Desalination 260 (2010) 114–118

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Desalination
j o u r n a l h o m e p a g e : w w w. e l s ev i e r. c o m / l o c a t e / d e s a l

A simple model for the prediction of CO2 solubility in H2O–NaCl system at geological
sequestration conditions
N.A. Darwish a,⁎, N. Hilal b
a
American University of Sharjah, College of Engineering, Department of Chemical Engineering, Sharjah, P.O. Box 26666, United Arab Emirates
b
The Centre for Clean Water Technologies, School of Engineering, Swansea University, Singleton Park, Swansea SA2 8PP, UK

a r t i c l e i n f o a b s t r a c t

Article history: Carbon dioxide (CO2) released in the atmosphere is the principal cause of the so-called global warming or
Received 16 February 2010 greenhouse phenomenon. One procedure for the mitigation of CO2 consists of the capture, transport and
Received in revised form 11 April 2010 geological storage (sequestration) of the gas in deep saline aquifers. In this work, a model for predicting CO2
Accepted 27 April 2010
solubility in H2O–NaCl system covering conditions typically encountered in geological sequestration (e.g.,
Available online 31 May 2010
300–500 K, 50–2000 bar, and 1–4 mol salt/kg) has been developed and validated by comparison with available
Keywords:
experimental and theoretical data. The model is a simple one with four adjustable parameters that is based on
Setschenov model an extension of the well-known Setschenov model [Kgs / Kg0 = (P / P0)f(Tr,m) with f(Tr,m) = (0.461 + 0.078 m)
Solubility (− 1 + Tr / (1.0 + 0.1267 m)]. The model is developed by exploiting interesting features in the behavior of
Sequestration solubility data of CO2 in saline water over the above-mentioned ranges of conditions. The model is capable of
Salting out predicting CO2 solubility in saline water with accuracy comparable to that made by multi-parameter models
CO2–NaCl–H2O system (having 20 parameters or more). It is also in very good agreement with the available experimental data with
root-mean-squared-error (RMSE) in the range of 0.03–0.225 mol CO2/kg H2O. The extrapolative power of the
model is acceptable at both ends of its range of applicability.
© 2010 Elsevier B.V. All rights reserved.

1. Introduction
The emission of greenhouse gases such as carbon dioxide, which
results from the combustion of fossil fuels, is a major source of
environmental concern in terms of its relation to the global warming
problem [1]. Regardless of the increasing world energy demand and
how well “zero emission” renewable energy is developed, it is
expected that carbon producing fossil fuels will continue to be the
major energy contributor over the coming decades [2]. CO2 released in
the atmosphere, therefore, must be reduced. One procedure towards
this end consists of the capture, transport, and geological storage
(sequestration) of the gas in deep saline aquifers [3]. Because of the
available massive underground capacity, as in depleted oil and gas
reservoirs and deep saline formations, geological sequestration is
anticipated to be an important choice for carbon capture and storage.
A minimum depth of 800 m is recommended to ensure the safe
potable water aquifers [4]. At this depth CO2 will reach supercritical
state (for CO2, the critical temperature (Tc) is 304.2 K, and the critical
pressure (Pc) is 73.8 bar).
It is well known that H2O, CO2 and NaCl are the most common
species in geological fluids [5]. In a recent study by Gilfillan et al. [6]
two mechanisms of CO2 trapping in geological storage sites were
⁎ Corresponding author.
E-mail address: ndarwish@aus.edu (N.A. Darwish).
studied, i.e., CO2 dissolving in formation water and CO2 forming
carbonate mineral precipitates. In view of findings of this study
geological mineral fixation is found to be a minor CO2 trapping
mechanism in natural gas fields. The study suggests that long-term
anthropogenic CO2 storage models in similar geological systems
should focus on the potential mobility of CO2 dissolved in water.
