Diffraction-Enabled Operando Nanoscale Tracking of Li-ion Dynamics of Solid Electrolyte and Inhomogeneous Diffusion in Composite Cathode, Angewandte Chemie International Edition, 65, e20281(2026)
Po-Jui Chu, Jheng-Yi Huang, Yu-Shuo Liu, Yun-Ping Chang, Yuan-Ting Hung, Ching-Yu Chiang, Yu-Cheng Shao, Wan-Zhen Hsieh, Hirofumi Ishii, and Ru-Shi Liu*
2026/05/07
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.
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