Electrolytic Dissolutions of UO2 and SIMFUEL in Carbonate Solutions at Several pHs
Electrolytic dissolution characteristics of UO2 and
SIMFUEL electrodes were studied at several potentials in carbonate
solutions of a high concentration at several pHs. The electrolytic
uranium dissolution was much affected by a corrosion product of
UO2CO3 generated at the electrode during the dissolution in carbonate
solution. The corrosion product distorted the voltammogram at UO2
and SIMFUEL electrodes in the potential region of oxygen evolution
and increased the overpotential of oxygen evolution at the electrode.
The effective dissolution in a carbonate solution could be obtained at
an applied potential such as +4 V (vs SSE) or more which had an
overpotential of oxygen evolution high enough to rupture the
corrosion product on the electrode surface.
[1] K.-W. Kim, D.-Y. Chung, H.-B. Yang, J.-K. Lim, E.-H. Lee, K.-C. Song,
and K. Song, "A Conceptual Process Study for Recovery of Uranium
Alone from Spent Nuclear Fuel by Using High-Alkaline Carbonate
Media," Nuclear Technology, vol. 166, pp. 170-179, May 2009.
[2] S. M. Pepper, L. F. Brodnax, S. E. Field, R .A. Zehnder, S. N. Valdez, and
W. H. Runde, "Kinetic Study of the Oxidative Dissolution of UO2 in
Aqueous Carbonate Media," Ind. Eng. Chem. Res., vol. 43, pp. 8188-8193,
2004.
[3] S. Goff, F. L. Taw, S. M. Pepper, L. F. Brodnax, S. E. Field, and W. H.
Runde, "Separation of uranium from fission product in spent nuclear fuel
using aqueous H2O2-carbonate solutions," AIChE 2006 Annual Meeting,
November 12-17, 2006, San Francisco.
[4] N. Asanuma, M. Harada, Y. Ikeda, and H. Tomiyasu, "New approach to
nuclear reprocessing in a non-aqueous solution," Global 2001, September
9-13, 2001, American Nuclear Society, Paris, France.
[5] C. Soderquist, and B. Hanson, "Dissolution of spent nuclear fuel in
carbonate-peroxide solution," J. Nucl. Mat., vol. 396, pp. 159-162,, 2010.
[6] S. M. Peper, B. K. McNamara, M. J. O-Hara, and M. Douglas, "Aqueous
dissolution of uranium oxides in oxidizing alkaline media," NRC7-7th
international Conference on Nuclear and Radiochemistry, August 24-29,
2008, Budapest, Hungary.
[7] W. Runde, "The Chemical Interactions of Actinides in the Environmen,"
Los Alamos Sci., vol. 26, pp. 392-411, 2000.
[8] D. W. Shoesmith, "Used Fuel and Uranium Dioxide Dissolution
StudiesÔÇöReview," NWMO TR-2007-03, Nuclear Waste Management
Organization, July 2007, pp. 1-60.
[9] D. L. Clark, D. E. Hobart, and M. P. Neu, "Actinide Carbonte Complexes
and Their Importance in Actinide Environmental Chemis," Chem. Rev.,
vol. 95, pp. 25-48, 1995.
[10] S. Rollin, K. Spahiu, and U. B. Eklund, "Determination of dissolution
rates of spent fuel in carbonate solutions under different redox conditions
with a flow-through experiment," J. Nucl. Mater., vol. 297, pp. 231-243,
2001.
[11] S, Sunder, N. H. Miller, and D.W. Shoesmith, "Corrosion of uranium
dioxide in hydrogen peroxide solutions," Corrosion Science, vol. 46, pp.
1095-1111, 2004.
[12] D. W. Shoesmith, "Fuel corrosion processes under waste disposal
conditions," J. Nucl. Mat., vol. 282, pp. 1-31, 2000.
[13] B. G. Santos, J. J. Nöel, and D.W. Shoesmith, "The effect of pH on the
anodic dissolution of SIMFUEL (UO2)," J. Electroanal. Chem., vol. 586,
pp. 1-11, 2006.
[14] D. W. Shoesmith, S. Sunder, M. G. Bailey, and G. J. Wallace, "The
corrosion of nuclear fuel (UO2) in oxygenated solutions," Corrosion Sci.,
vol. 29, No.9, pp. 1115-1128, 1989.
[15] J. S. Goldik, J. J. Noel, and D. W. Shoesmith, "Surface electrochemistry
of UO2 in dilute alkaline hydrogen peroxide solutions: Part II. Effects of
carbonate ions," Electrochimica Acta, vol. 51, pp. 3278-3286, 2006.
[16] B. G. Santos, J. J. Noel, and D. W. Shoesmith, "The influence of calcium
ions on the development of acidity in corrosion product deposits on
SIMFUEL, UO2," J. Nucl. Mat., vol. 350, pp. 320-331, 2006.
[17] P. G. Lucuta, R. A. Verrall, Hj Matzke, and B. J. Palmer, "Microstructural
features of SIMFUEL- Simulated high-burnup UO2-based nuclear fuel,"
J. Nucl. Mat., vol. 178, pp. 48-60, January 1991.
[1] K.-W. Kim, D.-Y. Chung, H.-B. Yang, J.-K. Lim, E.-H. Lee, K.-C. Song,
and K. Song, "A Conceptual Process Study for Recovery of Uranium
Alone from Spent Nuclear Fuel by Using High-Alkaline Carbonate
Media," Nuclear Technology, vol. 166, pp. 170-179, May 2009.
