Volumetric and transport properties of binary liquid mixtures with 1-ethyl-3-methylimidazolium ethyl sulfate as candidate solvents for regenerative flue gas desulfurization processes

doi:10.1016/j.jct.2017.12.023

The Journal of Chemical Thermodynamics

Volume 119, April 2018, Pages 135-154

https://doi.org/10.1016/j.jct.2017.12.023 Get rights and content

Highlights

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Potential solvents for flue gas desulfurization processes were investigated.
•
Densities, viscosities and refractive indices of four binary mixtures were measured.
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Thermal conductivity of two binary solutions was determined.
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Excess and deviation functions were calculated.
•
Modelling of viscosity and thermal conductivity was performed.

Abstract

This paper presents novel data on density, viscosity and refractive index of four binary mixtures constituted of ionic liquid 1-ethyl-3-methylimidazolium ethyl sulfate and N-methyl-2-pyrrolidone/or 1-hexanol/or liquid polyethylene glycols with molar mass 200/or 400, in the temperature range from T = 288.15 K to 333.15 K and at pressure of p = .1 MPa. Thermal conductivity has been measured for mixtures of ionic liquid and polyethylene glycol 200/or polyethylene glycol 400 in the temperature range from T = 303.15 to 323.15 K and at a pressure of p = .1 MPa. All these solutions have the potential for application in regenerative flue gas desulfurization processes. From experimental values of densities, viscosities, thermal conductivities and refractive indices, excess molar volumes and deviations in viscosity, thermal conductivity and refractive index have been calculated and correlated with Redlich-Kister polynomial equation. The values of excess and deviation functions were used for analysis of molecular interactions present in the investigated solutions. In addition, modeling of transport properties, viscosity and thermal conductivity, was carried out and the obtained results were interpreted taking into account the applied approaches and models.

Introduction

The results presented in this work are a continuation of our previous studies related to volumetric and transport properties of the environmentally friendly solutions with potential application in flue gas cleaning processes [1], [2], [3].

Main pollutants contained in exhaust gasses from the industrial and power plants facilities are sulfur oxides (SO_x), among which the most abundant is sulfur dioxide (SO₂). Sulfur oxides have strong environmental impact and are considered to be the main cause of acid rains. Understanding the seriousness of the problem was followed by establishing legislation related to the discharge of pollutants into the atmosphere and development of technological procedures for flue gas purification. Regenerative flue gas scrubbing processes, using organic solvents, already have relatively long history. Due to certain limitations of current technologies, like insufficient selectivity of the solvent or large energy requirements, efforts are continually invested in finding new solvents for use in regenerative cleaning processes as effective SO_x absorbents.

Some of the solvents investigated in this study, like N-methyl-2-pyrrolidone (NMP), have already found a commercial application. The others, like ionic liquid 1-ethyl-3-methylimidazolium ethyl sulfate ([Emim][EtSO₄]), and liquid polymers polyethylene glycols with molar weight 200 and 400 (PEG200 and PEG400), have been suggested as possible environmentally friendly replacements [4], [5], [6], [7], [8], [9], [10], [11]. Due to their favorable thermophysical properties (e.g. low vapor pressure, high chemical and thermal stability) ionic liquids (ILs) have been investigated as green solvents suitable as a replacement of volatile organic compounds. However, in some cases they have shown limited solute solubility, higher viscosity and many of them are more expensive than conventional solvents. The possible solution to this problem could be the use of cosolvent modified ILs. In this way it may be possible to obtain more affordable solvent with favorably modified properties. Since the ionic liquids have the advantages due to their low toxicity, it classifies them as a possible alternative or cosolvent choice for other environmentally friendly fluids, such as alcohols [12], [13], water [14] or polyethylene glycols [15].

Polyethylene glycols (PEG) are important environmentally friendly solvents characterized by low vapor pressure, high chemical stability and low melting points. In liquid form PEG is a highly polar substance [16], [17] which acts both as a proton donor and proton acceptor [18] and is capable of forming both intra- and inter-molecular hydrogen bonds [19], [20]. Industrial application of liquid PEG in the flue gas desulfurization processes is considered as a consequence of its advantages: the high solubility of SO₂ and relatively easy desorption, which would reduce power consumption during the phase of solvent regeneration [21].

