Browse > Article

Sorption Behavior of $^{241}Am,\;^{152}Eu,\;^{160}Tb\;and\;^{60}Co$ in the Geological Materials: Eu as an Optimum Analogue for Fate and Transport of Am Behavior in Subsurface Environment  

Lee, Seung-Gu (Groundwater and Geothermal Resources Division, Korea Institute of Geoscience and Mineral Resources)
Lee, Kil-Yong (Groundwater and Geothermal Resources Division, Korea Institute of Geoscience and Mineral Resources)
Cho, Soo-Young (Groundwater and Geothermal Resources Division, Korea Institute of Geoscience and Mineral Resources)
Yoon, Yoon-Yeol (Groundwater and Geothermal Resources Division, Korea Institute of Geoscience and Mineral Resources)
Kim, Yong-Je (Groundwater and Geothermal Resources Division, Korea Institute of Geoscience and Mineral Resources)
Publication Information
Economic and Environmental Geology / v.40, no.4, 2007 , pp. 361-374 More about this Journal
Abstract
Rare earth elements(REEs) have been used as an useful tool in understanding the various geological processes such as evolution and differentiation in the crust. The REEs also have been used as an analog of actinides for radioactive wastes at the water-rock interactions. Using physicochemical properties of the REEs and actinides, we have shown that Eu is an optimum analogue for understanding the behavior of Am in subsurface environments. Factors affecting sorption behavior of radioactive nuclides in groundwater were investigated by batch experiments. Four nuclides such as $^{241}Am,\;^{152}Eu,\;^{160}Tb\;and\;^{60}Co$ were selected to test our hypothesis, and $^{160}Tb$ and $^{60}Co$ were specifically used to compare to the sorption behavior between $^{241}Am-^{152}Eu$ and other radioactive nuclides. Four different rock samples and one groundwater were used in the batch experiments where solution pH for all experiments was fixed at 5.5. Our results demonstrate that $^{241}Am,\;^{152}Eu,\;and\;^{160}Tb$ show similar sorption behavior whereas $^{60}Co$ is different in sorption behavior at the mineral-water interface, suggesting that the sorption behavior of $^{60}Co$ is affected by different rock types. Our results also show that 1) Eu in REEs is optimum analogue of fate and transport of Am in subsurface environments, and 2) mineral compositions such as $SiO_2,\;TiO_2,\;P_2O_5$ and distribution of REEs such as Eu anomaly play key roles in affecting sorption behavior of radioactive nuclides even though physicochemical properties of geological materials such as specific surface area and cation exchange capacity can not be ruled out.
Keywords
Rare earth elements; Am; Eu; Analogue; Batch experiment; Sorption behavior;
Citations & Related Records
Times Cited By KSCI : 1  (Citation Analysis)
연도 인용수 순위
1 Angove, M.J., Johnson, B.B. and Wells, J.D. (1998) The influence of Temperature on the Adsorption of Cadmium(II) and Cobalt(II) on Kaolinite. Jour. Colloid Interface Sci. 204, 93-103   DOI   ScienceOn
2 Bauer, A., Rabung, T., Claret, E, Schfer, T., Buckau, G. and Fang Hnel, T. (2005) Influence of temperature on sorption of europium onto smectite: The role of organic contaminants. Appl. Clay Sci. 30, 1-10   DOI   ScienceOn
3 Guiterrez, M.G., Bidoglio, G., Avogadro, A., Mingarro, E. and D'Alessandro, M. (1991) Experimental Investigations of radionuclide transport through cored granite samples. Radiochim. Acta 52/53, 213-217
4 Henderson, P. (1984) Rare Earth Element Geochemistry: Developments in Geochemistry. Elsevier, Amsterdam-Oxford-New York-Tokyo, 510p
5 Johannesson, K.H., Zhou, X. and Stetzenbach, K.J. (1995a) Rare earth elements and groundwater mixing: An example from southern Nevada. EOS. 76, F276   DOI
6 Lee, S.G., Kim, Y., Chae, B.G., Koh, D.C. and Kim, K.H. (2004) The geochemical implication of a variable Eu anomaly in a fractured gneiss core: application for understanding Am behavior in the geological environment. Appl. Geochem. 19, 1711-1725   DOI   ScienceOn
7 Lipin, B.R. and McKay, G.A. (1989) Geochemistry and Mineralogy of Rare Earth Elements. Reviews in Mineralogy, vol. 21, Mineralogical Society of America, 348pp
