Abstract

While lithium-ion batteries have garnered significant success over the past decades, the development of next-generation batteries with higher energy densities is crucial for future electromobility demands such as long-range electric vehicles and electric aviation. In this context, solid-state batteries (SSBs), consisting of an inorganic solid electrolyte and lithium metal, are promising in simultaneously improving the energy density and safety. Despite their irrefutable promise, the realization of practical SSBs is predicated on overcoming important challenges pertaining to electro-chemo-mechanics, transport, and interface evolution. Myriad heterogeneities ranging from defects/voids at the lithium/solid electrolyte interface, grain boundaries in the solid electrolyte and singularities in the solid-state cathode have a pivotal influence on the onset of failure and electrochemical performance. In this presentation, the critical role of heterogeneities on the mechanistic interplay at solid-solid interfaces and the underlying failure mechanisms will be delineated. Governed by the manifestation of spatio-temporal heterogeneity at scales, the origin of solid/solid interface instability, resultant asymmetry in the plating/stripping response and electrode crosstalk implications will be discussed.

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