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Dynamic spatial progression of isolated lithium during battery operations

Author

Listed:
  • Fang Liu

    (Stanford University)

  • Rong Xu

    (Stanford University)

  • Yecun Wu

    (Stanford University)

  • David Thomas Boyle

    (Stanford University)

  • Ankun Yang

    (Stanford University)

  • Jinwei Xu

    (Stanford University)

  • Yangying Zhu

    (Stanford University)

  • Yusheng Ye

    (Stanford University)

  • Zhiao Yu

    (Stanford University)

  • Zewen Zhang

    (Stanford University)

  • Xin Xiao

    (Stanford University)

  • Wenxiao Huang

    (Stanford University)

  • Hansen Wang

    (Stanford University)

  • Hao Chen

    (Stanford University)

  • Yi Cui

    (Stanford University
    SLAC National Accelerator Laboratory)

Abstract

The increasing demand for next-generation energy storage systems necessitates the development of high-performance lithium batteries1–3. Unfortunately, current Li anodes exhibit rapid capacity decay and a short cycle life4–6, owing to the continuous generation of solid electrolyte interface7,8 and isolated Li (i-Li)9–11. The formation of i-Li during the nonuniform dissolution of Li dendrites12 leads to a substantial capacity loss in lithium batteries under most testing conditions13. Because i-Li loses electrical connection with the current collector, it has been considered electrochemically inactive or ‘dead’ in batteries14,15. Contradicting this commonly accepted presumption, here we show that i-Li is highly responsive to battery operations, owing to its dynamic polarization to the electric field in the electrolyte. Simultaneous Li deposition and dissolution occurs on two ends of the i-Li, leading to its spatial progression toward the cathode (anode) during charge (discharge). Revealed by our simulation results, the progression rate of i-Li is mainly affected by its length, orientation and the applied current density. Moreover, we successfully demonstrate the recovery of i-Li in Cu–Li cells with >100% Coulombic efficiency and realize LiNi0.5Mn0.3Co0.2O2 (NMC)–Li full cells with extended cycle life.

Suggested Citation

  • Fang Liu & Rong Xu & Yecun Wu & David Thomas Boyle & Ankun Yang & Jinwei Xu & Yangying Zhu & Yusheng Ye & Zhiao Yu & Zewen Zhang & Xin Xiao & Wenxiao Huang & Hansen Wang & Hao Chen & Yi Cui, 2021. "Dynamic spatial progression of isolated lithium during battery operations," Nature, Nature, vol. 600(7890), pages 659-663, December.
  • Handle: RePEc:nat:nature:v:600:y:2021:i:7890:d:10.1038_s41586-021-04168-w
    DOI: 10.1038/s41586-021-04168-w
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    Citations

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    Cited by:

    1. Chao Zhu & Till Fuchs & Stefan A. L. Weber & Felix. H. Richter & Gunnar Glasser & Franjo Weber & Hans-Jürgen Butt & Jürgen Janek & Rüdiger Berger, 2023. "Understanding the evolution of lithium dendrites at Li6.25Al0.25La3Zr2O12 grain boundaries via operando microscopy techniques," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    2. Yu Wang & Tairan Wang & Shuyu Bu & Jiaxiong Zhu & Yanbo Wang & Rong Zhang & Hu Hong & Wenjun Zhang & Jun Fan & Chunyi Zhi, 2023. "Sulfolane-containing aqueous electrolyte solutions for producing efficient ampere-hour-level zinc metal battery pouch cells," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    3. Wenxiao Huang & Yusheng Ye & Hao Chen & Rafael A. Vilá & Andrew Xiang & Hongxia Wang & Fang Liu & Zhiao Yu & Jinwei Xu & Zewen Zhang & Rong Xu & Yecun Wu & Lien-Yang Chou & Hansen Wang & Junwei Xu & D, 2022. "Onboard early detection and mitigation of lithium plating in fast-charging batteries," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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