Carbon sequestration, therefore, requires accurate evaluation of the
capacity of a saline aquifer for CO2 addition. Accurate prediction of
CO2 solubility over a wide range of temperature (T), pressure (P) and
ionic strength (m) is also of paramount importance for designing
separation equipment in chemical or oil-related industries [7]. The
precise knowledge of CO2 solubility in pure water is an essential
prerequisite for any modeling activity.
Usually, equations of state (EOS) are used as thermodynamic
models to calculate the phase equilibrium properties of fluid mixtures
[8]. The disadvantage of such models when used for large-scale
storage of CO2 in aquifers is that they involve computational
complexities and are relatively expensive [9]. There is a voluminous
amount of experimental equilibrium data on the CO2-brine systems
that have been used extensively in tuning EOS adjustable parameters.
There has also been extensive theoretical effort on modeling CO2
solubility in aqueous solutions. Although several models on CO2
solubility have been published, few can reliably predict CO2 solubility.
Furthermore, in most cases these are extremely complicated models
that require many adjustable parameters that have no physical
significance. For example, Bahadori et al. presented a model that

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doi:10.1016/j.desal.2010.04.056
 N.A. Darwish, N. Hilal / Desalination 260 (2010) 114–118
requires a total of 48 adjustable parameters to predict the solubility of
CO2 in NaCl–H2O system over only three levels of salt concentration
[10]. This drastically limits the extrapolative and interpolative power
of such models.
For many T–P–m conditions, CO2 solubility values are still
unknown and, in general, predicting these data is not accurate. For
example, Li and Ngheim [11] presented a model to calculate the
solubility of CO2 in pure water of up to 473 K and in NaCl solutions
with up to 4.0 M salt. Another example is presented by Harvey and
Prausnitz [12], who developed an EOS that overestimates CO2
solubility in NaCl aqueous solutions at elevated pressures. Specifically
oriented towards CO2 sequestration purposes, Yuanhui et al., [13]
reviewed and analyzed studies on the relevant phase equilibria and
densities on the system CO2–H2O–NaCl in the temperature and
pressure range for disposal of CO2 in deep saline aquifers and
suggested models in order to obtain more reliable predictions in a
wide temperature and pressure range. In this review three different
models (the electrolyte nonrandom two-liquid (ELEC-NRTL), the
electrolyte NRTL combining with Helgeson model (ENRTL-HG), and
Pitzer activity coefficient model combining with Helgeson model
(PITZ-HG)) are used to calculate the vapor-liquid phase equilibrium of
CO2–H2O and CO2–H2O–NaCI systems. According to this review, more
experimental data and more accurate thermodynamic calculations are
needed in the high temperature and pressure ranges (above 400 K
and 300 bar).
To study the effect of T, P, and salinity (m) on CO2 solubility in brine
solutions, Al-Anezi et al., [14] determined the solubility of CO2 in
different mixtures of aqueous solutions (normal water and different
composition of saline water) at temperature from 298 to 363 K and
pressure from 1 to 2 bar. Zuo and Guo [15] extended Patel-Teja EOS to
phase equilibrium calculations for electrolyte solutions. This model is
reported to be no more accurate than the Harvey–Prausnitz model for
CO2 solubility, where it underestimates CO2 solubility by more than
12% in 20 wt.% NaCl solutions at high pressures (N1000 bar) and
overestimates CO2 solubility by more than 10% in 6 wt.% NaCl solution
at moderate pressures [10]. These models are usually associated with
a large number of tuning parameters and require complex and long
computations. A great amount of work has been performed to
determine the solubility of CO2 in aqueous NaCl solutions based on
the Peng–Robinson EOS, Henry's law and the scaled-particle theory
[8]. Jaiwen Hu et al., [16] presented a comprehensive review of the
experimental PVTx properties and the thermodynamic models of
CO2–H2O and CO2–H2O–NaCl systems. Among other important
conclusions, this review shows that accuracy of the available data
and theoretical models is not sufficient for assessing CO2 sequestra-
tion. Evans and Powell [17] developed a method for activity
calculations in saline, mixed solvent, and supercritical aqueous
solutions. Non-ideal interactions are represented by an activity
coefficient term that combines a limited form of Debye–Huckel and
a van Laar formulation, which is reported to be thermodynamically
valid over a wide range of P, T and fluid composition. The model has
small number of calibration parameters. Conditions modeled include
P, T, m ranges of 200–1400 bar, 773–1173 K, 0–5.56 molality,
respectively. Koschel et al., [18] investigated the solubility of CO2 in
water and in aqueous solution of NaCl by measuring the heat of
mixing of supercritical CO2 (and H2S) with the liquid phase over a
range of 323.1–373.1 K, at pressures of up to 200 bar, and a salt
concentration of up to 3 m. The salting-out effect, as measured by
Setschenov constant, does not strongly vary with the T, P, or m. This
work presents an excellent literature review for the subject. In
particular, it cites many valuable review studies about both
experimental measurements and theoretical modeling for the topic
under consideration.
