Porous, robust, thermally stable, and flame retardant nanocellulose/polyimide separators for safe lithium-ion batteries

Abstract

The safety of lithium-ion batteries (LIBs) is paramount for all users. One effective way to improve safety is incorporating heat-resistant polyimide (PI) separators, which can increase the thermal stability of batteries and minimize the risk of thermal runaway. However, preparing PI separators with both an ideal pore structure and adequate mechanical properties remains as a challenge. Here, we introduced decabromodiphenyl ethane (DBDPE) and cellulose nanofibers (CNFs) into PI and produced a hybrid separator with an outstanding pore structure and excellent mechanical properties. Aided with DBDPE, the separators attain a well-defined and uniform pore size (20 nm), while demonstrating high porosities (78%) through phase inversion processes. Owing to the addition of CNFs, the mechanical properties of the separators were significantly improved, with a tensile strength of 25.4 MPa and an elastic modulus of 550.1 MPa. Moreover, the separators demonstrate high ion conductivity (0.45 mS cm⁻¹), excellent thermal-dimensional stability (up to 200 °C), remarkable flame retardancy, and outstanding electrolyte wettability. At room temperature, the batteries with the separators demonstrate comparable performance with those of polypropylene (PP) separators. However, when subjected to thermal shock treatments, the batteries with the separators outperform those with PP, showcasing their superior performance. The work introduces a novel strategy for designing high-performance separators, thereby paving the way for advancements in the fabrication of LIBs with enhanced safety features.