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Numerical procedures for natural gas accurate thermodynamic properties

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Article  in  Journal of Engineering Thermophysics · October 2012

DOI: 10.1134/S1810232812040017

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ISSN 1810-2328, Journal of Engineering Thermophysics, 2012, Vol. 21, No. 4, pp. 213–234. 
c Pleiades Publishing, Ltd., 2012.

Numerical Procedures for Natural Gas Accurate

Thermodynamic Properties Calculation
M. Farzaneh-Gord* and H. R. Rahbari
The Faculty of Mechanical Engineering, Shahrood University of Technology, Shahrood, Iran
Received August 15, 2011

Abstract—Natural gas (NG) is a mixture of 21 elements and widely used in the industries
and domestics. Knowledge of its thermodynamic properties is essential for designing appropriate
process and equipments. In this study, the detailed numerical procedures for computing most
thermodynamic properties of natural gas are discussed based on the AGA8 equation of state (EOS)
and thermodynamics relationships. To validate the procedures, the numerical values are compared
with available measured values. The validations show that the average absolute percent deviation
(AAPD) for density calculations is 0.0831%, for heat capacity at the constant pressure is 0.87%, for
heat capacity at the constant volume is 1.13%, for Joule–Thomson coefficient is 1.93%, for speed
of sound is 0.133%, and for enthalpy is 1.06%. Furthermore, in this work, the new procedures are
presented for computing the entropy and internal energy. Due to lack of experimental data for these
properties, the validation is done for pure methane. The validation shows that AAPD is 0.078% and
0.0133% for internal energy and entropy, respectively.

DOI: 10.1134/S1810232812040017

1. INTRODUCTION
Natural gas (NG) is a naturally occurring and complex mixture of hydrocarbons with minor amount
of inorganic compounds. Due to rich NG resources as well as lower emissions of greenhouse gases
than other fossil fuels, NG has many applications in domestics and the industry. The natural gas is
processed and transported before reaching its end users. Knowledge of thermodynamics properties of
NG is essential for designing appropriate process and equipments. Since NG is a mixture of different
gases with various properties, its properties are strongly influenced by its components.
The NG thermodynamic properties could be obtained either by the laboratory techniques or by
employing equations of state (EOS). Laboratory techniques have a high accuracy, but some of the
thermodynamic properties such as entropy, enthalpy, and internal energy are not measurable. The cost
and difficulty of launching devices are other negative factors, which resulted in reducing the use of
laboratory techniques.
By employing EOS, all thermodynamic properties could be calculated with acceptable accuracy and
without spending much time. Therefore, the use of EOS for calculating the properties has extended
dramatically in recent years. McCarthy [1] used the method of extended corresponding states (ECS)
for calculating the thermodynamic properties. He predicted the properties of the binary mixtures N2 –
CH4 and CH4 –C2 H6 . Estela-Uribe and Trusler [2] used the ECS equation of state for calculating the
thermodynamic properties of NG. They considered 12 major components of natural gases and calculated
compressibility factor and speed of sound with average deviations within ±0.036%. Estela-Uribe et al.
[3] also employed ECS and two optimized models and calculated density and speed of sound for 19
binary systems. The average absolute deviation for their density calculations was 0.12% and 0.03%, and
the average absolute deviation for their speed of sound calculations was 0.16% and 0.03%. The ECS
models [1–3] take the advantage of binary parameters, and, therefore, cannot be extended to natural gas
mixtures with heavy fractions.
*
E-mail: mahmood.farzaneh@yahoo.co.uk

