PVDF Binder in All-Solid-State Lithium Batteries with NCM/Sulfide/PVDF Cathode, Oxide/PEO SE Layer, and Li-metal Anode

Sulfide-based solid electrolyte such as Li6PS5Cl (LPSCl) is unstable in contact with Li metal electrode due to decomposing to by-product resulting in poor performance. Therefore, the introduction of an interlayer to suppress reactivity is essential. In this study, instead of an interlayer, an oxide/polymer composite electrolyte was applied to suppress side reactions, while a sulfide-based electrolyte was used at the cathode to improve interfacial control between the cathode and the electrolyte. All-solid-state lithium batteries (ASLBs) were prepared by applying sulfide-based solid electrolyte (argyrodite, Li6PS5Cl) including NCM424, polyvinylidene fluoride (PVDF), and Super-P in a composite cathode layer, and a composite solid electrolyte (CSE) layer by mixing an oxide-based solid electrolyte (garnet, Al-doped Li7La3Zr2O12 (LLZO)), polymer (PEO, polyethylene oxide) and lithium metal as the anode. In this study, NCM424 powder was coated with LiNbO3 to prevent chemical reaction with the sulfide electrolyte. As the PVDF binder was applied to the cathode of the ASLB, the discharge capacity of the cell was approximately 163 mAh g−1 at 70 °C, 0.1 C, and 4.2 V cut-off and its capacity retention was 83% after 50 cycles. The effects of the PVDF were evaluated using both pouch-type cells. The capacity and cycle retention are greatly dependent on the PVDF content of the cathode materials and the drying temperature during the fabrication of the cathode. When the cathode with PVDF binder was dried at 130 °C, initial cycling was required for activation of the pouch cell, and it was possible to overcome this by adding a plasticizer. Highlights The composite cathode was prepared with LPSCl, NCM424, Super-P, and PVDF binder. The all-solid-state battery with the LPSCl composite cathode showed a discharge capacity of 163 mAh g−1 at 0.1 C. The cycling performance of the battery was improved by improving the properties of the active material particles.