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Journal of Chemical & Engineering Data Article at this temperature are 48%, 16%, and 41%, respectively. In the current work, it was found that the water content has a significant effect on the viscosity of ChCl/urea, but there is no information about the water content in these literatures.9,17,18 Therefore, we may suggest that the discrepancies are due to trace water contents in ChCl/urea. Yadav et al.18 measured the viscosity of (ChCl/urea + water) at temperatures from 293.15 K to 363.15 K. The measured viscosity of (ChCl/urea + water) at 303.15 K and 333.15 K in this work was compared with that reported by Yadav et al.18 The comparison is shown in Figure 3b. It was found that the viscosity measured in this work is higher than that measured by Yadav et al.18 at lower water concentrations, but the experimental data agrees well with each other at higher water concentrations. The excess molar energy of activation (AE) was calculated from the measured viscosities on the basis of Eyring’s absolute reaction rate theory,31 that is AE =RT[ln(η V )−xln(ηV)−x ln(ηV)] mm 1 11 2 22 (5) where R is the gas constant and η is the viscosity. The calculated excess molar energy of activation is listed in Table 3. The calculated excess molar energies of activation were also correlated with the Redlich−Kister equation (eqs 3 and 4) by replacing VE with AE. The fitted temperature-dependent Redlich−Kister coefficients are listed in Table 2 with the fitting error of 2.7%. Figure 4 shows the excess molar activation energies at different temperatures over the entire mole fraction. At low Figure 4. Excess molar activation energy of {ChCl/urea (1) + water (2)}. Symbols: ■, 298.15 K; □, 303.15 K; ●, 308.15 K; ○, 313.15 K; ▲, 318.15 K; △, 323.15 K; ▼, 328.15 K; ▽, 333.15 K. Curves: correlations. temperatures, with increasing water content, the excess molar activation energy decreases to a minimum value at x2 ≈ 0.37 and then increases. At high temperatures, it shows an S-shape curve, that is, with increasing water content, the excess molar activation energy decreases to a minimum value at x2 ≈ 0.37 and then increases to a maximum value at 0.7 < x2 < 0.8. The values are negative in the whole region at low temperatures (298.15 K to 313.15 K), but they change to positive at high temperatures (318.15 K to 333.15 K) in the water-rich region. This tendency was also observed by Yadav et al.18 The negative excess molar activation energy implies the strong interaction between ChCl/urea and water. With increasing temperature, the interaction becomes weak. The positive excess molar activation energy at high temperatures and in the water-rich region is caused by the intensive hydrogen bonding network formed within the mixture as proposed by Yadav et al.18 3.3. CO2 Solubility in (ChCl/Urea + Water). Before the measurements of the CO2 solubility in (ChCl/urea + water), the CO2 solubility in water at 308.2 K was measured to calibrate the accuracy of the solubility equipment. The measured CO2 solubility in water was compared with the data reported by Valtz et al.32 as shown in Figure 5. The Figure 5. Solubilities of CO2 in water at 308.2 K: ■, this work; ○, Valtz et al.32 solubility data measured in this work and that from the literature32 are in good agreement, which implies that it is reasonable to neglect the vapor pressure of water and the measurements are reliable. The solubilities of CO2 in (ChCl/urea + water) were further measured at pressures up to 4.5 MPa and temperatures of 308.2 K, 318.2 K, and 328.2 K. The experimental results are listed in Table 4 and illustrated in Figure 6. Within the temperature and pressure ranges investigated in this work, the solubility of CO2 decreases with increasing water content. When the water content is high, the influence of water on the CO2 solubility is Table 4. Solubilities of CO2 (xCO2) in the Mixture of ChCl/ Urea (1) + Water (2)a 3348 dx.doi.org/10.1021/je500320c | J. Chem. Eng. Data 2014, 59, 3344−3352 308.2 K wH2O P xCO2 MPa 318.2 K P xCO2 MPa 328.2 K P xCO2 MPa 0.0185 0.651 0.043 0.726 1.527 0.083 1.592 2.453 0.120 2.499 3.455 0.152 3.454 4.376 0.169 4.352 0.0910 0.706 0.038 0.669 1.661 0.081 1.540 2.618 0.11 2.504 3.527 0.136 3.478 4.504 0.151 4.356 0.183 0.692 0.036 0.781 1.591 0.078 1.616 2.544 0.097 2.511 3.577 0.127 3.460 4.499 0.143 4.396 0.040 0.673 0.075 1.530 0.105 2.482 0.129 3.468 0.147 4.480 0.030 0.702 0.064 1.551 0.094 2.472 0.121 3.436 0.139 4.457 0.030 0.659 0.061 1.551 0.091 2.498 0.115 3.480 0.130 4.486 0.040 0.073 0.103 0.126 0.139 0.032 0.059 0.089 0.111 0.129 0.025 0.054 0.079 0.098 0.110 awH2O is the mass fraction of water in the (ChCl/urea + water). xCO2 is the mole fraction of CO2 in the (ChCl/urea + water). Standard uncertainties u are u(P) = 10 kPa and u(x) = 0.002.PDF Image | CO2 Separation with Ionic Liquids
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