Construction of a Multifunctional Separator Based on Poly(terephthaloyl-melamine) for the Thermally Safe Regulation of Lithium-Ion Batteries.

The poor thermal stability of commercial polyethylene (PE) separators hinders the further application of lithium-ion batteries (LIBs), yet previous modifications struggle to balance between safety and electrochemical performance. This study proposes an interface modification strategy by forming a poly(melamine terephthalamide) (PTM) coating on the PE separator surface, constructing a "thermal-mechanical-electrochemical synergistic barrier". The PTMs@PE separator achieves synergistic improvements in thermal shutdown behavior, thermal stability, mechanical strength, and electrochemical compatibility by taking advantage of the temperature-sensitive response of the PE separator, the flame-retardants of the rigid conjugated skeleton with the high nitrogen of PTM, and the electrolyte-affinity of its functional groups. Importantly, the principles between the molecular structure of the PTM coating and the thermal behavior is verified. The results demonstrate that PTM participates in the decomposition process of the PE separator and slows down the degradation rate of the PE chain structure, thereby resulting in a wide-temperature-range thermal shutdown temperature. The PTMs@PE effectively reduces the risk of runaway. The PTMs@PE separator achieves outstanding electrochemical compatibility, achieving a capacity retention rate of 99.27% at 2 C for 500 cycles. Notably, the separator shows high potential for scalable fabrication. This work provides a novel material system and technical pathway for developing highly safe and high-performance LIB separators.