Fluid Phase Equilibria 388 (2015) 182187

Contents lists available at ScienceDirect

Fluid Phase Equilibria

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

A thermodynamic consistency test for experimental isobaric data of

wax solubility in gaseous systems
Javad Kondori a , Hamed Hashemi b , Saeedeh Babaee b , Jafar Javanmardi a ,
Amir H. Mohammadi b,c, * , Deresh Ramjugernath b, **
a

Department of Chemical Engineering, Shiraz University of Technology, Shiraz, Iran

Thermodynamics Research Unit, School of Engineering, University of KwaZulu-Natal, Howard College Campus, King George V, Avenue, Durban 4041, South
Africa
c
Institut de Recherche en GnieChimiqueetPtrolier (IRGCP), Paris Cedex, France
b

A R T I C L E I N F O

A B S T R A C T

Article history:
Received 3 May 2014
Received in revised form 27 December 2014
Accepted 31 December 2014
Available online 3 January 2015

The ever-increasing demand for natural gas as an energy source has led to a great deal of interest and
numerous studies being undertaken by researchers in the eld. The efcient production of natural gas
from deep well reservoirs has always been an area of intense research in the gas production industry,
with immense efforts to understand and mitigate issues which can affect this efciency. The solubility of
the waxy compounds in some natural gases can be regarded as one of these issues that may affect
production efciency. In order to fully understand the phenomenon of wax solubility in natural gas,
reliable experimental data are required. This study aims to investigate the reliability of such data using a
thermodynamic model. For this purpose, the wax solubility in supercritical constituents of natural gas,
such as carbon dioxide and ethane, has been estimated using the PengRobinson equation of state and
two-uid van der Waals (vdW2) mixing rules. The residual enthalpies were evaluated using the results
obtained. The GibbsDuhem equation at constant pressure was applied for evaluation of the consistency
of the experimental data. From the analysis, the data were classied as thermodynamically consistent
(TC), not fully consistent (NFC), and thermodynamically inconsistent (TI).
2015 Elsevier B.V. All rights reserved.

Keywords:
Thermodynamic consistency test
Wax solubility
Isobaric experimental data
GibbsDuhem
Supercritical uids

1. Introduction
Natural gas, until the middle of the 20th century, was dismissed
as an impractical by-product of crude oil production. This has
changed signicantly with natural gas now accounting for
approximately 22% of the worlds energy consumption, with the
percentage likely to increase with every larger reserves being
discovered. It has been predicted by the International Energy
Agency that the demand for the natural gas will increase nearly
43% by 2035. Natural gas is regarded as the cleanest and most
economical conventional fuel compared to hydrocarbon fuels such
as oil and coal which produce high levels of greenhouse emissions.
The temperature depression in petroleum pipelines conveying
waxy crudes may result in the formation of solid compounds

* Corresponding author at: Institut de Recherche en GnieChimiqueetPtrolier

(IRGCP), Paris Cedex, France.
** Corresponding author.
E-mail addresses: a.h.m@irgcp.fr, amir_h_mohammadi@yahoo.com
(A.H. Mohammadi), ramjuger@ukzn.ac.za (D. Ramjugernath).
http://dx.doi.org/10.1016/j.uid.2014.12.048
0378-3812/ 2015 Elsevier B.V. All rights reserved.

which are comprised mainly of parafn hydrocarbons (C18C36),

known as parafn wax and naphthenic hydrocarbons (C30C60).
The presence of such compounds may be expected in some natural
gas production elds [1,2]. The extraction of these compounds by
supercritical constituents of natural gas, such as carbon dioxide
and ethane, in gas production from deep well or acid gas elds may
have catastrophic repercussions [1,2]. Therefore, the measurement
of solubility of such compounds in supercritical uids is an
important area of research [2]. Hence, before design of the related
facilities for natural gas production from gas reservoirs, the
solubility of waxes should be taken into account to avoid any
possible failure in the system (lost production, or failure of piping
system) [2]. For this purpose the knowledge of natural gas + wax
phase behavior is inevitable [2]. Accordingly, developing a reliable
model for predicting this phase behavior is necessary [2].
Unfortunately, there are a scarcity of experimental data in the
open literature which have considered this phenomenon [2]. The
reliability of the model depends on the accuracy of the
experimental data which are employed for the tting of model
parameters. The use of inaccurate or incorrect measured experimental data would result in parameters which produce a model

