Distribution and identification of Plutonium(IV) species in tri-n-butyl phosphate/HNO3 extraction system containing acetohydroxamic acid

  • P. Tkac
  • A. Paulenova
  • G. F. Vandegrift
  • J. F. Krebs
Radiochemistry

Abstract

There was a significant research progress achieved with the aim to modify conventional PUREX process by stripping of plutonium from the tri-n-butyl phosphate (TBP) extraction product in the form of non-extractable complexes upon addition of back-hold complexation agents. The present paper reports effects of such salt-free complexant, acetohydroxamic acid (HAHA), on distribution ratio of Pu(IV) under wide concentration of nitric acid and additional nitrate. General formula of plutonium species present in the organic phase can be described as Pu(OH)x(AHA)y(NO3)4−x−y·2TBP·wHNO3.

Preview

Unable to display preview. Download preview PDF.

Unable to display preview. Download preview PDF.

References

  1. 1.
    R. J. Taylor, I. May, A. L. Wallwork, I. S. Denniss, N. J. Hill, B. Y. Galkin, B. Y. Zilberman, J. All. Comp., 271–273 (1998) 534.CrossRefGoogle Scholar
  2. 2.
    I. May, R. J. Taylor, I. S. Denniss, A. L. Wallwork, Czech J. Phys., 49 (1999) 597.CrossRefGoogle Scholar
  3. 3.
    G. Karraker, Radiation chemistry of acetohydroxamic acid in the UREX process, Westinghouse Savannah River Company, WSRC-TR-2002-00283, (2002).Google Scholar
  4. 4.
    M. J. Carrott, O. D. Fox, C. J. Jones, C. Mason, R. J. Taylor, S. I. Sinkov, G. R. Choppin, Solv. Extr. Ion Exch., 25(6) (2007) 723.CrossRefGoogle Scholar
  5. 5.
    J. E. Birkett, M. J. Carrott, O. D. Fox, C. J. Jones, C. J. Maher, C. V. Roube, R. J. Taylor, D. A. Woodhead, J. Nucl. Sci. Tech., 44 (2007) 337.CrossRefGoogle Scholar
  6. 6.
    A. Paulenova, P. Tkac, B. S. Matteson, Speciation of Plutonium and Other Metals Under Urex Process Conditions, Proceeding of GLOBAL 2007: Advanced Nuclear Fuel Cycles and Systems, September 9–13, 2007, Boise, ID, USA, 723–727.Google Scholar
  7. 7.
    P. Tkac, A. Paulenova, The effect of acetohydroxamic acid on extraction and speciation of plutonium, Separ. Sci. Technol., 43 (2008) 2670.CrossRefGoogle Scholar
  8. 8.
    P. Tkac, A. Paulenova, G. F. Vandegrift, J. F. Krebs, Modeling of Pu(IV) extraction from acidic nitrate media by tri-n-butyl phosphate, J. Chem. Eng. Data, accepted for publication.Google Scholar
  9. 9.
    H. Nitsche, S. C. Lee, R. C. Gatti, J. Radioanal. Nucl. Chem., 124 (1988) 171.CrossRefGoogle Scholar
  10. 10.
    K. Veirs, C. A. Smith, J. M. Berg, B. D. Zwick, S. F. Marsh, P. Allen, S. D. Conradson, J. All. Comp., 213/214 (1994) 328.CrossRefGoogle Scholar
  11. 11.
    J. M. Berg, D. K. Veirs, R. B. Vaughn, M. A. Cisneros, C. A. Smith, J. Radioanal. Nucl. Chem., 235 (1998) 25.CrossRefGoogle Scholar
  12. 12.
    J. M. Berg, D. K. Veirs, R. B. Vaughn, M. R. Cisneros, C. A. Smith, Appl. Spec., 54(6) (2000) 812.CrossRefGoogle Scholar
  13. 13.
    H. Metivier, R. Guillaumont, Radiochem. Radioanal. Lett., 10(2) (1972) 27.Google Scholar
  14. 14.
    S. E. Solovkin, Atomic Energy, 30(6), (1971) 673.CrossRefGoogle Scholar
  15. 15.
    V. N. Rubisov, S. E. Solovkin, Atomic Energy, 52(6), (1982) 400.CrossRefGoogle Scholar
  16. 16.
    M. Alyapyshev, A. Paulenova, M. A. Cleveland, J. E. Bruso, P. Tkac, Hydrolysis of acetohydroxamic acid under UREX+ conditions, Proceeding of GLOBAL 2007: Advanced Nuclear Fuel Cycles and Systems, September 9–13, 2007, Boise, ID, USA, 1861–1864.Google Scholar
  17. 17.
    F. P. L. Andrieux, C. Boxall, I. May, R. J. Taylor, J. Solution. Chem., 37 (2008) 215.CrossRefGoogle Scholar
  18. 18.
    H. A. C. McKay, Tri-n-butyl Phosphate as an Extracting Agent for the Nitrates of the Actinide Elements, Proceedings of the International Conference on the Peaceful Uses of Atomic Energy, 7 (1956) 314.Google Scholar
  19. 19.
    G. Petrich, Z. Kolarik, The 1981 Purex Distribution Data Index, Kernforschungszentrum Karlsruhe, KfK 3081, 1981.Google Scholar
  20. 20.
    P. Tkac, A. Paulenova, Spectroscopic Evidence of Extraction of Hydrolyzed Pu(IV) Species by Tri-n-butyl Phosphate., Radiochim. Acta, submitted.Google Scholar
  21. 21.
    R. Chiarizia, M. P. Jensen, M. Borkowski, J. R. Ferraro, P. Thiyagarajan, K. C. Littrell, Solv. Extr. Ion Exch., 21(1) (2003) 1.CrossRefGoogle Scholar
  22. 22.
    P. Tkac, B. Matteson, J. Bruso, A. Paulenova, J. Radioanal. Nucl. Chem., 277(1) (2008) 31.CrossRefGoogle Scholar
  23. 23.
    P. Tkac, A. Paulenova, K. Gable, Appl. Spectrosc., 61(7) (2007) 772.CrossRefGoogle Scholar
  24. 24.
    P. Tkac, A. Paulenova, Sep. Sci. Technol., 43 (2008) 2641.CrossRefGoogle Scholar

Copyright information

© Akadémiai Kiadó, Budapest, Hungary 2009

Authors and Affiliations

  • P. Tkac
    • 1
  • A. Paulenova
    • 2
  • G. F. Vandegrift
    • 3
  • J. F. Krebs
    • 3
  1. 1.Radiation CenterOregon State UniversityCorvallisUSA
  2. 2.Department of Nuclear Engineering & Radiation Health PhysicsOregon State UniversityCorvallisUSA
  3. 3.Argonne National LaboratoryChemical Technology DivisionArgonneUSA

Personalised recommendations