Water in Protic Ionic Liquids: Properties and Use of a New Class of Electrolytes for Energy‐Storage Devices

Stettner, Timo; Gehrke, Sascha; Ray, Promit; Kirchner, Barbara; Balducci, Andrea

doi:10.1002/cssc.201901283

Cited by 42 publications

(43 citation statements)

References 47 publications

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“…ences in the type and extent of the ion pairing and, ultimately, in the degree of ion stabilization. [19,22,27] In any case, the use of high temperatures was a serious drawback in comparison to room-temperature conditions given not only the intrinsic experimental difficulties associated with high-temperature measurements but also the well-known occurrence of ESW narrowing along with the temperature increase. [29,32] (in a 1 : 1 molar ratio) resulted in mixtures that were liquid at room temperature.…”

Section: Resultsmentioning

confidence: 99%

“…Without being as remarkable as that shown by (for instance) "acetonitrile/ water in salt" (AWIS) electrolytes, [5] capacity retention was quite good, in the range of those reported for other PILs. [22] Nonetheless, we wondered if some capacity fading during cycling could be due to solvent evaporation, gas generation, and leakage, [57] but the steady values of the coulombic efficiency during cycling (Figure 10f) make this option unlikely. [58] We also investigated whether there was some growth of a solid-electrolyte interphase (SEI) layer ultimately responsible for the capacity fading during cycling.…”

Section: Thus [C][z][a]-typementioning

confidence: 99%

“…However, the typically narrow electrochemical stability window (ESW) of PILs (in both their neat form and dissolved in organic solvents) has most likely hampered their use as electrolytes in SC cells, and details about their performance can only be found in some few interesting works. [18][19][20][21][22] This work provides further insights about the suitability of aqueous co-solvent mixtures (e. g., water with acetonitrile (ACN) and/or DMSO) to prepare highly concentrated ZPIL-based electrolytes (WcS-in-ZPIL electrolytes) able to operate at ESWs of up to 2 V.…”

Section: Introductionmentioning

confidence: 99%

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Aqueous Co‐Solvent in Zwitterionic‐based Protic Ionic Liquids as Electrolytes in 2.0 V Supercapacitors

Vicent-Luna

Calero

et al. 2020

ChemSusChem

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High-performance energy-storage devices are receiving great interest in sustainable terms as a required complement to renewable energy sources to level out the imbalances between supply and demand. Besides electrode optimization, a primary objective is also the judicious design of high-performance electrolytes combining novel ionic liquids (ILs) and mixtures of aqueous solvents capable of offering "à la carte" properties. Herein, it is described the stoichiometric addition of a zwitterion such as betaine (BET) to protic ILs (PILs) such as those formed between methane sulfonic acid (MSAH) or p-toluenesulfonic acid (PTSAH) with ethanolamine (EOA). This addition resulted in the formation of zwitterionic-based PILs (ZPILs) containing the original anion and cation as well as the zwitterion. The ZPILs prepared in this work ([EOAH] + [BET][MSA] À and [EOAH] + [BET] [PTSA] À) were liquid at room temperature even though the original PILs ([EOAH] + [MSA] À and [EOAH] + [PTSA] À) were not. Moreover, ZPILs exhibited a wide electrochemical stability window, up to 3.7 V vs. Ag wire for [EOAH] + [BET][MSA] À and 4.0 V vs. Ag wire for [EOAH] + [BET][PTSA] À at room temperature, and a high miscibility with both water and aqueous co-solvent (WcS) mixtures. In particular, "WcS-in-ZPIL" mixtures of [EOAH] + [BET][MSA] À in 2 H 2 O/ACN/DMSO provided specific capacitances of approximately 83 F g À 1 at current densities of 1 A g À 1 , and capacity retentions of approximately 90 % after 6000 cycles when operating at a voltage of 2.0 V and a current density of 4 A g À 1 .

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Section: Resultsmentioning

confidence: 99%

Section: Thus [C][z][a]-typementioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Aqueous Co‐Solvent in Zwitterionic‐based Protic Ionic Liquids as Electrolytes in 2.0 V Supercapacitors

Vicent-Luna

Calero

et al. 2020

ChemSusChem

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“…Therefore, ILs are attractive for applications in energy storage, advanced materials design, pharmaceutical industry, and other fields . The presence of water can influence or change interactions between the cations and anions as well as the interaction of the ILs with the environment, which results in a change of physiochemical properties like viscosity, electrical conductivity, polarity, reactivity, solvation, or solubility . In general, mixtures of ILs with solvents are crucial for applications.…”

