Single-step wet-chemical fabrication of sheet-type electrodes from solid-electrolyte precursors for all-solid-state lithium-ion batteries

All-solid-state lithium-ion batteries (ASLBs) employing sulfide solid electrolytes (SEs) have emerged as promising next-generation batteries for large-scale energy storage applications in terms of safety and high energy density. While slurry-based fabrication processes using polymeric binders and solvents are inevitable to produce sheet-type electrodes, these processes for ASLBs have been overlooked until now. In this work, we report the first scalable single-step fabrication of bendable sheet-type composite electrodes for ASLBs using a one-pot slurry prepared from SE precursors (Li 2 S and P 2 S 5 ), active materials (LiNi 0.6 Co 0.2 Mn 0.2 O 2 or graphite), and polymeric binders (nitrile-butadiene rubber (NBR) or polyvinyl chloride (PVC)) via a wet-chemical route using tetrahydrofuran. At 30 °C, the LiNi 0.6 Co 0.2 Mn 0.2 O 2 and graphite electrodes wet-tailored from SE precursors and NBR exhibit high capacities of 140 mA h g −1 at 0.1C and 320 mA h g −1 at 0.2C, respectively. Particularly, the rate capability of the graphite electrode in an all-solid-state cell is superior to that of a liquid electrolyte-based cell. Additionally, the effects of the size of the SE precursors and the polymeric binders on the electrochemical performance are investigated. Finally, the excellent electrochemical performance of LiNi 0.6 Co 0.2 Mn 0.2 O 2 /graphite ASLBs assembled using the as-single-step-fabricated electrodes are also demonstrated not only at 30 °C but also at 100 °C.