Solubility of Hydrogen Sulfide in Ethanediol, 1, 2-Propanediol, 1

Article pubs.acs.org/jced

Solubility of Hydrogen Sulfide in Ethanediol, 1,2-Propanediol, 1‑Propanol, and 2‑Propanol: Experimental Measurement and Modeling Mohammad Shokouhi,* Ali Reza Rezaierad, Seyed-Majid Zekordi, Maryam Abbasghorbani, and Mehdi Vahidi Research Institute of Petroleum Industry (RIPI), P.O. Box 14665−137, Tehran, Iran ABSTRACT: The solubility of hydrogen sulfide in 1,2ethanediol, 1-propanol, 2-propanol, and 1,2-propanediol were experimentally measured. Gas concentrations were systematically measured by isochoric saturation method at temperatures from (303.15 to 353.15) K and total pressure from vapor pressure of solvent up to about 1.5 MPa. Results show that H2S dissolves in mentioned organic solvents in order 2-propanol ∼ 1-propanol > 1,2 -propanediol > 1,2-ethanediol. The experimental data were correlated by using (1) the Krichevsky−Ilinskaya (KI) equation and (2) a generic Redlich−Kwong (GRK) cubic equation of state.

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INTRODUCTION Impurity of natural gas including acids, sulfur compounds, as well as water must be handled with some physical and chemical solvents through sequence sweetening and dehydration processes. When natural gas is recovered, its water content may need to be lowered to prevent water from condensing or freezing in pipelines or from forming hydrocarbonhydrates. Hydrates can foul instruments and reduce line capacity. The hygroscopic nature of polyols makes it an effective dehydrating fluid for use in the natural gas processing industry. As the deep-sea pipelines are exposed to an ambient temperature only just above freezing, it is easy to see why the antifreeze function alone is of such considerable importance. Without dehydration, a free water phase (liquid water) could also drop out of the natural gas as it is either cooled or the pressure is lowered through equipment and piping. This free water phase will often contain some portions of acid gas (such as H2S and CO2) and can cause some limitations. Among physical solvents, polyols, due to its low vapor pressure and high water solubility, is highly used for inhibiting gas hydrate in the gas processing. Alcohols especially methanol and glycols, such as 1,2-ethandiol (ethylene glycol), (EG), 1,2-propanediol (propylene glycol), (PG), diethylenglycol (DEG), triethylene glycol (TEG) as well as glycerol are two classes of polyols that may be applied for this purpose. EG is a colorless, odorless, sweet-tasting chemical found in many household products, including antifreeze, deicing products, detergents, paints, and cosmetics. PG is a colorless, odorless, slightly sweetish, viscous, highly hygroscopic liquid. It is fully miscible with water, methanol, ethanol, acetone, diethyl ether, chloroform. The use of polyols as dehydrating agents are accompanied with an uncomfortable result: the polyols also dissolve an amount of © XXXX American Chemical Society

the gaseous components. This effect reduces the water removing efficiency. The knowledge about the amount of the dissolved acid gases is helpful for choosing the adequate dehydrating agent to design and optimize an effective dehydration system. Another motivation for the study deals with fundamental research, because studies of gas−liquid solubility provide important information for the understanding of the solubility mechanism and also help in the development of models and theories. Almost data reported in literature are related to the solubility of CO2 in methanol,1−3 ethanol,3−6 1-propanol,7−9 and 2-propanol10−13 and also in polyols such as ethylene glycol (EG),14−18 diethylene glycol (DEG),16,19−21 triethylene glycol (TEG), 22,23 1,2-propylene glycol (PG), 24 and glycerol (GLY).25The phase behavior for ternary mixtures of CO2 + glycerol + short chain alcohols, namely methanol, has been recently published as well.26−28 As far as know, except for solubility of hydrogen sulfide in EG,17 DEG,20,29,30 and TEG,22,23 no experimental data have been reported on solubility of hydrogen sulfide in PG and short chain alcohols. In this work, we present new experimental solubility data of H2S in EG and PG as dehydration agents in natural gas treatment and also some alcohols such as 1-propanol (1-PrOH) and 2-propanol (2-PrOH) for industrial and fundamental research purpose. All experimental trials were carried out via isochoric saturation method at a temperatures range from (303.15 to 353.15) K and total pressure up to 1.5 MPa. The solubility data are modeled using two distinct correlations related to two theoretical approaches: the new version of Redlich−Kwong (RK) cubic equation of state Received: August 10, 2015 Accepted: November 24, 2015

A

DOI: 10.1021/acs.jced.5b00680 J. Chem. Eng. Data XXXX, XXX, XXX−XXX

Journal of Chemical & Engineering Data

Article

The amount of remaining acid gas in the gas phase, nag, was determined from

proposed by Shiflett and Yokozeki for gas-ionic liquid systems,31−33 and the extended Henry’s law combined with twosuffix Margules equation known as the Krichevsky−Ilinskaya (KI) equation.34,35 Some characteristic partial molar thermodynamic properties of H2S dissolved at infinite dilution in that particular solvent were calculated from the solubility data.

nagg

■

chemical name hydrogen sulfide

H2 S

[7783-06-4]

1,2-ethanediol 1-propanol 2-propanol

C2H6O2 C3H8O C3H8O

[107-21-1] [71-23-8] [67-63-0]

1,2-propanediol

C3H8O2

[57-55-6]

purity (GC)

mag =

nagl wSolvent

xag =

99.95% (mol %)

Roham Gas Company ≥99% (mass %) Merck 99% (mass %) Aldrich ≥99.5% (mass %) Merck (EMPLURA) >99% (mass %) MerckSchuchardt

(5)

nagl

source

nagl +

wSolvent MSolvent

(6)

nlag

In which, is the amount of acid gas (in terms of mole) in the liquid phase, wSolvent is the mass of solvent in g, and MSolvent is molar mass of pure solvent in g mol−1. As mentioned above, the amount of dissolved gas is calculated from the amount of gas charged to the cell by subtracting a correction for the amount of gas that is still present in the vapor phase. That correction is calculated assuming that the volume of the vapor phase is the difference between the cell volume and the volume of the unloaded solvent (which is known from the preparation of the solvent). However, that procedure neglects a volume change (mostly a volume expansion) when a gas is dissolved in a liquid. In this case, eq 3 may be corrected as eq 7

All the materials were reagent grade and used without further purification.

