Build a High-Performance All-Solid-State Lithium Battery through Introducing Competitive Coordination Induction Effect in Polymer-Based Electrolyte.
Angew Chem Int Ed Engl
; 63(16): e202400960, 2024 Apr 15.
Article
in En
| MEDLINE
| ID: mdl-38385630
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 the practical application. Herein, we propose a concept of competitive coordination induction effects (CCIE) and reveal the essential correlation between the local coordination structure and the interfacial chemistry in PEO-based PICE. CCIE introduction greatly enhances the ionic conductivity and electrochemical performances of ASSLBs at 30 °C. Owing to the competitive coordination (Cs+
TFSI-
Li+, Cs+
C-O-C
Li+ and 2,4,6-TFA
Li
TFSI-) from the competitive cation (Cs+ from CsPF6) and molecule (2,4,6-TFA 2,4,6-trifluoroaniline), a multimodal weak coordination environment of Li+ is constructed enabling a high efficient Li+ migration at 30 °C (Li+ conductivity 6.25×10-4â
S cm-1; tLi +=0.61). Since Cs+ tends to be enriched at the interface, TFSI- and PF6 - in situ form LiF-Li3N-Li2O-Li2S enriched solid electrolyte interface with electrostatic shielding effects. The assembled ASSLBs without adding interfacial wetting agent exhibit outstanding rate capability (LiFePO4 147.44â
mAh g-1@1â
C and 107.41mAhg-1@2â
C) and cycling stability at 30 °C (LiFePO494.65 %@200cycles@0.5â
C; LiNi0.5Co0.2Mn0.3O2 94.31 %@200â
cycles@0.3â
C). This work proposes a concept of CCIE and reveals its mechanism in designing PICE with high ionic conductivity as well as high interfacial compatibility at near RT for high-performance ASSLBs.
Full text:
1
Collection:
01-internacional
Database:
MEDLINE
Language:
En
Journal:
Angew Chem Int Ed Engl
Year:
2024
Type:
Article