Experimental Determination of Gas Hydrates Dissociation Conditions

Article Cite This: J. Chem. Eng. Data XXXX, XXX, XXX−XXX

pubs.acs.org/jced

Experimental Determination of Gas Hydrates Dissociation Conditions in CO2/N2 + Ethanol/1-Propanol/TBAB/TBAF + Water Systems María F. Sánchez-Mora,† Luis A. Galicia-Luna,*,† Alfredo Pimentel-Rodas,† and Amir H. Mohammadi‡

Downloaded via UNIV OF KANSAS on January 21, 2019 at 19:19:01 (UTC). See https://pubs.acs.org/sharingguidelines for options on how to legitimately share published articles.

†

Laboratorio de Termodinámica, S.E.P.I.-E.S.I.Q.I.E. Instituto Politécnico Nacional, UPALM, Edif. Z, Secc. 6, 1ER piso, Lindavista C.P., México, Cd. México 07738, México ‡ Discipline of Chemical Engineering, School of Engineering, University of KwaZulu-Natal, Howard College Campus, King George V Avenue, Durban, 4041, South Africa ABSTRACT: The formation of gas hydrates is considered as a potential for oil and natural gas pipelines blockage and operational problems. It is also argued that gas hydrates can be considered as an alternative method to separate gases and many positive applications. The presence of additives in an aqueous solution can play an important role in determining gas hydrate formation conditions. In this work, hydrate dissociation conditions for the N2 + ethanol + water system, the N2 + 1-propanol + water system, and the CO2 + tetra-butyl-ammonium fluoride (TBAF) + water system have been measured and are reported. The mass fractions of alcohols were 0.05, 0.10, 0.20, and 0.30. The mass fractions of TBAF were 0.05 and 0.10. The experimental measurements were performed using an isochoric pressure search method (synthetic nonvisual method) in the 262.87−294.52 K temperature range and 0.79−33.06 MPa pressure range. The viability of the method used was verified by the experimental determination and comparison with previously published data in the literature of hydrate dissociation conditions for the N2 + H2O system, the CO2 + C2H6O + H2O system, and the CO2 + N2 + TBAB + H2O system. Finally, the thermodynamic inhibition and promotion effects of ethanol, 1-propanol, and TBAF in aqueous solutions are discussed in terms of hydrate dissociation pressures and temperatures

1. INTRODUCTION

gases, water desalination, sequestration of carbon dioxide, and air-conditioning use, etc.1,27,29,30 In the oil and gas industry, it is well-known that hydrate formation is responsible for an oil and gas producing pipelines blockage under low temperature and high pressure conditions,31,32 despite the several efforts that have been performed to prevent hydrate plugging in pipelines.7 For a successful flow assurance strategy, accurate knowledge of the thermodynamic stability (equilibria data) of hydrates as a function of concentrations of inhibitors (according to the system conditions) is crucial.33 Depending on the application, inhibition or promotion of hydrate formation is required. The thermodynamic inhibitors are hydrophilic compounds that depress the chemical potential of water, changing the phase equilibria conditions (higher pressure/lower temperature) under which hydrates may form, avoiding the hydrates from forming in the pipelines.33−35 Besides, the thermodynamic promoters are compounds of suitable molecular sizes to occupy the hydrate cages in a forming system, changing the phase equilibria conditions, promoting the hydrate formation

Gas hydrates or clathrate hydrates (denominated “hydrates” hereafter), are solid solutions composed of water molecules called the “host” that form cages by hydrogen bonds and enclose different molecules called “guests” within the cages;1−5 this phenomena occurs, generally, at high pressures and low temperatures (well above the triple point of water).6−8 The guest species are small hydrophobic molecules that may be gaseous or liquid at room conditions.9,10 The appearance of hydrate is ice-like (crystalline solid) and it consists of a framework of hydrogen-bonded water molecules, as mentioned earlier.11−15 Since its discovery in 1810 (Sir Humphry Davy discovered that a solid could be formed when an aqueous solution of chlorine was cooled below 282.15 K),16 hydrates have been extensively researched, initially, to determine their structures and properties, and17−22 currently, as a potential to cause operational problems in petroleum industry.23−26 It is generally acknowledged that hydrates have properties that involve a large capacity of gas storage, fractionation of gas mixtures, and a high heat of formation and decomposition.2,24,27,28 These properties enable gas hydrate to be applied for various technologies such as transportation and storage of natural © XXXX American Chemical Society

