Given the high theoretical capacity, alloy-based anodes are promising candidates for lithium-ion batteries (LIBs) to meet the stringent demand of today’s portable electronic devices and electric vehicles. However, the intrinsic...

Lithium borohydride (LiBH 4 ), with high compatibility to lithium anode, low grain boundary resistance, and light mass, is regarded as a promising solid-state electrolyte. However, poor ionic conductivity at room temperature limits its practical application in all-solid-state lithium-ion batteries (ASSLBs). In the present study, Li(NH 3 ) x BH 4 @SiO 2 (0 ≤ x ≤ 0.5) composites were obtained by ammonia absorption and simple ball-milling. Among them, Li(NH 3 ) 0.5 BH 4 @ SiO 2 exhibits a high ionic conductivity of 3.95 × 10 −2 S cm −1 at 60 °C, with a lithium transference number up to 0.9999 at 30 °C. More importantly, the experimental results and density functional theory (DFT) calculations show that the skeleton and interfacial interaction of silica can effectively improve the electrochemical performance of the full cell. All-solid-state lithium−sulfur batteries exhibit a specific discharge capacity of 1221.7 mAh g −1 after 10 cycles. Reversible capacities of 1589, 1381, 1176, 969, and 695 mAh g −1 could be achieved at 0.1, 0.2, 0.3, 0.5, and 1C, respectively. These findings prove that Li(NH 3 ) x BH 4 @SiO 2 is an attractive electrolyte for next-generation ASSLBs.

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