Build a High‐Performance All‐Solid‐State Lithium Battery through Introducing Competitive Coordination Induction Effect in Polymer‐Based Electrolyte

• DOI: 10.1002/ange.202400960
• Publication Date: 2024-02-22T13:36:22Z
• Authors: Tenghui Wang; Butian Chen; Chong Liu; Taiguang Li; Xiangfeng Liu
• Keywords: Polymer Electrolytes; Coordination polymer; Organic radical battery

Abstract Polymer‐inorganic composite electrolytes (PICE) have attracted tremendous attention in all‐solid‐state lithium batteries (ASSLBs) due to facile processability. However, the poor Li + conductivity at room temperature (RT) and interfacial instability severely hamper practical application. Herein, we propose a concept of competitive coordination induction effects (CCIE) reveal essential correlation between local structure chemistry PEO‐based PICE. CCIE introduction greatly enhances ionic electrochemical performances ASSLBs 30 °C. Owing (Cs … TFSI − , Cs C−O−C 2,4,6‐TFA ) from cation CsPF 6 molecule (2,4,6‐TFA: 2,4,6‐trifluoroaniline), multimodal weak environment is constructed enabling high efficient migration °C (Li conductivity: 6.25×10 −4 S cm −1 ; t =0.61). Since tends be enriched interface, PF situ form LiF‐Li 3 N‐Li 2 O‐Li solid electrolyte interface with electrostatic shielding effects. The assembled without adding wetting agent exhibit outstanding rate capability (LiFePO 4: 147.44 mAh g @1 C 107.41mAhg @2 C) cycling stability 4 :94.65 %@200cycles@0.5 C; LiNi 0.5 Co 0.2 Mn 0.3 O : 94.31 %@200 cycles@0.3 C). This work proposes reveals its mechanism designing PICE as well compatibility near RT for high‐performance ASSLBs.