Diffraction‐Enabled Operando Nanoscale Tracking of Li‐ion Dynamics of Solid Electrolyte and Inhomogeneous Diffusion in Composite Cathode
Journal
Angewandte Chemie International Edition
ISSN
1433-7851
1521-3773
Date Issued
2026-01-20
Author(s)
Chu, Po‐Jui
Huang, Jheng‐Yi
Liu, Yu‐Shuo
Chang, Yun‐Ping
Hung, Yuan‐Ting
Chiang, Ching‐Yu
Shao, Yu‐Cheng
Hsieh, Wan‐Zhen
Ishii, Hirofumi
Abstract
Li+ diffusion has mostly been studied in cathode active materials (CAMs) in liquid batteries, whereas it remains rarely explored in solid-state electrolytes (SSEs) and all-solid-state batteries. Herein, diffraction was established as an effective method for all-solid-state lithium batteries (ASSLBs) by focusing on SSE in composite cathodes. Operando synchrotron x-ray diffraction presented diffraction angle shifts of certain Li3InCl6 Bragg planes during the first ASSLB cycle due to lithiation/delithiation into its lattice, whose preferred Li+ migration pathways were suggested by the partiality of these shifts, and the three-phase evolution indicated the fundamental Li+ diffusion kinetics factors. X-ray nanodiffraction (XND) mapped nanoscale inhomogeneous Li+ distributions and diffusion within individual Li3InCl6 particles, revealing facilitated Li+ conduction in high-crystallinity regions and their role as pathways across SSE/CAM interfaces, and the most negatively strained regions were shown to be less susceptible to Li+ insertion. XND from various electrochemical techniques inferred high transient charging rates to be the culprit of irreversible Li+ diffusion instead of the overall charging depth. This study proved diffraction to be a potent tool to probe intricate Li+ dynamics in ASSLBs and provide microscopic insights for optimal battery designs.
Subjects
All-Solid-State battery
Composite cathode
Li-ion diffusion
Operando diffraction
Publisher
Wiley
Type
journal article