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Reprocessing of simulated voloxidized uranium-oxide SNF in the CARBEX process

  • Boyarintsev, Alexander V. (Dmitry Mendeleev University of Chemical Technology of Russia) ;
  • Stepanov, Sergei I. (Dmitry Mendeleev University of Chemical Technology of Russia) ;
  • Kostikova, Galina V. (A.N. Frumkin Institute of Physical Chemistry and Electrochemistry, Russian Academy of Sciences) ;
  • Zhilov, Valeriy I. (A.N. Frumkin Institute of Physical Chemistry and Electrochemistry, Russian Academy of Sciences) ;
  • Chekmarev, Alexander M. (Dmitry Mendeleev University of Chemical Technology of Russia) ;
  • Tsivadze, Aslan Yu. (A.N. Frumkin Institute of Physical Chemistry and Electrochemistry, Russian Academy of Sciences)
  • Received : 2019.03.08
  • Accepted : 2019.05.22
  • Published : 2019.10.25

Abstract

The concept of a new method, the CARBEX (CARBonate EXtraction) process, was proposed for reprocessing of spent uranium oxide fuel. The proposed process is based on use of water solutions of $Na_2CO_3$ or $(NH_4)_2CO_3$ and solvent extraction (SE) by the quaternary ammonium compounds for selective recovery and purification of U from the fission products (FPs). Applying of SE allows to reach high degree of purification of U from FPs. Carrying out the processes in poorly aggressive alkaline carbonate media leads to increasing safety of SNF's reprocessing and better selectivity of separation of lanthanides and actinides. Moreover carbonate reprocessing media allows to carry out a recycling and regeneration of reagents. We have been done laboratory scale experiments on the extraction components of simulated voloxidated spent fuel in the solutions of NaOH or $Na_2CO_3-H_2O_2$ and recovery of U from carbonate solutions by SE method using carbonate of methyltrioctylammonium in toluene. It was shown that the purification factors of U from impurities of simulated FPs reached values $10^3-10^5$. The received results support our opinion that CARBEX after the further development can become more safe, simple and profitable method of spent fuel reprocessing.

