Hostname: page-component-586b7cd67f-dsjbd Total loading time: 0 Render date: 2024-11-23T07:17:24.260Z Has data issue: false hasContentIssue false
  • English
  • Français

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, [email protected]
W.J. Weber
Affiliation:
Pacific Northwest National Laboratory, Richland, WA 99352
S.D. Conradson
Affiliation:
Los Alamos National Laboratory, Los Alamos, NM 87545
Get access

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

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

1 Weber, W.J., Wald, J.W., and McVay, G.L., Comm. Am. Ceram. Soc., p. C–253 (1985).Google Scholar
2 Weber, W.J., J. Mater. Res. 5, p. 2687 (1990).Google Scholar
3 Rehr, J.J., Zabinsky, S.I., and Albers, R.C., Phys. Rev. Let. 69, p. 3397 (1992).Google Scholar
4 Zabinsky, S.I., Rehr, J.J., Ankudinov, A., Albers, R.C., and Eller, M.J., Phys. Rev. B. 52, p. 2995 (1995).Google Scholar
5 Eller, P.G., Jarvinen, G.D., Purson, J.D., Penneman, R.A., Ryan, R.R., Lytle, F.W., and Greegor, R.B., Radiochem. Acta 39, p. 17 (1985).Google Scholar
6 Petiau, J., Calas, G., Petimaire, D., Bianconi, A., Benfatto, M., and Marcelli, A., Phys. Rev. B34, p. 7350 (1986).Google Scholar
7 Calas, G., Brown, G.E. Jr., Waychunas, G.A., and Petiau, J., Phys. Chem. Min. 15, p. 19 (1987).Google Scholar
8 Greaves, G.N., Barrett, N.T., Antonini, G.M., Thornley, F.R., Willis, B.T.M., and Steel, A., J. Am. Chem. Soc. 111, p. 4313 (1989).Google Scholar
9 Biwer, B.M., L. Soderholm, Greegor, R.B., and Lytle, F.W., Mater. Res. Soc Proc., 1996.Google Scholar
10 Smyth, J.R. and Bish, D.L., Crystal Structures and Cation Sites of the Rock-Forming Minerals, Allen & UNWIN, Boston, 1988, 332 p.Google Scholar
11 Calas, G. and Petiau, J., Solid State Comm. 48, p. 625 (1983).Google Scholar
12 Farges, F. and Calas, G., Am. Mineral. 76, p. 60 (1991).Google Scholar