Journal of Natural Gas Science and Engineering 26 (2015) 587e594

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Journal of Natural Gas Science and Engineering

journal homepage: www.elsevier.com/locate/jngse

Investigation on the kinetics of methane and carbon dioxide hydrates

by using a modified kinetic model
Shahin Khosharay, Hadi Roosta, Farshad Varaminian*
School of Chemical, Gas and Petroleum Engineering, Semnan University, Semnan, Iran

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

Article history: In this work, the experimental and modeling investigations are conducted on the formation kinetics of
Received 22 March 2015 methane and carbon dioxide hydrates. First, the hydrate formation experiments are done under constant
Received in revised form temperature and volume conditions. The experiments are also conducted at 400, 600 and 800 rpm stirrer
17 June 2015
speeds in the presence of pure water. Subsequently, a kinetic model based on the mass transfer re-
Accepted 18 June 2015
striction of the gas through the liquid film of the gaseliquid interface has been applied for describing the
Available online 9 July 2015
kinetics of hydrate formation. This kinetic model is expressed in terms of the mole fraction of hydrate
former in the gaseliquid interface. Also, in order to determine interfacial mole fraction of hydrate former,
Keywords:
Hydrate formation
the parachor model in terms of interfacial properties is applied. The results of this model have been
Kinetics applied for analyzing the effects of different parameters on kinetics of hydrate formation.
Methane © 2015 Elsevier B.V. All rights reserved.
Carbon dioxide

1. Introduction forces applied for describing hydrate formation kinetics, such

In recent years, clathrate hydrates or gas hydrates have been an
intriguing area of research for industrial applications. These crys-
talline solid structures are inclusion compounds made up of water
molecules and certain guest molecules with suitable sizes under
favorable thermodynamic conditions (elevated pressures and/or
low temperatures). The guest molecules are surrounded by water
cavities formed due to hydrogen bonding between the molecules of
water. The van der Waals forces between the guest molecules and
the cavities of water lead to thermodynamically stable structure of
gas hydrate. The crystallographic structure of gas hydrate mainly
depends on the size of cavities and guest molecules. Structure I (sI),
structure II (sII) and structure H (sH) are the three most common
structures of gas hydrates (Torre' et al., 2012; Mohebbi et al., 2012).
Gas hydrate is capable of being used as an industrial way of
water desalination, cool-energy storage, natural-gas storage, gas
separation, etc (Okutani et al., 2008). It is known that the
successful application of gas hydrate for industrial purposes
mainly depends on the hydrate formation kinetics. On the other
hand, gas hydrate formation is one of the most complex and
stochastic processes; therefore, in order to study this process,
using a kinetic model is of importance. According to the driving
* Corresponding author.
E-mail address: fvaraminian@semnan.ac.ir (F. Varaminian).
as temperature difference (Varaminian, 2000), concentration
difference (Skovborg and Rasmussen, 1994) and fugacity differ-
ence (Englezos et al., 1987), etc, different kinetic models have
been utilized for modeling the hydrate formation kinetics, for
instance, semi-empirical model versus the rate of gas consump-
tion (Vysniauskas and Bishnoi, 1983, 1985), the mass and heat
transfer models of hydrate formation (Varaminian, 2002; Clarke
and Bishnoi, 2005), the kinetic models versus hydrate growth
(Ribeiro and Lage, 2008) and the kinetic models in terms of non
equilibrium thermodynamics such as chemical affinity (Roosta
et al., 2013; Seyfi Mazraeno et al., 2013; ZareNezhad and
Varaminian, 2012; Mottahedin et al., 2011).
Various modeling and experimental efforts have already been
done in order to investigate the kinetics of hydrate formation
process. Monfort et al. (2000) conducted a complete experimental
investigation on the formation kinetics of ethane and propane
hydrates in an agitated and semi-batch cell. Furthermore, they sug-
gested new correlations for evaluating the rate of hydrate crystal
growth. Sun et al. (2003) investigated on the hydrate formation rate
of R12 (CCl2F2) at the temperature of 277.1 K and the pressures of
0.24 MPa and 0.32 MPa in a circulating flow system. By using the
material balance, they developed a mathematical model for gas
consumption, average hydrate particle size and shading ratio. Jerbi
et al. (2010) studied the kinetics of carbon dioxide hydrate forma-
tion and dissociation in semi-batch agitated cell. They concluded that
the hydrate growth rate of CO2 hydrate was approximately

