The prediction of mineral solubilities in natural waters: A chemical equilibrium model for the Na-K-Ca-Cl-SO4-H2O system to high concentration from 0 to 250°C

Greenberg, Joshua I.; Møller, Nancy

doi:10.1016/0016-7037(89)90124-5

Cited by 301 publications

(225 citation statements)

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“…Most of these include as a core the model of Greenber and Moller (1989) for the system Na-K-Ca-Cl-SO 4 -H 2 O , which covers the range 0-250 • C. This work also addresses mineral solubilities. The model of Pabalan and Pitzer (1987) for the system Na-K-Ca-Mg-Cl-SO 4 -OH-H 2 O extending to high temperature (˜300 • C in at least some parts) also directly addresses mineral solubilities and is equally notable.…”

Section: Pitzer's Equationsmentioning

confidence: 99%

“…More recent work is likely to be consistent with the above form in the first four terms, although the terms might be in a different order. It is noted that the eight-term form proposed by Greenber and Moller (1989) is overly complex and contains singularities with respect to temperature. When data are encountered in such a form, they should be recast into the more reasonable form given above.…”

Section: Species Combination Interaction Coefficientsmentioning

confidence: 99%

“…When data are encountered in such a form, they should be recast into the more reasonable form given above. This has been done for example for the Greenber and Moller (1989) …”

Section: Species Combination Interaction Coefficientsmentioning

confidence: 99%

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Mathematical Formulation Requirements and Specifications for the Process Models

Steefel¹,

Moulton²,

Pau³

et al. 2010

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Section: Pitzer's Equationsmentioning

confidence: 99%

Section: Species Combination Interaction Coefficientsmentioning

confidence: 99%

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Mathematical Formulation Requirements and Specifications for the Process Models

Steefel¹,

Moulton²,

Pau³

et al. 2010

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“…The parameters in the Yucca Mountain database are derived from a refit of the Moller, 20 and Greenberg and Moller 21 models, but without an explicit temperature dependent CaSO 4 ͑aq͒ ion pair. To examine the ability of the high temperature Pitzer parameters to accurately predict calcium sulfate solubility, we compare model calculations to literature anhydrite and bassanite solubility in solutions of varying sodium chloride concentrations.…”

Section: Ca 2+ and So 4 2−mentioning

confidence: 99%

Evaporative evolution of a Na–Cl–NO[sub 3]–K–Ca–SO[sub 4]–Mg–Si brine at 95 °C: Experiments and modeling relevant to Yucca Mountain, Nevada

Alai

2005

Geochem. Trans.

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A synthetic Topopah Spring Tuff water representative of one type of pore water at Yucca Mountain, NV was evaporated at 95°C in a series of experiments to determine the geochemical controls for brines that may form on, and possibly impact upon the long-term integrity of waste containers and drip shields at the designated high-level, nuclear-waste repository. Solution chemistry, condensed vapor chemistry, and precipitate mineralogy were used to identify important chemical divides and to validate geochemical calculations of evaporating water chemistry using a high temperature Pitzer thermodynamic database. The water evolved toward a complex "sulfate type" brine that contained about 45 mol % Na, 40 mol % Cl, 9 mol % NO 3 , 5 mol % K, and less than 1 mol % each of SO 4 , Ca, Mg, ͚CO 2 ͑aq͒, F, and Si. All measured ions in the condensed vapor phase were below detection limits. The mineral precipitates identified were halite, anhydrite, bassanite, niter, and nitratine. Trends in the solution composition and identification of CaSO 4 solids suggest that fluorite, carbonate, sulfate, and magnesium-silicate precipitation control the aqueous solution composition of sulfate type waters by removing fluoride, calcium, and magnesium during the early stages of evaporation. In most cases, the high temperature Pitzer database, used by EQ3/6 geochemical code, sufficiently predicts water composition and mineral precipitation during evaporation. Predicted solution compositions are generally within a factor of 2 of the experimental values. The model predicts that sepiolite, bassanite, amorphous silica, calcite, halite, and brucite are the solubility controlling mineral phases.