Received: October 30, 2018 Accepted: January 3, 2019

A

DOI: 10.1021/acs.jced.8b00998 J. Chem. Eng. Data XXXX, XXX, XXX−XXX

Journal of Chemical & Engineering Data

Article

to lower pressure/higher temperature.34 Lower alcohols which are considered thermodynamic inhibitors are known to disrupt the water’s hydrogen bonding network, which result in the inhibition of gas hydrates formation without being trapped in the hydrate cages.7,34 However, recent studies have reported that some alcohols, such as ethanol and 1-propanol serve as guests compounds of the hydrate structures in the presence of hydrophobic gases, such as CH4 and CO2.35 With this information, the question arises, what will be the behavior of ethanol and 1-propanol in the presence of another type of gas such as N2? In particular, the hydrates of N2 + ethanol and N2 + 1-propanol have not yet been investigated. In 2008, Sloan and Koh published several experimental and modeling studies for hydrate properties containing pure and mixed guest gas molecules,36 according to this study and briefly, the experimental equipment for high-pressure phase equilibria (macroscopic measurements) can be classified as follows: high pressure “visual” cell,25−38 high pressure “blind” cell,39−41 quartz crystal, microbalance (QCM) in a high pressure cell,42,43 cailletet,44,45 rocking cell,14,46 and highpressure differential scanning calorimetry.9,47 On the other hand, according to the classification of Dohrn et al.,48 there are two main classes of experimental methods for high pressure phase equilibria, depending on how the compositions of the equilibrium phases are determined and whether the mixture under study has been prepared with well-known initial composition (analytical methods and synthetic methods). In this work, a high pressure “blind” cell was selected and used. This is due to the advantages that it has, such as being capable to operate at high pressures (50 MPa), is the most used method (information is available in the international literature), it is a simple method and easy to handle, the initial composition is well-known at fixed, and the dissociation point is easy to determine (slope change between temperature and system pressure). Since the mixture to be investigated has been prepared (synthesized) with precisely known composition, no analysis of equilibrium phases are performed and the equipment used is a “blind” cell, and according to the classification proposed by Dohrn et al., the method used in this work is called a synthetic nonvisual method. This method was used to determine the dissociation points of gas hydrates (phase equilibrium) of mixtures containing N2 + ethanol + H2O and N2 + 1-propanol + H2O. Prior to the measurements of the mixture under study, dissociation points of gas hydrates from mixtures previously published in the literature were determined and compared with the aim of validating the instrument and/or method used. For this purpose, the mixtures CO2 + C2H6O + H2O, N2 + H2O, CO2 + TBAF + H2O, and CO2 + N2 + TBAB + H2O were measured. The experimental uncertainties were determined for pressure and temperature as combined uncertainties of 0.03 MPa and 0.049 K, respectively. The relative standard uncertainty in composition was estimated to be 0.009 in mass fraction.

by the supplier (checked by GC). All liquid substances were used as received from the manufacturer and were carefully degassed by agitation under vacuum prior to injection into the system. The water content for ethanol, 1-propanol, TBAB, and TBAF was determined using a Karl Fischer coulometer (Metrohm, 831) and the results are ethanol, 1.93 × 10−4 mass fraction; 1-propanol, 4.06 × 10−4 mass fraction; TBAB, 4.79 × 10−4 mass fraction; and TBAF, 2.3 × 10−1 mass fraction. The standard uncertainty of water content is 0.34 × 10−4 mass fraction. Table 1 shows the name of the substance used, source, CAS number, and purity in mass fraction. Table 1. Chemical Information compound N2 CO2

source Infra Air Products Infra Air Products Merck Sigma-Aldrich

ethanol 1propanol water Sigma-Aldrich TBAB Sigma-Aldrich TBAF Sigma-Aldrich a

mass fraction puritya

purification method

0.99995

none

0.9995

none

64-17-5 71-23-8

0.9990 0.9970

none none

7732-18-5 1643-19-2

0.9995 0.9980 0.9980

none none none

CASRN

Analysis method: Gas chromatography.

Apparatus. Phase equilibrium data (dissociation conditions) of the mixtures under study were measured in an experimental apparatus designed and built in house which is shown in Figure 1, consisting of a synthetic nonvisual

Figure 1. A schematic of the apparatus used in this study: equilibrium cell (EC), thermostatic bath (TB), stirrer system (SS), syringe pump (SP), vacuum pump (VP), temperature indicator (TI), pressure transducer (PT), acquisition data unit (ADU), gas supply (GS), valves (V1, V2, V3).

apparatus, according to the classification of Dohrn et al.48 The equilibrium cell is made of stainless steel. It can operate at a maximum working pressure of 30 MPa in a temperature range from 250 K up to 473 K. The cell provides a maximum volume of 25 cm3. The cell is equipped with two ports: one for temperature measurement with a platinum resistance probe (previously calibrated using a 25 Ω reference probe connected with an Automatic System Laboratories F300), and another for fluid feeding and absolute pressure measurement (by pressure transducer previously calibrated against a dead-weight balance DH 5304). The temperature of the system is set by a thermostatic bath that circulates a mixture of water (75% vol) + ethanol (25% vol) through a cooling jacket where the equilibrium cell is situated. The cell is connected to a syringe pump that is connected to the gas cylinder (CO2 or N2). The

2. EXPERIMENTAL SECTION Materials. Carbon dioxide (99.995% in mass fraction) and nitrogen (99.995% in mass fraction) were supplied by Infra México. Ethanol (99.9% in mass fraction) is from Merck. Water (99.95% in mass fraction), 1-propanol (99.7% in mass fraction), tetrabutylammonium bromide (TBAB, 99.8% in mass fraction), and tetrabutylammonium fluoride (TBAF, 76% in mass fraction) are from Sigma-Aldrich. The purity of each sample was obtained from the certificate of analysis acquired B



