Hostname: page-component-8448b6f56d-tj2md Total loading time: 0 Render date: 2024-04-16T11:52:15.400Z Has data issue: false hasContentIssue false

Deliquescence Behavior of Multicomponent Salts: Effects on the Drip Shield and Waste Package Chemical Environment of the Proposed Nuclear Waste Repository at Yucca Mountain, Nevada

Published online by Cambridge University Press:  21 March 2011

Roberto T. Pabalan
Affiliation:
Center for Nuclear Waste Regulatory Analyses, San Antonio, TX 78238-5166, U.S.A.
Lietai Yang
Affiliation:
Center for Nuclear Waste Regulatory Analyses, San Antonio, TX 78238-5166, U.S.A.
Lauren Browning
Affiliation:
Center for Nuclear Waste Regulatory Analyses, San Antonio, TX 78238-5166, U.S.A.
Get access

Abstract

Thermodynamic calculations were conducted to determine the deliquescence behavior of salt mixtures and to simulate the evaporation of Yucca Mountain groundwaters. The results are consistent with published experimental data that show the deliquescence points of salt mixtures are lower than that of individual salts. For mixtures of NaCl and KCl salts, the deliquescence point of pure NaNO3 salt is an appropriate lower bound. However, mixtures containing magnesium and calcium salts have much lower deliquescence points than pure NaNO3. If magnesium and calcium salts are deposited on waste package and drip shield surfaces, it could lead to earlier initiation of aqueous corrosion than assumed by the DOE in its performance assessment abstractions. Such salt mixtures can be formed by evaporation of waters with compositions similar to some Yucca Mountain porewaters and would be characterized by low deliquescence relative humidity, high chloride concentration, and low concentrations of anions such as free (uncomplexed) nitrate and sulfate that could mitigate against the chloride-enhanced corrosion of the waste package. Evaporation of Yucca Mountain groundwaters also could lead to fluoride concentrations that are above the threshold for accelerated corrosion of the titanium drip shield.

Type
Research Article
Copyright
Copyright © Materials Research Society 2002

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] Civilian Radioactive Waste Management System Management & Operating Contractor, TDR-WISRL-000001 Rev. 03., 2000.Google Scholar
[2] Ge, Z., Wexler, A. S., and Johnston, M. V., J. Phys. Chem. A, 102, 173 (1998).Google Scholar
[3] Bechtel SAIC Company, TDR-MGR-MD-000007 Rev. 00 ICN 01, 2001.Google Scholar
[4] Tang, I. N. and Munkelwitz, H. R., Atmos. Environ., 27A, 467 (1993).Google Scholar
[5] Civilian Radioactive Waste Management System, Management and Operating Contractor, ANLEBS-MD-000001, Rev. 00 ICN 01, 2000.Google Scholar
[6] Civilian Radioactive Waste Management System, Management and Operating Contractor, TDRWIS-MD-000002, Rev. 00 ICN 02, 2000.Google Scholar
[7] U.S. Department of Energy, DOE/RW-0539, 2000.Google Scholar
[8] Wexler, A. S. and Seinfeld, J. H., Atmos. Environ., 25A, 2731 (1991).Google Scholar
[9] Yang, L., Pabalan, R., and Browning, L., “Experimental determination of the deliquescence relative humidity and conductivity of multicomponent salt mixtures,” (MRS meeting, Boston, MA, 2001).Google Scholar
[10] Greenspan, L., J. Res. Nat. Bur. Stand., 81A, 89 (1977).Google Scholar
[11] Pabalan, R. T. and Pitzer, K. S., Geochim. Cosmochim. Acta, 51, 2429 (1987).Google Scholar
[12] Pabalan, R. T. and Pitzer, K. S., in Activity Coefficients in Electrolyte Solutions, ed. Pitzer, K. S., 2nd ed. (CRC Press, 1991) pp. 435490.Google Scholar
[13] Pabalan, R. T. and Pitzer, K. S., in Proceedings: 1987 Symposium on Chemistry in High-Temperature Water, ed. Izatt, R. M., Oscarson, J. L., and LindH, G. C. (EPRI, 1990) pp. D4f-1–D4f-13.Google Scholar
[14] Pitzer, K. S., J. Phys. Chem., 77, 268 (1973).Google Scholar
[15] Pitzer, K. S., in Activity Coefficients in Electrolyte Solutions, ed. Pitzer, K. S., 2nd ed. (CRC Press, 1991) pp. 75153.Google Scholar
[16] Pabalan, R. T., Software Validation Test Plan for SOLCALC, Version 1.0, Center for Nuclear Waste Regulatory Analyses, San Antonio, Texas, 2001.Google Scholar
[17] Yang, I. C., Rattray, G. W., and Pei, Y., U.S.G.S. Water-Res. Investigations Report 96–4058, 1996.Google Scholar
[18] Yang, I. C., Yu, P., Rattray, G. W., Ferarese, J. S., and Ryan, J. N., U.S.G.S. Water-Res. Investigations Report 98–4132, 1998.Google Scholar
[19] Painter, S., Manepally, C., and Hughson, D. L., Evaluation of U.S. Department of Energy Thermohydrologic Data and Modeling Status Report, Center for Nuclear Waste Regulatory Analyses, San Antonio, Texas, 2001.Google Scholar
[20] Cohen, M. D., Flagan, R. C., and Seinfeld, J. H., J. Phys. Chem., 91, 4563 (1987).Google Scholar
[21] CRC Handbook of Chemistry and Physics, 82 ed. (CRC Press, 2001) pp. 81088.Google Scholar
[22] Wolery, T. J., UCRL-MA-110662 Part III, 1992.Google Scholar
[23] Helgeson, H. C., Kirkham, D. H., and Flowers, G. C., Amer. J. Scim., 281, 1249 (1981).Google Scholar
[24] Bromley, L. A., J. Chem. Thermodyn., 4, 669 (1972).Google Scholar
[25] anderko, A., OLI Systems, Inc. (personal communication).Google Scholar
[26] Browning, L., Murphy, W. M., Leslie, B. W., and Dam, W. L., in Symposium on the Scientific Basis for Nuclear Waste Management XXIII, edited by and, R. Smith Shoesmith, D., (Mater. Res. Soc. Proc. 608, Warrendale, PA, 2000), pp. 237242.Google Scholar
[27] Civilian Radioactive Waste Management System, Management and Operating Contractor, B00000000-01717-5700-00019 Revision 00, 1998.Google Scholar
[28] Rosenberg, N. D., Knauss, K. G., and Dibley, M. J., UCRL-ID-134852, 1999.Google Scholar
[29] Harrar, J. E., Carley, J. F., Isherwood, W. F., and Raber, E., UCID-21867, 1990.Google Scholar
[30] Dunn, D. S., Brossia, C. S., Yang, L., Y.-Pan, M., Sridhar, N., and Cragnolino, G. A., “Localized Corrosion Susceptibility of Alloy 22 as a Waste Package Container Material,” (MRS meeting, Boston, MA, 2001).Google Scholar
lsqb;31] Brossia, C. S., Browning, L., Dunn, D. S., Moghissi, O. C., Pensado, O., and Yang, L. Effect of Environment on Corrosion of Waste Package and Drip Shield Materials, Center for Nuclear Waste Regulatory Analyses, San Antonio, Texas, 2001.Google Scholar