Interfacial tension between decane saturated with methane and water from 283.2 K to 298.2 K under pressures upto 10 MPa

Journal of Industrial and Engineering Chemistry 81 (2020) 360–366

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Interfacial tension between decane saturated with methane and water from 283.2 K to 298.2 K under pressures upto 10 MPa Masamichi Koderaa , Kosuke Watanabea , Maxence Lassiègea , Saman Alavib , Ryo Ohmuraa,* a b

Department of Mechanical Engineering, Keio University, 3-14-1 Hiyoshi, Kohoku-ku, Yokohama, Kanagawa, 223-8522, Japan Department of Chemistry and Biomolecular Sciences, University of Ottawa, Ottawa, Ontario K1N 6N5, Canada

A R T I C L E I N F O

A B S T R A C T

Article history: Received 2 July 2019 Received in revised form 8 August 2019 Accepted 15 September 2019 Available online 21 September 2019

Interfacial tension is one of the most important physical properties for high-precision simulations to develop the methods of preventing plugging of pipelines in the oil and natural gas industry. This paper reports experimental data with the pendant drop method for the interfacial tension of a decane + methane + water system at temperatures between 278.2 K to 298.2 K and pressures up to 10 MPa. The data show that in this temperature range the interfacial tension in the decane + methane + water system decreases almost linearly with increasing temperature. The results also show that by increasing the pressure of methane, the interfacial tension decreases from 53.98 mN m
1 to 50.23 mN m
1 at 283.2 K and 52.23 mN m
1 to 49.74 mN m
1 at 288.2 K. The nature of the methane pressure dependence of the interfacial tension changes for pressures above around 2.00 MPa. The interfacial tension decreases with the pressure up to 2.00 MPa, but has no pressure dependence above 2.00 MPa. It may be inferred that the decane/water interface is saturated with methane at pressures around 2.00 MPa and at higher pressure the interfacial tension is no longer affected by the presence of methane. © 2019 The Korean Society of Industrial and Engineering Chemistry. Published by Elsevier B.V. All rights reserved.

Keywords: Interfacial tension Natural gas Oil Multiphase flow Water Clathrate hydrates

Introduction World primary energy consumption has increased every year and especially the increase of natural gas consumption is remarkable. Natural gas is a more environmentally friendly energy resource than coal and other hydrocarbons and produces less CO2 per unit of energy released. Accordingly, it is predicted that world trend for development and consumption of natural gas will continue to increase [1]. The oil and natural gas industry will have to move towards deep sea and ultra-deep sea extraction to access natural gas [2], which are severer environmental conditions than those encountered before. Natural gas is produced under high temperature, but when it is transported in a pipeline, it is cooled to be a low-temperature and high-pressure multiphase flow with oil and water [3]. In such conditions natural gas hydrates readily form and cause the serious problem of ‘plugging the pipeline’ [4]. Natural gas hydrates are crystalline compounds formed by hydrogen-bonded water

* Corresponding author. E-mail address: [email protected] (R. Ohmura).

molecules in a lattice structure that is stabilized by encapsulating gas molecules such as methane, ethane, propane, and carbon dioxide [5]. To prevent pipelines from plugging as a result of gas hydrate formation, various methods are currently considered. In particular, the use of thermodynamic inhibitors and kinetic inhibitors of hydrate formation are common methods to solve this plugging problem [6–12]. It is also considered that crude oils can be utilized without inhibitors as a method for tackling this problem [13,14]. To develop methods of preventing pipeline plugging, it is essential to understand the dynamic behavior of the multiphase flow in the pipeline. Multiphase flow is now just starting to be understood by using fluid dynamics simulations [15–17]. The interfacial tension is one of the most fundamental thermodynamic properties that controls the dynamic behavior of multiphase flows in such mixed (natural gas + oil + water) flows. Therefore, it is one of the most important factors for high-precision simulations. Jennings [18] measured the interfacial tension in the decane + water system using the pendant drop method at temperatures from 298.2 K to 449.2 K, and pressures up to 81.7 MPa. Decane has been used as a simplified model for oil. He reported that the interfacial tension in decane + water system has little

https://doi.org/10.1016/j.jiec.2019.09.026 1226-086X/© 2019 The Korean Society of Industrial and Engineering Chemistry. Published by Elsevier B.V. All rights reserved.

