Automated extraction chromatographic separations of actinides using separation-optimized sequential injection techniques

(Note: The full text of this document is currently only available in the PDF Version )

Jay W. Grate, Oleg B. Egorov and Sandra K. Fiskum


Abstract

A sequential injection (SI) separation system has been developed for automated analytical separations of actinides using an actinide specific extraction chromatographic material (TRU-resin, Eichrom Industries, Inc., USA). On-line liquid scintillation counting was used to observe eluting species during method development, and fraction collection and alpha energy analysis were used for quantification. Several procedures for individual and group actinide elution are demonstrated and discussed, including elution of actinides as a single group; elution as groups based on valence state; selective separation of Pu using on-column redox chemistry; selective separation of Th; and various sequential actinide elution schemes. Eluent solution compositions and reagent chemistries were investigated with regard to elution peak shapes, selectivity, recoveries, carryover, and suitability for rapid automated procedures. The SI separation methods described serve as the basis for an automated actinide separation work station. An automated actinide separation procedure has been applied towards the analysis of Am, Cm, and Pu isotopes in three types of aged nuclear waste samples. Results from automated analytical separations followed by quantification by alpha spectroscopy were in good agreement with results obtained using manual separation techniques.


References

  1. M. D. Erickson, J. H. Aldstadt, J. S. Alvarado, J. S. Crain, K. A. Orlandin and L. L. Smith, J. Hazard. Mater., 1995, 41, 351 CrossRef CAS.
  2. R. L. Murray, Understanding Radioactive Waste, 4th edn., Battelle Press, Richland, Washington, 1994, p. 212 Search PubMed.
  3. E. P. Horwitz, R. Chiarizia, M. L. Dietz, H. Diamond and D. M. Nelson, Anal. Chim. Acta, 1993, 281, 361 CrossRef CAS.
  4. E. P. Horwitz, R. Chiarizia and M. L. Dietz, Solvent Extr. Ion Exch., 1992, 10, 313 Search PubMed.
  5. E. P. Horwitz, M. L. Dietz, R. Chiarizia, H. Diamond, S. L. Maxwell and M. R. Nelson, Anal. Chim. Acta, 1995, 310, 63 CrossRef CAS.
  6. M. L. Dietz and E. P. Horwitz, LC-GC, 1993, 11, 424 Search PubMed.
  7. S. L. Maxwell, Radioact. Radiochem., 1997, 8, 36 Search PubMed.
  8. J. L. Cortina and A. Warshawsky, Ion Exch. Solvent Extr., 1997, 13, 195 Search PubMed.
  9. E. P. Horwitz, M. L. Dietz, H. Diamond, J. J. LaRosa and W. D. Fairman, Anal. Chim. Acta, 1990, 238, 263 CrossRef CAS.
  10. R. S. Strebin, Separation of Am and Pu and Actinide Screen by Extraction Chromatography-PNL-ALO-417 in Analytical Chemsitry. Laboratory Procedure Compendium PNL-MA-599, Pacific North-west National Laboratory, 1993 Search PubMed.
  11. J. H. Kaye, R. S. Strebin and R. D. Orr, J. Radioanal. Nucl. Chem., 1995, 194, 191 CAS.
  12. Americium, Plutonium and Uranium in Water. Analytical Procedure, EIChrom Industries, Inc., Darien, IL, ACW03, 1995.
  13. S. L. Maxwell and M. R. Nelson, Institute of Nuclear Material Management 35th Annual Meeting, Naples, FL, 1994 Search PubMed.
  14. L. L. Smith, J. S. Crain, J. S. Yaeger, E. P. Horwitz, H. Diamond and R. Chiarizia, J. Radioanal. Nucl. Chem., 1995, 194, 151 CAS.
  15. J. S. Crain, L. L. Smith, J. S. Yaeger and J. A. Alvarado, J. Radioanal. Nucl. Chem., 1995, 194, 133 CAS.
  16. J. Ruzicka and E. H. Hansen, Flow Injection Analysis, 2nd edn.; Wiley, New York, 1988, vol. 62, p. 498 Search PubMed.
  17. Z. Fang, Flow Injection Separation and Preconcentration, VCH, Weinheim, 1993 Search PubMed.
  18. J. Ruzicka, Analyst, 1994, 119, 1925 RSC.
  19. J. W. Grate and O. B. Egorov, Anal. Chem., 1998, 70, 779A CAS.
  20. M. Hollenbach, J. Grohs, S. Mamich, M. Kroft and E. R. Denoyer, J. Anal. At. Spectrom., 1994, 9, 927 RSC.
  21. J. H. Aldstadt, J. M. Kuo, L. L. Smith and M. D. Erickson, Anal. Chim. Acta, 1996, 319, 135 CrossRef CAS.
  22. J. W. Grate, R. S. Strebin, J. Janata, O. Egorov and J. Ruzicka, Anal. Chem., 1996, 68, 333 CrossRef CAS.
  23. O. Egorov, M. J. O'Hara, J. Ruzicka and J. W. Grate, Anal. Chem., 1998, 70, 977 CrossRef CAS.
  24. O. Egorov, J. W. Grate and J. Ruzicka, J. Radioanal. Nucl. Chem., 1998, 234, 231 CAS.
  25. J. W. Grate and O. Egorov, Anal. Chem., 1998, 70, 3920 CrossRef CAS.
  26. J. W. Grate, S. K. Fadeff and O. Egorov, Analyst, 1999, 124, 203 RSC.
  27. O. Egorov, M. J. O’Hara, J. W. Grate and J. Ruzicka, Anal. Chem., 1998, 71, 345 CrossRef CAS.
  28. J. Ruzicka, Anal. Chim. Acta, 1992, 261, 3 CrossRef CAS.
  29. J. M. Cleveland, The Chemistry of Plutonium, Gordon and Breach, Science Publishers, New York, 1970 Search PubMed.
  30. Plutonium Handbook. A Guide to Technology., ed. O. Wick, Gordon and Breach Science Publishers: New York, 1967; vol. 1 Search PubMed.
  31. T. W. Newton, The Kinetics of the Oxidation-Reduction Reactions of Uranium, Neptunium, Plutonium, and Americium in Aqueous Solutions, ERDA Technical Information Center, Oak Ridge, TN, 1975 Search PubMed.
  32. The Chemsitry of the Actinide Elements, A. A. Katz, G. T. Seaborg and L. R. Morss, Chapman and Hall, New York, 1986, vol. 1,2 Search PubMed.
  33. K. L. R. P. G. Nash, E. P. Lessman, M. D. Mendoza, J. F. Feil and J. C. Sullivan, New Water-Soluble Phosphanate and Polycarboxylate Complexants For Enhanced Elements Separations, Plenum Press, New York, 1995 Search PubMed.
Click here to see how this site uses Cookies. View our privacy policy here.