Separation of protactinium from uranium-niobium alloys for 231Pa–235U radiochronometry in nuclear forensic investigations

Chen, Christine Yifeng; Higginson, Matthew A.; Kayzar-Boggs, Theresa M.; Denton, Joanna S.; Dunne, James; Edwards, Mark A.; Eng, Charlotte; Engel, John R.; Gaffney, Amy M.; Gilligan, Chris; Morris, Maya N.; Rolison, John M.; Sanborn, Matthew E.; Wende, Allison M.

doi:10.1007/s10967-023-08928-y

Title: Separation of protactinium from uranium-niobium alloys for ²³¹Pa–²³⁵U radiochronometry in nuclear forensic investigations

Journal Article · 18 May 2023 · Journal of Radioanalytical and Nuclear Chemistry

DOI: https://doi.org/10.1007/s10967-023-08928-y · OSTI ID:2006747

^[1]; Higginson, Matthew A. ^[2]; Kayzar-Boggs, Theresa M. ^[3]; Denton, Joanna S. ^[3]; Dunne, James ^[2]; Edwards, Mark A. ^[3]; Eng, Charlotte ^[1]; Engel, John R. ^[3]; Gaffney, Amy M. ^[1]; Gilligan, Chris ^[2]; Morris, Maya N. ^[1]; Rolison, John M. ^[1]; Sanborn, Matthew E. ^[3]; Wende, Allison M. ^[3]

Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Atomic Weapons Establishment (AWE), Aldermaston (United Kingdom)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

The isolation and purification of protactinium from uranium materials is essential for ²³¹Pa–²³⁵U radiochronometry, but separating Pa from uranium-niobium alloys, a common material in the nuclear fuel cycle, is challenging due to the chemical similarity of Pa and Nb. Here, in this work, we present three resin chromatography separation techniques for isolating Pa from U and Nb which were independently developed by three different laboratories through ad hoc adaptations of standard operating procedures. Our results underscore the need for and value of purification methods suitable for a diversity of uranium-based materials to ensure the operational readiness of nuclear forensics laboratories.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA), Office of Counter-terrorism and Counter-nonproliferation

Grant/Contract Number:: AC52-07NA27344; 89233218CNA000001

OSTI ID:: 2006747

Alternate ID(s):: OSTI ID: 2217505

Report Number(s):: LLNL-JRNL-843763; LA-UR-23-21440; 1066207

Journal Information:: Journal of Radioanalytical and Nuclear Chemistry, Vol. 332, Issue 7; ISSN 0236-5731

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

References (36)

