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

Published online by Cambridge University Press:  26 February 2011

Karrie-Ann Kubatko
Affiliation:
khughes1@nd.edu, University of Notre Dame, Civil Engineering and Geological Sciences, 156 Fitzpatrick Hall, Notre Dame, IN, 46556, United States, 574 631 7216
Katie M. Gunderson
Affiliation:
Katie.Gunderson.5@nd.edu
Mark Antonio
Affiliation:
mantonio@anl.gov
Peter C. Burns
Affiliation:
pburns@nd.edu
L. Soderholm
Affiliation:
ls@anl.gov
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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.

Type
Research Article
Copyright
Copyright © Materials Research Society 2006

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References

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