Fluid Phase Equilibria 207 (2003) 143154

Experimental study on the solubility of natural gas components

in water with or without hydrate inhibitor
Lu-Kun Wang, Guang-Jin Chen, Guang-He Han, Xu-Qiang Guo, Tian-Min Guo
High Pressure Fluid Phase Behavior & Property Research Laboratory, University of Petroleum,
P.O. Box 902, Beijing 100083, China
Received 30 September 2002; accepted 6 January 2003

Abstract
Solubility of methane, ethane and a (methane + ethane) gas mixture in pure water/alcohols (methanol/ethylene
glycol) as well as aqueous solutions of methanol/ethylene glycol have been measured systematically in the pressure
range of 2.0040.00 MPa for methane and the (methane + ethane) gas mixture, 0.504.50 MPa for ethane, and the
temperature range was 283.2303.2 K.
2003 Elsevier Science B.V. All rights reserved.
Keywords: Solubility; Natural gas component; Methanol; Ethylene glycol

1. Introduction
The solubility of natural gas components methane and ethane in pure water has been studied extensively
in the past few decades [114]. However, due to their extremely low solubility, the reported data are not
in good consistency. For hydrate inhibitor containing systems, limited data were reported by Battino [15],
Fauser [16], Hong et al. [17] and Schneider [18] for methanemethanol system; Schneider [18], Hayduk
[19], Yaacobi and Ben-Naim [20], McDaniel [21], Ma and Kokl [22], Ohgaki et al. [23] and Weber [24]
for the ethanemethanol system. Furthermore, similar solubility data in pure ethylene glycol and aqueous
solutions of alcohols as well as the solubility data for gas mixtures were scarcely reported in the literature.
In conventional hydrate formation calculations, the effect of gas solubility in the aqueous phase are
often neglected, however, for accurate prediction of hydrate formation conditions, its effect should not
be overlooked, especially for the inhibitor containing systems.
The major objective of this work is to expand the gas solubility data base for hydrate inhibitor containing
systems which are important for testing/improving hydrate models.

Corresponding author. Tel.: +86-10-62340132; fax: +86-10-62340132.

E-mail address: guotm@a-1.net.cn (T.-M. Guo).
0378-3812/03/$ see front matter 2003 Elsevier Science B.V. All rights reserved.
doi:10.1016/S0378-3812(03)00009-8

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L.-K. Wang et al. / Fluid Phase Equilibria 207 (2003) 143154

Fig. 1. Schematic of the ROP PVT unit: (1) air bath; (2) pressure controller; (3) primary cell; (4) magnetic stirrer; (5) temperature
controller; (6) secondary cell.

Fig. 2. Schematic of the RUSKA PVT unit: (1) motor; (2) oil bath; (3) equilibrium cell; (4) sampling system; (5) pressure gauge;
(6) temperature controller; (7) vacuum pump; (8) pressure-stabilizing cylinder; (9) electric metering pump; (10) gas booster;
(11) ethane cylinder.

L.-K. Wang et al. / Fluid Phase Equilibria 207 (2003) 143154

145

2. Experimental section
2.1. Materials
Analytical grade methane (99.99 vol.%) and ethane (99.95 vol.%) were supplied by Beifen Gas Industry
Corporation. Analytical grade (99.9 wt.%) methanol and ethylene glycol were purchased from Beijing
Chemicals Corporation. Distilled water was produced in our laboratory.
The composition of the synthetic gas mixture tested is 90.13 mol% methane and 9.87 mol% ethane.

Fig. 3. Liquid phase sampling system.

Fig. 4. Comparison of the methane solubility (x1 ) in water measured by authors and reported from literature [8] (T = 324.2 K).

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L.-K. Wang et al. / Fluid Phase Equilibria 207 (2003) 143154

Table 1
Methane solubility (x1 ) in water
T = 283.2 K

T = 293.2 K

T = 303.2 K

P (MPa)

x1 103 (mole fraction)

P (MPa)

x1 103 (mole fraction)

P (MPa)

x1 103 (mole fraction)

6.05
4.04
2.00

1.585
1.096
0.563

21.00
18.00
15.00
12.00
9.00
6.00
3.00

3.111
2.988
2.757
2.421
2.009
1.526
0.755

40.03
35.08
30.11
25.15
20.16
15.18
10.22

4.049
3.659
3.381
3.082
2.783
2.411
1.995

2.2. Experimental apparatus/instruments

For accelerating the experimental work, two PVT units were used simultaneously to measure the gas
solubility data in this work. The ROP unit (schematically shown in Fig. 1) was adopted for methane/gas
mixture systems and the RUSKA unit (schematically shown in Fig. 2) used for ethane system.
The ROP unit is a computer-controlled, dual cell, mercury-free high-pressure PVT system. The maximum working pressure is 82.7 MPa and the operating temperature range is 253473 K. The liquid volume
can be measured with an accuracy of 0.001 cm3 . The maximum volume of the primary/secondary cell
is 500 and 40 cm3 , respectively.

