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All-Solid-State Lithium Metal Batteries with Microdomain-Regulated Polycationic Solid Electrolytes.

Guo Ye1, Xufeng Hong1, Mengxue He1

  • 1Beijing Key Laboratory for Theory and Technology of Advanced Battery Materials, School of Materials Science and Engineering, Peking University, Beijing, 100871, China.

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Summary
This summary is machine-generated.

This study introduces a novel polycationic solid electrolyte (PCSE) for safer, high-energy solid-state lithium metal batteries (LMBs). The PCSE enhances ion conductivity and stability, enabling fast charging and long cycle life at ambient temperatures.

Keywords:
Li+ transference numberaggressive cathodesanion trappinglithium metal batteriespolycationic solid electrolytes

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Chemistry

Background:

  • Solid polymer electrolytes (SPEs) are crucial for developing high-energy and high-safety solid-state lithium metal batteries (LMBs).
  • Achieving stable and fast-charging high-voltage LMBs requires electrolytes with high ionic conductivity, good Li+ transference, and wide electrochemical windows.
  • Traditional SPEs often face challenges in balancing these properties for demanding battery applications.

Purpose of the Study:

  • To design and synthesize a novel polycationic solid electrolyte (PCSE) for advanced solid-state lithium metal batteries.
  • To leverage the unique properties of polycationic and fluorinated microdomains for enhanced electrolyte performance.
  • To demonstrate the efficacy of the PCSE in enabling stable and fast-charging high-voltage LMBs.

Main Methods:

  • Development of a polycationic solid electrolyte (PCSE) incorporating a fluorinated microdomain.
  • Utilizing the anion trapping (FMAT) effect for localized solvation and restricted anion mobility.
  • In situ thermal polymerization of the electrolyte within assembled Li|LiNi0.8Co0.1Mn0.1O2 cells.

Main Results:

  • The PCSE achieved a high ionic conductivity of 1.4 mS cm-1 and a Li+ transference number of 0.50.
  • A wide electrochemical window of approximately 5.5 V was observed at 25 °C.
  • Li|LiNi0.8Co0.1Mn0.1O2 cells demonstrated ultra-stable cycling with 98.1% capacity retention after 500 cycles at 0.2 C.

Conclusions:

  • The developed PCSE offers a promising strategy for creating stable and high-performance solid-state lithium metal batteries.
  • The molecular design, combining polycationic stability with fluorinated anion trapping, addresses key challenges in SPE development.
  • This approach paves the way for next-generation high-energy, long-life, ambient-temperature solid-state LMBs.