Fluid Phase Equilibria, 25 (1986) 65-90 65

Elsevier Science Publishers B.V., Amsterdam - Printed in The Netherlands

COMPRESSED LIQUID DENSITIES OF PROPANE-NORMAL

BUTANE MIXTURES BETWEEN 10 AND 60°C AT PRESSURES UP
TO 9.6 MPa

WM. R. PARRISH
Phillips Petroleum Company, BartlesuiNe, OK 74004 (U.S. A)
(Received May 9, 1985; accepted in final form June 6, 1985)

ABSTRACT

Parrish, Wm. R., 1986. Compressed liquid densities of propane-normal butane mixtures
between 10 and 60°C at pressures up to 9.6 MPa. Fluid Phase Equilibria, 25: 65-90.

Compressed liquid densities for propane-normal butane mixtures are reported at six
temperatures between 10 and 60% For each isotherm, there are at least seven compositions
ranging between 10 and 75 mol% propane at pressures from near saturation up to 9.65 MPa.
The derived excess volumes are negative and represent a maximum of 0.5 percent of the
mixture volume at 1O’C. At 60°C, the excess volume can be up to 2.2% of the mixture
volume. In addition to the binary data, limited density measurements were made on ternary
mixtures containing up to 17 molX ethane.

INTRODUCTION

Although large quantities of Natural Gas Liquids (NGL) are bought and
sold on a volumetric basis, there is a surprising paucity of density data for
NGL-like mixtures at typical metering temperatures and pressures. The
purpose of this paper is to provide density data on mixtures of the primary
components of NGL-propane, normal butane and ethane. These data can
be used to evaluate existing density correlations and to develop new correla-
tions if necessary.
Nine sets of density data exist in the open literature for the propane-n
butane system. However, the data of Hiza et al., (1977), and Thompson and
Miller (1980) were at LNG temperatures. The data of Kay (1970) started at
71°C. Kahre (1973) obtained saturated liquid densities of five
propane-butane mixtures at 15.6 and 54.4OC. Luo and Miller (1981) gave
the liquid density for an 89 mol% propane mixture at 156°C and 0.90 MPa.
The saturated liquid data of Nysewander et al. (1940) include six mixtures
and cover the 37.8-138°C range. Thomas et al. (1963) presented saturated

0378-3812/86,‘$03.50 @ 1986 Elsevier Science Publishers B.V.

66

liquid density data for three mixtures in the 20-50°C range. However, only
two studies have been made in the compressed liquid region where most
metering occurs. Acosta (1975) measured compressed liquid densities for
three propane-butane mixtures at 37.8”C at pressures between 3.4 and 13.8
MPa. Tomlinson (1971) reported densities on a 99.11 molS propane mixture
at temperatures between 6.7 and 54.4”C at pressures up to 13.8 MPa.
This paper presents compressed liquid densities for propane-normal
butane mixtures at 10.0, 15.6, 26.7, 37.8, 48.9 and 6O.O”C.For each isotherm,
data were obtained for seven or more compositions ranging between 10 and
75 mol% propane at pressures from near saturation to 9.65 MPa. Also, a
limited amount of data were obtained for mixtures containing up to 17 mol%
of added ethane. Wherever possible, the experimental results are compared
with the data of other investigators.

EXPERIMENTAL APPARATUS AND PROCEDURE

Figure 1 shows a schematic of the experimental apparatus which is a slight

modification of the one described previously (Parrish, 1984). The system
contains a Mettler-Paar DMA 512 vibrating tube densitometer, a 100 cm3
positive displacement pump and a magnetically-driven mixing pump. These
components are immersed in a constant-temperature silicone oil bath which

.
+ BUTANE
IN

RELIEF
VALVE
+e

CONSTANT TEMPERATURE BATH

ARGOid Tb
IN VENT
VACUUM

Fig. 1. Schematic diagram of density apparatus.

 67

is maintained constant to better than k O.Ol”C. The bath temperature is

monitored using a calibrated quartz thermometer.
System pressure is determined by measuring the pressure needed to null a
differential pressure gauge having a resolution of 35 Pa. This nulling pressure
is read using a O-13.8 MPa bourdon gauge with a digital resolution of 70 Pa.
The gauge was calibrated against an oil dead-weight gauge prior to starting
the experiments.
Pure n-butane, propane and ethane are charged to the system from
spheres, each of which hangs from a 400 g balance. The balances have a
0.001 mg resolution over an 80 g span. Each sphere is in a heated oven. For
propane and butane, the lines come off the bottom of the sphere. The sphere
temperatures are maintained above the bath temperature to ensure that the
lines to the system stay full of liquid.
Because of the high vapor pressure of ethane at room temperature, the line
from the sphere comes off the top. This line is heat-traced to prevent
condensation. Also, the high pressure required using a 360 g sphere. There-
fore, to use this sphere with the balance, we immersed the sphere in silicone
oil. Since only differences in weights are measured, no correction for
buoyancy is needed.
Prior to, and following each run, the densitometer is calibrated at 1.4 MPa
increments from 1.4 to 9.65 MPa using pure argon and butane. Pure grade
argon (99.998% minimum) is used without further purification. Before being
used, Phillips Research Grade butane, with a stated purity of 99.9 mol%, is
put through two low pressure flashes to reduce the possibility of dissolved air
in the liquid phase.
To provide a check on the densitometer, density measurements were made
on pure propane along each isotherm. Phillips Research Grade propane with
a stated purity of 99.99 mol% was used. It had also been put through two
low pressure flashes before use.
After calibrating the densitometer, the system is charged with a weighed
amount of pure butane. To minimize thermal upset during filling, the fluid is
added slowly. Once the system is liquid-full, the flow is controlled by
adjusting the pressure with the 100 cm3 pump. The system is then charged
with the weight of propane necessary to produce the desired mixture.
At this point the mixing pump is turned on to homogenize the mixture.
Depending upon how much propane is added, it takes from 30 to 120 min
before the densitometer indicates that the system is well mixed. At this time
the pump is turned off and the pressure set by adjusting the 100 cm3 pump.
Within 10 min the system is completely stable and the density measurement
taken. The system pressure is then adjusted for the next pressure-density
data point. Upon completion of a set of measurements, propane or ethane is
added and the mixing/measurement cycle repeated.
68