Fig. 5. Solubility of ethane in an aqueous solution of ethylene glycol (20 wt.%).

L.-K. Wang et al. / Fluid Phase Equilibria 207 (2003) 143154

147

The RUSKA PVT unit consists of an equilibrium cell of 600 cm3 , its maximum working temperature
and pressure are 423.2 K and 68.0 MPa, respectively. Constant temperature (0.1 K) was maintained
by using a silicone oil bath. A pressure-stabilizing cylinder (1500 cm3 ) was used for keeping constant
pressure in the equilibrium cell. The cylinder has a heating jacket, the maximum working temperature and pressure are 423.2 K and 83.0 MPa, respectively. An electric metering pump is connected to
the pressure-stabilizing cylinder and the pressure-transmitting medium is mercury. A motor is used for
rolling the equilibrium cell to accelerate the equilibrium process and a gas booster is available for raising
the gas pressure to the assigned value.
The composition of the tested gas mixture was analyzed by Hewlett-Packard 6890 gas chromatograph. An electronic balance (0200 g) was used for measuring the sample weight with a precision of
0.001 g.

Table 2
Methane solubility (x1 ) in the aqueous solutions of methanol
Concentration of methanol in the aqueous phase
P (MPa)

20 wt.%

40 wt.%

60 wt.%

80 wt.%

100 wt.%

x1 10 (mole fraction)
3

T = 283.2 K
40.05
35.06
30.06
25.04
20.04
15.05
10.05
5.05

6.332
6.133
5.824
5.383
4.755
4.093
3.179
1.846

10.40
10.15
9.553
8.919
7.858
6.783
5.334
3.126

25.00
23.84
22.55
20.47
18.70
16.33
12.62
7.062

69.09
67.01
62.55
57.90
50.45
42.50
31.53
18.84

289.4
261.4
234.2
204.6
177.4
148.9
103.8
45.95

T = 293.2 K
40.05
35.06
30.06
25.04
20.04
15.05
10.05
5.05

6.244
6.014
5.723
5.275
4.597
3.977
3.095
1.690

10.14
9.825
9.228
8.586
7.458
6.474
4.987
2.866

23.88
23.06
21.53
19.18
17.62
14.65
11.96
6.979

67.99
65.35
61.62
57.61
49.42
38.93
28.89
16.03

281.6
257.1
226.1
199.2
170.9
137.7
89.47
44.64

T = 303.2 K
40.05
35.06
30.06
25.04
20.04
15.05
10.05
5.05

6.068
5.848
5.480
5.132
4.571
3.887
3.013
1.521

9.803
9.455
8.807
8.259
7.442
6.276
4.889
2.540

23.14
22.28
20.90
18.75
16.88
14.22
11.32
6.574

67.91
65.11
61.26
56.15
48.80
38.35
27.19
14.50

277.5
249.5
219.0
190.0
162.0
126.0
83.13
42.31

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L.-K. Wang et al. / Fluid Phase Equilibria 207 (2003) 143154

2.3. Instruments calibration

For both PVT units, the digital manometers used for pressure measurements were calibrated against a
standard RUSKA dead-weight gauge. The precision of pressure measurement is 0.01 MPa. The platinum probes for temperature measurements were calibrated against a 25  standard probe connected
to a Hewlett-Packard Model 34401a digital multi-meter. The precision of temperature measurements is
estimated at 0.1 K.
2.4. Experimental procedure
The experimental method adopted in this work for ROP and RUSKA PVT units is similar to that reported
by Zheng et al. [25]. For saving space, detailed experimental procedure is given below for ROP unit only.
Table 3
Methane solubility (x1 ) in the aqueous solutions of ethylene glycol
Concentration of ethylene glycol in the aqueous phase
P (MPa)