Apparatus and Procedure. The details of the experimental method for the measurement of gas solubility have previously been presented36 and only a short description will be provided here. The double wall equilibrium cell was connected to a water recirculation bath (model T 2500 PMT Tamson) with temperature stability within ±0.02 K and the temperature was measured using a model TM-917 Lutron digital thermometer with a 0.01 K resolution equipped with a Pt-100 sensor inserted into the cell. The equilibrium cell pressure was measured using a model PA-33X KELLER pressure transmitter sensor in the range of (0 to 25) bar, which was accurate to within 0.1% of full scale and that of the gas container was measured using a Baroli type BD SENSORS digital pressure gauge in the range of (0 to 25) bar, which was accurate to within 0.1% of full scale. One can calculate the total number of moles of acid gas injected into the equilibrium cell using the procedure adopted by Park and Sandall37 and Hosseini Jenab et al.36 Vgc ⎛ Pi P⎞ ⎜ − f⎟ RTa ⎝ Z i Zf ⎠

(4)

The molality of the loaded gas in the liquid phase is defined as

a

nag =

(3)

nagl = nag − nagg

Table 1. Specifications and Sources of Chemicals Used in This Work That Contain Molecular Formula, CAS Registry Number, and Puritya CAS registry number

= Vgρag

ZagRT

where Vg is the gas phase volume, T is the equilibrium temperature of the cell, and Zag and ρag are the compressibility factor and density of acid gas at Pag and T, respectively. The amount of gas in the liquid phase was then determined from

EXPERIMENTAL SECTION Materials. Hydrogen sulfide gas (c.p. grade 99.95% min) was supplied by Roham Gas Company. The specifications and sources of the chemicals used in this work are summarized in Table 1.

molecular formula

=

Vgpage

nagg

⎛ ⎜ = ρag ⎜Vauto − ⎜ ⎝

(

mag wSolvent 1000

+ wSolvent ⎞⎟ ⎟⎟ ρ ⎠

)

(7)

mag is the molality of acid gas obtained from iteration technique or as an approximate estimation obtained from molality calculated with eqs 3−6. The error propagation theory was used to estimate the uncertainties of final results.39 In the base of this theory, the uncertainty u(q) of the interest variable q(R...U) is given by eq 8 ⎡⎛ ∂q ⎞ ⎤2 ⎡⎛ ∂q ⎞ ⎤2 u(q) = ± ⎢⎜ ⎟dR ⎥ + ... + ⎢⎜ ⎟dU ⎥ ⎣⎝ ∂R ⎠ ⎦ ⎣⎝ ∂U ⎠ ⎦

(1)

where Vgc denotes the volume of the gas container, Zi and Zf are the compressibility factors corresponding to the initial and final pressures, Pi and Pf, respectively, in the gas container before and after transferring gas, and Ta is the ambient temperature, which is equal to that in the gas container. Compressibility factors were calculated using NIST.38 Mixing and equilibration between liquid and vapor phases inside the cell were normally achieved within about 2 h after beginning of stirring and the partial pressure of gas at equilibrium in the equilibrium cell, Pag, was calculated as follows Pag = PT − PVP (2)

(8)

The measured quantity q is dependent upon the variables R...U that fluctuates in a random and independent manner. The uncertainties of all of the instruments used in the measurements were considered for estimating the uncertainty of the solubility of H2S in the liquid phase. The main contributions to the uncertainty of the solubility are attributed to errors in the pressure sensor for equilibrium cell and gas container (both are equal to 0.003 MPa), temperature sensors (0.10 K), and scale for the amount of solvent in equilibrium cell (0.001 g). The volumes of the gas sample and equilibrium cell were obtained by performing pressure swing experiments. The pressure swing experiments consisted of measuring the pressure drop when valve between unknown and reference volume are opened, where prior to its opening the reference volume was pressurized

where PT and PVP denote the total pressure and vapor pressure of solvent. B



Article

Table 2. Linear Correlation Equation for Density with Temperature Range and Correlation Coefficient, R2, and Antoine Constants, ln(PVP/kPa) = A + B/(T/K + C)a chemical name

temperature range (K) ρ (T) (g/cm3)

EG PG 1-PrOH 2-PrOH

a

250−473 298.15−440.35 273.15−333.15 298.15−373.15

EG

278.3−495.44

PG

303.15−423.26

1-PrOH

303.35−369.95

2-PrOH

300.35−508.24

α

R2

−4

−0.0050 −0.00317 0.01625 0.01325

0.9982 (−7.56281x × 10 )·T/K + 1.33520 (−8.41068 × 10−4)·T/K + 1.28595 0.9977 (−8.16214 × 10−4)·T/K + 1.04275 0.9998 (−9.29444 × 10−4)·T/K + 1.05782 0.9996 Antoine equation constants A B 16.57308 −4772.25 ARD% = 1.93, MRD% = 13.49 19.02037 −6446.4 ARD% = 2.81, MRD% = 14.97 19.4937 −5518.6 ARD% = 1.24, MRD% = 5.53 15.0937 −2758.2 ARD% = 1.37, MRD% = 9.67

C −71.5087 −11.9729 1.55165 −91.79

Dependency of gas solubility on density for each solvent was obtained using GRK EoS and correlated with linear equation, ρ(m,T) = α.mH2S + ρ(T).

1-PrOH are obtained from Dejoz et al.53 with which those data for each pure solvent correlated with Antoine equation. The Antoine equations for vapor pressure with the set of constants for the four liquids are reported in Table 2. All experimental solubilities of H2S in EG, PG, 1-PrOH, and 2-PrOH are, respectively, reported in Tables 3, 4, 5, and 6. Temperature and pressure dependency of H2S solubility, have graphically been shown in Figures 1−4. As expected the amount of dissolved gas increases with increasing pressure and decreases with increasing temperature. In Figure 5, H2S solubility in EG, PG, 1-PrOH, 2-PrOH, and some other typical organic solvents such as diethylenglycol20 and triethylene glycol22 have been compared at T = 323.15 K. Comparison of results shows that H2S dissolves in mentioned organic solvents in the order of triethylene glycol > diethylenglycol > 2-PrOH ∼ 1-PrOH > PG > EG. As may be seen, solubility of H2S in triethylene glycol is higher than others. The experimental gas solubility data were evaluated to determine the Henry’s constant on the mole fraction scale for the solubility of gas in solvents at zero pressure, h(0) H,x

(atmospheric value) and the unknown volume was evacuated. Using the several measurements by this method both gas container and equilibrium cell volumes and their uncertainty were obtained equal to (107.1 ± 1.3 cm3) and (131.8 ± 1.5 cm3), respectively. According to eqs 5 and 6, the gas solubility is related to the amount of absorbed gas in the liquid phase and that of solvent. The average calculated uncertainties of these two parameters for 1-PrOH at T = 323.15 K were calculated to be u(nlH2S) = 0.003 mol and u(wSolvent) = 0.001g, therefore the uncertainty in molality and mole fraction according to ess 5, 6, and 8 are equal to 0.0890 mol/kg and 0.0040, respectively.

