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Secondary Phase Formation During Nuclear Waste-Glass Dissolution

Published online by Cambridge University Press:  02 April 2024

T. A. Abrajano ,
J. K. Bates ,
A. B. Woodland ,
J. P. Bradley  and
W. L. Bourcier
T. A. Abrajano
Affiliation:
Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439
J. K. Bates
Affiliation:
Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439
A. B. Woodland
Affiliation:
Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439
J. P. Bradley
Affiliation:
McCrone Associates, Inc., 850 Pasquinelli Drive, Westmont, Illinois 60559
W. L. Bourcier
Affiliation:
Lawrence Livermore National Laboratory, Yucca Mountain Project, P.O. Box 5514, Livermore, California 94551
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Abstract

Secondary minerals formed during simulated weathering of nuclear waste glasses have been identified by analytical electron microscopy. A complete description of the reacted glass, from the outermost surface in direct contact with the leachant solution to the reacting front that migrates into the bulk glass, was obtained. Manganese and iron oxyhydroxide phases and saponite were found to have precipitated onto the residual glass surface from the leachant solution. Iron-bearing smectite, serpentine, and manganese and uranium-titanium oxyhydroxides formed in situ in the glass in several distinct bands at different depths beneath the original surface. This sequential development of secondary phases displays a clear trend toward more order and crystallinity in the phases farthest from the reaction front and indicates that complete restructuring of the glass into crystalline phases did not occur at the interface with fresh glass. Additionally, the formation of a discrete uranium-bearing phase, as opposed to uranium uptake by precipitated phases, suggests that stable actinide phase formation rather than ion exchange may be a possible mechanism for retarding radionuclide release to the environment.

Keywords

DissolutionGlassHydrationManganese oxideNuclear wasteSerpentineSmectiteUranium

Information

Type
Research Article
Information
Clays and Clay Minerals , Volume 38 , Issue 5 , October 1990 , pp. 537 - 548
Copyright
Copyright © 1990, The Clay Minerals Society

