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All‐solid‐state lithium batteries (ASSBs) have the potential to trigger a battery revolution for electric vehicles due to their advantages in safety and energy density. Screening of various possible solid electrolytes for ASSBs has revealed that garnet electrolytes are promising due to their high ionic conductivity and superior (electro)chemical stabilities. However, a major challenge of garnet electrolytes is poor contact with Li‐metal anodes, resulting in an extremely large interfacial impedance and severe Li dendrite propagation. Herein, an innovative surface tension modification method is proposed to create an intimate Li | garnet interface by tuning molten Li with a trace amount of Si3N4 (1 wt%). The resultant Li‐Si‐N melt can not only convert the Li | garnet interface from point‐to‐point contact to consecutive face‐to‐face contact but also homogenize the electric‐field distribution during the Li stripping/depositing process, thereby significantly decreasing its interfacial impedance (1 Ω cm2 at 25 °C) and improving its cycle stability (1000 h at 0.4 mA cm−2) and critical current density (1.8 mA cm−2). Specifically, the all‐solid‐state full cell paired with a LiFePO4 cathode delivered a high capacity of 145 mAh g−1 at 2 C and maintained 97% of the initial capacity after 100 cycles at 1 C. [ABSTRACT FROM AUTHOR]

Rapid development of electronic and grid storage technologies based on lithium-ion batteries are leading to tight supply of lithium resources in the future. Extracting lithium from seawater can completely solve the problem of lithium resource shortage. An electro-deposition method based on a lithium superionic conductive solid-state electrolyte, Li1.5Al0.5Ge1.5(PO4)3 (LAGP), has been reported to obtain metallic lithium from seawater. However, expensive LAGP increases the cost of lithium extraction, while Li1.3Al0.3Ti1.7(PO4)3 (LATP) with relatively lower prices cannot meet the stable requirements. Herein, a low-cost, stable glass–ceramics, Li1.5Al0.3Ti1.7Si0.2P2.8O12 (LATSP), has been prepared for lithium extraction from seawater. The LATSP glass–ceramics show good selectivity towards Li+ and exhibit a high ionic conductivity of 3.98 × 10−4 S cm−1 at 22 °C. After soaking in simulated seawater, LATSP showed much better stability than LATP, comparable to LAGP. The resultant LATSP glass–ceramics was successfully employed in a seawater lithium extraction device, with a high lithium extraction Coulombic efficiency of 94.0%. Moreover, the LATSP exhibits an ionic conductivity of 2.80 × 10−4 S cm−1 and maintains a complete structure after 45 h of lithium extraction. This work presents an effective and practical Li-ion conducting membrane for lithium extraction from seawater.Graphical Abstract: Rapid development of electronic and grid storage technologies based on lithium-ion batteries are leading to tight supply of lithium resources in the future. Extracting lithium from seawater can completely solve the problem of lithium resource shortage. An electro-deposition method based on a lithium superionic conductive solid-state electrolyte, Li1.5Al0.5Ge1.5(PO4)3 (LAGP), has been reported to obtain metallic lithium from seawater. However, expensive LAGP increases the cost of lithium extraction, while Li1.3Al0.3Ti1.7(PO4)3 (LATP) with relatively lower prices cannot meet the stable requirements. Herein, a low-cost, stable glass–ceramics, Li1.5Al0.3Ti1.7Si0.2P2.8O12 (LATSP), has been prepared for lithium extraction from seawater. The LATSP glass–ceramics show good selectivity towards Li+ and exhibit a high ionic conductivity of 3.98 × 10−4 S cm−1 at 22 °C. After soaking in simulated seawater, LATSP showed much better stability than LATP, comparable to LAGP. The resultant LATSP glass–ceramics was successfully employed in a seawater lithium extraction device, with a high lithium extraction Coulombic efficiency of 94.0%. Moreover, the LATSP exhibits an ionic conductivity of 2.80 × 10−4 S cm−1 and maintains a complete structure after 45 h of lithium extraction. This work presents an effective and practical Li-ion conducting membrane for lithium extraction from seawater. [ABSTRACT FROM AUTHOR]