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Using Lee-Kesler equation of state to compute the compressibility factor of

CO2 -content natural gas

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DOI: 10.1016/j.jngse.2016.07.032

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 Journal of Natural Gas Science and Engineering 34 (2016) 650e656

Contents lists available at ScienceDirect

Journal of Natural Gas Science and Engineering

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

Using Lee-Kesler equation of state to compute the compressibility

factor of CO2-content natural gas
Wenlong Jia a, b, *, Zhuoran Li a, Kexi Liao a, b, Changjun Li a, b
a
School of Petroleum Engineering, Southwest Petroleum University, Chengdu 610500, China
b
CNPC Key Laboratory of Oil & Gas Storage and Transportation, Southwest Petroleum University, Chengdu 610500, China

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

Article history: To improve the compressibility factor prediction of CO2-content natural gas, this short communication
Received 21 March 2016 proposes a new combinational Stewart-Burkhardt-Voo (SBV) þ Prausnitz-Gunn (PG) mixing rule for the
Received in revised form Lee-Kesler equation of state. The rule suggests using SBV and PG mixing rules for the pseudocritical
11 July 2016
temperature and pressure computations, respectively, when the reduced temperature is higher than one
Accepted 14 July 2016
Available online 18 July 2016
and the reduced pressure is higher than five; otherwise, the pseudocritical temperature and pressure is
calculated according to SBV mixing rule. Comparisons between experimental and calculation data show
that the maximum average relative deviation is 1.56% when the mole fraction of CO2 is less than 50%.
Keywords:
Carbon dioxide
© 2016 Elsevier B.V. All rights reserved.
Natural gas
Compressibility factor
Lee-Kesler equation of state
Mixing rule

1. Introduction wide range of conditions for pressures, temperatures, nonpolar and

slightly polar substances, large deviations between the actual and
Due to the worldwide lack of energy resources, the development calculated compressibility factors may be observed when it is
of gas fields is expanding to regions and deposits that were previ- applied to a natural gas with high CO2 content (Simon et al., 1977).
ously notably difficult to access. As a result, more CO2-content Lee-Kesler EoS (LK EoS) is a three-parameter correlation based
natural gas fields have been found worldwide, such as the Snøvhit on the corresponding state principle (CSP). The CSP refers that all
gas field in Norway and Jinlin gas field in China (Bjorheim et al., fluids have similar compressibility factors at the identical reduced
2015; Gaudernack and Lynum, 1998). It is essential to predict temperature and pressure (Lee and Kesler, 1975). Thus, LK EoS has
some thermodynamic properties of natural gas containing CO2 three key parameters: reduced temperature, reduced pressure and
during its development and transportation process, such as the reduced specific volume, which represent the fluid state. When it is
compressibility factor, density, enthalpy, entropy, fugacity and heat applied to a pure fluid, the reduced parameters can be calculated by
capacity (Moayyedi et al., 2015; Mohagheghian et al., 2015; Piper dividing the critical temperature/pressure/specific volume with the
et al., 1993). actual temperature/pressure/specific volume. When it is applied to
The equation of state is a widely used method to compute these a mixture, the pseudocritical parameters are used to replace the
parameters, such as PR, SRK, BWRS and Lee-Kesler EoSs (Poling actual critical temperature/pressure/specific volume (Li et al.,
et al., 2001; Li et al., 2014). Among many existing EoSs, the Lee- 2012). The pseudocritical parameters must be computed accord-
Kesler EoS is recommended by the API Technical Databook as the ing to a certain mixing rule, which significantly affects the calcu-
standard method to compute the compressibility factor of gas lation results. Thus, many mixing rules have been proposed in the
without or with low CO2 content (API, 2005). It is also recognized as past years (Piper et al., 1993), such as Kay's, Stewart-Burkhardt-Voo
the most accurate method to compute the enthalpy of hydrocarbon (SBV), SBV modified by Sutton (SSBV), and Plocker and Knapp
mixtures (Lee and Kesler, 1975). Although LK EoS is reliable over a mixing rules. However, there have been few reported applications
regarding CO2-content gas.
This short communication proposes a new combinational mix-
* Corresponding author. School of Petroleum Engineering, Southwest Petroleum ing rule to calculate the compressibility factor of CO2-content
University, Chengdu 610500, China. natural gas. The accuracy of the proposed mixing rule was validated
E-mail address: [email protected] (W. Jia).

