance was successfully validated using a genuine high burnup used nuclear fuel raffinate in a batch regime. Separation factors of nearly 100 for 154Eu over 241Am and were achieved. All these results indicate the process scalability to engineering scale.
- Authors:
-
[2];
[3];
[3];
- Univ. of Nevada, Las Vegas, NV (United States). Radiochemistry Program, Dept. of Chemistry and Biochemistry
- Argonne National Lab. (ANL), Argonne, IL (United States). Chemical and Fuel Cycle Technology Div.
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Nuclear Science Div.
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE)
- OSTI Identifier:
- 1575066
- Alternate Identifier(s):
- OSTI ID: 1708854
- Report Number(s):
- PNNL-SA-139206
Journal ID: ISSN 2045-2322; 153675; TRN: US2100310
- Grant/Contract Number:
- AC02-06CH11357; AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Scientific Reports
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2045-2322
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; fuel recycle, ALSEP, actinide separation
Citation Formats
Gelis, Artem V., Kozak, Peter, Breshears, Andrew T., Brown, M. Alex, Launiere, Cari, Campbell, Emily L., Hall, Gabriel B., Levitskaia, Tatiana G., Holfeltz, Vanessa E., and Lumetta, Gregg J. Closing the Nuclear Fuel Cycle with a Simplified Minor Actinide Lanthanide Separation Process (ALSEP) and Additive Manufacturing. United States: N. p., 2019.
Web. doi:10.1038/s41598-019-48619-x.
Gelis, Artem V., Kozak, Peter, Breshears, Andrew T., Brown, M. Alex, Launiere, Cari, Campbell, Emily L., Hall, Gabriel B., Levitskaia, Tatiana G., Holfeltz, Vanessa E., & Lumetta, Gregg J. Closing the Nuclear Fuel Cycle with a Simplified Minor Actinide Lanthanide Separation Process (ALSEP) and Additive Manufacturing. United States. https://doi.org/10.1038/s41598-019-48619-x
Gelis, Artem V., Kozak, Peter, Breshears, Andrew T., Brown, M. Alex, Launiere, Cari, Campbell, Emily L., Hall, Gabriel B., Levitskaia, Tatiana G., Holfeltz, Vanessa E., and Lumetta, Gregg J. Fri .
"Closing the Nuclear Fuel Cycle with a Simplified Minor Actinide Lanthanide Separation Process (ALSEP) and Additive Manufacturing". United States. https://doi.org/10.1038/s41598-019-48619-x. https://www.osti.gov/servlets/purl/1575066.
@article{osti_1575066,
title = {Closing the Nuclear Fuel Cycle with a Simplified Minor Actinide Lanthanide Separation Process (ALSEP) and Additive Manufacturing},
author = {Gelis, Artem V. and Kozak, Peter and Breshears, Andrew T. and Brown, M. Alex and Launiere, Cari and Campbell, Emily L. and Hall, Gabriel B. and Levitskaia, Tatiana G. and Holfeltz, Vanessa E. and Lumetta, Gregg J.},
abstractNote = {Expanded low-carbon baseload power production through the use of nuclear fission can be enabled by recycling long-lived actinide isotopes within the nuclear fuel cycle. This approach provides the benefits of a) more complete utilization of the energy potential of mined uranium, b) reduced footprint of nuclear geological repositories, and c) reduction in the radiotoxicity decay time for the disposed waste from one hundred thousand years to a few hundred years. A key step in achieving this goal is the separation of long-lived isotopes of americium and curium for recycle into fast reactors. To achieve this goal, a novel process was successfully demonstrated on a lab scale using a bank of 1.25-cm centrifugal contactors, fabricated by additive manufacturing, and a simulant containing the major fission products. Am and Cm were separated from the lanthanides with over 99.9% completion. The sum of the impurities of the Am/Cm product stream was found to be 3.2.10-3 g/L. The process performance was successfully validated using a genuine high burnup used nuclear fuel raffinate in a batch regime. Separation factors of nearly 100 for 154Eu over 241Am and were achieved. All these results indicate the process scalability to engineering scale.},
doi = {10.1038/s41598-019-48619-x},
journal = {Scientific Reports},
number = 1,
volume = 9,
place = {United States},
year = {2019},
month = {9}
}
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Works referenced in this record:
Nuclear safety regulation in the post-Fukushima era
journal, May 2017
- Lyman, Edwin; Schoeppner, Michael; von Hippel, Frank
- Science, Vol. 356, Issue 6340
Toward Mechanistic Understanding of Nuclear Reprocessing Chemistries by Quantifying Lanthanide Solvent Extraction Kinetics via Microfluidics with Constant Interfacial Area and Rapid Mixing
journal, October 2011
- Nichols, Kevin P.; Pompano, Rebecca R.; Li, Liang
- Journal of the American Chemical Society, Vol. 133, Issue 39
Actinide Lanthanide Separation Process—ALSEP
journal, January 2014
- Gelis, Artem V.; Lumetta, Gregg J.
- Industrial & Engineering Chemistry Research, Vol. 53, Issue 4
The Actinide-Lanthanide Separation Concept
journal, May 2014
- Lumetta, Gregg J.; Gelis, Artem V.; Carter, Jennifer C.
