A tailored concrete-like interface layer for guiding the growth of Li dendrites in all-solid-state batteries

Abstract

Abstract Solid-state electrolyte (SSE) is anticipated to exhibit proper mechanical strength and effectively inhibit the penetration of Li dendrites. However, in reality, the growth of Li dendrites is inevitable, which are driven by the intrinsic attributes of SSEs, such as grain boundaries, cracks, and pores. Hence, guiding the growth of Li dendrites in a controllable way is more feasible from a practical perspective than to aim for their complete prevention. Here we present a strategic design of concrete-like structure layer consisting of graded Li3N particle in different sizes (CLS-Li3N), which serves as guiding the growth of Li dendrites within restricted spaces. This CLS-Li3N layer is paired with a less Li-stable electrolyte (LZC or LGPS), enabling Li dendrites to be anchored within localized regions through a self-limiting mechanism akin to the expansion screw effect. The intentionally engineered CLS-Li3N|LZC electrolyte facilitates the dynamic stability for the SSEs/Li interface, enabling stable cycling in all-solid-state batteries featuring with Li metal anode and different cathodes. This concept of incorporating a concrete-like structure layer in electrolyte design holds broad applicability for regulating Li dendrites in all-solid-state Li-metal batteries.