http://dx.doi.org/10.1016/j.jngse.2015.06.043
1875-5100/© 2015 Elsevier B.V. All rights reserved.
588 S. Khosharay et al. / Journal of Natural Gas Science and Engineering 26 (2015) 587e594
1.8
1031% hydrate s1 at the stirring velocity of 450 rpm. This
investigation indicated that for their system, by using an isothermal
circulation loop, the kinetics of hydrate formation varied from
1.8
1031 to 1.8
103% hydrate s1. Tajima et al. (2010) conducted
the experimental and modeling investigation on the HFC 134a
hydrate formation kinetics in a static mixer. They found that the
hydrate formation rate was equal to the mass transfer rate of hydrate
shedding from the gas bubble. Furthermore, they determined the
kinetic constant of hydrate formation. Bergeron et al. (2010)
performed particle size distribution measurements for methane
hydrate formation in formation in a semi-batch stirred cell. They also
applied Bergeron and Servio (2008) model to estimate the reaction
rate constant for methane hydrate formation. Al-Otaibi et al. (2010)
obtained experimental data for the kinetics of pure methane and
ethane hydrates formation in a semi-batch and stirred cell. They also
used the particle size analyzer for their experiments. By using
experimental pressure, temperature, and particle size distribution,
they determine the kinetics of pure methane and ethane hydrates
formation. ZareNezhad and Varaminian (2012) used the chemical
affinity model for hydrate formation rate in the isothermal-isochoric
cell for different gas hydrates containing CH4 (methane), C2H6
(ethane), C3H8 (propane), CO2 (carbon dioxide) R-22 (hydro-
cholorofluorocarbon-22) and Xe (xenone). Mohebbi et al. (2012)
conducted experimental and modeling study on methane hydrate
formation rate in a stirred cell. They also applied a mass transfer
model based on Skovborg and Rasmussen (1994) model.
In this work, the modeling and experimental studies are
conducted on the kinetics of methane and carbon dioxide hydrates
in a stirred cell under constant volume and temperature conditions.
Subsequently, the hydrate formation rate is described in terms of
mass transfer through gaseliquid interface so that the kinetic
model of Skovborg and Rasmussen (1994) is expressed according to
the concentration of hydrate former in the interface phase. In the
model of Skovborg and Rasmussen (1994), the interfacial mole
fraction of hydrate former was set equal to mole fraction (solubility)
of hydrate former in the bulk liquid phase which is not true.
Therefore, to improve the kinetic model of Skovborg and
Rasmussen (1994), the mole fraction of hydrate former in the
interface phase is computed by using the parachor model based on
the work of Tjahjono and Garland (2010) and the interfacial prop-
erties. It should be mentioned that this investigation is just valid
when gas hydrate forms in pure water.
2. Experimental
2.1. Materials
Methane and carbon dioxide are supplied by Technical Gas
Services. These two hydrate formers have purities about 99.99%.
The information of hydrate formers and water used in experiments
has been listed in Table 1.
2.2. Apparatus
In this work, as it is shown in Fig. 1, the kinetic experiments of
hydrate formation were done in the cylindrical and stainless steel cell.
Table 1
Materials used for experiments.
Component Chemical Purity Supplier
formula
Carbon dioxide CO2 99.99% Technical gas services
Methane CH4 99.99% Technical gas services
Water H2O Deionized-distilled Bahrezolal, Iran
The total capacity of the cell was 600 cm3. The hydrate formation cell
had a four-blade mixer. It was also capable of operating in the pres-
sures ranged (0e100) bar and the temperatures ranged
(253.15e373.15) K. The mixture of (water þ ethylene glycol) was used
as a coolant which was circulated by using a circulation pump
through the jacket of the cell. This controllable circulator was utilized
for adjusting the temperature of the high pressure cell with the
accuracy of ±0.1 K. A PT100 thermometer (Pro-Temp Controls, Santa
Ana, California, United States) that had an accuracy of ±0.1 K was used
for measuring the temperature of the high pressure cell. Furthermore,
a BD-Sensors-Str.1 pressure transmitter that had an accuracy of
±0.1 bar was used for measuring the pressure of high pressure cell.
The hydrate formation cell had a data acquisition system.
2.3. Experimental procedure
Prior to conducting any hydrate formation experiment, the high
pressure cell was rinsed with de-ionized water for two times. Then
the high pressure cell was evacuated with a vacuum pump. The high
pressure cell was charged with 300 cc of de-ionized water. Subse-
quently, at each specified temperature, the high pressure cell was
pressurized up to 5 bar under the equilibrium pressure of methane or
carbon dioxide hydrate formation. The constant temperature bath
was turned on. After the high pressure cell reached the constant
specified temperature, the high pressure cell was pressurized up to
the specified pressure. This specified pressure was selected between
the saturation pressure of the hydrate former (gas) and the equilib-
rium pressure of hydrate formation. The initial operational and
equilibrium conditions of hydrate formation are shown in Figs. 2 and
3 for methane and carbon dioxide hydrates, respectively. Then the
stirrer started to work at the specified speed and pressure of high
pressure cell was recorded during the hydrate formation process until
the pressure of high pressure cell reaches to equilibrium pressure of
hydrate formation. Similar to the work of (Li et al., 2009; Mohebbi
et al., 2012; Karimi et al., 2014), based on the pressure drop in the
cell and vapor phase, the amount of hydrate former (gas) consumed
during the formation process was computed by using Eq. (1):



