Hostname: page-component-8448b6f56d-dnltx Total loading time: 0 Render date: 2024-04-24T13:18:29.645Z Has data issue: false hasContentIssue false

Phase Separation in Simulated Plutonium Glasses with Phosphate and Fluorine and the effect on Glass Corrosion in Water

Published online by Cambridge University Press:  03 September 2012

H. Li
Affiliation:
Pacific Northwest National Laboratory, Box 999, P8–37, Richland, WA 99352
J. D. Vienna
Affiliation:
Pacific Northwest National Laboratory, Box 999, P8–37, Richland, WA 99352
Y. L. Chen
Affiliation:
Pacific Northwest National Laboratory, Box 999, P8–37, Richland, WA 99352
L. Q. Wang
Affiliation:
Pacific Northwest National Laboratory, Box 999, P8–37, Richland, WA 99352
J. Liu
Affiliation:
Pacific Northwest National Laboratory, Box 999, P8–37, Richland, WA 99352
Get access

Abstract

The solubility limit of phosphate in glass was found to decrease as fluorine increased. Amorphous phase separation was found in the glass as a result of interaction between phosphate and fluorine, in which Ce and Gd strongly partitioned. The glasses exhibiting amorphous phase separation showed higher normalized B releases according to the 31-day product consistency test (PCT) compared to glasses without phase separation. Phosphate that leached from glass into water increased the concentrations of Ce and Gd in the 7- and 31-day PCT solutions by more than an order of magnitude. The liquid state 31P-NMR results suggested that phosphate in water interacts with Ce or Gd. Therefore, the observed concentration jump for Ce and Gd in the PCT solution may be attributed to the increases in the solubility limits of Ce and Gd as a result of phosphate complexation with Ce and Gd.

Type
Research Article
Copyright
Copyright © Materials Research Society 1997

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] Li, H., Vienna, J. D., Hrma, P., Schweiger, M.J., Smith, D.E., and Gong, M., in Ceramic Transaction (Am. Ceram. Soc. Proc, Westerville, OH, 1996) in press.Google Scholar
[2] Li, H., Darab, J.G., Smith, P.A., Schweiger, M.J., Smith, D.E., and Feng, X., in Nuclear Materials Management, Vol. XXIV (INMMProc, Northbrook, IL, 1995) p. 460465.Google Scholar
[3] Li, H., Schweiger, M., Hrma, P., and Feng, X., in Scientific Basis for Nuclear Waste Management XIX. Vol. 412, ed. by Murphy, W.M. and Knecht, D.A. (Mater. Res. Soc. Proc, Pittsburgh, PA, 1995) p. 213220.Google Scholar
[4] Vernaz, E.Y. and Godon, N., in Scientific Basis for Nuclear Waste Management XV. Vol. 257, ed. by Sombret, C.G. (Mater. Res. Soc. Proc, Pittsburgh, PA, 1992) p. 3748.Google Scholar
[5] Bates, J.K., Emery, J.W., Hoh, J.C., and Johnson, T.R., in Scientific Basis for Nuclear Waste Management XIX. Vol. 412, ed. by Murphy, W.M. and Knecht, D.A. (Mater. Res. Soc. Proc, Pittsburgh, PA, 1995) p. 5764.Google Scholar
[6] Jantzen, C.M., and Bibler, N.E., Report No. WSRC-TR-90–539 Rev. 1, Savannah River Laboratory, Aiken, SC, 1990.Google Scholar
[7] Li, H., Darab, J.G., Smith, P.A., Schweiger, M.J., Smith, D.E., and Hrma, P., in Nuclear Materials Management, Vol. XXIV, (INMM Proc, Northbrook, IL, 1995) p. 466471.Google Scholar
[8] Li, H., Vienna, J.D., Peeler, D.K., Hrma, P., and Schweiger, M.J., in Proceedings of the Plutonium Stabilization & Immobilization Workshop, CONF-951259, (U.S. Department of Energy, Washington DC, 1995) p. 241252.Google Scholar
[9] Li, H., Peng, B., and Vienna, J.D., Pacific Northwest National Laboratory, Richland, WA (unpublished).Google Scholar
[11] Ponader, C.W. and Brown, G.E. Jr., Geochem. Cosmochem. Acta, 53, 2905 (1989).10.1016/0016-7037(89)90167-1Google Scholar
[12] Ryerson, F.J. and Hess, P.C., Geochem. Cosmochem. Acta, 42, 921 (1978).Google Scholar
[13] Nelson, C., and Tallant, D.R., Phys. Chem. Glasses, 25, 31 (1984).Google Scholar
[14] Dupree, R., Holland, D. and Mortuza, M.G., Phys. Chem. Glasses, 29, 18 (1988).Google Scholar
[15] Gan, H., Hess, P.C., and Kirkpatrick, R.J., Geochem. Cosmochem. Acta, 58, 4633 (1994).10.1016/0016-7037(94)90196-1Google Scholar
[16] Rong, C., Li, H., Hrma, P., and Clio, H., in Ceramic Transactions (Am. Ceram. Soc. Proc, Westerville, OH, 1996) in press.Google Scholar
[17] Bingler, L.S. and Byrne, R.H., Polyhedron, 8, 1315 (1989).10.1016/S0277-5387(00)86529-8Google Scholar
[18] Lee, J.H. and Byrne, R.H., Geochem. Cosmochem. Acta, 56, 1127 (1992).10.1016/0016-7037(92)90050-SGoogle Scholar
[19] Rai, D., Felmy, A.R., Fulton, R.W., and Ryan, J.L., Radiochimica Acta, 58/59, 9 (1992).Google Scholar
[20] Rai, D., Felmy, A.R., and Fulton, R.W., Radiochimica Acta, 56, 7 (1992).Google Scholar