DATA REDUCTION

As described previously (Parrish, 1984), the density at a given pressure

and temperature is given by

where or represents the response of the densitometer at pressure Pr for the

fluid with density pr. Then the density, p2, is computed at pressure P from a
densitometer esponse r2. The calibration constant, k, is obtained by run-
ning two flui d s with known density at 1.4 MPa increments between 1.4 and
9.65 MPa. Calibration constants are calculated at each pressure, assuming B
to be zero, and then averaged. Then, the constant B is found by linear
regression of eqn. (1) using known values for p, and p2 and measured values
of 7r and TV.Including the B term reduces a systematic error of up to 0.3%
to < 0.004% over the range of densities measured in this work. It is assumed
that the calibration constant is a function of temperature only. Although k
appears to be slightly pressure dependent, this effect would cause less than
0.005% error. This correction is, therefore, neglected.
All pure fluid densities are calculated using a modified BWR equation of
state (McCarty, 1980). The appendix gives the equation along with the
coefficients used for argon, ethane, propane, and n-butane.
To check for systematic errors in the measurements, densities of pure
propane are measured on each isotherm and compared with those calculated
from the BWR equation of state. Figure 2 shows the deviation between
measured and calculated densities from this work. Also included are com-

Fig. 2. Comparison between pure propane experimental densities and densities computed
using modified BWR equation of state. The data plotted include (+) this work, ( X) Ely and
Kobayashi (1978), (A) Haynes (1983), (O), Kratzke and Mliller (1985), (0) Thomas and
Harrison (1982) and (0) Tomlinson (1971).
 69

TABLE 1
Comparison between experimental and calculated densities for pure propane ’

Reference Number of Deviation

Points Average Maximum b, % Bias
Ely (1978) 64 0.03 - 0.09 0.00
Haynes (1983) 10 0.21 0.25 0.21
Kahre (1973) 4’ 0.04 0.07 0.03
Kratzke and Miiller (1985) 7 0.04 0.09 0.03
Luo and Miller (1981) 1 0.15 0.15 0.15
Thomas and Harrison (1982) 94 0.09 0.17 0.09
Thomas et al. (1963) 5 0.11 - 0.21 -0.11
Tomlinson (1971) 39 d 0.02 0.06 0.01
This work 76 0.09 0.11 0.09

a Densities calculated using modified BWR equation of state given in the Appendix.
b Deviation defined as ( pcalc- p,,)/p,,,,. Average error is root mean square average
whereas bias is simple arithmetic average.
’ This excludes the 54.4”C data point which has a deviation of 0.37%.
d This excludes the 26.7”C, 1.62 MPa data point which has a deviation of - 3.37%.

parisons with the propane data of Ely (1978), Haynes (1983), Kratzke and
Miiller (1985), Tomlinson (1971), and Thomas and Harrison (1982) in the
temperature and pressure range of this study. Table 1 summarizes the
comparison between the various studies. The data of Thomas et al. (1963)
was omitted because the data show a systematic error which increased to
over one percent at the higher temperatures.

ERROR ANALYSIS

The sources of uncertainty (defined as three times the estimated random

error plus the estimated possible systematic error) for the density are in the
temperature (k O.l’C), pressure ( f 13 kPa), and density of the calibration
fluids (+0.2%). Monte Carlo error analysis of the experiment indicates that
the estimated total uncertainty in the measured densities should be 0.2%.
In addition to the density there is an uncertainty in the mixture composi-
tion. An estimated total uncertainty of 0.006 g for each weighing translates
into a maximum uncertainty of 0.0002 in the mixture mole fraction.

DISCUSSION

Tables 2 and 3 present the propane-n-butane and the ethane-propane-

n-butane density data points taken at six temperatures as a function of
70

TABLE 2
Densities and excess volumes of propane-n-butane mixtures as a function of temperature
and pressure

Temperature Mole fraction Pressure Density Excess

(“C) propane (MPa) (gm cme3) volume a
(cm3 mol-‘)
10.00 0.1016 1.38 0.5856 -0.15
2.76 0.5878 -0.16
4.14 0.5896 -0.13
5.52 0.5915 -0.13
6.89 0.5933 -0.11
8.27 0.5951 -0.11
9.65 0.5968 - 0.10
0.2001 1.38 0.5797 - 0.26
2.76 0.5818 -0.26
4.14 0.5838 - 0.24
5.52 0.5857 - 0.22
6.89 0.5876 - 0.20
8.27 0.5894 -0.19
9.65 0.5912 -0.18
0.3001 1.38 0.5732 -0.34
2.76 0.5754 - 0.32
4.14 0.5775 - 0.30
5.52 0.5795 - 0.27
6.89 0.5814 - 0.26
8.27 0.5833 - 0.24
9.65 0.5851 - 0.22
0.3996 1.38 0.5664 - 0.38
2.76 0.5688 - 0.37
4.14 0.5709 - 0.34
5.52 0.5729 - 0.31
6.89 0.5749 - 0.29
9.65 0.5788 - 0.25
0.5012 1.38 0.5591 - 0.40
2.76 0.5615 - 0.38
4.14 0.5637 - 0.35
5.52 0.5658 - 0.31
6.89 0.5679 - 0.29
8.27 0.5699 - 0.27
9.65 0.5719 - 0.25
0.4969 1.38 0.5594 - 0.41
2.76 0.5618 - 0.39
4.14 0.5641 -0.36
5.52 0.5662 - 0.33
6.89 0.5683 - 0.30
8.27 0.5703 - 0.28
9.65 0.5723 - 0.27
0.6008 1.38 0.5513 -0.35
2.76 0.5537 - 0.32
4.14 0.5561 - 0.29
 71

TABLE 2 (continued)