M. Kodera et al. / Journal of Industrial and Engineering Chemistry 81 (2020) 360–366

dependence on pressure under those experimental conditions. Zepperi et al. [19] also measured the interfacial tension in the decane + water system using the pendant drop method, but the conditions of their experiments were at lower temperatures than those investigated in the study by Jennings. Specifically, their conditions were limited to pressure at only 0.1 MPa and for temperatures from 283.2 K to 338.2 K. They showed that the interfacial tension in decane + water system decreases with increasing temperature. Yasuda et al. [20] measured the interfacial tension between water and methane which is the main component of natural gas, using the pendant drop method at temperatures from 278.15 K to 298.15 K, and pressures up to 10 MPa, which are near methane hydrate formation conditions. They observed that the water-gas interfacial tension decreases with increasing methane pressure and the dependence on temperature could not be observed for these conditions. Hayama et al. [21] measured the interfacial tension between (methane + ethane + propane) gas mixture and water from 283.2 K to 298.2 K under pressures up to 10 MPa. The gas mixture (methane + ethane + propane) is a more precise model of natural gas. They revealed that the interfacial tension between natural gas and water decreases when the pressure increases at all temperature conditions, but the dependence on temperature could not be confirmed. They also indicated that the interfacial tension gradient with respect to pressure was hardly influenced by interaction between gases. The molecular origins of the pressure and temperature effects on the methane + water and (methane + ethane + propane) + water systems have recently been studied using molecular dynamics simulations [22]. These studies show that at pressure — temperature ranges near hydrate formation and gas liquidation, the small hydrocarbon molecules do not form complete monolayer coverage at the water surface. As the study on the interfacial tension in (liquid + liquid + gas) ternary system, Bagalkot and Hamouda [23] measured the interfacial tension in CO2 + decane + water system. As mentioned above, the interfacial tensions in two phase gasliquid systems, which are simple models of the multiphase flow in the pipeline, have been widely reported. However, three phase oilwater-gas systems have yet to be studied near methane hydrate forming conditions in a pipeline. In this study, we modeled natural gas as methane and oil as n-decane and performed experimental measurements of the interfacial tension between n-decane and water both saturated with methane. The experimental pressuretemperature conditions were set at prescribed values in the range of pressure from 0.00 MPa to 10.00 MPa and of temperature from 278.15 K to 298.15 K. At each prescribed pressure and temperature, we saturated n-decane and water with methane. From here onwards, we will use decane for n-decane. From the data of these experiments, the temperature and pressure dependence of the interfacial tension in decane + methane + water system is discussed. Experimental methods Materials The specifications and sources of the compounds used in this study are summarized in Table 1. A gas cylinder containing