J. Kondori et al. / Fluid Phase Equilibria 388 (2015) 182187

Nomenclature
A
ARD
d
E
EoS
k
f
G
H
l
NDP
P
PR
R
T
TC
V
vdW2
y
Z

Area (m2)
Absolute relative deviation
Derivative operator
Error
Equation of state
Binary interaction parameter
Fugacity
Gibbs energy
Molar enthalpy
Binary interaction parameter
Number of experimental data points
Pressure (MPa)
PengRobinson
Universal gas constant (MPa m3/mol
Temperature (K)
Thermodynamically consistent data
Molar volume (m3/mol)
van der Waals 2 uid mixing rule
Mole fraction in gas phase
Compressibility factor

Greek symbols
f Fugacity coefcient
D Difference value
v Acentric factor

In this study, the consistency of isobaric wax solubility

experimental data in carbon dioxide and ethane have been
thermodynamically evaluated. The GibbsDuhem [3,6,7] equation,
in terms of residual molar enthalpy and molar volume, has been
applied for this purpose. The thermodynamic consistency, partial
consistency (not fully consistent), and thermodynamic inconsistency of data have been determined.
2. Thermodynamic consistency test
The GibbsDuhem [3,6,7] relation can be written in terms of
residual molar enthalpy (HR) and residual molar volume (VR) for a
homogeneous mixture as follows [6,14]:
" #
GR
HR
VR
S yi d i 2 dT dP
(1)
RT
RT
i
RT
where yi stands for the mole fraction of species i in the mixture, GRi
is the residual Gibbs energy, R represents the universal gas
constant, and P and T are the pressure and temperature of the
system, respectively. Residual Gibbs energy GRi can be expressed
by the following equation [57]:
GRi RTlni

(2)

in which fi represents the fugacity coefcient of component i in

the mixture. Substitution of Eq. (2) into Eq. (1) gives:

S yi dlni 

HR

Subscripts
A Area
c Critical property
i ith component in a mixture or ith experimental data set
j jth component in a mixture or jth individual calculated
area
T Refers to experimental PTy data
f Refers to calculated parameters of the model for evaluations of the integrals in Eqs. (8)(10)
1 Refers to supercritical CO2 or ethane
2 Refers to parafn wax
Superscripts
cal Calculated
exp Experimental
s
Solid
R
Residual property
sat Saturation (sublimation) pressure (MPa)

which is inaccurate or incorrect. Analyzing the reliability of

experimental data has become an area of interest for many
researchers.
The Slope Test, the Integral Test, the Differential Test and
the Tangent-Intercept Test are among the well-known
approaches which have been developed so date for evaluating
the consistency of experimental data [38]. Comprehensive
reviews of these methods can be found in literature [4,5].
Valderrama can be regarded one as the pioneers of thermodynamic consistency testing of experimental data [813]. The Gibbs
Duhem [3,6,7] equation has been adopted by Valderrama for this
purpose at constant temperature. In a previous study, a new
approach for assessing the water content of methane experimental
data at constant pressures was developed [14]. Hence depending
on experimental data being considered, and whether the data are
at constant pressure or temperature, either the constant pressure
or constant temperature approach can be employed.

183

RT

dT

VR
dP
RT

(3)

For the case of study (wax solubility in the gaseous system) only
R

two components are involved and Eq. (3) considering h HR =RT

can be simplied as follows [3,6,7]:
" #
R
h
(4)
dT y1 dln1 y2 dln2

T
where y1 and y2 are the mole fraction of supercritical uid and
solute (wax) in the gas phase, respectively and f1, f2 represent the
fugacity coefcients of the components in the gas phase. The
following equation is used for evaluation of hR:
R

ZV

h T

@Z dV
Z  1

@T V

(5)

where Z indicates the compressibility factor of the gas phase, and T

and V are temperature and molar volume of the system,
respectively. A mathematical re-arrangement of Eq. (4) in terms
of the wax composition in the gas phase (y2 = 1  y1) gives:
Z
Z
Z
1
1
1  y2
dT
d

d1
(6)
2
R
R
Ty2
h 2
h y2 1
in which the parameters, hR, f1, f2, and Z can be calculated using an
accurate thermodynamic model for the waxgas equilibria.
Further simplications can also be made by designating the left
and right hand sides of Eq. (6) by AT and Af, respectively, as follows
[8,14]:
Z
1
dT
(7)
AT
Ty2
A A1 A2
where
Z
A1

1  y2
h y2 1
R

(8)

d1

(9)

184

J. Kondori et al. / Fluid Phase Equilibria 388 (2015) 182187

Is ARD% within [0-25]%?

