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Presence and Persistence of Uranyl Peroxide Nanoclusters in Contact with Geological Media

  • Karrie-Ann Kubatko (a1), Katie M. Gunderson (a2), Mark Antonio (a3), Peter C. Burns (a4) and L. Soderholm (a5)...

Abstract

Recently uranyl peroxide nanoclusters containing 24, 28, and 32 uranyl polyhedra were chemically and structurally characterized under alkaline conditions. Such nanoclusters could conceivable form from oxidative alteration of nuclear waste in a geological repository by incorporating peroxide formed by alpha-radiolysis of water or in tanks where high-level waste is stored. The stability and persistence of uranyl peroxides in the vadose zone will be impacted by their interaction with geological media. Here we report batch experiments of solutions containing monodisperse nanoclusters in contact with crushed welded tuff. Within the first 72 hours, U concentrations in solution remained unchanged; however concentrations of Si, Al, Ca, Mg, Na, and Fe increased due to the dissolution of calcium-bearing aluminum silicate minerals in the welded tuff. Despite the presence of excess Li+ in solution, within two weeks crystals precipitated in which Ca2+ replaced Li+ in the nanocluster cage.

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1. Banfield, J. F., Zhang, H., Rev. Mineral. Geochem., 44, 1 (2001).
2. Burns, P. C., Kubatko, K. A, Sigmon, G., Fryer, B. J., Gagnon, J. G., Antonio, M. R., Soderholm, L., Angew. Chem., 117, 2173 (2005).
3. Sheldrick, G. M., SHELXTL, Version 6.12; Bruker AXC, Inc.: Madison, WI (1997).
4. Ibers, J. A., Hamilton, W. C., Eds., International Tables for X-ray Crystallography, IV. The Kynoch Press, Birmingham, U.K. (1974).

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