Large-scale manufacturing sulfide superionic conductor for advancing all-solid-state batteries
Shuo Wang (Wuhan University of Technology)
Chenjie Lou (Center for High Pressure Science and Technology Advanced Research)
Xinbin Wu (Tsinghua University)
Jing Lin (Karlsruhe Institut für Technologie)
Ajay Gautam (TU Delft - RST/Storage of Electrochemical Energy)
Zhu Cheng (TU Delft - RST/Storage of Electrochemical Energy)
Shengnan Zhang (TU Delft - RST/Storage of Electrochemical Energy)
Florian Strauss (Karlsruhe Institut für Technologie)
Mingxue Tang (Center for High Pressure Science and Technology Advanced Research)
Ce Wen Nan (Tsinghua University)
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Abstract
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.