In this study novel data on density, viscosity and refractive index, in the temperature range from T = 288.15 K to 323.15 K or 333.15 K and at pressure of p = .1 MPa, of the solutions consisting of ionic liquid [Emim][EtSO₄] and NMP/or 1-hexanol/or PEG200/or PEG400, have been presented. Thermal conductivity of [Emim][EtSO₄] and PEG200/or PEG400 binary mixtures have also been investigated in the temperature range from 303.15 to 323.15 and at a pressure of p = .1 MPa. Of all investigated solutions only the density data for [Emim][EtSO₄] and 1-hexanol mixture have been previously published at T = 298.15 K [13]. In addition to experimental values of densities, viscosities, thermal conductivities and refractive indices, excess molar volumes and deviations in viscosity, thermal conductivity and refractive index have been calculated for all investigated mixtures and correlated with Redlich-Kister polynomial equation [22]. The values of excess molar volumes were used for analysis of molecular interactions existing in the investigated solutions.

Viscosity modeling was done by two sets of models: group contribution UNIFAC-VISCO [23], [24] and ASOG-VISCO [25] models and correlative McAllister [26], Eyring-UNIQUAC [27] and NRTL-Eyring [28] models. In addition, the approach based on the application of equations of state (EOS) was used for simultaneous modeling of excess molar volume and viscosity [29]. Thermal conductivity was correlated by Filippov [30], Jamieson [31], Baroncini [32] and Rowley [33] models.

Section snippets

Chemicals

Data on the investigated pure chemicals, their suppliers and stated purities and purification methods are given in Table 1. The mixtures were prepared gravimetrically using Mettler Toledo balance with a stated accuracy of 1 · 10⁻⁷ kg, while the standard uncertainty in mole fraction calculation is estimated to be within ±1 · 10⁻⁴.

Prior to use, chemicals were kept in a dry, dark place in delivery bottles. Analysis of ionic liquid using the Mettler Toledo DL 38 Karl Fisher Titrator showed that the

Results and discussion

Experimental values of density (ρ), dynamic viscosity (η) and refractive index (n_D) of pure compounds and binary solutions are presented in Table 4. The same table also gives the calculated values of excess molar volume (V^E) and deviations in viscosity (Δη) and refractive index (Δn_D). Values of thermal conductivity (λ) and deviation in thermal conductivity (Δλ) are given in Table 5.

The excess molar volume V^E was determined from the equation: $V^{E} = \sum_{i = 1}^{2} x_{i} M_{i} [(\frac{1}{ρ}) - (\frac{1}{ρ_{i}})]$ where ρ and ρ_i are experimentally

Conclusions

In this paper an extensive research of thermophysical and transport properties of four binary mixtures was conducted. Mixtures were selected on the basis of their potential for application in flue gas desulfurization processes. Besides measurement of density, viscosity, refractive index and thermal conductivity, excess molar volumes and deviations in viscosity, thermal conductivity and refractive index have been calculated for all investigated mixtures and correlated with Redlich-Kister

Funding

The authors gratefully acknowledge the financial support received from the Research Fund of Ministry of Education, Science and Technological Development, Serbia and the Faculty of Technology and Metallurgy, University of Belgrade (project No 172063).

Notes

The authors declare no competing financial interest.

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Volumetric and transport properties of binary liquid mixtures with 1-ethyl-3-methylimidazolium ethyl sulfate as candidate solvents for regenerative flue gas desulfurization processes

Highlights

Abstract

Introduction

Section snippets

Chemicals

Results and discussion

Conclusions

Funding

Notes

J. Chem. Thermodyn.

Chem. Eng. Sci.

Chem. Eng. Sci.

Fluid Phase Equilibr.

Chem. Eng. Sci.

Fluid Phase Equilib.

J. Chem.Thermodyn.

J. Chem. Thermodyn.

Fluid Phase Equilib.

J. Chem. Thermodyn.

J. Chem.Thermodyn.

Fluid Phase Equilib.

J. Chem. Thermodyn.

J. Chem.Thermodyn.

J. Chem. Thermodyn.

J. Chem.Thermodyn.

J. Chem. Thermodyn.

J. Chem. Thermodyn.

J. Mol. Liq.

J. Chem. Thermodyn.

Fluid Phase Equilib.