http://dx.doi.org/10.1016/j.jngse.2016.07.032
1875-5100/© 2016 Elsevier B.V. All rights reserved.
 W. Jia et al. / Journal of Natural Gas Science and Engineering 34 (2016) 650e656 651

using experimental data with wide ranges of temperature, pressure 2.2. Mixing rules
and composition.
The reduced parameters in LK EoS are calculated based on the
critical parameters. For a pure fluid, we can use the actual critical
2. Compressibility factor calculation based on LK EoS temperature/pressure/specific volume of the fluid. For mixtures,
the pseudocritical parameters are preferred, which should be
2.1. LK EoS and compressibility factor calculation calculated according to the specified mixing rules. This paper ex-
amines five mixing rules: Lee-Kesler, Plocker-Knapp, Stewart-
LK EoS was proposed by Lee and Kesler in 1975 (Lee and Kesler Burkhardt-Voo, Kay and Wichert-Aziz, and Prausnitz-Gunn mix-
(1975)). Its general form is expressed by Eq. (1). ing rules.
!
Pr Vr B C D c g g a. Lee-Kesler (LK) mixing rule (Lee and Kesler, 1975)
¼ 1 þ þ 2 þ 5 þ 34 2 bþ exp (1)
Tr Vr Vr Vr Tr Vr Vr2 Vr2 " ! !
1 X
n Xn
2=3
pffiffiffiffiffiffi Xn
1=3
pffiffiffiffiffiffi
Tcm ¼ xv T þ3 xi vci Tci xi vvci Tci
where pr is the reduced pressure p/pc; p is the pressure; pc is the 4vcm i¼1 i ci ci i¼1 i¼1
critical pressure; Vr is the reduced specific mole volume pcV/RTc; V #
is the mole volume; Tr is the reduced temperature T/Tc; Tc is the

critical temperature; R is the gas constant; T is the temperature; B,
C, and D are defined by Eqs. (2)e(4).
(7)
. .
B ¼ b1  b2 =Tr  b3 Tr2  b4 Tr3 (2) !
P
0:2905  0:085 xi ui RTcm
. i¼1
C ¼ c1  c2=T þ c3 T 3 (3) pcm ¼ (8)
r r vcm

