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Build a High-Performance All-Solid-State Lithium Battery through Introducing Competitive Coordination Induction

Tenghui Wang1, Butian Chen1, Chong Liu1

  • 1Center of Materials Science and Optoelectronics Engineering, College of Materials Science and Optoelectronic Technology, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.

Angewandte Chemie (International Ed. in English)
|February 22, 2024
PubMed
Summary

This study introduces competitive coordination induction effects (CCIE) to enhance polymer-inorganic composite electrolytes (PICE) for all-solid-state lithium batteries (ASSLBs). CCIE improves ionic conductivity and interfacial stability at 30°C, enabling high-performance ASSLBs.

Keywords:
All-Solid-State Lithium BatteryCompetitive Coordination Induction EffectElectrochemical PerformanceInterfacial ChemistryPolymer-Inorganic Composite Solid Electrolyte

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Science

Background:

  • Polymer-inorganic composite electrolytes (PICE) offer facile processing for all-solid-state lithium batteries (ASSLBs).
  • Poor room temperature (RT) Li+ conductivity and interfacial instability limit PICE application in ASSLBs.

Purpose of the Study:

  • To propose and investigate the concept of competitive coordination induction effects (CCIE) in PEO-based PICE.
  • To establish the correlation between local coordination structure and interfacial chemistry in PICE.
  • To enhance ionic conductivity and electrochemical performance of ASSLBs at 30°C.

Main Methods:

  • Introduction of competitive cation (Cs+) and molecule (2,4,6-trifluoroaniline, TFA) to PEO-based PICE.
  • Construction of a multimodal weak coordination environment for Li+.
  • Analysis of interfacial chemistry and solid electrolyte interphase (SEI) formation.

Main Results:

  • CCIE significantly enhances Li+ migration and conductivity (6.25×10^-4 S cm^-1) at 30°C.
  • Cs+ enrichment at the interface promotes formation of a stable SEI layer (LiF-Li3N-Li2O-Li2S).
  • Assembled ASSLBs demonstrate excellent rate capability and cycling stability at 30°C without interfacial wetting agents.

Conclusions:

  • CCIE is a viable strategy for designing PICE with high ionic conductivity and interfacial compatibility.
  • This approach enables high-performance ASSLBs operating at near room temperature.
  • The findings provide a mechanism for optimizing PICE for practical ASSLB applications.