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Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications

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Modulating Phase Separation via Multiple Hydrogen Bonding in Polyurethane-Based Gel Polymer Electrolytes for

Puji Lestari Handayani¹, U Hyeok Choi¹

¹Department of Polymer Science and Engineering and Program in Environmental and Polymer Engineering, Inha University, Incheon, 22212, South Korea.

|July 1, 2025

Summary

Hybrid gel polymer electrolytes (GPEs) with enhanced ionic conductivity and mechanical strength were developed using thermoplastic polyurethane and ionic liquids. These GPEs show promise for advanced all-solid-state energy storage devices.

Keywords:

all‐solid‐state supercapacitors hydrogen bonding ionic liquids silica nanoparticles thermoplastic polyurethane

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Synthesizing a Gel Polymer Electrolyte for Supercapacitors, Assembling a Supercapacitor Using a Coin Cell, and Measuring Gel Electrolyte Performance

Synthesizing a Gel Polymer Electrolyte for Supercapacitors, Assembling a Supercapacitor Using a Coin Cell, and Measuring Gel Electrolyte Performance

Published on: November 30, 2022

Area of Science:

Materials Science
Electrochemistry
Polymer Science

Background:

Developing stable and efficient electrolytes is crucial for advanced energy storage devices.
Hybrid gel polymer electrolytes (GPEs) offer potential advantages over liquid electrolytes, including improved safety and mechanical integrity.
Thermoplastic polyurethane (PU) and ionic liquids (ILs) are promising components for GPEs due to their processability and ionic conductivity.

Purpose of the Study:

To synthesize novel hybrid gel polymer electrolytes (GPEs) based on thermoplastic polyurethane (PU) and ionic liquid (IL).
To investigate the effect of silica nanoparticles on the structure, properties, and performance of PU-IL GPEs.
To evaluate the potential of these GPEs in all-solid-state supercapacitors.

Main Methods:

One-pot in situ sol-gel process for synthesizing hybrid GPEs.
Incorporation of 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide [(BMIM)(TFSI)] ionic liquid and silica nanoparticles into a PU matrix.
Characterization using Fourier transform infrared (FTIR) Spectroscopy and differential scanning calorimetry (DSC).
Electrochemical performance evaluation in all-solid-state supercapacitors.

Main Results:

Increasing IL concentration weakened hydrogen bonding, reduced glass transition temperature, and suppressed phase separation.
Silica nanoparticles induced phase separation and enhanced room temperature ionic conductivity and mechanical strength.
The hybrid GPEs exhibited high energy density (183 Wh kg⁻¹) and power density (7 kW kg⁻¹) at 3.5 V.
Supercapacitors demonstrated excellent cycling stability, retaining 98% capacitance after 12,000 cycles.

Conclusions:

The developed hybrid GPEs possess a unique combination of ionic conductivity and mechanical robustness.
Silica nanoparticle incorporation is an effective strategy to tune the GPE's morphology and enhance its electrochemical performance.
These GPEs are promising candidates for next-generation all-solid-state energy storage devices.