[2] S. M. Pepper, L. F. Brodnax, S. E. Field, R .A. Zehnder, S. N. Valdez, and
W. H. Runde, "Kinetic Study of the Oxidative Dissolution of UO2 in
Aqueous Carbonate Media," Ind. Eng. Chem. Res., vol. 43, pp. 8188-8193,
2004.
[3] S. Goff, F. L. Taw, S. M. Pepper, L. F. Brodnax, S. E. Field, and W. H.
Runde, "Separation of uranium from fission product in spent nuclear fuel
using aqueous H2O2-carbonate solutions," AIChE 2006 Annual Meeting,
November 12-17, 2006, San Francisco.
[4] N. Asanuma, M. Harada, Y. Ikeda, and H. Tomiyasu, "New approach to
nuclear reprocessing in a non-aqueous solution," Global 2001, September
9-13, 2001, American Nuclear Society, Paris, France.
[5] C. Soderquist, and B. Hanson, "Dissolution of spent nuclear fuel in
carbonate-peroxide solution," J. Nucl. Mat., vol. 396, pp. 159-162,, 2010.
[6] S. M. Peper, B. K. McNamara, M. J. O-Hara, and M. Douglas, "Aqueous
dissolution of uranium oxides in oxidizing alkaline media," NRC7-7th
international Conference on Nuclear and Radiochemistry, August 24-29,
2008, Budapest, Hungary.
[7] W. Runde, "The Chemical Interactions of Actinides in the Environmen,"
Los Alamos Sci., vol. 26, pp. 392-411, 2000.
[8] D. W. Shoesmith, "Used Fuel and Uranium Dioxide Dissolution
StudiesÔÇöReview," NWMO TR-2007-03, Nuclear Waste Management
Organization, July 2007, pp. 1-60.
[9] D. L. Clark, D. E. Hobart, and M. P. Neu, "Actinide Carbonte Complexes
and Their Importance in Actinide Environmental Chemis," Chem. Rev.,
vol. 95, pp. 25-48, 1995.
[10] S. Rollin, K. Spahiu, and U. B. Eklund, "Determination of dissolution
rates of spent fuel in carbonate solutions under different redox conditions
with a flow-through experiment," J. Nucl. Mater., vol. 297, pp. 231-243,
2001.
[11] S, Sunder, N. H. Miller, and D.W. Shoesmith, "Corrosion of uranium
dioxide in hydrogen peroxide solutions," Corrosion Science, vol. 46, pp.
1095-1111, 2004.
[12] D. W. Shoesmith, "Fuel corrosion processes under waste disposal
conditions," J. Nucl. Mat., vol. 282, pp. 1-31, 2000.
[13] B. G. Santos, J. J. Nöel, and D.W. Shoesmith, "The effect of pH on the
anodic dissolution of SIMFUEL (UO2)," J. Electroanal. Chem., vol. 586,
pp. 1-11, 2006.
[14] D. W. Shoesmith, S. Sunder, M. G. Bailey, and G. J. Wallace, "The
corrosion of nuclear fuel (UO2) in oxygenated solutions," Corrosion Sci.,
vol. 29, No.9, pp. 1115-1128, 1989.
[15] J. S. Goldik, J. J. Noel, and D. W. Shoesmith, "Surface electrochemistry
of UO2 in dilute alkaline hydrogen peroxide solutions: Part II. Effects of
carbonate ions," Electrochimica Acta, vol. 51, pp. 3278-3286, 2006.
[16] B. G. Santos, J. J. Noel, and D. W. Shoesmith, "The influence of calcium
ions on the development of acidity in corrosion product deposits on
SIMFUEL, UO2," J. Nucl. Mat., vol. 350, pp. 320-331, 2006.
[17] P. G. Lucuta, R. A. Verrall, Hj Matzke, and B. J. Palmer, "Microstructural
features of SIMFUEL- Simulated high-burnup UO2-based nuclear fuel,"
J. Nucl. Mat., vol. 178, pp. 48-60, January 1991.
@article{"International Journal of Chemical, Materials and Biomolecular Sciences:60499", author = "Kwang-Wook Kim and Geun-Il Park and Eil-Hee Lee and Kune-Woo Lee and Kee-Chan Song", title = "Electrolytic Dissolutions of UO2 and SIMFUEL in Carbonate Solutions at Several pHs", abstract = "Electrolytic dissolution characteristics of UO2 and
SIMFUEL electrodes were studied at several potentials in carbonate
solutions of a high concentration at several pHs. The electrolytic
uranium dissolution was much affected by a corrosion product of
UO2CO3 generated at the electrode during the dissolution in carbonate
solution. The corrosion product distorted the voltammogram at UO2
and SIMFUEL electrodes in the potential region of oxygen evolution
and increased the overpotential of oxygen evolution at the electrode.
The effective dissolution in a carbonate solution could be obtained at
an applied potential such as +4 V (vs SSE) or more which had an
overpotential of oxygen evolution high enough to rupture the
corrosion product on the electrode surface.", keywords = "Anodic, Electrolytic, Dissolution, SIMFUEL,
Uranium dioxide, Carbonate", volume = "4", number = "11", pages = "715-4", }