Nuclear Engineering and Technology

Korean Nuclear Society (한국원자력학회)
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DETERMINATION OF THE TRANSURANIC ELEMENTS INVENTORY IN HIGH BURNUP PWR SPENT FUEL SAMPLES BY ALPHA SPECTROMETRY

  • Published : 2007.10.30
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Abstract

The contents of transuranic elements in high-burnup spent fuel samples were determined. The activity amounts of $^{238}Pu,\;^{239}Pu,\;^{240}Pu,\;^{241}Am,\;^{244}Cm\;and\;^{242}Cm$ were measured by alpha spectrometry using $^{242}Pu\;and\;^{243}Am$ as tracers, respectively. A spike addition method for $^{237}Np$ was established by an alpha and gamma spectrometry using $^{239}Np$ as a spike after the optimum conditions for the measurements of $^{237}Np\;and\;^{239}Np$, respectively, were obtained. A separation system using anion exchange chromatography and diethylhexylphosphoric acid extraction chromatography was applied for the separation of these elements. This method was applied to high-burnup spent nuclear fuel samples $(40{\sim}60GWD/MTU)$. The contents of the transuranic elements were compared with those by ORIGEN-2 code. Measurements and the calculations of the contents of the plutonium isotopes $^{238}Pu,\;^{239}Pu\;and\;^{240}Pu$ agreed to within 10% on average. The contents of $^{237}Np$ agreed to within approximately 5% except for one instance of a calculation, while those of $^{241}Am,\;^{244}Cm\;and\;^{242}Cm$ showed higher values by approximately 19%, 35% and 14% on average, respectively, compared to the calculations according to the burnup.

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References

  1. American Society for Testing and Materials, 'Standard Methods for Atom Percent Fission in Uranium and Plutonium Fuel (Neodymium-148 Method),' ASTM E 321-96(1996)
  2. Mark W. Huntley, 'Sequential Separation of Americium, Curium, Plutonium, Neptunium and Uranium in Various Matrices from the Electrometallurgic Treatment of Spent Nuclear Fuel,' Radiochim Acta, 89, 605-612(2001) https://doi.org/10.1524/ract.2001.89.10.605
  3. 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) https://doi.org/10.1016/j.apradiso.2003.11.078
  4. 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) https://doi.org/10.1039/b205001c
  5. 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) https://doi.org/10.1007/BF02043029
  6. C. S. Kim, C. K. Kim and K. J. Lee, 'Simultaneous Analysis of $^{237}Np$ and Pu Isotopes in Environmental Samples by ICP-MS Coupled with Automated Sequential Injection System,' J. Anal. At. Spectrom., 19, 743-750, 2004 https://doi.org/10.1039/b400034j
  7. Kih-Soo Joe, Tea-Hyun Kim, Young-Shin Jeon, Kwang- Yong Jee and Won-Ho Kim, 'Determination of $^{241}Am and ^{244}Cm in Radwaste Samples,' J. of the Korean Radioactive Waste Society, 3(1), 1-7(2005)
  8. Chang Heon Lee, Moo Yul Suh, Kwang Soon Choi, Jung Suk Kim, Byong Chul Song, Kwang Yong Jee and Won Ho Kim, 'Separation of Fission Products from Spent Pressurized Water Reactor fuels by Anion Exchange and Extraction Chromatography for Inductively Coupled Plasma Atomic Emission Spectrometric Analysis,' Analytica Chimica Acta, 428, 133-142(2001) https://doi.org/10.1016/S0003-2670(00)01120-X
  9. S. Bajo, J. Eikenberg, 'Electrodeposition of Actinides for Alpha-spectrometry,' J. Radioanal. and Nucl. Chem., 243(3), 745-751(1999)
  10. Kihsoo Joe, Chang-Heon Lee, Byong-Chul Song, Young-Shin Jeon, Won-Ho Kim and Jeong-Kee Suh, 'Electrodeposition of $^{241}Am and ^{244}Cm in Spent Nuclear Fuel Samples for Alpha-spectrometry,' Bull. Kor. Chem. Soc., 24(5), 657- 660(2003) https://doi.org/10.5012/bkcs.2003.24.5.657
  11. Kihsoo Joe, Young-Shin Jeon, Tae-Hyun Kim, Kwang- Yong Jee and Won-Ho Kim, 'Evaluation of uncertainty Associated with Determination of $^{241}Am$ in Radioactive Waste Samples', Workshop on Uncertainty 2005 in KAERI, March 18, pp26-44(2005)
  12. EURACHEM Measurement Uncertainty Working Group, Draft EURACHEM/CITAC Guide, 'Quantifying Uncertainty in Analytical Measurements', Second Edition, EURACHEM Workshop, Helsinki, June 1999
  13. Croff., A. G., 'A Revised and Updated Version of Oakridge Isotope Generation and Depletion Code,' ORNL-5621, ORIGEN-2, Oak Ridge National Laboratory (1980)
  14. Shin Ichi Koyama, Masahiko Osaka, Takeshi Namekawa, Masahiko Ito, Toshiaki Mitsukashra, 'Development of Analytical Method for Neptunium and Americium in Irradiated MOX fuels Applying a New Isolation Technique based on Ion Exchange and Oxidation,' Proceedings of the 4th KAERI-JAERI Joint Seminar on PIE Technology, October 16-18, pp321-331(2002)
  15. 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)
  16. Jung Suk Kim, 'Analysis of the Irradiated Nuclear Fuel using the Heavy Atom and Neodymium Isotope Correlations with Burnup,' J. Korean Nucl. Soc. 29(4), 327-335(1997)
  17. 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)

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