Diamond and Akinfiev [19] compiled and evaluated experimental
measurements from 25 literature sources of the solubility of CO2 in
pure water at pressures above 10 bar. Data that passed a certain
115
acceptance criterion have been correlated by a thermodynamic model
based on Henry's law and an equation of state. According to this study,
the assumption that the activity coefficients of aqueous CO2 are equal
to unity is found to be valid up to a solubility of approximately 2 mol%.
Portier and Rochelle [20] presented experimental data on the
solubility of CO2 in a mixed salt solution at CO2 sequestration pressure
and temperature conditions. The data were compared with predic-
tions made by a thermodynamic model for CO2 solubility in pure
water and in aqueous NaCl solutions of ionic strengths up to 3 m from
273 to 573 K and from 1 to 300 bar. Sieder and Maurer [21] extended
Peng–Robinson EOS by employing a Debye–Huckel term and a
Margules term to allow for the consideration of salts. The extended
Peng–Robinson equation of state is then used to predict the phase
equilibrium of quaternary systems of the type CO2–H2O–organic
solvent-salt.
Duan and Sun [8] developed a thermodynamic model for the
solubility of carbon dioxide (CO2) in pure water and in aqueous NaCl
solutions for temperatures from 273 to 533 K, pressures from 0 to
2000 bar, and ionic strength from 0 to 4.3 m. The model is based on a
specific particle interaction theory for the liquid phase and a highly
accurate equation of state for the vapor phase. The model is also
claimed to predict CO2 solubility in other systems, such as CO2–H2O–
CaCl2 with an accuracy of about 7%. In the development of their model,
Duan and Sun used an extensive data base on the system CO2–H2O–
NaCl and documented merits and limitations of some important
theoretical models, such as that of Li and Ngheim [11], Harvey and
Prausnitz [12], and the model of Zuo and Guo [15].
In this work we develop and employ a simple, Setschenov-type
model to predict the solubility of CO2 in NaCl–H2O system over
conditions of interest to geological sequestration of carbon dioxide,
i.e., from 300 to 500 K, 50–2000 bar, and 1–4 salt molality. The model
is a simple generalization of Setschenov constant which has only four
adjustable parameters. More importantly, the model is explicit in
solubility and doesn't require iterative algorithms for its use. The
model is developed following careful analysis of CO2 Setschenov
constants over the above-mentioned conditions of temperature,
pressure and salt concentration. Being a generalization of the simple
Setschenov model, which has been proven to be a successful model at
low salt concentrations, the model developed here requires the
availability of CO2 solubility in pure water.
2. The proposed mathematical model
The mathematical model employed in this study is a simple one,
which uses the framework advanced in 1889 by Setschenov [22], i.e.,
!
