Operando Transmission Electron Microscopy Study of All-Solid-State Battery Interface

Redistribution of Lithium among Interconnected Particles

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Abstract

With operando transmission electron microscopy visualizing the solid-solid electrode-electrolyte interface of silicon active particles and lithium oxide solid electrolyte as a model system, we show that (de)lithiation (battery cycling) does not require all particles to be in direct contact with electrolytes across length scales of a few hundred nanometers. A facile lithium redistribution that occurs between interconnected active particles indicates that lithium does not necessarily become isolated in individual particles due to loss of a direct contact. Our results have implications for the design of all-solid-state battery electrodes with improved capacity retention and cyclability. ©