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The Radiation Induced Chemistry of the Uranyl Cation in Carbonate –Bicarbonate Solutions as Followed by NMR Spectroscopy

Published online by Cambridge University Press:  26 February 2011

Bruce Kevin McNamara ,
Lanee A. Snow ,
Chuck Z. Soderquist ,
Sergei Sinkov ,
Herman M. Cho  and
Judah I. Friese
Bruce Kevin McNamara
Affiliation:
bruce.mcnamara@pnl.gov, Pacific Northwest National Laboratory, Environmental Technology Division, PO Box 999, Richland, Washington, 99352, United States, 509-376-1408
Lanee A. Snow
Affiliation:
Lanee.snow@pnl.gov, United States
Chuck Z. Soderquist
Affiliation:
chuck.soderquist@pnl.gov
Sergei Sinkov
Affiliation:
sergei.sinkov@pnl.gov
Herman M. Cho
Affiliation:
herman.cho@pnl.gov
Judah I. Friese
Affiliation:
judah.friese@pnl.gov
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Abstract

Hydrogen peroxide formed by radiolysis of carbonate –bicarbonate media was followed by 13C NMR using dissolved [233UO2(13CO3)3]4- as the alpha source (Dα=12.1 Gy/hr). It is shown that the speciation of the peroxide carbonates (or other species) that are formed in the pH region 5.9 and 11.6 by titration with hydrogen peroxide are common to those formed by hydrogen peroxide generated by radiolysis. Radiolytic generation of hydrogen peroxide was followed by observing the formation of a uranyl peroxide carbonate complex. Complex formation was observed to accelerate for about 1200 hours and to terminate between 1×10-4 and 5×10-4 M. It is assumed that either a steady state H2O2 production rate was established in solution or that some limiting feature of the experiment was responsible for slowing the yield of product.

Keywords

actinideradiation effectsnuclear magnetic resonance (NMR)
Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 893: Symposium JJ – Actinides 2005 – Basic Science, Applications and Technology , 2005 , 0893-JJ08-07
Copyright
Copyright © Materials Research Society 2006

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References

REFERENCES

1. Wronkiewicz, D., Buck, E., Uranium Mineralogy and the Geologic Disposal of Spent Nuclear Fuel, in Uranium: Minerology, Geochemistry and the Environment, Volume 38 Burns, P. C. & Finch, R., Eds, Mineralogical Society of America, 2005.Google Scholar
2. McNamara, B. K., Buck, E. C., Hanson, B. D.: Mater. Res. Soc.Symp. Proc., 757, 401 (2003).Google Scholar
3. Sattonnay, G.., Ardois, C., Corbel, C., Lucchioni, J. F., Barthe, M. F., Garrido, F., Gosset, D., J. Nucl. Mater. 288, 11 (2001).Google Scholar
4. Kubatko, K. A. H., Helean, K. B., Burns, P. C., Science, 302, 1191–1193, 2003.Google Scholar
5. Glasoe, P. K., Long, F. A., J. Phys. Chem., 64, 188 (1960).Google Scholar
6. Jeffery, G. H., Bassett, J., Mendham, J., Denney, R. C., Vogel's Textbook of Quantitative Chemical Analysis, 5th Edition, Longman Group UK Limited, Essex CM20 2JE, England, Page 372, 1989.Google Scholar
7. Allen, P. G., Bucher, J. J., Clark, D. L., Edelstein, N. M., Ekberg, S. A., Gohdes, J. W., Hudson, E. A., Kaltsoyannis, N., Lukens, W. W., Neu, M. P., Palmer, P. D., Reich, T., Shuh, D. K., Tait, C. D., and Zwick, B. D., Inorg. Chem., 34, 4797–4807 (1997).Google Scholar
8. Thompson, M. E., Nash, K. L., Sullivan, J. C., Isr. J. Chem., 25 (2) 155 (1985).Google Scholar
9. Zehnder, R. A., Peper, S. M., Scott, B. L., Runde, W. H., Acta Cryst., C61, i3 (2005).Google Scholar
10. Cai, Z., Li, X., Katsumura, Y., Urabe, O., Nuclear Technology, 136, 231 (2001).Google Scholar