Publication date: 21st July 2025
The development of sulfide-based lithium superionic conductors (>10−4 S cm−1) has addressed the challenge of low ionic conductivity in the solid state, spurring the development of all-solid-state batteries (ASSB) over the past decade [1]. Despite the suitable ionic conductivity of sulfide-based materials, they can be challenging to handle due to interfacial instability against active materials (electrodes and conductive binder) within the cell. The limited electrochemical window of sulfide solid electrolytes (of ca. 2–3 V vs. Li/Li+) can trigger chemical and electrochemical decomposition within the cell that leads to limited cell life. Herein Raman microscopy is demonstrated as a powerful analytical tool to monitor interfacial changes (both ex situ and operando) on electrodes containing a variety of solid electrolytes (β-Li3PS4, Li6PS5Cl, Li7Si2S7I and Li10GeP2S12) [2-4]. Furthermore, Raman microscopy was used to map the distribution of degradation products with the composite electrode, before and after cycling and highlighted degradation at sulfide electrolyte/conductive carbon/binder interface.
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