Aging Phenomena in TiS4- and VS4-based All-Solid-State Lithium Sulfide Batteries Analyzed by ToF-SIMS

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Abstract Nowadays, lithium ion batteries (LIBs) are dominating the rechargeable energy storage market. However, lithium/sulfur batteries (LSBs) offer higher energy densities with sulfur's economic and ecologic advantages, but exhibit poor cyclability, capacity utilization and lifetime. The utilization of metal sulfide active materials and solid-state electrolytes (SSE) show promise to alleviate these issues but coming with their own challenges such as material integrity. This study is focused on analyzing these aging effects by utilizing high lateral and mass resolution time-of-flight-secondary ion-mass spectrometry (ToF-SIMS) imaging of focused ion beam (FIB) cross sections. By measuring the pristine components, the identification of newly formed species as well as the individual particles in a composite was enabled. This work shows among others the formation of a carbon-electrolyte interphase, the accumulation of sodium, the degradation of the metal polysulfide and the decomposition of the SSE. By revealing different aging mechanisms, this research takes part in paving the way for long-lasting, energy dense, and safe SSE LSBs as a more environmentally friendly alternative to conventional commercial LIBs.

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