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Solid-state lithium metal batteries (SSLMBs) based on garnet-type Li6.5La3Zr1.5Ta0.5O12 (LLZTO) electrolytes have faced significant challenges due to surface Li2CO3 contamination, which leads to increased interfacial resistance and degraded electrochemical performance. Herein, we report a simple and cost-effective interfacial modification strategy via an AlCl3 aqueous solution to address these issues. By using the drop-casting method, this strategy effectively removes the Li2CO3 layers while maintaining the structural integrity of the garnet lattice. During the subsequent lithium melting process, the in situ-formed Li–Al alloy enhances lithiophilicity and Li+ diffusion kinetics, reducing the Li–LLZTO interfacial resistance from 38.80 to 13.23 Ω·cm2. The symmetric cell achieves a critical current density (CCD) of 1.1 mA cm–2 (compared with 0.3 mA cm–2 for the untreated cell) and demonstrates stable cycling for over 2000 h at 0.2 mA cm–2. The full cell paired with LiFePO4 (LFP) cathodes exhibits a discharge capacity of 130.5 mAh g–1 at 1.0C and retains 93.3% capacity after 100 cycles at 0.1C, with Coulombic efficiencies exceeding 99%. This work provides a feasible strategy for constructing garnet-based solid-state Li metal batteries.
Zhang et al. (Mon,) studied this question.