20 wt.%

40 wt.%

60 wt.%

80 wt.%

100 wt.%

x1 10 (mole fraction)
3

T = 283.2 K
40.06
35.06
30.05
25.05
20.05
15.05
10.05
5.00

3.389
2.868
2.129
1.319

4.538
4.277
4.032
3.691
3.341
2.946
2.324
1.319

5.600
5.199
4.917
4.441
3.900
3.237
2.291
1.458

9.108
8.571
7.994
7.274
6.469
5.568
4.146
1.896

21.53
21.10
20.13
18.68
16.47
13.22
9.954
4.887

T = 293.2 K
40.05
35.06
30.05
25.04
20.04
15.05
10.05
5.00

4.074
3.870
3.578
3.288
2.868
2.479
1.881
1.275

4.626
4.469
4.100
3.817
3.496
2.822
2.214
1.262

5.772
5.484
5.047
4.642
4.060
3.385
2.449
1.461

9.258
8.775
8.348
7.704
7.050
5.855
4.063
2.359

22.64
21.37
19.57
17.91
15.88
13.52
10.31
5.707

T = 303.2 K
40.06
34.95
30.06
25.05
20.04
15.05
10.05
5.00

4.400
4.097
3.726
3.359
2.939
2.575
2.059
1.306

4.761
4.509
4.151
3.910
3.383
2.740
2.131
1.100

6.097
5.774
5.392
4.985
4.498
3.791
2.940
1.535

10.17
9.915
9.100
8.257
7.164
6.113
5.196
3.500

23.16
22.02
19.94
18.08
15.92
13.08
10.08
5.919

L.-K. Wang et al. / Fluid Phase Equilibria 207 (2003) 143154

149

Table 4
Ethane solubility (x2 ) in water
T = 283.2 K

T = 293.2 K

T = 303.2 K

P (MPa)

x2 10 (mole fraction)

P (MPa)

x2 10 (mole fraction)

P (MPa)

x2 103 (mole fraction)

4.00
3.50
3.10
2.50
2.00
1.50
1.00
0.50

0.700
0.538
0.310

4.00
3.50
3.00
2.50
2.00
1.50
1.00
0.50

0.864
0.811
0.751
0.651
0.477
0.245

4.00
3.50
3.10
2.50
2.00
1.50
1.00
0.50

0.864
0.804
0.756
0.677
0.616
0.532
0.366
0.119

Table 5
Ethane solubility (x2 ) in the aqueous solutions of methanol
Concentration of methanol in the aqueous phase
P (MPa)

20 wt.%

40 wt.%

60 wt.%

80 wt.%

100 wt.%

x2 103 (mole fraction)

T = 283.2 K
3.00
2.50
2.00
1.50
1.00
0.50

1.705
1.517
1.271
0.987
0.688
0.305

3.476
3.115
2.659
2.019
1.558
0.894

12.52
11.21
9.247
7.204
5.150
2.561

49.33
44.10
36.52
26.76
16.62
8.163

253.7
201.9
157.2
114.6
77.48
35.68

T = 293.2 K
3.00
2.50
2.00
1.50
1.00
0.50

1.599
1.447
1.224
0.949
0.639
0.193

3.313
3.094
2.574
1.969
1.457
0.828

11.02
9.980
8.600
6.532
3.762
1.697

45.13
41.19
34.80
25.08
15.05
7.062

230.7
187.8
137.3
93.35
63.26
28.41

T = 303.2 K
4.00
3.50
3.00
2.50
2.00
1.50
1.00
0.50

1.838
1.705
1.558
1.415
1.171
0.908
0.592
0.133

3.803
3.459
3.172
2.904
2.432
1.835
1.336
0.699

13.52
11.92
10.59
9.277
7.805
5.781
3.257
0.805

53.43
49.59
42.22
35.42
29.74
21.97
12.87
4.361

280.1
236.5
194.3
146.5
106.5
75.74
50.99
27.03

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L.-K. Wang et al. / Fluid Phase Equilibria 207 (2003) 143154

Table 6
Ethane solubility (x2 ) in the aqueous solutions of ethylene glycol
Concentration of ethylene glycol in the aqueous phase
P (MPa)

20 wt.%

40 wt.%

60 wt.%

80 wt.%

100 wt.%

x2 103 (mole fraction)

