Dynamic control of lithium dendrite growth with sequential guiding and limiting in all-solid-state batteries.

Solid-state electrolyte (SSE) is anticipated to exhibit proper mechanical strength and effectively inhibit the penetration of lithium dendrites. However, the growth of lithium dendrites is inevitable, driven by the intrinsic properties of SSEs. Hence, guiding the growth of lithium dendrites in a controllable way is more feasible instead of completely preventing their growth. Here, we present a strategically designed structural layer composed of graded lithium nitride particles, which guides the growth of lithium dendrites within confined spaces. Meanwhile, this layer is paired with a less lithium-stable electrolyte and enables the guided lithium dendrites to self-limit within localized regions at the interface. The comprehensive analysis further reveals that the designed bilayer SSE effectively harnesses the interface-generated pressure during battery cycling, achieving dynamic control of lithium dendrite growth. This interfacial structure design of SSE holds broad applicability for regulating lithium dendrites in all-solid-state lithium-metal batteries.