Abstract
The effects of calcium, hydroxide, and carbonate on the displacement of Sr from four organic chelates: ethylenedinitrilotetraacetic acid (EDTA), N-(2-hydroxyethyl)ethylenedinitrilotriacetic acid (HEDTA) nitrilotriacetic acid (NTA), and iminidiacetic acid (IDA) was studied in solutions with high base and carbonate concentration. Comparison of solutions with and without added chelators allowed the speciation changes in solution to be directly determined. Increases in both carbonate and calcium concentration were effective in displacing Sr from the chelators even under high carbonate concentration. Increases in hydroxide were ineffective in removal of Sr from the chelators, even at base concentrations as high as 6M. Under certain specific conditions, most notably when both CaCO3(s) and SrCO3(s) are present in solution, chemical equilibrium constraints result in cancelation of activity coefficient changes for aqueous Sr and Ca organic chelate complexes. Under such conditions the predicted ratios of chelated Ca and Sr become independent of the ionic media and predictive relations using known equilibrium constants give very good representations of the experimental data. These results indicate that manipulation of metal ion displacement reactions during chemical processing of Sr–chelate solutions can result in the displacement of Sr from organic chelators. The implications of such strategies in processing high level waste supernatants stored at Department of Energy (DOE) sites is discussed.
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REFERENCES
N. A. Berg and E. M. Yakimets, Russ. J. Inorg. Chem. 17, 174 (1972).
R. A. Care and L. A. K. Staveley, J. Chem. Soc. 4, 4571 (1956).
F. F. Carini and A. E. Martell, J. Am. Chem. Soc., p. 2153 (1954).
R. G. Charles, J. Am. Chem. Soc., p. 5854 (1954).
H. S. Hendrickson, Anal. Chem. 39, 998 (1967).
W. C. E. Higginson, J. Chem. Soc. 2, 2761 (1962).
J. K. Hovey, L. G. Hepler, and P. R. Tremaine, J. Solution Chem. 15, 977 (1986).
J. K. Hovey and P. R. Tremaine, J. Phys. Chem. 89, 5541 (1985).
N. N. Matorina and N. D. Safornova, Russ. J. Inorg. Chem. 5, 151 (1960).
N. M. Prutkova, L. I. Martynenko, A. I. Grigor'ev, and N. D. Mitrofanova, Russ. J. Inorg. Chem. 12, 62 (1967).
R. W. Schmid and N. Reilley, J. Am. Chem. Soc., p.5513 (1956).
L. A. K. Staveley and T. Randall, Disc. Faraday Soc. 26, 157 (1958).
V. P. Vasil'ev and A. K. Belonogova, Russ. J. Inorg. Chem. 21, 31 (1976).
D. L. Wright, J. H. Holloway, and C. N. Reilley, Anal. Chem. 37, 884 (1965).
G. Anderegg, Critical Survey of Stability Constants for EDTA Complexes, (IUPAC Chemical Data Series No. 14. 1977).
G. Anderegg, Pure Appl. Chem. 54, 2693 (1982).
A. E. Smith and R. E. Martell, Critically Selected Stability Constants of Metal Complexes Database, Version 2.0 (NIST Standard Reference Data Program, Gaithersburg, MD, 1995).
A. P. Toste, R. B. Lucke, T. J. Lechner-Fish, D. J. and Hendren, in Proceedings, Waste Management '87, Tucson, Arizona, March 1–5. (1987).
J. A. Campbell, R. W. Stromatt, M. R. Smith, D. W. Koppenaal, R. M. Bean, T. E. Jones, D. M. Strachan, and H. Babad, Anal. Chem. 66, 1207A (1994a).
J. A. Campbell, S. A. Clauss, K. E. Grant, V. Hoopes, B. D. Lerner, R. B. Lucke, G. M. Mong, J. Rau, and R. Steele, PNL-10127 (Pacific Northwest Laboratory, Richland, Washington, 1994b).
J. A. Campbell, S. A. Clauss, K. E. Grant, V. Hoopes, B. D. Lerner, R. B. Lucke, G. M. Mong, J. Rau, and R. Steele, PNL-9062 (Pacific Nortwest Laboratory, Richland, Washington, 1994c).
J. A. Campbell, G. M. Mong, S. A. Clauss, and R. B. Lucke, in Proceedings of 43rd ASMS Conference on Mass Spectrometry and Allied Topics, Atlanta, Georgia, May 21–25, p. 846a (1995a).
J. A. Campbell, S. A. Clauss, V. Hoopes, J. Rau, K. L. Wahl, K. E. Grant, G. M. Mong, and R. T. Steele, PNL-10776, (Pacific Northwest Laboratory, Richland, Washington, 1995b).
K. E. Grant, R. B. Lucke, S. A. Clauss, G. M. Mong, B. D. Lerner, and J. A. Campbell, PNL-SA-26134, Pacific Northwest Laboratory, Richland, Washington (submitted to Anal. Chem.) (1995).
J. Duchesne and E. J. Reardon, Cement Concrete Res. 25, 1043 (1995).
G. J. Lumetta, I. E. Burgeson, M. J. Wagner, J. Liu, and Y. L. Chen, Washing and Caustic Leaching of Hanford Tank Sludge: Results of FY 1997 Studies. PNNL-11636 (Pacific Northwest National Laboratory, Richland, WA (1997).
L. A. Sadokhina, G. V. Zimina, V. N. Sbitneva, and I. F. Poletaev, Russ. J. Inorg. Chem. 32, 1353 (1987).
A. R. Felmy, D. A. Dixon, J. R. Rustad, M. J. Mason, and L. M. Onishi, J. Chem. Thermodyn. accepted for publication (1998).
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Felmy, A.R., Mason, M.J. The Displacement of Sr from Organic Chelates by Hydroxide, Carbonate, and Calcium in Concentrated Electrolytes. Journal of Solution Chemistry 27, 435–454 (1998). https://doi.org/10.1023/A:1022652621788
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DOI: https://doi.org/10.1023/A:1022652621788