No

Table 2
Sublimation pressures of the investigated parafn waxes at different temperatures
[2].

Change the correlang model

Yes
Are all A% in the range of [0-18]%?

Yes

The data are thermodynamically

consistent

Compound

T/K

Sublimation pressure/MPa

n-C25H52

308
313

1.58  1011
5.39  1011

n-C28H58

308
318
325

1.71 1013
2.67  1012
1.68  1011

n-C30H62

308
313

1.50  1014
6.46  1014

n-C32H66

308
313
318
319

1.02  1015
4.74  1015
2.12  1014
2.86  1014

n-C33H68

308
313
318

1.15  1015
5.43  1015
2.44  1014

No
Are the data outside the range of [018]% greater than 25% of the whole
dataset?

NO

The data are Not Fully Consistent

(NFC)

Yes
The data are Thermodynamically
Inconsistent (TI)

Fig. 1. Flowchart diagram of the thermodynamic consistency test used in this study
[8].

Z
A2

1
h 2
R

d2

(10)

In this study, the Simpson 3/8 integration method was used for
determination of AT and Af. The equivalency of AT and Af within an
acceptable deviation will determine the consistency of the dataset
considered. This deviation is dened using a percent area deviation
between experimental and calculated values [1,14]:


jA  AT i j
DAi 100 i
(11)
AT i
where i indicates the number of the dataset. The error propagation
method [15] has been used for the evaluation of the boundaries for
these deviations at constant pressure. Considering mole fraction of
wax in the gas phase as the independent measured variable and Af
as the dependent measured variable, the error in the calculated
areas, EA, and the percent error, %EA can be obtained using
following equations [16,17]:




@ A
@A
EA
DP
Dy
(12)
@P
@y

%EA 100j

EA
j
A j

(13)

where subscript j indicates the jth calculated area. In this study, a

maximum uncertainty of 0.1 MPa for the experimental pressure

and 5% for experimental solubility data of wax in carbon dioxide

and ethane are assumed. It should be noted that these
uncertainties are dependent on the experimental measurement
methods, for example the method which was used by Teja et al.
was based on dynamic method [2]. The relative average absolute
deviations range between [018]% for the solubility data of the
investigated waxes in supercritical carbon dioxide and ethane was
obtained applying the central nite difference method [18] in two
preceding equations. This range has been considered as the
maximum acceptable error for areas (DAi) in Eq. (11). A owchart
for the procedure used for the checking of the thermodynamic
consistency of the investigated dataset is shown in Fig. 1.
3. Thermodynamic model
In this study, the equality of the fugacities of solutes (wax) in
adjacent phases (pure solid and gas phase) has been used as the
equilibrium criteria [1,2]:
solid

fi

gas

fi

(14)

where f stands for the fugacity of component i in the mixture. In

this study, the following assumptions have been made for the
modeling of the waxgas system [1,2]:
1 The supercritical uid is not soluble in the solid (solute-

containing) phase.
2 The fugacity of the pure solid i represents the fugacity of the

solute i in the mixture.

Table 1
Experimental datasets used for the consistency test in this study.
System
CO2 + nC25H52
CO2 + nC28H58
CO2 + nC28H58
Ethane + nC30H62
Ethane + nC32H66
Ethane + nC33H68
a
b

NDPa P range/
MPa
4

10.3520.5

20

11

T range/K

y2  106 range/mole
fractionb

3 The pressure dependency of the solute molar volume has been

Ref.

308313

215952

308318

435689

308.15318.15 54.676

21

6.5713.64

308.1313.1

4861710

16

6.5720.2

308.1319.1

1492180

16

6.4720.2

308.1318.1

1832970

Number of data points.

Wax solubility.

neglected.
4 The solid phase is incompressible.
5 The saturated fugacity coefcient of the solute is assumed to be

unity.

