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Understanding Electrochemical Reaction Mechanisms of Sulfur in All-Solid-State Batteries through Operando and Theoretical Studies. | LitMetric

AI Article Synopsis

  • All-solid-state lithium-sulfur batteries (ASLSBs) are promising for future energy storage because they're safe and have high energy density, but their reaction mechanisms are not fully understood.
  • The study used advanced techniques like operando Raman spectroscopy and X-ray absorption spectroscopy to analyze sulfur's behavior in ASLSBs, revealing the presence of Li2S while no Li2S or Li2S were formed.
  • The research found that at full lithiation, incomplete reactions occur due to slow kinetics, with certain sulfur and Li2S phases remaining, indicating that Li2S is a metastable phase in the solid state.

Article Abstract

Due to its outstanding safety and high energy density, all-solid-state lithium-sulfur batteries (ASLSBs) are considered as a potential future energy storage technology. The electrochemical reaction pathway in ASLSBs with inorganic solid-state electrolytes is different from Li-S batteries with liquid electrolytes, but the mechanism remains unclear. By combining operando Raman spectroscopy and ex situ X-ray absorption spectroscopy, we investigated the reaction mechanism of sulfur (S ) in ASLSBs. Our results revealed that no Li S Li S and Li S were formed, yet Li S was detected. Furthermore, first-principles structural calculations were employed to disclose the formation energy of solid state Li S (1≤n≤8), in which Li S was a metastable phase, consistent with experimental observations. Meanwhile, partial S and Li S remained at the full lithiation stage, suggesting incomplete reaction due to sluggish reaction kinetics in ASLSBs.

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Source
http://dx.doi.org/10.1002/anie.202302363DOI Listing

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