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CO2 and decrease the pumping costs due to the reducing of friction losses,29 but the decrease of CO2 solubility (capacity) will lead to an increase of the amount circulated solvent and a large absorption tower. Therefore, how the addition of water will affect the whole performance of the process is still unclear. In addition, similar to HPWS, using aqueous ChCl/Urea for biogas-upgrading, the solvent can be regenerated easily by bubbling air, and no thermal energy is needed. Therefore, it will be highly interesting to compare these two techniques. The objective of this work was to investigate the performance of biogas upgrading using aqueous ChCl/Urea as liquid absorbents. Aspen Plus was used as a simulation tool. ChCl/Urea was input as a new user-defined component. The physical properties of ChCl/Urea measured experimentally were surveyed, evaluated and then fitted with semi-empirical equations, and the experimental results of vapor-liquid equilibrium were represented by the Non-Random Two-Liquid model and the Redlich-Kwong equation (NRTL-RK). All the fitted parameters were further implemented into Aspen Plus and used for process simulation. Based on the equilibrium approach, the sensitivity analysis was conducted to determine a set of optimal parameters, and the effect of ChCl/Urea content on the total energy utilization, the diameters and pressure-drops of absorber and desorber as well as the green degree of the process was studied. The performance of aqueous ChCl/Urea for biogas upgrading was compared with HPWS. 2. THERMOPHYSICAL PROPERTIES AND PHASE EQUILIBRIUM 2.1. Properties of pure components. In the process of biogas upgrading with aqueous ChCl/Urea, the components involved can be CO2, CH4, H2O, ChCl/Urea, N2, O2 and H2S. Assuming that H2S was removed before upgrading, the content of H2S was ignored in the simulation of this work. The physicochemical properties of the components other than ChCl/Urea (i.e. CO2, CH4, H2O, N2, and O2) were calculated using the parameters from the property databank in Aspen Plus without further study. ChCl/Urea can be obtained by mixing various molar ratios of choline chloride to urea. Among them, the ChCl/Urea with 1:2 on a molar basis showed the highest CO2 solubility. 23 Therefore, ChCl/Urea used in this work was all based on the molar ratio of 1:2 (choline chloride: urea). For ChCl/Urea (1:2), the physicochemical properties measured experimentally were surveyed, evaluated and then fitted with semi-empirical equations, and the fitted parameters were further implemented into the databank for performing the process simulation. The parameter fitting was performed within Aspen Plus. For the properties that have not been determined reliably or could not be determined, theoretical estimation was conducted to satisfy the simulation requirement of Aspen Plus. The detail was described in this section. 2.1.1. Critical properties of ChCl/Urea (1:2). The critical properties of pure components are required as one of inputs in the process simulation with Aspen Plus. For ILs, Valderrama et al.30, 31 developed an extended group contribution method to determine the critical properties, normal boiling temperatures and acentric factors of ILs, and it was stated that the estimated acentric factors were accurate enough for engineering calculations. For DESs, Emad et al.32 estimated the critical properties of 17 kinds of DESs including choline chloride-based DESs based on the group contribution methods. Mirza et al. estimated the critical properties of 39 different DESs including ChCl/Urea (1:2) by a combination of the modified Lydersen-Joback-Reid method with the Lee-Kesler mixing rules.33, 34 It was found that there was only a slight difference when different parameters were used in the extended group contribution method. Therefore, the critical properties of ChCl/Urea (1:2) used in this work were directly taken from the reference33 as listed in Table S1 (Supporting Information). 3PDF Image | CO2 Separation with Ionic Liquids
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