“Ionic liquids-in-salt” – a promising electrolyte concept for high-temperature lithium batteries?

Marczewski, Maciej; Stanje, Bernhard; Hanzu, Ilie; Wilkening, Martin; Johansson, Patrik

doi:10.1039/c4cp01133c

Cited by 80 publications

(83 citation statements)

References 31 publications

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“…However,i ti sn ot clear whether viscosity and conductivity are the only parameters restricting rate performance. Recently,s everal studies have provent hat concentrated electrolytes based on organic solvents [32] or ILs [33][34][35] exhibit improved rate capabilities compared with those of diluted electrolytes. In an effort to understand the difference in performance of cells containing concentrated and dilute electrolytes, particularly in terms of the seemingly counterintuitive faster lithium transport mechanism at high concentration, a series of FTFSI-based electrolyte with different concentrations was prepareda nd examined.…”

Section: Resultsmentioning

confidence: 99%

Concentrated Ionic‐Liquid‐Based Electrolytes for High‐Voltage Lithium Batteries with Improved Performance at Room Temperature

Gao

Mariani

et al. 2019

ChemSusChem

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Ionic liquids (ILs) have been widely explored as alternative electrolytes to combat the safety issues associated with conventional organic electrolytes. However, hindered by their relatively high viscosity, the electrochemical performances of IL‐based cells are generally assessed at medium‐to‐high temperature and limited cycling rate. A suitable combination of alkoxy‐functionalized cations with asymmetric imide anions can effectively lower the lattice energy and improve the fluidity of the IL material. The Li/Li1.2Ni0.2Mn0.6O2 cell employing N‐N‐diethyl‐N‐methyl‐N‐(2‐methoxyethyl)ammonium (fluorosulfonyl)(trifluoromethanesulfonyl)imide (DEMEFTFSI)‐based electrolyte delivered an initial capacity of 153 mAh g−1 within the voltage range of 2.5–4.6 V, with a capacity retention of 65.5 % after 500 cycles and stable coulombic efficiencies exceeding 99.5 %. Moreover, preliminary battery tests demonstrated that the drawbacks in terms of rate capability could be improved by using Li‐concentrated IL‐based electrolytes. The improved room‐temperature rate performance of these electrolytes was likely owing to the formation of Li+‐containing aggregate species, changing the concentration‐dependent Li‐ion transport mechanism.

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Section: Resultsmentioning

confidence: 99%

Concentrated Ionic‐Liquid‐Based Electrolytes for High‐Voltage Lithium Batteries with Improved Performance at Room Temperature

Gao

Mariani

et al. 2019

ChemSusChem

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“…Furthermore, the corrosion of Al current collector was considerably lower in the molten salt as compared with the conventional electrolytes of LIB. [74] This is the same molten salt introduced by Armand and co-workers, [66,70] but the "IL-in-salt" relied upon the idea of superconcentrated LiTFSI. [71][72][73] A key advantageous feature of LiTFSI as highlighted from the early works is its high solubility.…”

Section: Operating Potential Windowmentioning

confidence: 99%

“…Gaining this feature, Marczewski et al proposed the idea of "IL-in-salt" employing LiTFSI and 1-ethyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide (EMImTFSI). [74] This is the same molten salt introduced by Armand and co-workers, [66,70] but the "IL-in-salt" relied upon the idea of superconcentrated LiTFSI. Similarly, "polymer-in-salt" was reported utilizing LiTFSI and polyacrylonitrile (PAN).…”

