Criticality concerns of a group actinide co-crystallization separations approach to used nuclear fuel recycling

Kitcher, Evans D.; Burns, Jonathan D.

doi:10.1016/j.anucene.2018.02.006

Title: Criticality concerns of a group actinide co-crystallization separations approach to used nuclear fuel recycling

Abstract

We report the co-crystallization of hexavalent actinides with uranyl nitrate hexahydrate has been established as a viable approach to achieving group actinide separation in used nuclear fuel recycle while avoiding the difficulties associated with the solvent-extraction process altogether. A preliminary neutronics safety analysis has been performed to alleviate criticality concerns associated with this group hexavalent actinide co-crystallization approach. The basic uranyl nitrate hexahydrate material compositions used are representative of used fuel found at commercial pressurized water reactors all around the U.S. This material is subsequently doped with various percentages of either typical reactor grade plutonium or with the total transuranic vector, replacing the uranium atoms in the crystal lattice structure. Infinite and effective neutron multiplication factors were calculated using the state-of-the-art Monte Carlo neutron transport code MCNP in a variety of plausible material configurations, assuming an acceptable safety limit for criticality to be an effective neutron multiplication factor less than 0.95. The results indicate that the crystal structures form a very subcritical intrinsic geometry even with six water molecules being incorporated into the crystal structure. In conclusion, the results of this research suggest that significant opportunity exists for the safe transfer of the group actinide separation approach from a laboratorymore » to an operational scale.« less

Authors:

Kitcher, Evans D. ^[1];

^[1]

Texas A & M Univ., College Station, TX (United States). Center for Nuclear Security Science & Policy Initiatives, Department of Nuclear Engineering

Publication Date:: Thu Feb 22 00:00:00 EST 2018

Research Org.:: Texas A & M Univ., College Station, TX (United States)

Sponsoring Org.:: USDOE Office of Nuclear Energy (NE)

OSTI Identifier:: 1481880

Grant/Contract Number:: NE0008653; AC0500OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Annals of Nuclear Energy (Oxford)

Additional Journal Information:: Journal Name: Annals of Nuclear Energy (Oxford); Journal Volume: 115; Journal Issue: C; Journal ID: ISSN 0306-4549

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; Nuclear criticality safety; Actinides; MCNP; Reprocessing; Used nuclear fuel

Citation Formats


                    Kitcher, Evans D., and Burns, Jonathan D. Criticality concerns of a group actinide co-crystallization separations approach to used nuclear fuel recycling.  United States: N. p., 2018. 
Web.  doi:10.1016/j.anucene.2018.02.006.

Copy to clipboard


                    Kitcher, Evans D., & Burns, Jonathan D. Criticality concerns of a group actinide co-crystallization separations approach to used nuclear fuel recycling.  United States.  https://doi.org/10.1016/j.anucene.2018.02.006

Copy to clipboard


                    Kitcher, Evans D., and Burns, Jonathan D. Thu .  
"Criticality concerns of a group actinide co-crystallization separations approach to used nuclear fuel recycling".  United States.  https://doi.org/10.1016/j.anucene.2018.02.006.  https://www.osti.gov/servlets/purl/1481880.

Copy to clipboard


                    
@article{osti_1481880,

  title        = {Criticality concerns of a group actinide co-crystallization separations approach to used nuclear fuel recycling},

  author       = {Kitcher, Evans D. and Burns, Jonathan D.},

  abstractNote = {We report the co-crystallization of hexavalent actinides with uranyl nitrate hexahydrate has been established as a viable approach to achieving group actinide separation in used nuclear fuel recycle while avoiding the difficulties associated with the solvent-extraction process altogether. A preliminary neutronics safety analysis has been performed to alleviate criticality concerns associated with this group hexavalent actinide co-crystallization approach. The basic uranyl nitrate hexahydrate material compositions used are representative of used fuel found at commercial pressurized water reactors all around the U.S. This material is subsequently doped with various percentages of either typical reactor grade plutonium or with the total transuranic vector, replacing the uranium atoms in the crystal lattice structure. Infinite and effective neutron multiplication factors were calculated using the state-of-the-art Monte Carlo neutron transport code MCNP in a variety of plausible material configurations, assuming an acceptable safety limit for criticality to be an effective neutron multiplication factor less than 0.95. The results indicate that the crystal structures form a very subcritical intrinsic geometry even with six water molecules being incorporated into the crystal structure. In conclusion, the results of this research suggest that significant opportunity exists for the safe transfer of the group actinide separation approach from a laboratory to an operational scale.},

  doi          = {10.1016/j.anucene.2018.02.006},

  journal      = {Annals of Nuclear Energy (Oxford)},

  number       = C,

  volume       = 115,

  place        = {United States},

  year         = {Thu Feb 22 00:00:00 EST 2018},

  month        = {Thu Feb 22 00:00:00 EST 2018}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (DOE)

