• Received : 2012.08.27
  • Accepted : 2013.02.01
  • Published : 2013.06.25


A determination method for $^{237}Np$ in spent nuclear fuel samples was developed using an isotope dilution method with $^{239}Np$ as a spike. In this method, inductively coupled plasma mass spectrometry (ICP-MS) was taken for the $^{237}Np$ instead of the previously used alpha spectrometry. $^{237}Np$ and $^{239}Np$ were measured by ICP-MS and gamma spectrometry, respectively. The recovery yield of $^{237}Np$ in synthetic samples was $95.9{\pm}9.7$% (1S, n=4). The $^{237}Np$ contents in the spent fuel samples were 0.15, 0.25, and $1.06{\mu}g/mgU$ and these values were compared with those from ORIGEN-2 code. A fairly good agreement between the measurements (m) and calculations (c) was obtained, giving ratios (m/c) of 0.93, 1.12 and 1.25 for the three PWR spent fuel samples with burnups of 16.7, 19.0, and 55.9 GWd/MtU, respectively.


Supported by : National Research Foundation of Korea (NRF)


  1. T.M. Beasley, J.M. Kelley, T.C. Maiti and L.A. Bond, "$^{237}Np/^{239}Pu$ atom ratios in integrated global fallout: a reassessment of the production of $^{237}Np$", J. Environmental. Radioactivity, 38(2), 133-146(1998).
  2. St.N. Kalmykov, R.A. Aliev, D.Yu. Sapozhnikov, Yu. A. Sapozhnikov, A. M. Afinogenov, "Determination of Np-237 by radiochemical neutron activation analysis combined with extraction chromatography", Applied Radiation and Isotopes, 60, 595-599(2004).
  3. Kihsoo Joe, Byung-Chul Song, Young-Bok Kim, Sun-Ho Han, Young-Shin Jeon, Euo-Chang Jung and Kwang-Yong Jee, "Determination of the transuranic elements inventory in high burnup PWR spent fuel samples by alpha spectrometry", Nuclear Engineering and Technology, 39(5), 673-682(2007).
  4. Kihsoo Joe, Byung-Chul Song, Young-Bok Kim, Young-Shin Jeon, Sun-Ho Han, Euo-Chang Jung and Kyuseok Song, "Determination of the transuranic elements inventory in high burnup PWR spent fuel samples by alpha spectrometry-II", Nuclear Engineering and Technology, 41(1), 99-106 (2009).
  5. Gauld, I.C., Herman, O.W., Westfall, R.M., "ORIGEN-S: Scale system module to calculate fuel depletion, actinide transmutation, fission product burnup and decay, and associated radiation source terms", ORNL-TM-2005/39 Version 6, Oak Ridge National Laboratory (2009).
  6. Takeo Adachi, Mamoru Ohnuki, Sen-ichi etc., "Dissolution study of spent nuclear fuels," JAERI-M91-010, p43 (1991).
  7. C. E. Sanders, I. C. Gauld, "Isotopic analysis of high-burnup PWR spent fuel samples from the Takahama-3 reactor", NUREG/CR-6798, ORNL/TM-2001/259, (2003).
  8. Shin Ichi Koyama, Yuko Otsuka, Masahiko Osaka, Katsfumi Morozumi, Koichi Konno, Mikio Kajatani and, Toshiaki Mitsugashira, "Analysis of Minor Actinides in Mixed Oxide Fuel Irradiated in Fast Reactor, (I), Determination of Np-237", J. Nuclear Science and Technology, Vol 3(6), 406-410(1998).
  9. J. M. Barrero Moreno, M. Betti and J. I. Garcia Alonso, "Determination of Neptunium and plutonium in the presence of high concentration of uranium by ion chromatographyinductively coupled plasma mass spectrometry," J. Analytical Atomic Spectrometry, 12, 355-361 (1997).
  10. J.I. Garcia Alonso, Fabrizio Sena, Philippe Arbore, Maria. Betti and Lothar Koch, "Determination of fission products and actinides in spent nuclear fuels by isotope dilution ion chromatography inductively coupled plasma mass spectrometry." J. Analytical Atomic Spectrometry, 10, 381-393 (1995),
  11. M. C. Brady, T. L. Sanders, "A validated Methodology for Evaluating Burnup Credit in Spent Fuel Cask," CONF-910993-7, Oak Ridge National Laboratory (1991).
  12. U.S. DOE, "Isotope validation for PWR actinide-only burnup credit using Yankee Rowe Data," DOE/RW/00134-M97-020, U.S. DOE (1997).
  13. Meraj Rahimi, Dale Lancaster, Bernie Hoeffer and Marc Nicols, "Isotopic Biases for actinide-only burnup credit," CONF-970607-8, Oak Ridge National Laboratory (1997).
  14. Emilio Fuentes, Dale B. Lancaster and Meraj Rahimi, "Actinide-only burnup credit for pressurized water reactor spent nuclear fuel-II: Validation," Nuclear Technology, 125, 271-291 (1999).
  15. Nicolaou, G, "Provenance of unknown plutonium material", J. Environmental Radioactivity, 99, 1708-1710(2008).
  16. G. Rosner, R. Winkler, M. Yamamoto, "Simultaneous radiochemical determination of $^{237}Np\;and\;^{239}Np\;with\;^{235}Np$ as a tracer, and application to environmental samples", J. Radioanal. and Nucl. Chem., Articles, 173(2), 273-281 (1993).
  17. Timothy C. Kenna, "Determination of plutonium isotopes and neptunium-237 in environmental samples by inductively coupled plasma mass spectrometry with total sample dissolution", J. Anal. At. Spectrom., 17, 1471-1479(2002).

Cited by

  1. Atomic spectrometry update. Review of advances in the analysis of metals, chemicals and functional materials vol.29, pp.11, 2014,
  2. Tailored Bifunctional Polymer for Plutonium Monitoring vol.86, pp.13, 2014,
  3. Electrochemical preparation and spectroelectrochemical study of neptunium chloride complexes in LiCl–KCl eutectic melts vol.308, pp.1, 2016,