Suppressing water clusters by using “hydrotropic” ionic liquids for highly stable aqueous lithium-ion batteries

Zhang, Canfu; Chen, Binbin; Cai, Ziyang; Zhang, Fenglin; Huang, Renzhi; Yan, Mengdie; Liu, Yingchun; Pan, Huilin

doi:10.1039/d2ta04048d

Cited by 6 publications

(1 citation statement)

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“…However, the intrinsically narrow thermodynamic electrochemical stability window (1.23 V) of water restricts the utilization of common high‐capacity anodes and cathodes used in commercial Li‐ion batteries, leading to low energy density. [ 3 ] Moreover, severe side reactions occurring upon cycling deteriorate cycling stability and shorten battery lifetime resulting from continuous electrolyte consumption. Therefore, expanding the kinetic electrochemical window of aqueous electrolytes is a generally efficient approach to mitigate side reactions and enable long‐term aqueous battery operation.…”

Section: Introductionmentioning

confidence: 99%

A Green Asymmetric Bicyclic Co‐Solvent Molecule for High‐Voltage Aqueous Lithium‐Ion Batteries

Wang,

Ou,

Dong

et al. 2024

Advanced Materials

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Hybridizing aqueous electrolytes with organic co‐solvents is regarded as an effective strategy that can expand the stable voltage window of aqueous electrolytes while reducing salt usage and enhancing wettability, but reported organic co‐solvents are usually flammable and toxic, hardly achieving compatibility between safety and electrochemical performance. Here, we report a new non‐flammable and non‐toxic low‐salt‐concentration (1.85 m) aqueous electrolyte via hybridizing with a green and sustainable organic co‐solvent of isosorbide dimethyl ether (IDE) with a special asymmetric bicyclic molecular structure. Owing to the unique three‐dimensional (3D) spatial molecular structure of IDE, a five‐membered ring structure can be formed by binding the Li ion with the O atoms of the endo‐OCH3 and opposite cyclic ether in the same plane of IDE. Meanwhile, the steric hindrance effect induced by the 3D spatial bicyclic molecular structure of IDE weakens its solvation ability with Li ions, allowing more anions to participate in the primary solvation sheath of Li ion and thus generating a robust and uniform LiF‐rich SEI layer while containing elastic IDE‐derived organics. Moreover, the asymmetric bicyclic IDE molecules with multiple O atoms can effectively regulate the intermolecular hydrogen bonding networks, thus reducing H2O molecule activity and expanding the electrochemical window. Such unique solvation structures and optimized hydrogen bonding networks enabled by the asymmetric bicyclic molecular structure of IDE effectively suppress electrode/electrolyte interfacial side reactions, thus achieving a 4.3 V voltage window. The as‐developed Li4Ti5O12(LTO)||LiMn2O4(LMO) full cell delivers outstanding cycling performance with an average Coulombic efficiency of 99.35% over 450 cycles at 2 C.This article is protected by copyright. All rights reserved

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Section: Introductionmentioning

confidence: 99%

A Green Asymmetric Bicyclic Co‐Solvent Molecule for High‐Voltage Aqueous Lithium‐Ion Batteries

Wang,

Ou,

Dong

et al. 2024

Advanced Materials

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Regulation of Molecular Microheterogeneity in Electrolytes Enables Ampere‐Hour‐Level Aqueous LiMn₂O₄||Li₄Ti₅O₁₂ Pouch Cells