Table 3
Solid molar volumes (Vs) of the parafn waxes [2] investigated.
Solute

vs  103/m3/mol

n-C25H52
n-C28H58
n-C30H62
n-C32H66
n-C33H68

0.4513
0.4894
0.5222
0.555
0.5714

J. Kondori et al. / Fluid Phase Equilibria 388 (2015) 182187

Table 4
Acentric factors (v) and critical properties (Tc: critical temperature and Pc: critical
pressure) of the pure compounds investigated.
Compound

Tc/K

Pc/MPa

C2H6
CO2
n-C25H52
n-C28H58
n-C30H62
n-C32H66
n-C33H68

305.32
304.19
818.56
842.11
856.17
869.12
875.22

4.872
7.382
1.0256
0.9694
0.9421
0.9208
0.9119

0.099
0.2276
1.066
1.163
1.226
1.287
1.317

Considering the preceding assumptions and using Eq. (14), the

following equation will be obtained for calculation of the solid
solubility in the supercritical uid:

yi

s
Psat
i expvi P

i P

185

Psat
i =RT

(15)

Th PengRobinson equation of state [19] and the two-uid van

der Waals (vdW2) [20] mixing rules have been used for calculation
of the solid, solutes, and supercritical uids fugacity coefcients
(fi) in the mixture and also other required parameters. More
details in this regard are given elsewhere [1].
4. Consistency criteria
The accuracy of the model used for correlation / representation
of the experimental data is crucial in the thermodynamic
consistency test. In other words, the average absolute deviations
between the model predictions and the experimental data should
be within the acceptable margin of errors. In this study, the range

Table 5
Model predictions for the parafn waxes (2) solubility in CO2 and ethane (1).
 106
yexp
2

System

P/Mpa

T/K

CO2 + n-C25H52

10.35

308.00
313.00
308.00
313.00

215
321
602
952

308.00
318.00
308.15
318.15

689
435
54.6
76

20.50

CO2 + n-C28H58

20.00
11.00

Ethane + n-C32H66

6.57

10.10

12.02

13.64

16.67
20.20

Ethane + n-C33H68

6.47

10.20

12.12

13.64

16.67
20.20

Ethane + n-C30H62

6.57
10.10
12.02
13.64

a
b

kijb

lijb

6
ycal
2  10

ARD%

236.2
324.0
663.0
1043.0

9.90
1.00
10.20
9.60

0.194

751.1
439.5
82.3
69.3

8.90
1.00
50.73a
8.82

0.035

0.32

[2]
[2]
[21]
[21]

0.057

0.19

[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]

0.418

[2]
[2]
[2]
[2]

308.10
313.10
319.10
308.10
313.10
319.10
308.10
313.10
319.10
308.10
313.10
319.10
308.10
313.10
308.10
313.10

216
177
149
713
933
1280
801
1150
1440
959
1440
2140
1260
1730
1810
2180

258.4
208.9
196.8
855.6
1110.1
1675.1
962.9
1370.8
1889.3
1140.5
1709.7
2818.0
1527.1
2062.2
2184.7
2581.1

19.70
18.00
32.10a
20.00
19.00
30.90a
20.20
19.20
31.20a
18.90
18.70
31.70a
21.20
19.20
20.70
18.40

308.10
313.10
318.10
308.10
313.10
318.10
308.10
313.10
318.10
308.10
313.10
318.10
308.10
313.10
308.10
313.10

371
288
183
963
1540
1540
1140
1470
1960
1360
1720
2970
1640
2240
2370
2930

441.4
344.4
239.2
1155.6
1844.9
2005.1
1359.7
1754.9
2565.6
1627.1
2062.1
3890.7
1966.9
2658.2
2846.4
3508.4

18.98
19.58
30.71a
20.00
19.80
30.20a
19.27
19.38
30.90a
19.64
19.89
31.00a
19.93
18.67
20.10
19.74

0.35

0.151

[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]
[2]

308.10
313.10
308.10
313.10
308.10
313.10
308.10
313.10

549
486
1240
1450
1450
1450
1710
1710

667.0
610.8
1483.7
1801.0
1744.1
1832.8
2066.4
2171.4

21.49
25.68a
19.65
24.21
20.28
26.40a
20.80
27.00a

0.06

0.06

[2]
[2]
[2]

Data out of model predictions criteria (doutful data).

