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79Se: Geochemical and Crystallo-Chemical Retardation Mechanisms

Published online by Cambridge University Press:  10 February 2011

Fanrong Chen ,
Peter C. Burns  and
Rodney C. Ewing
Fanrong Chen
Affiliation:
Department of Nuclear Engineering and Radiological Sciences, The University of Michigan, Ann Arbor, MI 48109–2104
Peter C. Burns
Affiliation:
Department of Civil Engineering and Geological Sciences University of Notre Dame, Notre Dame, IN 46556
Rodney C. Ewing
Affiliation:
Department of Civil Engineering and Geological Sciences University of Notre Dame, Notre Dame, IN 46556
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Abstract

79Se is a long-lived (1.1×106 years) fission product which is chemically and radiologically toxic. Under Eh-pH conditions typical of oxidative alteration of spent nuclear fuel, selenite or selenate are the dominant aqueous species of selenium. Because of the high solubility of metalselenites and metal-selenates and the low adsorption of selenite and selenate aqueous species under alkaline conditions, selenium may be highly mobile. However, 79Se released from altered fuel may be immobilized by incorporation into secondary uranyl phases as low concentration impurities, and this may significantly reduce the mobility of selenium. Analysis and comparison of the known structures of uranyl phases indicate that (SeO3) may substitute for (SiO3OH) in structures with the uranophane anion-topology (α.-uranophane, sklodowskite, boltwoodite) which are expected to be the dominant alteration phases of UO2 in Si-rich groundwater. The structural similarity of guillemninite, Ba[(UO2)3 (SeO3)2O2](H2O) 3 to phurcalite, [(UO2)3(PO4)2O2](H2O)7, suggests that the substitution (SeO3)↔ (PO4) may occur in phurcalite. The close similarity between the sheets in the structures of rutherfordine and [(UO2)(SeO3)] implies that the substitution (SeO3) ↔ (CO3) can occur in rutherfordine. However, the substitutions: (SeO3) ↔ (SiO3OH) in soddyite and (SeO3) ↔ (PO4) in phosphuranylite may disrupt their structural connectivity and are unlikely to occur.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 556: Symposium QQ – Scientific Basis for Nuclear Waste Management XXII , 1999 , 1115
Copyright
Copyright © Materials Research Society 1999

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