Polybenzimidazole Composite Separators Engineered from MOFs‐HNTs Composites Applicated in Lithium‐Ion Batteries
Qian Zhou, Shabab Hussain, Jisong Hu, Guanghao Zhang, Wenxing Zhang, Bin Zhang, Lei Wang
Abstract
Abstract Incorporating inorganic nanostructured materials into polymeric separators for lithium‐ion batteries (LIBs) enhances properties such as ionic conductivity, electrolyte wettability, and thermal resistance. However, poor interfacial compatibility between inorganic materials and the polymeric matrix remains a significant challenge. In this study, Zr‐based UiO‐66 metal‐organic frameworks (MOFs) is employed as an interfacial binder between halloysite nanotubes (HNTs) and a poly‐(arylene ether benzimidazole) (OPBI) matrix, preparing porous separators using the non‐solvent phase separation (NIPS) method. The UiO‐66 MOFs promote strong adhesion of HNTs to the OPBI chains, creating a more cohesive inorganic‐organic system, as confirmed by molecular dynamics (MD) simulations of binding energy. The resulting OPBI@M‐H10 composite separator exhibits high porosity (80%), an electrolyte absorption capacity of 377%, and an ionic conductivity of 1.59 mS·cm⁻¹. Furthermore, LiFePO 4 half‐cells assembled with this composite separator show a discharge capacity of 161 mAh·g⁻¹ and a retention rate of 97.96% after 200 charge‐discharge cycles. The separator also demonstrates excellent electrode stability in the plating/stripping test of Li symmetric cells, lasting up to 1600 hours and effectively inhibiting dendrite growth on the Li anode. This approach provides a promising solution for high‐performance LIBs separators and paves the way for advancements in LIBs technology and energy storage applications.