A Fast Na‐Ion Conduction Polymer Electrolyte via Triangular Synergy Strategy for Quasi‐Solid‐State Batteries

Polymer electrolytes provide a visible pathway for the construction of high‐safety quasi‐solid‐state batteries due to their high interface compatibility and processability. Nevertheless, sluggish ion transfer at room temperature seriously limits their applications. Herein, a triangular synergy strat...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2023-12, Vol.62 (52), p.e202315076-n/a
Main Authors: Luo, Jun, Yang, Mingrui, Wang, Denghui, Zhang, Jiyu, Song, Keming, Tang, Guochuan, Xie, Zhengkun, Guo, Xiaoniu, Shi, Yu, Chen, Weihua
Format: Article
Language:English
Subjects:
Batteries
Cations
Conduction
Dissociation
Electrochemistry
Electrolytes
Electrolytic cells
Ion currents
Ion transport
Ionic Conductivity
Ionic liquids
Ions
Molten salt electrolytes
Polymer Electrolyte
Polymers
Room temperature
Safety
Salts
Sodium
Sodium-Ion Battery
Solid electrolytes
Solid-State Battery
Strategy
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Summary:Polymer electrolytes provide a visible pathway for the construction of high‐safety quasi‐solid‐state batteries due to their high interface compatibility and processability. Nevertheless, sluggish ion transfer at room temperature seriously limits their applications. Herein, a triangular synergy strategy is proposed to accelerate Na‐ion conduction via the cooperation of polymer‐salt, ionic liquid, and electron‐rich additive. Especially, PVDF‐HFP and NaTFSI salt acted as the framework to stably accommodate all the ingredients. An ionic liquid (Emim+‐FSI−) softened the polymer chains through a weakening molecule force and offered additional liquid pathways for ion transport. Physicochemical characterizations and theoretical calculations demonstrated that electron‐rich Nerolin with π‐cation interaction facilitated the dissociation of NaTFSI and effectively restrained the competitive migration of large cations from EmimFSI, thus lowering the energy barrier for ion transport. The strategy resulted in a thin F‐rich interphase dominated by NaTFSI salt's decomposition, enabling rapid Na+ transmission across the interface. These combined effects resulted in a polymer electrolyte with high ionic conductivity (1.37×10−3 S cm−1) and tNa+ (0.79) at 25 °C. The assembled cells delivered reliable rate capability and stability (200 cycles, 99.2 %, 0.5 C) with a good safety performance. A fast Na‐ion conduction polymer electrolyte was designed through a triangular synergy strategy, which limits the migration of ionic liquid and facilitates the dissociation of salt, resulting in a faster Na+ conduction in the polymer electrolyte. The modified polymer electrolyte led to a salt‐decomposition dominated interphase, which effectively suppressed gas evolution from ionic liquid decomposition, ensuring battery safety.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202315076