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The Chemical Behavior of Transuranium Elements and Barrier Functions in Natural Aquifer Systems

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The chemical behavior of transuranium elements in natural aquifer systems is governed by a variety of geochemical reactions, such as dissolution reaction (solubility), hydrolysis, complexation with inorganics or organics, redox reaction, colloid formation, geochemical interaction with surfaces of various minerals, coprecipitation, mineralization, etc. This paper reviews the present state of knowledge on some of these particular reactions. The emphasis here is on how the individual reactions can be appraised for long-term prediction of the geochemical behavior of transuranium elements in the natural environment. Of the various possible reactions, the primary thermodynamic processes are discussed with notable examples: dissolution of transuranium compounds in aquatic solution; complexation with important anions present in groundwater; and colloid generation. Various laser spectroscopic methods in use for chemical speciation are mentioned briefly for their spectroscopic capability, as well as for their applicability. The present paper attempts to better understand the migration behavior of transuranium elements in natural aquifer systems.

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References

  1. World Nuclear Status Report 1989, J. Europ. Nucl. Soc. X 7/8, 25 (1990).

  2. V. Fischer, H.W. Wiese, Report KfK 3014, Jan. 1983.

  3. R.G. Schreckhise, Health Phys. 38, 817 (1980).

    Article  CAS  Google Scholar 

  4. M.F. Sullivan, Health Phys. 38, 159 (1980).

    Article  CAS  Google Scholar 

  5. J.I. Kim, in Handbook on the Physics and Chemistry of Actinides, Vol. 4, edited by A.J. Freeman, C. Keller, (North Holland, Amsterdam, 1986), Chap. 8.

  6. J. Lewi, C. Izabel, Y. Kaluzny, Safety Assessment of Radioactive Repositories, (OECD Paris, 1990), 81.

    Google Scholar 

  7. ICRP Publication 30, Parts 1–3, Pergamon Press Oxford, 1980.

  8. J.I. Kim, E. Warnecke, eds., Approaches to the Radionuclide Migration in the Geosphere: National and International Aspects, (Harwood Academic London/New York, 1988), pp. 280.

    Google Scholar 

  9. The proceedings of “International Conference on Chemistry and Migrational Behaviour of Actinides and Fission Products in the Geosphere”, Special Issues of Radiochimica Acta, R. Oldenbourg Verlag München, Vol. I, 1989; Vol. II, 1991.

  10. J.I. Kim, Radiochim. Acta 52/53, 71 (1991).

    Google Scholar 

  11. J.I. Kim, R. Stumpe, R. Klenze, K. Yoshihara, Topics in Current Chemistry, Vol 157 (Springer-Verlag Berlin, 1990), 131.

