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Article pubs.acs.org/jced Effect of Water on the Density, Viscosity, and CO2 Solubility in Choline Chloride/Urea Yujiao Xie,*,† Haifeng Dong,‡ Suojiang Zhang,‡ Xiaohua Lu,§ and Xiaoyan Ji*,† †Division of Energy Science/Energy Engineering, Lulea University of Technology, 971 87 Lulea, Sweden ‡Beijing Key Laboratory of Ionic Liquids Clean Process, State Key Laboratory of Multiphase Complex System, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China §State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, China studied.12−15 For choline chloride/urea, the effect of water on the Henry’s constant of CO2, vapor pressure, and heat capacity have been studied. However, the effect of water on the CO2 solubility in choline chloride/urea up to high pressures has not yet been investigated. Therefore, more research work is required. The goal of this work was to systematically study the effect of water on some of the physical and thermodynamic properties of choline chloride/urea. The density and viscosity of choline chloride/urea with water were determined. Based on the experimental data measured in this work, the excess molar volume and excess molar activation energy were calculated to reveal the intermolecular interactions between choline chloride/urea and water. The CO2 solubilities in choline chloride/urea with water were measured and represented with a thermodynamic model, in which the fugacity coefficient of CO2 in the vapor phase was calculated with Redlich−Kwong (RK) equation of state and the activity coefficient of CO in the 2 liquid phase was calculated with nonrandom two-liquid (NRTL) model. In addition, the enthalpy of CO absorption 2 was estimated and analyzed based on the thermodynamic model (NRTL-RK). 2. EXPERIMENTAL SECTION 2.1. Materials. Choline chloride (ChCl, mass fraction ≥99%) was produced by Sinopharm Chemical Reagent Co, Received: April 10, 2014 Accepted: October 23, 2014 Published: November 4, 2014 ABSTRACT: To study the effect of water on the properties of choline chloride (ChCl)/urea mixtures (1:2 on a molar basis), the density and viscosity of ChCl/ urea (1:2) with water were measured at temperatures from 298.15 K to 333.15 K at atmospheric pressure, the CO2 solubility in ChCl/urea (1:2) with water was determined at 308.2 K, 318.2 K, and 328.2 K and at pressures up to 4.5 MPa. The results show that the addition of water significantly decreases the viscosity of ChCl/urea (1:2), whereas the effects on their density and CO2 solubility are much weaker. The CO2 solubility in ChCl/urea (1:2) with water was represented with the Nonrandom-Two-Liquid Redlich−Kwong (NRTL-RK) model. The excess molar volume and excess molar activation energy were further determined. The CO2 absorption enthalpy was calculated and dominated by the CO2 dissolution enthalpy, and the magnitude of the CO2 dissolution enthalpy decreases with the increase of water content. 1. INTRODUCTION CO2 separation plays an important role in the development of renewable energy and the mitigation of CO2 emissions.1−3 However, CO2 separation using the current state-of-the-art technology, the aqueous (water-based) amine technology, costs in the range of $50 to $100 per ton,4 which is much too high for most applications. In addition, this technology is environ- mentally unacceptable because of the volatility of amine. It is necessary to explore a cost-effective and environmentally benign CO2 separation technology. Ionic liquids (ILs) are environmentally benign solvents that have shown great potential to be used as liquid absorbents for CO2 separation.5,6 However, the complicated synthesis process leads to high prices for most ILs, which has hindered extensive research and applications of ILs in practice. Recently, deep eutectic solvents have received much more attention in chemical and physical sciences and are considered as a new type of IL.7−9 Among them, choline chloride-based ILs are cheap, biodegradable, and easily synthesized. In addition, it is also promising to use this kind of ILs for CO separation.10,11 based on choline chloride-based ILs, it is essential to obtain thermophysical properties of pure ILs and their mixtures with other solvents. Water, as an impurity of ILs and of CO2- mixtures for separation, is also a green and cheap solvent that can dramatically decrease the viscosity of some ILs. All of these make it crucial to study the effect of water on the properties of choline chloride-based ILs. The effects of water on the density, viscosity, vapor pressure, and heat capacity of choline chloride/ glycerol and choline chloride/ethylene glycol have been 2 In order to develop and design a new CO2 separation process © 2014 American Chemical Society 3344 dx.doi.org/10.1021/je500320c | J. Chem. Eng. Data 2014, 59, 3344−3352PDF Image | CO2 Separation with Ionic Liquids
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