Temperature Mole fraction Pressure Density Excess

(“C) propane (MPa) (gm cm-V volume a
(cm3 mol-‘)
10.00 0.6008 5.52 0.5583 - 0.27
6.89 0.5605 - 0.24
8.27 0.5626 - 0.22
9.65 0.5647 - 0.21
’ 0.7005 1.38 0.5434 - 0.32
2.76 0.5460 -0.30
4.14 0.5485 - 0.27
5.52 0.5508 - 0.24
6.89 0.5531 - 0.22
8.27 0.5553 - 0.21
9.65 0.5574 -0.19
0.7500 1.38 0.5391 - 0.27
2.76 0.5418 - 0.25
4.14 0.5443 - 0.22
5.52 0.5467 - 0.20
6.89 0.5491 -0.18
8.27 0.5513 -0.16
9.65 0.5534 -0.15
15.55 0.1020 1.38 0.5792 -0.14
2.76 0.5813 -0.13
4.14 0.5834 -0.12
5.52 0.5854 -0.11
6.89 0.5873 - 0.10
8.27 0.5892 - 0.09
9.65 0.5910 - 0.09
0.2022 1.38 0.5730 - 0.27
2.76 0.5753 - 0.26
4.14 0.5774 - 0.24
5.52 0.5794 - 0.22
6.89 0.5814 - 0.20
8.27 0.5834 -0.19
9.65 0.5853 -0.18
0.3087 1.38 0.5658 - 0.34
2.76 0.5682 - 0.33
4.14 0.5704 - 0.29
5.52 0.5726 - 0.27
6.89 0.5746 - 0.25
8.27 0.5766 - 0.23
9.65 0.5786 - 0.21
0.1017 0.28 0.5774 -0.14
0.34 0.5775 -0.15
72

TABLE 2 (continued)

Temperature Mole fraction Pressure Density Excess

(“C) propane (MPa) (gmcm
-3
) volume a
(cm3 mol-‘)

15.55 0.1017 0.41 0.5776 - 0.14

0.48 0.5777 - 0.14
0.55 0.5779 -0.14
0.62 0.5780 - 0.14
0.69 0.5781 -0.14
” 0.86 0.5783 - 0.14
1.03 0.5786 - 0.14
1.21 0.5789 -0.13
1.38 0.5792 -0.13
2.76 0.5813 -0.12
4.14 0.5834 -0.11
5.52 0.5854 -0.11
6.89 0.5873 - 0.10
8.27 0.5892 - 0.09
9.65 0.5910 - 0.08
0.2010 0.43 0.5715 - 0.29
0.48 0.5716 - 0.29
0.55 0.5717 - 0.29
0.62 0.5718 - 0.29
0.69 0.5720 - 0.29
0.86 0.5722 - 0.28
1.03 0.5725 - 0.28
1.21 0.5728 - 0.28
1.38 0.5731 -0.28
2.76 0.5754 - 0.26
4.14 0.5775 - 0.24
5.52 0.5796 - 0.22
6.89 0.5816 - 0.21
8.27 0.5835 -0.19
9.65 0.5854 -0.18
0.3009 0.46 0.5648 - 0.37
0.48 0.5649 - 0.37
0.55 0.5650 -0.37
0.62 0.5652 - 0.38
0.69 0.5653 -0.37
0.86 0.5656 - 0.37
1.03 0.5659 - 0.36
1.38 0.5665 - 0.36
2.76 0.5688 - 0.33
4.14 0.5710 - 0.31
5.52 0.5732 - 0.28
6.89 0.5752 - 0.26
8.27 0.5772 - 0.24
9.65 0.5792 - 0.23
 73

TABLE 2 (continued)

Temperature Mole fraction Pressure Density Excess

(“C) propane (MPa) (gm cmm3) volume a
(cm3 mol - ’ )
5.55 0.4009 0.50 0.5577 - 0.41
0.55 0.5578 - 0.41
0.62 0.5579 - 0.41
0.69 0.5581 - 0.41
0.86 0.5584 - 0.41
1.03 0.5587 -0.40
1.21 0.5590 - 0.40
1.38 0.5593 -0.39
2.76 0.5618 -0.35
4.14 0.5641 -0.33
5.52 0.5663 -0.29
6.89 0.5684 - 0.27
8.27 0.5705 -0.25
9.65 0.5725 -0.23
0.5005 0.47 0.5502 - 0.43
0.48 0.5502 - 0.43
0.55 0.5503 - 0.43
0.62 0.5505 - 0.43
0.69 0.5506 -0.42
0.86 0.5509 - 0.42
1.03 0.5513 - 0.41
1.21 0.5516 - 0.41
1.38 0.5519 - 0.41
2.76 0.5545 -0.36
4.14 0.5569 -0.33
5.52 0.5592 -0.30
6.89 0.5614 -0.27
8.27 0.5635 - 0.25
9.65 0.5656 - 0.23
0.5002 0.47 0.5502 - 0.43
0.48 0.5502 - 0.43
0.55 0.5504 - 0.43
0.62 0.5505 - 0.43
0.69 0.5506 -0.43
0.86 0.5510 - 0.42
1.03 0.5513 - 0.42
1.21 0.5516 - 0.41
1.38 0.5520 - 0.41
2.76 0.5545 - 0.37
4.14 0.5569 - 0.33
5.52 0.5592 -0.30
6.89 0.5614 -0.28
8.27 0.5636 -0.26
9.65 0.5657 -0.24
74

TABLE 2 (continued)

Temperature Mole fraction Pressure Density Excess

(“C) propane (MPa) (gm cmm3) volume a
(cm3 mol-‘)

