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Mechanism of stable lithium plating and stripping in a metal-interlayer-inserted anode-less solid-state lithium metal battery

Author

Listed:
  • Dong-Su Ko

    (Yeongtong-gu)

  • Sewon Kim

    (Yeongtong-gu)

  • Sangjun Lee

    (Yeongtong-gu)

  • Gabin Yoon

    (Yeongtong-gu)

  • Daeho Kim

    (Bundang-gu)

  • ChaeHo Shin

    (Yuseong-gu)

  • Dongmin Kim

    (Yeongtong-gu)

  • Jaewoo Lee

    (Yeongtong-gu)

  • Soohwan Sul

    (Yeongtong-gu)

  • Dong-Jin Yun

    (Yeongtong-gu)

  • Changhoon Jung

    (Yeongtong-gu)

Abstract

To reliably operate anode-less solid-state Li metal batteries, wherein precipitated Li acts as the anode, stabilizing the interface between the solid electrolyte and electrode is crucial. The interface can be controlled by a metal interlayer on the electrolyte to form a Li alloy buffer that facilitates stable Li plating/stripping, thereby mitigating the loss of physical contact and preventing short circuits. However, the mechanism governing stable Li plating/stripping in the metal interlayer without degrading battery materials remains unclear owing to an incomplete understanding of the dynamic and complex electrochemical reactions in the solid state. Through multiple operando and post-mortem analyses of the Li deposition behavior in the morphology, chemistry and microstructure, a close correlation is found between the Li-metal alloying process with the microstructural evolution and electrochemical performance when Ag, Au, Zn, and Cu interlayers were adopted on the garnet-type solid electrolyte Li6.5La3Zr1.5Ta0.5O12. The Ag interlayer improved the interfacial stability enabled by Ag-dissolved Li, which inhibited dendritic growth, passing through the phase-separated Li-Ag alloy microstructure, while the other metals did not because of the Li plating at the Li-metal alloy/solid electrolyte interface. This work provides fundamental guidance for material selection and interface design, advancing the development of anode-less solid-state batteries.

Suggested Citation

  • Dong-Su Ko & Sewon Kim & Sangjun Lee & Gabin Yoon & Daeho Kim & ChaeHo Shin & Dongmin Kim & Jaewoo Lee & Soohwan Sul & Dong-Jin Yun & Changhoon Jung, 2025. "Mechanism of stable lithium plating and stripping in a metal-interlayer-inserted anode-less solid-state lithium metal battery," Nature Communications, Nature, vol. 16(1), pages 1-13, December.
  • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-55821-1
    DOI: 10.1038/s41467-025-55821-1
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    References listed on IDEAS

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    1. Sewon Kim & Ju-Sik Kim & Lincoln Miara & Yan Wang & Sung-Kyun Jung & Seong Yong Park & Zhen Song & Hyungsub Kim & Michael Badding & JaeMyung Chang & Victor Roev & Gabin Yoon & Ryounghee Kim & Jung-Hwa, 2022. "High-energy and durable lithium metal batteries using garnet-type solid electrolytes with tailored lithium-metal compatibility," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
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    3. Yong-Gun Lee & Satoshi Fujiki & Changhoon Jung & Naoki Suzuki & Nobuyoshi Yashiro & Ryo Omoda & Dong-Su Ko & Tomoyuki Shiratsuchi & Toshinori Sugimoto & Saebom Ryu & Jun Hwan Ku & Taku Watanabe & Youn, 2020. "High-energy long-cycling all-solid-state lithium metal batteries enabled by silver–carbon composite anodes," Nature Energy, Nature, vol. 5(4), pages 299-308, April.
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