A newly-developed heat-resistance polyimide microsphere coating to enhance the thermal stability of commercial polyolefin separators for advanced lithium-ion battery

Polymer separators with high-temp dimensional stability is strongly demanded for high-safety lithium-ion batteries (LIBs). In this study, a novel polyimide (PI) microsphere coating slurry was prepared and then plated on Celgard polypropylene (PP) separator, producing PP@PI microsphere composite separator with excellent thermal stability, flame retardancy, high liquid retention capacity and high ionic conductivity by a simple blade-coating process. The results show that the thermal stability and liquid retention capacity of the PP@PI microsphere composite separator are significantly improved. Compared with the pure commercial PP separator which sharply shrank at 150 °C, the PI microsphere composite separator shows negligible shrinkage over 150 °C. The obtained PP@PI microsphere composite separators exhibited excellent thermal stability and fire-resistance properties. At the same time, the peel strength of composite separator reached 138.6 N·m −1 , with excellent adhesion. The surface density of PP@PI microsphere composite separator is 16.62 g·m −2 , which is lower than 30.22 g·m −2 of ceramic coated composite separator. Electrochemical characterizations indicate that the discharge capacity and capacity retention rate of the battery assembled with PP@PI microsphere composite separator are significantly higher than those assembled with the pure PP separator. The half-cell assembled with this composite separator shows a high capacity of 144.3 mAh·g −1 at 5C, which is much higher than the 117.8 mAh·g −1 of the commercial PP separator equipped battery. Moreover, the lithium-ion batteries assembled with the PP@PI microsphere composite separator show excellent cycle stability after 200 cycles at 1C. More importantly, the lithium-ion battery assembled with PP@PI microsphere composite separator has excellent safety at high temperature. These features demonstrate the potential of PP@PI microspheres composite membrane as high-security separator for LIBs.