PV PV
nci ¼ no  ni ¼  (1)
ZRT o ZRT i
In Eq. (1), nci is the consumed moles of hydrate former, n0 is the
initial mole of hydrate former, ni is the mole of hydrate former at
any time, P is the pressure, T is the temperature, Z is the
compressibility factor, V is the volume of hydrate former and R is
the universal constant of gases. Subscripts o and i show the initial
condition and the condition at any time, respectively.
In this study, the VTSRK EOS (Lin et al., 2006) was applied for
computing compressibility factor of methane or carbon dioxide. In
the high pressure cell, as it is shown in Eq. (2), the rate of gas
consumption during hydrate formation is considered as the
difference between initial condition of hydrate former and the
condition of the hydrate former at any time.



PV  PV
Dn n0  ni ZRT
0
ZRT
i
¼ ¼ (2)
Dt Dt Dt
In Eq. (2), t is the time.
3. The description of model
3.1. Kinetic model
As it is mentioned in the introduction part, different driving
forces can be considered for hydrate formation process. In this
 S. Khosharay et al. / Journal of Natural Gas Science and Engineering 26 (2015) 587e594
Fig. 1. Experimental hydrate formation apparatus.
Fig. 2. Initial operational and equilibrium conditions of methane hydrate.
study, the modification of Skovborg and Rasmussen (1994) is
applied for modeling the hydrate formation kinetics. Based on the
concentration difference as a driving force, Skovborg and
Rasmussen (1994) proposed a model for kinetics of hydrate for-
mation as follows:
dn
¼ Kcw0 ðxint  xb Þ
dt
In Eq. (3)
K ¼ kL Agl
In Eqs. (3) and (4), Ag1 is gaseliquid interface area, cw0 shows
the initial concentration of water, xint indicates the interfacial liquid
mole fraction of the hydrate former at given pressure and
temperature, xb is bulk liquid mole fraction of the hydrate former at
equilibrium condition of hydrate formation. kL and K are the mass
transfer coefficient and kinetic constants, respectively.
589
Fig. 3. Initial operational and equilibrium conditions of carbon dioxide hydrate.
In fact, Skovborg and Rasmussen (1994) considered the entire
hydrate kinetics as a mass transfer restriction of the hydrate former
through the liquid film of the gaseliquid interface. In previous
modeling investigations, in which the Skovborg and Rasmussen
(1994) model was used, the interfacial liquid mole fraction of the
(3)
hydrate former at given pressure and temperature was set equal to
mole fraction (solubility) of hydrate former in the bulk liquid phase
at given pressure and temperature. Therefore, the following
(4) method (see Fig. 4) was used for calculation of kinetic constant. As
it is shown in Fig. 4, first, according to the operating temperature of
hydrate formation, the equilibrium pressure of hydrate formation
should be calculated. Subsequently, at each operating temperature
and pressure, the solubility of hydrate former in liquid water phase
should be calculated, so the kinetic constant of hydrate formation
can be determined based on experimental pressures and operating
temperature.
590 S. Khosharay et al. / Journal of Natural Gas Science and Engineering 26 (2015) 587e594

Fig. 4. Calculation method for Skovborg and Rasmussen (1994) model.

