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Interfacial Microgel Self-Assembly Engineered for Superionic Conduction in PVDF Electrolyte.

Yanping Chen¹, Chengdong Fang¹, Qingquan Lin¹

¹State Key Laboratory For Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials 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, 361005, China.

Angewandte Chemie (International Ed. in English)

|February 16, 2026

Summary

This summary is machine-generated.

This study introduces an ion-mediated microgel self-assembly strategy for advanced polymer electrolytes. This method enhances ion conduction and stability in solid-state batteries, improving performance and safety.

Keywords:

Composite solid‐state electrolyte Interface dynamics Microgels Self‐assembly

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From Molecules to Materials: Engineering New Ionic Liquid Crystals Through Halogen Bonding

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Area of Science:

Materials Science
Electrochemistry
Polymer Science

Background:

Polyvinylidene fluoride (PVDF)-based electrolytes face limitations in ion conduction and stability.
Developing efficient solid-state electrolytes is crucial for next-generation batteries.

Purpose of the Study:

To develop an ion-mediated interfacial microgel self-assembly strategy for polymer electrolytes.
To overcome the intrinsic limitations of PVDF-based electrolytes by optimizing ion coordination.

Main Methods:

Ion-mediated interfacial microgel self-assembly.
Fabrication of M(D)-PVDF-HFP electrolyte.
Electrochemical characterization including ionic conductivity, transference number, and cycling stability.
Galvanostatic electrochemical impedance spectroscopy and finite element method simulations.

Main Results:

The M(D)-PVDF-HFP electrolyte exhibits high ionic conductivity (4.54 × 10⁻⁴ S cm⁻¹), a high Li⁺ transference number (0.63), and a wide operating window (4.8 V).
Demonstrated rapid response and uniform Li⁺ flux under operating conditions.
Achieved stable Li plating/stripping for over 5,000 hours in symmetric cells.
All-solid-state cells with a LiNi₀.₈Co₀.₁Mn₀.₁O₂ cathode delivered a high reversible specific capacity (181.08 mAh g⁻¹).

Conclusions:

The proposed strategy successfully induces uniform Li⁺ flux in heterogeneous polymer electrolytes.
Highlights the critical role of internal interface behavior in solid-state polymer electrolytes.
Offers a promising pathway for developing high-performance and safe solid-state batteries.