Abstract

Commercial polyolefin separators suffer from poor electrolyte wettability and low thermal stability, which give rise to unsatisfied electrochemical performance and severe safety hazards for lithium-ion batteries (LIBs). Herein, a novel paper-based composite separator composed of electrolyte-affinitive cellulose fibers (CFs) and thermally stable aramid nanofibers (ANFs) was successfully fabricated through the traditional papermaking method. The ANFs as a functional nanofiller played crucial roles in improving the defects of pure CF separator including large-sized pores, low mechanical strength and high flammability. Specifically, the CF/ANF composite separator with 20 wt% ANFs (CF/ANF-20) possessed narrow micropores, satisfied tensile strength (33 MPa), excellent thermal resistance (without dimensional shrinkage up to 200 °C) and flame retardancy, which greatly enhanced the safe operation of battery. Moreover, inheriting from the highly porous structure and exceptional electrolyte affinity of CF separator, the CF/ANF-20 composite separator exhibited appropriate porosity and superior electrolyte wettability, which brought about a high electrolyte uptake (157%), thus endowing it with better ionic conductivity (0.75 mS cm−1) and lower interfacial resistance compared to commercial polypropylene separator. Accordingly, the LiFePO4/Li half cells using CF/ANF-20 separator delivered outstanding rate capability and stable cycling performance. All results indicate that the CF/ANF-20 separator shown great balance between the electrochemical performance and safety is an intriguing candidate for advanced LIBs.

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