Deep Eutectic Solvents as Nonflammable Electrolytes for Durable Sodium‐Ion Batteries

Sloovere, Dries De; Vanpoucke, Danny E. P.; Paulus, Andreas; Joos, Bjorn; Calvi, Lavinia; Vranken, Thomas; Reekmans, Gunter; Adriaensens, Peter; Eshraghi, Nicolas; Mahmoud, Abdelfattah; Boschini, Frèdéric; Safari, Mohammadhosein; Bael, Marlies K. Van; Hardy, An

doi:10.1002/aesr.202270007

Cited by 15 publications

(31 citation statements)

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“…According to De Sloovere and co-workers, the reason for the higher electrochemical stability in more concentrated DESs is the strong interaction between the ions and the solvent in the NaTFSI:NMA mixture leading to a decreasing energy of the highest occupied molecular orbital (HOMO) of NMA with increasing salt concentration. [25] The resulting decomposition potentials for highly concentrated electrolytes correspond well to the values we found in our study. The stabilizing effect of a high share of NaTFSI will be discussed further below in more detail.…”

Section: Electrochemical Characterizationsupporting

confidence: 88%

“…Beside the disadvantageous wetting of the electrodes [28,29] , high salt concentrations can hinder salt dissociation and lower the ionic conductivity of the electrolyte. [25] At 1.5 C and after a dwell time of 70 h, NaTFSI:NMA 1:4 exhibits an improved performance. The Coulombic efficiency is relatively high (97.5%), accompanied by a capacity retention close to 1 (Figures S10A and B).…”

Section: Galvanostatic Cyclingmentioning

confidence: 89%

“…NaTFSI:NMA mixtures without recrystallization and melting have also been observed previously in DSC experiments with a heating rate of 10 °C•min -1 . [25] The same is true for mixtures of LiTFSI with different sulfonamidebased hydrogen bond donors. [26] In a LiTFSI:NMA DES, a glass transition and a melting peak dependent on the molar ratio have been observed by DSC measurements.…”

Section: Glass Transitionmentioning

confidence: 96%

“…Because of the decrease in HOMO energy, the oxidation of NMA shifts to higher potentials. [25] In DESs with lower salt concentrations than the eutectic ratio, non-complexed or not fully complexed NMA molecules are less stable causing continuous electrolyte decomposition at potentials higher than 1 V.…”

Section: Electrochemical Characterizationmentioning

confidence: 99%

“…For the mixtures with xNaTFSI ≤ 0.06, a small endothermic peak appears around 0 °C (Figure 1A), which is also observable in pure NMA (Figure S2) and has been detected previously. [25] It is probably connected to the residual water content of undried NMA.…”

Section: Glass Transitionmentioning

confidence: 99%

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Combining Deep Eutectic Solvents with TEMPO-based Polymer Electrodes: Influence of Deep Eutectic Solvents' Molar Ratio on Electrode Performance

Uhl

Geng

Schuster

et al. 2022

Preprint

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For sustainable storage of electrical energy, all-organic batteries based on redox-active polymers promise to become an alternative to conventional lithium ion batteries. Yet, polymers can only contribute to the goal of an all-organic cell as electrodes or as solid electrolytes. Here, we replace the electrolyte with a sustainable deep eutectic solvent (DES) composed of sodium bis(trifluoromethanesulfonyl)imide (NaTFSI) and N-methylacetamide (NMA), while using poly(2,2,6,6-tetramethylpiperidin-1-yl-oxyl methacrylate) (PTMA) as cathode. The successful combination of a DES with a polymer electrode is reported here for the first time. The electrochemical stability of PTMA electrodes in the DES at the eutectic molar ratio of 1:6 is comparable to conventional battery electrolytes. More viscous electrolytes with higher salt concentrations can hinder charging and discharging at high rates. Lower salt concentrations on the other hand lead to decreasing capacities and faster decomposition. The used eutectic mixture of 1:6 is best suited uniting high stability and moderate viscosity.