213
214 FARZANEH-GORD, RAHBARI

Jaeschke et al. [4] employed a truncated virial equation model to calculate the compressibility factor
of NG. The equation has generally been used in custody transfer. Kunz et al. [5] have presented an EOS
for natural gas with a wide range. Their equation is the form of the Helmholtz energy. This form has been
used successfully for refrigerant mixtures and natural gas mixtures.
Cubic EOSs including Redlich–Kwong (RK) [6], Soave–Redlich–Kwong (RKS) [7], Peng–
Robinson (PR) [8], and Valderrama–Patel–Teja (VPT) [9] are employed in most of the petroleum
industries due to simplicity. These EOSs are widely used for phase equilibrium calculation. Due to low
accuracy in calculating volumetric properties, application of these EOSs reduces for complex mixtures
such as NG [10].
Neubauer et al. [11] have employed Monte Carlo simulation in the NPT ensemble to determine
the molar volume and the compressibility factor of naturally occurring hydrocarbon gas mixtures.
Elsharkawy et al. [12] presented a new model for calculating the gas compressibility factor based on
compositional analysis of 1200 compositions of gas condensates. Elsharkawy [13] presented efficient
methods for calculating the compressibility factor, density, and viscosity of natural gases. This model is
derived from 2400 measurements of compressibility and density of various gases.
Wendland et al. [14] have employed BACKONE EOS to calculate NG thermodynamic properties
and to improve accuracy of calculation. Comparing their calculations with experimental data shows
that their calculations have high accuracy. Nasrifar and Bolland [15] employed 10 cubic EOSs and a
new cubic two-constant EOS to calculate the NG thermodynamic properties. The average absolute
error for their calculation was 0.47% for predicting the compressibility factors and 0.70% for predicting
the speed of sound. Martinez and Hall [16] calculated thermodynamic properties of light synthetic NG
using the RK–PR EOS. Comparing their calculations with experimental data shows good accuracy and
simplicity of calculating the NG thermodynamic properties, including density, fugacity coefficient, and
vapor-liquid equilibrium. Huber et al. [17] have provided a surrogate mixture model for thermophysical
property calculation.
The AGA8 equation of state [18–19] has been developed by American Gas Association. It incor-
porates both theoretical and empirical elements. This has provided the correlation with the degree of
numerical flexibility needed to achieve high accuracy for the compressibility factor and density of NG
for custody transfer. It shows good performance and high accuracy for the temperature range between
143.15 K and 676.15 K, and pressure up to 280 MPa. The AGA8 has been also subject to various
researches for thermodynamic property calculation. Isentropic exponent, Joule–Thomson coefficient,
and heat capacities at constant pressure and volume were calculated by Maric et al. [20] and Maric [21,
22]. Farzaneh-Gord et al. [23] have computed thermal properties of natural gas such as enthalpy and
internal energy in addition to the compressibility factor.
The current study has been extended extensively the above-mentioned studies by presenting detailed
numerical procedures for computing almost all thermodynamic properties of NG. The procedures have
been developed based on the AGA8 EOS. The procedures have been presented for computing density,
heat capacity, Joule–Thomson coefficient, speed of sound, entropy, enthalpy, and internal energy of NG.
To validate the results, comparisons have been done between numerical and available measured values.

2. AGA8 EOS
The general form of AGA8 equation of state is presented as follows [18]:
P = Zρm RT. (1)
In Eq. (1), P is pressure, Z is compressibility factor, ρm is molar density, R is universal gas constant,
and T is temperature.
The compressibility factor is calculated by employing the following equation [18]:

18 
18
Z = 1 + Bρm − ρr Cn∗ + Cn∗ Dn∗ . (2)
n=13 n=13

In Eq. (2), ρr is reduced density defined as follows:

ρr = K 3 ρm , (3)

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 NUMERICAL PROCEDURES FOR NATURAL GAS 215

where K is the mixture size parameter calculated using the following equation [18]:
N 2 −1 
 5
N N
5
5
K = xi Ki2
+2 5
xi xj (Kij − 1)(Ki Kj ) 2 . (4)
i=1 i=1 j=i+1

In Eq. (4), xi is the mole fraction of component i in the mixture, xj is the mole fraction of component j
in the mixture, Ki is the size parameter of component i, Kj is the size parameter of component j, Kij is
the binary interaction parameter for size, and N is the number of components in the gas mixture.
In Eq. (3), B is the second virial coefficient given by the following equation [18]:

18 
N 
N
−un ∗ un 3
B= an T xi xj Bnij Eij (Ki Kj ) 2 . (5)
n=1 i=1 j=1
∗ and E un are defined by the following equations [18]:
In Eq. (5), Bnij ij

∗ = (G + 1 − g )gn (Q Q + 1 − q )qn (F
Bnij
1/2 1/2
Fj + 1 − fn )fn
ij n i j n i
(6)
×(Si Sj + 1 − sn )sn (Wi Wj + 1 − wn )wn ,

∗
Eij = Eij (Ei Ej )1/2 . (7)
In Eq. (6), Gij is defined by the following equation [18]:
G∗ij (Gi + Gj )
Gij = . (8)
2
In Eqs. (5)–(8), T is the temperature, N is the number of components in gas mixture, an , fn , gn , qn , sn ,
un , and wn are the equation of state parameters, Ei , Fi , Gi , Ki , Qi , Si , and Wi are the corresponding
characterization parameters, and Eij ∗ . G∗ are the corresponding binary interaction parameters.
ij
In Eq. (2), Cn∗ , n = 1, . . . , 58, are temperature-dependent coefficients defined by the following
equation [18]:
Cn∗ = an (G + 1 − gn )gn (Q2 + 1 − qn )qn (F + 1 − fn )fn Unun T −un . (9)
In Eq. (9), G, F , Q, and U are the mixture parameters defined by the following equations [18]:
N 2 −1 
 5 
N N
5
5
U = xi Ei2 +2 xi xj (Uij5 − 1)(Ei Ej ) 2 , (10)
i=1 i=1 j=i+1


N 
N −1 
N
G= xi Gi + 2 xi xj (G∗ij − 1)(Gi + Gj ), (11)
i=1 i=1 j=i+1


N
Q= xi Qi , (12)
i=1


N
F = x2i Fi , (13)
i=1

where in Eq. (10), Uij is the binary interaction parameter for mixture energy.
In Eq. (2), Dn∗ is defined by the following equation:
Dn∗ = (bn − cn kn ρkr n )ρbrn exp(−cn ρkr n ). (14)

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216 FARZANEH-GORD, RAHBARI

Coefficients of Eq. (14) are presented in the references [18].