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RESULTS AND DISCUSSION Validation of the experimental apparatus and accuracy of data are recently investigated for CO2/dimethylformamid and also CO2/MDEA aqueous solution.40,41 As mentioned in Apparatus and Procedure, the amount of dissolved gas is calculated from the amount of gas charged to the cell by subtracting a correction for the amount of gas that is still present in the vapor phase. That correction is calculated assuming that the volume of the vapor phase is the difference between the cell volume and the volume of the unloaded solvent (which is known from the preparation of the solvent). Therefore, it is necessary to know the density of uncharged solvent. For this purpose, pure solvents mass density were taken from literature and correlated with linear equation in terms of temperature and reported in Table 2. Dortmund Data Bank Software and Separation Technology (DDBST)42 were used to obtain mass density correlation of pure EG and 2-PrOH. Mass density correlation for the case of PG was obtained from data reported by Atilhan et al.,43 Tsai et al.,44 and Sun et al.45 and that for 1-PrOH was obtained from data reported by Kumagai et al.46 and Assael et al.47 Density data correlated using linear equation and adjustable parameters associated with their coefficient correlation, R2, have been reported in Table 2. Vapor pressures of pure EG are obtained from Vasiltsova et al.,48 Verevkin,49 and (DDBST),42 and for PG the vapor pressures are obtained from Verlinde et al.,50 Steele et al.,51 and Chylinski et al.52 For the case of pure 2-PrOH, the vapor pressures are obtained from (DDBST)42 and those values for

(0) hH, x (T ) = lim

x→0

yH S ·ϕHg S·PT f ({y}, T , PT) 2 = lim 2 x→0 x x

(9)

where x is the mole fraction of acid gas in the solvent and f is the fugacity of acid gas in the gas phase at temperature T, total pressure PT, composition of gas phase {y}, and fugacity coefficient of H2S in gas phase, ϕHg 2S, which may be obtained using equation of state. (0) The obtained h(0) H,x and the estimated uncertainty u(hH,x) are given in Table 7. The influence of temperature on Henry’s constant was described by (0) n(hH, x /MPa) = A h, x (T /K) + B h, x +

C h, x (T /K)

(10)

Ah,x, Bh,x, and Ch,x are adjustable parameters reported in Table 8. The deviation between experimental and correlated Henry’s constant by means of eq 10 is comparable with experimental uncertainty for h(0) H,x given in Table 7. The variation with temperature of the solubility of solute expressed in Henry’s law constant is directly related to the thermodynamic properties of solution that in the case of gaseous C



Article

Table 3. Experimental Solubility of H2S in EGa T (K)

PH2S (MPa)

PT (MPa)

xH2S ± u (xH2S)

(xH2S)cor.

yH2S

ϕgH2S

molality (mol H2S/kg solvent)

303.15

0.086 0.179 0.379 0.512 0.810 0.969 1.079 0.091 0.191 0.400 0.620 0.770 0.950 1.069 1.279 0.103 0.209 0.445 0.695 0.900 1.079 1.232 1.500 0.114 0.229 0.491 0.767 0.988 1.199 1.377 1.623 0.131 0.269 0.573 0.903 1.167 1.419 1.629

0.086 0.179 0.379 0.512 0.810 0.969 1.079 0.091 0.191 0.400 0.620 0.770 0.950 1.069 1.279 0.103 0.209 0.445 0.695 0.900 1.079 1.232 1.500 0.114 0.229 0.491 0.767 0.988 1.199 1.377 1.623 0.132 0.270 0.574 0.904 1.168 1.420 1.630

0.0097 ± 0.0011 0.0202 ± 0.0015 0.0468 ± 0.0025 0.0619 ± 0.0031 0.1011 ± 0.0057 0.1240 ± 0.0050 0.1398 ± 0.0042 0.0090 ± 0.0011 0.0187 ± 0.0015 0.0388 ± 0.0025 0.0586 ± 0.0037 0.0760 ± 0.0057 0.0956 ± 0.0045 0.1087 ± 0.0042 0.1321 ± 0.0039 0.0085 ± 0.0011 0.0180 ± 0.0016 0.0371 ± 0.0025 0.0558 ± 0.0057 0.0733 ± 0.0058 0.0907 ± 0.0044 0.1044 ± 0.0043 0.1252 ± 0.0041 0.0081 ± 0.0011 0.0173 ± 0.0016 0.0355 ± 0.0026 0.0533 ± 0.0054 0.0704 ± 0.0051 0.0862 ± 0.0044 0.1000 ± 0.0044 0.1193 ± 0.0043 0.0076 ± 0.0011 0.0161 ± 0.0016 0.0332 ± 0.0027 0.0494 ± 0.0028 0.0652 ± 0.0048 0.0797 ± 0.0046 0.0919 ± 0.0047

0.0097 0.0202 0.0472 0.0626 0.1025 0.1258 0.1418 0.0090 0.0187 0.0390 0.0591 0.0768 0.0968 0.1104 0.1346 0.0085 0.0181 0.0374 0.0563 0.0742 0.0920 0.1062 0.1278 0.0081 0.0174 0.0358 0.0539 0.0713 0.0878 0.1021 0.1222 0.0076 0.0162 0.0334 0.0499 0.0661 0.0811 0.0938

0.9996 0.9998 0.9999 0.9999 1.0000 1.0000 1.0000 0.9992 0.9996 0.9998 0.9999 0.9999 0.9999 0.9999 0.9999 0.9984 0.9992 0.9996 0.9997 0.9998 0.9998 0.9998 0.9998 0.9970 0.9986 0.9993 0.9995 0.9996 0.9996 0.9997 0.9997 0.9910 0.9956 0.9977 0.9984 0.9987 0.9989 0.9990

0.9943 0.9880 0.9720 0.9632 0.9423 0.9318 0.9254 0.9942 0.9879 0.9747 0.9620 0.9512 0.9398 0.9328 0.9214 0.9941 0.9875 0.9740 0.9610 0.9492 0.9381 0.9299 0.9184 0.9941 0.9873 0.9737 0.9605 0.9481 0.9372 0.9281 0.9163 0.9939 0.9871 0.9732 0.9601 0.9475 0.9363 0.9272