Interaction parameters between the ith and jth compounds in the mixture, which are consistent with those reported in Ref. [2].

[2]
[2]
[2]
[2]

186

J. Kondori et al. / Fluid Phase Equilibria 388 (2015) 182187

of [025]% has been chosen as the acceptable range for the absolute
relative deviations (ARD) of the model predictions which is dened
as follows:
ARD% 100 

exp
jycal
j
i  yi

Not fully consistent (NFC) experimental datasets are dened as

data which are predicted by the model correctly, however less
than 25% of the data are outside the dened margin of errors, i.e.
[018]%.

(16)

yexp
i

Fig. 1 shows the procedure schematically [8].

where superscripts cal and exp stand for calculated and

experimental values, respectively.
According to what has been discussed so far, the following
procedure has been adopted for determination of thermodynamically consistent (TC), thermodynamically inconsistent (TI), and not
fully consistent (NFC) determination of experimental data:
1 Initially, the ARD% of the model should lie between 0 and 25%,

otherwise the poor prediction should be eliminated and the

correlating model changed. In these cases, the related experimental data are regarded as doubtful data and they are not used
in the test.
2 A dataset is deemed to be thermodynamically consistent (TC) if
the model provides acceptable error ranges (ARD%) and the area
test is met for all data points in the dataset.
3 Thermodynamically inconsistent (TI) experimental datasets are
dened as the datasets in which that the area test is not fullled
for most of the data (more than 25% of the areas) even though
the thermodynamic model correlates the experimental data
correctly (with ARD% between 0 and 25%).
4

5. Experimental data
48 isobaric experimental datasets were considered in this
study, most of which were taken from GPA research report 171 [2],
and are summarized in Table 1. These datasets include solubility of
parafn waxes (alkanes from n-C24 to n-C33) in CO2 and ethane.
Tables 2 and 3, show the sublimation pressures and solid molar
volumes of the parafn waxes, respectively. Acentric factors and
critical properties of the investigated compounds are reported in
Table 4.
6. Result and discussion
The consistency check procedure adopted in this study can be
divided in two parts: rst obtaining the thermodynamic model
predictions of the wax solubility data, and second evaluating the
experimental data using the obtained results. The results obtained
from the model for the prediction of the parafn wax solubility in
supercritical CO2 and ethane, as well as adjusted interaction
parameters of the model are reported in Table 5. As can been seen,

Table 6
Results of the thermodynamic consistency test for the experimental parafn waxes (2) solubility data in supercritical uids (1).
System

P/MPa

T/K

f1

f2

HR

AT

Af

DAi%

Test result

CO2 + n-C25H52

10.35

308
313
308
313

0.264
0.292
0.401
0.417

0.5210
0.5527
0.3310
0.3493

1.210  106
3.650  106
1.010  106
2.810  106

3.465
3.126
4.006
3.779

69.788

62.635

10.2

TC

21.873

19.036

14.9

TC

308
318

0.397
0.420

0.3337
0.3770

0.050  106
0.087  106

3.976
3.564

59.707

60.852

1.88

TC

308.1
313.1
308.1
313.1
308.1
313.1
308.1
313.1
308.1
313.1
308.1
313.1

0.254
0.285
0.326
0.343
0.378
0.386
0.415
0.422
0.484
0.491
0.5652
0.5695

0.5282
0.5610
0.3880
0.4165
0.3503
0.3728
0.3244
0.3456
0.2900
0.3095
0.2646
0.2824

0.037  106
0.085  106
0.029  106
0.044  106
0.032  106
0.049  106
0.040  106
0.059  106
0.094  106
0.093  106
0.040  106
0.059  106

3.496
3.167
3.883
3.942
3.907
3.736
3.959
3.803
4.0324
3.8809
4.0794
3.9376

42.077

46.598

9.70

TC

12.236

14.308

14.47

TC

17.073

17.393

1.83

TC

14.000

14.269

1.84

TC

11.055

11.336

2.48

TC

1.61

TC

308.1
313.1

0.333
0.343

0.3919
0.4164

0.416  107
0.631 107

3.832
3.644

12.05

12.27

1.82

TC

308.1
313.1
308.1
313.1
308.1
313.1
308.1
313.1
308.1
313.1
308.1
313.1

0.251
0.279
0.328
0.337
0.372
0.379
0.407
0.413
0.475
0.482
0.555
0.561

0.5343
0.5630
0.3861
0.4101
0.3450
0.3670
0.3211
0.3418
0.2860
0.3057
0.2610
0.2784

