Abstract
Studies of the stability of various metal EDTA, DTPA and DOTA complexes in order to evaluate their applicability as non-sorbing tracers have been performed. In laboratory tests, the stability generally increases for the individual metal ions in the EDTA<DTPA<DOTA order. For most metal ions, the same trend can be observed for the thermodynamic stability constants. In the in situ experiment, various metal EDTA tracers were used in very low concentrations; YbEDTA−, for example had a breakthrough and recovery which were very similar to the non-sorbing tracers used. According to the extremely low tracers concentrations used, thermodynamic data indicate that all metal EDTA tracers should have been decomplexed as a result of the competition with the naturally occurring cations in the groundwater. This was not found, which indicates that the decomplexation rate and sorption mechanism are important in estimating the applicability of the metal complexes as tracers. The DOTA complexes of elements in the middle of the lanthanide series have indicated high stability in the laboratory tests and therefore appear to be good candidates as non-sorbing tracers. However, in contrary to the metal EDTA, tracers, the DOTA complexes of La3+ and Lu3+ seemed to be slightly delayed in the in situ experiment.
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J. Byegård, G. Skarnemark, M. Skålberg, Mat. Res. Soc. Symp. Proc., 212 (1991) 677.
E. Gustafsson, R. Nordqvist, Swedish Nuclear Fuel and Waste Management Co., SKB Technical Report 93-25, Stockholm, 1993.
L. Birgersson, L. Moreno, I. Neretnieks, H. Widén, T. Ågren, Water Resour. Res., 29 (1993) 3867.
R. Cadic, P. Longère, C. Gauthier, J. C. Borgotti, P. Vié, Bull. Liaison Lab. Ponts Chausses, 166 (1990) 45.
P. Toulhoat, Mat. Res. Soc. Symp. Proc., 50 (1985) 755.
S. Bigot, M. Treuil, J. Domonceau, F. Fromage, J. Hydrol., 70 (1984) 133 (in French).
H. Behrens, H. Moser, E. Wildner, J. Radioanal. Chem., 38 (1977) 491.
P. Hanson, Ph. D. Thesis, Oregon State University, Oregon, 1970.
G. Knutsson, K. Ljunggren, H. G. Forsberg, in: Radioisotopes in Hydrology, IAEA, Vienna 1963, p. 347.
D. C. Girvin, P. L. Gassman, H. Bolton, Soil Sci. Soc. Am. J., 57 (1993) 47.
C. P. Huang, E. A. Rhoads, O. J. Hao, Wat. Res., 22 (1988) 1001.
A. R. Bowers, C. P. Huang, J. Colloid Interface Sci., 110 (1986) 575.
M. A. Blesa, E. B. Borghi, A. J. G. Maroto, A. E. Regazzoni, J. Colloid Interface Sci., 98 (1984) 295.
E. Brücher, P. Szarvas, Inorg. Chim. Acta, 4 (1970) 632.
E. Brücher, G. Laurenczy, J. Inorg. Nucl. Chem., 43 (1981) 2089.
T. Ryhl, Acta Chem. Scand., 26 (1972) 4001.
E. Brücher, L. Boros, Proc. XVth Intern. Conf. on Coordination Chemistry, 15 (1973) 420.
T. Ryhl, Acta Chem. Scand., 27 (1973) 20.
É. Tóth, E. Brücher, Inorg. Chim. Acta, 221 (1994) 165.
P. W. Cacheris, S. K. Nickle, A. D. Sherry, Inorg. Chem., 26, (1987) 958.
E. Brücher, G. Laurenczy, Zs. Makra, Inorg. Chim. Acta, 139 (1987) 141.
É. Tóth, E. Brücher, I. Lázár, I. Tóth, Inorg. Chem., 33 (1994) 4070.
