Graded Cathode Design for Enhanced Performance of Sulfide-Based Solid-State Batteries

Abstract

Solid-state batteries present a promising technology to overcome the energy density limitations of lithium-ion batteries. However, achieving a high areal loading in cathodes without introducing significant transport limitations remains a key challenge, particularly in thick electrodes. In this work, we study the impact of a three-layer graded cathode design on the performance of a LiNi_0.83Co_0.11Mn_0.06O₂ (NCM83)/Li₆PS₅Cl (LPSCl) composite cathode using a combination of experiments and microstructure-resolved simulations. An increased LPSCl content at the separator and higher NCM83 content toward the current collector improve effective charge transport, resulting in better rate performance and reduced overpotentials at high current densities. This comprehensive experimental and theoretical study demonstrates that the optimization of cathode design has the potential to significantly enhance the performance of solid-state batteries.