1.56  1012
0.127  1012
0.244  1012
0.65  1012
0.196  1012
0.485  1012
0.186  1012
0.435  1012
0.206  1012
0.446  1012
0.283  1012
0.585  1012

3.496
3.139
3.901
3.728
3.988
3.823
4.039
3.883
4.111
3.960
4.168
4.022

49.596

46.955

5.62

TC

13.611

12.890

5.58

TC

12.550

12.648

0.15

TC

10.609

10.625

4.71

TC

8.512

8.933

4.72

TC

6.149

6.203

0.86

TC

20.5

CO2 + n-C28H58

Ethane + n-C32H66

20

6.57
10.1
12.02
13.64
16.67
20.2

Ethane + n-C30H62

Ethane + n-C33H68

10.1

6.47
10.2
12.12
13.64
16.67
20.2

8.1457

8.2785

J. Kondori et al. / Fluid Phase Equilibria 388 (2015) 182187

the ability of the model used for prediction of the experimental

data is acceptable and for most of the data, absolute deviation
values lie within the range of [025]%. For some cases, the
thermodynamic model criteria was not met (model predictions
were not within the range of [025]%); in these cases the poor
predictions were eliminated and the data were not considered in
the consistency test. The results of the thermodynamic consistency
test for the datasets investigated are reported in Table 6. As can be
observed, all the datasets considered (the datasets which are well
correlated by the thermodynamic model) are thermodynamically
consistent. The same result was found in the previous study [1] at
constant temperature which conrms the reliability of the
proposed thermodynamic consistency test in this study. Several
factors should be taken into consideration when evaluating the
reliability or accuracy of an experimental dataset, such as the
procedure or technique used for the measurement of the
experimental dataset; the accuracy of the calibration methods;
the ability of the researcher performing the experiments; the
accuracy of the low solubility measurements; and so on. It can be
inferred from the thermodynamic consistency check of the
datasets analyzed in this study that researchers have taken great
care in the measurement of the experimental data. The results of
this study would conrm the reliability of experimental data which
can then be used with condence for the tuning of thermodynamic
model parameters. Thermodynamically inconsistent data or not
fully consistent data will result in erroneous predictions of the
model for further applications and the reason of such deviations
may not be identied easily.
It should be note that the proposed thermodynamic consistency
test is only applicable to isobaric experimental data and the
developed equations in this study are based on this assumption. In
a previous study [1] an isothermal procedure was performed for
the evaluation of the thermodynamic consistency of the experimental data. Hence, depending on the way in which the
experimental data has been presented (isothermal or isobaric)
either procedure (temperature constant or pressure constant) can
be applied. Looking for isobaric or isothermal experimental data is
one of the limitations of the proposed consistency tests. One
solution to this problem is generating pseudo experimental data
using statistical software. However, in generating such data
thermodynamically tested data are required.
7. Conclusions
A new thermodynamic consistency test based on calculation of
the residual enthalpies was applied at constant pressure for 48
experimental data of parafn wax solubilities in supercritical CO2
and ethane. The original GibbsDuhem [3,6,7] equation was used
to relate the calculated residual enthalpies to solubility and
fugacity coefcients of the components. The PR EoS [19] coupled
with vdW2 [20] mixing rule was used for the prediction of the
parafn wax solubilities in supercritical CO2 and ethane. The
results show that all the considered datasets which are within the
model capability seem to be thermodynamically consistent. These
results are in good agreement with the results obtained from a
previous study [1] in which the datasets were tested thermodynamically at constant temperature. Since all the datasets

