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Quantitative determination of chelators and their degradation products in mixed hazardous wastes from Tank 241-SY-101 using derivatization GC/MS

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Abstract

Considerable attention has been focused on chelators such as ethylenediaminetetraacetic acid (EDTA) and N-(2-hydroxyethyl)ethylenediaminetriacetic acid (HEDTA), which form water-soluble complexes with most heavy metals. Most radionuclides are included in this class of constituents. As a result, chelator complexes have become very important environmentally because of their tendency to enhance the mobility of heavy metals through the soil and potentially contaminate groundwater. In addition, there is a correlation between chelator concentration and crust formation/gas release. The chelators are a class of compounds whose low volatility and high polarity preclude analysis by gas chromatography/mass spectrometry (GC/MS) without prior derivatization. Waste samples from a double-shell storage tank at Hanford were derivatized with BF3/methanol and analyzed using GC/MS. Results indicate the presence of EDTA, HEDTA, nitrilotriacetic (NTA), and citric acid. Nitrosoiminodiacetic acid was identified and determined to be an artifact of the derivatization procedure; it is assumed to arise from nitrosation of iminodiacetic acid in the waste sample.

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References

  1. S. C. METCAFT, Determination of EDTA and HEDTA in Hanford Defense Waste by High Performance Liquid Chromatography, RHO-SA-218, 1991, Rockwell Hanford Operations, Richland, Washington, p 1.

    Google Scholar 

  2. J. L. MEANS, D. A. CRERAR, J. O. DUGID, Science, 200 (1978) 1477.

    Google Scholar 

  3. A. P. TOSTE, R. B. MYERS, The Relation Contributions of Natural and Waste-Derived Organics to the Subsurface Transport of Radionuclide, in: The Effects of Natural Organic Compounds and of Microorganisms on Radionuclide Transport, RWM-6, Radioactive Waste Management Committee, OECD Nuclear Energy Agency, Paris, France, 1986 p. 57.

    Google Scholar 

  4. A. P. TOSTE, J. Radioanal. Nucl. Chem., 161 (1992) 549.

    Google Scholar 

  5. D. M. STRACHAN, Minutes of the Tank Waste Science Panel, PNL-8278, March 25–27, Denver, Colorado, p. K. 1.

  6. S. A. BRYAN, L. R. PEDERSON, R. D. SCHEELE, Synthetic Waste Studies Final Report. 1992. PNL-8169, Pacific Northwest Laboratory, Richland, Washington, p. 1.

    Google Scholar 

  7. L. RUDLING, Water Res., 6 (1972) 871.

    Google Scholar 

  8. D. R. KNAPP, in: Handbook of Analytical Derivatization Reactions, John Wiley & Sons, Inc., New York, 1979, p. 21.

    Google Scholar 

  9. ORGANIC CHEMICAL DIVISION, General Procedure for the Determination of NTA, HEDTA, EDTA, and DTPA in Chelate and Metal Chelate Mixtures, RDSAP Number 0021, 1988, W. R. Grace and Company, Nashua, New Hampshire, p. 1.

    Google Scholar 

  10. J. BAUER, D. HEATCOTE, S. KROGH, J. Chromatogr. 369 (1986) 422.

    PubMed  Google Scholar 

  11. M. E. UNGER, E. MAINKA, W. KNONIG, Fresen. Anal. Chem., 329 (1987) 50.

    Google Scholar 

  12. J. DAI, G. R. HELZ, Anal. Chem., 60 (1988) 301.

    Google Scholar 

  13. J. A. CAMPBELL, R. B. LUCKE, S. A. CLAUSS, Applications of LC/MS to the Study of Chelators in Mixed Hazardous Wastes, in: Proc. 39th ASMS Conf. on Mass Spectrometry and Allied Topics, Nashville, Tennessee, May 19–24, 1991, p. 1334.

