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X-Ray Absorption Fine Structure of Aged, Pu-Doped Glass and Ceramic Waste Forms

Published online by Cambridge University Press:  10 February 2011

N.J. Hess ,
W.J. Weber  and
S.D. Conradson
N.J. Hess
Affiliation:
Pacific Northwest National Laboratory, Richland, WA 99352, nj_hess@pnl.gov
W.J. Weber
Affiliation:
Pacific Northwest National Laboratory, Richland, WA 99352
S.D. Conradson
Affiliation:
Los Alamos National Laboratory, Los Alamos, NM 87545
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Abstract

X-Ray Absorption Fine Structure (XAFS) spectroscopic studies were performed on a suite of compositionally identical Pu-doped simulated waste glasses prepared 15 years ago at different aactivities by varying the 239Pu/f238 Pu isotopic ratio. The resulting α-activities range from 1.9 × 107 to 4.2 × 109 Bq/g. These samples have a current, accumulated dose that ranges from 8.8 × 1018 to 1.9 × 1018 αdecays/g. A second suite of polycrystalline zircon samples that were synthesized 16 years ago with 10.0 wt.% Pu was also investigated. The 239Pu238Pu isotopic ratio in these samples resulted in α-activities of 2.5 × 108 and 5.6 × 1010 Bq/g and an accumulated dose of 1.2 × 1017 and 2.8 × 1019 α-decays/g. The multicomponent composition of the simulated waste glass permitted XAFS investigation at six elemental absorption edges. For both the glass and ceramic waste forms, initial analysis of Extended X-Ray Absorption Fine Structure (EXAFS) and X-Ray Absorption Near Edge Structure (XANES) indicate that the local environment around the cations exhibit different degrees of disorder as a result of the accumulated a-decay dose. In general cations with short cationoxygen bonds show little effect from self-radiation where as cations with long cation-oxygen bonds show a greater degree of disorder with accumulated a-decay dose.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 506: Symposium – Scientific Basis for Nuclear Waste Management XXI , 1997 , 169
Copyright
Copyright © Materials Research Society 1998

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References

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