Substituting Eq. (2) in Eq. (1), if the temperature, pressure, and composition of natural gas are
known, the only unknown parameter would be molar density. The molar density is calculated using
Newton–Raphson iterative method [24].
The density of natural gas is then calculated by using the following equation:
ρ = Mw ρm , (15)
where Mw and ρm are molecular weight and molar density, respectively. Knowing the molar density, the
compressibility factor is calculated using Eq. (1).
The AGA8 model is intended for a specific range of the gas components. It is not recommended for
the gases with mole percentages outside of the value given in Table 1 [18].

3. RESULTS AND DISCUSSION

In this section, the procedure for calculating each property is discussed firstly. Then, the comparison
with available measured values will be presented. To validate the results, the numerical and available
experimental values have been compared. The percent error and average absolute percent deviation
(AAPD) have been employed as comparisons tools:
P ropertyCal − P ropertyExp
Error (%) = ∗ 100. (16)
P ropertyExp
 
1   P ropertyCal − P ropertyExp 
AAP D (%) =  ∗ 100. (17)
n P ropertyExp

In Eqs. (16), (17): P ropertyCal , P ropertyExp, and n are numerical value, available measured value, and
the number of experimental data, respectively.

Table 1. Range of gas mixture characteristics in AGA8 model [18]

Component (mol %) Normal range Expanded range

Methane 45 to 100 0 to 100
Nitrogen 0 to 50 0 to 100
Carbon Dioxide 0 to 30 0 to 100
Ethane 0 to 10 0 to 100
Propane 0 to 4 0 to 12
Total Butanes 0 to 1 0 to 6
Total Pentanes 0 to 0.3 0 to 4
Hexanes Plus 0 to 0.2 0 to Dew Point
Helium 0 to 0.2 0 to 3
Hydrogen 0 to 10 0 to 100
Carbon Monoxide 0 to 3 0 to 3
Argon 0 0 to 1
Oxygen 0 0 to 21
Water 0 to 0.05 0 to Dew Point
Hydrogen Sulfide 0 to 0.02 0 to 100

JOURNAL OF ENGINEERING THERMOPHYSICS Vol. 21 No. 4 2012

 NUMERICAL PROCEDURES FOR NATURAL GAS 217

Fig. 1. Error percent in density calculation: (a) NG3; (b) NG1.

Fig. 2. Error percent in density calculation: (a) NG5; (b) NG6.

JOURNAL OF ENGINEERING THERMOPHYSICS Vol. 21 No. 4 2012

218 FARZANEH-GORD, RAHBARI

Table 2. Mole percent of natural gas components used in density calculation [25–27]

Component NG1 NG2 NG3 NG4 NG5 NG6

CH4 98.352 92.436 90.991 90.362 81.299 85.898
N2 0.841 5.751 2.031 1.474 13.575 1.007
CO2 0.066 0.052 0.403 0.676 0.994 1.498
C2 H 6 0.511 1.285 2.949 5.708 3.294 8.499
C3 H 8 0.153 0.345 1.513 1.124 0.637 2.296
O2 – – – 0.011 – –
He – – – 0.015 – –
i-C4 H10 0.021 0.041 0.755 0.301 0.101 0.351
n-C4 H10 0.031 0.046 0.755 0.169 0.1 0.347
i-C5 H12 0.008 0.015 0.299 0.059 – 0.051
n-C5 H12 0.011 0.014 0.304 0.029 – 0.053
n-C6 H14 0.005 0.012 – 0.058 – –
n-C7 H16 0.001 – – 0.035 – –
n-C8 H18 0.0003 – – 0.008 – –

Table 3. AAPD for density calculations

Mixture Reference Number of data T range [K] P range [MPa] AAPD (%)
NG1 Capla et al. [25] 28 253.15–323.15 1–15 0.0084
NG2 Capla et al. [25] 28 253.15–323.15 1–15 0.064
NG3 Patil et al. [26] 30 270–340 2–35 0.216
NG4 Capla et al. [25] 28 253.15–323.15 1–15 0.06013
NG5 Hwang et al. [27] 77 250–325 0.2–10.5 0.0997
NG6 Hwang et al. [27] 60 275–325 0.2–10.5 0.0533
Overall 251 0.0831

3.1. Density
Density is calculated by utilizing Eq. (15). Table 2 shows mole percent of natural gases used in
density calculation. Table 3 shows the range of temperature and pressure, and AAPD (%). Considering
the values in Table 3, one could conclude that the density calculation has high accuracy with an overall
AAPD of 0.0831%. Figures 1 and 2 illustrate error percent for density calculations. According to Figs. 1
and 2, as temperature increases or pressure decreases, error percent decreases. This shows that as the
natural gas behavior approaches closer to an ideal gas, accuracy of the AGA8 EOS for prediction density
increases.