15.55 0.5001 0.48 0.5501 - 0.41

0.55 0.5502 - 0.41
0.62 0.5503 - 0.40
0.69 0.5505 -0.40
0.86 0.5508 -0.39
1.03 0.5512 -0.39
1.21 0.5515 - 0.38
1.38 0.5518 - 0.38
2.76 0.5543 - 0.34
4.14 0.5568 -0.31
5.52 0.5591 - 0.28
6.89 0.5613 - 0.25
8.27 0.5635 - 0.23
9.65 0.5655 - 0.21
0.6007 0.51 0.5423 - 0.41
0.55 0.5424 - 0.41
0.62 0.5425 - 0.40
0.69 0.5426 - 0.40
0.86 0.5430 - 0.39
1.03 0.5433 - 0.39
1.21 0.5437 -0.38
1.38 0.5441 -0.38
2.76 0.5467 - 0.34
4.14 0.5492 - 0.31
5.52 0.5517 - 0.28
6.89 0.5540 - 0.25
8.27 0.5562 - 0.23
9.65 0.5584 - 0.21
0.7005 0.56 0.5341 -0.36
0.58 0.5342 - 0.36
0.62 0.5342 - 0.36
0.69 0.5344 -0.36
0.86 0.5348 - 0.36
1.03 0.5351 - 0.35
1.21 0.5355 - 0.35
1.38 0.5359 -0.34
2.76 0.5387 - 0.31
4.14 0.5414 - 0.27
5.52 0.5439 - 0.24
6.89 0.5463 - 0.22
8.27 0.5486 - 0.20
9.65 0.5509 -0.18
0.6998 0.57 0.5344 -0.39
0.62 0.5345 -0.39
 75

TABLE 2 (continued)

Temperature Mole fraction Pressure Density Excess

(“C) propane (MPa) (pm cmm3) volume ’
(cm3 mol-‘)
15.55 0.6998 0.69 0.5346 - 0.39
0.86 0.5350 -0.39
1.03 0.5354 -0.38
1.21 0.5357 -0.38
1.38 0.5361 - 0.38
2.76 0.5389 - 0.33
4.14 0.5416 - 0.30
5.52 0.5441 - 0.27
6.89 0.5465 - 0.25
8.27 0.5489 - 0.23
9.65 0.5511 - 0.21
0.7518 0.60 0.5301 - 0.38
0.61 0.5301 - 0.37
0.62 0.5301 - 0.38
0.69 0.5303 - 0.37
0.86 0.5307 -0.37
1.03 0.5310 - 0.36
1.21 0.5314 -0.36
1.38 0.5318 - 0.36
2.76 0.5347 - 0.32
4.14 0.5374 - 0.29
5.52 0.5400 - 0.26
6.89 0.5425 -0.24
8.27 0.5449 - 0.22
9.65 0.5472 - 0.20
26.67 0.1043 1.38 0.5665 - 0.24
2.76 0.5690 - 0.24
4.14 0.5713 - 0.22
5.52 0.5735 -0.19
6.89 0.5757 -0.19
8.27 0.5778 -0.18
9.65 0.5798 -0.16
0.1998 1.38 0.5599 -0.35
2.76 0.5625 - 0.32
4.14 0.5649 - 0.28
5.52 0.5673 - 0.26
6.89 0.5695 - 0.24
8.27 0.5716 - 0.22
9.65 0.5737 - 0.20
0.2999 1.38 0.5531 - 0.49
2.76 0.5558 - 0.46
4.14 0.5584 - 0.42
5.52 0.5608 - 0.38
6.89 0.5631 -0.35
76

TABLE 2 (continued)

Temperature Mole fraction Pressure Density Excess

(“C) propane (MPa) (gm cmp3) volume a
(cm3 mol-‘)
26.67 0.2999 8.27 0.5653 -0.32
9.65 0.5675 - 0.29
0.4002 1.38 0.5457 - 0.57
2.76 0.5486 - 0.54
4.14 0.5513 - 0.48
5.52 0.5538 - 0.44
6.89 0.5562 -0.39
8.27 0.5585 - 0.36
9.65 0.5608 - 0.33
0.5000 1.38 0.5378 - 0.60
2.76 0.5408 - 0.54
4.14 0.5437 - 0.49
5.52 0.5463 - 0.43
6.89 0.5488 - 0.39
8.27 0.5512 - 0.36
9.65 0.5536 -0.33
0.5001 1.38 0.5383 - 0.69
2.76 0.5414 - 0.64
4.14 0.5442 - 0.57
5.52 0.5467 - 0.51
6.89 0.5493 - 0.48
8.27 0.5517 -0.44
9.65 0.5540 - 0.40
0.6122 1.38 0.5287 - 0.62
2.76 0.5319 - 0.56
4.14 0.5349 -0.50
5.52 0.5377 - 0.45
6.89 0.5404 - 0.41
8.27 0.5429 -0.37
9.65 0.5454 - 0.35
0.7002 1.38 0.5211 - 0.59
2.76 0.5245 -0.53
4.14 0.5277 - 0.48
5.52 0.5306 - 0.44
6.89 0.5334 - 0.39
8.27 0.5360 - 0.35
9.65 0.5386 - 0.33
0.7501 1.38 0.5165 - 0.53
2.76 0.5200 - 0.48
4.14 0.5232 - 0.43
5.52 0.5262 - 0.38
6.89 0.5291 - 0.33
8.27 0.5318 - 0.31
9.65 0.5345 - 0.28
 77

TABLE 2 (continued)

Temperature Mole fraction Pressure Density Excess

(“C) propane (MPa) (gm cme3) volume a
(cm3 mol-‘)
37.78 0.0996 1.38 0.5532 - 0.29
2.76 0.5561 - 0.28
4.14 0.5587 - 0.25
5.52 0.5613 - 0.23
6.89 0.5637 - 0.20
8.27 0.5660 -0.17
9.65 0.5683 -0.17
0.1999 1.38 0.5464 - 0.54
2.76 0.5494 - 0.48
4.14 0.5522 - 0.43
5.52 0.5548 - 0.39
6.89 0.5574 -0.36
8.27 0.5598 -0.33
9.65 0.5621 - 0.30
0.3001 1.38 0.5392 - 0.76
2.76 0.5424 - 0.68
4.14 0.5453 - 0.60
5.52 0.5481 -0.54
6.89 0.5507 - 0.50
8.27 0.5532 - 0.45
9.65 0.5557 - 0.42
0.4022 1.38 0.5313 - 0.90
2.76 0.5346 - 0.80
4.14 0.5377 - 0.71
5.52 0.5407 - 0.64
6.89 0.5434 - 0.57
8.27 0.5460 - 0.52
9.65 0.5486 - 0.48
0.5001 1.38 0.5232 - 0.97
2.76 0.5267 - 0.85
4.14 0.5300 - 0.75
5.52 0.5330 - 0.67
6.89 0.5359 - 0.60
8.27 0.5387 - 0.54
9.65 0.5414 - 0.50
0.5109 1.38 0.5227 -1.06
2.76 0.5263 - 0.94
4.14 0.5296 - 0.83
5.52 0.5326 - 0.75
6.89 0.5355 - 0.68
8.27 0.5383 - 0.62
9.65 0.5410 - 0.58
78