Zhang,

Chen,

Chen

et al. 2024

Advanced Materials

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Aqueous batteries are attractive due to their high safety and fast reaction kinetics, but the narrow electrochemical stability window of H2O limits their applications. It is a big challenge to broaden the electrochemical operation window of aqueous electrolytes while retaining fast reaction kinetics. Here, a new organic aqueous mixture electrolyte of manipulatable (3D) molecular microheterogeneity with H2O‐rich and H2O‐poor domains is demonstrated. H2O‐poor domains molecularly surround the reformed microclusters of H2O molecules through interfacial H‐bonds, which thus not only inhibit the long‐range transfer of H2O but also allow fast and consecutive Li+ transport. This new design enables low‐voltage anodes reversibly cycling with aqueous‐based electrolytes and high ionic conductivity of 4.5 mS cm−1. LiMn2O4||Li4Ti5O12 full cells demonstrate excellent cycling stability over 1000 cycles under various C rates and a low temperature of −20 °C. 1 Ah pouch cell delivers a high energy density of 79.3 Wh kg−1 and high Coulombic efficiency of 99.4% at 1 C over 200 cycles. This work provides new insights into the design of electrolytes based on the molecular microheterogeneity for rechargeable batteries.

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Hybrid Aqueous/Non‐aqueous Electrolytes for Lithium‐Ion and Zinc‐Ion Batteries: A Mini‐Review

Zhang

Cai

Huang

et al. 2023

Batteries & Supercaps

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In recent years, the development of aqueous lithium‐ion batteries and aqueous zinc‐ion batteries has received extensive attention thanks to the advantages of high safety, environmental friendliness, and easy assembly conditions. However, aqueous batteries are always restricted in terms of limited cycling stability and low energy density due to their intrinsically narrow electrochemical window, hydrogen evolution, and side reactions. These problems can be remarkably alleviated by hybridizing aqueous/non‐aqueous electrolytes; however, few detailed discussions on relevant strategies have been reported. In this mini‐review, we summarize the latest progress and contributions of various hybrid aqueous/non‐aqueous electrolytes for rechargeable aqueous lithium‐ion batteries and aqueous zinc‐ion batteries. The current challenges and development directions are also discussed for hybrid electrolytes.

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Suppressing water clusters by using “hydrotropic” ionic liquids for highly stable aqueous lithium-ion batteries

Abstract: The state-of-the-art water-in-salt electrolytes exhibit wider electrochemical window than conventional dilute aqueous electrolytes. However, the extended electrochemical stability window via increasing salt concentration has reached a bottleneck. An alternative approach...

Cited by 6 publications

References 50 publications

A Green Asymmetric Bicyclic Co‐Solvent Molecule for High‐Voltage Aqueous Lithium‐Ion Batteries

A Green Asymmetric Bicyclic Co‐Solvent Molecule for High‐Voltage Aqueous Lithium‐Ion Batteries

Regulation of Molecular Microheterogeneity in Electrolytes Enables Ampere‐Hour‐Level Aqueous LiMn₂O₄||Li₄Ti₅O₁₂ Pouch Cells

Hybrid Aqueous/Non‐aqueous Electrolytes for Lithium‐Ion and Zinc‐Ion Batteries: A Mini‐Review

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Suppressing water clusters by using “hydrotropic” ionic liquids for highly stable aqueous lithium-ion batteries

Abstract: The state-of-the-art water-in-salt electrolytes exhibit wider electrochemical window than conventional dilute aqueous electrolytes. However, the extended electrochemical stability window via increasing salt concentration has reached a bottleneck. An alternative approach...

Cited by 6 publications

References 50 publications

A Green Asymmetric Bicyclic Co‐Solvent Molecule for High‐Voltage Aqueous Lithium‐Ion Batteries

A Green Asymmetric Bicyclic Co‐Solvent Molecule for High‐Voltage Aqueous Lithium‐Ion Batteries

Regulation of Molecular Microheterogeneity in Electrolytes Enables Ampere‐Hour‐Level Aqueous LiMn2O4||Li4Ti5O12 Pouch Cells

Hybrid Aqueous/Non‐aqueous Electrolytes for Lithium‐Ion and Zinc‐Ion Batteries: A Mini‐Review

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Product

Resources

About

Regulation of Molecular Microheterogeneity in Electrolytes Enables Ampere‐Hour‐Level Aqueous LiMn₂O₄||Li₄Ti₅O₁₂ Pouch Cells