Skip to main content
SpringerLink
Log in

A case study in plutonium radiochronometry using multiple isotope systems

  • Published:
Journal of Radioanalytical and Nuclear Chemistry Aims and scope Submit manuscript

Abstract

Radiochronometry analyses of two Pu metals were performed using the 237Np–241Am–241Pu, 234U–238Pu, 235U–239Pu, and 236U–240Pu decay series. For one sample, all radiochronometers yield concordant model dates in 1959–1960, indicating that the aqueous processing method used to purify Pu effectively removed U, Am and Np decay products from the bulk Pu. The second sample yields discordant model dates that are also older than the known production date in 1982. The excess U, Am and Np present in the sample indicate that the sample was purified during at least two different episodes, using a combination of aqueous methods and molten salt extraction.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4

Similar content being viewed by others

References

  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 44:555–579

    Article  CAS  Google Scholar 

  2. Sturm M, Richter S, Agrebe Y, Wellum R, Mialle S, Mayer K, Prohaska T (2014) Evaluation of chronometers in plutonium age determination for nuclear forensics: what if the ‘Pu/U clocks’ do not match? J Radioanal Nucl Chem 302(1):399–411

    Article  CAS  Google Scholar 

  3. 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 310:623–632

    Article  CAS  Google Scholar 

  4. Rolison JM, Treinen KC, McHugh KC, Gaffney AM, Williams RW (2017) Application of the 226Ra-230Th-234U and 227Ac-231Pa-235U radiochronometers to uranium certified reference materials. J Radioanal Nucl Chem 314:2459–2467

    Article  CAS  Google Scholar 

  5. Kayzar TM, Williams RW (2016) Developing 226Ra and 227Ac age-dating techniques for nuclear forensics to gain insight from concordant and non-concordant radiochronometers. J Radioanal Nucl Chem 307:2061–2068

    Article  CAS  Google Scholar 

  6. Christensen EL, Gray LW, Navratil JD, Schulz WW (1983) Present status and future directions of plutonium process chemistry. In: Carnall WT, Choppin GR (eds) Plutonium chemistry. ACS Symposium Series 216. ACS Publications, Washington, DC, p 349

    Chapter  Google Scholar 

  7. Nuclear materials, plutonium processing in the nuclear weapons complex (1992) United States General Accounting Office, GAO/RCED-92-109FS

  8. Gray, LW(1999) From separations to reconstitution—a short history of plutonium in the US and Russia. UCRL-JC-133802

  9. Mullins LN, Morgan AN (1981) A review of operating experience at the Los Alamos plutonium electrorefining facility, 1963–1977. LA-8943

  10. Christensen DC, Mullins LJ (1983) Plutonium metal production and purification at Los Alamos. In: Carnall WT, Choppin GR (eds) Plutonium chemistry. ACS Symposium Series 216. ACS Publications, Washington, DC, p 409

    Chapter  Google Scholar 

  11. Coops MS, Knighton JB, Mullins LJ (1983) Pyrochemical processing of plutonium. In: Carnall WT, Choppin GR (eds) Plutonium chemistry. ACS Symposium Series 216. ACS Publications, Washington, DC, p 381

    Chapter  Google Scholar 

  12. Bateman H (1910) The solution of a system of differential equations occurring in the theory of radioactive transformations. Proc Camb Philos Soc 15(V):423–427

    CAS  Google Scholar 

  13. Moody KJ, Grant PM, Hutcheon ID (2015) Nuclear forensic analysis. CRC Press, Boca Raton, FL, p 502

    Google Scholar 

  14. Decay Data Evaluation Project. http://www.nucleide.org/DDEP.htm

  15. National Nuclear Data Center, NuDat 2.6. http://www.nndc.bnl.gov/nudat2

  16. Cheng H, Edwards RL, Shen C-C, Polyak VJ, Asmerom Y, Woodhead J, Hellstrom J, Wang Y, Kong X, Spötl C, Wang X, Alexander EC Jr (2013) Improvements in 230Th dating, 230Th and 234U half-life values, and U–Th isotopic measurements by multi-collector inductively coupled plasma mass spectrometry. Earth Planet Sci Lett. https://doi.org/10.1016/j.epsl.2013.04.006i

    Article  Google Scholar 

  17. Jaffey AH, Flynn KF, Glendenin LE, Bentley WC, Essling AM (1971) Precision measurement of half-lives and specific activities of 235U and 238U. Phys Rev C 5:1889–1906

    Article  Google Scholar 

  18. Moser WS, Navratil JD (1984) Review of major plutonium pyrochemical technology. J Less Common Metals 100:171–187

    Article  CAS  Google Scholar 

  19. Knighton JB, Auge RG, Berry JW, Franchini RC (1976) Molten salt extraction of americium from molten plutonium metal. RFP-2365

  20. Knighton JB, Steunenberg RK (1965) Distribution of transuranium elements between magnesium chloride and zinc–magnesium alloy. J Inorg Nucl Chem 21:1457–1462

    Article  Google Scholar 

  21. Coops MS, Knighton JB, Mullins LJ (1982) Technology review report, pyrochemical processing of actinide metals. 184th National American Chemical Society Meeting, Kansas City, Missouri. UCRL-88116

Download references

Acknowledgements

This work was supported by the U.S. Department of Homeland Security and the U.S. Department of Energy. We thank Mike Blau and Jim McNeese for discussions on plutonium production methods. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. LLNL-JRNL-748960.

Author information

Authors and Affiliations

  1. Nuclear and Chemical Sciences Division, Lawrence Livermore National Laboratory, 7000 East Avenue L-231, Livermore, CA, 94550, USA

    Amy M. Gaffney, Josh B. N. Wimpenny, Tashi Parsons-Davis & Ross W. Williams

  2. Materials Sciences Division, Lawrence Livermore National Laboratory, 7000 East Avenue L-359, Livermore, CA, 94550, USA

    Richard A. Torres & Brandon W. Chung

Authors
  1. Amy M. Gaffney
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Josh B. N. Wimpenny
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Tashi Parsons-Davis
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Ross W. Williams
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Richard A. Torres
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Brandon W. Chung
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Amy M. Gaffney.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Gaffney, A.M., Wimpenny, J.B.N., Parsons-Davis, T. et al. A case study in plutonium radiochronometry using multiple isotope systems. J Radioanal Nucl Chem 318, 287–295 (2018). https://doi.org/10.1007/s10967-018-6131-7

Download citation

  • Received:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10967-018-6131-7

Keywords

Search

Navigation