0.1578 0.3322 0.7910 1.0631 1.8121 2.2806 2.6184 0.1463 0.3070 0.6504 1.0029 1.3252 1.7031 1.9649 2.4523 0.1381 0.2953 0.6208 0.9521 1.2744 1.6071 1.8781 2.3058 0.1316 0.2836 0.5930 0.9071 1.2201 1.5198 1.7902 2.1825 0.1234 0.2636 0.5533 0.8373 1.1237 1.3953 1.6305

313.15

323.15

333.15

353.15

a

The standard uncertainty (u) are u(T) = 0.10 K and u(Pt) = 0.003 MPa.

solutes at low pressures is practically identical to the thermodynamic properties of solution. The Gibbs energy of solution, corresponding to the change in Gibbs energy when the solute is transferred at constant temperature from the pure perfect gas at the standard pressure to the standard state of infinite dilution of the solute in the solvent is given by ⎛ h (0) ⎞ H,x Δsol Gm∞, x = RT ln⎜⎜ 0 ⎟⎟ ⎝ P ⎠

Δsol Sm∞, x =

T

(13)

The pressure range considered in this work is not too high to cause Henry’s law constant to be a strong function of pressure and Henry’s law is weakly dependent on pressure under the specified conditions. Therefore, it does not give rise to large errors if one ignores this pressure dependency. Equations 10−13 were used to estimate the changes of the partial molar Gibbs ∞ energy ΔsolG∞ m,x, the partial molar enthalpy ΔsolHm,x, the partial ∞ molar entropy ΔsolSm,x of gas when it is transferred from the ideal gas state at temperature T, and standard pressure P = P0 = 0.1 MPa to its reference state in the liquid solvent (i.e, a one molal solution of the gas in the particular solvent at temperature T where the dissolved gas experiences the same interactions as in infinite dilution). These properties are also given in Table 7. As it can be seen, the ΔsolG∞ m,x values are positive and increase with temperature in a similar manner for the solubility of gas in ∞ solvents. The ΔsolH∞ m,x and ΔsolSm,x values are negative. Because of probable hydrogen bonding interaction and also the number of

(11)

where P0 is the standard state pressure. The partial molar differences in enthalpy and entropy between the two states can be obtained by calculating the corresponding partial derivatives of the Gibbs energy with respect to temperature Δsol Hm∞, x = −T 2

(Δsol Hm∞, x − Δsol Gm∞,x )

∞ ⎡ ⎛ h (0) ⎞⎤ ∂ ∂ ⎛ Δsol Gm , x ⎞ H,x ⎟ = −RT 2 ⎢ln⎜⎜ 0 ⎟⎟⎥ ⎜ ∂T ⎝ T ∂T ⎢⎣ ⎝ P ⎠⎥⎦ ⎠

(12) D



Article

Table 4. Experimental Solubility of H2S in PGa T (K)

PH2S (MPa)

PT (MPa)

xH2S ± u(xH2S)

(xH2S)cor.

yH2S

ϕgH2S


303.15

0.082 0.224 0.376 0.524 0.691 0.872 0.089 0.259 0.431 0.602 0.797 1.014 0.099 0.29 0.486 0.679 0.895 1.141 0.11 0.32 0.54 0.753 0.997 1.28 0.121 0.35 0.589 0.824 1.082 1.377 0.133 0.378 0.638 0.892 1.163 1.468

0.082 0.224 0.376 0.524 0.691 0.872 0.089 0.259 0.431 0.602 0.797 1.014 0.099 0.290 0.486 0.679 0.895 1.141 0.110 0.320 0.540 0.753 0.997 1.280 0.122 0.351 0.590 0.825 1.083 1.378 0.134 0.379 0.639 0.893 1.164 1.469

0.0152 ± 0.0019 0.0421 ± 0.0041 0.0709 ± 0.0060 0.0975 ± 0.0058 0.1268 ± 0.0053 0.1585 ± 0.0050 0.0150 ± 0.0018 0.0402 ± 0.0041 0.0680 ± 0.0060 0.0934 ± 0.0058 0.1213 ± 0.0054 0.1522 ± 0.0051 0.0145 ± 0.0018 0.0386 ± 0.0041 0.0652 ± 0.0061 0.0896 ± 0.0058 0.1167 ± 0.0055 0.1465 ± 0.0052 0.0139 ± 0.0018 0.0372 ± 0.0041 0.0627 ± 0.0061 0.0862 ± 0.0059 0.1121 ± 0.0055 0.1415 ± 0.0052 0.0133 ± 0.0018 0.0356 ± 0.0041 0.0603 ± 0.0061 0.0803 ± 0.0059 0.1087 ± 0.0056 0.1369 ± 0.0053 0.0124 ± 0.0018 0.0336 ± 0.0041 0.0570 ± 0.0062 0.0784 ± 0.0060 0.1035 ± 0.0057 0.1300 ± 0.0054

0.0153 0.0422 0.0713 0.0981 0.1280 0.1601 0.0150 0.0403 0.0684 0.0941 0.1225 0.1540 0.0145 0.0388 0.0656 0.0904 0.1180 0.1484 0.0139 0.0373 0.0631 0.0870 0.1135 0.1436 0.0133 0.0358 0.0607 0.0838 0.1102 0.1391 0.0124 0.0338 0.0575 0.0794 0.1050 0.1324

0.9991 0.9997 0.9998 0.9999 0.9999 0.9999 0.9982 0.9993 0.9996 0.9997 0.9998 0.9998 0.9967 0.9987 0.9992 0.9994 0.9996 0.9996 0.9941 0.9978 0.9986 0.9990 0.9992 0.9993 0.9899 0.9961 0.9977 0.9982 0.9986 0.9988 0.9829 0.9935 0.9961 0.9971 0.9977 0.9980

0.9947 0.9848 0.9738 0.9634 0.9520 0.9398 0.9943 0.9843 0.9727 0.9620 0.9501 0.9371 0.9941 0.9837 0.9720 0.9609 0.9485 0.9349 0.9939 0.9834 0.9715 0.9602 0.9476 0.9333 0.9939 0.9833 0.9712 0.9598 0.9467 0.9323 0.9940 0.9836 0.9718 0.9607 0.9475 0.9334

0.2028 0.5776 1.0029 1.4198 1.9084 2.4754 0.2001 0.5504 0.9589 1.354 1.8142 2.3594 0.1934 0.5277 0.9166 1.2934 1.7363 2.2558 0.1853 0.5078 0.8791 1.2397 1.6593 2.1662 0.1771 0.4851 0.8433 1.1475 1.6028 2.0846 0.165 0.4569 0.7944 1.118 1.5173 1.9638