Acknowledgement

Supported by : Dmitry Mendeleev University of Chemical Technology of Russia

References

  1. S.I. Stepanov, A.M. Chekmarev, Concept of spent nuclear fuel reprocessing, Dokl. Chem. 423 (1) (2008) 276-278. https://doi.org/10.1134/S0012500808110037
  2. H. Tomiyasu, Y. Asano, Environmentally acceptable nuclear fuel cycle development of a new reprocessing system, Prog. Nucl. Energy 32 (1998) 421-427. https://doi.org/10.1016/S0149-1970(97)00037-1
  3. N. Asanuma, Y. Asano, H. Tomiyasu, Concept of a new nuclear fuel reprocessing in non-acidic aqueous solutions, in: The 5th International Conference on Recycling, Conditioning and Disposal, Proceedings, Paris, France, October 25-28, 1998.
  4. N. Asanuma, M. Harada, Y. Ikeda, H. Tomiyasu, New approach to the nuclear fuel reprocessing in non-acidic aqueous solutions, J. Nucl. Sci. Technol. 38 (10) (2001) 866-871. https://doi.org/10.1080/18811248.2001.9715107
  5. N. Asanuma, M. Harada, M. Nogami, K. Suzuki, T. Kikuchi, H. Tomiyasu, Y. Ikeda, Anodic dissolution of $UO_2$ pellet containing simulated fission products in ammonium carbonate solution, J. Nucl. Sci. Technol. 43 (3) (2006) 255-262. https://doi.org/10.1080/18811248.2006.9711087
  6. S.M. Peper, L.F. Brodnax, S.E. Field, R.A. Zehnder, S.N. Valdez, W.H, Runde Kinetic study of the oxidative dissolution of $UO_2$ in aqueous carbonate media, J. Ind. Eng. Chem. Res. 43 (2004) 8188-8193. https://doi.org/10.1021/ie049457y
  7. G.S. Goff, F.L. Taw, S.M. Peper, L.F. Brodnax, S.E. Field, W.H. Runde, Separation of uranium from fission products in spent nuclear fuel using aqueous $H_2O_2$-carbonate solutions, in: AIChE Annual Meeting, San Francisco, United States, November 12-17, 2006.
  8. G.S. Goff, L.F. Brodnax, M.R. Cisneros, K.S. Williamson, F.L. Taw, I. May, Development of a novel alkaline based process for spent nuclear fuel recycling, in: AIChE Annual Meeting, Salt Lake City, United States, November 4-9, 2007.
  9. G.S. Goff, L.F. Brodnax, M.R. Cisneros, W.H. Runde, Redox chemistry of actinides in peroxide-carbonate media: applications to developing a novel process for spent nuclear fuel reprocessing, in: AIChE Annual Meeting, Salt Lake City, United States, November 4-9, 2007.
  10. K.W. Kim, Y.H. Kim, S.M. Kim, H.S. Seo, D.Y. Chung, H.B. Yang, J.K. Lim, K.S. Joe, E.H. Lee, A study on a process for recovery of uranium alone from spent nuclear fuel in a high alkaline carbonate media, in: Seventh International Conference on Nuclear and Radiochemistry, Budapest, Hungary, 2008, pp. 24-29. August.
  11. S.I. Stepanov, A.M. Chekmarev, Extraction of Rare Metals by the Salts of Quaternary Ammonium Bases, IzdAT, Moscow, Russia, 2004.
  12. M.M. Metalidi, S.V. Shapovalov, R.V. Ismailov, M.I. Skriplev, V.I. Beznosyuk, Y.S. Fedorov, Thermochemical embrittlement of the zirconium cladding of a fuel rod and oxidative recrystallization of the fuel material in the course of spent nuclear fuel reprocessing, Radiochemistry 57 (1) (2015) 98-102. https://doi.org/10.1134/S1066362215010154
  13. P.M. Gavrilov, E.G. Kudryavtsev, Y.A. Revenko, V.V. Bondin, Y.S. Fedorov, A.V. Khaperskaya, O.P. Anisimov, B.Y. Zilberman, Full inspection of SNF reprocessing technology for ODC at FSUE GCC in hot cells, in: 7th Russian Conference on Radiochemistry, Dimitrovgrad, Russia, 15-19 October, 2012.
  14. S.I. Stepanov, A.V. Boyarintsev, A.M. Chekmarev, Physicochemical foundations of spent nuclear fuel leaching in carbonate solution, Dokl. Chem. 427 (2) (2009) 202-206. https://doi.org/10.1134/S0012500809080060
  15. S.I. Stepanov, A.V. Boyarintsev, M.V. Vazhenkov, B.F. Myasoedov, E.O. Nazarov, A.M. Safiulina, I.G. Tananaev, H.V. So, A.M. Chekmarev, A.Yu Civadze, CARBEX Process, A new technology of reprocessing of spent nuclear fuel, Russ. J. Gen. Chem. 81 (9) (2011) 1949-1959. https://doi.org/10.1134/S1070363211090404
  16. C.Z. Soderquist, B.K. McNamara, B.М. Oliver, Dissolution of uranium metal without hydride formation or hydrogen gas generation, J. Nucl. Mater. 378 (3) (2008) 299-304. https://doi.org/10.1016/j.jnucmat.2008.05.014
  17. S.C. Smith, S.M. Peper, M. Douglas, K.L. Ziegelgruber, E.C. Finn, Dissolution of uranium oxides under alkaline oxidizing conditions, J. Radioanal. Nucl. Chem. 282 (2009) 617-621. https://doi.org/10.1007/s10967-009-0182-8
