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Roles of an Ag Interlayer in Stabilizing the Li Stripping Reactions at the Lithium/Lithium Phosphorus Oxynitride Interface
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DOI：10.1002/sstr.70555.png)
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Abstract
En 中文
Lithium metal is a promising anode material for high-energy-density all-solid-state batteries. However, Li stripping at the Li/solid electrolyte (SE) interface often generates voids, leading to nonuniform Li plating and eventual short-circuiting. Although interlayers have been introduced to stabilize Li plating–stripping reactions, the mechanism by which they suppress void formation remains unclear. In this study, thickness-controlled Li–Ag multilayers on lithium phosphorus oxynitride (LiPON) films are prepared, and their Li-stripping reactions are investigated using electrochemical measurements combined with phase-field calculations. The remaining Li–Ag intermetallic γ2 phase enables a stable Li-stripping reaction at thicknesses greater than 10 μm under 25°C and 0.9 MPa, without void formation. Retention of the γ2 phase on the LiPON film promotes rapid Li diffusion and drives long-range phase-boundary movement via coexistence with the Li–Ag solid-solution δ phase. Furthermore, the γ2 phase is kinetically stabilized against phase transitions to lower-Li-content phases, thereby suppressing delamination of the Li–Ag layer from LiPON films. These findings provide fundamental guidelines for designing interlayers that stabilize Li plating–stripping reactions in all-solid-state batteries.
Keywords:
all-solid-state batteries
alloy interlayer
interface modification
lithium metal anode
phase boundary movement
void
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