Skip to main content
SpringerLink
Log in

Determination of plutonium isotope ratios in individual uranium–plutonium mixed particles with inductively coupled plasma mass spectrometry

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

Abstract

An analytical technique was developed by a combination of single particle dissolution, chemical separation of uranium, plutonium and americium with extraction chromatography using UTEVA resins and measurement with inductively coupled plasma mass spectrometry. This method was applied to plutonium isotope ratio analysis of individual U–Pu particles with U/Pu ratios ranging from 1 to 70. Consequently, 240Pu/239Pu, 241Pu/239Pu and 242Pu/239Pu isotope ratios were successfully determined, while it was impossible to determine 238Pu/239Pu ratios due to the high process blank values on m/z 238.

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
Fig. 5

Similar content being viewed by others

References

  1. 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 16:1283–1289

    Article  CAS  Google Scholar 

  2. Lind OC, Salbu B, Janssens K, Proost K, García-León M, García-Tenorio R (2007) Characterization of U/Pu particles originating from the nuclear weapon accidents at Palomares, Spain, 1966 and Thule, Greenland, 1968. Sci Total Environ 376:294–305

    Article  CAS  Google Scholar 

  3. Donohue DL (1998) Strengthening IAEA safeguards through environmental sampling and analysis. J Alloys Compd 11:271–273

    Google Scholar 

  4. Donohue DL (2002) Strengthened nuclear safeguards. Anal Chem 74:28A–35A

    Article  CAS  Google Scholar 

  5. Simons DS, Gillen G, Zeissler CJ, Fleming RH, McNitt PJ (1998) Automated SIMS for determining isotopic distributions in particle populations. Secondary ion mass spectrometry XI. Wiley, New York, pp 59–62

    Google Scholar 

  6. Tamborini G, Betti M, Forcina V, Hiernaut T, Giovannone B, Koch L (1998) Application of secondary ion mass spectrometry to the identification of single particles of uranium and their isotopic measurement. Spectrochim Acta B 53:1289–1302

    Article  Google Scholar 

  7. Esaka F, Esaka KT, Lee CG, Magara M, Sakurai S, Usuda S, Watanabe K (2007) Particle isolation for analysis of uranium minor isotopes in individual particles by secondary ion mass spectrometry. Talanta 71:1011–1015

    Article  CAS  Google Scholar 

  8. Ranebo Y, Hedberg PML, Whitehouse MJ, Ingeneri K, Littmann S (2009) Improved isotopic SIMS measurements of uranium particles for nuclear safeguard purpose. J Anal At Spectrom 24:277–287

    Article  CAS  Google Scholar 

  9. Hedberg PML, Peres P, Cliff JB, Rabemananjara F, Littmann S, Thiele H, Vincent C, Albert N (2011) Improved particle location and isotopic screening measurements of sub-micron sized particles by secondary ion mass spectrometry. J Anal At Spectrom 26:406–413

    Article  CAS  Google Scholar 

  10. Stetzer O, Betti M, Geel J, Erdmann N, Kratz JV, Schenkel R, Trautmann N (2004) Determination of the 235U content in uranium oxide particles by fission track analysis. Nucl Instrum Methods Phys Res A 525:582–592

    Article  CAS  Google Scholar 

  11. Esaka KT, Esaka F, Inagawa J, Iguchi K, Lee CG, Sakurai S, Watanabe K, Usuda S (2004) Application of fission track technique for the analysis of individual particles containing uranium in safeguard swipe samples. Jpn J Appl Phys 43:L915–L916

    Article  CAS  Google Scholar 

  12. Lee CG, Iguchi K, Inagawa J, Suzuki D, Esaka F, Magara M, Sakurai S, Watanabe K, Usuda S (2007) Development in fission track-thermal ionization mass spectrometry for particle analysis of safeguards environmental samples. J Radioanal Nucl Chem 272:299–302

    Article  CAS  Google Scholar 

  13. Willman C, Håkansson A, Osifo O, Bäcklin A, Svärd SJ (2006) A nondestructive method for discriminating MOX fuel from LEU fuel for safeguards purpose. Ann Nucl Energy 33:766–773