361

methane was supplied from Takachiho Chemical Industrial Co., Ltd. Decane was supplied from Sigma-Aldrich Co. LLC, with a purity of more than 99 mass% which is the purest grade offered. Water used in all experiments was deionized and double distilled in our laboratory (model WG 222, Yamato Scientific Co., Ltd.). The electrical conductivity of the water was less than 0.5  10
4 S m
1. The reliability of the water purification used in this study and other aspects of the experimental techniques were evaluated by comparing the value of the interfacial tension between methane and water measured by the pendant drop method with the results reported in a previous study [20]. Apparatus and procedure Fig. 1 shows a schematic illustration of the experimental apparatus used in this study and the pendant drop observed in this experiment. The reliability of the apparatus was confirmed in a previous study [24] in which the interfacial tension of the (CO2 + H2) gas mixture and water system was measured. The procedure and the details of this apparatus are also described in previous studies [23,24]. The apparatus is made from stainlesssteel and can withstand high pressure, up to 10 MPa. The 243 cm3 cylindrical test cell in the apparatus is equipped with a liquid stirrer. The inside pressure was measured by a pressure transducer (model PHB-A-10 MP, Kyowa Electronic Instruments Co., Ltd.) and the system temperature was measured by a platinum resistance thermometer (Class B, Ichimura Metal Co., Ltd.). The thermometer is inserted into the test cell from its side, with the tip of the thermometer located within 6 mm from the pendant drop. The 95% measurement uncertainty for the pressure and temperature were 0.03 MPa and 0.2 K, respectively. The system temperature was controlled by circulating water around the test cell. The circulating water temperature was regulated by a chiller (RTE740, M&S Instruments Inc.). A pair of inlets are attached to the side of the test cell to enable a clear separation of the inlet for gas (air and methane) from that for liquid (decane). Deionized and double distilled water was supplied through a stainless-steel tube inserted vertically into the test cell from a water reservoir located above the apparatus. A pendant drop was formed at the tip of the stainlesssteel tube. The shape of the suspended pendant drop was recorded with a CMOS camera (model EOS 50D, Canon, Inc.) through a glass window attached at the front of the cell. The diameter of the stainless-steel tube which suspended the pendant drop was measured as 1.65 mm by a micro meter (M210-25, Mitutoyo Corporation). In this study, the test cell was filled with the liquid decane. At the beginning of measurements, methane was supplied at a pressure that is higher approximately by 1 MPa than the target experimental pressure and the liquid decane was saturated with methane. A stirrer helped methane dissolve into decane faster. The saturation of methane was confirmed by the system pressure attaining a steady state value. Thereafter, the system pressure was adjusted to each prescribed level by the discharge of methane from the apparatus. The saturation of methane in decane at each prescribed pressure was ensured since once-dissolved, the concentration of methane decreases with the decrease of the

Table 1 Specifications and sources of the compounds used in this study. Substance

Source

Purity

Methane

Takachiho Chemical Industrial Co., Ltd. Sigma-Aldrich Co. LLC Laboratory made

99.999 vol%

Decane Water

99 mass% The electrical conductivity was less than 0:5  10
4  S  m
1

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Fig. 1. Schematic illustration of experimental apparatus used in this study and the pendant drop observed in this experiment.

pressure. In addition, water was also considered to be saturated with methane during this procedure because it took for more than 1 h to wait for the saturation of methane into the decane phase in this study. The saturation of methane into water in practice has a negligible effect on the interfacial tension measurements in our study. The mass fraction of saturated methane in water is 10
6 order, as shown in Table 2. Therefore, the densities of water phase saturated with methane are calculated to the same values as those

of pure water with REFPROP ver. 9.1 [25] to the number of decimal places used in the calculations. The pendant drops were formed six times every 10 minutes and just after formation, the images of each pendant drop were captured with the CMOS camera. We determined the average of the interfacial tension calculated from those images under each set of conditions. The measurements of the interfacial tension were performed under the following five temperature conditions: 278.2, 283.2,

Table 2 Mass fraction of methane in decane and water phases and densities under experimental conditions. Temperature

Pressure

Mass fraction of methane

T/K

P/MPa

in Decanea wCH4, decane/102

in Waterb wCH4, water/106

Decane rdecane/kg m
3

Water rwater/kg m
3

278.2 283.2 288.2 293.3 298.3

1.00 1.00 1.00 1.00 1.00

0.367 0.370 0.375 0.379 0.380

0.543 0.684 0.863 1.089 1.341

738.8 734.9 730.9 726.9 723.0

1000.4 1000.1 999.5 998.6 997.4

278.1 283.2 288.2 293.2 298.3

2.00 2.00 2.00 2.00 2.00

0.813 0.819 0.824 0.829 0.834

1.026 1.309 1.644 2.057 2.579

735.0 730.9 727.0 723.0 718.9

1000.9 1000.6 1000.0 999.1 997.9

283.2 288.2

3.00 3.00

1.349 1.354

1.865 2.354

726.4 722.4

1001.1 1000.4

283.2 288.2

4.00 4.00

1.953 1.953

2.372 3.000

721.2 717.2

1001.5 1000.9

283.2 288.2

5.00 5.00

2.609 2.601

2.823 3.575

715.7 711.8

1002.0 1001.4

283.1 288.2

6.00 6.00

3.297 3.277

3.215 4.097

710.2 706.3

1002.5 1001.8

283.1 288.2

6.99 7.00

3.987 3.962

3.572 4.571

704.7 700.7

1003.0 1002.3

288.2

10.09

6.066

5.738

684.5

1003.7

a b

wCH4, decane: the mass fraction of methane in the decane phase. wCH4, water: the mass fraction of methane in the water phase.

