Nano-micro letters · 2026
Hotspot to Homogeneous: Amorphous Interfacial Current Redistribution Enables Stable Solid-State Lithium-Metal Batteries.
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Yang Cuiyun, Lu Xupeng, Pan Yexin, Zhang Qimeng, Yu Ruohan, Yang Rongliang, Liu Huan, Duan Molong, Li Mitch Guijun, Zhu Ziyi, Yang Chenghao
Аннотация
Interfacial instability in oxide ceramic electrolyte (OCE)-based solid-state lithium metal batteries (SSLMBs) is conventionally attributed to chemical incompatibility or mechanical failure, yet the underlying atomic-scale mechanisms remain elusive. Here, we reveal that grain boundaries (GBs) in polycrystalline OCEs function as bipolar interfacial hotspots, accelerating three degradation pathways: lowering barriers for Li dendrite nucleation and enabling electron-leakage-driven reduction at anode side, while generating localized overpotentials for cathode phase transformation. To deactivate these GB-driven hotspots, we develop a laser-induced amorphization strategy that constructs a GB-free amorphous interlayer capable of homogenizing Li+ flux and blocking electron migration. Applied to a representative sodium superionic conductor-type electrolyte, Li1.3Al0.3Ti1.7(PO4)3, this approach delivers substantially increased critical current density in Li symmetric cells (1.4 to 2.4 mA cm-2) with stable cycling over 2000 h, and achieves an exceptional capacity retention of 101.9 mAh g-1 after 800 cycles in LiCoO2 full cells operated at 4.5 V. The generality of this strategy is further validated on garnet-type and perovskite-type OCEs. This work introduces amorphous interfacial current redistribution as a universal paradigm for engineering stable interfaces, providing a critical atomic-scale interface engineering route to unlock high-voltage, dendrite-free SSLMBs.