Section: Introductionmentioning

confidence: 99%

“…Examples are electrolytes for Li + ion batteries, fuel cells, dye‐sensitized solar cells, and supercapacitors . Although ILs show high viscosity at room temperature, which affects their electrical conductivity and thus limits their potential in energy storage devices, these restrictions can be overcome by using mixtures of ILs with water at varying concentration . Therefore, a detailed understanding of binary mixtures of ILs with water is crucial.…”

Section: Introductionmentioning

confidence: 99%

Impact of water on the hydrogen bonding between halide‐based ion‐pairs investigated by Raman scattering and density functional theory calculations

Pandey

Sanchora

Rana

et al. 2019

J Raman Spectroscopy

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We present a study of the impact of water on the size-and electronegativitydependent hydrogen bonds between cation and anion of imidazolium-based ionic liquids (ILs) with halide anions. We have combined Raman spectroscopy with density functional theory (DFT) computations to characterize the intermolecular associations of cation-anion-water moieties. The Raman band at~1,422 cm −1 , which is assigned to the ν(N─CH 2 ─CH 3 ) vibration of the ethyl chain in the neat ion pairs (pure ion pairs), is blue shifted by +7, +4, and +3 cm −1 for 1-ethyl-3-methylimidazolim (C 2 mim) cation-based C 2 mim X ion pairs with X = Cl, Br, and I, respectively, in a water-rich environment. Simultaneously, upon dilution, a new peak at~1,438 cm −1 starts to appear at the high-wavenumber side with continuously increasing intensity. These significant perturbations of the ν(N─CH 2 ─CH 3 ) vibrational mode in water environment are a clear indication of the change in the alkyl chain conformation. Further, the relative intensities of the Raman bands at~2,946 and~2,950 cm −1 corresponding to ν s (CH 2 ) and ν as (CH 3 ) of the ethyl chain, respectively, were significantly changed upon dilution, which also confirms the conformational change of the alkyl chain. The Raman band belonging to the C 4/5 ─H stretch mode was significantly blue shifted by +33, +41, and +42 cm −1 going from the studied neat ion pairs having Cl, Br, and I anions to the corresponding water mixtures, respectively. Significant changes were also observed for the ν(C 2 ─H) vibrational mode of the ion pairs in water environment;here, we observed blue shifts of +60, +51, and +50 cm −1 for ion pairs having Cl, Br, and I anions, respectively. These results confirm the weakening of the ion-pair interaction due to the interaction with water molecules. In contrast to the ILs with halide anions, C 2 mim BF 4 does not show any variation in the Raman peak positions upon dilution. Experimental results are nicely supported by the results of DFT calculations, and a sensible connection was established. K E Y W O R D Sionic liquids, hydrogen bonds, Raman spectroscopy, density functional theory calculations Deepak K. Pandey and Paridhi Sanchora Authors have contributed equally

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Ionic Liquid‐Based Redox Active Electrolytes for Supercapacitors

Sun

Zhuo

Chen

et al. 2022

Adv Funct Materials

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Supercapacitors (SCs) are fascinating energy storage devices due to their delivery of exceptional power density and long cycling stability. Unfortunately, their practical applications are still impeded by relatively inferior energy density, which is proportional to the square of the operating voltage of SCs. Ionic liquid (IL) electrolytes have a wide electrochemical stability window and thus can be used to significantly increase the energy density of SCs. The introduction of redox active species into IL-based electrolytes effectively contributes to pseudocapacitance. Accordingly, IL-based redox active electrolytes (IL-REs) for SCs are springing up rapidly in recent years. This review provides an overall insight into various IL-REs, including the ILs mixed with other redox active species, the ILs possessing redox active groups themselves, and the IL-based redox gel polymer electrolytes for SCs. The basic understanding of IL electrolytes and IL-REs is introduced and discussed as well as the application of the IL-REs in SCs. Then, the energy storage mechanisms of these IL-REs are discussed, and finally, current challenges and perspectives are highlighted for future research in this promising field.

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Water in Protic Ionic Liquids: Properties and Use of a New Class of Electrolytes for Energy‐Storage Devices

Abstract: Supporting Information and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.

Cited by 42 publications

References 47 publications

Aqueous Co‐Solvent in Zwitterionic‐based Protic Ionic Liquids as Electrolytes in 2.0 V Supercapacitors

Aqueous Co‐Solvent in Zwitterionic‐based Protic Ionic Liquids as Electrolytes in 2.0 V Supercapacitors

Impact of water on the hydrogen bonding between halide‐based ion‐pairs investigated by Raman scattering and density functional theory calculations

Ionic Liquid‐Based Redox Active Electrolytes for Supercapacitors

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