D ¼ d1 þ d2 =Tr (4) " ! !#

1 X n X
n
2=3
X
n
1=3
vcm ¼ xi vci þ 3 xi vci xi vci (9)
where b1, b2, b3, b4, c1, c2, c3, c4, d1, d2, b, and g are constants as listed 4
i¼1 i¼1 i¼1
in Table 1 (API, 2005).
According to Eq. (1), the compressibility factor is analytically where Tcm is the mixture pseudocritical temperature; vcm is the
expressed by the compressibility factor of a simple fluid and the mixture pseudocritical specific volume; pcm is the mixture pseu-
reference fluid compressibility factor, as shown in Eqs. (5) and (6). docritical pressure; x is the mole fraction; n is the total number of
The reference fluid is defined as propane by the API Technical components. The superscript i is for component i.
Databook (API, 2005).
b. Plocker-Knapp (PK) mixing rule (Plocker et al., 1978)
ðiÞ
ðiÞ pr Vr
z ¼
Tr
(5) 1 XX 1=4  1=2
Tcm ¼ 1=4
xi xj vcij Tci Tcj kij (10)
vcm i¼1 j¼1
u  ðrÞ 
z ¼ zð0Þ þ z  zð0Þ (6)
u ðrÞ !
P
0:2905  0:085 xi ui RTcm
where (i) ¼ (0) for a simple fluid, and (i) ¼ (r) for the reference fluid; i¼1
z is the fluid compressibility factor; z(0) and z(r) are the compress- pcm ¼ P P (11)
xi xj vcij
ibility factors of the simple fluid and reference fluid, respectively; u i¼1 j¼1
is the acentric factor of the fluid; u(r) is the acentric factor of the
reference fluid and is equal to 0.3978 for propane. z(0) and z(r) are  
1XX 1=3 1=3 3
calculated using Eq. (1) with the simple-fluid and reference-fluid vcm ¼ xi xj vci þ vcj (12)
constants in Table 1, respectively.
8
i¼1 j¼1
For a gas mixture at a specified temperature and pressure con-
dition, the reduced pressure and temperature can be calculated. 1 1=3 
1=3 3
The only unknown variable in Eq. (1) is the reduced volume Vr, vcij ¼ vci þ vcj (13)
8
which is solved using the Newton iteration method. In the iteration
process, the initial guess values Vr ¼ 0.08 and Vr ¼ pcV/RTc are
suggested for the liquid and gas phases, respectively. c. Stewart-Burkhardt-Voo (SBV) mixing rule (Sutton, 1985)

Table 1
Constants in Eqs. (2)e(4).

Constant Simple fluid Reference fluid Constant Simple fluid Reference fluid

b1 0.1181193 0.2026579 c3 0.0 0.016901

b2 0.265728 0.331511 c4 0.042724 0.041577
b3 0.154790 0.027655 d1  104 0.155488 0.48736
b4 0.30323 0.203488 d2  104 0.623689 0.074036
c1 0.0236744 0.0313385 b 0.65392 1.226
c2 0.0186984 0.0503618 g 0.060167 0.03754
652 W. Jia et al. / Journal of Natural Gas Science and Engineering 34 (2016) 650e656

Table 2 Table 4
Seven mixing rules for LK EoS. ARDs of different mixing rules.

Combinational mixing rule Tr > 1 and Pr > 5 Other regions Mixing rule Sample 1 Sample 2 Sample 3 Overall
region
LK 1.05 3.17 4.67 2.96
Tcm Pcm Tcm Pcm PK 1.88 1.85 1.40 1.71
SBV 1.47 1.45 0.80 1.24
LK LK
Kay þ WA 1.67 5.54 4.02 3.74
PK PK
LK þ PG 1.05 2.38 1.91 1.78
SBV SBV
PK þ PG 1.88 1.82 1.31 1.67
Kay þ WA Kay þ WA
SBV þ PG 1.45 1.31 0.74 1.17
LK þ PG LK PG LK LK
PK þ PG PK PG PK PK
SBV þ PG SBV PG SBV SBV
In this paper, we do not consider the H2S content in the gas, and
the H2S-related terms in Eqs. (21) and (22) should be removed.

K2 e. Prausnitz-Gunn mixing rule (API, 2005)

