Eco-Friendly Membrane Separators Based on Furanoate Polymers for Li-Ion Batteries

Conventional lithium-ion battery separators made from petroleum-based polymers pose environmental concerns due to their non-renewable origin and energy-intensive production. Novel bio-based alternatives, such as poly(alkylene 2,5-furanoate)s (PAFs), offer improved sustainability and favorable thermomechanical properties. This work investigated electrospun mats of poly(butylene 2,5-furandicarboxylate) (PBF) and poly(pentamethylene 2,5-furandicarboxylate) (PPeF), which, despite structural similarity, exhibit distinct behaviors. PBF mats demonstrated superior performance with fiber diameters of about 1.0 µm and porosity of 53.6% with high thermal stability (T_g = 25 °C, T_m = 170 °C, 18.8% crystallinity). The semicrystalline PBF showed higher electrolyte uptake (531-658 wt%) and had a lower MacMullin number (<i>N_M</i> = 3-10) than commercial Celgard separators (<i>N_M</i> = 15), indicating enhanced ionic conductivity. Electrochemical testing revealed stability up to 5 V and successful cycling performance with specific capacity of 135 mAh/g after 100 cycles and coulombic efficiency near 100%. In contrast, PPeF's amorphous nature (T_g = 14 °C) resulted in temperature-sensitive pore closure that enhanced safety by reducing short-circuit risk, although its solubility in carbonate electrolytes limited its application to aqueous systems. These findings highlight the potential of PAF-based separators to improve both the environmental impact and performance of batteries, supporting the development of safer and more sustainable energy storage systems.