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“…The works of Møller (1988), and Greenberg and Møller (1989) exemplify such efforts by generating empirical functions that fit Pitzer interaction parameters as a function of both ionic strength (I) and temperature. Their approach utilizes a formulation containing eight fitting coefficients to describe the variations in the Pitzer interaction parameter as a function of temperature: where χ represents any parameter of interest within the Pitzer model [Møller (1988) and Greenberg and Møller (1989) used "P" in their notation], and T corresponds to the absolute temperature. a 1 , a 2 , a 3 ,…, a 8 are the coefficients used for fitting the temperature dependence of the parameter.…”

Section: I-32 Temperature Functions For Pitzer Interaction Parametersmentioning

confidence: 99%

In-Drift Precipitates/Salts Model

Mariner¹

2003

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Revision to qualify and document major improvements to the In-Drift Precipitates/Salts model. These improvements include the use of a new software version of EQ3/6 (version 8.0) and a new Pitzer database, which together are designed to predict aqueous chemical reactions in highly concentrated brines. Additional model validation simulations are included for deliquescence points and the evaporation of seawater. Overall model uncertainties are estimated for output parameters used in TSPA-LA. These changes were extensive and required a full revision of the document. OFFICE OF CIVILIAN RADIOACTIVE WASTE MANAGEMENT MODEL REVISION RECORD ACKNOWLEDGMENTSTwo key contributions to this document must be acknowledged. One is the Pitzer thermodynamic database developed and documented in Attachment I. Carlos Jove-Colon with the assistance of Tom Wolery, Joseph Rard, Ananda Wijesinghe, and Russell Jarek developed the Pitzer database and provided the documentation included in Table 3, Table 4, and Attachment I. The other key contribution is the mineral suppression methodology presented in Section 6.6.2.6. This methodology was developed by Darren Jolley with the assistance of Richard Metcalf.The work presented in this document was supported by the Office of Repository Design as part of the Civilian Radioactive Waste Management Program, managed by the U.S. Department of Energy.In-Drift Precipitates/Salts Model Example The scope of this document is to develop, describe, and validate the IDPS model. This model is a quasi-equilibrium model. All reactions proceed to equilibrium except for several suppressed minerals in the thermodynamic database not expected to form under the proposed repository conditions within the modeling timeframe. In this revision, upgrades to the EQ3/6 code (Version 8.0) and Pitzer thermodynamic database improve the applicable range of the model. These new additions allow equilibrium and reaction-path modeling of evaporation to highly concentrated brines for potential water compositions of the system Na-K-H-Mg-Ca-Al-Cl-F-NO 3 -SO 4 -Br-CO 3 -SiO 2 -CO 2 -O 2 -H 2 O at temperatures in the range of 0ºC to 125ºC, pressures in the atmospheric range, and relative humidity in the range of 0 to100 percent. This system applies to oxidizing conditions only, and therefore limits the model to applications involving oxidizing conditions.A number of thermodynamic parameters in the Pitzer database have values that have not been determined or verified for the entire temperature range. In these cases, the known values are used to approximate the values for the rest of the temperature range. Although such treatment contributes to uncertainty in model outputs, the model validation test cases indicate that the model, with its associated uncertainty, is valid for its intended use.The intended use of this model is to estimate and tabulate, within an appropriate level of confidence, the effects of evaporation, deliquescence, and potential environmental conditions on the pH, ionic strength, and chemical compositions of water an...

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The prediction of mineral solubilities in natural waters: A chemical equilibrium model for the Na-K-Ca-Cl-SO4-H2O system to high concentration from 0 to 250°C

Cited by 301 publications

References 27 publications

Mathematical Formulation Requirements and Specifications for the Process Models

Mathematical Formulation Requirements and Specifications for the Process Models

Evaporative evolution of a Na–Cl–NO[sub 3]–K–Ca–SO[sub 4]–Mg–Si brine at 95 °C: Experiments and modeling relevant to Yucca Mountain, Nevada

In-Drift Precipitates/Salts Model

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