Tcm ¼ (14)
J
Prausnitz and Gunn proposed a mixing rule to calculate the
Tcm pseudocritical pressure under the condition of supercritical tem-
Pcm ¼ (15) peratures (Tr > 1) and high pressures (Pr > 5), as shown in Eq. (23).
J
Pn
" RTcm i¼1 zci
X
n   X
n  0:5 #2 pcm ¼ Pn (23)
1 Tci 2 Tci i¼1 xi vci Mi
J¼ xi þ xi (16)
3 Pci 3 Pci
i¼1 i¼1
where M is the molecular weight and zc is the critical compress-
! ibility factor.
X
n
Tci
K¼ xi (17) In the above equations, all basic parameters of each component,
0:5
Pci
i¼1 such as the molecular weight, critical volume, critical temperature,
critical pressure, critical compressibility factor and acentric factor,
are obtained from the API Technical Databook (API, 2005).
d. Kay's mixing rule and Wichert-Aziz Correlation (Kay þ WA) It should be noted that the Prausnitz and Gunn mixing rule is
(Sutton, 1985) valid for a limited temperature and pressure region and only for the
pcm calculation. Thus, the Tcm that corresponds to pcm should be
Kay's mixing rule is a mole fraction weighted method, as calculated using other mixing rules. Hence, we can develop three
expressed by Eqs. (18) and (19). new combinational mixing rules based on these mixing rules and
obtain seven mixing rules in total, as listed in Table 2. Using these
X
n
mixing rules and Eqs. (1)e(6), the compressibility factors of natural
Tcm ¼ xi Tci (18)
i¼1
gas with CO2 can be calculated.

X
n
Pcm ¼ xi Pci (19) 3. Evaluation of mixing rules
i¼1
To evaluate the mixing rules, the compressibility factors of three
Based on Kay's mixing rule, Wichert and Aziz suggest adjusting gas samples are tested by experimental methods. The compositions
the pseudocritical parameters using Eqs. (20) and (21) when the gas of the samples are listed in Table 3, which indicates that the mole
contains hydrogen and carbon dioxide.
0
Tcm ¼ Tcm  ε (20)

0
Pcm Tcm
0  
Pcm ¼ (21)
Tcm þ xH2 S 1  xH2 S ε

h 0:9  1:6 i h 0:5

ε ¼ 120 xH2 S þ xCO2  xH2 S þ xCO2 þ 15 xH2 S
 4 i
 x H2 S
(22)

Table 3
Compositions of three gas samples.

Component CO2 CH4 C2H6 C3H8 i-C4H10 i-C5H12 i-C6H14 C7H16þ

Sample 1 0.00 90.03 4.75 2.03 1.03 0.42 0.35 1.40

Sample 2 25.00 67.52 3.56 1.52 0.77 0.32 0.26 1.05
Sample 3 50.00 45.02 2.38 1.02 0.52 0.21 0.18 0.70
Fig. 1. Comparisons between the calculated z factors and the experimental values.
 W. Jia et al. / Journal of Natural Gas Science and Engineering 34 (2016) 650e656 653

Table 5
Compositions of natural-gas samples with CO2.

Component N2 CO2 CH4 C2H6 C3H8 iC4H10 nC4H10 iC5H12 i-C6H14 Data source

Sample 4 0.53 5.06 89.77 4.64 (Buxton and Campbell, 1967)

Sample 5 0.57 10.13 85.2 4.10
Sample 6 0.52 20.16 74.58 4.74
Sample 7 10.91 75.93 13.16
Sample 8 12.92 58.41 28.67

Sample 9 96.61 2.67 0.51 0.21 (Adisoemarta et al., 2004)

Sample 10 25 72.46 2.01 0.28 0.16
Sample 11 50 48.31 1.34 0.26 0.11
Sample 12 75.00 24.15 0.67 0.13 0.05

Sample 13 2.05 9.84 86.02 1.67 0.31 0.04 0.05 0.01 (Bian et al., 2012)
Sample 14 1.24 28.86 67.73 1.59 0.42 0.06 0.07 0.03
Sample 15 50.83 50.99 46.54 1.16 0.33 0.05 0.06 0.02 0.01

