A Morphologically Stable Li/Electrolyte Interface for All-Solid-State Batteries Enabled by 3D-Micropatterned Garnet

Adv Mater. 2021 Dec;33(49):e2104009. doi: 10.1002/adma.202104009. Epub 2021 Oct 10.

Abstract

Morphological degradation at the Li/solid-state electrolyte (SSE) interface is a prevalent issue causing performance fading of all-solid-state batteries (ASSBs). To maintain the interfacial integrity, most ASSBs are operated under low current density with considerable stack pressure, which significantly limits their widespread usage. Herein, a novel 3D-micropatterned SSE (3D-SSE) that can stabilize the morphology of the Li/SSE interface even under relatively high current density and limited stack pressure is reported. Under the pressure of 1.0 MPa, the Li symmetric cell using a garnet-type 3D-SSE fabricated by laser machining shows a high critical current density of 0.7 mA cm-2 and stable cycling over 500 h under 0.5 mA cm-2 . This excellent performance is attributed to the reduced local current density and amplified mechanical stress at the Li/3D-SSE interface. These two effects can benefit the flux balance between Li stripping and creep at the interface, thereby preventing interfacial degradation such as void formation and dendrite growth.

Keywords: 3D-micropatterned garnet; all-solid-state batteries; electrochemomechanics; interfacial degradation; solid-state electrolytes; void formation.