Solubilities of actinides in a domestic groundwater and a bentonite porewater calculated by using PHREEQC

Seung Soo Kim; Min Hoon Baik; Kwang Cheol Kang; Soo Han Kwon; Jong Won Choi

Journal of Industrial and Engineering Chemistry, Vol.14, No.6, 739-746, November, 2008

DOI10.1016/j.jiec.2008.07.005 Export Citation

Solubilities of actinides in a domestic groundwater and a bentonite porewater calculated by using PHREEQC

Seung Soo Kim^{1, †}, Min Hoon Baik¹, Kwang Cheol Kang^{1, 2}, Soo Han Kwon², and Jong Won Choi¹

¹Korea HLW Disposal Research Center, Korea Atomic Energy Research Institute, Yusong, Daejeon 305-353, Republic of Korea
²Department of Chemistry, Chungbuk National University, Cheongju 360-764, Republic of Korea

E-mail:

This study presents the solubilities and speciations of actinides, calculated by the PHREEQC (V.2) code in a granitic groundwater and a Cabentonite porewater under a reducing condition. The respective solubilities for the amorphous U, Am, Th, Np and Pu compounds in the groundwater were 2.2 × 10^(-5), 1.2 × 10^(-7), 3.1 × 10^(-9), 3.4 × 10^(-9) and 6.3 × 10^(-11) mole/L, and these values are comparable to the results calculated by the MUGREMand EQ3/6 codes. The major dissolved species for U, Am, Th, Np and Pu were UO2(OH)3-, Am(OH)2 +, Th(OH)4(aq), Np(OH)3CO3- and Pu(OH)3CO3-, respectively. However, carbonate complex ions were anticipated as the major species in the porewater except for thorium due to an increase of the carbonate concentration and a decrease of the pH.

Keywords:Actinides;Solubility;Geochemical code;Species

[References]

KAERI, Progress report on the R&D program for the disposal of HLWin Korea: Appendix, Deajeon, Korea, 2002
Kim SS, Chun KS, Kang KC, Baik MH, Kwon SH, Choi JW, J. Ind. Eng. Chem., 13(6), 959 (2007)
Nitsche H, Solubility and speciation studies for nuclear repository performance assessment, CONF-9010497-1, LBL-31181
Parkhurst DL, Appelo CAJ, User’s guide to PHREEQC (Version 2)-a computer program for speciation, batch-reaction, one-dimensional transport and inverse geochemical calculations, Water-Resources Investigations Report 99-4259, Denver, Colorado, 1999
Choppin GR, Mar. Chem., 99, 83 (2006)
IAEA, Geochemistry of long-lived transuranic actinides and fission products, IAEA-TECDOC-637, 1992
Hummel W, Berner U, Curti E, Pearson FJ, Thoenen T, Nagra/PSI Chemical Thermodynamic Data base 01/01, Universal Publishers, Florida, USA, 2002
Mompean FJ, Illemassene M, Domenech-Orti C, Said KB, Chemical Thermodynamics 5: Update on the Chemical Thermodynamics of Uranium, Neptunium, Plutonium, Americium and Technetium, Elsevier, 2003
Keum DK, Baik MH, Hahn PS, J. Korean Nucl. Soc., 34, 517 (2002)
OCRWM, Dissolved concentration limits of radioactive elements, ANLWIS-MD-000010 REV 02, 2003
Takeda S, Shima S, Kimura H, Matsuzuru H, The aqueous solubility and speciation analysis for uranium, neptunium and selenium by the geochemical code (EQ3/6), JAERI Research 95-069, Japan Atomic Energy Research Institute, 1995
Puigdomenech I, Bruno J, Modeling uranium solubilities in aqueous solutions: validation of a thermodynamic data base for the EQ3/6 geochemical codes, SKB-TR-88-21, 1988
Runde W, Conradson SD, Efurd DW, Lu NP, van Pelt CE, Tait CD, Appl. Geochem., 7, 837 (2002)
Butorin S, Ollila K, Albinsson Y, Reduction of uranyl carbonate and hydroxyl complexes and neptunyl carbonate complexes studied with chemical-electrochemical methods and RIXS spectroscopy, POSIVA 2004-01, 2004
Neck V, Kim JI, Radiochim. Acta, 89, 1 (2001)
Chandratillake M, Trivedi DP, Randall MG, Humphreys PN, Kelly EJ, J. Alloys Compd., 273, 821 (1998)
Ollila K, Determination of U oxidation state in anoxic(N2) aqueous solutions-method development and testing, POSIVA-96-01, 1996
Grambow B, Loida A, Esparza AM, Arocas PD, de Pablo J, Paul JL, Marx G, Glatz JP, Lemmens K, Ollila K, Christensen H, Long-term safety of radioactive waste disposal: source term for performance assessment of spent fuel as a waste form, Final report, FZKA-6420, Forschungszentrum Karlsruhe, 2000
Rai D, Felmy A, Ryan J, Inorg. Chem., 29, 260 (1990)
Strickert RG, Rai D, Fulton RW, Effect of aging on the solubility and crystallinity of Np(IV) hydrous oxide, Geochemical behavior of disposed radioactive waste, Am. Chem. Soc., Washington, D.C., 1984, p. 135

