Computation of gas solubilities in choline chloride urea and choline chloride ethylene glycol deep eutectic solvents using Monte Carlo simulations

Salehi, Hirad S.; Hens, Remco; Moultos, Othonas A.; Vlugt, Thijs J. H.

doi:10.1016/j.molliq.2020.113729

Cited by 34 publications

(63 citation statements)

References 122 publications

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“…The DES were modeled using the GAFF 53 force field consistently with our previous studies. 21 , 24 , 26 , 27 , 54 For choline, urea, and ethylene glycol, 1–4 interactions were scaled by a factor of 0.5 for both Lennard-Jones and Coulombic interactions. The charges of choline chloride were scaled by a factor of 0.8 and 0.9 in reline and ethaline, respectively.…”

Section: Methodsmentioning

confidence: 99%

Solubilities and Transport Properties of CO₂, Oxalic Acid, and Formic Acid in Mixed Solvents Composed of Deep Eutectic Solvents, Methanol, and Propylene Carbonate

et al. 2022

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Recently, deep eutectic solvents (DES) have been considered as possible electrolytes for the electrochemical reduction of CO 2 to value-added products such as formic and oxalic acids. The applicability of pure DES as electrolytes is hindered by high viscosities. Mixtures of DES with organic solvents can be a promising way of designing superior electrolytes by exploiting the advantages of each solvent type. In this study, densities, viscosities, diffusivities, and ionic conductivities of mixed solvents comprising DES (i.e., reline and ethaline), methanol, and propylene carbonate were computed using molecular simulations. To provide a quantitative assessment of the affinity and mass transport of CO 2 and oxalic and formic acids in the mixed solvents, the solubilities and self-diffusivities of these solutes were also computed. Our results show that the addition of DES to the organic solvents enhances the solubilities of oxalic and formic acids, while the solubility of CO 2 in the ethaline-containing mixtures are in the same order of magnitude with the respective pure organic components. A monotonic increase in the densities and viscosities of the mixed solvents is observed as the mole fraction of DES in the mixture increases, with the exception of the density of ethaline-propylene carbonate which shows the opposite behavior due to the high viscosity of the pure organic component. The self-diffusivities of all species in the mixtures significantly decrease as the mole fraction of DES approaches unity. Similarly, the self-diffusivities of the dissolved CO 2 and the oxalic and formic acids also decrease by at least 1 order of magnitude as the composition of the mixture shifts from the pure organic component to pure DES. The computed ionic conductivities of all mixed solvents show a maximum value for mole fractions of DES in the range from 0.2 to 0.6 and decrease as more DES is added to the mixtures. Since for most mixtures studied here no prior experimental measurements exist, our findings can serve as a first data set based on which further investigation of DES-containing electrolyte solutions can be performed for the electrochemical reduction of CO 2 to useful chemicals.

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Section: Methodsmentioning

confidence: 99%

Solubilities and Transport Properties of CO₂, Oxalic Acid, and Formic Acid in Mixed Solvents Composed of Deep Eutectic Solvents, Methanol, and Propylene Carbonate

et al. 2022

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“…The effect of charge scaling factor on the computed properties was investigated as this parameter has been shown to significantly influence the properties of ILs and DESs. 34 , 43 − 48 A hydrogen bond analysis was performed to investigate the interactions of the various mixture components, which result in the computed interfacial tensions and density profiles.…”

Section: Introductionmentioning

confidence: 99%

Interfacial Properties of Hydrophobic Deep Eutectic Solvents with Water

2021

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Hydrophobic deep eutectic solvents (DESs) have recently gained much attention as water-immiscible solvents for a wide range of applications. However, very few studies exist in which the hydrophobicity of these DESs is quantified. In this work, the interfacial properties of hydrophobic DESs with water were computed at various temperatures using molecular dynamics simulations. The considered DESs were tetrabutylammonium chloride−decanoic acid (TBAC−dec) with a molar ratio of 1:2, thymol− decanoic acid (Thy−dec) with a molar ratio of 1:2, and DL-menthol−decanoic acid (Men−dec) with a molar ratio of 2:1. The following properties were investigated in detail: interfacial tensions, water-in-DES solubilities (and salt-inwater solubilities for TBAC−dec/water), density profiles, and the number densities of hydrogen bonds. Different ionic charge scaling factors were used for TBAC−dec. Thy−dec and Men−dec showed a high level of hydrophobicity with negligible computed water-in-DES solubilities. For charge scaling factors of 0.7 and 1 for the thymol and decanoic acid components of Thy−dec, the computed interfacial tensions of the DESs are in the following order: TBAC−dec (ca. 4 mN m −1 ) < Thy−dec (20 mN m −1 ) < Men−dec (26 mN m −1 ). The two sets of charge scaling factors for Thy−dec did not lead to different density profiles but resulted in considerable differences in the DES/water interfacial tensions due to different numbers of decanoic acid−water hydrogen bonds at the interfaces. Large peaks were observed for the density profiles of (the hydroxyl oxygen of) decanoic acid at the interfaces of all DES/water mixtures, indicating a preferential alignment of the oxygen atoms of decanoic acid toward the aqueous phase.