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References

Abrajano, T. A. Jr. Bates, J. K., Gerding, T. J. and Ebert, W. L., 1988 The reaction of glass in a gamma irradiated saturated tuff environment, Part 3: Long-term experiments at 1 × 104 rad/hour: Argonne Natl. Lab. Rept. 88 1 – 117.Google Scholar
Abrajano, T. A. Jr. Bates, J. K., Bradley, J. P. and Mellinger, G., 1989 Analytical electron microscopy of leached nuclear waste glasses Ceramic Transactions, Vol. 9, Nuclear Waste Management IH Ohio American Ceramic Society, Westerville.Google Scholar
Bates, J. K., Lam, D. J., Steindler, M. J. and Brookins, D. G., 1983 Extended leach studies of actinide doped SRL 131 glass Scientific Basis for Nuclear Waste Management VI New York North-Holland 183 – 190.Google Scholar
Bourcier, W. L., 1989 Geochemical modeling of radioactive waste glass Lawrence Liver more Natl. Lab. Rept. 1 – 7.Google Scholar
Bourcier, W. L., Peiffer, D. W., Knauss, K. G., McKeegan, K. D., Smith, D. K., Oversby, V. and Brown, P., 1990 A kinetic model for bo-rosilicate glass dissolution based on dissolution affinity of a surface alteration layer Scientific Basis for Nuclear Waste Management XIII Pittsburgh Materials Research Society 209 – 216.Google Scholar
Bradley, J. P., 1988 Analysis of chondritic interplanetary dust thin sections Geochim. Cosmochim. Acta 52 889 – 900.CrossRefGoogle Scholar
Bradley, J. P. and Brownlee, D. E., 1989 Cometary particles: Thin sectioning and electron beam analysis Science 231 1542 – 1544.CrossRefGoogle Scholar
Bradley, J. P., Germani, M. S. and Brownlee, D. E., 1989 Automated thin-film analysis of anhydrous interplanetary dust particles in the analytical electron microscope Earth Planet. Sci. Lett. 93 1 – 13.CrossRefGoogle Scholar
Chen, C. C., Golden, D. C. and Dixon, J. B., 1986 Transformation of synthetic birnessite to cryptomelane: An electron microscope study Clays & Clay Minerals 34 565 – 571.CrossRefGoogle Scholar
Cliff, G. and Lorimer, G. W., 1975 The quantitative analysis of thin sections J. Microsc. 103 203 – 207.CrossRefGoogle Scholar
DOE, 1989 Site characterization plan, Yucca Mountain Site: Nevada Research and Development Area U.S. Dept. of Energy Rept..Google Scholar
Doremus, R. H., 1973 Glass Science New York Wiley 76 – 92.Google Scholar
Ebert, W. L., Bates, J. K. and Gerding, T. J., 1990 The reaction of glass during gamma irradiation in a saturated tuff environment, Part 4: SRL 165, ATM-lc, and ATM-8 glasses at 1E3 R/h and 0 R/h Argonne Natl. Lab. Rept. 5 – 17.CrossRefGoogle Scholar
Egerton, R. R., 1986 Electron Energy-Loss Spectroscopy in the Electron Microscope New York Plenum Press.Google Scholar
Giovanoli, R. and Balmer, B., 1981 A new synthesis of hollandite. A possibility for immobilization of nuclear waste Chima 35 53 – 55.Google Scholar
Giovanoli, R., Stahli, E. and Feitkuecht, W., 1970 Über Oxihydroxide des vierwertigen Mangans mit Schichtengitter 1. Natrium-Mangan(II,III) Manganat(IV) Helv. Chim. Acta 53 209 – 215.CrossRefGoogle Scholar
Golden, D. C., Dixon, J. B. and Chen, C. C., 1986 Ion exchange thermal transformations and oxidizing properties of birnessite Clays & Clay Minerals 34 511 – 520.CrossRefGoogle Scholar
Godon, N., Thomassin, J., Touray, J. and Vernaz, E., 1988 Experimental alteration of R7T7 nuclear model glass in solutions with different salinities (90°C, 1 bar): Implications for the selection of geological repositories J. Mat. Sci. 23 126 – 132.CrossRefGoogle Scholar
Grambow, B., Jantzen, M., Stone, J. A. and Ewing, R. C., 1985 A general rate equation for nuclear waste glass corrosion Scientific Basis for Nuclear Waste Management VIII, C. Pittsburgh Materials Research Society 15 – 27.Google Scholar
Lutze, W., Malow, G., Rabe, H. and Brookins, D. G., 1983 Surface layer formation on a nuclear waste glass Scientific Basis for Nuclear Waste Management VI New York North-Holland 37 – 45.Google Scholar
Mendel, J. E., 1984 Final report of the defense high level waste leaching mechanisms program Battelle Pacific Northwest Lab. Rept. .CrossRefGoogle Scholar
Murakami, T., Bamba, T., Jercinovic, M., Ewing, R., Lutze, W. and Ewing, R., 1989 Formation and evolution of alteration layers on borosilicate and basalt glasses: Initial stage Scientific Basis for Nuclear Waste Management XII Pittsburgh Materials Research Society 65 – 72.Google Scholar
Newman, S., Stolper, E. M. and Epstein, S., 1986 Measurement of water in rhyolitic glasses: Calibration of an infrared spectroscopic technique Amer. Mineral. 71 1527 – 1541.Google Scholar
Ringwood, A. E. and Kesson, S. E., 1988 SYNROC Radioactive Waste Forms for the Future New York North-Holland 156 – 177.Google Scholar
Sheridan, P., 1989 Determination of experimental and theoretical KAS: Factors for a 200 keV analytical electron microscope J. Electron Microsc. Tech. 11 41 – 61.CrossRefGoogle Scholar
Slate, S. C., Jantzen, C., Stone, J. and Ewing, R., 1985 Standardized waste form test methods Scientific Basis for Nuclear Waste Management VIII Pittsburgh Materials Research Society 741 – 746.Google Scholar
Tafto, J. and Zhu, J., 1982 Electron energy loss near edge structure (ELNES), a potential technique in the studies of local atomic arrangements Ultramicroscopy 9 349 – 454.CrossRefGoogle Scholar
Wicks, F. G., O’Hanley, D. S. and Bailey, S. W., 1988 Serpentine minerals: Structures and petrology Hydrous Phyllosilicates (Exclusive of Micas), Reviews in Mineralogy, Vol. 19 Washington, D.C. Mineralogical Society of America 91 – 167.CrossRefGoogle Scholar
Wicks, G. G., Stone, J. A., Chandler, G. T. and Williams, S., 1986 Long-term leaching behavior of simulated, Savannah River Plant waste glass: E.I. du Pont de Nemours Co. Savannah River Lab. Rept. 1 – 37.Google Scholar
Wilson, M. D. and Pittman, E. D., 1977 Authigenic clays in sandstones: Recognition and influence of reservoir properties and Paleoenvironmental analysis J. Sed. Pet. 47 3 – 31.Google Scholar