Article

with data previously published in the literature for hydrate dissociation conditions of the N2 + H2O system, the CO2 + C2H6O + H2O system, and the CO2 + N2 + TBAB + H2O system. The hydrate dissociation conditions for the N2 + H2O system were measured in the 274.76−278.75 K temperature range and 19.43−28.43 MPa pressure range. Figure 3 shows a

syringe pump provides the pressure into the cell. A magnetic stirrer is located inside the equilibrium cell to agitate the test fluids and hydrate solids. The stirrer was driven by a magnetic stirring grate mounted outside the cell. The temperature measurement combined uncertainty is estimated to be 0.049 K and the pressure measurement combined uncertainty is 0.03 MPa. Experimental Procedure. The experimental procedure to determine the hydrate dissociation pressure as a function of temperature is described as follows: Initially, the equilibrium cell is carefully degassed and cleaned and the apparatus is assembled. A specified amount of aqueous solution (measured with a precision balance) is introduced into the cell at ambient conditions and the gas (CO2 or N2) is injected using the syringe pump (until it reaches the desired pressure). After the assembly of the apparatus, the desired temperature in the thermostatic bath is set (depending of the investigated system) and the stirring system is turned on. While this happens, the pressure decreases as a function of temperature (cooling). A change in the slope is observed through a pressure versus temperature plot, which means that the gas hydrate begins to form. Once the temperature is reached, the system is stabilized for 6 h, ensuring the complete formation of the gas hydrate (there are no slope changes and the pressure and temperature conditions are constant). The temperature is set to about 5 K above the initial set, initiating the gas hydrate dissociation. After that, the pressure in the cell is gradually and slowly increased (by increasing the temperature in the recirculation bath, about 0.15 K per hour) so as to dissociate the hydrate (heating). Between pressure changes, the system is kept steady for 30 min to monitor pressure and temperature changes (if the rate of change between temperature and pressure is preserved, the temperature is again increased; this process is repeated until the hydrates completely dissociate). The slow increase in temperature is stopped until a change in the slope formed between the temperature and pressure conditions is observed (dissociation point), which means the complete dissociation of the gas hydrate will have been achieved. Figure 2 illustrates the experimental process. This procedure is repeated for each initial pressure so as to find the hydrate equilibrium temperature.

Figure 3. Experimental hydrate dissociation conditions for the N2 + H2O system: (●) this work; (△) Duc et al.;11 (■) Cleef and Diepen;22 (▼) Mohammadi et al.;42 (○) Nixdorf and Oellrich.49

comparison of the equilibrium pressures for the dissociation of the aforementioned system. As can be observed, the data obtained in this work are placed on the equilibrium curve formed by those reported in the literature;11,22,42,49 therefore, it is considered that the data are in good agreement with the literature. The experimental data are listed on Table 2. With these results, the method used for the determination of hydrate dissociation conditions at high pressures was validated. Table 2. Experimental Hydrate Dissociation Conditions Measured in this Work for N2 + Water Systema

3. RESULTS AND DISCUSSION Method Validation. The viability of the experimental method was verified by the determination and comparison

temp/K

pressure/MPa

274.76 275.69 276.85 277.56 278.16 278.75

19.43 21.28 23.75 25.28 26.85 28.43

a

Combined uncertainties uc are uc(P) = 0.03 MPa and uc(T) = 0.049 K.

Given that the mixtures under study contain alcohols, the dissociation points of gas hydrates of the mixture CO2 + C2H6O + H2O were determined and compared with data previously published in the literature at 273.21−279.37 K temperature range and up to 3.35 MPa. Figure 4 shows the behavior of the experimental data obtained in this work at wC2H6O = 0.10, as well as the data of Mohammadi et al.50 and Maekawa.51 As can be observed, the experimental data are on the equilibrium curve obtained by the aforementioned authors, which means that the results are in good agreement with the literature. Also, the experimental data obtained at wC2H6O = 0.053 are shown, which can be compared with Mohammadi et

Figure 2. Schematic experimental process performed. Pressure against temperature behavior (P vs T diagram). C



Article

good agreement between them (see Figure 5). On the other hand, experimental data were obtained at wTBAB = 0.30, which

