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Local environment of iron and uranium ions in vitrified iron phosphate glasses studied by Fe K and U LIII-edge x-ray absorption fine structure spectroscopy

Published online by Cambridge University Press:  31 January 2011

M. Karabulut ,
G. K. Marasinghe ,
C. S. Ray ,
D. E. Day ,
G. D. Waddill ,
P. G. Allen ,
C. H. Booth ,
J. J. Bucher ,
D. L. Caulder  and
D. K. Shuh
...Show all authors
M. Karabulut
Affiliation:
Department of Physics and Graduate Center for Materials Research, University of Missouri–Rolla, Rolla, Missouri 65409–1170, and Department of Physics, University of Kafkas, Kars, Turkey
G. K. Marasinghe
Affiliation:
Department of Physics and Graduate Center for Materials Research, University of Missouri–Rolla, Rolla, Missouri 65409–1170
C. S. Ray
Affiliation:
Department of Physics and Graduate Center for Materials Research, University of Missouri–Rolla, Rolla, Missouri 65409–1170
D. E. Day
Affiliation:
Department of Physics and Graduate Center for Materials Research, University of Missouri–Rolla, Rolla, Missouri 65409–1170
G. D. Waddill
Affiliation:
Department of Physics and Graduate Center for Materials Research, University of Missouri–Rolla, Rolla, Missouri 65409–1170
P. G. Allen
Affiliation:
Analytical and Nuclear Chemistry Division, Lawrence Livermore National Laboratory, Livermore, California 94551
C. H. Booth
Affiliation:
Chemical Sciences Division, The Glenn T. Seaborg Center, Lawrence Berkeley National Laboratory, Berkeley, California, 94720
J. J. Bucher
Affiliation:
Chemical Sciences Division, The Glenn T. Seaborg Center, Lawrence Berkeley National Laboratory, Berkeley, California, 94720
D. L. Caulder
Affiliation:
Chemical Sciences Division, The Glenn T. Seaborg Center, Lawrence Berkeley National Laboratory, Berkeley, California, 94720
D. K. Shuh
Affiliation:
Chemical Sciences Division, The Glenn T. Seaborg Center, Lawrence Berkeley National Laboratory, Berkeley, California, 94720
M. Grimsditch
Affiliation:
Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439
M-L. Saboungi
Affiliation:
Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439
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Abstract

The local structure of iron and uranium ions in a series of iron phosphate glasses with the general composition (40 – x)Fe2O3–xUO2–60P2O5 and (1–x–y)(40Fe2O3–60P2O5)– xUO2–y(Na2O or CaO) was investigated using Fe K-edge and U LIII-edge x-ray absorption fine structure spectroscopy. Replacing Fe2O3 by UO2 in the glass caused more distortion in the coordination environment of Fe(III) ions. Extended x-ray absorption fine structure fits revealed that the Fe–P bonds observed in the base glass also existed in all the waste-loaded glasses. X-ray absorption near-edge structure showed that the uranium ions were predominantly present as U(IV) in the glasses. Uranium ions were coordinated to approximately 8 ± 1 oxygen atoms and 2.5 ± 0.6 phosphorus atoms at an average distance of 2.47 ± 0.02 and 3.8 ± 0.02 Å, respectively. There were no Fe–U or U–Fe neighbors observed, indicating that uranium ions occupied voids in the glass away from the PO4 units. These conclusions were supported by Mössbauer, x-ray photoelectron, and Raman spectroscopic data.

Type
Articles
Information
Journal of Materials Research , Volume 15 , Issue 9 , September 2000 , pp. 1972 - 1984
Copyright
Copyright © Materials Research Society 2000

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