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Lithium diffusion-controlled Li-Al alloy negative electrode for all-solid-state battery

Author

Listed:
  • Yuju Jeon

    (University of California, San Diego)

  • Dong Ju Lee

    (University of California, San Diego)

  • Hongkui Zheng

    (University of California, Irvine)

  • Sesha Sai Behara

    (Santa Barbara)

  • Jung-Pil Lee

    (LG Science Park)

  • Junlin Wu

    (University of California, San Diego)

  • Feng Li

    (University of California, San Diego)

  • Wei Tang

    (University of California, San Diego)

  • Lanshuang Zhang

    (University of California, San Diego)

  • Yu-Ting Chen

    (University of California, San Diego)

  • Dapeng Xu

    (University of California, San Diego)

  • Jiyoung Kim

    (LG Science Park)

  • Min-Sang Song

    (LG Science Park)

  • Anton Ven

    (Santa Barbara)

  • Kai He

    (University of California, Irvine)

  • Zheng Chen

    (University of California, San Diego
    University of California, San Diego)

Abstract

Metal alloy negative electrodes are promising candidates for lithium all-solid-state batteries due to their high specific capacity and low cost. However, chemo-mechanical degradation and atomic transport limitations in the solid state remain unresolved challenges. Herein, we demonstrate a lithium-aluminum alloy negative electrode design (LixAl1, x = molar ratio of lithium to aluminum) based on a comprehensive understanding of the underlying diffusion mechanisms within the lithium-poor α (0 ≤ x ≤ 0.05) and lithium-rich β phases (0.95 ≤ x ≤ 1). The lithium-aluminum alloy negative electrodes with a higher lithium to aluminum ratio facilitate lithium migration through the β-LiAl phases, which serve as highly lithium-conductive channels with a lithium diffusion coefficient that is ten orders of magnitude higher than that of the α phase. In addition, a bulk dense negative electrode and an intimate negative electrode-electrolyte interface is demonstrated in the cross-sections of the lithium-aluminum alloy negative electrodes. Consequently, a high-rate capability of 7 mA cm−2 is attained in LiNi0.8Co0.1Mn0.1O2-based full-cell operation. The optimal cell configuration of Li0.5Al1 | |LiNi0.8Co0.1Mn0.1O2 shows stable lithium reversibility during 2000 cycles with a capacity retention of 83% at 4 mA cm−2 with a LiNi0.8Co0.1Mn0.1O2 loading of 5 mAh cm−2.

Suggested Citation

  • Yuju Jeon & Dong Ju Lee & Hongkui Zheng & Sesha Sai Behara & Jung-Pil Lee & Junlin Wu & Feng Li & Wei Tang & Lanshuang Zhang & Yu-Ting Chen & Dapeng Xu & Jiyoung Kim & Min-Sang Song & Anton Ven & Kai , 2025. "Lithium diffusion-controlled Li-Al alloy negative electrode for all-solid-state battery," Nature Communications, Nature, vol. 16(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-64386-y
    DOI: 10.1038/s41467-025-64386-y
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    References listed on IDEAS

    as
    1. Hongyi Li & Takitaro Yamaguchi & Shingo Matsumoto & Hiroaki Hoshikawa & Toshiaki Kumagai & Norihiko L. Okamoto & Tetsu Ichitsubo, 2020. "Circumventing huge volume strain in alloy anodes of lithium batteries," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    2. Yuhgene Liu & Congcheng Wang & Sun Geun Yoon & Sang Yun Han & John A. Lewis & Dhruv Prakash & Emily J. Klein & Timothy Chen & Dae Hoon Kang & Diptarka Majumdar & Rajesh Gopalaswamy & Matthew T. McDowe, 2023. "Aluminum foil negative electrodes with multiphase microstructure for all-solid-state Li-ion batteries," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
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