8 Lippold, H., Miler, N. and Kupsch, H. (2005) Effect of humic acid on the pH-dependent adsorption of terbium(III) onto geological materials. Appl. Geochem. 20, 1209-1217   DOI   ScienceOn
9 Metz, V., Kienzler, B. and Schier, W. (2003) Geochemical evaluation of different groundwater-host rock systems for radioactive waste disposal. Jour. Contam. Hydro. 61, 265-279   DOI   ScienceOn
10 Papelis, C. (2001) Cation and anion sorption on granite from the Project Shoal Test Area, near Fallen, Nevada, USA. Advanced Environ.l Res. 5, 151-166   DOI   ScienceOn
11 Sakuragi, T., Sato, S., Kozaki, T., Mitsugashira, T., Hara, M. and Suzuki, Y. (2004) Am(III) and Eu(III) uptake on hematite in the presence of humic acid. Radiochim Acta 92, 697-702   DOI   ScienceOn
12 Lee, S.G., Lee, K.Y., Cho, S.Y., Yoon, Y.Y. and Kim, Y. (2006) Sorption properties of $^{152}Eu\;and\;^{241}$Am in geological materials: Eu as an analogue for monitoring Am behaviour in heterogeneous geological environments. Geosci. Jour. 10, 103-114   DOI   ScienceOn
13 Stipp, S.L.S., Lakstanov, L.Z., Jensen, J.T. and Baker, J.A. (2003) Preliminary results from coprecipitation experiments and observations with surface-sensitive techniques. Jour. Contam. Hydro. 61, 33-43   DOI   ScienceOn
14 Bau, M. (1996) Controls on the fractionation of isovalent trace elements in magmatic and aqueous systems: evidence from Y/Ho, Zr/Hf, and lanthanide tetrad effect. Contr. Mineral. Petrol. 123, 323-333   DOI
15 Wood, S.A., Middlesworth, P.V., Gibsson, P. and Ricketts, A. (1997) The mobility of REE, U and Th in geological environments in Idaho and their relevance to radioactive waste disposal. Jour. Alloy. Comp. 249, 136-141   DOI   ScienceOn
16 Takahashi, Y., Kimura, T., Kato, Y., Minai, Y. and Tominaga, T. (1998a) Characterization of Eu(III) Species Sorbed on Silica and Montmorillonite by Laser-Induced Fluorescence Spectroscopy. Radichim. Acta 82, 227-232
17 Takahashi, Y., Minai Y., Kimura, T. and Tominga, T. (1998b) Adsorption of europium(III) and americium(III) on kaolinite and montmorillonite in the presence of humic acid. Jour. Radioanal. Nuclear Chem. 243, 277-282
18 Menard, O., Advocat, T., Ambroai, J. P. and Michard, M.A. (1998) Behaviour of the actinides (Th, U, Np and Pu) and rare earths (La, Ce, and Nd) during aqueous leaching of a nuclear glass under geological disposal conditions. Appl. Geochem. 13, 105-126   DOI   ScienceOn
19 Heath, M. J., Montoto, M., Rodriguez rey; A., Ruiz de Argandoa, V.G. and Menendez, B. (1992) Rock Matrix Diffusion as a Mechanism of Radionuclide Retardation: A Natural Analogue Study of El Berrocal Granite, Spain. Radiochim. Acta 58/59, 379-384
20 Johansson, B. and Rosengren, A. (1975) Interpolation scheme for the cohesive energies for the lanthanides and actinides. Physic. Rev., B11, 1367-1373
21 Neretnieks, I., Eriksen, T. and Thtinen, P. (1982) Tracer Movement in a Single Fissure in Granitic Rock: Some Experimental Results and Their Interpretation. Water Res. Res. 18, 849-858   DOI
22 Berry, J.A. and Bond, K.A. (1992) Studies of the Extent of Surface Diffusion in the Migration of Radionuclides through Geological Materials. Radiochimi. Acta, 58/59, 329-335
23 Curti, E. (1999) Coprecipitation of radionuclides with calcite: estimation of partition coefficients based on a review of laboratory investigations and geochemical data. Appl. Geochem. 14, 433-445   DOI   ScienceOn
24 Lee, K.Y., Yoon, Y.Y., Lee, S.G., Lee, D.H., Kim, Y. and Woo, N.C. (2001) Sorption of radionuclides on the container wall during batch migration studies. Jour. Radioanal. Nuclear Chem. 249, 271-278   DOI   ScienceOn
25 Masuda, A. Nakamura, N. and Tanaka, T. (1973) Fine Structure of mutually normalized rare-earth patterns of chondrites. Geochim. Cosmochim. Acta 37, 239-248   DOI   ScienceOn
26 Samadfam, M., Jintoku, T., Sato, S., Ohashi, H., Mitsugashira, T. and Hara, M. (2000) Effects of humic acid on the sorption of Am(III) and Cu(III) on kaolinite. Radichim. Acta 88, 717-721   DOI   ScienceOn
27 Baik., M.H., Hyun, S.P., Cho, W.J. and Hahn, P. S. (2004) Contribution of minerals to sorption of U(IV) on granite. Radiochim. Acta 92, 663-669   DOI   ScienceOn