3.2. Heat Capacity at Constant Volume (Cv )

To calculate the heat capacity at constant volume, the procedure presented by Maric et al. [20–22] is
followed. The heat capacity at constant volume is defined as follows:
 
∂u
Cv = , (18)
∂T ν

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 NUMERICAL PROCEDURES FOR NATURAL GAS 219

where in Eq. (18), Cv is heat capacity at constant volume, ν is specific volume, u is internal energy, and
T is temperature. Equation (18) can be written as follows:
   
∂um ∂sm
Cm,v = . (19)
∂sm νm ∂Tm νm
In Eq. (19), Cm,v is molar heat capacity at constant volume, um is molar internal energy, sm is molar
entropy,
 and νm is molar specific volume. Using one of the thermodynamics relationships in the form of
∂um
T = ∂sm and differentiating Eq. (19), the following equation could be obtained:
νm
 
  
∂Cm,v ∂ ∂sm ∂ 2 sm
= T =T . (20)
∂νm ∂νm ∂Tm νm ∂νm ∂T
  ∂P
∂sm
By using the Maxwell relation, ∂ν m T
= ∂T νm , Eq. (20) becomes as follows:
   2 
∂Cm,v ∂ P
=T . (21)
∂νm ∂T 2 νm
The integral of Eq. (21) can be evaluated by changing the variable from νm to ρm . This would result in
the following equation:
ρm
    
1 ∂2Z ∂Z
Cm,v = Cm,pI − RT − RT T +2 dρm . (22)
ρm ∂T 2 ρm ∂T ρm
ρmI→0 (T =const)

In Eq. (22), Cm,pI is molar heat capacity at constant pressure of the ideal gas mixture and could be
obtained by following equation:

N
j
Cm,pI = xj Cm,pi , (23)
j=1

j
where xj is the mole fraction and Cm,pi is the ideal molar heat capacity at constant pressure of
component j. The proposed equation for the ideal molar heat capacity at constant pressure is as
follows [28]:
⎛ cj ⎞2 ⎛ ej ⎞
j
Cm,pi = aj + bj ⎝ T ⎠ + d ⎝
cj j
T ⎠ .
ej (24)
sinh sinh
T T
The following equation could be obtained for calculating the heat capacity at constant volume by
integrating Eq. (24):
Cm,v = Cm,pI − RT − RT [ρm (2Z0 + T Z1 ) + (2Z2 + T Z3 )], (25)
where

18
Z0 = B  − K 3 Cn∗ , (26)
n=13


18
Z1 = B  − K 3 Cn∗ , (27)
n=13


18
Z2 = Cn∗ ρbrn exp(−cn ρkr n ), (28)
n=13

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220 FARZANEH-GORD, RAHBARI

Fig. 3. Error percent for heat capacity at constant volume calculation.

Table 4. The mole percent and AAPD for heat capacity in constant volume calculations

Mixture Reference Number of data T range [K] P range [MPa] AAPD (%)

0.6553CH4 + 0.3147C2H6 Mayrath and Magee [29] 66 250–323 6.9–35.68 1.13


18
Z3 = Cn∗ ρbrn exp(−cn ρkr n ). (29)
n=13

In Eqs. (26)–(29), B  and B  are first and second derivations of Eq. (5) with respect to temperature.
And also, Cn∗ and Cn∗ are first and second derivations of Eq. (9) with respect to temperature.
To validate numerical results for the heat capacity at constant pressure, the measured values of a
binary mixture similar to natural gas have been compared with the numerical values. Table 4 shows the
mole percent of the binary mixture. Furthermore, this table shows the range of temperature and pressure
and the amount of AAPD. AAPD is found to be 1.13% for all data, which shows accuracy of the method.
Figure 3 shows the error percent versus temperature at a few constant molar density modes. According
to Fig. 3, as temperature increases the error percent decreases.

3.3. Heat Capacity at Constant Pressure (CP )

Following the procedure presented by Maric et al. [20, 22], the heat capacity at constant pressure
calculation starts by its definition as follows:
 
∂h
CP = , (30)
∂T P
where CP is the heat capacity at constantpressure,
P is pressure, h is enthalpy, and T is temperature.
∂sm ∂P

Using Eq. (18) and the Maxwell relation, ∂νm = ∂T νm , and differentiating the entropy related to
T
temperature and molar volume obtain:
 
Cm,ν ∂P
dsm = dT + dνm . (31)
T ∂T νm

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 NUMERICAL PROCEDURES FOR NATURAL GAS 221

Fig. 4. Error percent in calculation of heat capacity at constant pressure for Mix3.

 m  ∂νm
Using Eq. (30) and Maxwell relation ∂s
∂P T = − ∂T P , and differentiating of the entropy related
to temperature and pressure obtain:
 
Cm,P ∂νm
dsm = dT − dP. (32)
T ∂T P
By combining Eqs. (31) and (32), the following equation could be obtained:
   
∂νm ∂P
Cm,P = Cm,ν + T . (33)
∂T P ∂T νm
Partial differentiations of Eq. (33) are calculated using Eq. (1) and AGA8 EOS as follows:
   
