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Meta-Autunite Solubility as Related to Uranium Minerals in Concrete Waste Forms

Published online by Cambridge University Press:  01 February 2011

Shas Mattigod ,
Dawn Wellman ,
Julie Glovack ,
Bruce Arey  and
Marcus Wood
Shas Mattigod
Affiliation:
shas.mattigod@pnl.gov, Pacific Northwest National Laboratory, Energy & Environmental Directorate, 902 Battelle Blvd, Richland, WA, 99354, United States
Dawn Wellman
Affiliation:
dawn.wellman@pnl.gov, Pacific Northwest National Laboratory, Richland, WA, 99354, United States
Julie Glovack
Affiliation:
jglovack@mines.edu, Colorado School of Mines, Golden, CO, 80401, United States
Bruce Arey
Affiliation:
bruce.arey@pnl.gov, Pacific Northwest National Laboratory, Richland, WA, 99354, United States
Marcus Wood
Affiliation:
SMTP:Marcus_I_Wood@rl.gov, Fluor Hanford Inc., Richland, WA, 99354, United States
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Abstract

Previous in situ examination of U(VI) spiked concrete indicated that uranyl-oxyhydroxide phases that were initially formed, later led to the formation of mixed uranyl-oxyhydroxide/silicates, which subsequently transformed into uranyl-silicates, and finally altered into mixed uranyl-silicate/phosphate and uranyl-phosphate phases. We conducted solubility studies of the identified final uranyl-phosphate phase (calcium meta-autunite) in phosphate solutions ranging in concentration from 0.001 – 0.1M as a function of pH. These studies indicated a secondary phosphate phase that formed during the solubility of meta-autunite regulated the uranium concentrations at relatively low levels under high pH conditions (>12) typically encountered in cement pore waters. The importance of uranyl-phosphate minerals in concrete waste forms has, to date, been neglected because of the minimal amount of phosphorus present in most concrete compositions. However, because concrete is a continuously reacting solid, the thermodynamic stability of uranyl minerals that form at the later stages of reaction may have a substantial impact on the long-term fate of uranium in the waste forms. This study suggests that any future investigations should consider the potential benefit of including phosphorus in concrete waste forms.

Keywords

Usolution depositionscanning electron microscopy (SEM)
Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 1104: Symposium NN – Actinides 2008—Basic Science, Applications and Technology , 2008 , 1104-NN07-08
Copyright
Copyright © Materials Research Society 2008

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References

1 Mann, F. M., Puigh, R. J. II, Finfrock, S. H., E.J., J. Freeman, Khaleel, R., Bacon, D. H., Bergeron, M. P., McGrail, P. B. and Wurstner, S. K.. Hanford Immobilized Low-Activity Waste Performance Assessment: 2001 Version. Pacific Northwest National Laboratory, 2001.Google Scholar
2 Wood, M. I., Khaleel, R., Rittman, P. D., Lu, A. H., Finfrock, S., Serne, R. J. and Cantrell, K. J.. Performance Assessment for the Disposal of Low-Level Waste in the 218-W-5 Burial Ground. Westinghouse Hanford Company, 1995.10.2172/105099Google Scholar
3 Sutton, M., Warwick, P. and Hall, A.. Royal Society of Chemistry 5, 922–928 (2003).Google Scholar
4 Altenhein-Hasse, C., Bischoff, H., Fu, L., Mao, J. and Marx, G.. Journal of Alloys and Compounds 213/214, 554–556 (1994).Google Scholar
5 Matzen, S. L., Beiriger, J. M., Torretto, P. C., Zhao, P. and Viani, B. E.. Radiochimica Acta 88, 657–664 (2000).Google Scholar
6 Moroni, L. P. and Glasser, F. P.. Waste Management 15 (3), 243–254 (1995).Google Scholar
7 Sylwester, E. R., Allen, P. G., Zhao, P. and Viani, B. E.. Interactions of Uranium and Neptunium with Cementitious Materials studied by XAFS, pp. 1–7. Lawrence Livermore National Laboratory, 1999.Google Scholar
8 Sposito, G., The Chemistry of Soils (Oxford University Press, 1989) 277.Google Scholar
9 Bogue, R. H.. Chemistry of Portland Cement (Reinhold Publishing Corporation, 1955).Google Scholar
10 W. Taylor, H. F.. Cement Chemistry (Academic Press, 1990).Google Scholar
11 Wellman, D. M., Mattigod, S. V., Arey, B. W., Wood, M. I. and Forrester, S. W.. Cement and Concrete Research (2007).Google Scholar
12 Sutton, M., Warwick, P., Hall, A. and Jones, C.. Journal of Environmental Monitoring 1, 177 (1999).Google Scholar
13 Sutton, M., PDoctoral, h. D. Uranium Solubility, Speciation and Complexation at High pH., Loughborough University, 1999.Google Scholar
14 Serne, R. J., Rai, D., Martin, P. F., Felmy, A. R., Rao, L. and Ueta, S.. Leachability of Nd, U, Th, and Sr From Cements in a CO2 Free Atmosphere, in Leachability of Nd, U, Th, and Sr From Cements in a CO2 Free Atmosphere, Proceedings of Scientific Basis for Nuclear Waste Management XIX, Pittsburgh, Pennsylvania, (1996).Google Scholar
15 Serne, R. J., Lokken, R. O. and Criscenti, L. J.. Waste Management 12, 271–287 (1992).Google Scholar
16 Glasser, F. P.. Mineralogical Magazine 65 (5), 621–633 (2001).Google Scholar
17 Sandino, A. and Bruno, J.. Geochimica et Cosmochimica Acta 56, 4135–4145 (1992).10.1016/0016-7037(92)90256-IGoogle Scholar
18 Grenthe, I., Fuger, J., M. Konings, R. J., Lemire, R. J., Muller, A. B., Nguyen-Trung, C. and Wanner, H.. Chemical thermodynamics of uranium, editied by Wanner, H. and Forest, I. (OECD Nuclear Energy Agency, 1992), pp. 30–83.Google Scholar
19 Langmuir, D.. Aqueous Geochemistry of Uranium in Aqueous Environmental Chemistry (ed. McConnin, R.), (1997) pp. 494–512. Prentice-Hall.Google Scholar
20 Clark, D. L., Hobart, D. E. and Neu, M. P.. Chemical Reviews 95, 25–48 (1995).Google Scholar