The solubility of hydrogen sulfide in three ionic liquids, 1-butyl-3-methylimidazolium hexafluorophosphate ([bmim][PF 6 ]), 1-butyl-3-methylimidazolium tetrafluoroborate ([bmim][BF 4 ]), and 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([bmim][Tf 2 N]), at temperatures ranging from (303.15 to 343.15) K and pressures up to 1 MPa was determined. The solubility data were correlated using the Krichevsky-Kasarnovsky equation, and Henry's law constants at different temperatures were obtained. From the solubility data, the partial molar thermodynamic functions of solution such as Gibbs energy, enthalpy, and entropy were calculated. Comparison showed that the solubility of H 2 S in these three ionic liquids was in sequence: [bmim][Tf 2 N] > [bmim][BF 4 ] > [bmim][PF 6 ].
Gaseous solubilities of carbon dioxide (1), hydrogen sulfide (2), and their binary mixture (x(2) ≈ 0.2, 0.5, 0.8) have been measured in the ionic liquid 1-octyl-3-methylimidazolium bis(trifluoromethyl)sulfonylimide ([C(8)mim][Tf(2)N]) at temperatures ranging from (303.15 to 353.15) K and at pressures under 2 MPa. The observed PTx solubility data were used to obtain Henry's law constants and correlated by three models: (1) the simple Krichevsky-Kasarnovsky (KK) equation, (2) a model comprised of the extended Henry's law and the Pitzer's virial expansion for the excess Gibbs free energy, and (3) the generic Redlich-Kwong (RK) cubic equation of state proposed for gas-ionic liquid systems. The correlations from the three models show quite good consistency with the experimental data for IL/CO(2) and IL/H(2)S binary mixtures within experimental uncertainties. For IL/CO(2)/H(2)S ternary mixtures, the RK model shows the best correlation with the experimental data. The comparison showed that the solubility of H(2)S is about two times as great as that of CO(2) in the ionic liquid studied in this work. It was further found, by comparison of the experimental data of this study with those of previous reports, that the solubility of H(2)S in [C(n)mim][Tf(2)N] ILs increases as the number of carbon atoms in the alkyl substituent of methylimidazolium cation, n, increases. In addition, quantum chemical calculations at DFT/B3LYP level of theory using 6-311+G(d) and 6-311++G(2d,2p) basis sets were performed on the isolated systems studied in this work to provide explanations from a molecular point of view for the observed experimental trends.
In this paper, oil recovery and permeability reduction of a tight sandstone core sample in miscible CO 2 flooding processes due to asphaltene deposition were studied using an Iranian bottom hole live oil sample in order to distinguish between the mechanical plugging and adsorption mechanisms of asphaltene involved in the interfacial interaction of the asphaltene/ mineral rock system. A novel experimental method was designed and proposed to measure the amount of deposited asphaltene due to different mechanisms using the cyclohexane or toluene reverse flooding and spectrophotometer. In this work, the bottom hole live oil sample was injected first to a long core and then CO 2 injection was performed which is close to reservoir conditions, whereas in the majority of previous works, the mixture of recombined oil (mixture dead oil and associated gas) and CO 2 was injected in a short core sample which is far from reservoir conditions. Then, the cyclohexane and toluene reverse flooding was performed, and the amount of deposited asphaltene was measured by spectrophotometer. It was found that by increasing the flow rate of injected CO 2 , pressure drop across the core increased significantly and then decreased. These significant increases in pressure drops indicate more asphaltene deposition and consequently more permeability reduction. Also, it has been found that 20−40% permeability reduction by asphaltene deposition was caused by adsorption mechanism in the CO 2 flooding process during a slow process, whereas 60−80% of formation damage is due to a mechanical plugging mechanism and takes place in a short time. Also, a modified model based on multilayer adsorption theory and four material balance equations (oil, asphaltene, light components, and water phase) was developed to account asphaltene adsorption in core sample during CO 2 flooding and the model was verified using experimental data obtained in this work. The results show that the developed model based on multilayer adsorption theory and four material balance equations is more accurate than those obtained from the monolayer adsorption theory and two material balance equations (the existing models) and is in good agreement with the experimental data reported in this work.
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