313.15

323.15

333.15

343.15

353.15

a


hydrogen bonding between H2S and the −OH group of the solvents, the magnitudes of ΔsolH∞ m,x values are greater for solubility of H2S in the PG and EG than PrOHs. The ΔsolS∞ m,x values show the degree of ordering in solution associated with the gas dissolution. It can be seen from Table 7 that more ordering occurs with H2S solubility in PG and GE than that in PrOHs. The comparison on solubility capacity may be carried out on the basis of molality scale; in this case, Henry’s constant in mole fraction scale could be correlated with via ‐1 (0) (0) hH, m /MPa · kg = hH, x /MPa ·

MSolvent 1000

the solubility increase with the deviations lower than 2% that is comparable with uncertainty values of solubility. It is worth noting that the effect of loaded liquid phase density on solubility values were experimentally investigated and the comparison of solubility values obtained from density of fresh (unloaded) solution (or liquid phase) and those obtained from density of loaded solution shows that data extracted from the isochoric saturation method are validated.54,55 Modeling. Two models were used to correlate the experimental results for the solubility of a single gas in solvents. The Generic Redlich−Kwong Cubic EoS. A generic Redlich−Kwong type of cubic equation of state (GRK EoS), was proposed by Shiflett and Yokozeki31−33 to correlate the solubility of gases in an ionic liquid. For a pure component, the GRK EoS is

(14)

For a more realistic estimation, volume change of liquid phase due to gas loading has been considered using densities of the charged solutions obtained by equation of state and solubility data have been recalculated using eq 7, (xH2S)Cor. Corrected solubility data have been reported in Tables 3−6, and densities of charged solutions were correlated using linear equation in terms of temperature and molality and reported in Table 2, as well. Comparisons of data in Tables 3−6 between corrected and uncorrected solubility data show that volume expansion causes

P=

a(T ) RT − υ−b υ(υ + b)

a(T ) = 0.427480 E

R2TC2 α (T ) PC

(15)

(16) DOI: 10.1021/acs.jced.5b00680 J. Chem. Eng. Data XXXX, XXX, XXX−XXX


Article

Table 5. Experimental Solubility of H2S in 1-PrOHa T (K) 303.15

PH2S (MPa) 0.066 0.159 0.264 0.427 0.646 0.077 0.181 0.301 0.493 0.729 0.086 0.203 0.336 0.552 0.820 0.095 0.226 0.372 0.611 0.910 0.248 0.410 0.672 0.999 0.271 0.448 0.730 1.094

313.15

323.15

333.15

343.15

353.15

a

PT (MPa) 0.070 0.163 0.268 0.431 0.650 0.084 0.188 0.308 0.500 0.736 0.098 0.215 0.348 0.564 0.832 0.115 0.246 0.392 0.631 0.930 0.281 0.443 0.705 1.032 0.322 0.499 0.781 1.145

xH2S ± u(xH2S) 0.0177 ± 0.0027 0.0405 ± 0.0038 0.0666 ± 0.0047 0.1074 ± 0.0044 0.1543 ± 0.0040 0.0172 ± 0.0027 0.0398 ± 0.0038 0.0653 ± 0.0047 0.1051 ± 0.0044 0.1516 ± 0.0041 0.0169 ± 0.0027 0.0390 ± 0.0038 0.0641 ± 0.0047 0.1032 ± 0.0044 0.1489 ± 0.0041 0.0166 ± 0.0027 0.0382 ± 0.0038 0.0630 ± 0.0047 0.1014 ± 0.0045 0.1464 ± 0.0041 0.0374 ± 0.0027 0.0617 ± 0.0038 0.0996 ± 0.0047 0.1439 ± 0.0045 0.0363 ± 0.0022 0.0599 ± 0.0047 0.0970 ± 0.0048 0.1400 ± 0.0047

(xH2S)cor. 0.0177 0.0406 0.0667 0.1077 0.1548 0.0172 0.0398 0.0654 0.1054 0.1522 0.0169 0.0390 0.0643 0.1035 0.1496 0.0166 0.0383 0.0631 0.1018 0.1471 0.0374 0.0618 0.0999 0.1447 0.0364 0.0601 0.0974 0.1409

ϕgH2S 0.9954 0.9892 0.9817 0.9702 0.9581 0.9951 0.9885 0.9807 0.9687 0.9557 0.9947 0.9878 0.9797 0.9672 0.9536 0.9945 0.9872 0.97882 0.9660 0.9519 0.9867 0.9781 0.9650 0.9504 0.9866 0.9778 0.9645 0.9498

yH2S 0.9050 0.9591 0.9756 0.9850 0.9893 0.8607 0.9381 0.9628 0.9767 0.9834 0.8071 0.9105 0.9452 0.9655 0.9753 0.7449 0.8757 0.9225 0.9506 0.9645 0.8332 0.8938 0.9315 0.9505 0.7827 0.8581 0.9073 0.9323

molality (mol H2S/kg solvent) 0.2998 0.7024 1.1873 2.0022 3.0360 0.2912 0.6897 1.1625 1.9543 2.9734 0.2861 0.6753 1.1397 1.9149 2.9112 0.2809 0.6609 1.1188 1.8777 2.8539 0.6465 1.0942 1.8407 2.7970 0.6268 1.0602 1.7875 2.7088


b = 0.08664

RTC PC

kij =

(17)

The mathematical form of α(T) as used by Shiflett and Yokozeki is

∑ λk(Tr‐1 − Tr)k k=0

(18)

Pc and Tc are the critical pressure and critical temperature of the pure component, respectively, υ is the molar volume, Tr = T/Tc is the reduced temperature, and λk’s are adjustable parameters. The critical properties for pure H2S and for EG, 1-PrOH, 2-PrOH, and PG are from literature43,56−58 and reported in Table 9. The parameters λ0 through λ3 were taken from Shiflett and Yokozeki59 for H2S, whereas for solvents used in this work they were considered as adjustable parameters and either set to zero (λ2 and λ3) or were obtained through fitting together with the binary parameters of the model to the new gas solubility data (see below). Table 9 shows all pure component parameters. The EoS was extended to mixtures by applying the modified van der Waals-Berthelot mixing rule proposed by Yokozeki60

(ARD)P % =

∑

aiaj fij (T )(1 − kij)xixj

i,j=1

1 b= 2

∑ i=1

Picor(T , x) − Piexp(T , x) Piexp(T , x)

(23)