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Section: Electrochemical Characterizationsupporting

confidence: 88%

Section: Galvanostatic Cyclingmentioning

confidence: 89%

Section: Glass Transitionmentioning

confidence: 96%

Section: Electrochemical Characterizationmentioning

confidence: 99%

Section: Glass Transitionmentioning

confidence: 99%

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Combining Deep Eutectic Solvents with TEMPO-based Polymer Electrodes: Influence of Deep Eutectic Solvents' Molar Ratio on Electrode Performance

Uhl

Geng

Schuster

et al. 2022

Preprint

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Nonflammable Succinonitrile‐Based Deep Eutectic Electrolyte for Intrinsically Safe High‐Voltage Sodium‐Ion Batteries

Chen,

Yang,

et al. 2024

Advanced Materials

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Intrinsically safe sodium‐ion batteries (SIBs) are considered a promising candidate for large‐scale energy storage systems. However, the high flammability of conventional electrolytes may pose serious safety threats and even explosions. Herein, we propose a strategy of constructing a deep eutectic electrolyte (DEE) to boost the safety and electrochemical performance of succinonitrile (SN)‐based electrolyte. The strong hydrogen bond between S = O of 1,3,2‐dioxathiolane‐2,2‐dioxide (DTD) and the α‐H of SN endows the enhanced safety and compatibility of SN with Lewis bases. Meanwhile, the DTD participates in the inner Na+ sheath and weakens the coordination number of SN. The unique solvation configuration promotes the formation of robust gradient inorganic‐rich electrode‐electrolyte interphase, and merits stable cycling of half cells in a wide temperature range, with a capacity retention of 82.8% after 800 cycles (25 °C) and 86.3% after 100 cycles (60 °C). Correspondingly, the full cells deliver tremendous improvement in cycling stability and rate performance.This article is protected by copyright. All rights reserved

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Chlorination Design for Highly Stable Electrolyte toward High Mass Loading and Long Cycle Life Sodium‐Based Dual‐Ion Battery

Lin,

Shang,

Liu

et al. 2024

Advanced Materials

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Sodium‐based dual ion batteries (SDIBs) have garnered significant attention as novel energy storage devices offering the advantages of high‐voltage and low‐cost. Nonetheless, conventional electrolytes exhibit low resistance to oxidation and poor compatibility with electrode materials, resulting in rapid battery failure. In this study, for the first time, we propose a chlorination design of electrolytes for SDIB. Using ethyl methyl carbonate (EMC) as a representative solvent, chlorine‐substituted EMC (Cl‐EMC) not only demonstrates increased oxidative stability ascribed to the electron‐withdrawing characteristics of chlorine atom, electrolyte compatibility with both the cathode and anode have also been greatly improved by forming Cl‐containing interface layers. Consequently, a discharge capacity of 104.6 mAh g−1 within voltage range of 3.0‐5.0 V is achieved for Na||graphite SDIB that employs a high graphite cathode mass loading of 5.0 mg cm−2, along with almost no capacity decay after 900 cycles. Notably, the Na||graphite SDIB can be revived for additional 900 cycles through the replacement of a fresh Na anode. As the mass loading of graphite cathode increased to 10 mg cm−2, Na||graphite SDIB is still capable of sustaining over 700 times with ≈100% capacity retention. These results mark the best outcome among reported SDIBs. This study corroborates the effectiveness of chlorination design in developing high‐voltage electrolytes and attaining enduring cycle stability of Na‐based energy storage devices.This article is protected by copyright. All rights reserved

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Deep Eutectic Solvents as Nonflammable Electrolytes for Durable Sodium‐Ion Batteries

Cited by 15 publications

References 0 publications

Combining Deep Eutectic Solvents with TEMPO-based Polymer Electrodes: Influence of Deep Eutectic Solvents' Molar Ratio on Electrode Performance

Combining Deep Eutectic Solvents with TEMPO-based Polymer Electrodes: Influence of Deep Eutectic Solvents' Molar Ratio on Electrode Performance

Nonflammable Succinonitrile‐Based Deep Eutectic Electrolyte for Intrinsically Safe High‐Voltage Sodium‐Ion Batteries

Chlorination Design for Highly Stable Electrolyte toward High Mass Loading and Long Cycle Life Sodium‐Based Dual‐Ion Battery

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