Lithium argyrodites with high ionic conductivities are favorable solid electrolytes (SEs) for all-solid-state batteries (ASSBs). However, their low preparation efficiency and poor cycling performance hinder their large-scale applications. In this work, we demonstrate successful l
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Lithium argyrodites with high ionic conductivities are favorable solid electrolytes (SEs) for all-solid-state batteries (ASSBs). However, their low preparation efficiency and poor cycling performance hinder their large-scale applications. In this work, we demonstrate successful large-scale production (over 1 kg per batch for the first time) of Li5.5PS4.5Cl0.75Br0.75 (LPSCB) by fast dry mixing followed by annealing, which presents high room temperature ionic conductivities of 13 mS cm−1 for cold-pressed and 25 mS cm−1 for sintered pellets. Combining neutron powder diffraction and 6Li → 7Li tracer-exchange nuclear magnetic resonance (NMR) spectroscopy measurements, we show that intercage jumps frequently occur through the 48h-16e-48h pathway in LPSCB, promoting the overall lithium conduction. The assembled ASSBs using LPSCB and a LiNi0.83Co0.11Mn0.06O2 electrode can be cycled for over 2,500 cycles at a 0.5 C rate and 1,800 cycles at a 2 C rate without any capacity degradation. Our results will accelerate the commercialization of sulfide SE for ASSBs.
