Effect of acetohydroxamic acid on the extraction of plutonium by dilute tri-n-butyl phosphate/n-dodecane in the presence of a high concentration of Al(NO3)3

Abstract

Acetohydroxamic acid (AHA) is a hydrophilic organic complexing agent with excellent masking or stripping effects on the tetravalent actinides in the extraction operations. Therefore, AHA is a promising reagent for the spent nuclear fuel reprocessing. In the reprosessing of spent uranium-aluminum fuel with a high U-235 enrichment which is used in research reactor, the dissolver solution contains a high concentration of Al(NO3)3, several orders of magnitude higher than that of minor actinides such as plutonium, and dilute tri-n-butyl phosphate(TBP)/n-dodecane is adopted as the extractant. In this research, complexation of Pu(IV) with AHA under the condition of U-Al fuel reprocessing is investigated. Results show that Al(NO3)3 insignificantly affects the mentioned complexation reaction. Further, the possibility of uranium purification against Pu(VI) is also investigated by using AHA in the presence of a high concentration of Al(NO3)3 by simulating some experiments on the separation process.

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References

  1. 1.

    Chatterjee B (1978) Donor Properties of Hydroxamic Acids. Coord Chem Rev 26:281–303

    CAS  Article  Google Scholar 

  2. 2.

    Tkac P, Matteson B, Bruso J, Paulenova A (2008) Complexation of uranium(VI) with acetohydroxamic acid. J Radioanal Nucl Chem 282:31–36

    Article  Google Scholar 

  3. 3.

    Weifang Z, Zefu Z, Zhangji L (2001) Study on separation of Np from Acetohyroxamic acid in Purex process. Chin J Nucl Sci Eng 21:369–374

    Google Scholar 

  4. 4.

    Brent S, Matteson D (2010) The chemistry of acetohydroxamic acid related to nuclear reprocessing, Oregon stage university.

  5. 5.

    Monzyk B, Crumbliss AL (1980) Acid dissociation constants(Ka) and their temperature dependencies(△Ha, △Sa) for a series of carbon- and nitrogen- substituted hydroxamic acids in aqueous solution. J Org Chem 45:4670–4675

    CAS  Article  Google Scholar 

  6. 6.

    Andrieux FPL, Boxall C, Taylor RJ (2007) The hydrolysis of hydroxamic acid complexants in the presence of non-oxidising metal ions 1: Ferric ions. J Solution Chem 36:1201–1217

    CAS  Article  Google Scholar 

  7. 7.

    Farkas E, Kozma E, Kiss T (1995) Role of the NH3+ Moiety in Iron(III)-, Aluminium(III)- and Gallium(III)-Aminohydroxamate Interactions. J Chem Soc Dalton Trans 3:477–481

    Article  Google Scholar 

  8. 8.

    Carrott MJ, Fox OD, Jones CJ, Mason C, Taylor RJ, Sinkov SI, Choppin GR (2007) Solvent extraction of plutonium ions in the presence of simple hydroxamic acids. Solvent Extr Ion Exch 25:723–745

    CAS  Article  Google Scholar 

  9. 9.

    Zhaokun L (1987) Aluminum hydrochemical reaction and its morphological composition. Chin J Environ Eng 8:1–9

    Google Scholar 

  10. 10.

    Metivier H, Guilaumont R (1972) Hydrolyse du plutonium tetravalent. Radiochem Radioanal Lett 10:27–35

    CAS  Google Scholar 

  11. 11.

    Berg JM, Veirs DK, Vaughn RB et al (1998) Plutonium(IV) mononitrate and dinitrate complex formation in acid solutions as a function of ionic strength. J Radioanal Nucl Chem. 235:25–29

    CAS  Article  Google Scholar 

  12. 12.

    Xiao C-L, Wu Q-Y, Wang C-Z et al (2014) Quantum chemistry study of uranium(VI), neptunium(V), and plutonium(IV, VI) complexes with preorganized tetradentate phenanthrolineamide ligands. J Inorg Chem. 53:10846–10853

    CAS  Article  Google Scholar 

  13. 13.

    Tkac P, Paulenova A, Vandegrift GF, etc, (2010) Modeling of Pu(IV) Extraction by Tri-n-butyl Phosphate from Acidic Nitrate Media Containing Acetohydroxamic Acid. J Chem Eng Data 55:3445–3450

    CAS  Article  Google Scholar 

  14. 14.

    Gelis AV, Kozak P, Breshears AT et al (2019) Closing the nuclear fuel cycle with a simplified minor actinide lanthanide separation process (ALSEP) and additive manufacturing. Sci Rep. 9:12842

    Article  Google Scholar 

  15. 15.

    Mingjian He (2019). Complexation of actinides and analogues with hydroxamate ligands. Radiochemistry. Universite Paris-Saclay. NNT: 2019SACLS413.

  16. 16.

    Quach DL, Mincher BJ, Wai CM (2014) Supercritical fluid extraction and separation of uranium from other actinides. J Hazard Mater 274:360–366

    CAS  Article  Google Scholar 

  17. 17.

    Andreas W, Fabian K, Dimitri S et al (2020) Countercurrent actinide lanthanide separation process(ALSEP) demonstration test with a simulated PUREX raffinate in centrifugal contactors on the laboratory scale. Appl Sci 10:7217–7237

    Article  Google Scholar 

  18. 18.

    Garcia IS, Bonales LJ, Galan H, Perlado JM, Cobos J (2019) Spectroscopic study of acetohydroxamic acid (AHA) hydrolysis in the presence of europium. Implications in the extraction system studies for lanthanide and actinide separation. New J Chem. 43:15714–15722

    Article  Google Scholar 

  19. 19.

    Johnson GL, Toth LM R (1978) ORNL/TM-6365, Plutonium(IV) and Thorium(IV) Hydrous Polymer Chemistry. https://inis.iaea.org/collection/NCLCollectionStore/_Public/09/407/9407265.pdf

  20. 20.

    Berg JM, Veirs DK, Vaughn RB, Cisneros MA, Smith CA (1998) Plutonium(IV) mononitrate and dinitrate complex formation in acid solutions as a function of ionic strength. J Radioanal Nucl Chem 235:25–29

    CAS  Article  Google Scholar 

  21. 21.

    Tkac P, Paulenova A, Vandegrift GF, Krebs JF (2009) Modeling of Pu(IV) extraction from acidic nitrate media by tri-n-butyl phosphate. J Chem Eng Data 54:1967–1974

    CAS  Article  Google Scholar 

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Correspondence to Hui Wang.

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Sun, Y., Liu, F., Wang, X. et al. Effect of acetohydroxamic acid on the extraction of plutonium by dilute tri-n-butyl phosphate/n-dodecane in the presence of a high concentration of Al(NO3)3. J Radioanal Nucl Chem 327, 1121–1129 (2021). https://doi.org/10.1007/s10967-021-07602-5

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Keywords

  • U-Al fuel
  • Spent nuclear fuel reprocessing
  • Acetohydroxamic acid
  • Plutonium