  
∂P ∂P ∂Z
= = Rρm Z + T , (34)
∂T νm ∂T ρm ∂T ρm
     
∂νm R ∂Z
= Z+T . (35)
∂T P P ∂T P
The validation for heat capacity at constant pressure is carried out for three natural gas mixtures.
Table 5 shows the mole percent of these mixtures. Table 6 also shows the range of temperature and
pressure, and the amount of AAPD. The AAPD for 140 data is found to be 0.87%. Nasrifar and Bolland
[15] have calculated AAPD for the same number of data and found it to be 1.46% by employing the cubic
EOS. Comparing the results with Nasrifar and Bolland [15] values, one could conclude that the current
model is more accurate. Figure 4 shows the error percent for the mixture Mix3 versus temperature and
for various pressures. According to Fig. 4, the error percent generally is in the range of −1% to +2%.

3.4. Joule–Thomson Coefficient (μJT )

The Joule–Thomson coefficient is defined as follows:
 
∂T
μJT = , (36)
∂P h

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222 FARZANEH-GORD, RAHBARI

Table 5. Mole percent of natural gas components used in heat capacity in constant pressure calculations

Component Mix1 Mix2 Mix3

CH4 85 79.942 89.569
N2 – 9.939 0.494
CO2 – 2.09 –
C2 H 6 15 5.029 8.348
C3 H 8 – 3 1.197
i-C4 H10 – – 0.149

Table 6. AAPD for heat capacity in constant pressure calculations

Mixture Reference Number of data T range [K] P range [MPa] AAPD (%)
Mix1 Ernst et al. [30] 56 250–350 0.6–30 0.5066
Mix2 Ernst et al. [30] 54 250–350 0.6–30 1.122
Mix3 Barreau et al. [31] 30 307–406 14.92–40.03 1.088
Overall 140 0.87

Table 7. AAPD for Joule–Thomson coefficient calculations

Mixture Reference Number of data T range [K] P range [MPa] AAPD (%)
Mix1 Ernst et al. [30] 48 250-350 0.5-30 1.718
Mix2 Ernst et al. [30] 39 250–350 0.5–30 2.188
Overall 87 1.93

where μJT is Joule–Thomson coefficient, P is pressure, h is enthalpy, and T is temperature. Differenti-

ation of enthalpy related to temperature and molar volume gives [10]:
   
∂νm
dhm = Cm,P dT + νm − T dP. (37)
∂T P

Assuming a constant enthalpy process, the following equation has been obtained:
   
∂νm
  T − νm
∂T ∂T P
μJT = = . (38)
∂P h Cm,P

The Joule–Thomson coefficient validation is done for Mix1 and Mix2 (Table 4). Table 7 shows
the range of temperature and pressure, and the amount of AAPD. The overall AAPD is found to be
1.93%. Nasrifar and Bolland [15] calculated the Joule–Thomson coefficient for Mix2. The AAPD of
their calculations was found to be 5.03%, while the AAPD for the current study is 2.188% (Table 7).
This shows that the method employed in the current work is more accurate than the one with cubic
EOS. Figure 5a compares Joule–Thomson coefficient with the measured value of Ernst et al. [30]. Note
from the figure, good agreement is observed. Fig. 5b shows error percent versus pressure at various
temperatures. According to Figure 5b, by increasing temperature and pressure, error percent is reduced.
Maric [22] also calculated the Joule–Thomson coefficient for natural gas mixtures using AGA8 EOS
and obtained similar results.

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 NUMERICAL PROCEDURES FOR NATURAL GAS 223

Fig. 5. (a) Joule–Thomson coefficient; (b) error percent in Joule–Thomson coefficient calculation for Mix2.

3.5. Speed of Sound (usound )

Speed of sound is the distance traveled per unit time by a sound wave propagating through an elastic
medium. The speed of sound is defined as follows:
 
∂P
usound = . (39)
∂ρ
s

In Eq. (39), usound is the speed of sound, ρ is the density, s is entropy, and P is pressure. Using Eq. (15)
and the thermodynamics relationships, the speed of sound can be written as follows:
 ∂P
1
2
usound =  ∂T s . (40)
Mw ∂ρm
∂T s

Using the second law of thermodynamics [10] and assuming constant entropy process, the following
equations could be obtained:
 
∂P CP m
=  ∂νm , (41)
∂T s T ∂T
P
 
∂ρm ρ2
= Cνm  ∂Pm . (42)
∂T s T ∂T νm

Combining Eqs. (40)–(42), the following equation could be developed for calculating the speed of sound:
 ∂P
1 C P m ∂T ρ
u2sound = × 2
 ∂νm m . (43)
Mw Cνm ρm ∂T
P

CP m and Cνm have been calculated as discussed in the previous sections. Partial differential relation-
ships in Eq. (43) are calculated using Eqs. (34) and (35).

