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In-Built Reactive Polymer as Versatile Electrolyte to Shield the Bi-Electrode Surfaces for Practical Li-Metal

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A new reactive polymer electrolyte (PTGI) stabilizes interfaces in high-voltage lithium metal batteries (LMBs), enabling over 1000 cycles by preventing parasitic reactions and degradation for improved energy storage.

Keywords:
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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Chemistry

Background:

  • High-voltage lithium metal batteries (LMBs) face interfacial instability issues at electrodes, limiting performance.
  • Degradation of cathodes like single-crystal LiNi0.8Co0.1Mn0.1O2 (SC-NCM) and lithium metal anodes hinders cycle life.

Purpose of the Study:

  • To develop a novel reactive polymer electrolyte (PTGI) for high-voltage LMBs.
  • To enhance interfacial stability and suppress parasitic reactions.
  • To improve the cycle life and safety of LMBs.

Main Methods:

  • In situ preparation of a reactive polymer electrolyte (PTGI) with a narrow orbital energy gap.
  • Formation of robust cathode electrolyte interphase (CEI) and solid electrolyte interphase (SEI).
  • Electrochemical testing of Li|PTGI|SC-NCM and Li|PTGI|LiFePO4 cells, including pouch cell assembly.

Main Results:

  • PTGI forms stable CEI/SEI layers, suppressing interfacial reactions and SC-NCM degradation across temperatures.
  • PTGI scavenges HF and promotes Li+ migration via a loose solvation shell.
  • Li|PTGI|SC-NCM cells achieved over 1000 cycles at 1C; Li|PTGI|LiFePO4 cells cycled for 1700 cycles (76.1% retention).
  • 1.5 Ah pouch cells demonstrated good cycling stability.

Conclusions:

  • The in situ reactive PTGI strategy effectively enhances interfacial stability in high-voltage LMBs.
  • This approach significantly improves cycle life and safety for next-generation energy storage.
  • PTGI offers a promising pathway for developing advanced lithium metal batteries.