Monday, 10 October 2022: 10:40
Galleria 4 (The Hilton Atlanta)
All-solid-state batteries (ASSBs) offer a fundamental solution to mitigate the safety and reliability issues of conventional lithium-ion batteries utilizing flammable liquid electrolytes. However, interfacial resistances between the cathode materials and solid electrolytes, which originate from poor solid-solid contacts and detrimental interfacial reactions, limit the electrochemical performances of ASSBs. Recently, various approaches have been developed to realize high-capacity composite cathodes with improved cycling stability. For example, single-crystal LiNi0.8Co0.1Mn0.1O2 (NCM811) has been reported to mitigate the capacity fading resulting from cracking of commonly adopted multi-crystal NCM811. Also, halide-type solid electrolytes are reported to exhibit high Li-ion conductivity and electrochemical stability with NCM. In this work, we systematically study the interfacial and charge-transport impedances of NCM composite cathodes with halide solid electrolytes. The composite cathodes comprising single- or multi-crystal NCM811 and Li6PS5Cl or Li3InCl6 (and conductive agents) are fabricated to characterize their electrochemical impedance behaviors. In particular, we analyze the evolution of the interfacial and charge-transport impedances during charge–discharge cycling based on a multi-rail transmission line model combined with interfacial reactions. In addition, we investigate the chemical, electrochemical, and mechanical degradations of composite cathodes using various analytical tools to elucidate performance-determining factors of ASSBs.