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Overcoming the Electrolyte-Derived Interphase Through Sequential Reactions for Stable Lithium Metal Anode.

Jiangning Liu1, Baoyu Sun1, Lijuan Zhao1

  • 1State Key Laboratory for Mechanical Behavior of Materials, Shaanxi International Research Center for Soft Matter, Xi'an Jiaotong University, Xi'an 710049, China.

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This study introduces a sequential reaction strategy to precisely control the solid electrolyte interphase (SEI) layer in lithium metal batteries. This method enhances stability and achieves ultrahigh energy density for practical applications.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Lithium metal batteries offer high energy density potential (>400 Wh kg-1).
  • Heterogeneous solid electrolyte interphase (SEI) formation leads to poor cycling stability due to uncontrolled dendrite growth and nonuniform ion diffusion.
  • Conventional SEI formation relies on electrolyte decomposition, lacking precise control.

Purpose of the Study:

  • To develop a precise SEI regulation strategy for lithium metal anodes.
  • To overcome limitations of conventional electrolyte-driven SEI decomposition.
  • To enhance the cycling stability and energy density of lithium metal batteries.

Main Methods:

  • A sequential reactions strategy involving controlled chemical and electrochemical processes.
  • Utilizing sulfurized polyethylenimine to chemically induce an Li2S layer for homogeneous Li-ion transport.
  • Forming a Li2S/Li3N intermediate layer electrochemically to accelerate Li-ion migration.

Main Results:

  • A tailored SEI layer was successfully constructed, ensuring robust structural integrity.
  • A LiNi0.8Co0.1Mn0.1O2||Li pouch cell achieved 480.5 Wh kg-1 specific energy under lean electrolyte conditions (1.35 g Ah-1) and high areal capacity (6.0 mAh cm-2).
  • The cell demonstrated impressive capacity retention of 85.9% after 100 cycles.

Conclusions:

  • The sequential reactions strategy provides a new paradigm for rational SEI design.
  • Precise SEI regulation via controlled sequential reactions significantly enhances lithium metal anode stability.
  • This approach offers valuable insights for developing practical, high-performance lithium metal batteries.