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

Authors
Jung, Wo DumKim, Ji-SuChoi, SungjunKim, SeongminJeon, MinjaeJung, Hun-GiChung, Kyung YoonLee, Jong-HoKim, Byung-KookLee, Jong-HeunKim, Hyoungchul
Issue Date
8-4월-2020
Publisher
AMER CHEMICAL SOC
Keywords
Li-ion conductors; Li-argyrodites; mechanical alloying; rapid-thermal annealing; all-solid-state batteries
Citation
NANO LETTERS, v.20, no.4, pp.2303 - 2309
Indexed
SCIE
SCOPUS
Journal Title
NANO LETTERS
Volume
20
Number
4
Start Page
2303
End Page
2309
URI
https://scholar.korea.ac.kr/handle/2021.sw.korea/56638
DOI
10.1021/acs.nanolett.9b04597
ISSN
1530-6984
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 similar to 70% crystallized; subsequent RTA using an infrared lamp increases this crystallinity to similar to 82% within 25 min. Surprisingly, this HRLA exhibits the highest Li-ion conductivity among Li-argyrodites (10.2 mS cm(-1) at 25 degrees 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).
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