TABLE 2 (continued)

Temperature Mole fraction Pressure Density Excess

(“C) propane (MPa) (gm cmw3) volume a
(cm3 mol-‘)

37.78 0.6000 1.38 0.5146 -1.02

2.76 0.5184 - 0.90
4.14 0.5218 - 0.79
5.52 0.5251 - 0.71
6.89 0.5282 - 0.63
8.27 0.5311 - 0.58
9.65 0.5338 - 0.53
0.7000 1.38 0.5050 - 0.93
2.76 0.5091 -0.81
4.14 0.5129 - 0.71
5.52 0.5163 - 0.63
6.89 0.5196 - 0.56
8.27 0.5226 - 0.50
9.65 0.5255 - 0.46
0.7501 1.04 0.4988 - 0.87
1.10 0.4990 - 0.86
1.17 0.4992 - 0.84
1.24 0.4994 - 0.84
1.31 0.4996 - 0.83
1.38 0.4999 - 0.82
2.76 0.5041 - 0.70
4.14 0.5080 - 0.61
5.52 0.5116 - 0.53
6.89 0.5149 - 0.48
8.27 0.5181 - 0.43
9.65 0.5211 - 0.39
48.89 0.1003 1.37 0.5388 - 0.41
2.76 0.5421 - 0.34
4.14 0.5452 - 0.30
5.52 0.5482 - 0.26
6.89 0.5510 - 0.23
8.27 0.5536 - 0.21
9.65 0.5562 -0.19
0.2001 1.38 0.5315 - 0.75
2.76 0.5350 - 0.64
4.14 0.5383 - 0.55
5.52 0.5414 - 0.48
6.89 0.5443 - 0.42
8.27 0.5471 - 0.38
9.65 0.5498 - 0.35
0.3004 1.38 0.5235 - 1.01
2.76 0.5273 -0.84
4.14 0.5308 - 0.72
5.52 0.5340 - 0.62
 79

TABLE 2 (continued)

Temperature Mole fraction Pressure Density Excess

(“C) propane (MPa) (gm cme3) volume a
(cm3 mol-‘)
48.89 0.3004 6.89 0.5371 - 0.55
8.21 0.5400 - 0.48
9.65 0.5428 - 0.44
0.4003 1.38 0.5152 - 1.23
2.76 0.5192 -1.02
4.14 0.5229 - 0.86
5.52 0.5263 - 0.74
6.89 0.5296 - 0.65
8.27 0.5326 - 0.58
9.65 0.5356 -0.53
0.5004 1.38 0.5062 - 1.35
1.55 0.5067 - 1.30
1.72 0.5073 - 1.27
1.90 0.5078 -1.24
2.07 0.5084 - 1.21
2.76 0.5105 -1.09
4.14 0.5144 - 0.92
5.52 0.5181 - 0.79
6.89 0.5215 - 0.69
8.27 0.5248 - 0.62
9.65 0.5278 - 0.55
0.5002 1.38 0.5060 -1.31
2.76 0.5104 - 1.07
4.14 0.5143 - 0.90
5.52 0.5179 - 0.76
6.89 0.5214 - 0.66
8.27 0.5246 -0.58
9.65 0.5276 -0.51
0.6003 1.38 0.4966 - 1.37
2.76 0.5012 -1.11
4.14 0.5055 - 0.92
5.52 0.5093 -0.78
6.89 0.5130 - 0.67
8.27 0.5164 - 0.58
9.65 0.5196 - 0.52
0.7002 1.38 0.4859 - 1.22
1.72 0.4872 -1.13
2.76 0.4910 - 0.95
4.14 0.4956 - 0.77
5.52 0.4998 - 0.65
6.89 0.5037 - 0.55
8.27 0.5073 - 0.47
9.65 0.5108 - 0.41
80

TABLE 2 (continued)
Temperature Mole fraction Pressure Density Excess
(“C) propane (MPa) (pm cme3) volume a
(cm3 mol-‘)
48.89 0.7500 1.38 0.4804 - 1.12
1.45 0.4807 - 1.10
1.52 0.4810 -1.09
1.59 0.4813 - 1.08
1.65 0.4816 - 1.07
1.72 0.4819 - 1.06
1.90 0.4825 - 1.01
2.07 0.4832 - 0.99
2.41 0.4845 - 0.93
2.76 4.4858 - 0.88
4.14 0.4907 - 0.73
5.52 0.4951 - 0.60
6.89 0.4991 - 0.50
8.27 0.5029 - 0.43
9.65 0.5064 - 0.38
60.00 0.0990 1.38 0.5236 - 0.62
2.76 0.5276 - 0.48
4.14 0.5312 - 0.39
5.52 0.5346 - 0.33
6.89 0.5378 - 0.28
8.27 0.5409 - 0.24
9.65 0.5438 - 0.22
0.2033 1.38 0.5155 - 1.25
2.76 0.5197 - 0.96
4.14 0.5236 - 0.78
5.52 0.5272 - 0.66
6.89 0.5306 - 0.56
8.27 0.5338 - 0.49
9.65 0.5368 - 0.44
0.2996 1.38 0.5073 - 1.70
2.76 0.5118 - 1.30
4.14 0.5159 - 1,04
5.52 0.5197 - 0.86
6.89 0.5233 - 0.74
8.27 0.5267 -0.64
9.65 0.5298 - 0.57
0.3991 1.38 0.4981 - 2,07
2.76 0.5030 - 1.56
4.14 0.507s - 1.24
5.52 0.511s - 1.02
6.89 0.5153 - 0,86
8.27 0.5189 = 0.75
9.65 0.5222 - 0.66
 81

