Skip to main content
SpringerLink
Log in

Measurement and thermodynamic modeling of Np(V) solubility in aqueous K2CO3 solutions to high concentrations

  • Published:
Journal of Solution Chemistry Aims and scope Submit manuscript

Abstract

The solubility of Np(V) solids was studied in 0.01 to 6.38 mol-Kg-1 2CO3 solutions. Two series of experiments were conducted from undersaturation using NpO2OH(s) or KNpO2CO3(s) as the starting solid. The Np(V) solid phases observed at steady state are KNpO2CO3(s) and K3NpO2(CO3)2(s). The activity coefficient formalism of Pitzer was used to obtain a thermodynamic interpretation of these data, including the solubility constants:\(\begin{gathered} KNpO_2 CO_3 (s) \rightleftharpoons K^ + + NpO_2^ + + CO_3^{2 - } log K_s = - 13.6 \pm 0.1(2\sigma ) \hfill \\ K_3 NpO_2 (CO_3 )_2 (s) \rightleftharpoons 3K^ + + NpO_2^ + + 2CO_3^{2 - } log K_s = - 15.9 \pm 0.1(2\sigma ) \hfill \\ \end{gathered} \) To model these data, we propose values for several binary and ternary ion interaction parameters among the carbonate ion, potassium ion, and the neptunyl triscarbonato ion. With these new parameters, the thermodynamic data base for Np(V) solubility in concentrated aqueous solutions has been extended to the NaK-C1-C1O4-CO3-H-OH-H2O system.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Similar content being viewed by others

References

  1. Th. FanghÄnel, V. Neck, and J. I. Kim,Radiochim. Acta 3, 169 (1995).

    Google Scholar 

  2. W. Runde, M. P. Neu, and D. L. Clark,Geochim. et Cosmochim. Acta 60, 2065 (1995).

    Article  Google Scholar 

  3. C. F. Novak, H. Nitsche, H. B. Silber, K. Roberts, Ph. C. Torretto, T. Prussin, K. Becraft, S. A. Carpenter, D. E. Hobart, and I. Al Mahamid,Radiochim. Acta 74, 31 (1996).

    CAS  Google Scholar 

  4. G. I. Visyashcheva, Y. F. Volkov, G. A. Simakin, I. I. Kapshukov, A. S. Bevz, and G. N. Yakovlev,Soviet Radiochem 832 (1975). Translated fromRadiokhim,16,853 (1974).

    Google Scholar 

  5. T. K. Keenan and F. H. Kruse,Inorg. Chem 3, 1231 (1964).

    Article  CAS  Google Scholar 

  6. Yu. F. Volkov, 1.1. Kapshukov, G. I. Visyashcheva, and G. N. Yakovlev,Soviet Radiochem. 846 (1975). Translated fromRadiokhim,16, 868 (1974).

  7. K. S. Pitzer,Activity Coefficients in Electrolyte Solutions, (CRC Press, Boca Raton, Florida, 1991), Chap. 3, pp. 75–153.

  8. C. E. Harvie, N. MØller, and J. H. Weare,Geochim. et Cosmochim. Ada 48, 723 (1984).

    Article  CAS  Google Scholar 

  9. S. C. Babb, C. F. Novak, R. C. Moore, and A. R. Felmy,User’s Manual for NONLIN Version 2.0, (Sandia National Laboratories, Albuquerque, New Mexico, 1995), SWCF WPO 30740.

  10. C. E. Harvie, J. P. Greenberg, and J. H. Weare,Geochim. et Cosmochim. Acta 51, 1045 (1987).

    Article  CAS  Google Scholar 

  11. S. C. Babb and C. F. Novak,FMT Version 2.00, User’s Manual, (Sandia National Laboratories, Albuquerque, New Mexico, 1995), SWCF WPO 28119.

  12. W. R. Smith and R. W. Missen,Chemical Reaction Equilibrium Analysis: Theory and Algorithms, (John Wiley and Sons, New York, New York, 1982) pp. 141–145.

    Google Scholar 

  13. K. Ueno and A. Saito,Radiochem. Radioanal. Lett 22, 127 (1975).

    CAS  Google Scholar 

  14. C. F. Novak and K. E. Roberts,Scientific Basis for Nuclear Waste Management XVIII, Materials Research Society Symposium Proceedings, Kyoto, Japan, October 23–27, 1994, (Materials Research Society, Pittsburgh, Pennsylvania, 1995),353, Part 2, 1119–1128.

    Google Scholar 

  15. D. Rai, A. F. Felmy, S. M. Sterner, D. A. Moore, M. J. Mason, and C. F. Novak,Radiochim Acta, in press (1997).

  16. R. N. Roy, K. M. Vogel, C. E. Good, W. B. Davis, L. N. Roy, D. A. Johnson, A. R. Felmy, and K. S. Pitzer,J. Phys. Chem 96, 11065 (1992).

    Article  CAS  Google Scholar 

  17. J. Fuger and F. L. Oetting,The Chemcial Thermodynamics of Actinide Elements and Compounds: Part 2. The Actinide Aqueous Ions, (International Atomic Energy Agency, Vienna, Austria, 1976), pp. 64–67.

    Google Scholar 

Download references

Author information

Authors and Affiliations

  1. Sandia National Laboratories, P.O. Box 5800, 87185-1320, Albuquerque, New Mexico

    Craig F. Novak

  2. Lawrence Berkeley National Laboratory, Berkeley, California

    Ilham Al Mahamid, Kevin A. Becraft, Scott A. Carpenter, Nadia Hakem & Traudel Prussin

Authors
  1. Craig F. Novak
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Ilham Al Mahamid
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Kevin A. Becraft
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Scott A. Carpenter
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Nadia Hakem
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Traudel Prussin
    View author publications

    You can also search for this author in PubMed Google Scholar

Rights and permissions

Reprints and permissions

About this article

Cite this article

Novak, C.F., Mahamid, I.A., Becraft, K.A. et al. Measurement and thermodynamic modeling of Np(V) solubility in aqueous K2CO3 solutions to high concentrations. J Solution Chem 26, 681–697 (1997). https://doi.org/10.1007/BF02767621

Download citation

  • Received:

  • Revised:

  • Issue Date:

  • DOI: https://doi.org/10.1007/BF02767621

Key Words

Search

Navigation