187

considered in this study are thermodynamically consistent, the

procedure applied by Teja et al. [2] in their measurements can be
concluded as reliable.
Given the importance of solubility data of parafn waxes in
supercritical uids and the fact that these kinds of data are indeed
rare, the results obtained in this study can be used for further
applications in natural gas systems.
Acknowledgements
This work is based upon research supported by the South
African Research Chairs Initiative of the Department of Science and
Technology and National Research Foundation.
References
[1] A.H. Mohammadi, A. Eslamimanesh, D. Richon, Wax solubility in gaseous
system: thermodynamic consistency test of experimental data, Ind. Eng.
Chem. Res. 50 (8) (2011) 47314740.
[2] A.S. Teja, V.S. Smith, T.S. Sun, J. Mendez-Santiago, Solids deposition in natural
gas systems, Res. Rep. 171 (2000) 905993 GPA project.
[3] J.M. Prausnitz, R.N. Lichtenthaler, E.G. de Azevedo, Molecular
Thermodynamics of Fluid-Phase Equilibria, Pearson Education, 1998.
[4] J. Raal, A. Mhlbauer, Phase Equilibria: Measurement and Computation, Taylor
& Francis, Washington, 1998.
[5] B. Poling, J. Prausnitz, J. OConnell, The Properties of Gases and Liquids, fth ed.,
New York, Mc-Graw Hill, 2001.
[6] J. Smith, H. van Ness, M. Abbott, Introduction to Chemical Engineering
Thermodynamics, sixth ed., McGraw-Hill, New York, 2003.
[7] H. van Ness, M. Abbott, Classical Thermodynamics of Non-Electrolyte
Solutions, McGraw-Hill, New York, 1982.
[8] J.O. Valderrama, V.H. Alvarez, A versatile thermodynamic consistency test for
incomplete phase equilibrium data of high-pressure gasliquid mixtures,
Fluid Phase Equilib. 226 (12) (2004) 149159.
[9] C.A. Fandez, J.F. Daz-Valds, J.O. Valderrama, Consistency test of solubility
data of ammonia in ionic liquids using the modied PengRobinson equation
of Kwak and Mansoori, Fluid Phase Equilib. 348 (2013) 3338.
[10] J.O. Valderrama, A. Retegui, W.W. Sanga, Thermodynamic consistency test of
vaporliquid equilibrium data for mixtures containing ionic liquids, Ind. Eng.
Chem. Res. 47 (21) (2008) 84168422.
[11] J.O. Valderrama, P.A. Robles, A. Retegui, Data analysis, modeling and
thermodynamic consistency of CO2 + b-carotene high pressure mixtures, J.
Supercrit. Fluids 55 (2) (2010) 609615.
[12] J.O. Valderrama, P.A. Robles, Thermodynamic consistency of high pressure
ternary mixtures containing a compressed gas and solid solutes of different
complexity, Fluid Phase Equilib. 242 (1) (2006) 93102.
[13] J.O. Valderrama, J. Zavaleta, Thermodynamic consistency test for high pressure
gassolid solubility data of binary mixtures using genetic algorithms, J.
Supercrit. Fluids 39 (1) (2006) 2029.
[14] J. Kondori, J. Javanmardi, A. Eslamimanesh, A.H. Mohammadi, Thermodynamic
consistency test for isobaric experimental data of water content of methane,
Fluid Phase Equilib. 347 (2013) 5461.
[15] H.S. Mickley, T.K. Sherwood, C.E. Reed, Applied Mathematics in Chemical
Engineering, McGraw-Hill, New York, 1957.
[16] A. Eslamimanesh, A.H. Mohammadi, D. Richon, Thermodynamic consistency
test for experimental data of water content of methane, AIChE J. 57 (9) (2011)
25662573.
[17] A. Eslamimanesh, A.H. Mohammadi, D. Richon, Thermodynamic consistency
test for experimental data of sulfur content of hydrogen sulde, Ind. Eng.
Chem. Res. 50 (6) (2011) 35553563.
[18] A. Constantinides, N. Mostou, Numerical Methods for Chemical Engineers
with MATLAB Applications, Prentice Hall, New Jersey, 1999, pp. 443.
[19] D.-Y. Peng, D.B. Robinson, A new two-constant equation of state, Ind. Eng.
Chem. Fundam. 15 (1) (1976) 5964.
[20] M. Mukhopadhyay . Natural Extracts Using Supercritical Carbon Dioxide, CRC
Press.
[21] E. Reverchon, P. Russo, A. Stassi, Solubilities of solid octacosane and
triacontane in supercritical carbon dioxide, J. Chem. Eng. Data 38 (1993)
458460.