Krichevsky−Ilinskaya Equation. The solubility of a single gas in pure physical solvents is described by the Krichevsky− Ilinskaya equation34 on the mole fraction scale

(20)

⎛ vH∞ S(PT − P s) ⎞ (0) ⎜⎜ 2 ⎟⎟xγx = f ({y}, T , PT) ( )exp hH, T x RT ⎝ ⎠

τij T

N

(24)

∑ (bi + bj)(1 − mij)(1 − kij)xixj

fij (T ) = 1 +

100 N

(19)

N i,j=1

(22)

⎞ ⎛ P cor(T , x) − P exp(T , x) i (MRD)P % = max⎜⎜ i × 100⎟⎟ exp Pi (T , x) ⎠ ⎝

N

a(T ) =

l jixi + lijxj

where τij = τji, τii, = 0, mij = mji, mii = 0, and kii = 0. There are four interaction parameters per binary system: lij, lji, mij, and τij,. These interaction parameters were adjusted to the experimental gas solubility data and the pure component parameters (λ0 and λ1) of four pure solvents were adjusted to their own vapor pressure. Table 10 gives the numerical values of the binary interaction parameters and also the quality of correlation, using the average relative deviation, (ARD)P%, and the maximum relative deviation, (MRD)P%, of pressure, which is defined in eqs 23 and 24. The results of KI correlation have been graphically shown in Figures 1−5, as well.

≤3

α (T ) =

lijl ji(xi + xj)

(21) F

(25)



Article

Table 6. Experimental Solubility of H2S in 2-PrOHa T (K)

PH2S (MPa)

PT (MPa)

xH2S ± u(xH2S)

(xH2S)cor.

yH2S

ϕgH2S


303.15

0.115 0.244 0.358 0.587 0.737 0.131 0.279 0.4 0.662 0.854 0.147 0.313 0.449 0.742 0.961 0.163 0.346 0.497 0.823 1.066 0.177 0.379 0.542 0.903 1.171 0.19 0.41 0.587 0.984 1.271

0.123 0.252 0.366 0.595 0.745 0.145 0.293 0.414 0.676 0.868 0.171 0.337 0.473 0.766 0.985 0.202 0.385 0.536 0.862 1.105 0.239 0.441 0.604 0.965 1.233 0.284 0.504 0.681 1.078 1.365

0.0283 ± 0.0041 0.0607 ± 0.0043 0.0856 ± 0.0045 0.1442 ± 0.0041 0.1896 ± 0.0038 0.0277 ± 0.0041 0.0593 ± 0.0043 0.0842 ± 0.0045 0.1416 ± 0.0042 0.1856 ± 0.0038 0.0271 ± 0.0041 0.0581 ± 0.0043 0.0825 ± 0.0045 0.1391 ± 0.0042 0.1824 ± 0.0039 0.0266 ± 0.0041 0.0570 ± 0.0043 0.0809 ± 0.0045 0.1367 ± 0.0042 0.1795 ± 0.0039 0.0260 ± 0.0039 0.0558 ± 0.0043 0.0794 ± 0.0045 0.1343 ± 0.0042 0.1767 ± 0.0039 0.0254 ± 0.0041 0.0543 ± 0.0043 0.0774 ± 0.0045 0.1309 ± 0.0043 0.1728 ± 0.0040

0.0284 0.0608 0.0858 0.1447 0.1905 0.0278 0.0594 0.0844 0.1422 0.1866 0.0272 0.0582 0.0827 0.1398 0.1835 0.0266 0.0571 0.0812 0.1374 0.1807 0.0261 0.0559 0.0798 0.1352 0.1781 0.0254 0.0545 0.0777 0.1318 0.1743

0.8904 0.9484 0.9633 0.9774 0.9820 0.8444 0.9240 0.9457 0.9662 0.9730 0.7889 0.8928 0.9225 0.9514 0.9612 0.7265 0.8546 0.8934 0.9324 0.9459 0.6582 0.8093 0.8582 0.9088 0.9268 0.5875 0.7567 0.8161 0.8795 0.9030

0.9920 0.9827 0.9756 0.9601 0.9498 0.9915 0.9817 0.9742 0.9580 0.9470 0.9910 0.9808 0.9730 0.9561 0.9445 0.9907 0.9801 0.9720 0.9545 0.9424 0.9908 0.9796 0.9713 0.9532 0.9406 0.9912 0.9795 0.9710 0.9527 0.9396

0.4846 1.0753 1.5577 2.8038 3.8931 0.4741 1.0490 1.5299 2.7449 3.7922 0.4635 1.0264 1.4962 2.6886 3.7123 0.4547 1.0058 1.4647 2.6349 3.6403 0.4442 0.9834 1.4352 2.5814 3.5714 0.4337 0.9554 1.3960 2.5062 3.4761

313.15

323.15

333.15

343.15

353.15

a


Figure 1. Experimental data for solubility of H2S in 1,2-ethanediol (EG) at different temperatures and pressure (points) compared with KI model (solid lines) and those data reported by Jou et al.17 G



Article

Figure 2. Experimental data for solubility of H2S in 1,2-propanediol (PG) system at different temperatures and pressure (points) compared with KI model (solid lines).

Figure 3. Experimental data for solubility of H2S in 1-propanol (1-PrOH) system at different temperatures and pressure (points) compared with KI model (solid lines).

⎛ f ({y}, T , PT) ⎞ ln⎜ ⎟ ⎝ ⎠ x =

(0) ln(hH, x (T ))

+

vH∞2S(PT − P s) RT

where A is binary parameters and xs is mole fraction of solvent. The influence of temperature on binary interaction parameter is approximated by + ln(γx)

(26)

A=

where γx is the activity coefficient of gas on the mole fraction scale and vH∞2S is the molar volume of dissolved gas at infinite dilution. The activity coefficient, γx, was calculated from two-suffix Margules equation34 on the mole fraction scale ln γm = A(xs 2 − 1)

A 0 + A1 T(K)

(28)

Prausnitz et al.35 have discussed that the application of that type ∞ of equation needs to have information about h(0) H,x and v . Bender 61 62 et al. and also Deshmukh−Mather have presented the connection of (KI) equation and Peng−Robinson equation of state to obtain the parameters of KI equation from the equation of state.

(27) H



Article

Figure 4. Experimental data for solubility of H2S in 2-propanol (2-PrOH) system at different temperatures and pressure (points) compared KI model (solid lines).

Figure 5. Comparison of solubility of H2S in EG, 1-PrOH, 2-PrOH, PG, diethylenglycol,20 and triethylene glycol22 at that given temperature.