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224 FARZANEH-GORD, RAHBARI

Table 8. The mole percent of mixture component for speed of sound calculations

Component Mix4 Mix5 Mix6 Mix7 Mix8

CH4 80 85 90 80 80
N2 – – 10 20 10
CO2 – – – – 2
C2 H 6 20 15 – – 5
C3 H 8 – – – – 3

Table 9. AAPD for speed of sound calculations

Mixture Reference Number of data T range [K] P range [MPa] AAPD (%)
Mix4 Trusler [32] 47 200–375 0.1–14 0.063
Mix5 Costa Gomes and Trusler [33] 36 250–350 0.5–21 0.18
Mix6 Estela-Uribe et al. [34] 100 220–400 0.1–30 0.09
Mix7 Estela-Uribe et al. [34] 109 220–400 0.1–30 0.16
Mix8 Costa Gomes and Trusler [33] 35 250–350 0.51–20 0.23
Overall 327 0.133

In this work, the speed of sound for four binary mixtures and one mixture similar to natural gas
has been calculated and compared with available measured values. Table 8 shows the mole percent of
mixture components. Table 9 shows the range of temperature, pressure, and the AAPD for speed of
sound calculation.
Figures 6 and 7 show the error percent versus pressure at various temperatures for sound speed
calculation. As shown in Figs. 7 and 8, increasing temperature and decreasing pressure (approaching
to ideal gas behavior) resulted in error percent reduction. The AAPD for 327 experimental data is found
to be 0.133%. Nasrifar and Bolland [15] have calculated AAPD to be 0.7% using cubic EOS and 371
experimental data. Thus, the AGA8 EOS has much higher accuracy than the cubic EOS in sound speed
calculation.

3.6. Enthalpy (h)

One of the important thermal properties of natural gas is enthalpy. Assuming the enthalpy is a
function of temperature and molar specific volume, the enthalpy residual function could be defined as
follows:
νm
   νm  
∂P ∂Z
hm − hm,I = T − P dνm + RT dνm . (44)
∂T νm ∂νm T
νm,I →∞ νm,I →∞

In Eq. (44), hm is the molar enthalpy for real gas mixture, hm,I is molar enthalpy for ideal gas mixture,
and νm,I is molar specific volume for ideal gas mixture. By changing the variable from νm to ρm and
integrating Eq. (44), the enthalpy residual function becomes as follows:
ρm 
∂Z dρm
hm − hm,I = −RT 2
+ RT (Z − 1). (45)
∂T ρm ρm
0

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 NUMERICAL PROCEDURES FOR NATURAL GAS 225

Fig. 6. Error percent for calculating sound speed: (a) Mix6; (b) Mix7.

Fig. 7. Error percent for calculating sound speed: (a) Mix8; (b) Mix5; (c) Mix4.

The molar enthalpy for the ideal gas mixture could be calculated as follows:

N
hm,I = xj hjm,i , (46)
j=1

where hjm,i is the molar enthalpy of component j in the ideal gas mixture [28].
c e
j j
hjm,i = hjm,i0 + aj T + bj cj coth − dj ej tanh , (47)
T T

where hjm,i0 is the molar enthalpy of component j in the mixture at the reference state (25◦ C,
101.325 kPa). By integrating from Eq. (45) and computing the ideal molar enthalpy for all components

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226 FARZANEH-GORD, RAHBARI

Table 10. Type of mixture and AAPD for the isobaric enthalpy increment process

Reference Number of data T1 [K] Constant P [MPa] AAPD (%)

Pure CH4 Day et al. [35] 51 304–525 3 0.474
Pure CH4 Day et al. [35] 40 313–513 7 0.468
0.89CH4 + 0.11C2 H6 Day et al. [35] 21 376–474 7 1.72
0.75CH4 + 0.25C2 H6 Day et al. [35] 20 375–428 7 1.44
Mix9 Ashton and Haselden [36] 24 361–367 13–55 2.211
Overall 156 1.03

Table 11. Type of mixture and AAPD for temperature drop in the isenthalpic process calculation

Number of data T1 [K] Pressure drop [MPa] AAPD (%)

Pure CH4 23 304–557 3–0.17 1.54
Pure CH4 21 313–535 7–0.17 1.32
0.89CH4 + 0.11C2 H6 15 376–524 7–0.17 0.62
0.75CH4 + 0.25C2 H6 15 375–488 7–0.17 0.7
Overall 74 1.12

