Ionically conducting, porous separator
membranes with submicrometer
size pores play an important role in governing the outcome of lithium-ion
batteries (LIBs) in terms of life, safety, and effective transport
of ions. Though the polyolefin membranes have dominated the commercial
segment for the past few decades, to develop next-generation batteries
with high-energy density, high capacity, and enhanced safety, there
is a need to develop advanced separators with superior thermal stability,
electrolyte interfacial capabilities, high melting temperature, and
mechanical stability at elevated temperatures. Here, aramid nanofiber
separators with enhanced mechanical and thermal stability dried at
the critical point are processed and tested for mechanical strength,
wettability, electrochemical performance, and thermal safety aspects
in LIBs. These separators outperform Celgard polypropylene in all
aspects such as delivering a high Young’s modulus of 6.9 ±
1.1 GPa, and ultimate tensile strength of 170 ± 25 MPa. At 40
and 25 °C, stable 200 and 300 cycles with 10% and 11% capacity
fade were obtained at 1 C rate, respectively. Multimode calorimetry,
specially designed to study thermal safety aspects of LIB coin cells,
demonstrates low exothermicity for critical-point-dried aramid nanofiber
separators, and post-diagnosis illustrates preservation of structural
integrity up to 300 °C, depicting possibilities of developing
advanced safer, high-performance LIBs.