Exploring optimal cathode composite design for high-performance all-solid-state batteries

Abstract

All-solid-state batteries (ASSBs) have attracted considerable attention due to their high stability, offering a safer alternative to currently used batteries. Extensive research has been conducted to improve cathode part performance. However, the conventional hand mixing (HM) process results in inhomogeneous particle distribution, causing poor interparticle contact due to uneven stress distribution, and the solution process causes unwanted solid electrolyte (SE) deterioration when using a polar solvent although it ensures uniform SE distribution. To overcome these limitations, based on the design rule considering SE surface coverage of less than 100 %, we propose a cathode/SE composite, showing decent ionic/electronic conductivities, uniform SE distribution, and intimate interparticle contact, achievable through a mass-producible mechanical mixing (MM) process. Unlike the HM cell, the MM cell forms well-defined ionic percolating pathways and shows excellent structural stability. Consequently, the MM cell exhibits improved capacity retention during 1000 cycles and stable cyclability even under the harsh condition of 7 wt% SE. Finite element analysis theoretically demonstrates that uniform electrode and electrolyte currents are responsible for the improved performances including increased cathode utilization efficiency and reduced overpotentials. This study reveals the importance of composite design and uniform SE distribution in developing high-performance ASSBs at a practical cell level.