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OSMOTIC COEFFICIENTS, SOLUBILITIES, AND DELIQUESCENCE RELATIONS IN MIXED AQUEOUS SALT SOLUTIONS AT ELEVATED TEMPERATURE

Description: While thermodynamic properties of pure aqueous electrolytes are relatively well known at ambient temperature, there are far fewer data for binary systems extending to elevated temperatures and high concentrations. There is no general theoretically sound basis for prediction of the temperature dependence of ionic activities, and consequently temperature extrapolations based on ambient temperature data and empirical equations are uncertain and require empirical verification. Thermodynamic properties of mixed brines in a wide range of concentrations would enhance the understanding and precise modeling of the effects of deliquescence of initially dry solids in humid air in geological environments and in modeling the composition of waters during heating, cooling, evaporation or condensation processes. These conditions are of interest in the analysis of waters on metal surfaces at the proposed radioactive waste repository at Yucca Mountain, Nevada. The results obtained in this project will be useful for modeling the long-term evolution of the chemical environment, and this in turn is useful for the analysis of the corrosion of waste packages. In particular, there are few reliable experimental data available on the relationship between relative humidity and composition that reveals the eutonic points of the mixtures and the mixture deliquescence RH. The deliquescence RH for multicomponent mixtures is lower than that of pure component or binary solutions, but is not easy to predict quantitatively since the solutions are highly nonideal. In this work we used the ORNL low-temperature and high-temperature isopiestic facilities, capable of precise measurements of vapor pressure between ambient temperature and 250 C for determination of not only osmotic coefficients, but also solubilities and deliquescence points of aqueous mixed solutions in a range of temperatures. In addition to standard solutions of CaCl{sub 2}, LiCl, and NaCl used as references, precise direct-pressure measurements were also made at elevated temperatures. The project included multicomponent mixtures ...
Date: February 22, 2006
Creator: Gruszkiewicz, M.S. & Palmer, D.A.
Partner: UNT Libraries Government Documents Department

Measurements of water vapor adsorption on The Geysers rocks

Description: One of the goals of this project is to determine the dependence of the water retention capacity of the rocks as a function of temperature. The results show a significant dependence of the adsorption and desorption isotherms on the grain size of the sample. The increase in the amount of water retained with temperature observed previously between 90 and 30{degrees}C for various reservoir rocks from The Geysers may be due to the contribution of slow chemical adsorption and may be dependent on the time allowed for equilibration. In contrast with the results of Shang, some closed and nearly closed hysteresis loops on the water adsorption/desorption isotherms were obtained in this study. In these cases the effects of activated processes were not present, and no increase in water adsorption with temperature was observed.
Date: April 1, 1996
Creator: Gruszkiewicz, M.S.; Horita, J.; Simonson, J.M. & Mesmer, R.E.
Partner: UNT Libraries Government Documents Department

Water adsorption at high temperature on core samples from The Geysers geothermal field

Description: The quantity of water retained by rock samples taken from three wells located in The Geysers geothermal reservoir, California, was measured at 150, 200, and 250 C as a function of pressure in the range 0.00 {le} p/p{sub 0} {le} 0.98, where p{sub 0} is the saturated water vapor pressure. Both adsorption (increasing pressure) and desorption (decreasing pressure) runs were made in order to investigate the nature and the extent of the hysteresis. Additionally, low temperature gas adsorption analyses were performed on the same rock samples. Nitrogen or krypton adsorption and desorption isotherms at 77 K were used to obtain BET specific surface areas, pore volumes and their distributions with respect to pore sizes. Mercury intrusion porosimetry was also used to obtain similar information extending to very large pores (macropores). A qualitative correlation was found between the surface properties obtained from nitrogen adsorption and the mineralogical and petrological characteristics of the solids. However, there is in general no proportionality between BET specific surface areas and the capacity of the rocks for water adsorption at high temperatures. The results indicate that multilayer adsorption rather than capillary condensation is the dominant water storage mechanism at high temperatures.
Date: June 1, 1998
Creator: Gruszkiewicz, M.S.; Horita, J.; Simonson, J.M. & Mesmer, R.E.
Partner: UNT Libraries Government Documents Department

Water adsorption at high temperature on core samples from The Geysers geothermal field