Sample 16 89.94 9.44 0.21 0.10 0.06 0.06 0.16 (Simon et al., 1977)

fraction of CO2 is 0e50%. Twenty-six data points for each sample Table 6 shows that the minimum RD is 0e0.45% and the
are collected at pressures from 3.45 to 34.47 MPa and temperatures maximum RD is 0.92e9.18% for all thirteen samples. The maximum
of 282.6 K and 377 K (Adisoemarta et al., 2004). RD may be caused by abnormal experimental data. For example, the
Seventy-eight set compressibility factors are calculated using LK experimental data of samples 10e12 in Fig. 2 are not sufficiently
EoS with four basic mixing rules and three combinational mixing smooth, which is not consistent with the reality. Unlike the
rules under identical pressure and temperature conditions to the experimental data, the calculations always give smooth results for
experiments. The relative deviation (RD) and average relative de- all samples, although the curves are notably complicated (sample
viation (ARD) between the experimental and calculated 16).
compressibility factors are defined in Eqs. (24) and (25), respec- Table 6 illustrates that the proposed method has satisfactory
tively, to quantitatively evaluate the mixing rule. accuracy in wide pressure and temperature ranges if the CO2 con-
tent is below 50%. For example, the maximum ARD is 1.56% for
Zcal  Zexp samples 4 to 11, which were in the pressure range of
RD ¼  100% (24)
Zexp 0.34e48.44 MPa and temperature range of 310.9e377.0 K. How-
ever, the deviations between calculations and experimental data
N
from Bian's article (Bian et al., 2012) are larger than 2.0%, possibly
1 X Zcali  Zexp i
ARD ¼  100% (25) because of the specific experimental methods.
N i¼1 Zexp i If the CO2 content is above 50%, larger deviations are observed.
For example, the ARDs of samples 12, 15 and 16 are 3.18%, 3.80% and
where N is the total number of data points; Zcali and Zexpi are the 3.02%, respectively. The ARD of sample 16 in this work is slightly
calculated and experimental compressibility factors, respectively. better than that in Simon's results (Simon et al., 1977), which are
The ARDs with regard to the combinations of LK EoS and 3.80% and 3.20% when the CSP method and BWR EoS are applied,
different mixing rules are listed in Table 4. The results show that the respectively.
Kay þ WA mixing rule gives the worst results, and the SBV þ PG The comparisons show that the proposed method is reliable for
combinational mixing rule has the best accuracy. When the PG the calculation of compressibility factors when the CO2 mole frac-
mixing rule is combined with the LK, PK or SBV mixing rules, the tion is below 50.0%. To enhance the accuracy of LK EoS and the
accuracy of the three original mixing rules is significantly corresponding mixing rules for CO2-content natural gas, additional
improved. The ARD of the SBV þ PG combinational mixing rule is improvement methods should be studied based on more experi-
1.17%. mental data in the future.
The comparisons between experimental and calculated values
using the SBV þ PG mixing rule are shown in Fig. 1. If all calculated
5. Conclusions
values are consistent with the experimental data, the scatter points
should lie on the 45 line on the plot. The plot demonstrates that
Based on the Lee-Kesler EoS, the compressibility calculation
most calculated values are notably consistent with the experi-
method for natural gas with CO2 was studied. Seven mixing rules
mental data. Thus, we suggest using the new SBV þ PG mixing rule
were applied to compute the pseudocritical temperature and
to predict the compressibility factors of natural gas with CO2. In the
pressure of the gas. We found that the combination of the SBV þ PG
following section, more experimental data are examined to validate
mixing rule and LK EoS could accurately predict the compressibility
the proposed method.
factors of natural gas with CO2. The new SBV þ PG mixing rule
suggests using SBV and PG mixing rules for the pseudocritical-
4. Results and discussion temperature and pressure computations, respectively, when the
reduced temperature is higher than one and the reduced pressure
In this section, the experimental compressibility factors of is higher than five. Otherwise, both pseudocritical temperature and
thirteen gas samples are collected from four studies to validate the pressure should be calculated according to the SBV mixing rule.
proposed combination of LK EoS and SBV þ PG mixing rule. The In total, 490 sets of experimental compressibility factors were
compositions are listed in Table 5. The mole fractions of CO2 in the applied to validate the proposed method, which covered wide
gas samples are 5.06e89.94%. The comparisons between the pressure and temperature ranges of 0.34e47.44 MPa and
experimental and calculated compressibility factors are shown in 273.2e377.0 K. The results showed that the maximum ARD is 1.56%
Fig. 2. The deviation analysis is listed in Table 6. when the mole fraction of CO2 is below 50%. Otherwise, the ARD
654 W. Jia et al. / Journal of Natural Gas Science and Engineering 34 (2016) 650e656

Fig. 2. Comparisons between the experimental and calculated compressibility factors.

