Deciphering the influence of multi-component blends and their electronic band structure on the performance of All-Solid-State Batteries

Abstract

The emergence of all-solid-state batteries (ASSBs) introduces a paradigm shift in energy storage technology, offering enhanced safety compared to conventional liquid-based metal-ion batteries. Significant effort is directed toward optimizing the solid-electrolyte blend composition to enhance the battery’s electrochemical performance. Despite some promising results, a lack of guidelines persists, particularly for optimizing multicomponent solid electrolytes given their large parameter window. This study aims to address this challenge by implementing a unified diffuse-interface approach to model and simulate the solid electrolyte morphologies and their corresponding electrochemical performance when incorporated in a battery. The electrolyte microstructures are simulated using the Cahn-Hilliard formulation while a diffuse-interface framework formulated in terms of electrochemical potential is utilized for exploring Li-ion transport across the battery. It is found that, while the variegated microstructures arising from various solid electrolyte blend compositions influence the power density of the battery, the electronic band structure of the blend phases is an important consideration. The proposed model is versatile and can be adapted for various battery technologies beyond ASSBs. This expands its potential impact and could lead to innovations in energy storage technology.