Density

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288.2, 293.2, and 298.2 K. At 283.2 K and 288.2 K, the experiment was conducted under pressure conditions from 0.00 MPa to 10.09 MPa: i.e., 0.00, 1.00, 2.00, 4.00, 6.00, 7.00, and 10.09 MPa. At the other temperatures, the pressure conditions were 0.00, 1.00, and 2.00 MPa. These conditions are around conditions of multiphase flow in gas pipelines [26] and are located outside the thermodynamic region of hydrate formation in the phase diagram [27,28]. To measure the interfacial tension as precisely as possible, the surface-active impurities in the decane were removed using purification methods described in the previous studies [29]. In this study we used two methods for decane purification: the separating funnel method and the alumina column method. In the separating funnel method, a decane/water interface was made in the separating funnel after shaking the decane/water mixture. Then, that surface was removed. In the alumina column method, decane was passed through an alumina column. We attempted these procedures nine times and five times, respectively. To confirm the reliability of decane used in the experiments, the interfacial tension in decane + water system at 0.00 MPa was also measured under six temperature conditions from 278.2 K to 298.2 K before the experiments with methane and we compared our results with those from the previous study [19]. In this study, the values of the interfacial tension were deduced by analyzing the images of pendant drop obtained using the above procedure utilizing the selected plane method [30], which is based on a practical and theoretical technique using the following equations:

g¼

Dr gde 2 H

  1 ds   ¼  f H de

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Table 3 Interfacial tension values in methane + water system and decane + water system. Temperaturea T/K

Pressureb P/MPa

Interfacial tension g/mN m
1

Uncertainty Uc(g)/mN m
1

methane + waterc (this study) 288.0 1.00 286.9 1.00

72.43 71.62

1.51 1.64

methane + water [20] 288.1 1.00 1.00 288.2

71.52 71.31

1.22 1.08

decane + waterc (this study) 278.2 0.00 283.3 0.00 288.2 0.01 293.1 0.01 295.6 0.01 298.3 0.01

54.50 53.98 52.23 51.40 51.33 51.16

1.03 1.10 1.08 1.02 0.94 1.06

a b c

U(T) = 0.2 K (k = 2). U(P) = 0.03 MPa (k = 2). Using double distilled water.

ð1Þ

ð2Þ

in which g denotes the interfacial tension, Dr is the density difference between the decane phase and the water phase, g is the gravitational acceleration, de represents the equatorial diameter and ds represents the droplet diameter which is located by measuring vertically a distance equal to de from the lower end. H is the Bond number and 1/H is a function of the ratio of the two diameters ds =de [31]. Because the mutual solubility between decane and water is 10
9 in mass fraction [32], it was assumed that the mutual solution hardly influences the density of each phase. Therefore, the mutual solution in decane and water system was neglected on the calculation of the density difference. The density of decane and water saturated with methane were calculated using REFPROP ver. 9.1 [25]. The calculated compositions of decane and water phases under the experimental conditions are summarized in Table 2 as well as the calculated densities of each phase. The combined standard uncertainty obtained for each interfacial tension measurement was estimated to be 1.26 mN m
1 or smaller. Results and discussion The experimental data of the interfacial tension between methane and water and between decane and water are summarized in Table 3. We measured the interfacial tension between decane and water under 0.00 MPa or 0.01 MPa pressure to eliminate the effect of any other substances except decane and water. Fig. 2 shows the data for the interfacial tension between decane and water at 0.00 or 0.01 MPa (ambient pressure) at different temperatures from this work in comparison with those reported in the previous studies [19,29,33–36]. The values of the interfacial tension between decane and water obtained from this study are also consistent with those from the previous studies

Fig. 2. Temperature dependence of the interfacial tension between decane and water compared to previous studies. 4, this work; , Zeppieri et al. [19]; , Goebel & Lunkenheimer [29]; , Susnar et al. [33]; , Wiegend & Franck [34]; , Cai et al. [35]; , Georgiadis et al. [36].