T = 283.2 K
3.00
2.50
2.00
1.50
1.00
0.50

1.118
1.032
0.894
0.722
0.479
0.231

1.230
1.116
0.975
0.779
0.486
0.207

1.618
1.423
1.174
0.898
0.576
0.200

3.167
2.958
2.594
2.071
1.368
0.459

11.18
10.01
8.637
6.770
4.708
2.320

T = 293.2 K
3.00
2.50
2.00
1.50
1.00
0.50

1.021
0.946
0.812
0.637
0.409
0.188

1.230
1.116
0.975
0.779
0.486
0.207

1.542
1.360
1.103
0.794
0.529
0.162

3.018
2.811
2.462
1.882
1.234
0.368

10.37
9.578
8.074
6.086
3.885
1.731

T = 303.2 K
4.00
3.50
3.00
2.50
2.00
1.50
1.00
0.50

1.086
1.021
0.940
0.825
0.685
0.528
0.326
0.096

1.382
1.304
1.194
1.069
0.941
0.743
0.447
0.146

1.851
1.686
1.485
1.302
1.022
0.723
0.461
0.117

3.408
3.157
2.912
2.707
2.337
1.795
1.155
0.222

11.43
10.64
9.918
9.078
7.707
5.803
3.486
1.188

In starting the experiment, the temperature of air bath was raised to the selected value. When the
temperature became stable, the whole system was evacuated. Gas species was charged into the primary
cell from a gas cylinder until the gas volume in the primary cell is about 450 cm3 and the pressure reached
5.0 MPa. Then about 25 ml liquid solvent was injected into the primary cell and the system pressure was
raised to the maximum value (40.0 MPa). In order to accelerate the equilibrium process under constant
Table 7
Solubility of methane (x1 ) and ethane (x2 ) in water for a (CH4 + C2 H6 ) gas mixture
T = 275.2 K

T = 283.2 K

P (MPa)

x1 10
(mole fraction)

x2 10
(mole fraction)

P (MPa)

x1 103
(mole fraction)

x2 103
(mole fraction)

1.80
1.50
1.00

1.032
0.913
0.711

0.0986
0.1147
0.1128

4.00
3.00
2.00
1.00

1.150
1.066
0.947
0.643

0.1447
0.1412
0.1451
0.1475

L.-K. Wang et al. / Fluid Phase Equilibria 207 (2003) 143154

151

pressure, the gas and liquid was circulating between the two cells. When system pressure and total fluid
volume remain unchanged, the system is considered in the equilibrium state. The liquid outlet valve of
the primary cell was opened slightly and about 20 ml liquid was charged to the sampling system (Fig. 3,
kept at ambient conditions) under constant pressure mode. The collected liquid sample flashes in Flask 1,
and the flashed gas displaces a portion of the water filled in Flask 2 into Flask 3. The amount of liquid in
Flask 1 and water in Flask 3 was weighed, respectively, and the gas solubility was then calculated from
the measured data. For guarantee the data quality, at least three parallel runs were conducted and the
maximum deviation allowed was 5.0%. The above experimental procedure was repeated at a decreasing
pressure-step of 5.0 MPa for each selected temperature.
When measuring the solubility data of each component in the synthetic (methane+ethane) gas mixture,
the flashed gas sample was injected into a gas chromatograph (Hewlett-Packard 6890) for composition
analysis, and the composition of the aqueous phase can thus be determined from material balance.

Table 8
Solubility of methane (x1 ) and ethane (x2 ) in the aqueous solutions of methanol for a (CH4 + C2 H6 ) gas mixture
Methanol
concentration
(wt.%)

T = 275.2 K
P (MPa)

T = 283.2 K
x1 103
(mole fraction)

x2 103
(mole fraction)

P (MPa)

x1 103
(mole fraction)

x2 103
(mole fraction)

20

4.95
4.00
3.00
2.00
1.30

3.276
2.861
2.416
1.959
1.658

0.2829
0.3500
0.3793
0.3528
0.3354

15.00
10.00
5.00

4.640
3.549
2.304

0.3606
0.3023
0.2666

40

40.00
30.00
20.00
10.00
5.00

11.49
11.05
9.483
7.211
4.464

0.6062
0.6739
0.6268
0.6219
0.7400

40.00
30.00
20.00
10.00
5.00

10.68
10.33
8.736
6.083
4.135

0.6131
0.6105
0.5537
0.4348
0.6464

60

40.00
30.00
20.00
10.00
5.00

45.83
40.21
32.36
19.78
9.417

4.727
4.158
3.552
2.512
1.393

40.00
30.00
20.00
10.00
5.00

43.16
37.54
28.74
16.51
8.209

4.616
4.320
3.379
2.215
1.881

80

40.00
30.00
20.00
10.00
5.00

59.18
53.37
45.22
29.69
16.26

5.982
5.661
5.412
6.727
6.785

40.00
30.00
20.00
10.00
5.00

55.12
51.01
42.70
26.69
17.08

5.646
5.423
5.234
4.794
4.683

100

40.00
30.00
20.00
10.00
5.00

202.2
182.4
148.9
82.27
42.80

40.00
30.00
20.00
10.00
5.00

169.1
152.6
121.5
65.11
34.03

24.59
22.61
22.27
21.93
15.73

21.04
22.30
20.11
15.49
12.76

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L.-K. Wang et al. / Fluid Phase Equilibria 207 (2003) 143154