Publisher's Version of Record

https://doi.org/10.1016/j.anucene.2018.02.006

Other availability

Search WorldCat to find libraries that may hold this journal

Citation Metrics:

Cited by: 6 works

Citation information provided by
Web of Science

Figures / Tables:

Table 1: Fresh fuel composition

All figures and tables (8 total)

Save / Share:

Export Metadata

Save to My Library

Figures / Tables found in this record:

Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

Similar Records in DOE PAGES and OSTI.GOV collections:

Recovery of Oxidized Actinides, Np(VI), Pu(VI), and Am(VI), from Cocrystallized Uranyl Nitrate Hexahydrate: A Single Technology Approach to Used Nuclear Fuel Recycling

Journal Article Einkauf, Jeffrey D. ; Burns, Jonathan D. - Industrial and Engineering Chemistry Research

In this work, the utility of recovering cocrystallized Np, Pu, and Am from a uranyl nitrate hexahydrate crystalline phase has been examined. Progressive dissolution studies were carried out on samples of either Np(VI), Pu(VI), or Am(VI) cocrystallized with uranyl nitrate hexahydrate, resulting in a linear relationship between the amount of actinides dissolved as a function of volume of HNO₃ added, which indicates homogeneous distribution of the transuranic species throughout the crystalline solid. The ratio of the concentration of U to the heavier actinides was maintained over the entire dissolution and mimicked that of the starting cocrystallization solution. A series ofmore »« less
https://doi.org/10.1021/acs.iecr.0c00381

Full Text Available
A New Group Crystallization Approach in Used Nuclear Fuel Recycling: A Look at Fission Product Behaviors

Journal Article Bunsen, James C. ; Burns, Jonathan D. - Transactions of the American Nuclear Society

Nuclear energy has the potential to play a large role in meeting future needs of the U.S. sustainable energy strategy, as a clean, carbon-free power source. However, to take advantage of the inherent benefits, many hurdles must be overcome in order for nuclear power to achieve these expectations. One of the largest challenges faced, is the management of used nuclear fuel (UNF). Currently, no strategy has been identified to deal with the growing UNF problem, and so the UNF remains stored on site at nuclear power plants either in cooling pools or in dry cast storage. The amount of storedmore »« less
A New Group Crystallization Approach in Used Nuclear Fuel Recycling: A Look at Fission Product Behaviors

Journal Article Wilcox, Andrew J. ; Burnsa, Jonathan D. ; Moyer, Bruce A. - Transactions of the American Nuclear Society

Nuclear energy has the potential to play a large role in meeting future needs of the U.S. sustainable energy strategy, as a clean, carbon-free power source. However, to take advantage of the inherent benefits, many hurdles must be overcome in order for nuclear power to achieve these expectations. One of the largest challenges faced, is the management of used nuclear fuel (UNF). Currently, no strategy has been identified to deal with the growing UNF problem, and so the UNF remains stored on site at nuclear power plants either in cooling pools or in dry cask storage. The amount of storedmore »« less
Sigma Team for Advanced Actinide Recycle FY2015 Accomplishments and Directions

Technical Report Moyer, Bruce A.

The Sigma Team for Minor Actinide Recycle (STAAR) has made notable progress in FY 2015 toward the overarching goal to develop more efficient separation methods for actinides in support of the United States Department of Energy (USDOE) objective of sustainable fuel cycles. Research in STAAR has been emphasizing the separation of americium and other minor actinides (MAs) to enable closed nuclear fuel recycle options, mainly within the paradigm of aqueous reprocessing of used oxide nuclear fuel dissolved in nitric acid. Its major scientific challenge concerns achieving selectivity for trivalent actinides vs lanthanides. Not only is this challenge yielding to researchmore »« less
https://doi.org/10.2172/1263841

Full Text Available
Spectroscopic characterization of neptunium(VI), plutonium(VI), americium(VI) and neptunium(V) encapsulated in uranyl nitrate hexahydrate

Journal Article Yu, Xiaojuan ; Einkauf, Jeffrey ; Bryantsev, Vyacheslav S. ; ... - Physical Chemistry Chemical Physics. PCCP

The coordination of crystalline products resulting from the co-crystallization of Np(VI), Pu(VI), Am(VI), and Np(V) with uranyl nitrate hexahydrate (UNH) has been revealed through solid-state spectroscopic characterization via diffuse reflectance UV-Vis-NIR spectroscopy, SEM-EDS, and extended X-ray absorption fine structure (EXAFS) spectroscopy. Density functional and multireference wavefunction calculations were performed to analyze the An(VI/V)O₂(NO₃)₂·2H₂O electronic structures and to help assign the observed transitions in the absorption spectra. EXAFS show a similar coordination between the U(VI) in UNH and Np(VI) and Pu(VI); while Am resulted in a similar coordination to Am(III), as reduction of Am(VI) occurred prior to EXAFS data being obtained.more »« less
https://doi.org/10.1039/D1CP01047

Full Text Available

Similar Records