Section: Operating Potential Windowmentioning

confidence: 99%

High‐Energy Aqueous Lithium Batteries

Eftekhari¹

2018

Advanced Energy Materials

152

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research, aqueous electrolytes were occasionally employed for the investigation of cathode materials instead of the conventional nonaqueous electrolytes. [9,10] It was discussed that the simplicity of an aqueous electrolyte provides a better opportunity for the fundamental studies of the process of intercalation/deintercalation of Li-ions as opposed to the nonaqueous electrolytes. For instance, although the formation of solid electrolyte interphase (SEI) is of utmost importance for the cyclability of LIB, the significant role of the electrolyte does not allow to exclusively study the electrochemical behavior of the electrode material under consideration. The current research has specifically targeted the development of ARLBs, but in practice, most of the recent papers have followed the same line of research in investigating a limited range of cathode and anode materials in the same aqueous electrolytes. [11][12][13][14][15][16][17][18][19][20][21][22][23][24][25][26][27][28] A possible reason is that the key advantage of ARLBs was low cost, and thus, the focus was limited to a few inexpensive materials (e.g., lithium salts). Aqueous electrolytes are definitely excellent choices for the fundamental studies of electrode materials, but the practical development of ARLBs needs overcoming the key obstacles rather than finding more cathode materials.In any case, aqueous electrolytes were occasionally used during the 2000s by various research groups, but there was no vivid plan for the development of ARLBs. These works have been extensively reviewed before, [29][30][31][32][33] and it is not aimed to repeat the general works on aqueous electrolytes here. During the recent years, new opportunities have been introduced, which can extend the stable potential window of aqueous electrolyte to the range of 3-4 V. Upon this advancement, aqueous electrolytes can fairly compete with the conventional nonaqueous electrolytes for the fabrication of cheaper and safer LIBs. On the other hand, novel designs such as self-healing [34] or flexible [16,35,36] ARLBs have paved the path for new practical potentials of aqueous electrolytes. The present paper specifically focuses on the recent advancements and attempts to foster the strategy of research to shed light on the pathway of this emerging area of research. Two factors are directly responsible for achieving a high energy density, the specific capacity, and the cell voltage. Since the former is not massively controlled by the electrolyte and the specific capacity of most electroactive Owing to the high voltage of lithium-ion batteries (LIBs), the dominating electrolyte is non-aqueous. The idea of an aqueous rechargeable lithium battery (ARLB) dates back to 1994, but it had attracted little attention due to the narrow stable potential window of aqueous electrolytes, which results in low energy density. However, aqueous electrolytes were employed during the 2000s for the fundamental studies of electrode materials in the absence of side reactions such as the decomposition of organic spec...

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“…When the fraction of salt exceeds that of an IL, we get a superconcentrated IL-in-salt electrolyte. 22 Although an increased concentration of alkali metal ions significantly increases the viscosity of the system and decreases the ionic conductivity, some promising electrochemical behavior of note have been demonstrated. For example, at increased alkali metal salt concentrations, significant enhancements in electrochemical stability and rate 0021-9606/2018/148(19)/193813/9/$30.00…”

Section: Introductionmentioning

confidence: 99%

Cation effect on small phosphonium based ionic liquid electrolytes with high concentrations of lithium salt

Chen

Kerr

Forsyth

2018

The Journal of Chemical Physics

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Ionic liquid electrolytes with high alkali salt concentrations have displayed some excellent electrochemical properties, thus opening up the field for further improvements to liquid electrolytes for lithium or sodium batteries. Fundamental computational investigations into these high concentration systems are required in order to gain a better understanding of these systems, yet they remain lacking. Small phosphonium-based ionic liquids with high concentrations of alkali metal ions have recently shown many promising results in experimental studies, thereby prompting us to conduct further theoretical exploration of these materials. Here, we conducted a molecular dynamics simulation on four small phosphonium-based ionic liquids with 50 mol. % LiFSI salt, focusing on the effect of cation structure on local structuring and ion diffusional and rotational dynamics-which are closely related to the electrochemical properties of these materials.

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“Ionic liquids-in-salt” – a promising electrolyte concept for high-temperature lithium batteries?

Cited by 80 publications

References 31 publications

Concentrated Ionic‐Liquid‐Based Electrolytes for High‐Voltage Lithium Batteries with Improved Performance at Room Temperature

Concentrated Ionic‐Liquid‐Based Electrolytes for High‐Voltage Lithium Batteries with Improved Performance at Room Temperature

High‐Energy Aqueous Lithium Batteries

Cation effect on small phosphonium based ionic liquid electrolytes with high concentrations of lithium salt

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