X. Wang, J. Tianzhu, V. Comblin, A. Lopez-Mut, E. Merciny, J. F. Desreux, Inorg. Chem., 31 (1992) 1095.
J. Byegård, G. Skarnemark, M. Skålberg, Submitted to J. Cont. Hydrology.
R. M. Smith, A. E. Martell, Critical Stability Constants, Plenum Press, New York, 1976.
E. T. Clarke, A. E. Martell, Inorg. Chim. Acta, 190 (1991) 27.
E. T. Clarke, A. E. Martell, Inorg. Chim. Acta, 190 (1991) 37.
S. Chaves, R. Delgado, J. J. R. Frausto Da Silva, Talanta, 39 (1992) 249.
W. v. d. Linden, G. Anderegg, Helv. Chim. Acta, 53 (1970) 569 (in German).
V. P. Antonovitch, E. M. Nevskaya, E. Suvorova, Zh. Neorg. Khim., 22 (1977) 1278 (in Russian).
M. M. Taquikhan, G. Ramachandraiah, Indian J. Chem., 21 (1982) 441.
S. Å. Larsson, E. L. Tullborg, S. Lindblom, PRAV-Reprot, 4-20, Swedish Nuclear Power Inspectorate, Stockholm 1981.
I. Puigdomènech, K. Nordstrom, SKB Technical Report 87-15, Swedish Nuclear Fuel and Waste Management Co., Stockholm, 1987.
P. Andersson, R. Nordqvist, T. Persson, C. O. Eriksson, E. Gustafsson, T. Ittner, Swedish Nuclear Fuel and Waste Management Co., SKB Technical Report 93-26, Stockholm, 1993.
W. J. Lacey, W. De Laguna, Science, 124 (1956) 402.
E. Halevy, A. Nir, Y. Harpaz, S. Mandel, in: Proc. 2nd Intern. Conf. on the Peaceful Uses of Atomic Energy, Vol. 20. Genève 1958, p. 158.
R. J. Heemstra, J. W. Watkins, F. E. Armstrong, Nucleonics, 19 (1961) 92.
I. B. Hazzaa, R. K. Girgis, K. F. Saad, F. M. Swailem, A. A. Bakr, Intern. J. Appl. Radiation Isotopes, 17 (1966) 621.
D. W. Margerum, D. R. Cayley, D. C. Weatherburn, G. K. Pagenkopf, Coordination Chemistry,A. E. Martell (Ed.), ACS Monogr. No. 174, American Chemical Society, Washington, DC, 1978.
G. Knutsson, H. G. Forsberg, in: Isotopes in Hydrology, IAEA, Vienna, 1967, p. 629.
G. Knutsson, in: Ground Water Problems,E. Erksson, Y. Gustafsson, K. Nilsson (Eds.), Pergamon Press, Oxford, 1968, p. 123.
J. Bond, D. B. Hobson, J. Chem. Soc. A, (1969) 2155.
R. R. Das, J. Indian Chem. Soc., LI (1974) 1024.
K. Saito, M. Tsuchimoto, J. Inorg. Nucl. Chem., 25 (1963) 145.
I. Drabæk, J. Radioanal. Chem., 75 (1982) 97.
W. A. Jester, M. Brienco, A. R. Jarret, S. H. Sakuma, C. Yu, J. Radioanal. Nucl. Chem., 110 (1987) 215.
M. Magerstadt, O. A. Gansow, M. W. Brechbiel, D. Colcher, L. Baltzer, R. H. Knop, M. E. Girton, M. Naegele, Magn. Reson. Med., 3 (1986) 808.
D. Parker, K. Pulukkody, T. J. Norman, A. Harrison, L. Royle, C. Walker, J. Chem. Soc. Chem. Commun., (1992) 1441.
M. R. Spirlet, J. Rebizant, J. F. Desreux, M. F. Loncin, Inorg. Chem., 23 (1984) 359.
J. L. Hoard, B. Lee, M. D. Lind, J. Am. Chem. Soc., 87 (1965) 1611.
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Byegård, J., Skarnemark, G. & Skålberg, M. The stability of some metal EDTA, DTPA and DOTA complexes: Application as tracers in groundwater studies. J Radioanal Nucl Chem 241, 281–290 (1999). https://doi.org/10.1007/BF02347463
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DOI: https://doi.org/10.1007/BF02347463