Lithium-ion batteries (LIBs) have an extremely diverse application nowadays as an environmentally friendly and renewable new energy storage technology. The porous structure of the separator, one essential component of LIBs, provides an ion transport channel for the migration of ions and directly affects the overall performance of the battery. In this work, we fabricated a composite separator (GOP-PH-ATP) via simply laminating an electrospun polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) nanofibrous membrane coated with attapulgite (ATP) nanoparticles onto a PP nonwoven microfibrous fabric, which exhibits a unique porous structure with a pore-size gradient along the thickness direction that ranges from tens of microns to hundreds of nanometers. As a result, besides the enhanced thermal stability given by the chosen materials, the GOP-PH-ATP separator was endowed with a superhigh porosity of ~95%, strong affinity with electrolyte, and great electrolyte uptake of ~760%, thus effectively enabling an ionic conductivity of 2.38 mS cm−1 and a lithium-ion transference number of 0.62. Furthermore, the cell with the GOP-PH-ATP separator shows an excellent cycling performance with a capacity retention of 91.2% after 150 cycles at 1 C, suggesting that the composite separator with a pore-size gradient structure has great potential to be applied in LIBs.
