Abstract
The presence of laterally-extensive zones of zeolitized tuff underlying the proposed high-level nuclear waste repository at Yucca Mt., Nevada, has focused attention on the potential role of zeolite minerals, particularly clinoptilolite, in sorbing radionuclides and thereby retarding their migration. Ion exchange between zeolites and aqueous solutions depends on factors including compositions of the aqueous and zeolite phases and solution concentration. In addition, the thermodynamic stability of zeolite minerals and their susceptibility to diagenetic alteration also depend on aqueous and solid phase compositions. Therefore, spatial variations in zeolite compositions which have been observed at Yucca Mt., as well as natural or repository-induced changes in groundwater chemistry, may result in variations in the effectiveness of the zeolite minerals as retardation agents. p]Ion exchange experiments were conducted to obtain isotherm data and to evaluate the use of thermodynamic models in describing and predicting the solid solution and ion exchange properties of clinoptilolite. The experimental data were interpreted using excess Gibbs energy models for the aqueous solution and zeolite phases to account for nonideality in the system. The results indicate that the thermodynamic models allow predictions of clinoptilolite ion exchange behavior at ionic strengths and relative concentrations for which data are absent, and provide a foundation for the interpretation of ion exchange equilibria in multicomponent geochemical systems.
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W.R. Daniels, K. Wolfsberg, R.S. Rundberg, A.E. Ogard, J.F. Kerrisk, C.J. Duffy, T.W. Newton, S.D. Knight, F.O. Lawrence, V.L. Rundberg, M. Sykes, G. Thompson, B. Travis, E. Treher, R. Vidale, G. Walter, R. Aguilar, M. Cisneros, S. Maestas, A. Mitchell, P. Oliver, P. Oliver, N. Raybold, and P. Wanek, Summary Report on the Geochemistry of Yucca Mountain and Environs. LA-9328-MS, Los Alamos Nat. Lab., Los Alamos, NM (1982).
R.E. Meyer, W.D. Arnold, F.I. Case, G.D. O'Kelley, and J.F. Land, Effects of Mineralogy on Sorption of Strontium and Cesium onto Calico Hills Tuff, NUREG/CR-5463 ORNL-6589, Oak Ridge Nat. Lab., Oak Ridge, TN (1987).
D.E. Broxton, R.G. Warren, R.C. Hagan, and G. Luedemann, Chemistry of Diagenetically Altered Tuffs at a Potential Nuclear Waste Repository, Yucca Mountain, Nve County, Nevada. LA-10802-MS, Los Alamos Nat. Lab., Los Alamos, NM (1986).
R.M. Barrer, in Natural Zeolites: Occurrence, Properties. Use, edited by L.B. Sand and F.A. Mumpton (Pergamon Press, New York, 1978) p. 385.
T.S. Bowers and R.G. Burns, Amer. Min. 75, 601 (1990).
L.L. Ames, Amer. Min. 49, 127 (1964); 49, 1099 (1964).
M.J. Semmens and M. Seyfarth, in Natural Zeolites: Occurrence, Properties. Use (Pergamon Press, New York, 1978), p. 517.
R.P. Townsend and M. Loizidou, Zeolites 4, 191 (1984).
M.F. Cheleshev, B.G. Berenschtein, T.A. Berenschtein, H.K. Grebanova, and H.C Martinova, Dokl. Akad. Nauk SSSR 210, 1110 (1973).
M.A. Jama and H. Yucel, Sep. Sci. Technol. 24, 1393 (1990).
D.W. Breck. Zeolite Molecular Sieves (Wiley, New York, 1976), p. 699.
R.M. BarrerR. M. and J. Klinowski, J. Chem. Soc, Faraday Trans. I 70, 2080 (1974).
R.M. Barrer, in Natural Zeolites: Occurrence, Properties. Use, edited by L.B. Sand and F.A. Mumpton (Pergamon Press, New York, 1978) p. 385.
F. Helfferich, Ion Exchange (McGraw-Hill, New York, 1962).
A. Dyer, H. Enamy and R.P. Townsend, Sep. Sci. Technol. 16, 173 (1981).
A.P. Vanselow, Soil Sci. 33, 95 (1932).
R.P. Townsend, Pure Appl. Chem. 58, 1359 (1986).
G.L. Gaines and H.G. Thomas, J. Chem. Phys. 21, 714 (1953).
G. Sposito, Thermodynamics of Soil Solutions (Clarendon Press, Oxford, 1981).
W.J. Argersinger, A.W. Davidson and O.D. Bonner, Trans. Kansas Acad. Sci. 53, 404 (1950).
R.M. Barrer and A.J. Walker, Trans. Far. Soc. 60, 171 (1964).
P. Fletcher and R. Townsend, J. Chem. Soc. Far. Trans. I 81, 1731 (1985).
E. Glueckauf, Nature 163, 414 (1949).
K.S. Pitzer, J. Phys. Chem. 77, 268 (1973).
K.S. Pitzer, Rev. Mineralogy 17, 97 (1987).
G. Scatchard, J. Amer. Chem. Soc. 90, 3124 (1968).
E.A. Guggenheim, Philos. Mag. 19, 588 (1935).
S.A. Grant and D.L. Sparks, J. Phys. Chem. 93, 6265 (1989).
J. Ganguly and S.K. Saxena, Mixtures and Mineral Reactions (Springer-Verlag, Berlin, 1987), p. 14.
R.P. Townsend, P. Fletcher, and M. Loizidou, in Proceedings of the 6th International Zeolite Conf., edited by D. Olson and A. Bisio (Butterworths, U.K., 1984), p. 110.
R.T. Pabalan and W.M. Murphy, Progress in Experimental Studies on the Thermodynamic and Ion Exchange Properties of Clinoptilolite. CNWRA-89-006, Center for Nuclear Waste Regulatory Analyses, San Antonio, TX 78228-0510 (1990).
Acknowledgements
The assistance of P. Bertetti with the experiments, the helpful discussions with W.M. Murphy, and the thorough review by B. Vianni are gratefully acknowledged. This work was supported by the U.S. Nuclear Regulatory Commission under Contract No. NRC-02-88-005 and was conducted for the Waste Management Branch of the Office of Nuclear Regulatory Research.
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Pabalan, R.T. Nonideality Effects on the Ion Exchange Behavior of the Zeolite Mineral Clinoptilolite. MRS Online Proceedings Library 212, 559–567 (1990). https://doi.org/10.1557/PROC-212-559
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DOI: https://doi.org/10.1557/PROC-212-559