TABLE 2 (continued)

Temperature Mole fraction Pressure Density Excess

(“C) propane (MPa) (gm cme3) volume ’
(cm3 mol - ’ )
60.00 0.4997 1.38 0.4880 - 2.29
2.76 0.4934 - 1.69
4.14 0.4982 - 1.32
5.52 0.5026 -1.07
6.89 0.5066 - 0.90
8.27 0.5104 - 0.77
9.65 0.5140 - 0.67
0.6007 1.72 0.4787 -2.18
2.16 0.4831 -1.73
4.14 0.4884 - 1.34
5.52 0.4932 -1.09
6.89 0.4975 - 0.90
8.27 0.5016 - 0.77
9.65 0.5054 - 0.67
0.7002 1.72 0.4673 - 2.09
2.76 0.4722 - 1.64
4.14 0.4781 -1.25
5.52 0.4833 -1.00
6.89 0.4880 -0.83
8.27 0.4923 - 0.70
9.65 0.4964 -0.60
0.7504 1.72 0.4610 - 1.95
2.07 0.4629 -1.78
2.76 0.4663 -1.52
4.14 0.4725 -1.15
5.52 0.4780 - 0.91
6.89 0.4830 - 0.75
8.27 0.4875 -0.63
9.65 0.4916 -0.54
0.4999 1.38 0.4881 - 2.33
2.76 0.4935 -1.72
4.14 0.4983 -1.35
5.52 0.5027 -1.10
6.89 0.5068 -0.93
8.27 0.5105 -0.80
9.65 0.5141 - 0.70

a The excess volumes are tabulated to 0.01 cm3 mol-’ to show trends only. Uncertainty in
the pure fluid molar volumes is - 0.2 cm3 mol- ‘.
82

TABLE 3
Densities and excess volumes of ethane-propane- n-butane mixtures as a function of temper-
ature and pressure

Temperature Mole fraction Mole fraction Pressure Density Excess

(“C) ethane propane (MPa) (gm cm-‘) volume a
(cm3 mol-‘)
15.55 0.0523 0.4743 0.87 0.5449 - 129.86
1.03 0.5452 - 106.73
1.21 0.5456 - 89.25
1.38 0.5459 - 76.07
2.76 005486 - 1.14
4.14 0.5511 -0.85
5.52 0,5535 - 0.70
6.89 0.5558 - 0.60
8.27 0.5580 - 0.53
9.65 0.5602 - 0.47
0.0470 0.7165 0.69 0.5247 - 150.58
0.71 0.5247 - 145.49
0.86 0.5251 - 117.74
1.03 0,5255 - 95.79
1.21 0.5259 - 80.03
1.38 0.5263 - 68.21
2.76 0.5293 - 0.89
4.14 0.5321 - 0.64
5.52 0.5348 - 0.52
6.89 0.5374 - 0.44
8.27 0,5398 - 0.37
9.65 0.5422 - 0.33
0.1096 0.6694 0.82 0.5181 - 290.43
0.86 0.5183 - 274.16
1.03 0.5187 - 222.99
1.21 0.5191 - 186.36
1.38 0.5195 - 158.78
2.76 0.5227 - 1.78
4.14 0.5257 - 1.24
5.52 0.5285 - 0.98
6.89 0.5311 - 0.81
8.27 0.5337 - 0.70
9.65 0.5361 -0.61
0.1529 0.6368 0.94 0.5135 - 346.28
1.03 0.5138 - 310.98
1.21 0.5143 - 259.88
1.38 0.5147 - 221.40
2.76 0.5180 - 2.39
4.14 0.5211 - 1.64
5.52 0.5240 - 1.29
6.89 0.5267 - 1.07
 83

TABLE 3 (continued)

Temperature Mole fraction Mole fraction Pressure Density Excess

(“C) ethane propane (MPa) (gm cmm3) volume a
(cm3 mol-‘)
0.5293 - 0.92
9.65 0.5319 - 0.80
26.68 0.0505 0.7122 1.38 0.5100 - 77.56
2.76 0.5137 - 30.75
4.14 0.5171 - 12.54
5.52 0.5202 - 0.92
6.89 0.5232 - 0.70
8.27 0.5261 -0.58
9.65 0.5288 - 0.49
37.77 0.0517 0.4743 1.38 0.5166 - 84.20
2.76 0.5203 - 34.85
4.14 0.5237 - 17.20
5.52 0.5269 - 3.63
6.89 0.5300 - 1.57
8.27 0.5329 - 1.23
9.65 0.5357 - 1.04
0.0554 0.7085 1.38 0.4929 - 89.86
2.76 0.4973 - 36.99
4.14 0.5014 - 18.13
5.52 0.5052 - 3.61
6.89 0.5088 - 1.43
8.27 0.5121 - 1.08
9.65 0.5152 -0.88
0.1003 0.6749 1.38 0.4864 - 161.71
1.55 0.4870 - 140.66
1.72 0.4876 - 123.81
2.07 0.4888 - 98.40
2.76 0.4912 - 66.22
4.14 0.4955 - 32.18
5.52 0.4995 - 6.01
6.89 0.5032 -2.11
8.27 0.5066 - 1.50
9.65 0.5099 - 1.19
48.88 0.0539 0.4734 1.93 0.5006 - 61.95
2.07 0.5011 - 56.89
2.76 0.5033 - 39.07
4.14 0.5075 - 20.69
5.52 0.5114 - 10.40
6.89 0.5150 - 3.41
8.27 0.5184 - 1.87
9.65 0.5216 - 1.41
0.1007 0.4631 1.72 0.4922 - 131.68
2.07 0.4935 - 105.33
2.76 0.4958 - 72.13
4.14 0.5003 - 37.91
5.52 0.5044 - 18.78
84

TABLE 3 (continued)