Description: The quantity of water retained by rock samples taken from three wells located in The Geysers geothermal field, California, was measured at 150, 200, and 250 C as a function of steam pressure in the range 0.00 {le} p/p{sub 0} {le} 0.98, where p{sub 0} is the saturated water vapor pressure. Both adsorption and desorption runs were made in order to investigate the extent of the hysteresis. Additionally, low temperature gas adsorption analyses were made on the same rock samples. Mercury intrusion porosimetry was also used to obtain similar information extending to very large pores (macropores). A qualitative correlation was found between the surface properties obtained from nitrogen adsorption and the mineralogical and petrological characteristics of the solids. However, there was no direct correlation between BET specific surface areas and the capacity of the rocks for water adsorption at high temperatures. The hysteresis decreased significantly at 250 C. The results indicate that multilayer adsorption, rather than capillary condensation, is the dominant water storage mechanism at high temperatures.
Date: June 1, 1998
Creator: Gruszkiewicz, M.S.; Horita, J.; Simonson, J.M. & Mesmer, R.E.
Partner: UNT Libraries Government Documents Department

High temperature water adsorption on The Geysers rocks

Description: In order to measure water retention by geothermal reservoir rocks at the actual reservoir temperature, the ORNL high temperature isopiestic apparatus was adapted for adsorption measurements. The quality of water retained by rock samples taken from three different wells of The Geysers geothermal reservoir was measured at 150{sup degree}C, 200{sup degree}C, and 250{sup degree}C as a function of pressure in the range 0.00 {<=}p/p{sub degree} {<=} 0.98, where p{sub degree} is the saturated water vapor pressure. Both adsorption (increasing pressure) and desorption (decreasing pressure) runs were made in order to investigate the nature and the extent of the hysteresis. Additionally, low temperature gas adsorption analyses were performed on the same rock samples. Nitrogen or krypton adsorption and desorption isotherms at 77 K were used to obtain BET specific surface areas, pore volumes and their distributions with respect to pore sizes. Mercury intrusion porosimetry was also used to obtain similar information extending to very large pores (macropores). A correlation is sought between water adsorption, the surface properties, and the mineralogical and petrological characteristics of the solids.
Date: August 1, 1997
Creator: Gruszkiewicz, M.S.; Horita, J.; Simonson, J.M. & Mesmer, R.E.
Partner: UNT Libraries Government Documents Department

Experimental studies in high temperature aqueous chemistry at Oak Ridge National Laboratory

Description: Experimental research is conducted and models developed in a long- standing program at Oak Ridge on aqueous chemistry at high temperatures of broad classes of electrolytes emphasizing thermodynamics of reaction equilibria and excess thermodynamic properties of electrolytes. Experimental methods, their capabilities, data analysis, and results are summarized. Relevance of the work to problems in power plants, natural and industrial processes as well as basic solution chemistry and geochemistry are given. Progress in potentiometry, electrical conductivity, flow calorimetry, and isopiestic research is described. Future in this field demands greater precision in measurements and significant gains in our understanding of the solvation phenomena especially in the vicinity and beyond the critical point for water. The communities who do research on scattering, spectroscopy, and computer simulations can help guide these efforts through studies at extreme conditions.
Date: January 1, 1996
Creator: Mesmer, R.E.; Palmer, D.A.; Simonson, J.M.; Holmes, H.F.; Ho, P.C.; Wesolowski, D.J. et al.
Partner: UNT Libraries Government Documents Department

The Partitioning of Acetic, Formic, and Phosphoric Acids Between Liquid Water and Steam

Description: The chemical carryover of impurities and treatment chemicals from the boiler to the steam phase, and ultimately to the low-pressure turbine and condenser, can be quantified based on laboratory experiments preformed over ranges of temperature, pH, and composition. The two major assumptions are that thermodynamic equilibrium is maintained and no deposition, adsorption or decomposition occurs. The most recent results on acetic, formic and phosphoric acids are presented with consideration of the effects of hydrolysis and dimerization reactions. Complications arising from thermal decomposition of the organic acids are discussed. The partitioning constants for these acids and other solutes measured in this program have been incorporated into a simple thermodynamic computer code that calculates the effect of chemical and mechanical carryover on the composition of the condensate formed to varying extents in the water/steam cycle.
Date: June 22, 1999
Creator: Gruszkiewicz, M. S.; Marshall, S. L.; Palmer, D. A. & Simonson, J. M.
Partner: UNT Libraries Government Documents Department