28 Emrn, A.T. (1993) The influence of heterogeneous rock chemistry on the sorption of radionuclides in flowing groundwater. Jour. Contam. Hydro. 13, 131-141   DOI   ScienceOn
29 Lee, S.G., Lee, D.H., Kim, Y., Chae, B.G., Kim, W.Y. and Woo, N.C. (2003) Rare earth elements as an indicator of groundwater environment changes in a fractured rock system: Evidence from fractured-filling calcite. Appl. Geochem. 18, 135-143   DOI   ScienceOn
30 Pacheco, G., Nava-Galve, G., Bosch, P. and Bulbulian, S. (1995) $^{60}Co$ sorption-desorption in Mexican montmorillonites. Jour. Radioanal. Chem. Lett. 200, 259-264   DOI
31 Masuda, A. (1975) Abundances of mono isotopic REE, consistent with the Leedey chondritic values. Geochem. Jour. 9, 183-184   DOI
32 Petit, J.-C. (1991) Natural Analogue Aspects of Radionuclide Transport in the Geosphere. Radiochim. Acta 52/53, 337-340
33 Saripalli, K.P., McGrail, B.P. and Girvin, D.C. (2002) Adsorption of molybdenum on to anatase from dilute aqueous solutions. Appl. Geochem. 17, 649-656   DOI   ScienceOn
34 Sverjensky, D.A. (1984) Europium redox equilibria in aqueous solution. Earth. Planet. Sci. Lett., 67, 70-78   DOI   ScienceOn
35 Sakuragi, T.S., Sato, S., Kozaki, T. (2002) Sorption of Eu(III) on Kaolinite in the presence of humic acid: Effects of Ionic Strength. Chem. Lett. 656-657
36 Turin, H.J., Groffman, A.R., Wolfsberg, L.E., Roach, J.L. and Strietelmeier, B.A. (2002) Tracer and radionuclide sorption to vitric tuffs of Busted Butte, Nevada. Appl. Geochem. 17, 825-836   DOI   ScienceOn
37 Irber, W. (1999) The lanthanide tetrad effect and its correlation with KlRb, $Eu/Eu^{*}$, Sr/Eu, Y/Ho, and Zr/Hf of evolving peraluminous granite suites. Geochim. Cosmochim. Acta 63, 489-508   DOI   ScienceOn
38 Hilton, J., Nolan, L. and Jarvis, K.E. (1997) Concentrations of stable isotopes of cesium and strontium in fresh waters in northern England and their efforts on estimates of sorption coefficients (Kd). Geochim. Cosmochim. Acta 61, 1115-1124   DOI   ScienceOn
39 Johannesson, K.H., Stetzenbach, K.J. and Hodge, V.F. (1995b) Speciation of the rare earth element neodymium in groundwaters of the Nevada test sites and the Yucca Mountain and implications for the actinide solubility. Appl. Geochem. 10, 565-572   DOI   ScienceOn
40 Schlegel, M.L., Charlet, L. and Manceau, A. (1999) Sorption of Metal Ions on Clay Minerals: II. Mechanism of Co Sorption on Hectorite at High and Low Ionic Strength and Impact on the Sorbent Stability. Jour. Colloid Interface Sci. 220, 392-405   DOI   ScienceOn
41 Buddemeier, R.W., Finkel, R.C., Marsh, K.V., Ruggieri, M.R., Rego, J.H. and Silva, R.J. (1991) Hydrology and Radionuclide at the Nevada Test Site. Radiochim. Acta, 52/53, 275-282
42 Runde, W., Conradson, S. D., Efurd, W., Lu, N-P., VanPelt, C. E. and Tait, C. D. (2002) Solubility and sorption of redox-sensitive radionuclides (Np, pu) in J-13 water from Yucca Mountain site: comparison between experiment and theory. Appl. Geochem 17, 837-853   DOI   ScienceOn
43 Johannesson, K., Stetzenbach, K.J., Hodge, V.H. and Lyons, W.B. (1996) Rare earth element complexation behaviour in circumneutral pH groundwaters: Assessing the role of carbonate and phosphate ions. Earth Planet. Sci. Lett., 139, 305-319   DOI   ScienceOn
44 Krauskopf, K.B. (1986a) Aqueous geochemistry of radioactive waste disposal. Appl. Geochem. 1, 15-23   DOI   ScienceOn
45 Kashparov. V.A., Protsak, V.P., Ahamdach, N., Stammose, D., Peres, J.M., Yoscheko, V.I. and Zvarich, S.I. (2000) Dissolution kinetics of particles of irradiated Chernobyl nuclear fuel: influence of pH and oxidation state on the release of radionuclides in the contaminated soil of Chernobyl. Jour. Nuclear Mat. 279, 225-233   DOI   ScienceOn
46 Krauskopf, K.B. (1986b) Thorium and rare earth metalsas as analogs for actinide elements. Chem. Geol. 55, 323-335   DOI   ScienceOn
47 Meece, D.E. and Benninger, L.K. (1993) The coprecipitation of Pu and other radionuclide with $CaCO_{3}$ Geochim. Cosmochim. Acta 57, 1447-1458   DOI   ScienceOn
48 McCarthy, J.F., Sanford, W.E. and Stafford, P.L. (1998) Lanthanide Field Tracers Demonstrate Enhanced Transport of Transuranic Radionuclides by Natural Organic Matter. Environ. Sci. Technol. 32, 3901-3906   DOI   ScienceOn