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Study of Natural Minerals of U-Ryrochlore-Type Structure as Analogues of Plutonium Ceramic Waste-form

Published online by Cambridge University Press:  21 March 2011

Roman V. Bogdanov ,
Yuri F. Batrakov ,
Elena V. Puchkova ,
Andrey S. Sergeev  and
Boris E. Burakov
Roman V. Bogdanov
Affiliation:
Department of Chemistry, Saint-Petersburg State University, University Emb., 7/9, St. Petersburg, 199034, Russia; tel.: (7)-(812) 328-9446; fax: (7)-(812)-328-2835; e-mail:r.bogdanov@RB7584.spb.edu
Yuri F. Batrakov
Affiliation:
Department of Chemistry, Saint-Petersburg State University, University Emb., 7/9, St. Petersburg, 199034, Russia; tel.: (7)-(812) 328-9446; fax: (7)-(812)-328-2835; e-mail:r.bogdanov@RB7584.spb.edu
Elena V. Puchkova
Affiliation:
Department of Chemistry, Saint-Petersburg State University, University Emb., 7/9, St. Petersburg, 199034, Russia; tel.: (7)-(812) 328-9446; fax: (7)-(812)-328-2835; e-mail:r.bogdanov@RB7584.spb.edu
Andrey S. Sergeev
Affiliation:
Department of Geology, Saint-Petersburg State University, St. Petersburg, 199034, Russia
Boris E. Burakov
Affiliation:
V.G. Khlopin Radium Institute, St. Petersburg, 194021, Russia
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Abstract

At present, crystalline ceramic based on titanate pyrochlore, (Ca,Gd,Hf,Pu,U)2Ti2O7, is considered as the US candidate waste form for the immobilization of weapons grade plutonium. Naturally occuring U-bearing minerals with pyrochlore-type structure: hatchettolite, betafite, and ellsworthite, were studied in orders to understand long-term radiation damage effects in Pu ceramic waste forms. Chemical shifts (δ) of U(Lδ1)– and U(Lβ1) – X-ray emission lines were measured by X-ray spectrometry. Calculations were performed on the basis of a two-dimensional δLá1- and δLδ1- correlation diagram. It was shown that 100% of uranium in hatchettolite and, probably, 95-100% of uranium in betafite are in the form of (UO2)2+. formal calculation shows that in ellsworthite only 20% of uranium is in the form of U4+ and 80% of the rest is in the forms of U5+ and U6+. The conversion of the initial U4+ ion originally occurring in the pyrochlore structure of natural minerals to (UO2)2+ due to metamict decay causes a significant increase in uranium mobility.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 713: Symposium JJ – Scientific Basis for Nuclear Waste Management XXV , 2002 , JJ2.2
Copyright
Copyright © Materials Research Society 2002

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