within the range of uncertainty. The values of the interfacial tension between methane and water obtained in the present study are consistent with those from the previous study [20] within the range of uncertainty. These agreements of the data obtained in the present study with the corresponding literature data support the reliability of double distilled water, methane, decane, and the procedure and experimental apparatus used in this study. Table 4 gives the summary of the values of the interfacial tension in decane + methane + water system. Fig. 3 shows temperature dependence of the interfacial tension in decane + methane + water system at 1.00 and 2.00 MPa in the temperature range of 278.2 to 298.3 K. For comparison, the values of the interfacial tension in water, water + methane, and decane systems are also plotted in Fig. 3(a). Fig. 3(b) specifies only the interfacial tensions between decane and water. It can be seen that the water + decane interfacial tension has a magnitude between that of the pure water and decane interfacial tensions. The interfacial tension in the decane + methane + water system decreases almost linearly with increasing temperature in this range. This phenomenon may be

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Table 4 Interfacial tension values in decane + water system saturated with methane. Temperaturea T/K

Pressureb P/MPa

Interfacial tension g/mN m
1

Uncertainty Uc(g)/mN m
1

278.2 283.3 288.2 293.1 295.6 298.3

0.00 0.00 0.01 0.01 0.01 0.01

54.50 53.98 52.23 51.40 51.33 51.16

1.03 1.10 1.08 1.02 0.94 1.06

278.2 283.2 288.2 293.3 298.3

1.00 1.00 1.00 1.00 1.00

53.17 51.88 51.46 50.08 50.13

1.02 1.16 0.92 0.91 0.90

278.1 283.2 288.2 293.2 298.3

2.00 2.00 2.00 2.00 2.00

53.34 52.15 50.46 50.01 49.47

1.07 0.96 0.89 0.95 0.93

283.2 288.2

4.00 4.00

50.45 50.35

0.97 0.93

283.1 288.2

6.00 6.00

50.08 50.24

1.13 1.06

283.1 288.2

6.99 7.00

50.23 49.74

0.91 0.93

288.2

10.09

50.41

1.26

a b

U(T) = 0.2 K (k = 2). U(P) = 0.03 MPa (k = 2).

ascribed to a weakening of intermolecular interactions with the increase of molecular thermal motions at higher temperatures. Above 2.00 MPa, temperature dependence of the interfacial tension in this three phase system is not observed in the range of temperature from 283.1 K to 288.2 K since the values remain relatively constant. The temperature dependence of the interfacial tension, @g =@T, are calculated and summarized in Table 5. From Table 4, the values of @g =@T at three different pressures are similar within the range of uncertainty regardless of pressure and presence of methane. This result indicates that the temperature dependence of the interfacial tension between the water/decane interface does not depend on the presence of methane molecules. Yasuda et al. reported that the temperature dependence of interfacial tension between methane and water could not be observed for the conditions from 278.15 K to 298.15 K, for pressures up to 3 MPa [20]. Those conditions are almost in the same range of temperature and pressure of this study. Based on the results from the previous study, methane molecules could have an influence on temperature dependence of the interfacial tension in decane + methane + water system, but Table 4 does not show the clear change of the  @g =@T values. It is inferred that the concentration of dissolved methane is so small that it has little effect on @g =@T in the decane + methane + water system. The largest mass fraction of methane in the decane phase under the experimental conditions is calculated to only be 0.0083 with REFPROP ver. 9.1 [25]. Within the range of temperature and pressure of this study, methane has the highest solubility in decane at 2.00 MPa and 298.2 K. Fig. 4 shows the methane pressure dependence of the interfacial tension in decane + methane + water system at 283.2 K and 288.2 K up to 10 MPa methane pressure. The interfacial tension at a given temperature decreases with increase in the pressure up to 2.00 MPa while no pressure dependence above 2.00 MPa. This behavior of pressure dependence incorporates a

Fig. 3. (a) Temperature dependence of the interfacial tension in various systems considered in this work. (b) Temperature dependence of the interfacial tension in decane + water system saturated with methane. Petrova [37];