    Google Scholar 

  12. R. Klenze, J.I. Kim, H. Wimmer, Radiochim. Acta 52/53, 97 (1991).

    Google Scholar 

  13. C.F. Baes Jr., R.E. Mesmer, Hydrolysis of Cations, (John Wiley + Sons New York, 1976).

    Google Scholar 

  14. M.H. Lloyd, R.G. Haire, Radiochim. Acta 25, 139 (1978).

    Article  CAS  Google Scholar 

  15. T.W. Newton, D.E. Hobart, P.D. Palmer, Radiochim. Acta 39, 139 (1986).

    Article  CAS  Google Scholar 

  16. D. Rai, Radiochim. Acta 35, 97 (1984).

    Article  CAS  Google Scholar 

  17. J.I. Kim, B. Kanellakopulos, Radiochim. Acta 48, 145 (1989).

    CAS  Google Scholar 

  18. K. Andersson, Mat. Res. Soc. Symp. Proc. 127, 693 (1989).

    Article  CAS  Google Scholar 

  19. J.M. Cleaveland, T.F. Rees, K.L. Nash, Nucl. Technol. 62, 298 (1983).

    Article  Google Scholar 

  20. J.M. Cleaveland, T.F. Rees, K.L. Nash, Science 222, 1323 (1983).

    Article  Google Scholar 

  21. H.J. Simpson, R.M. Trier, C.R. Olson, D.E. Hammond, A. Ege, L. Miller, J.M. Melack, Science 207, 1071 (1980).

    Article  CAS  Google Scholar 

  22. G. Meinrath, J.I. Kim, Radiochim. Acta 52/53, 29 (1991).

    Article  Google Scholar 

  23. E.M. Standifer, H. Nitsche, Lathanide and Actinide Res. 2, 383 (1988).

    CAS  Google Scholar 

  24. H. Wimmer, J.I. Kim, to be published.

  25. J.I. Kim, G. Buckau, H. Rommel, B. Sohnius, Mat. Res. Soc. Symp. Proc. 127, 849 (1989).

    Article  CAS  Google Scholar 

  26. G. Meinrath, PhD thesis, Technische Universität München, 1991.

  27. G.R. Choppin, Radiochim. Acta 32, 43 (1983).

    Article  CAS  Google Scholar 

  28. W.R. Wadt, J. Am. Chem. Soc. 103, 6053 (1981).

    Article  CAS  Google Scholar 

  29. S. Stadler, J.I. Kim, Radiochim.Acta 44/45, 39 (1988).

    Article  Google Scholar 

  30. Ch. Lierse, W. Treiber, J.I. Kim, Radiochim. Acta 38, 27 (1985).

    Article  CAS  Google Scholar 

  31. Ch. Lierse, PhD thesis, Technische Universität München, 1985.

  32. J.I. Kim, M. Bernkopf, Ch. Lierse, F. Koppold, ACS Symp. Ser. 246, 115 (1984).

    Article  CAS  Google Scholar 

  33. L. Righetto, G. Bidoglio, B. Marcandalli, R. Bellobono, Radiochim. Acta 44/45, 73 (1988).

    Article  Google Scholar 

  34. W. Stumm, J.J. Morgan, Aquatic Chemistry, 2nd ed., (John Wiley + Sons New York, 1981).

    Google Scholar 

  35. R.M. Smith, A.E. Martell, Critical Stability Constants, (Plenum New York, 1976).

    Book  Google Scholar 

  36. J.I. Kim, W. Runde, G. Meinrath, V. Neck, Thermodynamic Constants of Hydrolysis Reactions and Carbonate Complexation of Actinides, to be published.

  37. F.J. Stevenson, Humic Chemistry, (John Wiley + Sons New York, 1982).

    Google Scholar 

  38. M.H.B. Hays, P. McCathy, R.L. Malcom, R.S. Swift, Humic Substances II: In Search of Structure, (John Wiley + Sons New York, 1989).

    Google Scholar 

  39. S. Yariv, S. Cross, Geochemistry of Colloid Systems, (Springer-Verlag Berlin, 1979).

    Book  Google Scholar 

  40. A.J. Francis, Soil Reclamation Process, edited by R.L. Tate III, D.A. Klein, (Marcel Dekker New York, 1985), Chap. 9.

    Google Scholar 

  41. J.I. Kim, G. Buckau, E. Bryant, R. Klenze, Radiochim. Acta 48, 135 (1989).

    CAS  Google Scholar 

  42. M. Whitfield, R.M. Pytkowicz, Activity coefficients in Electrolyte Solutions, Vol. 2, (CRC-Press Boca Raton, 1979), p. 153.

    CAS  Google Scholar 

  43. D.A. Livingstone, USGS Professional Papers 440-G, 6th ed., (US Government. Printing Office Washington D.C., 1963), Chap. G 47.

    Google Scholar 

  44. J.P. Riley, G. Skirrows, Chemical Oceanography, Vol. 1, 2nd ed., (Academic Press London, 1975).

  45. H.J. Rösier, H. Lange, Geochemical Tables, (Elsevier Amsterdam, 1973).

    Google Scholar 

  46. J.I. Kim, J. Heitz, B. Delakowitz, F. Dienstbach, B. Kornprobst, Ch. Pissinger, Ch. Stöwer, S. Dietrich, E. Otto, Nuklide Migration (Tc, Np, Pu, Am) im Deckgebirge des Endlagerortes Gorleben, Report RCM-00190, Technische Universität München, 1990.