The Henry’s law constants h(0) H,x were calculated from eq 9 and the partial molar volumes of solutes at infinite dilution were calculated by GRK EoS and listed in Table 9. Parameters A0 and A1 were adjusted to minimize the sum of percent relative deviation between the calculated and the experimental results for the pressure of the gas. The results of the correlations (interaction parameters) are given in Table 10. The quality of the KI correlation is reported using the average relative deviation ARD% and the maximum relative deviation MRD% on pressure

and also mole fraction in Table 10 as defined by eqs 23 and 24 and graphically shown in Figures 1−5. In Table 11, H2S solubility in EG reported by Jou et al.,17 Afzal et al.30 and Short et al.63 at some given temperatures have been compared with calculated mole fraction values obtained using KI correlation in this work. As may be seen except for four data points marked with star in Table 11, the rest of the data are within the mole fraction uncertainty reported in Table 3. As may be seen from Table 11 and Figure 1, our reported data I



Article

Table 7. Thermodynamic Properties of H2S Solubility in EG, PG, 1-PrOH, and 2-PrOHa T (K)

h(0) H,x (MPa)

h(0) H,m (MPa.kg/mol)

ΔsolG∞ m,x (kJ/mol)

ΔsolH∞ m,x (kJ/mol)

ΔsolS∞ m,x (J/mol)

v∞ (cm3/mol)

−10.04 −10.71 −11.41 −12.13 −13.63

−51.20 −53.79 −56.03 −58.05 −62.43

43.10 ± 0.15 43.52 ± 0.20 44.15 ± 0.25 44.77 ± 0.25 46.15 ± 0.30

−11.18 −11.93 −12.71 −13.51 −14.33 −15.18 −9.44 −10.08 −10.73 −11.41 −12.11 −12.83

−50.69 −53.32 −55.78 −58.12 −60.54 −62.99 −42.22 −44.67 −46.76 −48.81 −50.88 −52.87

44.77 ± 0.30 45.51 ± 0.40 46.30 ± 0.35 47.13 ± 0.40 48.00 ± 0.45 48.89 ± 0.40 43.12 ± 0.80 44.21 ± 0.85 45.41 ± 0.90 46.73 ± 0.95 49.11 ± 0.95 50.65 ± 1.00

−9.38 −10.01 −10.66 −11.32 −12.01 −12.72

−42.63 −44.46 −46.86 −48.95 −50.87 −52.67

47.98 ± 1.00 49.33 ± 1.00 50.83 ± 1.05 52.49 ± 1.10 54.32 ± 1.15 56.34 ± 1.20

1-PrOH - H2S 303.15 313.15 323.15 333.15 353.15

8.79 ± 0.35 10.53 ± 0.30 12.09 ± 0.25 13.52 ± 0.20 17.60 ± 0.20

0.546 0.654 0.751 0.839 1.093

303.15 313.15 323.15 333.15 343.15 353.15 303.15 313.15 323.15 333.15 343.15 353.15

5.26 ± 0.09 6.23 ± 0.07 7.24 ± 0.08 8.28 ± 0.07 9.58 ± 0.09 11.10 ± 0.11 3.87 ± 0.07 4.49 ± 0.05 5.10 ± 0.03 5.75 ± 0.05 6.52 ± 0.05 7.31 ± 0.09

0.400 0.474 0.551 0.631 0.729 0.845 0.236 0.272 0.311 0.351 0.397 0.445

303.15 313.15 323.15 333.15 343.15 353.15

4.08 ± 0.15 4.49 ± 0.15 5.31 ± 0.17 6.05 ± 0.16 6.75 ± 0.17 7.42 ± 0.19

0.248 0.281 0.318 0.359 0.406 0.459

EG-H2S 5.48 6.13 6.70 7.21 8.42 PG-H2S 4.18 4.76 5.32 5.86 6.45 7.07 3.36 3.91 4.38 4.85 5.35 5.84 2-PrOH-H2S 3.54 3.91 4.49 4.99 5.45 5.88

a T, temperature; h, Henry’s law constant in both mole fraction and molality base; v∞, partial molar volume at infinite dilution obtained from GRK ∞ ∞ EoS; ΔsolG∞ m,x, Gibbs free energy of solution; ΔsolHm,x, enthalpy of solution; ΔsolSm,x, entropy of solution at infinite dilution (all in mole fraction scale).

Table 8. Numerical Values of the Parameters of Equation 9 Associated with ARD% and MRD% Ah,x 0.013142

0.01243

Bh,x

Ch,x

EG-H2S −1.77302 ARD% = 1.20% MRD% = 3.81% 1-PrOH-H2S −2.41156 ARD% = 0.69% MRD% = 3.50%

Ah,x

−0.02057

Bh,x

0.014636

6.825845

0.012223

Ch,x

PG-H2S −2.76151 ARD% = 0.35% MRD% = 0.96% 2-PrOH-H2S −2.28267 ARD% = 0.96% MRD% = 1.69%

−0.01695

−5.26377

Table 9. EoS Constants for Pure Compounds Used in Present Study molar mass (g/mol) Tc (K) Pc (MPa) λ0 λ1 λ2 λ3

H2S

EG

PG

1-PrOH

2-PrOH

34.08 373.60 9.008 0.99879 0.33206 −0.049417 0.0046387

62.068 719 8.2 0.5329 0 0 0

76.09 676.4 5.9 0.56549 0 0 0

60.093 536.8 5.169 0.60636 0 0 0

60.093 508.15 4.755 0.63549 0 0 0

■

have acceptable comparability with data reported by Jou et al.17 at the pressure lower than 1.5 MPa. Owing to the fact that the KI model has been correlated with data points with pressure lower than 1.5 MPa and temperature from (303.15 to 353.15) K range, deviation has been revealed at higher pressure. The same result has been seen for Afzal et al.30 and Short et al.63 in Table 11, as well.