Figure 4. Experimental hydrate dissociation conditions for CO2 + C2H6O + H2O systems: (●) this work at wC2H6O = 0.053; (◆) Mohammadi et al. at wC2H6O = 0.05;50 (○) this work at wC2H6O = 0.10; (◇) Mohammadi et al. at wC2H6O = 0.10;50 (▲) Maekawa at wC2H6O = 0.10.51 Pure CO2 hydrate: (□) Ferrari et al.,31 (▼) Fournaison et al.,52 (△) Mohammadi et al.,53 (■) Lirio and Pessoa.54 Figure 5. Experimental hydrate dissociation conditions for CO2 + N2 + TBAB + H2O systems at xCO2 = 0.750: (●) this work at wTBAB = 0.05; (○) Meysel et al. at wTBAB = 0.05;55 (▼) this work at wTBAB = 0.30; (△) Meysel et al. at wTBAB = 0.20.55 Data from Belandria et al.25 at wTBAB = 0.05: (■) wCO2 = 0.83, (□) wCO2 = 0.51, (◆) wCO2 = 0.22. Data from Belandria et al.25 at wTBAB = 0.30: (◇) xCO2 = 0.83, (▲) xCO2 = 0.51.

al.50 at similar composition (wC2H6O = 0.05), where the trend of the experimental data is in agreement between the different works. To show the effect of ethanol on the hydrate formation for this system, pure CO2 hydrate reference data are shown in the same figure.31,52−54 It is well-known that the effect of ethanol is inverse with respect to the dissociation temperature, which means that increasing the ethanol composition decreases the dissociation temperature of the hydrate (thermodynamic inhibitor), consistent with the observed. The experimental data are shown in Table 3. Therefore, the experimental apparatus is able to perform equilibrium dissociation data for systems containing alcohols.

can be compared with the data from Meysel et al. at wTBAB = 0.20.55 As can be observed, when increasing the TBAB composition, the hydrate dissociation temperature increases, consistent with the effect of a thermodynamic promoter. Also, data from Belandria et al.25 are shown at wCO2 = 0.83, 0.51, and 0.22, and wTBAB = 0.05 and 0.30, and as can be observed, the increase in the composition of N2 is reflected in an increase in pressure; however, the effect of TBAB is maintained, an increase in the composition of TBAB causes an increase in the dissociation temperature of the hydrate. Experimental dissociation data for this system are shown in Table 4. With these results, the method used in the measurements of hydrate dissociation conditions was validated. New Experimental Hydrate Dissociation Data. We have measured hydrate dissociation conditions for the N2 + ethanol + water system, the N2 + 1-propanol + water system, and the CO2 + TBAF + water system. Experimental hydrate dissociation pressures conditions for the CO2 + TBAF + water system were measured previously by Li et al. at wTBAF = 0.04 and 0.083.56 Figure 6 shows the experimental data obtained in this work at wTBAF = 0.05 and 0.10, those obtained by Li et al.56 as well as the data of pure CO2 hydrate. As can be observed, when the TBAF composition increases, the dissociation temperature increases, consistent with the effect of a thermodynamic promoter. Experimental dissociation data for this system are shown in Table 5. Also, experimental dissociation data for systems containing nitrogen, alkanol, and water are presented. Experimental hydrate dissociation conditions measured in this work for N2 + C2H6O + water aqueous solution systems at four ethanol

Table 3. Experimental Hydrate Dissociation Conditions Measured in this work for CO2 + C2H6O + Water Aqueous Solution Systemsa C2H6O mass fraction

temp/K

pressure/MPa

0.053

273.21 275.31 276.90 278.27 279.37 273.98 274.95 275.34 276.75 277.96

1.54 1.89 2.39 2.84 3.33 2.03 2.29 2.40 2.87 3.35

0.10

a

Combined uncertainties uc are uc(P) = 0.03 MPa and uc(T) = 0.049 K. The relative stand ard uncertainty is estimated to be ur (wi) = 0.0009.

The validation of the method used concluded with the determination of the hydrate dissociation conditions for CO2 + N2 + TBAB + H2O system at xCO2 = 0.750, 281.00−291.00 K temperature range and 0.67−3.90 MPa pressure range. The experimental data obtained at wTBAB = 0.05 were compared against the Meysel et al. data at wTBAB = 0.05,55 obtaining a D



Article

Table 4. Experimental Hydrate Dissociation Conditions Measured in This Work for CO2 + N2 + TBAB + Water Aqueous Solution Systems (xCO2 = 0.750)a TBAB mass fraction

0.05

0.30

temp/K

pressure/MPa

281.00 281.50 282.80 284.20 286.20 286.60 287.90 289.00 289.70 291.00

0.67 0.91 1.47 2.31 3.48 1.07 1.73 2.39 2.70 3.70

a Combined uncertainties uc are uc(P) = 0.03 MPa and uc(T) = 0.049 K. The relative standard uncertainty is estimated to be ur (wi) = 0.0009.