    Google Scholar 

  47. B.S. Jensen, Migration Phenomena of Radionuclides into the Geosphere, (Harwood Academic London, 1982), B12.

    Google Scholar 

  48. T.W. Newton, J.C. Sullivan, in Handbook on the Physics and Chemistry of Actinides, edited by A.J. Freeman, C. Keller, (North Holland Amsterdam, 1985), Chap. 11.

    Google Scholar 

  49. M. Schnitzer, S.U. Kahn, Soil Organic Matter, (Elsevier Amsterdam, 1978).

    Google Scholar 

  50. D.S. Gamble, Can. J. Chem. 51, 3217 (1973).

    Article  CAS  Google Scholar 

  51. J.A. Marinsky, W.M. Anspach, J. Phys. Chem. 79, 439 (1975).

    Article  CAS  Google Scholar 

  52. J.I. Kim, G. Buckau, W. Zhuang, Mat. Res. Soc. Symp. Proc. 84, 747 (1987).

    Article  CAS  Google Scholar 

  53. J.I. Kim, G. Buckau, R. Klenze, in Natural Analogues in Radioactive Waste Disposal, edited by B. Come, N. Chapman, (Graham + Trotman London, 1987), p. 289.

    Book  Google Scholar 

  54. G. Buckau, R. Stumpe, J.I. Kim, J. Less Common Metals 122, 555 (1986).

    Article  CAS  Google Scholar 

  55. G. Buckau, PhD thesis, Freie Universität Berlin, 1991.

  56. K.L. Nash, G.R. Choppin, J. Inorg. Nucl. Chem. 42, 1045 (1980).

    Article  CAS  Google Scholar 

  57. J.V. Ibarra, T. Oscar, J.M. Gavilan, An. Quirn. 77, 224 (1981).

    CAS  Google Scholar 

  58. W.C. Li, D.M. Victor, C.L. Chakrabati, Anal. Chem. 52, 520 (1980).

    Article  CAS  Google Scholar 

  59. P.M. Shanbhag, G.R. Choppin, J. Inorg Nucl. Chem. 43, 3369 (1981).

    Article  CAS  Google Scholar 

  60. B. Kribeck, J. Podlah, Org. Geochem. 2, 93 (1980).

    Article  Google Scholar 

  61. All literatures of the Am humate complexation are to be found in Refs. 41 and 65.

  62. J.I. Kim, H. Wimmer, R. Klenze, Radiochim. Acta, in print.

  63. T. Sekine, J.I. Kim, to be presented at this symposium.

  64. J.I. Kim, CEC Report EUR 12858 EN, (B. Come, ed.), Brussels, 1990.

    Google Scholar 

  65. J.I. Kim, D.S. Rhee, G. Buckau, Radiochim.Acta 52/53, 49 (1991)

    Google Scholar 

  66. J.I. Kim, G. Buckau, G.H. Li, H. Duschner, N. Psarros, Frezenius J. Anal. Chem. 338, 245 (1990)

    Article  CAS  Google Scholar 

  67. E.L. Bertha, G.R. Choppin, Inorg. Nucl. Chem. 40, 655 (1978).

    Article  CAS  Google Scholar 

  68. A. Maes, J. De Brabandere, A. Cremers, Radiochim. Acta 52/53, 41 (1991).

    Article  Google Scholar 

  69. M. Yamamoto, M. Sakanoue, J. Radiat. Res. 23, 261 (1982).

    Article  CAS  Google Scholar 

  70. R.A. Torres, G.R. Choppin, Radiochim. Acta 35, 143 (1984).

    Article  CAS  Google Scholar 

  71. V. Moulin, PhD thesis, University of Lyon France, 1985.

  72. S. Ahland, J.O. Lilijenzin, J. Rydberg, Comprehensive Inorganic Chemistry, Vol. 5, edited by J.C. Bailer, (Pergamon Oxford, 1973).

  73. B. Allard, H. Kipatsi, J.O. Lilijenzin, J. Inorg. Nucl. Chem. 42, 1015 (1980).

    Article  CAS  Google Scholar 

  74. C.C. Musikas, in Gmelin Handbuch der anorganischen Chemie, Bd. 20, edited by G. Koch, (Springer-Verlag, 1975), Chap. 2.