Fluid Phase Equilib.

Volumetric and viscometric behavior of binary systems 2-butanol + PEG200, +PEG400, +tetraethylene glycol dimethyl ether, and + N-methyl-2-pyrrolidone

J. Chem. Eng. Data

Volumetric properties, viscosities, and refractive indices of the binary systems 1-butanol + PEG200, +PEG400, and +TEGDME

Int. J. Thermophys.

Density, viscosity, and excess properties for aqueous poly(ethylene glycol) solutions from (298.15 to 323.15) K

J. Chem. Eng. Data

Gas-liquid equilibrium data for the mixture gas of sulfur dioxide + nitrogen with poly(ethylene glycol) aqueous solutions at 298.15 K and 122.61 kPa

J. Chem. Eng. Data

Solubility of dilute sulfur dioxide in aqueous poly-ethylene glycol 1000 solutions at 298.15 K and 123.15 kPa

Asian J. Chem.

Measurement of SO2 solubility in ionic liquids

J. Phys. Chem. B

hydroxyl ammonium ionic liquids: synthesis, properties and solubility of SO2

J. Chem. Eng. Data

chemical absorption of sulfur dioxide in room-temperature ionic liquids

Ind. Eng. Chem. Res.

Separation of carbon dioxide and sulfur dioxide using room-temperature ionic liquid [bmim][MeSO4]

Energy Fuels

Reversible physical absorption of SO2 by ionic liquids

Chem. Commun.

Solvatochromic probe behavior within ternary room-temperature ionic liquid 1-butyl-3-methylimidazolium hexafluorophosphate + ethanol + water solutions

J. Phys. Chem. B

Phase equilibria and volumetric properties of (1-ethyl-3-methylimidazolium ethylsulfate + alcohol or water) binary systems

J. Solution Chem.

Solvatochromic probe behavior within binary room-temperature ionic liquid 1-butyl-3-methyl imidazolium hexafluorophosphate plus ethanol solutions

Appl. Spectrosc.

Interactions within a [ionic liquid + poly(ethylene glycol)] mixture revealed by temperature-dependent synergistic dynamic viscosity and probe-reported microviscosity

J. Phys. Chem. B

Dielectric properties of low molecular weight poly(ethylene glycol)s

Polym. Int.

Apparent specific polarization and dipole moment of some poly(oxyethylene) glycols in 1,4-dioxane and benzene solutions at 298.15 K

Monatsh. Chem.

Dipolarity, hydrogen-bond basicity and hydrogen-bond acidity of aqueous poly(ethylene glycol) solutions

Anal. Sci.

volumetric properties and spectroscopic studies of pyridine or nicotine solutions in liquid polyethylene glycols

J. Phys. Chem. B

Hydrogen bonds in dilute solutions of poly(ethylene glycol)

Macromolecules

Algebraic representation of thermodynamic properties and the classification of solutions

Ind. Eng. Chem.

Prediction of kinematic viscosities for binary and ternary liquid mixtures with an ASOG-VISCO Group Contribution Method

Int. J. Thermophys.

The viscosity of liquid mixtures

AIChE J.

Excess gibbs free energy model for calculating the viscosity of binary liquid mixtures

Ind. Eng. Chem. Res.

Relationship between the intrinsic viscosity and Eyring–NRTL viscosity model parameters

Ind. Eng. Chem. Res.

Volumetric and viscometric behavior of binary systems 2-butanol + PEG200, +PEG400, +tetraethylene glycol dimethyl ether, and + N-methyl-2-pyrrolidone

Volumetric properties, viscosities, and refractive indices of the binary systems 1-butanol + PEG200, +PEG400, and +TEGDME

Gas-liquid equilibrium data for the mixture gas of sulfur dioxide + nitrogen with poly(ethylene glycol) aqueous solutions at 298.15 K and 122.61 kPa

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Separation of carbon dioxide and sulfur dioxide using room-temperature ionic liquid [bmim][MeSO₄]

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Solvatochromic probe behavior within ternary room-temperature ionic liquid 1-butyl-3-methylimidazolium hexafluorophosphate + ethanol + water solutions

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