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Visualizing the morphological and compositional evolution of the interface of InLi-anode|thio-LISION electrolyte in an all-solid-state Li–S cell by in operando synchrotron X-ray tomography and energy dispersive diffraction

Sun, Fu; Dong, Kang; Osenberg, Markus; Hilger, André; Risse, Sebastian; Lu, Yan; Kamm, Paul H.; Klaus, Manuela; Markötter, Henning; García-Moreno, Francisco; Arlt, Tobias; Manke, Ingo

Dynamic and direct visualization of interfacial evolution is helpful in gaining fundamental knowledge of all-solid-state-lithium battery working/degradation mechanisms and clarifying future research directions for constructing next-generation batteries. Herein, in situ and in operando synchrotron X-ray tomography and energy dispersive diffraction were simultaneously employed to record the morphological and compositional evolution of the interface of InLi-anode|sulfide-solid-electrolyte during battery cycling. Compelling morphological evidence of interfacial degradation during all-solid-state-lithium battery operation has been directly visualized by tomographic measurement. The accompanying energy dispersive diffraction results agree well with the observed morphological deterioration and the recorded electrochemical performance. It is concluded from the current investigation that a fundamental understanding of the phenomena occurring at the solid–solid electrode|electrolyte interface during all-solid-state-lithium battery cycling is critical for future progress in cell performance improvement and may determine its final commercial viability.
Published in: Journal of Materials Chemistry A: Materials for Energy and Sustainability, 10.1039/C8TA08821G, Royal Society of Chemistry