Figure 7. Experimental hydrate dissociation conditions for N2 + ethanol + H2O systems: (□) this work at wC2H6O = 0.05; (◆) this work at wC2H6O = 0.10; (◇) this work at wC2H6O = 0.20; (▲) this work at wC2H6O = 0.30. Pure N2 hydrate: (●) this work, (△) Duc et al.,11 (■) Cleef and Diepen,22 (▼) Mohammadi et al.,42 (○) Nixdorf and Oellrich.49

Table 6. Experimental Hydrate Dissociation Conditions Measured in This Work for N2 + C2H6O + Water Aqueous Solution Systemsa C2H6O mass fraction

temp/K

pressure/MPa

0.05

273.96 275.17 276.04 277.11 277.79 278.40 272.59 273.43 274.54 275.56 276.43 277.03 268.84 269.83 271.02 271.89 272.62 273.16 263.36 264.38 265.68 266.52

20.25 23.01 25.25 28.00 30.00 31.75 20.05 21.85 24.41 27.10 29.50 31.25 20.01 22.00 24.55 26.70 28.65 30.25 19.05 20.87 23.65 25.50

0.10

Figure 6. Experimental hydrate dissociation conditions for CO2 + TBAF + H2O systems: (●) this work at wTBAF = 0.05; (○) Li et al. at wTBAF = 0.04;56 (▼) this work at wTBAF = 0.10; (Δ) Li et al. at wTBAF = 0.083.56 Pure CO2 hydrate: (◇) Ferrari et al.,31 (■) Fournaison et al.,52 (□) Mohammadi et al.,53 (◆) Lirio and Pessoa.54 0.20

Table 5. Experimental Hydrate Dissociation Conditions Measured in This Work for CO2 + TBAF + Water Aqueous Solution Systemsa TBAF mass fraction

0.05

0.10

temp/K

pressure/MPa

287.48 287.97 288.68 289.27 289.00 293.08 293.71 294.03 294.52

0.79 1.17 1.57 2.23 1.81 0.87 1.25 1.65 2.09

0.30

a

Combined uncertainties uc are uc(P) = 0.03 MPa and uc(T) = 0.049 K. The relative standard uncertainty is estimated to be ur(wi) = 0.0009.

a Combined uncertainties uc are uc(P) = 0.03 MPa and uc(T) = 0.049 K. The relative standard uncertainty is estimated to be ur(wi) = 0.0009.

thermodynamic inhibition effect occurs and increases with an increase in ethanol compositions as is generally observed in the conventional inhibitor-added systems.7 This effect can be attributed to the thermodynamic inhibitors disruption of the water−water hydrogen bonding network, making it difficult to convert all water to hydrate, resulting in a shift of the equilibria curve to the inhibition region.7

concentrations (0.05, 0.10, 0.20, and 0.30 mass fraction) are shown in Figure 7 with the relevant reference data (pure N2 hydrate)11,22,42,49 and listed in Table 6. As can be seen, a E



Article

equilibrium temperature increase/equilibrium pressure reduction, consequence of the inclusion of 1-propanol molecules in the hydrate cages.34,35 The promotion effect increased up to 0.20 mass fraction, and at 1-propanol 0.30 mass fraction, it is slightly decreased perhaps due to the presence of excess 1propanol molecules that are not enclathrated in the hydrate cages and thus may function as inhibitors.7,34,35 The effect observed here is interesting, allows the discussion of hydrates containing N2 and an alkanol and can be considered as a basis for further study.

Further, the hydrate phase equilibria of the N2 + C3H8O + water aqueous solution systems at four 1-propanol concentrations (0.05, 0.10, 0.20, and 0.30 mass fraction) are shown in Figure 8 with the relevant reference data (pure N 2

■

CONCLUSIONS New hydrate dissociation data for the N2 + ethanol + water system, the N2 + 1-propanol + water system, and the CO2 + TBAF + water system were measured using the isochoricpressure search method. The mass fractions of alcohols were 0.05, 0.10, 0.20, and 0.30. The mass fractions of TBAF were 0.05 and 0.10. It was found that 1-propanol, unlike ethanol, behaves as a thermodynamic promoter, perhaps because 1propanol serves as guest compound of the hydrate structures in the presence of N2. Besides, TBAF is an interesting option as a thermodynamic promoter. From the results reported in this work, promoters and thermodynamic inhibitors that may be of interest for the petroleum industry were studied.

Figure 8. Experimental hydrate dissociation conditions for N2 + 1propanol + H2O systems: Pure N2 hydrate, (●) this work, (△) Duc et al.,11 (■) Cleef and Diepen,22 (▼) Mohammadi et al.,42 (○) Nixdorf and Oellrich;49 (□) this work at wC3H8O = 0.050; (◆) this work at wC3H8O = 0.10; (◇) this work at wC3H8O = 0.20; (▲) this work at wC3H8O = 0.30.

■

Corresponding Author

*E-mail: [email protected]. ORCID

hydrate)11,22,42,49 and listed in Table 7. Contrary to the effect observed with ethanol, a thermodynamic promotion is presented when 1-propanol is added, represented by an

Luis A. Galicia-Luna: 0000-0003-1862-8499 Alfredo Pimentel-Rodas: 0000-0002-5379-003X Funding

The authors would like to thank the Instituto Politécnico Nacional and CONACyT for the financial support of this research.

