In-situ measurements of stress evolution in composite sulfur cathodes
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2018 Elsevier B.V. Owing to their enormous capacities, Li-S batteries have emerged as a prime candidate for economic and sustainable energy storage. Still, potential mechanics-based issues exist that must be addressed: lithiation of sulfur produces an enormous volume expansion (~ 80%). In other high capacity electrodes, large expansions generate considerable stresses that can lead to mechanical damage and capacity fading. However, the mechanics of electrochemical cycling of sulfur is fundamentally distinct from other systems due to solid-to-liquid, liquid-to-liquid, and liquid-to-solid phase transformations, and thus remains poorly understood. To this end, we measure the evolution of stresses in composite sulfur cathodes during electrochemical cycling and link these stresses to structural evolution. We observe that nucleation and growth of solid lithium-sulfur phases induces significant stresses, including irreversible stresses from structural rearrangements during the first cycle. However, subsequent cycles show highly reversible elastic mechanics, thereby demonstrating strong potential for extended cycling in practical applications.
