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Stable Cycling Lithium-Sulfur Solid Batteries with Enhanced Li/Li10GeP2S12 Solid Electrolyte Interface Stability.

Ediga Umeshbabu, Bizhu Zheng, Jianping Zhu

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    |April 30, 2019
    PubMed
    Summary

    Researchers improved lithium-metal solid-state battery performance by using an ionic liquid to stabilize the interface between the Li$_{10}$GeP$_{2}$S$_{12}$ solid electrolyte and Li metal, achieving stable cycling and high capacity in Li-S cells.

    Keywords:
    LiGePS solid electrolytecarbon materialselectrode/electrolyte interface stabilityionic liquidlithium−sulfur batteries

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    Area of Science:

    • Materials Science
    • Electrochemistry
    • Solid-State Batteries

    Background:

    • Interface instability between solid electrolytes and lithium metal hinders the development of high-performance solid-state batteries.
    • Lithium superionic conducting Li$_{10}$GeP$_{2}$S$_{12}$ (LGPS) is a promising solid electrolyte, but its interface with Li metal requires stabilization.
    • Achieving stable lithium stripping/plating is crucial for the longevity of lithium-based batteries.

    Purpose of the Study:

    • To enhance the interface stability between the LGPS solid electrolyte and Li metal using an ionic liquid.
    • To investigate the formation of an in situ solid electrolyte interphase (SEI) layer for improved interfacial properties.
    • To fabricate and evaluate Li-S solid-state batteries utilizing the modified interface and optimized cathode materials.

    Main Methods:

    • Employing 1 M lithium bis(trifluoromethanesulfonyl)imide (LiTFSI)/ N-methyl- N-propylpyrrolidinium bis(trifluoromethanesulfonyl)imide (PYR$_{13}$TFSI) ionic liquid as an interface modifier.
    • Fabricating Li/LGPS/Li symmetric cells to assess interfacial resistance and Li stripping/plating performance.
    • Constructing Li-S solid-state batteries with S@C composite cathodes (S@KBC, S@PBX51C, S@MCNTs) and LGPS solid electrolyte.

    Main Results:

    • The ionic liquid modifier formed an in situ SEI layer, significantly improving Li/LGPS interface stability.
    • Interfacial resistance was reduced from 2021 to 142 Ω cm$^2$, and stable Li stripping/plating was achieved over 1000 hours.
    • Li-S batteries with S@Ketjen black carbon (KBC) cathodes exhibited superior discharge capacity (1017 mA h g$^{-1}$) and stability compared to other carbon types.

    Conclusions:

    • The ionic liquid effectively stabilizes the Li/LGPS interface, enabling robust lithium metal cycling.
    • The S@KBC cathode demonstrates excellent performance in Li-S solid-state batteries due to its high surface area and favorable pore structure.
    • This approach offers a promising strategy for developing high-performance and stable lithium-sulfur solid-state batteries.