Cg0
Log = Kgs m ð1Þ
Cgs
where Cg0 stands for the solubility of the gas (CO2) in pure water, Cgs is
the solubility of the gas in saline water, Kgs is the Setschenov constant
in kg/mol and m is the molal concentration (mol/kg) of the salt in the
aqueous phase. Originally, this relation was intended to represent
(salting-out) effects of dissolved salts on gas solubility in water. The
Setschenov relation (Eq. (1)) found good success at low-to-moderate
conditions of temperature (T), pressure (P), and salt concentration
(m), where the constant Kgs becomes constant independent of these
variables. This independence, however, is expected to break down at
the high values of T, P and m encountered in CO2 sequestration. To
investigate this, Fig. 1 is generated using the model developed in this
study for two levels of temperatures (363 and 513 K) and two levels of
salt concentration (1 and 4 m). Shown also in the same figure, are
predictions made by the Duan and Sun model [8] (referred to
hereafter as D–S model). It is quite evident from this figure that a
single value of the Setschenov constant cannot describe gas solubility
116 N.A. Darwish, N. Hilal / Desalination 260 (2010) 114–118
Fig. 1. Effects of temperature, pressure, and salt concentration on Setschenov constant
(Kgs) as predicted by the model in this work and Duan and Sun [8] model.
in saline water over conditions such as those encountered in
sequestration processes. The figure does show, however, that the
dependence of Kgs on T, P, and m is not strong.
The model developed in this study is based on utilizing the same
simple framework of Eq. (1) above by explicitly stating the functional
dependence of Kgs on T, P, and m, i.e., finding Kgs = f(T,P,m). The form
of the mathematical functionality employed here is based on some
interesting features of the solubility data of CO2 in NaCl–H2O system
over the ranges of T, P, and m of 300–500 K, 50–2000 bar, and 1–4 m,
respectively. Analysis of CO2 solubility data in NaCl–H2O system over
the mentioned ranges of T, P, and m, as obtained from D–S model [8]
led to the following observations:
1) For a given value of salt concentration (m), it was found that there
is a unique value of temperature (T0) at which the Setschenov
constant becomes around Kg0 = 0.086, independent of pressure. In
essence, for pressure beyond 100 bar, at temperatures above T0,
Kgs becomes a monotonic increasing function in P, whereas at
temperatures below T0, Kgs becomes a monotonic decreasing
function in P.
2) T0 was also found to correlate nicely with the salt molality
according to this relation:
T0
Tr0 = = 1:0 + 0:1267 × m ð2Þ
Tc
3) Independent of T and m, there is a single value of pressure (P0) that
gives the same value of Kg0 = 0.086, which, for the system under
consideration, occurs around 50 bar.
4) log10(Kgs/Kg0) versus log10(P/P0) goes linearly through the origin
(a zero y-intercept) for all values of T and m, with a slope of −α(θ):
!  
Kgs P T T T error (RMSE) in the gas solubility (defined as the square root of the
log =  αðθÞ × log with θ = 0 = 1  r and Tr = T = Tc;CO2
Kg0 P0 T0 Tr0
ð3Þ
5) α(θ) goes linearly with θ according to the relation:
αðθÞ = βðmÞ × θ with βðmÞ = 0:078 × m + 0:461 ð4Þ
The goodness of fit in all of the above linear relationships is judged
by the value of the squared correlation coefficient (R2), which is found
to be better than 0.98 in all cases.
