DISSOLUTION AND BURNUP DETERMINATION OF IRRADIATED U-Zr ALLOY NUCLEAR FUEL BY CHEMICAL METHODS

  • Published : 2006.04.01

Abstract

Destructive methods were used for the burnup determination of U-Zr alloy nuclear fuel irradiated in the High-flux Advanced Neutron Application Reactor (HANARO) at KAERI. The dissolution rate of unirradiated U-Zr alloy fuel in $HNO_3$/HF mixtures was investigated for the experimental conditions of a different temperature, and initial concentrations of HF and $HNO_3$. The irradiated U-Zr alloy fuel specimen was dissolved in a mixed acid condition of 3 M HNO3 and 1 M HF at $90^{\circ}C$ for 8 hours under reflux. The total burnup was determined from measurement of the Nd isotope burnup monitors. The method includes U, Pu, $^{148}Nd,\;^P{145}Nd+^{146}Nd,\;^{144}Nd+^{143}Nd$ and total Nd isotopes determination by the isotope dilution mass spectrometric method (IDMS) using triple spikes $(^{233}U,\;^{242}Pu\;and\;^{150}Nd)$. The effective fission yield was calculated from the weighted fission yields averaged over the irradiation period. The results are compared with that obtained by the destructive -spectrometric measurement of the $^{137}Cs$ monitor.

Keywords

References

  1. American Society for Testing and Materials Standard Method E 321-96, 'Atom Percent Fission in Uranium and Plutonium Fuel(Neodymium-148 Method)', 1 (1996)
  2. J. S. Kim, S. H. Han, M. Y. Suh, K. S. Joe and T. Y. Eom, 'Burnup Measurement of Irradiated Uranium Dioxide Fuel by Chemical Methods', J. Korean Nucl. Soc. 21(4), 277 (1989)
  3. J. S. Kim, Y. S. Jeon, K. S. Choi, B. C. Song, S. H. Han and W. H. Kim, 'Burnup Measurement of Spent U3Si/Al Fuel by Chemical Method Using Neodymium Isotope Monitors'. J. Korean Nucl. Soc. 33(4), 375 (2001)
  4. American Society for Testing and Materials Standard Method E 321-69, 'Atom Percent Fission in Uranium and Plutonium Fuel(Neodymium-148 Method)', 1045 (1969)
  5. W. J. Maeck, Review Paper No. 5, IAEA Fission Product Nuclear Data Conference, IAEA-169, Bologna, Italy, Nov.(1973)
  6. L. W. Green, N. L. Elliot, F. C. Miller and J. J. Leppinen, 'Mass Spectrometric Determination of Burnup of $(U, Pu)O_2$ Fuel Using Nanogram Quantities of Isotopes', J. Radioanal. & Nucl. Chem. Art., 131(2), 299 (1989) https://doi.org/10.1007/BF02060595
  7. H. Sorantin, 'Determination of Uranium and Plutonium in Nuclear Fuels', Kernchemie in Einzeldarstellungen; Vol. 5, Verlag Chemie, Germany (1975)
  8. Z. Goncalves and H. Munzel, 'Dissolution Kinetics of Zircaloy in $HNO_3/HF$ Mixtures', J. Nucl. Mater., 170, 261 (1990) https://doi.org/10.1016/0022-3115(90)90297-Z
  9. S. G. Ro, J. M. Park, D. K. Min, P. I. Choi and H. S. Shin, 'Radioisotope Inventories in Spent Fuel from KNU PWR', KAERI/PIED/note-001/87 (1987)
  10. L. Koch, 'Post-Irradiation Isotopic Analysis of Reactor Fuels', Analytical Chemistry of Nuclear Fuels, IAEA STI/PUB/337, 111 (1972)
  11. American Society for Testing and Materials Standard Method E 244-80 (Reapproved 1995), 'Atom Percent Fission in Uranium and Plutonium Fuel (Mass Spectrometric Method)', 1 (1996)
  12. J. E. Rein and C. F. Metz, 'Advantages and Limitations of Mass Spectrometry for the Measurement of the Isotopic Distributions of Uranium and Plutonium and Application to Nuclear Fuel Burnup', Analytical Chemistry in Nuclear Fuel Reprocessing, IAEA STI/PUB/337, 135 (1978)
  13. J. S. Kim, 'Analysis of the Irradiated Nuclear Fuel Using the Heavy Atom and Neodymium Isotope Correlations with Burnup', J. Korean Nucl. Soc., 29(4), 327 (1997)
  14. J. E. Rein, 'Status of Burnup Measurement Methodology', Analytical Methods in the Nuclear Fuel Cycle, IAEA-SM-149/40, 449 (1972)
  15. P. De Regge, De Huys, R. Boden and C. Ballaux, 'Actual Experience in Burnup Determination of Mixed Oxide Fuel', Proc. of a Technical Committee Meeting Organized by the International Atomic Energy Agency and Held in Karlsruhe, IWGFPT/31, 23 (1989)
  16. P. De Regge and R. Boden, 'Determination of Neodymium Isotopes as Burnup Indicator of Highly Irradiated $(U, Pu)O_2$ LMFBR Fuel', J. Radioanal. Chem., 35, 173 (1977) https://doi.org/10.1007/BF02518224
  17. American Society for Testing and Materials Standard Method E 219-80 (Reapproved 1985), 'Atom Percent Fission in Uranium Fuel(Radiochemical Method)', 57 (1987)
  18. W. H. Walker, Atomic Energy of Canada Limited Report AECL-3037, Part 1 and 2, Chalk River Nuclear Laboratory (1972)
  19. W. J. Maeck, W. A. Emel, L. L. Dickerson, J. E. Delmore, J. H. Keller, F. A. Duce and R. L. Tromp, 'Discrepancies and Comments Regarding 235U and 239Pu Thermal Fission Yields and the Use of 148Nd as a Burnup Monitor', Idaho Chemical Programs Report ICP-1092, Idaho National Engineering Laboratory (1976)
  20. T. R. England and B. F. Rider, 'ENDF-349 Evaluation and Compilation of Fission Product Yields 1993', Los Alamos National Laboratory Report LA-UR-94-3106, Los Alamos National Laboratory (1994)
  21. H. Kim, H. R. Kim, K. H. Lee and J. B. Lee, 'Design Characteristics and Startup Tests of HANARO', J. Nucl. Sci. Tech, 33(7), 527 (1996) https://doi.org/10.3327/jnst.33.527
  22. D. R. Lide, CRC Handbook of Chemistry and Physics, 74th ed., 11-35, CRC Press, Inc., U.S.A. (1993)