  14. J. A. CAMPBELL, H. R. UDSETH, R. B. LUCKE, Application of Electrospray Mass Spectrometry to the Analysis of Chelator and Chelator Fragments in Mixed Hazardous Wastes, in: Proc. 40th ASMS Conf. on Mass Spectrometry and Allied Topics, Washington, D. C., May 24–June 2, 1992.

  15. A. P. TOSTE, R. B. LUCKE, T. J. LECHNER-FISH, D. J. HENDREN, in: Proc. Waste Management '87, Vol. 3, March 1–5, 1987, Tucson, Arizona, p. 323.

  16. R. B. LUCKE, J. A. CAMPBELL, K. L. MCKEETA, S. A. CLAUSS, Analysis of Chelator and Chelator Fragments in Mixed Hazardous Wastes by Derivatization GC/MS, in: Proc. 39th ASMS Conference on Mass Spectrometry and Allied Topics, Nashville, Tennessee, 1991, p. 720.

  17. A. P. TOSTE, F. T. HARA, D. J. HENDREN, T. J. LECHNER-FISH, Chemical and Radiochemical Analysis of Hanford Radioactive Wastes, 1987, PNL-6360, Pacific Northwest Laboratory, Richland, Washington.

    Google Scholar 

  18. R. O. LOKKEN, R. D. SCHEELE, D. M. STRACHAN, A. P. TOSTE, Complex Concentrate Pretreatment, FY 1986 Progress Report, PNL-7687, 1986, Pacific Northwest Laboratory, Richland, Washington.

    Google Scholar 

  19. J. A. CAMPBELL, R. W. STROMATT, M. R. SMITH, D. W. KOPPENAAL, R. M. BEAN, T. E. JONES, D. M. STRACHAN, H. BABAD, Anal. Chem., 66 (1994) 1207A.

    Google Scholar 

  20. G. M. MONG, J. A. CAMPBELL, R. B. LUCKE, B. D. LERNER, K. L. WAHL, S. A. CLAUSS, K. E. GRANT, Progress in the Analysis and Speciation of Organic Chelator Compounds in Hanford Waste Tanks, in: Waste Management 95, February 27–March 3, 1995, Tucson, Arizona, in press.

  21. J. A. CAMPBELL, S. A. CLAUSS, K. E. GRANT, V. HOOPES, B. D. LERNER, R. B. LUCKE, G. M. MONG, J. RAU, R. STEELE, Flammable Gas Safety Program, Analytical Methods Development: FY 1994 Progress Report, PNL-10127, Pacific Northwest Laboratory Richland, Washington.

  22. J. A. CAMPBELL, S. A. CLAUSS, K. E. GRANT, V. HOOPES, B. D. LERNER R. B. LUCKE, G. M. MONG, J. RAU, R. STEELE, Flammable Gas Safety Program, Analytical Methods Development: FY 1993 Progess Report, PNL-9062, Pacific Northwest Laboratory Richland, Washington.

  23. A. VÁNYÓLOS, Rev. Chim. (Bucharest), 6 (1955) 378.

    Google Scholar 

  24. D. L. BALDWIN, R. W. STROMATT, W. I. WINTERS, Comparative Study of Total Organic Carbon Methods for High-Level Waste, PNL-SA-23718, Pacific Northwest National Laboratory, Richland, Wa, June 1994.

    Google Scholar 

  25. E. C. ASHBY, E. K. BAREFIELD, C. L. LIOTTA, H. M. NEUMANN, D. BOATRIGHT, F. DOCTORVICH, A. DESHPANDE, C. F. YAO, Mechanisms of the Chemical Decomposition of Complexants in Hanford HLW Simulants, presented at the 208th American Chemical Society National Meeting, Washington, D. C., August 21–25, 1994.

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Grant, K.E., Mong, G.M., Lucke, R.B. et al. Quantitative determination of chelators and their degradation products in mixed hazardous wastes from Tank 241-SY-101 using derivatization GC/MS. Journal of Radioanalytical and Nuclear Chemistry, Articles 211, 383–402 (1996). https://doi.org/10.1007/BF02039706

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