Thermodynamic Properties of Aqueous Aerosols to High Supersaturation: I—Measurements of Water Activity of the System Na+−Cl−−NO−3−SO2−4−H2O at ~ 298.15 K

Chan, Chak Keung; Zheng, Ling; Zheng, Jian; Clegg, Simon L.; Brimblecombe, Peter

doi:10.1080/02786829708965477

Cited by 63 publications

(67 citation statements)

References 26 publications

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“…(NH4)2SO 4 can exist in a ternary solution of higher total I and lower a w than the I and aw limits found in its binary solutions. Similar observations have been reported for other mixtures [Cohen et al, 1987b;Chan et al, 1997].…”

supporting

confidence: 79%

A simple method to derive the water activities of highly supersaturated binary electrolyte solutions from ternary solution data

Chan¹,

Ha²

1999

J. Geophys. Res.

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Abstract. Using mixing rules in electrolyte models for estimating the thermodynamic properties of multicomponent mixtures requires knowledge of data for each binary solution. Very often, a ternary solution in a single-particle levitation experiment can achieve a higher ionic strength as compared with the ionic strengths derived from any of the binary solutions alone. Using water activity data of ternary solutions and the Zdanovskii-Stokes-Robinson and the Kusik and Meissner (KM) equations, water activities of binary solutions of (NH4)2SO4, NaC1, and NH4C1 at supersaturations higher than any previously reported are calculated. With available data from the literature on aqueous supersaturated droplets of NH4NO3-(NH4)2SO 4 ternary solutions and letovicite at ambient temperatures, water activities (>0.32) of (NH4)2SO 4 solutions for ionic strengths up to 112 mol kg -• are obtained. The new water activity relation enables the use of the KM and Pitzer models at higher ionic strengths than in previous research. Applying the same method to the data on (NH4)2SO4-NaC1 and NH4NO3-NaC1 systems yields water activities In single-particle experiments using an electrodynamic balance, laboratory-generated ternary solution droplets can often attain a higher total ionic strength I or lower a w than any of the binary solutions alone before crystallization occurs. For example, Chan et al. [1992] found that an NH4NO3-(NH4)2SO 4 mixture can achieve a maximum attainable ionic strength (/max) and a minimum aw (aw,min) between the limits of the two binary solutions, as demonstrated in Table 1 In this paper, we present a method to calculate the water activities of binary supersaturated solutions from the data of ternary solutions using the ZSR and KM equations. The NH4NO3-(NH4)2SO 4 system is used as an example because its water activity data at different compositions are available and these data are comparable with estimations of the ZSR and KM equations [Chan et al., 1992]. The aim here is to obtain water activities of (NH4)2SO 4 solutions at lower values than any previously reported. Data from the acidic sulfate (H2SO 4-(NH4)2504) system, where applicable, are also included in the analysis. A similar approach is used for calculating the water activities of NaC1 and NH4C1 solutions using data from the literature and newly measured data of ternary solutions con- 30,193

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supporting

confidence: 79%

A simple method to derive the water activities of highly supersaturated binary electrolyte solutions from ternary solution data

Chan¹,

Ha²

1999

J. Geophys. Res.

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“…For several salts water activity data in the supersaturated concentration range exist from single-particle levitation experiments [38][39][40][41]. Such data were used together with isopiestic vapor pressure data at concentrations below saturation in a least squares analysis to determine the interaction parameters at 298.15 K. In the case of NaSO 4 (aq) and NaNO 3 (aq) the available isopiestic data were used directly [42][43][44][45][46][47][48][49][50], while in the case of NaCl(aq) and MgSO 4 (aq) smoothed values of osmotic coefficients are available [51,52], that were used in the least squares treatment.…”

Section: Activity Coefficients and Water Activitymentioning

confidence: 99%

Crystal growth in porous materials—I: The crystallization pressure of large crystals

Steiger

2005

Journal of Crystal Growth

445

270

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“…Comparison between the experimental and calculated water activities along with the corresponding fraction of unoccupied sites are shown in figure 5. The agreement in a w between the BET model and measurements (9,10,22) show excellent agreement from just below saturation (5.591 mol · kg −1 ) to highly supersaturated concentrations. Figure 5 shows that even at fractional unoccupied sites as low as 0.1, the agreement in a w compares very well with experimental data as in the case of (NH 4 ) 2 SO 4 .…”

Section: Application To Supersaturated Solutionsmentioning

confidence: 61%

“…A linear fit of EDB data (9,10,22) between 12.1 mol · kg −1 to 16.7 mol · kg −1 corresponding to 0.5054 > a w > 0.3911 respectively, is given in figure 4 where m · a w /55.5084(1 − a w ) is the ordinate and a w is the abscissa. At the 95 per cent CI, the slope, (c − 1)/c · r and intercept, 1/c · r are (0.2594 ± 0.00574) and (0.0921 ± 0.00825), respectively.…”

Section: Application To Supersaturated Solutionsmentioning

confidence: 99%

“…Experiments on individual particles generated in the laboratory have shown that substantial supersaturation with respect to dissolved salts is possible before a solid phase is precipitated. (9)(10)(11) The resulting concentrated liquid droplets at moderate-to-low relative humidity are chemically stable. Modeling the equilibrium thermodynamics of these aerosols, especially in the supersaturated region, is limited by the capabilities of current models (11) to represent activities and other thermodynamic properties at extreme concentrations where molalities far exceed those at saturation.…”

Section: Introductionmentioning

confidence: 98%

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Activities and osmotic coefficients of tropospheric aerosols: (NH4)2SO4(aq) and NaCl(aq)

Ally

Clegg

Braunstein

et al. 2001

The Journal of Chemical Thermodynamics

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Thermodynamic Properties of Aqueous Aerosols to High Supersaturation: I—Measurements of Water Activity of the System Na⁺−Cl⁻−NO⁻₃−SO²⁻₄−H₂O at ~ 298.15 K

Cited by 63 publications

References 26 publications

A simple method to derive the water activities of highly supersaturated binary electrolyte solutions from ternary solution data

A simple method to derive the water activities of highly supersaturated binary electrolyte solutions from ternary solution data

Crystal growth in porous materials—I: The crystallization pressure of large crystals

Activities and osmotic coefficients of tropospheric aerosols: (NH4)2SO4(aq) and NaCl(aq)

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