Results from a controlled depleted uranium metal casting experiment designed to investigate nuclear Forensic Radiochronometry Signatures Kayzar-Boggs, Theresa M.; Luitjohan, Kara E.; Imhoff, Seth D. Journal of Radioanalytical and Nuclear Chemistry, Vol. 332, Issue 6 https://doi.org/10.1007/s10967-023-08881-w	journal	April 2023
Separation of Protactinium Employing Sulfur-Based Extraction Chromatographic Resins Mastren, Tara; Stein, Benjamin W.; Parker, T. Gannon Analytical Chemistry, Vol. 90, Issue 11 https://doi.org/10.1021/acs.analchem.8b01380	journal	April 2018
The state of nuclear forensics Kristo, Michael J.; Tumey, Scott J. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 294 https://doi.org/10.1016/j.nimb.2012.07.047	journal	January 2013
Nuclear forensics in law enforcement applications Grant, P. M.; Moody, K. J.; Hutcheon, I. D. Journal of Radioanalytical and Nuclear Chemistry, Vol. 235, Issue 1-2 https://doi.org/10.1007/BF02385950	journal	September 1998
Ion exchange in aqueous and in aqueous-organic solvents Kim, J. I.; Lagally, H.; Born, H. -J. Analytica Chimica Acta, Vol. 64, Issue 1 https://doi.org/10.1016/S0003-2670(00)86889-0	journal	March 1973
Nuclear forensic analysis of uranium oxide powders interdicted in Victoria, Australia Kristo, Michael Joseph; Keegan, Elizabeth; Colella, Michael Radiochimica Acta, Vol. 103, Issue 7 https://doi.org/10.1515/ract-2014-2363	journal	January 2015
Nuclear Forensics: Scientific Analysis Supporting Law Enforcement and Nuclear Security Investigations Keegan, Elizabeth; Kristo, Michael J.; Toole, Kaitlyn Analytical Chemistry, Vol. 88, Issue 3 https://doi.org/10.1021/acs.analchem.5b02915	journal	January 2016
The effect of quench rate on the microstructure, mechanical properties, and corrosion behavior of U-6 wt pct Nb Eckelmeyer, K. H.; Romig, A. D.; Weirick, L. J. Metallurgical Transactions A, Vol. 15, Issue 7 https://doi.org/10.1007/BF02648560	journal	July 1984
²³⁰ Th- ²³⁴ U model ages of some uranium standard reference materials Williams, R. W.; Gaffney, A. M. Proceedings in Radiochemistry, Vol. 1, Issue 1 https://doi.org/10.1524/rcpr.2011.0005	journal	September 2011
International cooperation in age-dating uranium standards for nuclear forensics using the 231Pa/235U radiochronometer Denton, Joanna S.; Treinen, Kerri C.; Chen, Yan Journal of Radioanalytical and Nuclear Chemistry, Vol. 324, Issue 2 https://doi.org/10.1007/s10967-020-07084-x	journal	March 2020
Application of the 226Ra–230Th–234U and 227Ac–231Pa–235U radiochronometers to UF6 cylinders Rolison, John M.; Williams, Ross W. Journal of Radioanalytical and Nuclear Chemistry, Vol. 317, Issue 2 https://doi.org/10.1007/s10967-018-5955-5	journal	June 2018
Nuclear forensic analysis of an unknown uranium ore concentrate sample seized in a criminal investigation in Australia Keegan, Elizabeth; Kristo, Michael J.; Colella, Michael Forensic Science International, Vol. 240 https://doi.org/10.1016/j.forsciint.2014.04.004	journal	July 2014
Adsorption of Elements from Hydrofluoric Acid by Anion Exchange Faris, J. P. Analytical Chemistry, Vol. 32, Issue 4 https://doi.org/10.1021/ac60160a019	journal	April 1960
Alternative method for the production date determination of impure uranium ore concentrate samples Varga, Zsolt; Wallenius, Maria; Mayer, Klaus Journal of Radioanalytical and Nuclear Chemistry, Vol. 290, Issue 2 https://doi.org/10.1007/s10967-011-1233-5	journal	June 2011
Nuclear Forensic Science: Analysis of Nuclear Material Out of Regulatory Control Kristo, Michael J.; Gaffney, Amy M.; Marks, Naomi Annual Review of Earth and Planetary Sciences, Vol. 44, Issue 1 https://doi.org/10.1146/annurev-earth-060115-012309	journal	June 2016
Improved protactinium spike calibration method applied to 231Pa–235U age-dating of certified reference materials for nuclear forensics Treinen, Kerri C.; Gaffney, Amy M.; Rolison, John M. Journal of Radioanalytical and Nuclear Chemistry, Vol. 318, Issue 1 https://doi.org/10.1007/s10967-018-6149-x	journal	August 2018
Isolation and purification of protactinium-231 Jerome, S. M.; Collins, S. M.; Happel, S. Applied Radiation and Isotopes, Vol. 134 https://doi.org/10.1016/j.apradiso.2017.07.051	journal	April 2018
235U–231Pa age dating of uranium materials for nuclear forensic investigations Eppich, Gary R.; Williams, Ross W.; Gaffney, Amy M. Journal of Analytical Atomic Spectrometry, Vol. 28, Issue 5 https://doi.org/10.1039/c3ja50041a	journal	January 2013
Anion Exchange Studies. III. Protactinium in Some HCl—HF Mixtures: Separation of Niobium, Tantalum and Protactinium¹ Kraus, Kurt A.; Moore, George E. Journal of the American Chemical Society, Vol. 73, Issue 6 https://doi.org/10.1021/ja01150a140	journal	June 1951