Temperature Mole fraction Mole fraction Pressure Density Excess

(“C) ethane propane (MPa) (gm cmm3) volume a
(cm3 mol-‘)
0.1007 0.4631 6.89 0.5083 - 5.80
8.27 0.5118 - 2.99
9.65 0.5152 -2.19
0.1729 0.4260 2.41 0.4839 - 147.30
2.76 0.4855 - 122.87
4.14 0.4904 - 64.31
5.52 0.4949 - 31.60
6.89 0.4990 - 9.39
8.27 0.5028 - 4.64
9.65 0.5063 - 3.31
0.0510 0.7117 2.07 0.4762 - 53.49
2.76 0.4790 - 36.64
4.14 0.4842 - 19.29
5.52 0.4889 - 9.56
6.89 0.4931 - 2.95
8.27 0.4970 - 1.52
9.65 0.5007 - 1.10
0.1088 0.6684 2.41 0.4693 - 92.45
2.76 0.4709 - 77.08
4.14 0.4765 - 40.24
5.52 0.4815 - 19.66
6.89 0.4860 - 5.70
8.27 0.4901 - 2.72
9.65 0.4940 -1.88
60.00 0.0543 0.7097 2.07 0.4533 - 60.05
2.76 0.4572 - 41.55
4.14 0.4640 - 22.73
5.52 0.4700 - 12.85
6.89 0.4753 - 6.45
8.27 0.4801 - 2.90
9.65 0.4845 -1.71
0.1077 0.6696 3.10 0.4501 - 68.71
4.14 0.4557 - 43.97
5.52 0.4622 - 24.62
6.89 0.4679 - 12.09
8.27 0.4730 - 5.17
9.65 0.4777 - 2.90

a The excess volumes are tabulated to 0.01 cm3 mol-’ to show trends only. Uncertainty in
the pure fluid molar volumes is - 0.2 cm3 mol-‘.
 85

0” -0.6
w

0 0.2 0.4 0.6 0.8 1.0

MOLE FRACTION PROPANE

Fig. 3. Excess volume of propane-butane mixtures at 1000 psia as a function of composition

and temperature. Open symbols denote this work while closed symbols represent data of
Acosta (1975). The bar (I) in the lower left corner corresponds to 0.1% in mixture molar
volume.

pressure and composition. Also included in the table are excess volumes VE,
calculated using

where V,,, , and V; represent the molar volumes of the mixture and the pure
fluid i, respectively, all at the same temperature and pressure; xi is the
mixture mole fraction of component i. All pure fluid volumes in this paper
were calculated using the BWR equation given in the Appendix. It should be
noted that there is a systematic deviation of 0.08-0.11 cm3 mol-’ between
the calculated and measured propane molar volumes. (There is no systematic
deviation for the butane data because calculated values were used in the
calibration of the densitometer.) This deviation has the effect of reducing the
size of excess volume and introduces a possible bias in the excess volumes of
up to 0.1 cm3 mol -‘. Hence, the values are tabulated to 0.01 cm3 mol-’ to
indicate trends only.
Figure 3 shows excess volumes for the propane-butane system at 6.90
MPa as a function of composition at three temperatures. The figure shows a
good comparison between this work and Acosta’s data (1975) which had a
reported estimated uncertainty of 0.4%. At this pressure the maximum error
in assuming the system to be ideal ( VE = 0) would be -=z1% over the entire
composition range.
One would expect the minimum in the excess volume to occur at a
propane mole fraction of 0.6-0.7 instead of near equimolar as indicated in
Fig. 3. Correcting for the possible bias in the propane molar volumes
86

I
! I I I I I I I, I / I1
2.0 4.0 6.0 8.0 10.0 12.0 14.0
PRESSURE, (MPa)

Fig. 4. Equimolar excess volumes for the propane-butane system as a function of pressure
and temperature. Open symbols represent this work. The symbol (A) denotes the saturated
liquid data point of Kahre (1973) for a 0.4830 mole fraction propane mixture. Other closed
symbols indicate Acosta’s (1975) data for a 0.50191 mole fraction propane mixture. The bar
(I) represents - 0.1% in molar volume.

mentioned above shifts the minimum to between 0.6 and 0.7 mole fraction.
However, the correction is unjustifiable since it is one-half of the estimated
uncertainty in the actual data.

0.1 -
0.0 0.50 0.10 0.15
MOLE FRACTION ETHANE IN 3/ 1
PROPANE/BUTANE MIXURE

Fig. 5. Excess volume at 60°F of an ethane-propane-butane mixture as a function of ethane

content and pressure. On an ethane-free basis the mixture contains 0.7518 mole fraction
propane.
 87

Figure 4 presents the effect of temperature and pressure on the equimolar

excess volume. As would be expected, the excess volume increases with
increasing temperature and decreasing pressure. Also included are the
equimolar excess volumes calculated from Acosta’s (1975) data and Kahre’s
(1973) data at saturation. Agreement with Kahre’s (1973) saturated liquid
value is very good, and while Acosta’s (1975) data shows some scatter at
higher pressures, they are still within the 0.4% uncertainty claimed by the
author.
Whereas the propane-butane system is nearly ideal, the system containing
ethane is far from ideal. Figure 5 illustrates the effect of ethane content and
pressure on the excess volume when the ethane-free mixture contains 0.7518
mole fraction propane. One obtains nearly the same change in excess volume
as a function of ethane content for the equimolar system on an ethane-free
basis. It is somewhat unrealistic even to calculate excess volumes for a
mixture containing a gaseous component such as ethane at the lower
pressures. However, the excess volumes seem reasonable at 2.8 MPa, even
though the vapor pressure of ethane is roughly 3.4 MPa at 15.6OC.

CONCLUSIONS

Compressed liquid density data were obtained for binary mixtures of

propane and normal butane and for some ternary mixtures containing
ethane, propane and n-butane. The data cover the typical temperatures and
pressures encountered in metering of NGL streams. These data should be
useful for evaluating existing density correlation methods used for NGL-like
mixtures. Also, they should be useful in testing new density models and
liquid theories.

ACKNOWLEDGMENT

J.L. Durm provided excellent technical support by constructing the ap-

paratus and obtaining the data reported here.

