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Multiscale interfacial stabilization via prelithiation separator engineering for Ah-level anode-free lithium batteries

Author

Listed:
  • Ahu Shao

    (Northwestern Polytechnical University)

  • Helin Wang

    (Northwestern Polytechnical University)

  • Min Zhang

    (Northwestern Polytechnical University)

  • Jiacheng Liu

    (Northwestern Polytechnical University)

  • Lu Cheng

    (Northwestern Polytechnical University)

  • Yunsong Li

    (Northwestern Polytechnical University)

  • Yuxiang Guo

    (Northwestern Polytechnical University)

  • Zhiqiao Wang

    (Northwestern Polytechnical University)

  • Qiurong Jia

    (Northwestern Polytechnical University
    Zhengzhou BAK Battery Co. Ltd)

  • Xin Wang

    (Shaanxi Raisight Energy Tech Co. Ltd)

  • Xiaoyu Tang

    (Northwestern Polytechnical University)

  • Xiaodong Zhao

    (Fujian Blue Ocean & Black Stone Technology Co. Ltd)

  • Yue Ma

    (Northwestern Polytechnical University)

Abstract

Anode-free lithium batteries represent a promising avenue for high-energy-density storage, yet their practical application is hindered by lithium inventory loss from parasitic interfacial reactions, cathode degradation, and limited Li+ reversibility. Herein, we propose a polyolefin separator integrated with a Li2S@C sacrificial layer, achieving multiscale interfacial stabilization in Ah-class anode-free pouch cells. This approach simultaneously replenishes the customized Li+ inventory during the formation cycle and establishes the lithium polysulfide-containing cathode interface with high-voltage tolerance (till 4.5 V). Real-time tracking via in-situ electrochemical impedance spectroscopy and transmission-mode operando X-ray diffraction reveals accelerated Li+ diffusion kinetics and stabilized phase evolution in LiNi0.8Co0.1Mn0.1O2 cathode interfaced with Li2S@C|PE prelithiation separator. Consequently, a 1.22 Ah pouch cell with an Ag-modified Cu foil and LiNi0.8Co0.1Mn0.1O2 cathode is assembled with Li2S@C|PE separator and exhibits gravimetric and volumetric energy densities of 450 Wh kg-1 and 1355 Wh L-1, respectively. This prelithiation protocol demonstrates upscaling potential and generic applicability to secure the interfacial chemistries for anode free/less lithium metal batteries.

Suggested Citation

  • Ahu Shao & Helin Wang & Min Zhang & Jiacheng Liu & Lu Cheng & Yunsong Li & Yuxiang Guo & Zhiqiao Wang & Qiurong Jia & Xin Wang & Xiaoyu Tang & Xiaodong Zhao & Yue Ma, 2025. "Multiscale interfacial stabilization via prelithiation separator engineering for Ah-level anode-free lithium batteries," Nature Communications, Nature, vol. 16(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-59521-8
    DOI: 10.1038/s41467-025-59521-8
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    References listed on IDEAS

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    1. A. J. Louli & A. Eldesoky & Rochelle Weber & M. Genovese & Matt Coon & Jack deGooyer & Zhe Deng & R. T. White & Jaehan Lee & Thomas Rodgers & R. Petibon & S. Hy & Shawn J. H. Cheng & J. R. Dahn, 2020. "Diagnosing and correcting anode-free cell failure via electrolyte and morphological analysis," Nature Energy, Nature, vol. 5(9), pages 693-702, September.
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