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“…Recently, Blazquez et al [52] showed that the scaling of charges of even simple electrolytes such as NaCl can lead to an improved prediction of the salting out effect of methane in water. In the past few years, various studies have shown that simulations using the GAFF force field combined with scaled charges yield relatively accurate thermodynamic and transport properties of neat reline, ethaline, and glyceline [6,16,34,35,49,51,53].…”

Section: Force Fieldsmentioning

confidence: 99%

Thermal conductivity of aqueous solutions of reline, ethaline, and glyceline deep eutectic solvents; a molecular dynamics simulation study

2021

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Accurate knowledge and control of thermal conductivities is central for the efficient design of heat storage and transfer devices working with deep eutectic solvents (DESs). The addition of water is a straightforward and cost-efficient way of tuning many properties of DESs. In this work, the thermal conductivities of aqueous solutions of reline, ethaline, and glyceline are reported for the first time. The non-equilibrium molecular dynamics Müller-Plathe (MP) method was used, along with the well-established GAFF and SPC/E force fields for DESs and water, respectively. We show that thermal conductivities of neat DESs are in excellent agreement with available experimental data. The addition of 25 wt% water results in nearly 2 times higher thermal conductivities in all DESs. A further increase in the fraction of water to 75 wt%, causes an increase in the thermal conductivities of DESs ca. 3 times. This behaviour is mainly due to the change in the microscopic structure of the DESs (i.e. hydrogen bonding) upon the addition of water. Our simulations reveal that thermal conductivities of aqueous DESs do not significantly depend on temperature. We also show that thermal conductivities strongly depend on system-size. System-sizes bigger larger than ca. 5 nm should be used.

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Computation of gas solubilities in choline chloride urea and choline chloride ethylene glycol deep eutectic solvents using Monte Carlo simulations

Cited by 34 publications

References 122 publications

Solubilities and Transport Properties of CO₂, Oxalic Acid, and Formic Acid in Mixed Solvents Composed of Deep Eutectic Solvents, Methanol, and Propylene Carbonate

Solubilities and Transport Properties of CO₂, Oxalic Acid, and Formic Acid in Mixed Solvents Composed of Deep Eutectic Solvents, Methanol, and Propylene Carbonate

Interfacial Properties of Hydrophobic Deep Eutectic Solvents with Water

Thermal conductivity of aqueous solutions of reline, ethaline, and glyceline deep eutectic solvents; a molecular dynamics simulation study

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Computation of gas solubilities in choline chloride urea and choline chloride ethylene glycol deep eutectic solvents using Monte Carlo simulations

Cited by 34 publications

References 122 publications

Solubilities and Transport Properties of CO2, Oxalic Acid, and Formic Acid in Mixed Solvents Composed of Deep Eutectic Solvents, Methanol, and Propylene Carbonate

Solubilities and Transport Properties of CO2, Oxalic Acid, and Formic Acid in Mixed Solvents Composed of Deep Eutectic Solvents, Methanol, and Propylene Carbonate

Interfacial Properties of Hydrophobic Deep Eutectic Solvents with Water

Thermal conductivity of aqueous solutions of reline, ethaline, and glyceline deep eutectic solvents; a molecular dynamics simulation study

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Solubilities and Transport Properties of CO₂, Oxalic Acid, and Formic Acid in Mixed Solvents Composed of Deep Eutectic Solvents, Methanol, and Propylene Carbonate

Solubilities and Transport Properties of CO₂, Oxalic Acid, and Formic Acid in Mixed Solvents Composed of Deep Eutectic Solvents, Methanol, and Propylene Carbonate