Table 7. Experimental Hydrate Dissociation Conditions Measured in This Work for N2 + C3H8O + Water Aqueous Solution Systemsa C3H8O mass fraction

temp/K

pressure/MPa

0.05

277.42 277.87 278.92 278.42 279.15 280.04 281.22 282.01 282.62 278.99 279.44 280.32 281.23 282.20 282.82 278.28 278.84 279.87 280.74 281.67 282.46

21.02 22.03 24.47 20.98 22.67 25.01 28.00 30.21 31.77 21.56 23.00 25.12 27.50 30.01 31.75 21.00 22.54 25.49 28.03 30.55 32.90

0.10

0.20

0.30

AUTHOR INFORMATION

Notes

The authors declare no competing financial interest.

■

ACKNOWLEDGMENTS Special thanks to Pedro Esquivel-Mora for his invaluable contribution to the development of the experimental method.

■

REFERENCES

(1) Javanmardi, J.; Moshfeghian, M. Energy consumption and economic evaluation of water desalination by hydrate phenomenon. Appl. Therm. Eng. 2003, 23, 845−857. (2) Mohammadi, A. H.; Eslamimanesh, A.; Richon, D. Semiclathrate hydrate phase equilibrium measurements for the CO2 + H2/ CH4 + tetra-n-butylammonium bromide aqueous solution system. Chem. Eng. Sci. 2013, 94, 284−290. (3) Imasato, K.; Tokutomi, H.; Ohmura, R. Crystal Growth Behavior of Methane Hydrate in the Presence of Liquid Hydrocarbon. Cryst. Growth Des. 2015, 15, 428−433. (4) Lee, J. D.; Song, M.; Susilo, R.; Englezos, P. Dynamics of Methane-Propane Clathrate Hydrate Crystal Growth from Liquid Water with or without the Presence of n-Heptane. Cryst. Growth Des. 2006, 6, 1428−1439. (5) Seo, Y.; Lee, H. A New Hydrate-Based Recovery Process for Removing Chlorinated Hydrocarbons from Aqueous Solutions. Environ. Sci. Technol. 2001, 35, 3386−3390. (6) Straume, E. O.; Kakitani, C.; Salomao, L. A., Jr.; Morales, R. E. M.; Sum, A. K. Gas Hydrate Sloughing as Observed and Quantified

a

Combined uncertainties uc are uc(P) = 0.03 MPa and uc(T) = 0.049 K. The relative standard uncertainty is estimated to be ur(wi) = 0.0009. F



Article

Tetra-n-butylammonium Bromide Aqueous Solution. Cryst. Growth Des. 2015, 15, 3963−3968. (30) Nakajima, M.; Ohmura, R.; Mori, Y. H. Clathrate Hydrate Formation from Cyclopentane-in-Water Emulsions. Ind. Eng. Chem. Res. 2008, 47, 8933−8939. (31) Ferrari, P. F.; Guembaroski, A. Z.; Neto, M. A. M.; Morales, R. E. M.; Sum, A. K. Experimental measurements and modelling of carbon dioxide hydrate phase equilibrium with and without ethanol. Fluid Phase Equilib. 2016, 413, 176−183. (32) Østergaard, K. K.; Tohidi, B.; Anderson, R.; Todd, A. C.; Danesh, A. Can 2-Propanol Form Clathrate Hydrates? Ind. Eng. Chem. Res. 2002, 41, 2064−2068. (33) Østergaard, K. K.; Masoudi, R.; Tohidi, B.; Danesh, A.; Todd, A. C. A general correlation for predicting the suppression of hydrate dissociation temperature in the presence of thermodynamic inhibitors. J. Pet. Sci. Eng. 2005, 48, 70−80. (34) Yasuda, K.; Ohmura, R.; Sum, A. K. Guest−guest and guest− host interactions in ethanol, propan-1-ol, and propan-2-ol clathrate hydrate forming systems. New J. Chem. 2018, 42, 7364−7370. (35) Lee, Y.; Lee, S.; Jin, Y. K.; Seo, Y. 1-Propanol as a co-guest of gas hydrates and its potential role in gas storage and CO2 sequestration. Chem. Eng. J. 2014, 258, 427−432. (36) Sloan, E. D.; Koh, C. A. Clathrate Hydrates of Natural Gases, 3rd ed., CRC Press: Boca Raton, 2008. (37) Shi, L.; Liang, D. Phase Equilibria of Double Semiclathrate Hydrates Formed with Tetraamylammonium Bromide Plus CH4CO2 or N2. J. Chem. Eng. Data 2015, 60, 2749−2755. (38) Lee, S.; Lee, Y.; Park, S.; Kim, Y.; Lee, J. D.; Seo, Y. Thermodynamic and Spectroscopic Identification of Guest Gas Enclathration in the Double Tetra-n-butylammonium Fluoride Semiclathrates. J. Phys. Chem. B 2012, 116, 9075−9081. (39) Ngema, P. T.; Naidoo, P.; Mohammadi, A. H.; Richon, D.; Ramjugernath, D. Experimental Clathrate Hydrate Dissociation Data for Systems Comprising Refrigerant + CaCl2 Aqueous Solutions. J. Chem. Eng. Data 2016, 61, 827−836. (40) Qi, J.; Wang, Y.; Fan, S.; Lang, X.; Li, Q.; Li, G.; Chen, J. Hydrate Equilibrium Measurements for CH4 and CO2/CH4 Mixture in the Presence of Single 2-Methyl-2-propanol and 1,1-Dichloro-1fluoroethane. J. Chem. Eng. Data 2018, 63, 3145−3149. (41) Ilani-Kashkouli, P.; Mohammadi, A. H.; Naidoo, P.; Ramjugernath, D. Thermodynamic stability conditions for semiclathrate hydrates of CO2CH4 or N2 with tetrabutyl ammonium nitrate (TBANO3) aqueous solution. J. Chem. Thermodyn. 2016, 96, 52−56. (42) Mohammadi, A. H.; Tohidi, B.; Burgass, R. W. Equilibrium Data and Thermodynamic Modeling of Nitrogen, Oxygen, and Air Clathrate Hydrates. J. Chem. Eng. Data 2003, 48, 612−616. (43) Lee, B. R.; Sa, J. H.; Park, D. H.; Cho, S.; Lee, J.; Kim, H. J.; Oh, E.; Jeon, S.; Lee, J. D.; Lee, K. H. Continuous” Method for the Fast Screening of Thermodynamic Promoters of Gas Hydrates Using a Quartz Crystal Microbalance. Energy Fuels 2012, 26, 767−772. (44) Jager, M. D.; de Deugd, R. M.; Peters, C. J.; Arons, J. de S.; Sloan, E. D. Experimental determination and modeling of structure II hydrates in mixtures of methane + water + 1,4-dioxane. Fluid Phase Equilib. 1999, 165, 209−223. (45) Peters, C. J.; de Roo, J. L.; de Swaan Arons, J. Phase equilibria in binary mixtures of propane and hexacontane. Fluid Phase Equilib. 1993, 85, 301−312. (46) Mohammadi, A.; Manteghian, M.; Mohammadi, A. H. Dissociation Data of Semiclathrate Hydrates for the Systems of Tetra-n-butylammonium Fluoride (TBAF) + Methane + Water, TBAF + Carbon Dioxide + Water, and TBAF + Nitrogen + Water. J. Chem. Eng. Data 2013, 58, 3545−3550. (47) Davies, S. R.; Hester, K. C.; Lachance, J. W.; Koh, C. A.; Sloan, E. D. Studies of hydrate nucleation with high pressure differential scanning calorimetry. Chem. Eng. Sci. 2009, 64, 370−375. (48) Dohrn, R.; Peper, S.; Fonseca, J. M. S. High-pressure fluidphase equilibria: Experimental methods and systems investigated (2000−2004). Fluid Phase Equilib. 2010, 288, 1−54.