- Solvent Extraction and Ion Exchange, Vol. 32, Issue 4
ORIGEN2: A Versatile Computer Code for Calculating the Nuclide Compositions and Characteristics of Nuclear Materials
journal, September 1983
- Croff, Allen G.
- Nuclear Technology, Vol. 62, Issue 3
Kinetics and Mechanism of the Interfacial Mass Transfer of Eu(III) in the System: Bis(2-ethylhexyl)phosphoric Acid, n -Dodecane-NaCl, Lactic Acid, Polyaminocarboxylic Acid, Water
journal, May 1982
- Danesi, P. R.; Cianetti, C.
- Separation Science and Technology, Vol. 17, Issue 7
High Precision Droplet-Based Microfluidic Determination of Americium(III) and Lanthanide(III) Solvent Extraction Separation Kinetics
journal, February 2016
- Launiere, C. A.; Gelis, A. V.
- Industrial & Engineering Chemistry Research, Vol. 55, Issue 7
The Chemistry of TALSPEAK: A Review of the Science
journal, December 2014
- Nash, Kenneth L.
- Solvent Extraction and Ion Exchange, Vol. 33, Issue 1
Extraction behaviour of actinides and lanthanides in TALSPEAK, TRUEX and NPEX processes of UREX+
journal, January 2009
- Gelis, A. V.; Vandegrift, Georg F.; Bakel, Allen
- Radiochimica Acta, Vol. 97, Issue 4-5
Stability constants for europium(III) complexes with substituted methane diphosphonic acids in acid solutions
journal, March 1990
- Nash, K. L.; Horwitz, E. P.
- Inorganica Chimica Acta, Vol. 169, Issue 2
The EURO-GANEX Process: Current Status of Flowsheet Development and Process Safety Studies
journal, January 2016
- Taylor, Robin; Carrott, Mike; Galan, Hitos
- Procedia Chemistry, Vol. 21
Effect of HEH[EHP] impurities on the ALSEP solvent extraction process
journal, December 2017
- Holfeltz, Vanessa E.; Campbell, Emily L.; Peterman, Dean R.
- Solvent Extraction and Ion Exchange, Vol. 36, Issue 1
Time-Dependent Implementation of Argonne’s Model for Universal Solvent Extraction
journal, September 2012
- Frey, Kurt; Krebs, John F.; Pereira, Candido
- Industrial & Engineering Chemistry Research, Vol. 51, Issue 40
Futuristic back-end of the nuclear fuel cycle with the partitioning of minor actinides
journal, October 2007
- Madic, C.; Boullis, B.; Baron, P.
- Journal of Alloys and Compounds, Vol. 444-445
Use of Soft Heterocyclic N-Donor Ligands To Separate Actinides and Lanthanides
journal, June 2012
- Hudson, Michael J.; Harwood, Laurence M.; Laventine, Dominic M.
- Inorganic Chemistry, Vol. 52, Issue 7
Use of Polyaminocarboxylic Acids as Hydrophilic Masking Agents for Fission Products in Actinide Partitioning Processes
journal, November 2012
- Sypula, Michal; Wilden, Andreas; Schreinemachers, Christian
- Solvent Extraction and Ion Exchange, Vol. 30, Issue 7
Alternatives to HDEHP and DTPA for Simplified TALSPEAK Separations
journal, June 2011
- Braley, Jenifer C.; Grimes, Travis S.; Nash, Kenneth L.
- Industrial & Engineering Chemistry Research, Vol. 51, Issue 2
Speciation of Select f -Elements with Lipophilic Phosphorus Acids and Diglycol Amides in the ALSEP Backward-Extraction Regime
journal, October 2017
- Gullekson, Brian J.; Brown, M. Alex; Paulenova, Alena
- Industrial & Engineering Chemistry Research, Vol. 56, Issue 42
Accomplishing Equilibrium in ALSEP: Demonstrations of Modified Process Chemistry on 3-D Printed Enhanced Annular Centrifugal Contactors
journal, January 2016
- Brown, M. Alex; Wardle, Kent E.; Lumetta, Gregg
- Procedia Chemistry, Vol. 21
Review Article: A Review of the Development and Operational Characteristics of the TALSPEAK Process
journal, October 2007
- Nilsson, Mikael; Nash, Kenneth L.
- Solvent Extraction and Ion Exchange, Vol. 25, Issue 6
Comparison of Covalency in the Complexes of Trivalent Actinide and Lanthanide Cations
journal, August 2002
- Jensen, Mark P.; Bond, Andrew H.
- Journal of the American Chemical Society, Vol. 124, Issue 33
The EURO-GANEX Process: Current Status of Flowsheet Development and Process Safety Studies
text, January 2016
- Taylor, Robin; Carrott, Mike; Galan, Hitos
- Karlsruhe
Effect of HEH[EHP] impurities on the ALSEP solvent extraction process [Supplemental Data]
figure, December 2017
- Holfeltz, Vanessa; Campbell, Emily; Peterman, Dean
- figshare-Supplementary information for journal article at DOI: 10.1080/07366299.2017.1412111, 1 PDF file (302.27 kB)