3. Experimental results and discussion

For testing the reliability of the ROP/RUSKA PVT unit and the operating procedure adopted, the
solubility of methane in water at 324.2 K has been measured in both units and compared with literature
data reported by OSullivan and Smith [8]. Test results are presented in Fig. 4, in which the gas solubility
(x1 ) is expressed in mole fraction.
From Fig. 4, we can see that the agreement between the measured solubility data using ROP/RUSKA
unit and the data reported in literature [8] is fairly good.
In this work, the solubility of pure methane/ethane and a gas mixture (90.13 mol% methane+9.87 mol%
ethane) in water/pure alcohol (methanol/ethylene glycol)/aqueous solution of methanol/ethylene glycol
have been measured systematically in the pressure ranges of 5.040.0 MPa for methane/gas mixture,
0.54.5 MPa for ethane, and under three temperatures, 283.2, 293.2 and 303.2 K. The measured solubility
data are listed in Tables 19, where x1 and x2 denote respectively the mole fraction of methane and ethane
in the aqueous phase. In order to prevent hydrate formation, the operating pressures were carefully

Table 9
Solubility of methane (x1 ) and ethane (x2 ) in the aqueous solutions of ethylene glycol for a synthetic (CH4 + C2 H6 ) gas mixture
Methanol
concentration
(wt.%)

T = 275.2 K
P (MPa)

T = 283.2 K
x1 103
(mole fraction)

x2 103
(mole fraction)

P (MPa)

x1 103
(mole fraction)

x2 103
(mole fraction)

20

2.21
1.00
0.50

0.7987
0.5362
0.2023

0.1424
0.0995
0.0394

14.00
10.00
5.00

2.511
2.272
1.633

0.1760
0.1710
0.1432

40

15.00
10.00
5.00

3.465
2.915
1.824

0.5109
0.4476
0.3310

40.00
30.00
20.00
10.00
5.00

4.673
4.376
3.611
2.659
1.808

0.2222
0.2328
0.2313
0.2627
0.2258

60

40.00
30.00
20.00
10.00
5.00

6.827
6.353
5.261
3.616
2.402

0.3525
0.3633
0.3239
0.3468
0.3189

40.00
30.00
20.00
10.00
4.99

6.230
5.782
4.731
3.108
2.005

0.3745
0.3489
0.2865
0.2325
0.2554

80

40.00
30.00
20.00
10.00
5.00

8.900
8.225
6.971
4.526
2.756

0.6425
0.6267
0.5840
0.5231
0.4283

40.00
30.00
20.00
10.00
4.99

8.176
7.653
6.331
4.033
2.313

0.5824
0.5513
0.4927
0.4427
0.4484

100

40.00
30.00
20.00
10.00
5.00

2.622
2.437
2.217
2.009
2.189

40.00
30.00
20.00
10.00
4.99

27.45
25.19
21.75
16.85
12.75

26.10
23.70
20.22
15.39
12.12

2.562
2.399
2.157
1.895
1.876

L.-K. Wang et al. / Fluid Phase Equilibria 207 (2003) 143154

153

controlled within the range where hydrate formation can be avoided. As a typical example, the solubility
of ethane in an aqueous solution of ethylene glycol (20 wt.%) is shown in Fig. 5.
The measured data show that for each inhibitor concentration, the gas solubility increases with increasing pressure and decreases with increasing temperature. However, the temperature dependency for
ethylene glycol containing systems is less obvious.
At constant pressure and temperature, the gas solubility increases smoothly with the increase of inhibitor
concentration in the aqueous phase up to 80 wt.%. However, the gas solubility curve increases sharply
when the inhibitor concentration exceeds 80 wt.%. Under the same T, P conditions the gas solubility in
the aqueous methanol solutions is always greater than in the aqueous ethylene glycol solutions.
4. Conclusions
In this work, the solubilities of methane, ethane and a (90.13 mol% methane + 9.87 mol% ethane) gas
mixture in water and aqueous solutions of methanol/ethylene glycol have been measured using ROP and
RUSKA PVT units. The data can be used for testing/improving thermodynamic models. The presence of
inhibitor (methanol/ethylene glycol) affects the gas solubility significantly. The gas solubility increases
with increasing inhibitor concentration in the aqueous phase.
Acknowledgements
The financial support received from the National Natural Science Foundation of China (Grant Nos.
29806009 and 20176028) is gratefully acknowledged.
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