The working equations for the CO2–NaCl–H2O model of this work,
therefore, become:
!  f ðT ;mÞ
Kgs P r
= ð5Þ
Kg0 P0
 
Tr
f ðTr ; mÞ = ð0:461 + 0:078 × mÞ × −1 1≤m≤4
ð1:0 + 0:1267 × mÞ
ð6Þ
where: Kg0 = 0.086 mol CO2 per kg water, P0 = 50 bar (a constant
specific for the CO2–NaCl–H2O system), Tr is the reduced temperature
based on the critical temperature of CO2 (T / Tc,CO2), and m is the
(molality) concentration of NaCl in the aqueous phase. Eqs. (5) and
(6) are solved with Eq. (1) for the solubility of CO2 in NaCl–H2O
system at any T, P, and m in the reported range. Obviously, the
solubility of CO2 in pure water is needed for the application of this
model. This is also the case with the original Setschenov model, which
assumes the availability of the solubility data of the gas in the pure
solvent. These solubility data are better obtained from accurate
experimentation. However, experimental data are not always avail-
able for all encountered ranges of temperature and pressures. In this
case, recourse to the available reliable models can furnish these
apriori required data. In this work, these solubility data will be those
predicted and reported by Duan and Sun [8]. This validates our
comparison with this latter model, which has 20 adjustable
parameters, and maintains consistency in comparisons with different
experimental data.
3. Results and discussions
In this section we discuss and evaluate the performance of the
proposed model by presenting comparisons of CO2 solubility in NaCl–
H2O brine system predicted by using the model of this work with
experimental data and with predictions made by D–S model [8]. The
D–S model is selected for comparison because it is based on the same
ranges of temperatures, pressures and salt concentrations. It is to be
emphasized here that the model used in this study is a very simple
one, with only four adjustable parameters. Mathematical models used
to predict CO2 solubility in NaCl–H2O system usually involve the
regression of many adjustable parameters. For example, the model
used by D–S [8] involves optimizing 20 adjustable parameters,
whereas that of Bahadori et al., [10] requires the use of 48 adjustable
parameters to cover three levels (m = 1, 2, and 4 m) of salt
concentration.
Fig. 2 shows a comparison of CO2 solubility in aqueous NaCl
solution at 323 and 373 K, pressures of up to 200 bar, and salt
concentration of 1 and 3 m. The experimental data referred to in this
figure are those of Koschel et al. [18] who studied the dissolution of
CO2 in water and in aqueous solution of NaCl by measuring the heat of
mixing of a supercritical CO2 with the liquid phase. It is quite evident
that the model used here is in very good agreement with the
experimental data. The model is seen powerful enough to match the
temperature cross-over shown for the 323 and 373 K isotherms at salt
concentrations of 3 and 1 m, respectively. The root-mean-squared-
arithmetic mean of squared residuals) as predicted by this model over
the indicated range of T, P, and m, is 0.03 mol/kg. A similar comparison
with two sets of experimental data (at 423 and 473 K, with a salt
concentration of 1.09 m) is provided by Fig. 3 [23]. The RMSE in CO2
solubility as predicted by this model over the indicated range of T, P,
and m, is 0.13 mol/kg. Shown also in Fig. 3 are predictions made by the
 N.A. Darwish, N. Hilal / Desalination 260 (2010) 114–118
Fig. 2. Comparison of CO2 solubility in aqueous NaCl solution at 323 and 373 K,
pressures of up to 200 bar and salt concentration of 1 and 3 m.
D–S [8] model, which is based on a specific particle interaction theory for
the liquid phase and an equation of state for the vapor phase. The simple
model of this work is in perfect agreement with the D–S model over the
whole pressure range at 473 and 1.09 salt molality. Both models equally
reproduce the experimental data at 473 K and m = 1.09. For the 423 K
isotherm, the figure shows a perfect match between the two models of
up to a pressure of 1200 bar, after which the model in this work deviates
positively and progressively from the D–S model. Both models also start
overestimating CO2 solubility after a pressure of around 800 bar.
Another comparison of CO2 solubility in aqueous NaCl solution at
523 and 363 K, up to 2000 bar and salt concentration from 1 to 4 m are
displayed in Figs. 4 and 5, respectively. At 523 K, as shown in Fig. 4, the
two models are in excellent agreement with each other of up to a
pressure of 1400 bar over all salt concentrations. After 1400 bar, this
Fig. 3. Comparison of CO2 solubility in 1.09 m aqeuous NaCl solution at 423 K and 473 K
over a pressure range of 50 to 2000 bar.
