A zeolite/polyimide composite separator with a spongy-like structure was prepared by phase inversion methods based on heat-resistant polyimide (PI) polymer matrix and ZSM-5 zeolite filler, with the aim to improve the thermal stability and electrochemical properties of corresponding batteries. The separator exhibits enhanced thermal stability and no shrinkage up to 180 °C. The introduction of a certain number of ZSM-5 zeolites endows the composite separator with enhanced wettability and electrolyte uptake, better facilitating the free transport of lithium-ion. Furthermore, the composite separator shows a high ionic conductivity of 1.04 mS cm−1 at 25 °C, and a high decomposition potential of 4.7 V. Compared with the PP separator and pristine PI separator, the ZSM-5/PI composite separator based LiFePO4/Li cells have better rate capability (133 mAh g−1 at 2 C) and cycle performance (145 mAh g-1 at 0.5 C after 50 cycles). These results demonstrate that the ZSM-5/PI composite separator is promising for high-performance and high-safety lithium-ion batteries.
Commercial separators (polyolefin separators) for lithium-ion batteries still have defects such as low thermostability and inferior interface compatibility, which result in serious potential safety distress and poor electrochemical performance. Zeolite/Polyacrylonitrile (Z/PAN) composite separators have been fabricated by electrospinning a polyacrylonitrile (PAN) membrane and then dip-coating it with zeolite (ZSM-5). Different from commercial separators, the Z/PAN composite separators exhibit high electrolyte uptake, excellent ionic conductivity, and prominent thermal stability. Specifically, the Z/PAN-1.5 separator exhibits the best performance, with a high electrolyte uptake of 308.1% and an excellent ionic conductivity of 2.158 mS·cm−1. The Z/PAN-1.5 separator may mechanically shrink less than 10% when held at 180 °C for 30 min, proving good thermal stability. Compared with the pristine PAN separator, the Li/separator/LiFePO4 cells with the Z/PAN-1.5 composite separator have excellent high-rate discharge capacity (102.2 mAh·g−1 at 7 C) and favorable cycling performance (144.9 mAh·g−1 at 0.5 C after 100 cycles). Obviously, the Z/PAN-1.5 separator holds great promise in furthering the safety and performance of lithium-ion batteries.
The traditional commercial polyolefin separators suffer from high-temperature thermal shrinkage, low electrolyte wettability and other issues. In order to improve the overall performance of the separators, electrostatic spinning technology was applied to obtain PAN nanofiber separators with an average diameter of 320 nm. Then cellulose acetate (CA) resin and nano-hydroxyapatite (HAP) were introduced to fabricate the PAN/CA/HAP composite separators through the constant temperature hot pressing and dip-coating crafts. The composite separator has a good thermal stability, with no significant dimensional change after a constant temperature treatment of 200 °C for 35 min. The electrolyte uptake rate of the PAN/CA/HAP-1.0 composite separator reaches 281%, which exhibits an efficient ionic conductivity. At the same time, it also attains a tensile strength of 11.18 MPa, which meets the requirement for separator use. Button cells assembled from PAN/CA/HAP-1.0 composite separators have an excellent rate of performance (160.42 mAh·g−1 at 0.2 C) and cycle capability (157.6 mAh·g−1 after 50 cycles at 0.5 C). The results support that lithium-ion batteries assembled with PAN/CA/HAP-1.0 composite separators will exhibit higher safety stability and better electrochemical performance than that of polyolefin separators, with a very immense potential for application.