Polyvinylidene fluoride gel‐polyethylene composite separator optimizing the interface compatibility between the separator and the electrode

Abstract The interface issue concerning lithium dendrite formation between the separator and electrode remains a significant impediment to the further advancement of lithium‐ion batteries (LIB). Due to the inadequate interface compatibility between the conventional polyolefin separator and the electrode, there is a propensity for lithium dendrite growth. In this work, the surface of the polyethylene (PE) separator is coated with polyvinylidene fluoride (PVDF) gel using a simple phase transformation method, resulting in the preparation of a composite separator consisting of PE and PVDF. The results demonstrate an enhanced interface compatibility following the introduction of the gel layer, with a polarization voltage as low as 0.14 V observed after 250 h of cycling. Additionally, the ionic conductivity of the PE/PVDF composite separator (1.77 mS cm −1 ) is enhanced, attributed to the incorporation of F functional group in PVDF gel, which could facilitate the formation of a rapid ion transport pathway through the interaction between F functional group and Li + . After the introduction of the gel layer, the discharge capacity of the battery after 250 cycles measures ~1.28 mAh, with a mere 27% decay in capacity. This study presents a novel concept for the design of composite separator in LIB.