  18. K.W. Kim, J.T. Hyun, E.H. Lee, G.I. Park, K.W. Lee, M.J. Yoo, K.C. Song, J.K. Moon, Dissolution of uranium oxides under alkaline oxidizing conditions nuclear fuel scrap using dissolution and precipitation in carbonate media, J. Nucl. Mater. 418 (2011) 93-97. https://doi.org/10.1016/j.jnucmat.2011.06.019
  19. D.Y. Chung, H.S. Seo, J.W. Lee, H.B. Yang, E.H. Lee, K.W. Kim, Oxidative leaching of uranium from SIMFUEL using $Na_2CO_3-H_2O_2$ solution, J. Radioanal. Nucl. Chem. 284 (2010) 123-129. https://doi.org/10.1007/s10967-009-0443-6
  20. G.S. Goff, K.M. Long, S.D. Reilly, G.D. Jarvinen, W.H. Runde, Americium/Lanthanide separation in alkaline solution for advanced nuclear fuel cycles, in: 36th Actinide Separations Conference, Chattanooga, United States, 2012, 21-24 May.
  21. C.Z. Soderquist, A.M. Johsen, B.K. McNamara, B.D. Hanson, J.W. Chenault, K.J. Carson, S.M. Peper, Dissolution of irradiated commercial $UO_2$ fuels in ammonium carbonate and hydrogen peroxide, J. Ind Eng Chem Res. 50 (2011) 1813-1818. https://doi.org/10.1021/ie101386n
  22. S.I. Stepanov, A.V. Boyarincev, A.A. Chehlov, A.M. Chekmarev, A.Yu Tsivadze, Chemistry of the CARBEX Process. Identification of the absorption bands of the ligands in the electronic spectra of U(VI) extracts with methyltrioctylammonium carbonate, Dokl. Chem. 473 (1) (2017) 63-66. https://doi.org/10.1134/S0012500817030065
  23. G. Hongcheng, Z. Maoliang, P. Qixiu, P. Lie, W. Wenqing, The extraction of uranium from carbonate solutions by trialkyl-methyl ammonium chloride, He Hua Xue Yu Fang She Hua Xue 3 (2) (1981) 88-96.
  24. P.L. Zanonato, Z. Szabo, V. Vallet, P.D. Bernardoa, I. Grenthe, Alkali-metal ion coordination in uranyl(VI) poly-peroxo complexes in solution, inorganic analogues to crown-ethers. Part 2. Complex formation in the tetramethyl ammonium-, $Li^+-,\;Na^+-$ and $K^+$-uranyl(VI)-peroxide-carbonate systems, J. Chem. Soc., Dalton Trans. 44 (2015) 16565-16572. https://doi.org/10.1039/C5DT01710F
  25. P.L. Zanonato, P.D. Bernardoa, I. Grenthe, Chemical equilibria in the binary and ternary uranyl(VI)-hydroxide-peroxide systems, J. Chem. Soc., Dalton Trans. 41 (2012) 3380-3386. https://doi.org/10.1039/C1DT11276G
  26. M. Nogami, S.Y. Kim, N. Asanuma, Y. Ikeda, Adsorption behavior of amidoxime resin for separating actinide elements from aqueous carbonate solutions, J. Alloy. Comp. 374 (2004) 269-271. https://doi.org/10.1016/j.jallcom.2003.11.099
  27. H.B. Pan, W. Liao, C.M. Wai, Y. Oyola, C.J. Janke, G. Tianc, L. Raoc, Carbonate-$H_2O_2$ leaching for sequestering uranium from seawater, J. Chem. Soc., Dalton Trans. 43 (2014) 10713-10718. https://doi.org/10.1039/C3DT53404A
  28. K.W. Kim, Y.H. Kim, S.Y. Lee, J.W. Lee, K.S. Joe, E.H. Lee, J.S. Kim, K. Song, K.C. Song, Precipitation characteristics of uranyl ions at different pHs depending on the presence of carbonate ions and hydrogen peroxide, Environ. Sci. Technol. 43 (7) (2009) 2355-2361. https://doi.org/10.1021/es802951b
  29. E.H. Lee, H.B. Yang, K.Y. Lee, K.W. Kim, D.Y. Chung, J.K. Moon, Removal of uranium by an alkalization and an acidification from the thermal decomposed solid waste of uranium-bearing sludge, J. Korean Radioact. Waste Soc. 11 (2) (2013) 85-93. https://doi.org/10.7733/jkrws.2013.11.2.85
  30. K.W. Kim, J.T. Hyun, K.Y. Lee, E.H. Lee, K.W. Lee, K.C. Song, J.K. Moon, Effects of the different conditions of uranyl and hydrogen peroxide solutions on the behavior of the uranium peroxide precipitation, J. Hazard Mater. 193 (2011) 52-58. https://doi.org/10.1016/j.jhazmat.2011.07.032
  31. K.W. Kim, Y.H. Kim, E.H. Lee, K. Song, K.C. Song, Study on electrolytic recoveries of carbonate salt and uranium from a uranyl peroxy carbonato complex solution generated from a carbonate-leaching process, J. Ind. Eng. Chem. Res. 49 (2009) 2085-2092.
  32. K.W. Kim, Y.H. Kim, S.Y. Lee, E.H. Lee, K. Song, K.C. Song, Continuous electrolytic decarbonation and recovery of a carbonate salt solution from a metal-contaminated carbonate solution, J. Hazard Mater. 171 (2009) 606-612. https://doi.org/10.1016/j.jhazmat.2009.06.043
  33. Certificate of authorship USSR N 664355 (1979) S.I. Stepanov, Y.A. Leikin, V.D. Gorchakov, V.V. Sergievsky, G.A. Yagodin, V.N. Andrievsky, The method of obtaining salts or hydroxides of Quaternary ammonium bases.
  34. S.I. Stepanov, A.V. Boyarintsev, A.M. Chekmarev, Oxidative leaching of uranium(IV) in carbonate systems, in: Uranium of Russia, Proceedings of Scientific and Technical Conference, Moscow, Russia, 20-21 November, 2007.