On the other hand, for (water þ gas) systems, the results of

several investigations (Li et al., 2008; Lafitte et al., 2010; Miqueu Fig. 5. Calculation method for the present model.
et al., 2011; Khosharay et al., 2014; Khosharay and Varaminian,
2014) show the enrichment of gases at the wateregas interface first point contains the operating temperature (T) and pressure (Pi).
which describes the adsorption of gas molecules at the wateregas The second point contains the operating pressure (Pi) and tem-
interface. This proves that the interfacial mole fraction of hydrate perature corresponding to the equilibrium temperature for oper-
former is different from fraction (solubility) of hydrate former in ating pressure (Teq). In fact, the driving force is computed by using
the bulk liquid phase. So, the simplifications of previous model of Eq. (6).
Skovborg and Rasmussen (1994) in which it was assumed that the
eq  
interfacial liquid mole fraction of the hydrate former was set equal Driving force ¼ xint ðT; Pi Þ  xint Teq ; Pi (6)
to mole fraction (solubility) of hydrate former in the bulk liquid
phase is not true. In this investigation, the interfacial mole fraction
of the hydrate former (gas) at given pressure and temperature is
computed based on the experimental surface tensions of 3.2. Parachor model
(water þ gas) system at given pressure and temperature. Therefore,
in this study, by calculating the interfacial mole fraction of hydrate It is known that hydrostatic pressure changes the surface
former on the basis of the surface tension of water/gas system, the tension of (gas þ water) system because of enrichment of the
previous model of Skovborg and Rasmussen (1994) is improved. To interface with the gas molecules. On the other hand, Tjahjono and
achieve this aim, the parachor method based on the work of Garland (2010) proposed a parachor model (Ashrafizadeh and
(Tjahjono and Garland, 2010) is used. In this investigation, the Ameri Ghasrodashti, 2011; Ayirala and Rao, 2004; Ayirala et al.,
method described in Fig. 5 is applied for modeling the kinetics of 2006; Rao and Ayirala, 2006) in terms of surface properties for
hydrate formation. One can see in Fig. 5 that the equilibrium con- calculating the composition of liquid mixtures in the surface phase.
ditions of hydrate formation should be determined. For each In this investigation, the same equation is applied for computing
operating temperature and pressure, according to the surface ten- the composition of surface phase.
sion of water/gas system at each operating temperature and pres- X
1
sure and the applied parachor method, the interfacial mole fraction g4 ¼ rS Psi xSi (7)
of hydrate former can be calculated so that the kinetic constant of i
hydrate formation can be determined based on experimental
In Eq. (7), S shows surface phase, g is the surface tension, Ps is
pressures and operating temperature and the surface tension of
the parachor and r is the mole density.
water/gas system at each operating temperature and pressure. The
suggested model can be expressed as follows:

dn  
eq
¼ Kcw0 xint  xint (5)
dt
In Eq. (5), xint shows the interfacial mole fraction of the hydrate
eq
former (gas) at given pressure and temperature and xint is the
interfacial mole fraction of the hydrate former at equilibrium con-
ditions (equilibrium pressure and temperature) of hydrate forma-
tion. In this study, xint is considered at operating temperature (T)
and pressures between the initial and equilibrium pressure (Peq)
and xeqint
is considered at Pi and the corresponding equilibrium
temperature (Teq) of Pi. These conditions are shown in Fig. 6. It can
be seen in Fig. 6 that for each operating condition, the interfacial
mole fraction of the hydrate former is calculated for two points: The Fig. 6. The hydrate formation conditions and driving force.
 S. Khosharay et al. / Journal of Natural Gas Science and Engineering 26 (2015) 587e594 591

