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Journal of Chemical & Engineering Data Article The NRTL model was used to represent the activity coefficient of CO2 in the liquid phase. The CO2 solubility was measured at a certain fixed molar ratio of water to ChCl/ urea. It was assumed that the solution with a fixed molar ratio of water to ChCl/urea was one pseudocomponent in the liquid phase. Based on this assumption, there are two components, that is, CO2 (1) and solvent (2), the mixture of ChCl/urea and water, in the liquid phase, and the activity coefficient of CO2 in the liquid phase can be calculated by the following equations: (11) G12 = exp(−ατ12)andG21 = exp(−ατ21) In this work, α was assumed to be 0.2, and the binary interaction parameters τ12 and τ21 were dependent on the temperature and water content and modeled by measured data are reliable, and we think that the data obtained in this work are reliable. Based on the obtained Henry’s constant, τ(i), τ(i), and V∞ 12 21 CO2 were set as adjustable parameters and obtained from the fitting of the CO2 solubility in ChCl/urea with water measured in this work. The fitted parameters are listed in Tables 5 and 6. The Table 6. Parameters for NRTL-RK Model ⎡2⎤ ⎛G⎞τG parameters τ12 (0) τ12 −14.6147 (1) τ12 175.847 τ(2) −176.112 12 τ(3) −16401.9 12 τ(4) −10229.3 12 τ(5) 30128.6 12 parameters (0) τ21 τ21 (1) τ21 τ(2) 21 τ(3) 21 τ(4) 21 τ(5) 21 −357.036 489.858 −104.946 155484 −248619 86311.6 lnγ=x2⎢τ⎜ 21 ⎟+ 12 12 ⎥ 1 2 21 2 ⎧τ ⎪ 12 ⎪ ⎪ ⎪ /T ⎨ ⎪τ ⎪ 21 ⎪ ⎩ comparison of the model results with the measured at 308.2 K, 318.2 K, and 328.2 K is shown in Figure 6, which shows that NRTL-RK model can be used to represent the CO2 solubility in ChCl/urea with water accurately. TheenthalpyofCO absorptionin(ChCl/urea+water)can 2 be further calculated from the following equations: ΔHabs = ΔHdis + (1 + n)ΔHex (14) 2⎛ ∂ln HCO2(T , P) ⎞ ΔHdis = −RT ⎜ ⎟ ⎝ ∂T ⎠ (15) (16) ⎢ ⎝x+xG⎠ (x+xG)⎥ ⎣1221 2112⎦ = τ(0) + τ(1)w 12 12 ChCl/urea + τ(2)w2 12 ChCl/urea experimental data + (τ(3) + τ(4)w + τ(5)w2 ) 12 12 ChCl/urea 12 ChCl/urea = τ(0) + τ(1)w 21 21 ChCl/urea + τ(2)w2 21 ChCl/urea + (τ(3) + τ(4)w + τ(5)w2 21 ChCl/urea ) 21 /T 21 ChCl/urea In modeling, H the measured CO2 solubility data (eq 8) with the corresponding fugacity coefficient of CO2 calculated with RK equation of state. The obtained HCO2(T) at different temper- atures are listed in Table 5. HCO2(T) changes slightly with water Table 5. Henry’s Law Constants (HCO2) and Infinite Dilution Partial Volume (V∞ ) of CO in the Mixture of ChCl/Urea (1) + Water (2)a CO2 2 (T) was obtained by an extrapolation of CO2 (13) 0.0185 14.2 16.2 20.3 0.0910 16.6 20.9 22.3 0.183 18.0 22.1 23.8 83.9 84.0 84.1 where ΔHabs is the enthalpy of CO2 absorption, ΔHdis is the enthalpy of CO2 dissolution, ΔHex is the excess enthalpy, and n is the moles of solution to absorb one mole of CO2. The enthalpy of CO2 absorption in (ChCl/urea + water) at 308.2 K with different water contents is illustrated in Figure 7. The excess enthalpy is positive when the mass fractions of water is 0.0185 are 0.0910, which means a positive deviation of ideal state. When the mass fraction of water is 0.183, the excess enthalpy is negative. The magnitude of the CO2 dissolution enthalpy decreases with increasing water content. Compared to the excess enthalpy, the CO2 dissolution enthalpy is dominant, and the contribution to the overall absorption enthalpy of CO2 in (ChCl/urea + water) is around 78% to 97%. Thus, the overall absorption enthalpy of CO2 in (ChCl/urea + water) is dominated by the enthalpy of CO2 dissolution. The enthalpy of CO2 absorption in (ChCl/urea + water) at other temperatures shows similar tendency to that at 308.2 K. 4. CONCLUSION The effect of water on the density, viscosity and CO2 solubility in ChCl/urea was studied. The density and viscosity of ChCl/ urea with water were measured at different temperatures and atmospheric pressure, it was found that both density and viscosity decrease with increasing temperature and water content. The water content has a significant influence on the viscosity of (ChCl/urea + water). The solubilities of CO2 in (ChCl/urea + water) were measured at temperatures of 308.2 K, 318.2 K, and 328.2 K and pressures from 0.6 MPa to 4.5 MPa. The CO2 solubility decreases with increasing water content, but the influence of the water content on the CO2 ΔHex =−RT2∑x i ∂T ∂ln γ i w H V∞ H2O CO2 MPa 308.2 K 318.2 K CO2 cm−3·mol awH2O is the mass fraction of water in the mixture of (ChCl/urea + water). V∞ is the infinite dilution partial volume of CO in solvent. content due to the slight decreases in CO2 solubility with increasing water content. For example, at 308.2 K, HCO2(T) varies from 14.2 MPa to 18.0 MPa when the mass fraction of water changes from 0.0185 to 0.183. In the work of Su et al.,19 the CO2 solubility in (ChCl/urea + water) was measured at atmospheric pressure (0.1 MPa) and the Henry’s constant was obtained based on very limited gas solubility data. The Henry’s constants reported by Su et al.19 vary from (31.8 to 55) MPa when the mass fractions of water change from 0.0106 to 0.183 at 308 K, which is much higher than those from this work. As no original solubility data was reported in the work of Su et al.,19 we could not draw more comparisons and analyses. In this work, the solubility data were measured systematically, the calibration has shown that the CO2 2 328.2 K 3350 dx.doi.org/10.1021/je500320c | J. Chem. Eng. Data 2014, 59, 3344−3352PDF Image | CO2 Separation with Ionic Liquids
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