Superionic Halogen-Rich Li-Argyrodites Using In Situ Nanocrystal Nucleation and Rapid Crystal Growth

Nano Letters
Wo Dum JungHyoungchul Kim

Abstract

Although several crystalline materials have been developed as Li-ion conductors for use as solid electrolytes in all-solid-state batteries (ASSBs), producing materials with high Li-ion conductivities is time-consuming and cost-intensive. Herein, we introduce a superionic halogen-rich Li-argyrodite (HRLA) and demonstrate its innovative synthesis using ultimate-energy mechanical alloying (UMA) and rapid thermal annealing (RTA). UMA with a 49 G-force milling energy provides a one-pot process that includes mixing, glassification, and crystallization, to produce as-milled HRLA powder that is ∼70% crystallized; subsequent RTA using an infrared lamp increases this crystallinity to ∼82% within 25 min. Surprisingly, this HRLA exhibits the highest Li-ion conductivity among Li-argyrodites (10.2 mS cm-1 at 25 °C, cold-pressed powder compact) reported so far. Furthermore, we confirm that this superionic HRLA works well as a promising solid electrolyte without a decreased intrinsic electrochemical window in various electrode configurations and delivers impressive cell performance (114.2 mAh g-1 at 0.5 C).

References

Dec 29, 2007·Angewandte Chemie·Hans-Jörg DeiserothMarc Schlosser
Aug 2, 2011·Nature Materials·Noriaki KamayaAkio Mitsui
May 16, 2015·Nature Communications·E AllahyarovH Löwen
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Aug 21, 2019·Nature Materials·Theodosios FamprikisChristian Masquelier

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Citations

Mar 10, 2021·Chemical Communications : Chem Comm·Sung Soo ShinHyoungchul Kim
Jun 23, 2020·Chemistry of Materials : a Publication of the American Chemical Society·Marina BrinekH Martin R Wilkening

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