Tailoring Solution-Processable Li Argyrodites Li6+xP1-xMxS5I (M = Ge, Sn) and Their Microstructural Evolution Revealed by Cryo-TEM for All-Solid-State Batteries

Song, Yong Bae; Kim, Dong Hyeon; Kwak, Hiram; Han, Daseul; Kang, Sujin; Lee, Jong Hoon; Bak, Seong-Min; Nam, Kyung-Wan; Lee, Hyun-Wook; Jung, Yoon Seok

doi:10.1021/acs.nanolett.0c01028

Title: Tailoring Solution-Processable Li Argyrodites Li_6+xP_1-xM_xS₅I (M = Ge, Sn) and Their Microstructural Evolution Revealed by Cryo-TEM for All-Solid-State Batteries

Journal Article · Tue May 05 00:00:00 EDT 2020 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.0c01028· OSTI ID:1642414

Song, Yong Bae ^[1]; Kim, Dong Hyeon ^[1]; Kwak, Hiram ^[1]; Han, Daseul ^[2]; Kang, Sujin ^[3]; Lee, Jong Hoon ^[4];

^[5];

^[2];

^[3];

^[1]

Hanyang Univ., Seoul (Korea, Republic of)
Dongguk Univ., Seoul (Korea, Republic of)
Ulsan National Institute of Science and Technology (UNIST), Ulsan (Korea, Republic of)
UNIST Central Research Facilities (UCRF), Ulsan (Korea, Republic of)
Brookhaven National Lab. (BNL), Upton, NY (United States)

Owing to their high Li⁺ conductivities, mechanical sinterability, and solution processability, sulfide Li argyrodites have attracted much attention as enablers in the development of high-performance all-solid-state batteries with practicability. However, solution-processable Li argyrodites have been developed only for a composition of Li₆PS₅X (X = Cl, Br, I) with insufficiently high Li⁺ conductivities (~10^–4 S cm^–1). In this work, we report the highest Li⁺ conductivity of 0.54 mS cm^–1 at 30 °C (Li_6.5P_0.5Ge_0.5S₅I) for solution-processable iodine-based Li argyrodites. Furthermore, a comparative investigation of three iodine-based argyrodites of unsubstituted and Ge- and Sn-substituted solution-processed Li₆PS₅I with varied heat-treatment temperature elucidates the effect of microstructural evolution on Li⁺ conductivity. Notably, local nanostructures consisting of argyrodite nanocrystallites in solution-processed Li_6.5P_0.5Ge_0.5S₅I have been directly captured by cryogenic transmission electron microscopy, which is a first for sulfide solid electrolyte materials. Specifically, the promising electrochemical performances of all-solid-state batteries at 30 °C employing LiCoO₂ electrodes tailored by the infiltration of Li_6.5P_0.5Ge_0.5S₅I–ethanol solutions are successfully demonstrated.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Research Foundation of Korea (NRF); National Research Council of Science & Technology (NST)

Grant/Contract Number:: SC0012704; NRF-2017M1A2A2044501; NRF-2018R1A2B600499; 2019R1C1C1009324

OSTI ID:: 1642414

Report Number(s):: BNL-216186-2020-JAAM

Journal Information:: Nano Letters, Vol. 20, Issue 6; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 42 works

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25 ENERGY STORAGE
Solid-state batteries
solid electrolytes
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sulfides
solution processes
electrodes
physical and chemical processes
electrical conductivity

Title: Tailoring Solution-Processable Li Argyrodites Li6+xP1-xMxS5I (M = Ge, Sn) and Their Microstructural Evolution Revealed by Cryo-TEM for All-Solid-State Batteries

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Title: Tailoring Solution-Processable Li Argyrodites Li_6+xP_1-xM_xS₅I (M = Ge, Sn) and Their Microstructural Evolution Revealed by Cryo-TEM for All-Solid-State Batteries