117
Fig. 4. Comparison of CO2 solubility in aqueous NaCl solution at 523 K, pressures of up
to 2000 bar and salt molality of up to 4 m.
model predicts higher values of CO2 solubility. Both models also are in
excellent agreement with the experimental data of Takenouchi and
Kennedy [23]. The RMSE values of CO2 solubility at 523 K as predicted
by this model for both salt concentrations of 1.0 and the 4.0 M are 0.12
and 0.22 mol/kg, respectively. At 363 K, where there is no experi-
mental data to compare with, Fig. 5 shows excellent agreement
between the two models at salt concentrations of 1 and 2 m over the
whole pressure range of up to 2000 bar. For the 4-m isotherm,
however, the two models start deviating from each other after a
pressure of 200 bar. For pressures of up to 1700 bar, the difference in
the predicted CO2 solubility from the two models lies within ±
0.1 mol/kg. Actually, the trend taken by this 4-m isotherm in Fig. 5 as
predicted by the D–S [8] model looks abnormal as it tends to make an
intersection with the 2-m isotherm predicted by the same model.
Fig. 5. Comparison of CO2 solubility in aqueous NaCl solution at 363 K, pressures of up
to 2000 bar and salt concentration of 1, 2, and 4 m.
118 N.A. Darwish, N. Hilal / Desalination 260 (2010) 114–118

Fig. 6 displays a bar chart comparison among predictions made by

the model of this work, that of D–S [8], and the experimental work of
Gehrig [8,24] at different combinations of high values of T and P (408–
528 K, 887–2717 bar) at a salt concentration of 1.09 m. It is shown
that even outside its intended range of application the simple model
of this work performs well. The agreement is very good between the
two models and the experimental data. It is observed that the factor
having the greatest impact on the model's performance is salt
concentration rather than the temperature and pressure. The
agreement among the two models and the experimental data, as
revealed by Fig. 6, is probably due to the relatively low salt
concentration of m = 1.09 m.
To explore the extrapolative performance of the simple model of
this work outside the lower end of its intended range of applicability,
the behavior of the model over salt concentrations of 1–4 m at a
temperature of 273 K and over a pressure range of 1–10 bar, is shown
in Fig. 7. At higher salt concentration, this model deviates significantly
from that of D–S at 273.15 K. At low salt concentrations, the
agreement between the two models is seen to be very good for the
273 K isotherm. Schumpe [25,26] developed a generalized model for
the effects of different electrolytes, such as NaCl, CaCl2... on the
solubility of many gases, like CO2, CH4... valid over low-to-moderate
ranges of T, P, and salt molality m. The model is based on assuming
ion-specific constants, such as hNa+, hCl−.. and gas-specific constants Fig. 7. Performance of the model in predicting CO2 solubility in NaCl + H2O system over
conditions of temperature and pressure lower than its intended range of applicability
like hCO2, hH2S... For example, for the CO2–NaCl–H2O system, the value
(273.15 K and 1–10 bar).
reported by Schumpe for hCO2 is −0.0183. Using the model of this
work for the same system at 298 K, 1 bar, and a unit salt molality, hCO2
is − 0.016. This shows also another positive sign towards the mental data. The model, however, being an extension of Setschenov
extrapolative feature of the model in this work. However, like any model, requires accurate data on the solubility of CO2 in pure water.
other empirical model, working with this model outside its intended
range should be done only with extreme caution. References

[1] S.H. Schneider, Adv. Ecol. Res. 22 (1992) 1–32.

4. Conclusions
The Setschenov solubility model has been generalized for the
prediction of CO2 solubility in NaCl–H2O system for temperatures
from 300 to 500 K, pressures from 50 to 2000 bar, and salt
concentration from 1 to 4 m. This has been achieved by considering
pressure, temperature, and salt concentration effects on the Setsche-
nov constant (Kgs). It has been shown that Kgs cannot be assumed
constant for conditions such as those encountered in carbon
sequestration. The model has four adjustable parameters and gives
prediction comparable to models with 20 adjustable parameters. Over
its range of application, it shows excellent agreement with experi-
[2] B. Alpern, M.J. Lemos de Sousa, Int. J. Coal Geol. 50 (1–4) (2002) 3–41.