In order to compute the surface composition by using Eq. (7), of model are presented in Table 3 and Figs. 7 and 8. Fig. 7 shows the
the mole density of surface phase (rS ) must be related to the surface consumed mole of carbon dioxide versus time for carbon dioxide
composition (xSi ). One way to achieve this aim is to use an appro- hydrate at 277.15 K, initial pressure of 21.9 bar and 800 rpm stirring
priate equation of state (Eq. (8)). In this work, the CPA EOS is rate and compares the experimental data and the results of the
applied for this aim. All the constants and binary interaction pa- model. Also, the consumed mole of methane versus time for
rameters of CPA EOS are given from the work of Abolala and methane hydrate at 275.15 K, initial pressure of 54.2 bar and
Varaminian (2013). 800 rpm stirring rate is presented in Fig. 8. As it is mentioned in
 n o previous part, in order to apply the present model for the kinetics of
P ¼ f T; rS ; xSi (8) hydrate formation, the interfacial composition of hydrate former is
needed. Table 4 shows a sample of surface tensions of water/
As it is shown in Eq. (9), the sum of the surface mole fractions of methane and water/carbon dioxide for different pressures and
components is also equal to unity. temperatures. A sample of calculation based on parachor model has
been reported in Table 5 for methane/water and carbon dioxide/
xS1 þ xS2 ¼ 1 (9) water systems.
The experimental surface tensions of methane/water and
The required information of this calculation is the parachors of
carbon dioxide/water systems are given from (Jho et al., 1978; Peng
pure components and surface tension of (water þ gas) system. The
et al., 2009) and (Chun and Wilkinson, 1995), respectively. For some
parachors of pure components (see Table 2) are computed based on
pressure and temperatures, no experimental surface tension exists.
the work of Quayle (1953). By using the NewtoneRaphson method,
In order to overcome this problem, the model in the work of
the set of equations (Eqs. (7)e(9)) are simultaneously solved and
Khosharay and Varaminian (2014) has been applied to determine
the surface mole fractions of components are found.
the surface tension. Furthermore, the solubility of methane and
carbon dioxide in water has been calculated by using the flash
4. Results and discussion calculations (Michelsen and Mollerup, 2004). The equilibrium
conditions of methane and carbon dioxide hydrate formation are
In the presence of pure water, the experiments of hydrate for-
mation are conducted at the temperature of 275.15 K for methane
hydrate and two different temperatures of 275.15 K and 277.15 K for
carbon dioxide hydrate. The initial pressure range of methane
hydrate formation is (48.4e58.8) bar. Also, the hydrate formation
experiments for carbon dioxide are conducted at the pressures
ranged (21.9e34.2) bar. Furthermore, these experiments are
conducted at 400, 600 and 800 rpm stirrer speeds. Also, in order to
make sure the experiments were correct and they could be
repeated, each experiment was done for three times. The experi-
mental conditions of the experiments are presented in Table 3.
The pressure and temperature variations of high pressure cell in
terms of time are measured and shown on a computer. The results

Table 2
Parachors of the applied fluids.

Fluid Parachor

Water 54.2
Methane 73.2
Fig. 7. Consumed mole of carbon dioxide versus time for carbon dioxide hydrate at
Carbon dioxide 91.2
277.15 K, initial pressure of 21.9 bar and 800 rpm stirring rate.

Table 3
The operational conditions of hydrate formation experiments and results of kinetic model.

Hydrate former Temperature (K) Initial pressure (bar) Stirrer speed (rpm) K*108

Methane 275.15 48.4 400 0.3345

Methane 275.15 48.4 600 2.753
Methane 275.15 48.4 800 5.678
Methane 275.15 54.2 800 6.356
Methane 275.15 58.8 800 7.835
Carbon dioxide 275.15 21.9 400 9.4604
Carbon dioxide 275.15 21.9 600 30.306
Carbon dioxide 275.15 21.9 800 43.662
Carbon dioxide 275.15 24.0 800 44.386
Carbon dioxide 275.15 28.2 800 46.861
Carbon dioxide 275.15 33.0 800 48.581
Carbon dioxide 277.15 25.8 400 3.602
Carbon dioxide 277.15 25.8 600 15.089
Carbon dioxide 277.15 25.8 800 20.879
Carbon dioxide 277.15 28.0 800 23.454
Carbon dioxide 277.15 31.3 800 24.234
Carbon dioxide 277.15 34.2 800 25.992
592 S. Khosharay et al. / Journal of Natural Gas Science and Engineering 26 (2015) 587e594

phase and interface are different. As it has been mentioned in

Fig. 8. Consumed mole of methane versus time for methane hydrate at 275.15 K, initial
pressure of 54.2 bar and 800 rpm stirring rate.
given from (Nakamura et al., 2003; Vlahakis et al., 1972). Although
the experimental surface compositions are not available in litera-
ture, one can see in Table 5 that the mole fractions of hydrate
formers (methane and carbon dioxide) in gaseliquid interface are
greater than their mole fraction in the bulk liquid phase. These
results show the hydrate formers (methane and carbon dioxide) are
preferentially adsorbed in the interface so that the compositions of
hydrate formers (methane and carbon dioxide) in the bulk liquid
previous part, for (water/gas) systems, the results of gradient the-
ory in several investigations (Li et al., 2008; Lafitte et al., 2010;
Miqueu et al., 2011; Khosharay et al., 2014; Khosharay and
Varaminian, 2014) prove the enrichment of gases at the water-
egas interface which confirms the results of the present model.
The results of model in Table 3 show that kinetic constants of
carbon dioxide hydrate is greater than the ones for methane hy-
drate; therefore, carbon dioxide hydrate shows higher formation
rate than the methane hydrate. The higher formation rate for
carbon dioxide hydrate could be attributed to the lower surface
tensions of carbon dioxide/water system (see Table 4). When the
surface tension value is lower, the interaction among water mole-
cules in gaseliquid interface is weaker and subsequently the
gas-uptake rate is higher (the mass transfer resistance in
gaseliquid interface is lower). On the other hand, as it is seen in
Table 5, the interfacial mole fractions of carbon dioxide are higher
than methane. The higher mole fraction of carbon dioxide in the
interface leads to higher driving force of hydrate formation so that
the carbon dioxide hydrate forms at higher rates. Also, the results of
modeling shows that increase in initial pressure leads to higher
hydrate formation rate for both methane and carbon dioxide
hydrates. At the pressures and temperatures applied this study and
constant temperature, as it is shown in Table 4, the surface tension
of water/gas systems decreases if the pressure increases. So, the
interaction of interfacial water molecules is weaker and absorption
of the gas in the interface is higher. Therefore, according to these
explanations, the gas uptake rate, driving force and subsequently

