Nuclear Engineering and Technology

  • 제34권5호
  • /
  • Pages.517-531
  • /
  • 2002
  • /
  • 1738-5733(pISSN)
  • /
  • 2234-358X(eISSN)
한국원자력학회 (Korean Nuclear Society)
권호 표지

Speciation and Solubility of Major Actinides Under the Deep Groundwater Conditions of Korea

  • 발행 : 2002.10.01
PDF 다운로드
⟨ 이전 논문 다음 논문 ⟩

초록

The speciation and solubility of Am, Np, Pu and U have been analyzed by means of the geochemical code MUGREM, under the chemical conditions of domestic deep groundwater, in order to support the preliminary safety assessment for a Korean HLW disposal concept. Under the conditions of groundwaters studied, the stable solid phase is AmOHC $O_3$(s) or Am(OH)$_3$(s), soddyite((U $O_2$)$_2$ $SiO_2$.2$H_2O$) or N $a_2$ $U_2$ $O_{7}$ (c), Np(OH)$_4$(am), and Pu(OH)$_4$(am) for Am, U, Np, and Pu, respectively. The dominating aqueous species are as follows: the complexes of Am(III), Am(OH)$_2$$^{+}$ and Am(C $O_3$)$_2$$^{[-10]}$ , the complexes of U(VI), U $O_2$(OH)$_3$$^{[-10]}$ and U $O_2$(C $O_3$)$_3$$^{4-}$, the complexes of Np(IV), Np(OH)$_4$(aq) and Np(OH)$_3$C $O_3$, and the complexes of Pu(IV), Pu(OH)$_4$(aq) and Pu(OH)$_3$C $O_3$$^{[-10]}$ . The calculated solubilities exist between 1.9E-10 and 1.3E-9 mol/L for Am, between 5.6E-6 and 1.2E-4 mol/L for U, between 3.1E-9 and 1.3E-8 mol/L for Np, and between 6.6E-10 and 2.4E-10 mol/L for Pu, depending on groundwater conditions. The present solubilities of each actinide agree well with the results of other studies obtained under similar conditions.s.

