Measuring key Sm isotope ratios in irradiated UO2 for use in plutonium discrimination nuclear forensics

  • Kevin J. Glennon
  • Jeremy M. Osborn
  • Jonathan D. Burns
  • Evans D. Kitcher
  • Sunil S. Chirayath
  • Charles M. FoldenIIIEmail author


As part of an experimental validation of a nuclear forensics methodology for Pu source reactor-type discrimination, destructive analysis has been performed on two irradiated UO2 pellets with different irradiation histories. Analysis has focused on measuring key Sm fission product isotope ratios used in a previously published maximum likelihood methodology to determine the most likely irradiation history of the pellets. A total of 21 Sm isotope ratios were measured within the irradiated pellets, and generally agreed within 20% of the irradiations as simulated using the Monte Carlo Radiation Transport and material depletion code, MCNP6. Results indicate the chosen approach can accurately measure the isotope ratios within 5% experimental error.


Nuclear forensics Cation exchange chromatography Isotope ratios Separated plutonium Irradiated UO2 



The authors would like to thank Dr. Brent Miller (Geology & Geophysics, Texas A&M) for his time and effort in setting up the Thermo Fisher Scientific iCAP RQ mass spectrometer for use with significant activities of long-lived radionuclides. Sample preparation, chemical separation, and mass spectrometry was supported by the Department of Energy National Nuclear Security Administration under Award Number DE-NA0003180. This work was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereof, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. All pellet irradiations and simulations were supported by the U.S. Department of Homeland Security, Domestic Nuclear Detection Office under Grant Award Numbers: NSF Grant Nos. ECCS-1140018, DHS-2012-DN-077-ARI1057-02&03 and DHS-2015-DN-077-ARI1099. The views and conclusions contained in this document are those of the authors and should not be interpreted as necessarily representing the official policies, either expressed or implied, of the U.S. Department of Homeland Security.


