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Overcoming low initial coulombic efficiencies of Si anodes through prelithiation in all-solid-state batteries

Author

Listed:
  • So-Yeon Ham

    (University of California San Diego)

  • Elias Sebti

    (University of California)

  • Ashley Cronk

    (University of California San Diego)

  • Tyler Pennebaker

    (University of California)

  • Grayson Deysher

    (University of California San Diego)

  • Yu-Ting Chen

    (University of California San Diego)

  • Jin An Sam Oh

    (and Research (A*STAR))

  • Jeong Beom Lee

    (LG Science Park)

  • Min Sang Song

    (LG Science Park)

  • Phillip Ridley

    (University of California San Diego)

  • Darren H. S. Tan

    (University of California San Diego)

  • Raphaële J. Clément

    (University of California)

  • Jihyun Jang

    (University of California San Diego
    Sogang University)

  • Ying Shirley Meng

    (University of California San Diego
    University of Chicago)

Abstract

All-solid-state batteries using Si as the anode have shown promising performance without continual solid-electrolyte interface (SEI) growth. However, the first cycle irreversible capacity loss yields low initial Coulombic efficiency (ICE) of Si, limiting the energy density. To address this, we adopt a prelithiation strategy to increase ICE and conductivity of all-solid-state Si cells. A significant increase in ICE is observed for Li1Si anode paired with a lithium cobalt oxide (LCO) cathode. Additionally, a comparison with lithium nickel manganese cobalt oxide (NCM) reveals that performance improvements with Si prelithiation is only applicable for full cells dominated by high anode irreversibility. With this prelithiation strategy, 15% improvement in capacity retention is achieved after 1000 cycles compared to a pure Si. With Li1Si, a high areal capacity of up to 10 mAh cm–2 is attained using a dry-processed LCO cathode film, suggesting that the prelithiation method may be suitable for high-loading next-generation all-solid-state batteries.

Suggested Citation

  • So-Yeon Ham & Elias Sebti & Ashley Cronk & Tyler Pennebaker & Grayson Deysher & Yu-Ting Chen & Jin An Sam Oh & Jeong Beom Lee & Min Sang Song & Phillip Ridley & Darren H. S. Tan & Raphaële J. Clément , 2024. "Overcoming low initial coulombic efficiencies of Si anodes through prelithiation in all-solid-state batteries," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-47352-y
    DOI: 10.1038/s41467-024-47352-y
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    References listed on IDEAS

    as
    1. Xinghao Zhang & Denghui Wang & Xiongying Qiu & Yingjie Ma & Debin Kong & Klaus Müllen & Xianglong Li & Linjie Zhi, 2020. "Stable high-capacity and high-rate silicon-based lithium battery anodes upon two-dimensional covalent encapsulation," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    2. 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.
    3. Shuting Luo & Zhenyu Wang & Xuelei Li & Xinyu Liu & Haidong Wang & Weigang Ma & Lianqi Zhang & Lingyun Zhu & Xing Zhang, 2021. "Growth of lithium-indium dendrites in all-solid-state lithium-based batteries with sulfide electrolytes," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
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