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Chlorination of TRU/RE/SrOx in Oxide Spent Nuclear Fuel Using Ammonium Chloride as a Chlorinating Agent

  • Received : 2022.05.30
  • Accepted : 2022.06.28
  • Published : 2022.06.30

Abstract

Thermodynamically, TRUOx, REOx, and SrOx can be chlorinated using ammonium chloride (NH4Cl) as a chlorinating agent, whereas uranium oxides (U3O8 and UO2) remain in the oxide form. In the preliminary experiments of this study, U3O8 and CeO2 are reacted separately with NH4Cl at 623 K in a sealed reactor. CeO2 is highly reactive with NH4Cl and becomes chlorinated into CeCl3. The chlorination yield ranges from 96% to 100%. By contrast, U3O8 remains as UO2 even after chlorination. We produced U/REOx- and U/SrOx-simulated fuels to understand the chlorination characteristics of the oxide compounds. Each simulated fuel is chlorinated with NH4Cl, and the products are dissolved in LiCl-KCl salt to separate the oxide compounds from the chloride salt. The oxide compounds precipitate at the bottom. The precipitate and salt phases are sampled and analyzed via X-ray diffraction, scanning electron microscope-energy dispersive spectroscopy, and inductively coupled plasma-optical emission spectroscopy. The analysis results indicate that REOx and SrOx can be easily chlorinated from the simulated fuels; however, only a few of U oxide phases is chlorinated, particularly from the U/SrOx-simulated fuels.

Keywords

Acknowledgement

This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korean Ministry of Science, ICT (MSIT) (No. 2021M2E3A1040059) and the KAERI Institutional Project (No. 522320-22).

References

  1. H.S. Park, "The Status of the Radioactive Waste Management in Korea", Int. Symp. on Technologies for the Management of Radioactive Waste From Nuclear Power Plants and Back End Nuclear Fuel Cycle Activities, IAEA-SM-357/62, IAEA (2001).
  2. B. Aguila, D. Banerjee, Z. Nie, Y. Shin, S. Ma, and P.K. Thallapally, "Selective Removal of Cesium and Strontium Using Porous Frameworks From High Level Nuclear Waste", Chem. Commun., 52, 5940-5942 (2016). https://doi.org/10.1039/c6cc00843g
  3. W.L. Lennemann, "The Management of High-Level Radioactive Wastes", IAEA Bull., 21(4), 1-16 (1979).
  4. H. Felveson, Z. Mian, M.V. Ramana, and F.V. Hippel. Managing Spent Fuel From Nuclear Power Reactors. Experience and Lessons From Around the World, International Panel on Fissile Materials Report (2011).
  5. International Atomic Energy Agency, Spent Fuel Reprocessing Options, IAEA-TECDOC-1587 (2009).
  6. J.P. Ackerman, "Chemical Basis for Pyrochemical Reprocessing of Nuclear Fuel", Ind. Eng. Chem. Res., 30(1), 141-145 (1991). https://doi.org/10.1021/ie00049a022
  7. Nuclear Energy Agency. Pyrochemical Separations in Nuclear Applications: A Status Report, NEA Report, NEA No. 5427 (2004).
  8. M.F. Simpson and J.D. Law. Nuclear Fuel Reprocessing, Idaho National Laboratory Report, INL/EXT-10-17753 (2010).
  9. N. Aizawa, D. Maeda, K. Owada, and T. Iwasaki, "Development of Radiation Characteristics Analysis Code System for Geological Disposal and Application to Vitrified Waste Disposal With Various LWR Burnup Conditions", Ann. Nucl. Energy, 167, 108761 (2022). https://doi.org/10.1016/j.anucene.2021.108761
  10. G. Bracke, F. Charlier, A. Liebscher, F.R. Schilling, and T. Rockel, "About the Possibility of Disposal of HLRW in Deep Boreholes in Germany", Geosciences, 7(3), 58 (2017). https://doi.org/10.3390/geosciences7030058
  11. B. Jeon, S. Choi, S. Lee, and S. Jeon, "A Conceptual Study for Deep Borehole Disposal of High Level Radioactive Waste in Korea", Tunn. Undergr. Space, 29(2), 75-88 (2019). https://doi.org/10.7474/TUS.2019.29.2.075
  12. H. Lee, G.I. Park, J.W. Lee, K.H. Kang, J.M. Hur, J.G. Kim, S. Paek, I.T. Kim, and I.J. Cho, "Current Status of Pyroprocessing Development at KAERI", Sci. Technol. Nucl. Install., 2013, 343492 (2013).
  13. International Atomic Energy Agency, Spent Fuel and High Level Waste: Chemical Durability and Performance Under Simulated Repository Conditions, IAEA-TECDOC-1563 (2007).
  14. H.S. Park, I.T. Kim, Y.Z. Cho, S.W. Park, and E.H. Kim, "Stabilization/Solidification of Radioactive Molten Salt Waste by Using xSiO2-yAl2O3-zP2O5 Material", Atalante 2008-Nuclear Fuel Cycle for a Sustainable Future, P4-18, Atalante, Montpellier (2008).
  15. H.C. Eun, J.H. Choi, I.H. Cho, H.S. Park, and G.I. Park, "Separation and Solidification of Rare Earth Nuclides From LiCl-KCl Based Eutectic Waste Salts Using a Series of Phosphorylation/Distillation/Solidification Processes", J. Nucl. Fuel Cycle Waste Technol., 11(4), 325-332 (2013). https://doi.org/10.7733/JNFCWT-K.2013.11.4.325
  16. G.I. Park, M.K. Jeon, J.H. Choi, K.R. Lee, S.Y. Han, I.T. Kim, Y.Z. Cho, and H.S. Park, "Recent Progress in Waste Treatment Technology for Pyroprocessing at KAERI", J. Nucl. Fuel Cycle Waste Technol., 17(3), 279-298 (2019). https://doi.org/10.7733/jnfcwt.2019.17.3.279
  17. W.M. Haynes, CRC Handbook of Chemistry and Physics, 95th ed., CRC Press, Hoboken, New Jersey (2014).
  18. H.G. Stewart, T.D. Humphries, D.A. Sheppard, M.S. Tortoza, M.V. Sofianos, S. Liu, and C.E. Buckley, "Ammonium Chloride-metal Hydride Based Reaction Cycle for Vehicular Aapplications", J. Mater. Chem. A, 7, 5031-5042 (2019). https://doi.org/10.1039/c9ta00192a
  19. A. Roine, "HSC Chemistry Software (version 10.0.6.7)", Metso Outotec, Available from: www.outotec.com/HSC (2021).
  20. J.W. Lee, S.C. Jeon, J.H. Lee, K.Y. Lee, and Y.Z. Cho, "Thermal Treatment for the Detachment of RE-rich Particles precipitated by the High-Temperature Oxidation of (U, RE)3O8 Powder", Ceramics International, 42(14), 16120-16126 (2016). https://doi.org/10.1016/j.ceramint.2016.07.128