Self-organized hetero-nanodomains actuating super Li+ conduction in glass ceramics

Easy-to-manufacture Li2S-P2S5 glass ceramics are the key to large-scale all-solid-state lithium batteries from an industrial point of view, while their commercialization is greatly hampered by the low room temperature Li+ conductivity, especially due to the lack of solutions. Herein, we propose a nanocrystallization strategy to fabricate super Li+-conductive glass ceramics. Through regulating the nucleation energy, the crystallites within glass ceramics can self-organize into hetero-nanodomains during the solid-state reaction. Cryogenic transmission electron microscope and electron holography directly demonstrate the numerous closely spaced grain boundaries with enriched charge carriers, which actuate superior Li+-conduction as confirmed by variable-temperature solid-state nuclear magnetic resonance. Glass ceramics with a record Li+ conductivity of 13.2mS cm(-1) are prepared. The high Li+ conductivity ensures stable operation of a 220 mu m thick LiNi0.6Mn0.2Co0.2O2 composite cathode (8mAh cm(-2)), with which the all-solid-state lithium battery reaches a high energy density of 420Wh kg(-1) by cell mass and 834WhL(-1) by cell volume at room temperature. These findings bring about powerful new degrees of freedom for engineering super ionic conductors.

Automated summary

By regulating the nucleation energy, crystallites within glass ceramics can self-organize into hetero-nanodomains during the solid-state reaction, resulting in numerous closely spaced grain boundaries with enriched charge carriers, enabling superior Li+-conduction.