[3] H. Herzog, D. Golomb, in: C.J. Cleveland (Ed.), Encyclopedia of Energy, 2004,
pp. 277–287.
[4] X. Xie, M.J. Economides, J. Nat. Gas Sci. Eng. 1 (2009) 103–111.
[5] E. Roedder, Fluid inclusions, Reviews in Mineralogy, vol. 12, Mineralogical Society
of America, Virginia, 1984.
[6] S.M.V. Gilfillan, B.S. Lollar, G. Holland, D. Blagburn, S. Stevens, M. Schoell, M.
Cassidy, Z. Ding, Z. Zhou, G. Lacrampe-Couloume, C.J. Ballentine, Nature 458
(2009) 614–618.
[7] B. Rumpf, H. Nicolaisen, C. Ocal, G. Maurer, J. Solution Chem. 23 (3) (1994)
431–448.
[8] Z. Duan, R. Sun, Chem. Geol. 193 (2003) 257–271.
[9] H. Hassanzadeh, M.P. Darvish, A.M. Elsharkawy, D.W. Keith, Y. Leonenko, Int. J.
Greenhouse Gas Control 2 (2008) 65–77.
[10] A. Bahadori, H.B. Vuthaluru, S. Mokhatab, Int. J. Greenhouse Gas Control 3 (2009)
474–480.
[11] Y. Li, L.X. Ngheim, Can. J. Chem. Eng. 64 (1986) 486–496.
[12] A.H. Harvey, J.M. Prausnitz, AIChE J. 35 (4) (1989) 635–644.
[13] J. Yuanhui, J. Xiao, F. Xin, L. Chang, L. Linghong, L. Xiaohua, Chin. J. Chem. Eng. 15
(3) (2007) 439–448.
[14] K. Al-Anezi, C. Somerfielda, D. Mee, N. Hilal, Desalination 222 (2008) 548–571.
[15] Y. Zuo, T.M. Guo, Chem. Eng. Sci. 46 (1991) 3251–3258.
[16] J. Hu, Z. Duan, C. Zhu, I.M. Chou, Chem. Geol. 238 (2007) 249–267.
[17] K. Evans, R. Powell, Geochim. Cosmochim. Acta 70 (2006) 5488–5506.
[18] D. Koschel, J.-Y. Coxam, L. Rodier, V. Majer, Fluid Phase Equilib. 247 (2006)
107–120.
[19] L.W. Diamond, N.N. Akinfiev, Fluid Phase Equilib. 208 (2003) 265–290.
[20] S. Portier, C. Rochelle, Chem. Geol. 217 (2005) 187–199.
[21] G. Sieder, G. Maurer, Fluid Phase Equilib. 225 (2004) 85–99.
[22] J.M. Prausnitz, R.N. Lichtenthaler, E.G. de Azevedo, Molecular thermodynamics of
fluid-phase equilibria, 3rd ed.Prentice-Hall Inc., New Jersey, 1999.
[23] S. Takenouchi, G.C. Kennedy, Am. J. Sci. 263 (1965) 445–454.
[24] M. Gehrig, 1980. Phasengleichgewichte und pVT-daten ternarer Mischungen aus
Wasser, Kohlendioxid und Natriumchlorid bis 3 kbar und 550 jC. PhD thesis, Univ.
Karlsrushe, Freiburg.
[25] A. Schumpe, Chem. Eng. Sci. 48 (1993) 153–158.
[26] A. Schumpe, Chem. Eng. Sci. 50 (1995) 1673–1675.

Fig. 6. Performance of the simple model used in this study in predicting CO2 solubility in
1.09 m NaCl–H2O system.