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Multiple Dynamic Bonds-Driven Integrated Cathode/Polymer Electrolyte for Stable All-Solid-State Lithium Metal

Jing Chen1, Xuetian Deng1, Yiyang Gao1

  • 1School of Chemistry, Xi'an Jiaotong University, Engineering Research Center of Energy Storage Materials and Devices, Ministry of Education, State Key Laboratory of Electrical Insulation and Power Equipment, Xi'an, 710049, P. R. China.

Angewandte Chemie (International Ed. in English)
|July 11, 2023
PubMed
Summary

Researchers developed dynamic supramolecular ionic conductive elastomers (DSICE) for solid-state lithium metal batteries. This material integrates electrolytes and binders, improving interfacial contact and enabling stable, high-performance energy storage with enhanced safety.

Keywords:
Dynamic BondsElectrode-Electrolytes InterfaceLithium Metal BatteriesPolymer ElectrolytesSolid-State Battery

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Chemistry

Background:

  • All-solid-state lithium metal batteries (LMBs) offer higher energy and safety but face challenges with interfacial issues.
  • Limited solid contact between electrolytes and electrodes causes poor charge transport and high interfacial resistance, hindering performance.
  • Existing LMBs struggle with discontinuous ion transport and non-uniform lithium deposition, limiting their practical application.

Purpose of the Study:

  • To develop an integrated cathode/polymer electrolyte system for all-solid-state LMBs.
  • To address interfacial challenges by creating intimate contact at the electrolyte-electrode interface.
  • To enhance the electrochemical performance, stability, and safety of solid-state batteries.

Main Methods:

  • Designed and synthesized dynamic supramolecular ionic conductive elastomers (DSICE) with dynamic bonds.
  • Utilized DSICE as both the polymer electrolyte and cathode binder for lithium iron phosphate (LFP) cathodes.
  • Fabricated and tested Li|DSICE|LFP-DSICE cells, including pouch cells, to evaluate electrochemical performance, flexibility, and safety.

Main Results:

  • Achieved an ultrathin pure polymer electrolyte (12 μm) with excellent electrochemical and mechanical properties.
  • DSICE integration created molecular-level interfacial contact, enabling continuous Li+ transport and uniform Li+ deposition.
  • Demonstrated superior long-term charge/discharge stability (>600 cycles, >99.8% Coulombic efficiency) and high capacity retention (80% after 400 cycles).

Conclusions:

  • The integrated DSICE material effectively resolves interfacial issues in all-solid-state LMBs.
  • The developed cells exhibit excellent electrochemical performance, flexibility, and safety, paving the way for practical applications.
  • DSICE shows significant potential as a multifunctional material for advanced solid-state battery technologies.