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Updated: Jan 15, 2026

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Polyamine-Mediated Proton/TFSI- Dual Capture Enables High-Voltage PEO-Based All-Solid-State Li Batteries.

You Fan1, Mingli Zhu1, Huicai Wang1

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|January 14, 2026
PubMed
Summary
This summary is machine-generated.

A novel polyamine agent effectively captures protons and TFSI anions, preventing degradation in high-voltage all-solid-state lithium batteries (ASSLBs) and enhancing their stability and energy density.

Keywords:
Proton/TFSI− captureall‐solid‐state Li batterieshigh voltagepolyethylene oxidepolymer electrolytes

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Chemistry

Background:

  • Poly(ethylene oxide) (PEO)-based solid polymer electrolytes (SPEs) in all-solid-state lithium batteries (ASSLBs) degrade at high voltages (>3.8 V vs. Li+/Li).
  • This degradation is caused by corrosive acids, primarily bis(trifluoromethanesulfonyl)imide (HTFSI), limiting ASSLB energy density.
  • Current passive strategies fail to inhibit HTFSI generation effectively.

Purpose of the Study:

  • To develop a proactive strategy for mitigating degradation in high-voltage ASSLBs.
  • To inhibit the formation of corrosive acids (HTFSI) within the PEO matrix.
  • To enhance the cycling stability and energy density of ASSLBs.

Main Methods:

  • A polyamine-based agent was designed for dual capture of protons (H+) and TFSI- anions.
  • The agent utilizes Brønsted-base sites and H-bond donors for electrostatic and H-bonding interactions.
  • The agent was implemented in 4.2 V LiCoO2-based ASSLBs.

Main Results:

  • The polyamine agent effectively captured H+ and TFSI- ions, suppressing HTFSI formation.
  • ASSLBs with the agent showed exceptional cycling stability (>600 cycles at 1.0 C, 65°C).
  • 95.5% capacity retention was achieved, outperforming existing high-voltage polymer-based ASSLBs.

Conclusions:

  • A dual capture active strategy effectively mitigates both interfacial and bulk degradation in high-voltage ASSLBs.
  • This approach significantly suppresses acid-catalyzed chain scission in the PEO matrix.
  • The findings offer new insights for designing high-energy-density ASSLBs.