Advanced electrochemical and diagnostic analysis tools for sulfide-based all-solid-state lithium batteries

초록

All-solid-state batteries (ASSBs) are among the most promising next-generation energy storage systems due to their high energy density and improved safety. Sulfide-based solid-state electrolytes have garnered significant attention owing to their high ionic conductivity and excellent processability, but intrinsic limitations, including interfacial reactivity, poor atmospheric stability, and structural degradation, still hinder commercialization. This review systematically summarizes advanced characterization techniques for probing material properties, understanding electrochemical processes, and elucidating degradation behaviors in sulfide-based ASSBs. Spectroscopic analyses (XPS, XAS, Raman, and NMR), electron microscopy (SEM, TEM, and EELS), imaging techniques (X-ray CT, AFM, and STM), mass spectrometry (SIMS, DEMS, and TG-MS), and electrochemical analyses (EIS and TLM) are introduced, with an emphasis on their ability to probe interfacial chemistry, structural evolution, gas generation, and resistive components. Rather than simply cataloging individual characterization methods, this review establishes a degradation-oriented diagnostic perspective that connects specific analytical tools with cathode-side reactions, anode-side interfacial instability, chemo-mechanical failure, gas evolution, and microstructure-dependent resistance growth. The combination of advanced analysis techniques provides multidimensional insights into ASSB degradation and guidelines for improving performance. By outlining the scope, strengths, limitations, and complementary roles of these techniques, this review aims to guide the selection of effective diagnostic strategies to design durable sulfide-based ASSBs. Highlights •Framework for diagnosing degradation in sulfide all-solid-state batteries•Multimodal tools link chemistry, microstructure, and electrochemistry•Compares spectroscopy, microscopy, and electrochemical diagnostics•Identifies key degradation mechanisms in sulfide-based ASSBs

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