Combined diffuse and sharp interface approach to unravel morphological dynamics in solid-state Li-ion batteries

Addressing the limitations of traditional Li-ion batteries, this study focuses on the crucial transition to All-Solid- State Batteries (ASSBs) by emphasizing the paramount importance of solid electrolyte morphology on battery performance. Utilizing a computational phase-field approach, the study simulates binary solid-electrolyte morphologies and integrates them into ASSBs through a robust process to assess their impact on electrochemical characteristics. The intricate process of transitioning from simulated morphology to Computer-Aided Design geometry is thoroughly explored in the manuscript. Furthermore, upon the successful incorporation of solid- electrolyte morphology, simulations are performed at a constant discharge current density of 5 A.m-2, revealing a significant order of magnitude difference in the discharging times for ASSBs with varying volume fractions, underscoring the pivotal role of solid-electrolyte's morphology. Additionally, mechanical strength is evaluated across volume fractions ranging from 0.3 to 0.7, showcasing a substantial threefold enhancement under a compressive stress of 10 MPa. Guided by mechano-electrochemical characteristics, an optimal blend ratio for the solid-electrolyte is identified. These findings underscore the crucial role of tailoring solid-electrolyte morphology for optimal ASSB performance, providing valuable guidance for advancing high-performance, safe, and sustainable battery technologies.