    Google Scholar 

  75. H. Nitsche, Radiochim. Acta 52/53, 3 (1991).

    Article  Google Scholar 

  76. S. Magirius, W.T. Carnall, J.I. Kim, Radiochim. Acta 38, 29 (1985)

    Article  CAS  Google Scholar 

  77. K. Büppelmann, J.I. Kim, Ch. Lierse, Radiochim. Acta 44/45, 65 (1988).

    Article  Google Scholar 

  78. T. Fukusawa, Ch. Lierse, J.I. Kim, to be published.

  79. H. Wimmer, P. Zeh, J.I. Kim, to be published.

  80. J.F. McCarthy, J.M. Zachara, Environ. Sci. Technol. 23, 496 (1989)

    CAS  Google Scholar 

  81. C. Delgueldre, B. Werni, Anal. Chim. Acta 195, 211 (1987).

    Article  Google Scholar 

  82. K.H. Lieser, B. Gleitsmann, S. Peschke, Th. Steinkopf, Radiochim. Acta 40, 39 (1986).

    CAS  Google Scholar 

  83. J.D.F. Ramsay, Radiochim. Acta 44/45, 165 (1988).

    Google Scholar 

  84. J.I. Kim, G. Buckau, F. Baumgärtner, C.H. Moon, Mat. Res. Soc. Symp. Proc. 26, 31 (1984).

    Article  CAS  Google Scholar 

  85. W. Stumm, Environ. Sci. Technol. 11, 1066 (1977).

    Article  CAS  Google Scholar 

  86. A. Saito, G.R. Choppin, Anal. Chem. 55, 2454 (1983).

    Article  CAS  Google Scholar 

  87. G.R. Choppin, A. Saito, Radiochim. Acta 35, 149 (1984).

    Article  CAS  Google Scholar 

  88. P.A. Bertrand, G.R. Choppin, Radiochim. Acta 31, 135 (1982).

    Article  CAS  Google Scholar 

  89. S.C. Foti, E.C. Freiling, Talanta 11, 385 (1964).

    Article  CAS  Google Scholar 

  90. W. Schrepp, R. Stumpe, J.I. Kim, H. Walther, Appl.Phys. B32, 207 (1983).

    Article  CAS  Google Scholar 

  91. R. Stumpe, J.I. Kim, W. Schrepp, H. Walther, Appl.Phys. B34, 203 (1984).

    Article  CAS  Google Scholar 

  92. Th. Berthoud, P. Mauchien, N. Omenetto, G. Rossi, Anal. Chim. Acta 153, 265 (1983).

    Article  CAS  Google Scholar 

  93. Ch. Moulin, N. Delorme, Th. Berthoud, P. Mauchien, Radiochim. Acta 44/45, 103 (1988).

    Google Scholar 

  94. I. Grenthe, G. Bidoglio, N. Omenetto, Inorg. Chem. 28, 71 (1989).

    Article  CAS  Google Scholar 

  95. N. Delorme, Radiochim. Acta 52/53, 405 (1991).

    Article  Google Scholar 

  96. Ch. Moulin, P. Decambox, P. Mauchien, V. Moulin, M. Theyssier, Radiochim. Acta 52/53, 119 (1991).

    Article  Google Scholar 

  97. J.V. Beitz, Radiochim. Acta 52/53, 35 (1991).

    Article  Google Scholar 

  98. R. Klenze, J.I. Kim, Radiochim. Acta 44/45, 77 (1988).

    Article  Google Scholar 

  99. R. Klenze, H. Wimmer, unpublished.

  100. L.G.M. Baas, I.R. Kaplan, D. Moore, J. Geol. 68, 243 (1960).

    Article  Google Scholar 

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Authors and Affiliations

  1. Kernforschungszentrum Karlsruhe, Institut für Nukleare Entsorgungstechnik, D-7500, Karlsruhe, Germany

    Jae-Il Kim

  2. Institut für Radiochemie, Technische Universität München, D-8046, Garching, Germany

    Jae-Il Kim

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Kim, JI. The Chemical Behavior of Transuranium Elements and Barrier Functions in Natural Aquifer Systems. MRS Online Proceedings Library 294, 3–21 (1992). https://doi.org/10.1557/PROC-294-3

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