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Journal of Chemical & Engineering Data Article ⎧P= RT − Figure 6. Solubilities of CO2 in (ChCl/urea + water). Symbols are ⎪ (V − b) a T1/2V(V + b) Py φν =H x γ* CO2 CO2 CO2 CO2 CO2 (6a) where P is the pressure, yCO2 is the mole fraction of CO2 in the vaporphase,φν isthefugacitycoefficientofCO inthevapor phase, HCO2 is the Henry’s law constant, xCO2 is the CO2 mole fraction in the liquid phase, and γ* is the activity coefficient of CO2 CO2 in the liquid phase at the infinite dilution reference state. For the system studied in this work, the vapor pressure of ChCl/urea is negligible. Based on previous investigation,33 for H2O−CO2 system, the maximum water content in the vapor phase is less than 0.004 (mole fraction) at 323.15 K and 4.51 MPa. The effect of ChCl/urea upon is a “salt-in effect”, that is, the water content in the vapor phase decreases with increasing content of ChCl/urea in the liquid phase. Therefore, it is reasonable to assume that only CO2 exists in the vapor phase, thatis,yCO2 =1.Duringtheexperimentalmeasurements,itwas assumed that the water in the vapor phase was very low and was neglected. This discussion confirms the reliability of the measurements. Following this, the CO2 solubility in (ChCl/ CO2 2 urea + water) can be simplified as Pφν =H x γ* CO2 CO2 CO2 CO2 (6b) The Henry’s law constant of CO2 was expressed by ⎛V∞ P⎞ HCO (T, P) = HCO (T)exp⎜ CO2 ⎟ ⎝ RT ⎠ (7) H (T)=lim (Pφν /x ) 22 CO2 xi→0 CO2 CO2 (8) where HCO2 (T,P) is the Henry’s law constant of CO2 at system temperature and pressure, HCO2(T) is the Henry’s law constant of CO at zero pressure, and V∞ is the infinite dilution partial 2 CO2 volume of CO2 in solvent. The Redlich −Kwong (RK) equation of state was used to calculate the fugacity of CO2 in the vapor phase34 experimental data at different mole fractions of water: ■, 0.0185; ●, 0.0910; ▲, 0.183. Curve: results of NRTL-RK model. not notable, for example, at 308.2 K and 3.5 MPa, the solubility of CO2 is 0.152 when the mass fraction of water (wH2O) is 0.0185, and it decreases to 0.127 when wH2O = 0.183. With increasing temperature, the solubility of CO2 decreases, but the influence is small, for example, at 3.4 MPa and wH2O = 0.0185, the solubilities of CO2 are 0.152, 0.129, and 0.126 when the temperatures are 308.2 K, 318.2 K, and 328.2 K, respectively. The addition of water has an effect on the CO2 solubility in ChCl/urea but it decreases the viscosity of ChCl/urea significantly. The decrease of viscosity will enhance the heat and mass transfer and decrease the size of equipment, whereas the decrease of CO2 solubility will decrease the capacity and then increase the energy consumption in the CO2 separation process. Thus, a balance between viscosity and CO2 solubility should be considered in order to capture CO2 with a high efficiency. The CO2 solubility measured in this work can be represented with the following equation: ⎪ ⎪2 a 0.4278Tc ⎪A = R2T2.5 = PT2.5 2.5 ⎪ c ⎪ b 0.0867T ⎪B= = c ⎪ RT PT ⎨c ⎪2 ⎪Z = 1 ⎪ (1 − h) − (A /B)h (1 + h) 3349 dx.doi.org/10.1021/je500320c | J. Chem. Eng. Data 2014, 59, 3344−3352 ⎪Z = PV ⎪ RT ⎪ BP b ⎪h= = ⎩ZV (9) where a, b, A, and B are parameters calculated from the critical temperature and pressure. The critical temperature and pressure of CO2 were obtained from NIST webbook35 with the values of 304.2 K and 7.38 MPa, respectively. The fugacity coefficient of CO2 was calculated with 2 ln φ = Z − 1 − ln(Z − BP) − (A /B)ln(1 + BP/Z) (10)PDF Image | CO2 Separation with Ionic Liquids
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