APPENDIX

To compute the pure fluid densities needed in this work we used the
32-term modified equation of state (McCarty, 1980). The mathematical form
of the equation is
P = pRT+ p’(G(l)T+ G(2)T”‘+ G(3) + G(4)/T+ G(5)/T2)

+p3(G(6)T+ G(7) + G@)/T+ G(9)/T2)

TABLE Al

Coefficients for calculating pure fluid densities using eqn. Al

Ethane a Propane a Argon a n-Butane b

G(1) 1.88506940933E- 03 - 6.70761309910E - 04 343426572424E - 03 1.53740104603E - 02

wj 3.33782436373E - 01 9.21772888298E - 01 5.78570366814E - 02 -1.6098003~118-01
G(3) - 1.25068032925E+ 01 - 3.02645199385E+ 01 - 2.69824708123E+ 00 - 9.79782459OlOE -I-00
G(4) 1.25534652639E + 03 3.88806890775E+ 03 1.64816552853E+02 4.99660674504E + 02
G(5) - 2.3836507119OE+ 05 - 7.42816624597E+ 05 - 1.28494724204E + 04 -l.O2115607687E+O6
G(6) 1.50425791494E-04 - l.l0482897982E-04 - 3.26364908947E- 04 2.36032147756E - 03
G(7) 3.82510906119E- 01 8.16694426032E-01 246294701908E - 01 -1.37475757093E+OO
G(8) -1.91836120580E+02 - 3.71129992879ElO2 - 6.95854456978E+ 01 - 9.07038733865E + 02
G(9) 1.38111709155E+O4 8.39414320969E+ 04 1.919615693978 + 04 3.85421748213E+05
G(L0) 2.58975112878E-05 6.73749481858E - 05 1.66039098056E - 05 - 3.494537107OOE- 05
G(l1) - L50561848757E - 02 - l.l9076170729E-02 - 1.08603163454E - 02 1.57361122714E-01
G(L2) - 2.56565287319E+ 00 - 3.68723981025E+ 01 3_32317590049E+ 00 1.023014740688 + 02
G(13) 9.16028091065E - 04 4.43982040167E- 03 2.17763619471E - 05 1.82335737331E-02
G(L4) 5.52522627849E - 02 3.40582644423E- 01 5.16150858128E- 03 - 4.04114307787E + 00
G(l5) - 3.64493951450E + 00 - l.l1892692666E+Ol - l.l3667054073E+OO 1.87979855783E + 00
G(l6) - 1.80161508795E-03 - 1.53644965463E- 02 -290185176189E-04 3.620887950408 - 01
G(17) 4.08677752238E - 06 2.08523231528E- 04 3.78982896981E - 06 - 7.38762248266E - 03
G(l8) 1.51383996553E-02 4.07673861569E-03 1.10304897910E - 03 - 2.18618590563E +00
G(l9) - 3.92859631208E-04 4.576413753818-04 - 1.46740929430E - 05 l.l8802729027E+OO
G(20) 8.20224567729E + 04 1.84402735334E+05 - 1.14796107162E + 04 7.06854198713E + 05
Cw) - 1.47417650202E+07 -4.763781161238+07 - 3.93933129638E+ 05 - 2.19469885796E+ 08
G(22) 5222275184OlE+02 1.53437834289E+ 03 - 9.96200843073E + 01 - 1.82454361268E + 04
G(23) 3.01705434005E + 07 3.43016311993E+08 - 1.85753470460E + 04 2.067903772778+ 09
Gv4) 1.67947683870E + 00 3.5271908939OE+ 01 - 2.93934838711E- 01 l.l1757550145E+02
G(25) 164636759854E+03 4.99822902697E + 03 1.64085880868E + 01 5.58779925986E304
G(26) 3.88562230575E - 02 6.15066508008E-01 - 4.04471742294E - 04 - 1.59579054026E + 01
~(27) - 2.50583522815E+O3 -l.O2496516571E+05 - 2.08200071660E+ 00 - 1.48034214622E -I-06
G(28) 8.5903352914OE -05 - 8.1716149102OE-03 - 5.49693206496E - 07 - 2.45206328201E - 01
Gt29) 2.4728508265OE - 02 6.23704452977E3 00 7.51374052777E-05 2.18305259309E + 02
G(30) - 2.94415158564E - 07 451237597357E-06 -286674255182E - 10 - 9.23990627338E- 05
G(31) 1.96471554077E-04 - 1.48764254246E- 02 - 6.30037228668E- 08 - 2.05267776639E + 00
G(32) 3.51922898193E - 03 8.872052517828- 01 2.528741344OPE - 06 3.87639044820E + 01
Gamma 2.1626298OOOOE - 02 4.-E - 02 5.5-E-03 6.508tHNOOOOE - 02

a Coefficients from Ely (personal communication, 1982).

.r. fiv -:--A- C*nrn Flv (nersonal communication, 1984).
 89

+ p”(G(lO)T + G(ll) + G(12)/T) + ~‘(G(13))

+p6(G(14)/T+ G(15),‘T2) + p7(G(16)/T)
+p8(G(17)/T+ G(18)T’) + p9(G(19)/T2)
+ p3(G(20)/T2 + G(21)/T3) exp( yp2)
+ p5(G(22)/T2 + G(23)/T4) exp( yp”)

+p7(G(24)/T2 + G(25)/T3) exp( yp2)

+ p9(G(26)/T2 + G(27)/T4) exp( yp2)
+ $l(G(28)/T2 + G(29)/T3) exp( yp’)

+ a3(G(30)/T2 + G(31)/T3) + G(32)/r4) exp( yp2) (Al)

where P, p, R and T represent pressure, density, gas constant and absolute
temperature, respectively. Table Al lists the coefficients used for computing
the densities of pure argon, ethane, propane, and normal butane. These
coefficients were obtained by PVT data simultaneously with other properties
including heat capacities. Units for the ethane, propane, and butane equa-
tion are bar (10’ Pa), mol 1-l and Kelvin. For argon, they are atmospheres
(0.01325 MPa), mol 1-l and Kelvin.

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