  1. 1.
    Kristo MJ, Gaffney AM, Marks N, Knight K, Cassata WS, Hutcheon ID (2016) Nuclear forensic science: analysis of nuclear material out of regulatory control. Annu Rev Earth Planet Sci 44(1):555–579. CrossRefGoogle Scholar
  2. 2.
    Kristo MJ, Tumey SJ (2013) The state of nuclear forensics. Nucl Instrum Methods Phys Res B 294:656–661. CrossRefGoogle Scholar
  3. 3.
    May M, Abedin-Zadeh R, Barr D, Carnesale A, Coyle P, Davis J, Dorland W, Dunlop W, Fetter S, Glaser A, Hutcheon I, Slakey F, Tannenbaum B (2008) Nuclear forensics: role, state of the art, program needs. Joint report from the American Physical Society and the American Association for the Advancement of ScienceGoogle Scholar
  4. 4.
    Chirayath SS, Osborn JM, Coles TM (2015) Trace fission product ratios for nuclear forensics attribution of weapons-grade plutonium from fast and thermal reactors. Sci Global Secur 23(1):48–67. CrossRefGoogle Scholar
  5. 5.
    Wallenius M, Peerani P, Koch L (2000) Origin determination of plutonium material in nuclear forensics. J Radioanal Nucl Chem 246(2):317–321. CrossRefGoogle Scholar
  6. 6.
    Byerly BL, Stanley F, Spencer K, Colletti L, Garduno K, Kuhn K, Lujan E, Martinez A, Porterfield D, Rim J, Schappert M, Thomas M, Townsend L, Xu N, Tandon L (2016) Forensic investigation of plutonium metal: a case study of CRM 126. J Radioanal Nucl Chem 310(2):623–632. CrossRefGoogle Scholar
  7. 7.
    Moody KJ, Hutcheon ID, Grant PM (2015) Nuclear forensic analysis. CRC Press, Boca RatonGoogle Scholar
  8. 8.
    Favalli A, Vo D, Grogan B, Jansson P, Liljenfeldt H, Mozin V, Schwalbach P, Sjöland A, Tobin SJ, Trellue H, Vaccaro S (2016) Determining initial enrichment, burnup, and cooling time of pressurized-water-reactor spent fuel assemblies by analyzing passive gamma spectra measured at the Clab interim-fuel storage facility in Sweden. Nucl Instrum Methods Phys Res A 820(Supplement C):102–111. CrossRefGoogle Scholar
  9. 9.
    Lantzos I, Kouvalaki C, Nicolaou G (2015) Plutonium fingerprinting in nuclear forensics of spent nuclear fuel. Prog Nucl Energy 85:333–336. CrossRefGoogle Scholar
  10. 10.
    Nash KL, Nilsson M (2015) Introduction to the reprocessing and recycling of spent nuclear fuels. In: Taylor R (ed) Reprocessing and recycling of spent nuclear fuel. Woodhead Publishing, Oxford, pp 3–25. CrossRefGoogle Scholar
  11. 11.
    Gerber MS (1993) A brief history of the PUREX and UO3 facilities. Westinghouse Hanford Co., Richland. CrossRefGoogle Scholar
  12. 12.
    Benedict M, Pigford TH, Hans Wolfgang L (1981) Fuel reprocessing. nuclear chemical engineering, vol 10, 2nd edn. McGraw-Hill Education, New YorkGoogle Scholar
  13. 13.
    Mendoza PM, Chirayath SS, Folden CM III (2016) Fission product decontamination factors for plutonium separated by PUREX from low-burnup, fast-neutron irradiated depleted UO2. Appl Radiat Isot 118:38–42. CrossRefPubMedGoogle Scholar
  14. 14.
    Rim JH, Kuhn KJ, Tandon L, Xu N, Porterfield, Worley CG, Thomas, Spencer KJ, Stanley FE, Lujan EJ, Garduno K, Trellue HR (2017) Determination of origin and intended use of plutonium metal using nuclear forensic techniques. Forensic Sci Int 273(Supplement C):e1–e9. CrossRefPubMedGoogle Scholar
  15. 15.
    Wallenius M, Lützenkirchen K, Mayer K, Ray I, de las Heras LA, Betti M, Cromboom O, Hild M, Lynch B, Nicholl A, Ottmar H, Rasmussen G, Schubert A, Tamborini G, Thiele H, Wagner W, Walker C, Zuleger E (2007) Nuclear forensic investigations with a focus on plutonium. J Alloys Compd 444–445:57–62. CrossRefGoogle Scholar
  16. 16.
    Osborn JM, Kitcher ED, Burns JD, Folden CM III, Chirayath SS (2017) Nuclear forensics methodology for reactor-type attribution of chemically separated plutonium. Nucl Technol. CrossRefGoogle Scholar
  17. 17.
    Osborn JM, Glennon KJ, Kitcher ED, Burns JD, Folden CM III, Chirayath SS (2018) Experimental validation of a nuclear forensics methodology for source reactor-type discrimination of chemically separated plutonium. Nucl Eng Technol. CrossRefGoogle Scholar
  18. 18.
    Osborn JM, Glennon KJ, Kitcher ED, Burns JD, Folden CM III, Chirayath SS (2018) Computational and experimental forensics characterization of weapons-grade plutonium produced in a thermal neutron environment. Nucl Eng Technol. CrossRefGoogle Scholar
