A Polyvinylidene Fluoride‐Hexafluoropropylene (PVDF‐HFP)/Carboxylated g‐C3N4 Composite Separator for High‐Performance Lithium‐Ion Batteries

Abstract Polyvinylidene fluoride‐hexafluoropropylene (PVDF‐HFP) is a standard electrolyte membrane and binder material for lithium‐ion batteries (LIBs) because of the benefits of membrane formation and strong mechanical properties. Still, its use is limited due to unavoidable defects such as high crystallinity and poor electrochemical performance. In this paper, a larger specific surface area and three‐dimensional (3D) permeable lamellae carboxylated g‐C 3 N 4 (HCN) were successfully prepared by HNO 3 and introduced into the PVDF‐HFP to obtain a high‐performance composite separator. The wettability and electrolyte absorption of PVDF‐HFP separator can be improved through the carboxylated HCN. More crucially, because PVDF‐HFP has several active sites and low crystallinity, adding HCN can greatly increase the ionic conductivity of separators. The ionic conductivity of PH‐HCN at 25 °C is 0.52 S cm −1 , 4.7 times higher than the initial PVDF‐HFP membrane, and the oxidation potential can reach 4.8 V. The assembled lithium‐ion batteries half‐cell has a capacity of 71 % at a 5 C rate and 94 % after 400 cycles at a 2 C rate. Therefore, the improved separator has the potential to be applied to high‐performance LIBs.