 Fig. 2. (continued).

Table 6
Accuracy analysis of the calculation results.

Sample Pressure (MPa) Temperature (K) Data points xCO2 (%) Max. RD Min. RD ARD Data source

Sample 4 7.07e48.44 310.9e344.3 33 5.06 1.62 0.45 0.87 (Buxton and Campbell, 1967)
Sample 5 7.07e48.44 310.9e344.3 33 10.13 0.92 0.00 0.32
Sample 6 7.07e48.44 310.9e344.3 33 20.16 3.28 0.15 1.16
Sample 7 7.07e48.44 310.9e344.3 33 10.91 1.29 0.02 0.79
Sample 8 7.07e48.44 310.9e344.3 33 12.92 3.11 0.34 1.26

Sample 9 0.34e34.45 310.9e377.0 39 0 3.32 0.00 1.56 (Adisoemarta et al., 2004)

Sample 10 0.34e34.45 310.9e377.0 39 25 4.84 0.05 1.49
Sample 11 0.34e34.45 310.9e377.0 39 50 4.53 0.05 1.26
Sample 12 0.34e34.45 310.9e377.0 39 75 5.19 0.09 3.18

Sample 13 3e15 273.2e313.2 35 9.84 6.17 0.20 2.38 (Bian et al., 2012)
Sample 14 3e15 273.2e313.2 35 28.86 8.71 0.00 3.39
Sample 15 3e15 273.2e313.2 35 50.99 9.18 0.01 3.80

Sample 16 4.69e20.69 282.6e320.0 64 89.94 5.76 0.02 3.02 (Simon et al., 1977)
656 W. Jia et al. / Journal of Natural Gas Science and Engineering 34 (2016) 650e656

may be higher than 3.0%. The results of this paper provide guidance Gaudernack, B., Lynum, S., 1998. Hydrogen from natural gas without release of CO2
to the atmosphere. Int. J. Hydrogen Energy 23, 1087e1093.
and a useful method to calculate the compressibility of natural gas
Lee, B.I., Kesler, M.G., 1975. A generalized thermodynamic correlation based on
with CO2. three-parameter corresponding states. AlChE J. 21, 510e527.
Li, C., Jia, W., Wu, X., 2012. Temperature prediction for high pressure high tem-
Acknowledgments perature condensate gas flow through chokes. Energies 5, 670e682.
Li, C., Peng, Y., Dong, J., 2014. Prediction of compressibility factor for gas condensate
under a wide range of pressure conditions based on a three-parameter cubic
This study was funded by a sub-project of the National Science equation of state. J. Nat. Gas. Sci. Eng. 20, 380e395.
and Technology Major Project of China (No. 2016ZX05028-001- Moayyedi, M., Azamifard, A., Gharesheikhlou, A., Mosaferi, E., 2015. Constructing a
unique two-phase compressibility factor model for lean gas condensates.
006), the National Natural Science Foundation of China (No. Korean J. Chem. Eng. 32, 323e327.
51504026, No. 51474184.) and the Research Project of the Education Mohagheghian, E., Zafarian-Rigaki, H., Motamedi-Ghahfarrokhi, Y., Hemmati-
Department of Sichuan Province (No. 15ZB0050). Sarapardeh, A., 2015. Using an artificial neural network to predict carbon di-
oxide compressibility factor at high pressure and temperature. Korean J. Chem.
Eng. 32, 2087e2096.
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