Batch and column studies of radium, actinium, thorium and protactinium on CL resin in nitric acid, hydrochloric acid and hydrofluoric acid Kmak, Kelly N.; Shaughnessy, Dawn A.; Vujic, Jasmina Journal of Radioanalytical and Nuclear Chemistry, Vol. 328, Issue 1 https://doi.org/10.1007/s10967-021-07636-9	journal	February 2021
A phenomenological study of the shape memory effect in polycrystalline uranium-niobium alloys Vandermeer, R. A.; Ogle, J. C.; Northcutt, W. G. Metallurgical Transactions A, Vol. 12, Issue 5 https://doi.org/10.1007/BF02648337	journal	May 1981
The estimation of thorium and uranium at the submicrogram level in bone by neutron activation Edgington, D. N. The International Journal of Applied Radiation and Isotopes, Vol. 18, Issue 1 https://doi.org/10.1016/0020-708X(67)90167-6	journal	January 1967
Round-robin 230Th–234U age dating of bulk uranium for nuclear forensics Gaffney, Amy M.; Hubert, Amélie; Kinman, William S. Journal of Radioanalytical and Nuclear Chemistry, Vol. 307, Issue 3 https://doi.org/10.1007/s10967-015-4334-8	journal	July 2015
Nuclear forensic investigations: Two case studies Wallenius, M.; Mayer, K.; Ray, I. Forensic Science International, Vol. 156, Issue 1 https://doi.org/10.1016/j.forsciint.2004.12.029	journal	January 2006
A chromatography chemistry for purifying Pa from U-Nb metal alloys Engel, John R.; Denton, Joanna S.; Lamont, Stephen P. Journal of Radioanalytical and Nuclear Chemistry, Vol. 332, Issue 2 https://doi.org/10.1007/s10967-022-08747-7	journal	January 2023
Adsorption of Protactinium from Hydrochloric Acid Solutions by Anion Exchange Resins¹ Kraus, Kurt A.; Moore, George E. Journal of the American Chemical Society, Vol. 72, Issue 9 https://doi.org/10.1021/ja01165a525	journal	September 1950
Development of rapid methodologies for uranium age dating Higginson, Matthew; Gilligan, Chris; Taylor, Fiona Journal of Radioanalytical and Nuclear Chemistry, Vol. 318, Issue 1 https://doi.org/10.1007/s10967-018-6021-z	journal	August 2018
Evaluation of chronometers in plutonium age determination for nuclear forensics: What if the ‘Pu/U clocks’ do not match? Sturm, M.; Richter, S.; Aregbe, Y. Journal of Radioanalytical and Nuclear Chemistry, Vol. 302, Issue 1 https://doi.org/10.1007/s10967-014-3294-8	journal	July 2014
Establishing discordance as a radiochronometric signature for nuclear forensic investigations: a multi-laboratory intercomparison exercise Higginson, Matthew A.; Kayzar-Boggs, Theresa M.; Chen, Christine Y. Journal of Radioanalytical and Nuclear Chemistry, Vol. 331, Issue 12 https://doi.org/10.1007/s10967-022-08428-5	journal	August 2022
Behaviour of 18 elements in HF and HF−NH4F media on anion exchanger in various ionic forms Caletka, R.; Krivan, V. Journal of Radioanalytical and Nuclear Chemistry Articles, Vol. 142, Issue 2 https://doi.org/10.1007/BF02040306	journal	October 1990
Crystallographic and kinetic origins of acicular and banded microstructures in U–Nb alloys Field, R. D.; Thoma, D. J. Journal of Nuclear Materials, Vol. 436, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2013.01.309	journal	May 2013
Developing 226Ra and 227Ac age-dating techniques for nuclear forensics to gain insight from concordant and non-concordant radiochronometers Kayzar, Theresa M.; Williams, Ross W. Journal of Radioanalytical and Nuclear Chemistry, Vol. 307, Issue 3 https://doi.org/10.1007/s10967-015-4435-4	journal	September 2015
The Radiochemistry of Thorium Hyde, E. K. https://doi.org/10.2172/4241632	report	April 1959
A new method for separation of niobium from zirconium with silica gel. Yoshida, Michiko; Numata, Yasushi; Seki, Riki RADIOISOTOPES, Vol. 39, Issue 12 https://doi.org/10.3769/radioisotopes.39.12_547	journal	January 1990
Melting and Casting of Uranium Ripley, Edward B. Uranium Processing and Properties https://doi.org/10.1007/978-1-4614-7591-0_2	book	January 2013
An interlaboratory collaboration to determine consensus 231Pa/235U model ages of a uranium certified reference material for nuclear forensics Kayzar-Boggs, Theresa M.; Treinen, Kerri C.; Okubo, Ayako Journal of Radioanalytical and Nuclear Chemistry, Vol. 323, Issue 3 https://doi.org/10.1007/s10967-020-07030-x	journal	February 2020

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
radiochronometry
nuclear forensics
uranium alloy
231Pa–235U
actinide separations
protactinium

Title: Separation of protactinium from uranium-niobium alloys for 231Pa–235U radiochronometry in nuclear forensic investigations

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References (36)

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Title: Separation of protactinium from uranium-niobium alloys for ²³¹Pa–²³⁵U radiochronometry in nuclear forensic investigations