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Li1.5Al0.5Ge1.5(PO4)3 (LAGP) is among the most promising solid electrolytesfor the next generation all-solid-state lithium batteries. However, preparingLAGP electrolytes is timeand energy-intensive. In this work, LAGP glassypowders were sintered and crystallized in 180 seconds by ultrafasthigh-temperature sintering (UHS) under conditions attractive for continuousindustrial processes (i.e., ambient pressure and atmosphere). The fast heatingrates characteristic of UHS significantly delay crystallization, potentiallydecoupling crystallization and sintering. Furthermore, EIS characterizationsreveal that LAGP sintered and crystallized by UHS has an ionic conductivity of1.15 10-4 S/cm, slightly lower than conventionally annealed samples (1.75 10-4S/cm). The lower conductivity can be attributed to poorer intergrain contact.To overcome this issue, additives such as B2O3 and Li3BO3 are used, resultingin 2 and 5 times higher grain boundary conductivity for LAGP+1 wt B2O3 andLAGP+1 wt Li3BO3, respectively, compared to LAGP. Overall, this work providesinsights into unraveling the impact of UHS sintering on the LAGP Li+ conductionmechanism.

Ultrafast crystallization and sintering of Li1.5Al0.5Ge1.5(PO4)3 glass and its impact on ion conduction