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

Wo Dum Jung, Ji Su Kim, Sungjun Choi, Seongmin Kim, Minjae Jeon, Hun Gi Jung, Kyung Yoon Chung, Jong Ho Lee, Byung Kook Kim, Jong Heun Lee, Hyoungchul Kim

Research output: Contribution to journalArticle

3 Citations (Scopus)

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).

Original languageEnglish
JournalACS Applied Materials and Interfaces
DOIs
Publication statusAccepted/In press - 2020

Keywords

  • Li-argyrodites
  • Li-ion conductors
  • all-solid-state batteries
  • mechanical alloying
  • rapid-thermal annealing

ASJC Scopus subject areas

  • Materials Science(all)

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    Jung, W. D., Kim, J. S., Choi, S., Kim, S., Jeon, M., Jung, H. G., Chung, K. Y., Lee, J. H., Kim, B. K., Lee, J. H., & Kim, H. (Accepted/In press). Superionic Halogen-Rich Li-Argyrodites Using in Situ Nanocrystal Nucleation and Rapid Crystal Growth. ACS Applied Materials and Interfaces. https://doi.org/10.1021/acs.nanolett.9b04597