Robust, High-Temperature-Resistant Polyimide Separators with Vertically Aligned Uniform Nanochannels for High-Performance Lithium-Ion Batteries

Abstract

Separator is an essential component of lithium-ion batteries (LIBs), playing a pivotal role in battery safety and electrochemical performance. However, conventional polyolefin separators suffer from poor thermal stability and nonuniform pore structures, hindering their effectiveness in preventing thermal shrinkage and inhibiting lithium (Li) dendrites. Herein, we present a robust, high-temperature-resistant polyimide (PI) separator with vertically aligned uniform nanochannels, fabricated via ion track-etching technology. The resultant PI track-etched membranes (PITEMs) effectively homogenize Li-ion distribution, demonstrating enhanced ionic conductivity (0.57 mS cm^–1) and a high Li⁺ transfer number (0.61). PITEMs significantly prolong the cycle life of Li/Li cells to 1200 h at 3 mA cm^–2. For Li/LiFePO₄ cells, this approach enables a specific capacity of 143 mAh g^–1 and retains 83.88% capacity after 300 cycles at room temperature. At 80 °C, the capacity retention remains at 85.92% after 200 cycles. Additionally, graphite/LiFePO₄ pouch cells with PITEMs display enhanced cycling stability, retaining 73.25% capacity after 1000 cycles at room temperature and 78.41% after 100 cycles at 80 °C. Finally, PITEMs-based pouch cells can operate at 150 °C. This separator not only addresses the limitations of traditional separators, but also holds promise for mass production via roll-to-roll methods. We expect this work to offer insights into designing and manufacturing of functional separators for high-safety LIBs.