using Eq. (47), the molar enthalpy could be calculated. The enthalpy per unit mass then could be
computed as follows:
hm
h= . (48)
Mw
For validating the enthalpy calculation, the measured values of an isobaric enthalpy increment and
temperature drop in an isenthalpic process have been compared with the numerical values. Based on the
measured values, error percent and AAPD have been computed.
For the isobaric enthalpy increment, temperature, pressure, and mixture mole percent are known. The
enthalpy has been calculated at inlet and outlet, and the enthalpy increment has been computed. Finally,
the measured and numerical values are compared. Table 10 shows the type of mixture, inlet temperature,
pressure and AAPD for the enthalpy increment validation and calculations. The calculations include:
pure methane and two binary mixtures of natural gas and a mixture similar to natural gas. Mix9
is a mixture of Methane, Ethane, Propane, Nitrogen, iso-Butane and Normal-Butane whose range
of mole percent of composition for this mixture includes: Methane: 89–92%, Ethane: 2.31–2.33%,
Propane: 0.4–0.48, Nitrogen: 4.45–8%, iso-Butane: 0.3–0.4%, and Normal-Butane: 0.04–0.05%.
AAPD calculations for pure methane and mixture are 0.471%, 1.82%, respectively. For the total data,
the AAPD is found to be 1.03%, which is acceptable in the engineering applications.
Figure 8 shows the error percent in the isobaric enthalpy increment for two binary mixtures versus the
inlet temperature. Figure 9 shows the error percent for Mix9 at various pressures. According to Fig. 8,
the error percent for most data is less than 2% and according to Fig. 9 the error percent for most data is
between −1% to +3%.
The temperature drop in the isenthalpic process has been calculated numerically by an iterative
method. The inlet temperature, pressure, and mole percent composition of the mixture have been
specified, and the inlet enthalpy has been calculated. Based on the equality of inlet and outlet enthalpy,
and specifying pressure at the outlet, the outlet temperature and temperature drop have been calculated.
Table 11 shows the type of mixture, inlet temperature, the pressure drop, and AAPD for the isenthalpic
process. The numerical calculations in this work include: pure methane for two processes and two binary

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 NUMERICAL PROCEDURES FOR NATURAL GAS 227

Fig. 8. Error percent in the isobaric enthalpy increment (Day et al. [35]).

Fig. 9. Error percent in the isobaric enthalpy increment for Mix9 (Ashton and Haselden [36]).

mixtures. The AAPD calculations for pure methane and mixture are 1.435% and 0.66%, respectively.
The AAPD is found to be 1.12% for 74 experimental data, which show accuracy of the numerical
method.
Figure 10 shows temperature drop versus inlet temperature for pure methane and two binary
mixtures. For all data in Fig. 10, inlet and outlet pressures are 7 MPa and 0.17 MPa, respectively. It
could be realized from Fig. 10, for the same inlet temperature, the temperature drop increases as methane
percent in the mixture decreases. Thus, it could be concluded that the gas composition has a great effect
on the temperature drop. Figure 11 shows the error percent versus inlet temperature. Note from Fig. 11,

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228 FARZANEH-GORD, RAHBARI

Fig. 10. Temperature drop in the isenthalpic process (experimental data of Day et al. [35]).

Fig. 11. Error percent in the temperature drop calculation.

the error percent is less than 2% generally, which again shows accuracy of the numerical methods. It
should be noted that accurate temperature drop predication for an isenthalpic process (e.g., flow across
a regulating valve) is essential for many places in natural gas processing.

3.7. Internal Energy (u)

Assuming internal energy is a function of temperature and molar specific volume, the internal energy
residual function can be expressed as follows:
νm
  
∂P
um − um,I = T − P dνm , (49)
∂T νm
νm,I →∞

where um and um,I are the molar internal energy for the real and ideal gas mixture, respectively.
Combining in Eqs. (49) and (34) and changing variables from νm to ρm , the following equation could be

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 NUMERICAL PROCEDURES FOR NATURAL GAS 229

Fig. 12. Error percent in calculation of internal energy for pure methane.

Table 12. AAPD for internal energy calculation for pure methane

Reference Number of data T range [K] P range [MPa] AAPD (%)

Pure CH4 Setzmann and Wagner [37] 299 250–350 1–60 0.078

obtained:
ρm 
∂Z dρm
um − um,I = −RT 2
. (50)
∂T ρm ρm
0

The molar internal energy for the ideal gas mixture could be calculated using the following equation:
um,I = hm,I − P νm = hm,I − RT, (51)

where hm,I is the molar enthalpy for ideal gas mixture and calculated using Eq. (46). T is temperature
and R is universal gas constant. The internal energy per unit mass could be calculated by its definition
as follows:
um
u= . (52)
Mw

There are no available measured values of internal energy in the literature for a natural gas mixture
or a similar mixture. Thus, in this work, the numerical values have been compared with experimental
values of pure methane for validation purposes. The numerical values have been compared with data of
Setzmann and Wagner [37]. The error percent and AAPD have been calculated and presented in Fig. 12
and Table 12. Table 12 shows the range of temperature, pressure, and AAPD for the internal energy
calculation. Figure 12 shows error percent for the internal energy calculations for pure methane versus
pressure at various temperatures. According to Fig. 12, the absolute error percent of calculation is less
than 0.2%. Also, the AAPD for 299 data is found to be 0.078%. This shows high accuracy in internal
energy calculations using AGA8 EOS.