키워드

참고문헌

  1. OECD/NEA, Geological disposal of Radioactive Waste: An overview of the Current States of Understanding and Development, OECD/NEA, p.111, (1984)
  2. Dormuth, K.W., 'Assessment of the Canadian Nuclear Fuel Disposal Concept,' Proceeding of Symposium on safety Assessment of Radioactive Waste Repositories, OECD/NEA, 211 (1993)
  3. Golder Associates, Performance Evaluations Related to Area Characterization of Crystalline Rock, Golder Associates, Office Crystalline Repository Division, OH, BMI/OCRD-27, (1988)
  4. Nagra, Project Gewahr 1985, Nagra, Baden, Project Report, NGB 85-09, (1985)
  5. PNC, Research and Development on Geological Waste: Final Progress Report, PNC, Tokyo, Tech. Report, TN1410 93-018, (1992)
  6. SKB, SKB-91; Final Disposal of Spent Nuclear Fuel-Importance of the Bedrock for Safety, SKB, Stockholm, Tech. Report, TR 92-20, (1992)
  7. SKI, SKI Project 90 Summary, SKI, Stockholm, Tech. Report 91-23, (1991)
  8. TVO, Final Disposal of Spent Nuclear Fuel in Finnish Bedrock, YJT, Helsinki, Tech. Report YJT-92-31E, (1992)
  9. Keum, D.K. and P.S. Hahn, 'Application and Development of a Multi-geochemical Reaction Equilibrium Model (MUGREM),' Environ. Eng. Res., 4, 113(1999)
  10. Bond, K.A., T.G. Heath, and C.J. Tweed, HATCHES: A Reference Thermodynamic Database for Chemical Equilibrium Studies, Nirex, Switzerland, Report NSS/R379, December (1997)
  11. Fuger, J., I.L. Khodakovsky, E.I. Sergeyeva, V.A. Medvedev and J.D. Narvratil, The Chemical Thermodynamics of Actinide Elements and Compounds, Part 12;The Actinide Aqueous Inorganic Complexes, IAEA, Vienna, Austria, (1992)
  12. Frlmy, A.R., D. Girvin, and E. A. Jenne, MINTEQ: A Computer Program for Calculating Aqueos Geochemical Equilibria, U.S. Environmental Protection Agency, by Battelle, Pacific Northwest laboratories, Richland, Washington, EPA-600/3-84-032, (1984)
  13. Grenthe, I., J. Fuger, R.J.M. Konings, R.J. Lemire, A.B. Muller, C.N. Gregu, and H. Wanner, Chemical Thermodynamics Series 1: Chemical Thermodynamics of Uranium: NEA-TDB, OECD, p.715, North Holland Elsevier Science Publishers, (1992)
  14. Lemire, R.J., J. Fuger, H. Nitsche, P. Potter, M.H. Rand, J. Rydberg, K. Spahin, J. C. Sullivanl, W.J. Ullman, P. Vitorge, and H. Wanner, Chemical Thermodynamics Series 4: Chemical Thermodynamics of Neptunium and Plutonium: NEA-TDB, OECD, p.845, North-Holland Elsevier Science Publishers, (2001)
  15. Pearson, F.J. and H.N. Waber, NAGRA/PSI Thermodynamic Data Base: Preparation of a Version for PHREEQC, NAGRA, Switzerland, TM-44-99-01, (1999)
  16. Silva, R.J., G. Bidoglio, M.H. Rand, P.B. Robouch, H. Wanner, and I. Puigdomenech, Chemical Thermodynamics Series 2: Chemical Thermodynamics of Americium: NEA-TDB, OECD, p.374, North-Hollland Elsevier Science Publishers, (1995)
  17. Wolery, T.J., Calculation of Chemical Equilibrium between Aqueous Solutions and Minerals: The EQ3/6 Software package, Lowrence Livermore National Lab., Livermore, CA, UCRL-52658, (1992)
  18. Keum, D.K., M.H. Baik and P.S. Hahn, Thermodynamic data of Am, Th, U, Np and Pu and their application for HLW disposal, KAERI, Technical report, KAERI/TR-2046/02, (2002)
  19. Neck, V. and J.I. Kim, 'Thermodynamics of Tetravalent Actinides: A Critical Assessment of Uncertainties,' Prodeeding of Actinides Conferences 2001, Hajuyama, Japan, (2001)
  20. Takeda, S., S. Shima and H. Kimura, The aqueous solubility and speciation analysis for uranium, neptunium and selenium by the EQ3/6, JAERI research 95-069, (1995)
  21. Grambow, B., A. Loida, A. Martinez-Esparza, P. Diaz-Arocas, J. de Pablo, J.L. Paul, G. Marx, J.P. Glatz, K. Lemmens, K. Ollola, and H. Christensen, Long-term Safety of Radioactive Waste Disposal: Source Term for Performance Assessment of Spent Fuel as a Waste Form, Final Report, Forschungszentrum Karlsruhe, Germany, FZKA 6420, (2000)
  22. Neck, V. and J.I. Kim, 'Solubility and Hydrolysis of Tetravalent Actinides,' Radiochimica Acta, 89, 1(2001) https://doi.org/10.1524/ract.2001.89.1.001
  23. Neck, V. and J.I. Kim, 'An Electrostatic Approach for the prediction of actinide Complexation Constants with Inorganic Ligands-Application to Carbonate Complexes,' Radiochimica Acta, 88, 815(2000) https://doi.org/10.1524/ract.2000.88.9-11.815
  24. Neck, V. and V. Metz, Kenntnisstand zur Aquatischen Chemie und Thermodynamik von Hexavalenten Actiniden, Forschungszentrum, Karlsruhe, Germany, FZK/INE 010/00 (internal report, unpublished),(2001)
  25. Neck, V., W. Runde, J.I. Kim and B. Kanellakipulos, 'Solid-Liquid Equilibrium Reactions of Neptunium(V) in Carbonate Solution at Different Ionic strength,' Radiochimica Acta, 65, 29(1994)
  26. Neck, V., Th. Fanghanel, and J.I. Kim, Aquatische Chemie und Thermodynamische Modellierung von Trivalenten Actiniden, Forschungszentrum Karlsruhe, Germany, FZKA 6110, (1998)
  27. Moll, H., G. Geipel, W. Metz, G. Bernhard, and H. Nitsche, 'Solubility and Speciation of $(UO_2)_2SiO_42H_2O$ in Aqueous Systems,' Radiochimica Acta, 74, 3(1996)
  28. Dpeiaz, A.P. and B. Grambows, 'Soild-Liquid phase Equilibria of U(VI) in NaCl Brines,' Geochim. Cosmochim Acta, 62, 236(1998) https://doi.org/10.1016/S0016-7037(97)00337-2
  29. Fanghanel, Th., V. Neck and J.I. Kim, 'Thermodynamics of Neptunium(V) in Concentrated Salt Solutions: II.Ion Interaction (Pitzer) parameters for Np(V) Hydrolysis Species and Carbonate Complexes,' Radiochimica Acta, 69, 169(1995)
  30. Sandino, A., and B. Grambow, 'Solubility Equilibria in U(VI)-Ca-K-Cl-$H_2O$ Systems: Transformation of Schoepite into Becquerelite and Compreignacite,' Radiochmica Acta, 66/67, 37(1994)