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Manipulating the diffusion energy barrier at the lithium metal electrolyte interface for dendrite-free long-life batteries

Author

Listed:
  • Jyotshna Pokharel

    (The University of Texas at Dallas
    South Dakota State University)

  • Arthur Cresce

    (U.S. CCDC Army Research Laboratory)

  • Bharat Pant

    (University of Texas at Arlington)

  • Moon Young Yang

    (California Institute of Technology)

  • Ashim Gurung

    (South Dakota State University)

  • Wei He

    (South Dakota State University)

  • Abiral Baniya

    (South Dakota State University)

  • Buddhi Sagar Lamsal

    (South Dakota State University)

  • Zhongjiu Yang

    (The University of Texas at Dallas)

  • Stephen Gent

    (South Dakota State University)

  • Xiaojun Xian

    (South Dakota State University)

  • Ye Cao

    (University of Texas at Arlington)

  • William A. Goddard

    (California Institute of Technology)

  • Kang Xu

    (U.S. CCDC Army Research Laboratory
    SolidEnergy Systems LLC)

  • Yue Zhou

    (The University of Texas at Dallas)

Abstract

Constructing an artificial solid electrolyte interphase (SEI) on lithium metal electrodes is a promising approach to address the rampant growth of dangerous lithium morphologies (dendritic and dead Li0) and low Coulombic efficiency that plague development of lithium metal batteries, but how Li+ transport behavior in the SEI is coupled with mechanical properties remains unknown. We demonstrate here a facile and scalable solution-processed approach to form a Li3N-rich SEI with a phase-pure crystalline structure that minimizes the diffusion energy barrier of Li+ across the SEI. Compared with a polycrystalline Li3N SEI obtained from conventional practice, the phase-pure/single crystalline Li3N-rich SEI constitutes an interphase of high mechanical strength and low Li+ diffusion barrier. We elucidate the correlation among Li+ transference number, diffusion behavior, concentration gradient, and the stability of the lithium metal electrode by integrating phase field simulations with experiments. We demonstrate improved reversibility and charge/discharge cycling behaviors for both symmetric cells and full lithium-metal batteries constructed with this Li3N-rich SEI. These studies may cast new insight into the design and engineering of an ideal artificial SEI for stable and high-performance lithium metal batteries.

Suggested Citation

  • Jyotshna Pokharel & Arthur Cresce & Bharat Pant & Moon Young Yang & Ashim Gurung & Wei He & Abiral Baniya & Buddhi Sagar Lamsal & Zhongjiu Yang & Stephen Gent & Xiaojun Xian & Ye Cao & William A. Godd, 2024. "Manipulating the diffusion energy barrier at the lithium metal electrolyte interface for dendrite-free long-life batteries," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-47521-z
    DOI: 10.1038/s41467-024-47521-z
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    References listed on IDEAS

    as
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    2. Jianming Zheng & Mark H. Engelhard & Donghai Mei & Shuhong Jiao & Bryant J. Polzin & Ji-Guang Zhang & Wu Xu, 2017. "Electrolyte additive enabled fast charging and stable cycling lithium metal batteries," Nature Energy, Nature, vol. 2(3), pages 1-8, March.
    3. Richard Schmuch & Ralf Wagner & Gerhard Hörpel & Tobias Placke & Martin Winter, 2018. "Performance and cost of materials for lithium-based rechargeable automotive batteries," Nature Energy, Nature, vol. 3(4), pages 267-278, April.
    4. Guoxing Li & Zhe Liu & Qingquan Huang & Yue Gao & Michael Regula & Daiwei Wang & Long-Qing Chen & Donghai Wang, 2018. "Stable metal battery anodes enabled by polyethylenimine sponge hosts by way of electrokinetic effects," Nature Energy, Nature, vol. 3(12), pages 1076-1083, December.
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