CONCLUSION In this investigation, we have measured the solubility of H2S as a function of partial pressure of acid gas in 1,2-ethanediol, 1-propanol, 2-propanol, and 1,2-propanediol over a wide temperature range (between 303.15 and 353.15 K) and pressure from vapor pressure of solvent up to about 1.5 MPa. Results show that H2S dissolves in mentioned organic solvents in the J



Article

Table 10. Optimal Binary Interaction Parameters in GRK and KI Equation, and Also (ARD)P%, (MRD)P% of Both Models, Accompany with (ARD)x% and (MRD)x% of KI Model l12 l21 τ12 = τ21 m12 = m21 A0 A1 (ARD)P% (GRK) (MRD)P% (GRK) (ARD)P% (KI) (MRD)P% (KI) (ARD)x% (KI) (MRD)x% (KI)

H2S/EG

H2S/PG

H2S/1-PrOH

H2S/2-PrOH

0.189041 0.169569 30.569 −0.20134 −3.9483 1467.09 2.11% 7.24% 2.93% 8.28% 2.98% 7.62%

0.175698 0.123198 30.49372 −0.20475 0.70359 −196.55 1.48% 6.32% 2.25% 6.17% 2.24% 5.83%

0.111073 0.018197 0 −0.08568 0.18362 −57.913 2.63% 6.56% 1.24% 7.80% 1.21% 7.28%

0.114909 0.017662 0 −0.0979 0.59027 −129.39 2.13% 7.59% 1.96% 6.27% 1.96% 5.54%

Results in Figures 1−5 and ARD% and MRD% in Table 8 show that both models have comparable abilities in correlation of gas pressure.

Table 11. H2S Solubility in EG Reported in Open Literature at Three Given Temperatures That Have Been Compared with Calculated Mole Fraction Values Obtained Using KI Prediction in This Work T/K 298.15

323.15

348.15

a

P 0.00324 0.0055 0.054 0.153 0.677 1.03 1.56 2.03 0.0032 0.00497 0.0356 0.186 0.621 1.89 3.04 3.52 0.0049 0.0564 0.148 0.629 2.39 3.49 4.73 5.66

298.15 333.15

0.1013 0.1013

298.22 29816 298.16 298.06 307.93 322.77 332.11

0.353 0.659 0.971 1.077 1.265 1.549 1.734

x Jou et al.17 0.000511 0.000901 0.007649 0.02165 0.09558 0.1535 0.2532 0.4055 0.000335 0.000499 0.00316 0.01468 0.05057 0.1676 0.3104 0.4494 0.000337 0.00335 0.00848 0.03558 0.1412 0.2057 0.3287 0.482 Short et al.63 0.0122 0.00718 Afzal et al.30 0.044 0.084 0.129 0.145 0.134 0.118 0.120

x (KI model)

(PRD)x%

Δx

0.00046 0.00064 0.0064 0.0183 0.0875 0.1414 0.2360 0.3367 0.0003 0.0004 0.0030 0.0158 0.0541 0.1767 0.3082 0.3941 0.0003 0.0034 0.0089 0.0374 0.1322 0.1826 0.2302 0.2590

11.00 28.51 16.77 15.54 8.46 7.91 6.81 16.98 19.40 16.03 4.99 7.22 4.85 2.28 15.75 33.32 11.57 1.79 5.39 5.05 6.39 11.21 29.95 46.27

0.0001 0.0003 0.0013 0.0034 0.0081 0.0121a 0.0172a 0.0688a 0.0001 0.0001 0.0002 0.0011 0.0036 0.0091a 0.0022 0.0553a 0.0000 0.0001 0.0005 0.0018 0.0090a 0.0231a 0.0985a 0.2230a

0.0128 0.0078

5.25 6.13

0.0006 0.0004

0.0434 0.0850 0.1319 0.1493 0.1459 0.1350 0.128

1.39 1.20 2.22 2.96 8.87 14.3 6.67

0.0006 0.0010 0.0029 0.0043 0.0119a 0.0169a 0.008a

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AUTHOR INFORMATION

Corresponding Author

*E-mail: [email protected]; [email protected]. Tel: 98 21-48252467. Notes

The authors declare no competing financial interest.

■

ACKNOWLEDGMENTS We are thankful to the Research Council of the Research Institute of Petroleum Industry (R.I.P.I.) and the Research and Development of the National Iranian Oil Company (N.I.O.C.) for their support of this work.

■

Data being out of mole fraction uncertainty interval reported in Table 3.

orderof 1-PrOH ∼ 2-PrOH > PG > EG. The experimental data were correlated by using (1) Krichevsky−Ilinskaya equation, and (2) a generic Redlich−Kwong cubic equation of state. K

LIST OF SYMBOLS NIST; National Institute of Standards and Technology DDBST; Dortmund Data Bank Software and separation Technology PG; 1,2-Propylene glycol EG; Ethylene glycol DEG; Diethylenglycol TEG; Triethylene glycol DDBST; Dortmund Data Bank Software and Separation Technology KI; Krichevsky-Ilinskaya equation RK EoS; Redlich−Kwong equation of state GRK; Generic Redlich-Kowang equation of state R; Universal gas constant Vgc; Volume of the gas container (or gas sample) Vg; Gas-phase volume in the equilibrium cell Zi and Zf; Compressibility factors of the initial and final state in the gas container Ta; Ambient temperature P0; Initial pressure of solution PT; Total absolute pressure PVP or Ps; Vapor pressure of pure solvent PH2S; Partial pressure of H2S at equilibrium state ngag; Amount of acid gas in the gas phase at equilibrium state nlag; Amount of acid gas in the liquid phase at equilibrium state xH2S; Mole fraction of H2S in liquid phase yH2S; Mole fraction of H2S in gas phase u(n)i; Uncertainty of amount of species i u(xH2S); Uncertainty of mole fraction of hydrogen sulfide DOI: 10.1021/acs.jced.5b00680 J. Chem. Eng. Data XXXX, XXX, XXX−XXX


Article

mj; Molality of component j, mol·kg−1 wSolvent; Mass of solvent charge into cell ρag; Density of acid gas in gas phase at equilibrium state ρ; Density of pure liquid in (g/cm3) Tr; Reduced temperature Tc; The critical temperature Pc; The critical pressure α(T); Temperature dependent parameter in RK equation of state b; RK covolume constant R2; Correlation coefficients ARD; Average of relative deviations MRD; Maximum relative deviation PRD; Percent relative deviation h(0) H,x; The Henry’s law constant on mole fraction base h(0) H,m; The Henry’s law constant on molality base f H2S (T,p); Fugacity of H2S in gas phase ϕHg 2S; Fugacity coefficient of H2S in gas phase γx; The activity coefficient of gas on the mole fraction scale vH∞2S; Molar volume of dissolved gas at infinite dilution λk, lij, lji, mij, τij; Adjustable parameters in GRK EoS ΔsolG∞ m,x; The partial molar Gibbs free energy of solubility at reference state ΔsolH∞ m,x; The partial molar enthalpy of solubility at reference state ΔsolS∞ m,x; The partial molar entropy of solubility at reference state

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Solubility of Hydrogen Sulfide in Ethanediol, 1, 2-Propanediol, 1

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