[Referenced By]

[1] KAERI, Progress report on the R&D program for the disposal of HLWin Korea: Appendix, Deajeon, Korea, 2002

[2] Kim SS, Chun KS, Kang KC, Baik MH, Kwon SH, Choi JW, J. Ind. Eng. Chem., 13(6), 959 (2007)

[3] Nitsche H, Solubility and speciation studies for nuclear repository performance assessment, CONF-9010497-1, LBL-31181

[4] Parkhurst DL, Appelo CAJ, User’s guide to PHREEQC (Version 2)-a computer program for speciation, batch-reaction, one-dimensional transport and inverse geochemical calculations, Water-Resources Investigations Report 99-4259, Denver, Colorado, 1999

[5] Choppin GR, Mar. Chem., 99, 83 (2006)

[6] IAEA, Geochemistry of long-lived transuranic actinides and fission products, IAEA-TECDOC-637, 1992

[7] Hummel W, Berner U, Curti E, Pearson FJ, Thoenen T, Nagra/PSI Chemical Thermodynamic Data base 01/01, Universal Publishers, Florida, USA, 2002

[8] Mompean FJ, Illemassene M, Domenech-Orti C, Said KB, Chemical Thermodynamics 5: Update on the Chemical Thermodynamics of Uranium, Neptunium, Plutonium, Americium and Technetium, Elsevier, 2003

[9] Keum DK, Baik MH, Hahn PS, J. Korean Nucl. Soc., 34, 517 (2002)

[10] OCRWM, Dissolved concentration limits of radioactive elements, ANLWIS-MD-000010 REV 02, 2003

[11] Takeda S, Shima S, Kimura H, Matsuzuru H, The aqueous solubility and speciation analysis for uranium, neptunium and selenium by the geochemical code (EQ3/6), JAERI Research 95-069, Japan Atomic Energy Research Institute, 1995

[12] Puigdomenech I, Bruno J, Modeling uranium solubilities in aqueous solutions: validation of a thermodynamic data base for the EQ3/6 geochemical codes, SKB-TR-88-21, 1988

[13] Runde W, Conradson SD, Efurd DW, Lu NP, van Pelt CE, Tait CD, Appl. Geochem., 7, 837 (2002)

[14] Butorin S, Ollila K, Albinsson Y, Reduction of uranyl carbonate and hydroxyl complexes and neptunyl carbonate complexes studied with chemical-electrochemical methods and RIXS spectroscopy, POSIVA 2004-01, 2004

[15] Neck V, Kim JI, Radiochim. Acta, 89, 1 (2001)

[16] Chandratillake M, Trivedi DP, Randall MG, Humphreys PN, Kelly EJ, J. Alloys Compd., 273, 821 (1998)

[17] Ollila K, Determination of U oxidation state in anoxic(N2) aqueous solutions-method development and testing, POSIVA-96-01, 1996

[18] Grambow B, Loida A, Esparza AM, Arocas PD, de Pablo J, Paul JL, Marx G, Glatz JP, Lemmens K, Ollila K, Christensen H, Long-term safety of radioactive waste disposal: source term for performance assessment of spent fuel as a waste form, Final report, FZKA-6420, Forschungszentrum Karlsruhe, 2000

[19] Rai D, Felmy A, Ryan J, Inorg. Chem., 29, 260 (1990)

[20] Strickert RG, Rai D, Fulton RW, Effect of aging on the solubility and crystallinity of Np(IV) hydrous oxide, Geochemical behavior of disposed radioactive waste, Am. Chem. Soc., Washington, D.C., 1984, p. 135