Flow patterns of ionic liquid based aqueous biphasic systems in small channels

Phakoukaki, Yiota-Victoria; O‘Shaughnessy, Paul; Angeli, Panagiota

doi:10.1016/j.ces.2022.118197

Cited by 7 publications

(6 citation statements)

References 63 publications

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“…For the 5 m (mol.kg −1 ) LiTFSI–10 m LiCl biphasic system, the interfacial tension is estimated as ≈ 3 mN.m −1 . This value is similar to IL–salt ABSs (0.4 to 2.3 mN.m −1 ) ( 25 ) but 10 times lower than values reported for ITIES (20 to 30 mN.m −1 ) ( 27 ) and higher than that reported for polymer–polymer ABSs (0.01 to 500 μN.m −1 ) ( 22 , 38 ). Decreasing the molalities to 3 m LiTFSI–6 m LiCl, the interfacial tension decreases down to values 200 μN.m −1 .…”

Section: Resultssupporting

confidence: 75%

“…However, for salt–salt ABSs to be efficiently implemented in electrochemical devices, mastering the ion transfer at liquid–liquid interface is critical as it directly controls the (dis)charging rate by inducing an interfacial overpotential if too slow or can induce self-discharge when not selective. Despite this key role, interfaces of ABSs are poorly understood, almost entirely via surface tension measurements ( 22 – 25 ). Classically, the surface tension between two phases α and β is captured by the Gibbs adsorption equation:

…”

mentioning

confidence: 99%

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Direct imaging of micrometer-thick interfaces in salt–salt aqueous biphasic systems

Degoulange

Pandya

Deschamps

et al. 2023

Proc. Natl. Acad. Sci. U.S.A.

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Unlike the interface between two immiscible electrolyte solutions (ITIES) formed between water and polar solvents, molecular understanding of the liquid–liquid interface formed for aqueous biphasic systems (ABSs) is relatively limited and mostly relies on surface tension measurements and thermodynamic models. Here, high-resolution Raman imaging is used to provide spatial and chemical resolution of the interface of lithium chloride - lithium bis(trifluoromethanesulfonyl)imide - water (LiCl–LiTFSI–water) and HCl–LiTFSI–water, prototypical salt–salt ABSs found in a range of electrochemical applications. The concentration profiles of both TFSI anions and water are found to be sigmoidal thus not showing any signs of a positive adsorption for both salts and solvent. More striking, however, is the length at which the concentration profiles extend, ranging from 11 to 2 µm with increasing concentrations, compared to a few nanometers for ITIES. We thus reveal that unlike ITIES, salt–salt ABSs do not have a molecularly sharp interface but rather form an interphase with a gradual change of environment from one phase to the other. This knowledge represents a major stepping-stone in the understanding of aqueous interfaces, key for mastering ion or electron transfer dynamics in a wide range of biological and technological settings including novel battery technologies such as membraneless redox flow and dual-ion batteries.

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Section: Resultssupporting

confidence: 75%

…”

mentioning

confidence: 99%

Direct imaging of micrometer-thick interfaces in salt–salt aqueous biphasic systems

Degoulange

Pandya

Deschamps

et al. 2023

Proc. Natl. Acad. Sci. U.S.A.

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“…For the 5 m (mol.kg -1 ) LiTFSI -10 m LiCl biphasic system, the interfacial tension is estimated as ≈ 3 mN.m -1 . This value is similar to IL-salt ABSs (0.4 to 2.3 mN.m -1 ) 26 but ten times lower than values reported for ITIES (20 to 30 mN.m -1 ) 28 and higher than that reported for polymer-polymer ABSs (0.01 to 500 μN.m -1 ) 23,39 . Decreasing the molalities to 3 m LiTFSI -6 m LiCl, the interfacial tension decreases down to values ≈ 200 μN.m -1 .…”

Section: Phase Diagram Surface Tension and Temperature Behavior Of Th...supporting

confidence: 65%

“…Despite this key role, interfaces of ABSs are poorly understood, almost entirely via surface tension measurements [23][24][25][26] . Classically, the surface tension between two phases α and β is captured by the Gibbs adsorption equation:…”

Section: Introductionmentioning

confidence: 99%

Direct Imaging of Micrometer Thick Interfaces in Salt-Salt Aqueous Biphasic Systems

Degoulange

Pandya

Deschamps

et al. 2022

Preprint

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Unlike the interface between two immiscible electrolyte solutions (ITIES) formed between water and polar solvents, molecular understanding of the liquid-liquid interface formed for aqueous biphasic systems (ABSs) is relatively limited and mostly relies on surface tension measurements and thermodynamic models. Here, high-resolution Raman imaging is used to provide spatial and chemical resolution of the interface of LiCl-LiTFSI-water and HCl-LiTFSI-water, prototypical salt-salt ABSs found in a range of electrochemical applications. The concentration profiles of both TFSI anions and water are found to be sigmoidal, in agreement with an increasing surface tension as a function of concentration, both being typical of a negative adsorption mechanism. More striking, however, is the length at which the concentration profiles extend, ranging from 11 to 2 m with increasing concentrations, compared to a few nanometers for ITIES. We thus reveal that unlike ITIES, salt-salt ABSs do not have a molecularly sharp interface but rather form an interphase with a gradual change of environment from one phase to the other. This knowledge represents a major stepping-stone in the understanding of aqueous interfaces, key for mastering ion or electron transfer dynamics in a wide range of biological and technological settings including novel battery technologies such as membraneless redox flow and dual ion batteries.

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“…To address these challenges, recent advances have focused on developing more efficient and cost-effective methods for purifying ILs. 21 Recently, aqueous biphasic systems (ABSs), a type of extractive platform, have emerged as a novel methodology for purifying hydrophilic ILs, including [bmim]-[BF 4 ]. 22,23 In this method, inorganic salts, carbohydrates, and polymers are introduced to form a two-phase aqueous system.…”

Section: Introductionmentioning

confidence: 99%

Economically Viable Process for Synthesizing and Purifying Ionic Liquids: 1-Butyl-3-methyl Imidazolium Tetrafluoroborate

Choi,

Lim,

Kwon

et al. 2024

Ind. Eng. Chem. Res.

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Ionic liquids (ILs) have been utilized in a variety of applications owing to their nonflammability, low volatility, and tunable chemical properties. However, removing impurities during the synthesis process is complex and costly. In this work, we introduce a novel and cost-effective method to purify [bmim][BF 4 ], an IL, by inducing phase separation using a halocarbon refrigerant such as chlorodifluoromethane . The technique utilizes a ternary phase diagram consisting of [bmim][BF 4 ], water, and halocarbons to achieve a purity greater than 99% and simplify the purification process. Large-scale process simulations based on experimental data were performed using the ASPEN Plus process simulator. The minimum [bmim][BF 4 ] sales price of the developed process was estimated to be $12,004 per metric ton, making it an economically viable option for [bmim][BF 4 ] production.

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Flow patterns of ionic liquid based aqueous biphasic systems in small channels

Cited by 7 publications

References 63 publications

Direct imaging of micrometer-thick interfaces in salt–salt aqueous biphasic systems

Direct imaging of micrometer-thick interfaces in salt–salt aqueous biphasic systems

Direct Imaging of Micrometer Thick Interfaces in Salt-Salt Aqueous Biphasic Systems

Economically Viable Process for Synthesizing and Purifying Ionic Liquids: 1-Butyl-3-methyl Imidazolium Tetrafluoroborate

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