    Article  CAS  Google Scholar 

  14. Esaka F, Magara M, Suzuki D, Miyamoto Y, Lee CG, Kimura T (2011) Feasibility study of isotope ratio analysis of individual uranium-plutonium mixed oxide particles with SIMS and ICP-MS. Mass Spectrom Lett 2:80–83

    Article  CAS  Google Scholar 

  15. Raptis K, Duhamel G, Ludwig R, Balsley S, Bürger S, Mayorov V, Koepf A, Hara S, Itoh Y, Yamaguchi Y, Yamaguchi T, Ninagawa J (2013) Measurement of non-separated U/Pu samples: optimization of TIMS procedures for safeguards purposes at Rokkasho on-site laboratory. J Radioanal Nucl Chem 296:585–592

    Article  CAS  Google Scholar 

  16. Esaka F, Magara M, Suzuki D, Miyamoto Y, Lee CG, Kimura T (2010) Isotope ratio analysis of individual sub-micrometer plutonium particles with inductively coupled plasma mass spectrometry. Talanta 83:569–573

    Article  CAS  Google Scholar 

  17. Suzuki D, Esaka F, Miyamoto Y, Magara M (2015) Direct isotope ratio analysis of individual uranium-plutonium mixed particles with various U/Pu ratios by thermal ionization mass spectrometry. Appl Radiat Isot 96:52–56

    Article  CAS  Google Scholar 

  18. Morgenstern A, Apostolidis C, Carlos-Marquez R, Mayer K, Molinet R (2002) Single-column extraction chromatographic separation of U, Pu, Np and Am. Radiochim Acta 90:81–85

    CAS  Google Scholar 

  19. Esaka F, Lee CG, Magara M, Kimura T (2012) Fission track-secondary ion mass spectrometry as a tool for detecting the isotopic signature of individual uranium containing particles. Anal Chim Acta 721:122–128

    Article  CAS  Google Scholar 

  20. Erdmann N, Betti M, Stetzer O, Tamborini G, Kratz JV, Trautmann N, Geel J (2000) Production of monodisperse uranium oxide particles and their characterization by scanning electron microscopy and secondary ion mass spectrometry. Spectrochim Acta B 55:1565–1575

    Article  Google Scholar 

  21. Aggarwal SK, Alamelu D (2005) A novel approach for the determination of 238Pu by thermal ionization mass spectrometry (TIMS) using interfering element correction methodology. Int J Mass Spectrom 241:83–88

    Article  CAS  Google Scholar 

  22. Aggarwal SK, Alamelu D, Khodade PS, Shah PM (2007) Determination of 238Pu in plutonium bearing fuels by thermal ionization mass spectrometry. J Radioanal Nucl Chem 273:775–778

    Article  CAS  Google Scholar 

Download references

Acknowledgments

This work was performed under the auspices of the Nuclear Regulation Authority, Japan. The authors wish to thank Dr. K. Watanabe for the helpful discussion, Mr. N. Kohno and Mr. T. Watanabe for particle production, Mr. H. Fukuyama, Mr. T. Onodera for sample preparation and Mr. Y. Takahashi for ICP-MS measurement.

Author information

Authors and Affiliations

  1. Research Group for Analytical Chemistry, Japan Atomic Energy Agency (JAEA), 2-4 Shirakata-Shirane, Tokai, Naka, Ibaraki, 319-1195, Japan

    Fumitaka Esaka, Daisuke Suzuki, Yutaka Miyamoto & Masaaki Magara

Authors
  1. Fumitaka Esaka
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Daisuke Suzuki
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Yutaka Miyamoto
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Masaaki Magara
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Fumitaka Esaka.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Esaka, F., Suzuki, D., Miyamoto, Y. et al. Determination of plutonium isotope ratios in individual uranium–plutonium mixed particles with inductively coupled plasma mass spectrometry. J Radioanal Nucl Chem 306, 393–399 (2015). https://doi.org/10.1007/s10967-015-4113-6

Download citation

  • Received:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10967-015-4113-6

Keywords

Search

Navigation