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Self-Assembled Ionic Clusters Accelerate Li-Ion Transport Through Microphase-Separated Polyelectrolytes.

Cheng-Dong Fang1, Yu-Hang Zhang1, Si-Fan Hu2

  • 1State Key Laboratory For Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Material of Fujian Province (IKKEM), Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Engineering Research Center of Electrochemical Technologies of Ministry of Education, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, Fujian, China.

Angewandte Chemie (International Ed. in English)
|February 22, 2026
PubMed
Summary
This summary is machine-generated.

Researchers developed an elastic microphase polyelectrolyte (EMP) for advanced solid polymer electrolytes. This material self-assembles ionic clusters, enhancing ion transport and mechanical properties for next-generation solid-state lithium batteries.

Keywords:
elastomerionic clusterself‐assemblysolid polymer electrolytesolid‐state battery

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Science

Background:

  • Solid polymer electrolytes are crucial for next-generation batteries, but require improved ionic conductivity and mechanical stability.
  • Achieving molecular-level control over ion coordination and mesoscale morphology is key to enhancing performance.

Purpose of the Study:

  • To introduce a novel elastic microphase polyelectrolyte (EMP) for solid-state lithium batteries.
  • To demonstrate how supramolecular ionic assembly can enhance ion transport, mechanical properties, and electrochemical stability.

Main Methods:

  • Fabrication of an elastic microphase polyelectrolyte (EMP) utilizing thermodynamically driven microphase separation.
  • Characterization of ionic conductivity, Li+ transference number, and mechanical properties (elasticity, self-healing).
  • Operando galvanostatic impedance spectroscopy to study field-responsive conductivity changes.
  • Electrochemical testing of solid-state cells with a LiNi0.8Co0.1Mn0.1O2 cathode.

Main Results:

  • The EMP self-assembles Li+-rich ionic clusters, forming a dynamic, percolating conduction network.
  • Achieved high ionic conductivity (2.9 × 10-4 S cm-1) and Li+ transference number (0.67) at room temperature.
  • Observed a field-responsive conductivity boost (4.1 × 10-4 to 1.9 × 10-3 S cm-1) with increasing current density.
  • Demonstrated excellent mechanical properties including high elasticity and self-healing.
  • Solid-state cells retained 93.92% capacity after 50 cycles under high-capacity loading.

Conclusions:

  • Supramolecular ionic assembly in EMPs effectively couples ion transport, mechanics, and electrochemical stability.
  • The EMP provides a versatile design platform for high-performance, mechanically robust solid-state lithium batteries.
  • This approach offers a pathway to overcome limitations of current solid polymer electrolytes.