Abstract
Plutonium dioxide recovered in the course of reprocessing of SNF from WWER reactors (so-called high-level PuO2) was subjected to dissolution in 0.6–3.0 M HNO3 in the presence of Am(III) ions under ozonation with an ozone-oxygen mixture containing 30–180 mg l−1 O3. Measurements of the rate of the PuO2 dissolution in 3 M HNO3 in the temperature interval from 30 to 80°C showed that, with an increase in the ozone concentration in the ozone-oxygen mixture from 30 to 180 mg l−1, the dissolution rate increases by a factor of 4–5. The acceleration of the PuO2 dissolution is attributed to the formation of Am(V,VI) by homogeneous oxidation of Am(III) ions with ozone dissolved in HNO3. The Am dioxocations formed act as PuO2 oxidants and are continuously regenerated by the oxidation of Am(III) with ozone. This assumption is confirmed by an additional increase in the dissolution rate, observed on introducing Am(III) into the initial electrolyte for the PuO2 dissolution.
Similar content being viewed by others
References
The Chemistry of Actinide Elements, Katz, J.J., Seaborg, G.T., and Morss, L.R., Eds., London: Chapman and Hall, 1986, 2nd ed.
Ryan, J.L., Bray, L.A., Wheelwright, E.J., and Bryan, G.H., Catalyzed Electrolytic Plutonium Oxide Dissolution (CEPOD): The Past Seventeen Years and Future Potential, PNL-SA-18 018, CONF-900 846-5, 1990.
Nikitina, G.P., in Radievyi inst. im. V.G. Khlopina: K 75-letiyu so dnya osnovaniya (Khlopin Radium Inst.: To 75th Foundation Anniversary), St. Petersburg, 1997, pp. 53–58.
Runde, W.H. and Shultz, W.W., The Chemistry of Actinide Elements, Morss, L., Edelstein, N., Fuger, J., and Katz, J.J., Eds., New York: Springer, 2005, vol. 2, ch. 8: Americium, pp. 1265–1338.
Spravochnik khimika (Chemist’s Handbook), Nikol’skii, B.P., Ed., Moscow: Khimiya, 1963, 2nd ed., vol. 3, p. 378.
Tsushima, S., Nagasaki, S., and Suzuki, A., Sep. Sci. Technol., 1996, vol. 31, no. 7, pp. 2443–2453.
Ward, M. and Welch, G.A., J. Chem. Soc., 1954, part 4, p. 4038.
Vdovenko, V.M., Khimiya urana i transuranovykh elementov (Chemistry of Uranium and Transuranium Elements), Moscow: Nauka, 1960, pp. 406–408.
Hara, M. and Suzuki, S., J. Radioanal. Chem., 1977, vol. 36, no. 1, p. 95.
Mincher, B.J., Martin, L.R., and Schmitt, N.C., Inorg. Chem., 2008, vol. 47, no. 15, pp. 6984–6989.
Boldt, A.L., Bray, L.A., and Ryan, J.L., US Patent 4 686 019, 1987.
Panich, N.M. and Ershov, B.G., Zh. Fiz. Khim., 2008, vol. 82, no. 8, pp. 1423–1426.
Nikitina, G.P., Ivanov, Yu.E., Shumkov, V.G., and Egorova, V.P., Radiokhimiya, 1999, vol. 41, no. 4, pp. 323–330.
Gbor, P.K. and Jia, Ch.Q., Chem. Eng. Sci., 2004, vol. 59, pp. 1979–1987.
Ekmekyapar, A., Oya, R., and Künkül, A., Chem. Biochem. Eng. Q., 2003, vol. 17, no. 4, pp. 261–266.
Aarabi-Karasgani, M., Rashchi, F., Mostoufi, N., and Vahidi, E., Hydrometallurgy, 2010, vol. 102, no. 1, pp. 14–21.
Ivanov, Yu.E. and Nikitina, G.P., Radiokhimiya, 1995, vol. 37, no. 3, pp. 214–220.
Author information
Authors and Affiliations
Corresponding author
Additional information
Original Russian Text © V.M. Gelis, Yu.B. Shumilova, B.G. Ershov, A.G. Maslennikov, V.V. Milyutin, O.V. Kharitonov, M.V. Logunov, Yu.A. Voroshilov, A.V. Bobritskii, 2011, published in Radiokhimiya, 2011, Vol. 53, No. 6, pp. 516–521.
Rights and permissions
About this article
Cite this article
Gelis, V.M., Shumilova, Y.B., Ershov, B.G. et al. Use of ozone for dissolving high-level plutonium dioxide in nitric acid in the presence of Am(V,VI) ions. Radiochemistry 53, 612–618 (2011). https://doi.org/10.1134/S1066362211060087
Received:
Published:
Issue Date:
DOI: https://doi.org/10.1134/S1066362211060087