High areal capacity, long cycle life 4 V ceramic all-solid-state Li-ion batteries enabled by chloride solid electrolytes

All-solid-state Li batteries (ASSBs) employing inorganic solid electrolytes offer improved safety and are exciting candidates for next-generation energy storage. Herein, we report a family of lithium mixed-metal chlorospinels, Li2InxSc0.666-xCl4 (0 <= x <= 0.666), with high ionic conductivity (up to 2.0 mS cm(-1)) owing to a highly disordered Li-ion distribution, and low electronic conductivity (4.7 x 10(-10) S cm(-1)), which are implemented for high-performance ASSBs. Owing to the excellent interfacial stability of the SE against uncoated high-voltage cathode materials, ASSBs utilizing LiCoO2 or LiNi0.85Co0.1Mn0.05O2 exhibit superior rate capability and long-term cycling (up to 4.8 V versus Li+/Li) compared to state-of-the-art ASSBs. In particular, the ASSB with LiNi0.85Co0.1Mn0.05O2 exhibits a long life of >3,000 cycles with 80% capacity retention at room temperature. High cathode loadings are also demonstrated in ASSBs with stable capacity retention of >4 mAh cm(-2) (similar to 190 mAh g(-1)).

Automated summary

A series of new lithium mixed-metal chlorospinels are reported as solid electrolytes for all-solid-state lithium batteries, which exhibit high ionic conductivity and low electronic conductivity, showing potential for high-performance all-solid-state lithium batteries.