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230 FARZANEH-GORD, RAHBARI

Table 13. AAPD for entropy calculation for pure methane

Reference Number of data T range [K] P range [MPa] AAPD (%)

Pure CH4 Setzmann and Wagner [37] 300 250–350 1–60 0.0133

3.8. Entropy (s)

Using one of Maxwell’s relations, the following relationship for entropy could be derived:
   
∂sm ∂P
= , (53)
∂νm T ∂T νm

where sm is the molar entropy. By integrating from Eq. (53) and changing variables, the following
equation for the molar entropy could be obtained:
ρm
  
∂Z dρm
sm = sm,I − R Z +T , (54)
∂T ρm ρm
0

where sm is the molar entropy for the real gas mixture and sm,I is the molar entropy for the ideal mixture.
The molar entropy for the ideal mixture is defined as follows:

N
sm,I = xj sm,i j , (55)
j=1

where sjm,i is molar entropy of component j in the ideal mixture, which could be presented as below:

sjm,i (T, P, xj ) = sjm,i (T ) − RLn(xj P ), (56)

where sjm,i (T ) is molar entropy for component j in the ideal mixture at the reference pressure. This could
be expressed by the following equation [28]:
 c c   c 
j j j
sjm,i (T ) = sjm,i0 + aj Ln(T ) + bj coth − Ln sinh
T T T
 e e   e  (57)
j j j
−dj coth − Ln cosh ,
T T T

where sjm,i0 is the molar entropy for component j in the ideal mixture at reference temperature and
pressure. Entropy per unit mass then could be calculated as follows:
sm
s= . (58)
Mw

As there were no measured values of entropy for the natural gas mixture, the numerical and measured
values of entropy for pure methane have been compared in this work. The validation has been carried out
for experimental data of Setzmann and Wagner [37]. The error percent and AAPD have been calculated
and presented in Table 13 and Fig. 13. Table 13 also shows the range of temperature, pressure, and
AAPD for entropy calculations. Figure 13 shows error percent for the entropy calculations for pure
methane versus pressure at various temperatures. According to Fig. 13, the error percent is between
±0.03%. Furthermore, the AAPD for 300 data is found to be 0.0133%, which proved very high accuracy
in entropy calculations.

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 NUMERICAL PROCEDURES FOR NATURAL GAS 231

Fig. 13. Error percent in calculation of entropy for pure methane.

4. CONCLUSIONS
Given the current surge in natural gas businesses, trustworthy estimates of thermodynamic proper-
ties are necessary for designing engineering processes. Accurate prediction of thermodynamic properties
for natural gas is an essential requirement in optimum design and operation of most process equipment
involved in petrochemical production, transportation, and processing.
Here, based on the AGA8 EOS and thermodynamic relationships, the detailed procedures for
computing almost all thermodynamic properties of natural gas are presented. To validate the numerical
procedures, the numerical values have been compared with available measured values. The validations
show that the AAPD for density calculation is 0.0831%, for heat capacity at constant pressure
calculation is 0.87%, for heat capacity at constant volume calculation is 1.13%, for Joule–Thomson
coefficient calculation is 1.93%, for speed of sound calculation is 0.133%, for enthalpy calculation is
1.06%, for internal energy calculation is 0.078%, and for entropy calculation is 0.0133%. The AAPD
values indicate that the numerical procedure could predict thermodynamic properties of natural gas with
very high accuracy. The results also show that the natural properties calculation based on AGA8 is more
accurate than the cubic EOSs.

NOTATIONS
B–second virial coefficient
Cn∗ —temperature and composition dependent coefficient
CP —heat capacity at constant pressure (kJ/kg·K)
Cv —heat capacity at constant volume (kJ/kg·K)
h—enthalpy (kJ/kg)
hspecif ic —specific enthalpy (kJ/kg)
Kj —size parameter of component j
Kij —binary interaction parameter
Mw —molecular weight (kg/kmol)
N —number of component in gas mixture
n—number of experimental data
P —pressure (MPa)

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232 FARZANEH-GORD, RAHBARI

R—universal gas constant (kJ/kmol·K)

s—entropy (kJ/kg·K)
sspecif ic—specific entropy (kJ/kg·K)
T —temperature (K)
usound —speed of sound (m/s)
u—internal energy (kJ/kg)
uspecif ic —specific internal energy (kJ/kg)
x—mole fraction of component
Z—compressibility factor
∗ —binary energy interaction parameter for second virial coefficient
Eij
Ei —characterization energy parameter for ith component (K)
Eij —binary energy parameter for second virial coefficient (K)
F —mixture high-temperature parameter
Fi —high-temperature parameter for ith component
G—mixture orientation parameter
G∗ij —binary interaction parameter for orientation
Q—quadrupole parameter
Uij —binary interaction parameter for mixture energy
Wi —Association parameter for ith component

Greek Letters
ρm —molar density (kmol/m3 )
ρr —reduced density (kmol/m3 )
γ—gas gravity
vm —molar specific volume (m3 /kmol)
μJT —Joule–Thomson coefficient (K/MPa)

Abbreviations
AAPD—average absolute percent deviation
EOS—equation of state
ECS—extended corresponding states
AGA8—American Gas Association report no. 8

ACKNOWLEDGMENTS

The authors would like to thank officials in Semnan Gas Company for providing financial support for
this research.

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 NUMERICAL PROCEDURES FOR NATURAL GAS 233

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