Solution-Processable Thermally Crosslinked Organic Radical Polymer Battery Cathodes.

Area of Science:

• Materials Science
• Electrochemistry
• Polymer Chemistry

Background:

• Organic radical polymers offer rapid charge transfer and high cycling stability, making them attractive for next-generation batteries.
• A key challenge is the dissolution of these polymer electrodes in electrolytes, leading to capacity fade.
• Existing crosslinking methods often lack carbon additive compatibility or compromise solution processability.

Purpose of the Study:

• To develop a one-step, post-synthetic, carbon-compatible crosslinking method for organic polymer electrodes.
• To improve the stability and performance of organic radical polymer electrodes for batteries.
• To enable easy solution processing of these enhanced electrodes.

Main Methods:

• A novel one-step post-synthetic crosslinking strategy was employed.
• The method was designed to be compatible with carbon additives.
• Electrochemical quartz crystal microbalance with dissipation monitoring (EQCM-D) was used for in situ mass transfer analysis.

Main Results:

• The highest electrode capacity of 104 mAh g⁻¹ (vs. theoretical 111 mAh g⁻¹) was achieved with 1 mol% crosslinker.
• Optimal capacity retention of 99.6% was obtained using 3 mol% crosslinker.
• The crosslinking method demonstrated compatibility with solution processing and carbon additives.

Conclusions:

• The developed crosslinking method effectively enhances the performance of organic radical polymer electrodes.
• This approach overcomes limitations of previous crosslinking techniques, enabling both stability and processability.
• The findings provide a pathway for designing advanced organic electrodes for fast-charging, high-capacity batteries.