from Multiphase Flow Conditions. Energy Fuels 2018, 32, 3399− 3405. (7) Koh, C. A.; Sloan, E. D.; Sum, A. Natural Gas Hydrates in Flow Assurance; Gulf Professional Publishing: Burlington, 2011. (8) Sfaxi, I. B. A.; Durand, I.; Lugo, R.; Mohammadi, A. H.; Richon, D. Hydrate phase equilibria of CO2+ N2+ aqueous solution of THF,TBAB or TBAF system. Int. J. Greenhouse Gas Control 2014, 26, 185−192. (9) Dalmazzone, D.; Hamed, N.; Dalmazzone, C. DSC measurements and modelling of the kinetics of methane hydrate formation in water-in-oil emulsion. Chem. Eng. Sci. 2009, 64, 2020−2026. (10) Seif, M.; Kamran-Pirzaman, A.; Mohammadi, A. H. Phase equilibria of clathrate hydrates in CO2/CH4 + (1-propanol/2propanol) + water systems: Experimental measurements and thermodynamic modeling. J. Chem. Thermodyn. 2018, 118, 58−66. (11) Duc, N. H.; Chauvy, F.; Herri, J. M. CO2 capture by hydrate crystallization - A potential solution for gas emission of steelmaking industry. Energy Convers. Manage. 2007, 48, 1313−1322. (12) Kakati, H.; Kar, S.; Mandal, A.; Laik, S. Methane Hydrate Formation and Dissociation in Oil-in-Water Emulsion. Energy Fuels 2014, 28, 4440−4446. (13) Tumba, K.; Hashemi, H.; Naidoo, P.; Mohammadi, A. H.; Ramjugernath, D. Dissociation Data and Thermodynamic Modeling of Clathrate Hydrates of Ethene, Ethyne, and Propene. J. Chem. Eng. Data 2013, 58, 3259−3264. (14) Stoporev, A. S.; Semenov, A. P.; Medvedev, V. I.; Kidyarov, B. I.; Manakov, A. Y.; Vinokurov, V. A. Nucleation of gas hydrates in multiphase systems with several types of interfaces. J. Therm. Anal. Calorim. 2018, 134, 783−795. (15) Cha, M.; Shin, K.; Lee, H. Structure identification of binary 1propanol+methane hydrate using neutron powder diffraction. Korean J. Chem. Eng. 2017, 34, 2514−2518. (16) Davy, H. The Bakerian Lecture. On Some of the Combinations of Oxymuriatic Gas and Oxygene, and on the Chemical Relations of these Principles to Inflammable Bodies. Philos. Trans. R. Soc. London 1811, 101, 1−35. (17) Barrer, R. M.; Stuart, W. I. Non-stoicheiometric clathrate compounds of water. Proc. R. Soc. A 1957, 242, 172−189. (18) Muller, H. R.; Stackelberg, M. v. Naturwissenschaften 1952, 39, 20−21. (19) van der Waals, J. H. The statistical mechanics of clathrate compounds. Trans. Faraday Soc. 1956, 52, 184−193. (20) Stackelberg, M. v.; Muller, H. R. On the Structure of Gas Hydrates. J. Chem. Phys. 1951a, 1319−1320. (21) Englezos, P. Clathrate Hydrates. Ind. Eng. Chem. Res. 1993, 32, 1251−1274. (22) van Cleef, A.; Diepen, G. A. M. Gas Hydrates of Nitrogen and Oxygen. Recl. Trav. Chim. 1960, 79, 582−586. (23) Hammerschmidt, E. G. Formation of Gas Hydrates in Natural Gas Transmission Lines. Ind. Eng. Chem. 1934, 26, 851−855. (24) Yin, Z.; Chong, C. R.; Tan, H. K.; Linga, P. Review of gas hydrate dissociation kinetic models for energy recovery. J. Nat. Gas Sci. Eng. 2016, 35, 1362−1387. (25) Belandria, V.; Mohammadi, A. H.; Richon, D. Compositional analysis of the gas phase for the CO2 + N2 + tetra-n-butylammonium bromide aqueous solution systems under hydrate stability conditions. Chem. Eng. Sci. 2012, 84, 40−47. (26) Mohammadi, A. H.; Richon, D. Clathrate Hydrates of Isopentane + Carbon Dioxide and Isopentane + Methane: Experimental Measurements of Dissociation Conditions. Oil Gas Sci. Technol. 2010, 65, 879−882. (27) Chatti, I.; Delahaye, A.; Fournaison, L.; Petitet, J. A. Benefits and drawbacks of clathrate hydrates: a review of their areas of interest. Energy Convers. Manage. 2005, 46, 1333−1343. (28) Javanmardi, J.; Nasrifar, Kh.; Najibi, S. H.; Moshfeghian, M. Economic evaluation of natural gas hydrate as an alternative for natural gas transportation. Appl. Therm. Eng. 2005, 25, 1708−1723. (29) Akiba, H.; Ueno, H.; Ohmura, R. Crystal Growth of Ionic Semiclathrate Hydrate Formed at the Interface between CO2 Gas and G