Table 4
Sample of surface tensions of water/methane and water/carbon dioxide for different pressures and temperatures.

System Operating Operating Corresponding equilibrium Surface tension at Surface tension at equilibrium
temperature (K) pressure (bar) temperature (K) operating condition (mN/m) condition (mN/m)

Methane 275.15 58.8 281.24 65.66 65.26

Methane 275.15 53.1 280.24 67.99 67.55
Methane 275.15 47.9 279.23 69.00 68.96
Methane 275.15 43.3 278.24 70.05 69.95
Methane 275.15 35.5 276.22 71.32 71.25
Methane 275.15 32.2 275.25 72.36 72.36
Carbon dioxide 275.15 21.9 278.2 59.34 60.67
Carbon dioxide 275.15 21.37 277.8 60.04 60.75
Carbon dioxide 275.15 21.03 277.6 60.95 61.88
Carbon dioxide 275.15 19.51 277.2 61.34 62.05
Carbon dioxide 275.15 18.48 276.5 62.67 63.45
Carbon dioxide 275.15 17.17 276.2 63.44 64.08
Carbon dioxide 275.15 16.13 275.4 64.33 65.00
Carbon dioxide 275.15 15.1 275 65.51 66.39

Table 5
Sample of required calculations for the kinetic model.

Hydrate former Operating Operating Corresponding x in bulk liquid x in bulk liquid xint at operating xint at Deriving
temperature (K) pressure (bar) equilibrium at operating at equilibrium condition equilibrium force
temperature condition condition condition

Methane 275.15 58.8 281.24 0.00371 0.00310 0.0913 0.0868 0.0045

Methane 275.15 53.1 280.24 0.00344 0.00293 0.0805 0.0763 0.0042
Methane 275.15 47.9 279.23 0.00313 0.00277 0.0759 0.072 0.0039
Methane 275.15 43.3 278.24 0.00288 0.00262 0.0711 0.0682 0.0029
Methane 275.15 35.5 276.22 0.00243 0.00235 0.0654 0.0647 0.0007
Methane 275.15 32.2 275.25 0.00223 0.00223 0.0609 0.0609 0
Carbon dioxide 275.15 21.9 278.2 0.0195 0.0180 0.3175 0.29 0.0275
Carbon dioxide 275.15 21.37 277.8 0.0191 0.0178 0.3086 0.2904 0.0182
Carbon dioxide 275.15 21.03 277.6 0.0189 0.0176 0.2973 0.2797 0.0176
Carbon dioxide 275.15 19.51 277.2 0.0175 0.0166 0.2922 0.2763 0.0159
Carbon dioxide 275.15 18.48 276.5 0.0167 0.0161 0.2757 0.2617 0.014
Carbon dioxide 275.15 17.17 276.2 0.0155 0.0151 0.2662 0.2549 0.0113
Carbon dioxide 275.15 16.13 275.4 0.0146 0.0145 0.2553 0.2466 0.0087
Carbon dioxide 275.15 15.1 275 0.0137 0.0137 0.2412 0.2412 0
 S. Khosharay et al. / Journal of Natural Gas Science and Engineering 26 (2015) 587e594 593

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Company. The authors would like to owe great thanks to the Lafitte, T., Mendiboure, B., Pineiro, M.M., Bessieres, D., Miqueu, C., 2010. Interfacial
properties of water/CO2: a comprehensive description through a gradient
Semnan Gas Province Company for financial support of this
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