  19. 19.
    Wacker J (2001) New advances in inductively coupled plasma—mass spectrometry (ICP-MS) for routine measurements in the nuclear industry. J Radioanal Nucl Chem 249(1):103–108. CrossRefGoogle Scholar
  20. 20.
    Becker JS (2005) Inductively coupled plasma mass spectrometry (ICP-MS) and laser ablation ICP-MS for isotope analysis of long-lived radionuclides. Int J Mass Spectrom 242(2):183–195. CrossRefGoogle Scholar
  21. 21.
    Boulyga SF, Testa C, Desideri D, Becker JS (2001) Optimisation and application of ICP-MS and alpha-spectrometry for determination of isotopic ratios of depleted uranium and plutonium in samples collected in Kosovo. J Anal At Spectrom 16(11):1283–1289. CrossRefGoogle Scholar
  22. 22.
    Stanley FE, Stalcup AM, Spitz HB (2013) A brief introduction to analytical methods in nuclear forensics. J Radioanal Nucl Chem 295(2):1385–1393. CrossRefGoogle Scholar
  23. 23.
    Gharibyan N, Bene BJ, Sudowe R (2017) Chromatographic separation of thulium from erbium for neutron capture cross section measurements—Part I: trace scale optimization of ion chromatography method with various complexing agents. J Radioanal Nucl Chem 311(1):179–187. CrossRefGoogle Scholar
  24. 24.
    Trikha R, Sharma BK, Sabharwal KN, Prabhu K (2015) Elution profiles of lanthanides with α-hydroxyisobutyric acid by ion exchange chromatography using fine resin. J Sep Sci 38(21):3810–3814. CrossRefPubMedGoogle Scholar
  25. 25.
    Schwantes JM, Rundberg RS, Taylor WA, Vieira DJ (2006) Rapid, high-purity, lanthanide separations using HPLC. J Alloys Compd 418(1–2):189–194. CrossRefGoogle Scholar
  26. 26.
    Datta A, Sivaraman N, Srinivasan TG, Rao PRV (2013) Single-stage dual-column HPLC technique for separation and determination of lanthanides in uranium matrix: application to burnup measurement on nuclear reactor fuel. Nucl Technol 182(1):84–97. CrossRefGoogle Scholar
  27. 27.
    Swinney MW, Folden CM III, Ellis RJ, Chirayath SS (2017) Experimental and computational forensics characterization of weapons-grade plutonium produced in a fast reactor neutron environment. Nucl Technol 197(1):1–11. CrossRefGoogle Scholar
  28. 28.
    Horwitz EP, Dietz ML, Chiarizia R, Diamond H, Essling AM, Graczyk D (1992) Separation and preconcentration of uranium from acidic media by extraction chromatography. Anal Chim Acta 266(1):25–37. CrossRefGoogle Scholar
  29. 29.
    Marinov G, Marinova A, Milanova M, Happel S, Lebedev NA, Drokhlyansky A, Mirzayev N, Karaivanov DV, Filosofov DV (2017) Sorption of rare-earth elements and Ac on UTEVA resin in different acid solutions. Solvent Extr Ion Exch 35(4):280–291. CrossRefGoogle Scholar
  30. 30.
    Gray LW, Holliday KS, Murray A, Thompson M, Thorp DT, Yarbro S, Venetz TJ (2015) Separation of plutonium from irradiated fuels and targets. Lawrence Livermore Natl Lab. CrossRefGoogle Scholar
  31. 31.
    Savina JA, Steeb JL, Savina MR, Mertz CJ, Fortner JA, Sullivan VS, Bennett ME, Chamberlain DB (2017) A non-destructive internal nuclear forensic investigation at Argonne: discovery of a Pu planchet from 1948. J Radioanal Nucl Chem 311(1):243–252. CrossRefGoogle Scholar
  32. 32.
    Schwantes JM, Douglas M, Bonde SE, Briggs JD, Farmer OT, Greenwood LR, Lepel EA, Orton CR, Wacker JF, Luksic AT (2009) Nuclear archeology in a bottle: evidence of pre-trinity U.S. weapons activities from a waste burial site. Anal Chem 81(4):1297–1306. CrossRefPubMedGoogle Scholar

Copyright information

© Akadémiai Kiadó, Budapest, Hungary 2019

Authors and Affiliations

  • Kevin J. Glennon
    • 1
    • 2
  • Jeremy M. Osborn
    • 3
    • 4
  • Jonathan D. Burns
    • 3
  • Evans D. Kitcher
    • 3
  • Sunil S. Chirayath
    • 3
    • 4
  • Charles M. FoldenIII
    • 1
    • 2
    Email author
  1. 1.Cyclotron InstituteTexas A&M UniversityCollege StationUSA
  2. 2.Department of ChemistryTexas A&M UniversityCollege StationUSA
  3. 3.Center for Nuclear Security Science and Policy InitiativesTexas A&M UniversityCollege StationUSA
  4. 4.Department of Nuclear EngineeringTexas A&M UniversityCollege StationUSA

Personalised recommendations