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Interfacial electrochemical methods focus on the phenomena occurring at the boundary between an electrode and a solution, as opposed to bulk methods that concentrate on the solution's overall properties. These interfacial methods are classified as either static or dynamic based on the presence of a nonzero current in the electrochemical cell and the consistency of analyte concentrations. Static methods, such as potentiometry, measure the cell's potential without any significant current...
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Multifunctional Covalent Organic Framework Electrolyte with Bidirectional Interfacial Engineering for PEO-Based

Yucheng Wen1,2, Houkai Qi2, Jieying Ding1

  • 1School of Materials Science and Engineering, Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials, South China University of Technology, Guangzhou, China.

Small (Weinheim an Der Bergstrasse, Germany)
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Summary

This study introduces a novel composite electrolyte using functionalized covalent organic frameworks (COFs) to improve solid-state battery performance. The new design enhances ionic conductivity and interfacial stability for high-performance all-solid-state batteries.

Keywords:
Li metal anodeall‐solid‐state Li metal batteriescovalent organic frameworkpoly (ethylene oxide)

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Science

Background:

  • Polyethylene oxide (PEO)-based solid-state electrolytes suffer from low ionic conductivity and poor interfacial stability.
  • These limitations hinder the practical application of high-performance all-solid-state batteries.

Purpose of the Study:

  • To develop a multi-level synergistic strategy to enhance ion transport and electrode/electrolyte interfacial stability.
  • To design a composite electrolyte that overcomes the limitations of traditional PEO-based solid-state electrolytes.

Main Methods:

  • Fabrication of a composite electrolyte using a covalent organic framework (COF) functionalized with oligomeric ethylene oxide chains (TPB-BMTP-COF).
  • Incorporation of SnF2 and LiNO3 to form a robust solid electrolyte interphase (SEI).
  • Addition of lithium difluoro(oxalato)borate (LiDFOB) to create a hybrid organic-inorganic cathode electrolyte interphase (CEI).

Main Results:

  • The composite electrolyte achieved an ionic conductivity of 1.5 × 10^-4 S cm^-1 at 30°C.
  • Lithium symmetric cells exhibited stable polarization for over 1200 hours.
  • Li//LFP full cells showed nearly 100% capacity retention after 180 cycles at 30°C.
  • Li//NCM811 cells maintained over 80% capacity retention after 100 cycles at 45°C and 60°C.

Conclusions:

  • The synergistic electrolyte design strategy effectively enhances bulk ion transport and stabilizes interfaces.
  • This approach offers a promising pathway for developing practical, high-performance all-solid-state batteries.
  • The study provides new insights into molecular-level architecture and dual-interface engineering for solid-state electrolytes.