, surface tension of water,

, interfacial tension between methane and water, Yasuda et al. [20];

, this work at P  0.01 MPa; at P  2.00 MPa;

, this work at P  1.00 MPa;

, this work

, surface tension of decane, Jasper & Kring (1955) [38].

combination of two results from the previous studies [18,20]. First is the interfacial tension between methane and water reported by Yasuda et al. [20], and the other is the interfacial tension between decane and water reported by Jennings [18]. Yasuda et al. revealed that the interfacial tension between methane and water decrease with increasing pressure and Jennings revealed that the interfacial tension between decane and water has little dependence on pressure. Accordingly, pressure dependence of the interfacial tension in decane + methane + water system changing around 2.00 MPa may be a special characteristic of this three phase system. One of the differences between the three-phase systems from the above two-phase systems is the dissolution of methane into the decane phase. If the solubility of methane into the decane phase changes drastically at a given pressure, it is inevitable that the pressure dependence of the interfacial tension also changes at that pressure. However, the solubility of methane in decane linearly increases with increasing pressure, even beyond the range of 2.00 MPa like Table 2 shows [25]. Therefore, the dissolution of

M. Kodera et al. / Journal of Industrial and Engineering Chemistry 81 (2020) 360–366

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Table 5 Interfacial tension gradients with respect to temperature. Pressureb

System

P/MPa decane + water decane + methane + water decane + methane + water methane + water [20]

0.01 1.00 2.00 1.00 2.00 0.1 0.1

water + air [37] decane + air [38] a b

The temperature dependence of the interfacial tension (@g /@Ta )/mN (mT)
1

Uc(@g /@T) (g )/mN (mT)
1


0.18
0.16
0.20 –

0.04 0.07 0.06 –


0.15
0.09197

– –

Uncertainty

U(T) = 0.2 K (k = 2). U(P) = 0.03 MPa (k = 2).

Fig. 4. Pressure dependence of the interfacial tension in decane + methane + water system.

, T  283.2 K;

The molecular mechanism of the effect of methane gas on the interfacial tension decane + methane + water system can be studied by molecular dynamics simulations of this system. Molecular dynamics simulation would provide the direct and independent theoretical understanding of the molecular scale behavior around the interface, since the molecular dynamics simulations are independent to the interfacial tension experiments. Such simulations, which are planned for the future, would clarify the nature of the interactions between the methane molecules at the decane/water interface. These simulations would determine whether the adsorption of the methane at the interface is static or dynamic, with exchange of methane molecules between the bulk phases and the interface. Simulations would also address the nature of the saturation effect of methane at pressures of 2.00 MPa or above on the interfacial tension. It could be determined whether this limit is determined by the saturation of fixed surface adsorption sites with methane molecules or by the dynamic exchange of methane between the interface and bulk phases.

, T  288.2 K.

Declarations of interest methane into the decane could not alone lead to the observed change of pressure dependence of the interfacial tension observed at around 2.00 MPa pressure or greater in the decane + methane + water system. There should be other factors causing the phenomenon of pressure dependence in this system. It may be inferred that one possibility is that the observed phenomenon of pressure dependence in decane + methane + water system results from the saturation of the decane and water interface with respect to methane at around 2.00 MPa. Conclusion To develop methods of preventing plugging of the pipeline, the dynamic behavior of the multiphase flow in the pipeline is now just starting to be understood by using fluid dynamics simulations. The interfacial tension is one of the most fundamental thermodynamic properties that controls the dynamic behavior of multiphase flows and one of the most important factors for high-precision simulations. Interfacial tension measurements in the decane + methane + water system were performed using the pendant drop method at temperatures from 278.2 K to 298.2 K and pressures up to 10 MPa. The obtained data show that the interfacial tension in the decane + methane + water system decreases almost linearly with the increasing temperature. The data also reveal that the interfacial tension decreases with the increasing pressure up to 2.00 MPa while having no pressure dependence above 2.00 MPa. The observed phenomenon could be caused by the saturation of methane on the decane/water interface. Therefore, the interfacial tension no longer decreases above 2.00 MPa.

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