Article

(49) Nixdorf, J.; Oellrich, L. R. Experimental determination of hydrate equilibrium conditions for pure gases, binary and ternary mixtures and natural gases. Fluid Phase Equilib. 1997, 139, 325−333. (50) Mohammadi, A. H.; Afzal, W.; Richon, D. Experimental Data and Predictions of Dissociation Conditions for Ethane and Propane Simple Hydrates in the Presence of Distilled Water and Methane, Ethane, Propane, and Carbon Dioxide Simple Hydrates in the Presence of Ethanol Aqueous Solutions. J. Chem. Eng. Data 2008, 53, 73−76. (51) Maekawa, T. Equilibrium Conditions for Carbon Dioxide Hydrates in the Presence of Aqueous Solutions of Alcohols, Glycols, and Glycerol. J. Chem. Eng. Data 2010, 55, 1280−1284. (52) Fournaison, L.; Delahaye, A.; Chatti, I.; Petitet, J. P. CO2 Hydrates in Refrigeration Processes. Ind. Eng. Chem. Res. 2004, 43, 6521−6526. (53) Mohammadi, A. H.; Anderson, R.; Tohidi, B. Carbon Monoxide Clathrate Hydrates: Equilibrium Data and Thermodynamic Modeling. AIChE J. 2005, 51, 2825−2833. (54) Lirio, C. F. S.; Pessoa, F. L. P. Enthalpy of Dissociation of Simple and Mixed Carbon Dioxide Clathrate Hydrate. Chem. Eng. Trans. 2013, 32, 577−582. (55) Meysel, P.; Oellrich, L.; Bishnoi, P. R.; Clarke, M. A. Experimental investigation of incipient equilibrium conditions for the formation of semi-clathrate hydrates from quaternary mixtures of (CO2 + N2 + TBAB + H2O). J. Chem. Thermodyn. 2011, 43, 1475− 1479. (56) Li, S.; Fan, S.; Wang, J.; Lang, X.; Wang, Y. Semiclathrate Hydrate Phase Equilibria for CO2 in the Presence of Tetra-n-butyl Ammonium Halide (Bromide, Chloride, or Fluoride). J. Chem. Eng. Data 2010, 55, 3212−3215.

H


Experimental Determination of Gas Hydrates Dissociation Conditions

Recommend Documents