Hostname: page-component-7479d7b7d-68ccn Total loading time: 0 Render date: 2024-07-12T03:41:01.949Z Has data issue: false hasContentIssue false
  • English
  • Français

Determination of liquid-solid partition coefficients (Kd) of radionuclide anionic species from a contaminated aquifer

Published online by Cambridge University Press:  21 March 2011

François Carona ,
Michael K. Haas ,
Edward L. Cooper  and
David E. Robertson
François Carona
Affiliation:
Current address: Dept. of Chemistry & Biochemistry, Laurentian University, Sudbury, ON, Canada, P3E 2C6;
Michael K. Haas
Affiliation:
Atomic Energy of Canada Limited, Environmental Technologies Branch, Chalk River, ON, Canada, K0J 1J0;
Edward L. Cooper
Affiliation:
Atomic Energy of Canada Limited, Environmental Technologies Branch, Chalk River, ON, Canada, K0J 1J0;
David E. Robertson
Affiliation:
Pacific Northwest National Laboratories, Richland, WA;
Get access

Abstract

Contaminated groundwater from a former liquid waste discharge area at the Chalk River Laboratories was treated with ion exchange resins to isolate aqueous extracts of selected radionuclides (60Co, 106Ru, 137Cs, 238Pu, 239/240Pu, 241Am and 244Cm). The extracts were then mixed with native uncontaminated soil material to determine their liquid-solid partitioning coefficients (Kd). Separate Kd values of the same elements were also obtained with the usual short-term “batch” technique for comparison, but using different radioisotopes as tracers (57Co and 134Cs), spiked to the extracts. The comparison included separate Kd determinations with 239/240Pu and 241Am as tracers, added to uncontaminated groundwater.

In all cases, the radionuclides originally present in the contaminated groundwater extracts exhibited low Kd values, compared to the values obtained in the “batch” method with tracers (57Co, 134Cs, 239/240Pu and 241Am). The difference was up to two orders of magnitude. This was attributed to differences in aqueous speciation of the nuclides in the contaminated groundwater, allowing limited interactions of complexed radionuclide species with soil material. Our results indicated that all the radionuclides were predominantly in anionic form in the groundwater, whereas in the tracer “batch” experiment, 57Co and 134Cs were predominantly cationic, Pu and Am were predominantly anionic. Hydrolysis partially explains the dominant anionic character of Am and Pu in the tracer experiments, however dissolved organics are suspected to dominate the speciation of the radionuclides in contaminated groundwater. Our experiment implies that in some cases, if Kd values obtained using the “batch” method with tracers are used in transport models, radionuclide transport could be underestimated.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 713: Symposium JJ – Scientific Basis for Nuclear Waste Management XXV , 2002 , JJ5.2
Copyright
Copyright © Materials Research Society 2002

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

1. ASTM, Method D 4319-83. American Society for Testing and Materials, Philadelphia, PA (1984).Google Scholar
2. Robertson, D.E.et al., NUREG/CR-6627, PNNL-12185, U.S. Nucl. Reg. Comm., Washington, DC (2000).Google Scholar
3. Cooper, E.L. and McHugh, J.O., Sci. Tot. Environ., 28 (1983) 215.Google Scholar
4. Killey, R.W.D., McHugh, J.O., Champ, D.R., Cooper, E.L. and Young, J.L., Environ. Sci. Technol., 18 (1984) 148.Google Scholar
5. Rao, R.R. and Cooper, E.L., J. Radioanal. Nucl. Chem. (Art.), 197 (1995) 133.Google Scholar
6. Champ, D.R. and Robertson, D.E., In Bulman, R.A. and Cooper, J.R. (Eds.), Speciation of Fission and Activation Products in the Environment. Elsevier Appl. Sci., London, UK, 1986, p.114.Google Scholar
7. Champ, D.R., Young, J.L., Robertson, D.E. and Abel, K.H., Water Poll. Res. J. Canada, 19 (1984) 35.Google Scholar
8. Ticknor, K.V., Boisvenue, L. and Vandergraaf, T.T., AECL report TR-755, (1996).Google Scholar
9. Wulfsberg, G. Inorganic Chemistry, University Science books, Sausalito, CA, 2000.Google Scholar
10. Allard, B. Kipatsi, H. and Liljenzin, J.O., J. Inorg. Nucl., 42 (1980) 1015.Google Scholar
11. Baes, C.F. and Maesmer, R.E., The Hydrolysis of Cations, Wiley-Interscience, New York, NY, (1976).Google Scholar
12. Cotton, F.A. and Wilkinson, G. Advanced Inorganic Chemistry (4th Edition), J. Wiley and Sons, New York, NY, 1980.Google Scholar
13. Caron, F. AECL report TR-605 (COG-94-208-i), (1998).Google Scholar
14. Fortin, C. and Caron, F. Anal. Chim. Acta, 410 (2000) 107.Google Scholar
15. Caron, F. Elchuk, S. and Walker, Z.H., J. Chromatogr., 739 (1996) 281.Google Scholar