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Electronic-State Polarization Engineering-Regulated Fluorinated Covalent Organic Framework Nanocables for Fast

Kaifu Xu1, Jianfei Shi1, Yuting Qin1

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Fluorinated covalent organic frameworks (COFs) integrated with carbon nanotubes (CNTs) boost lithium-ion battery anodes. This electronic-state polarization engineering enhances ion transport and stability for high-performance energy storage.

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electronic‐state polarization engineeringfluorinated covalent organic frameworkhigh‐rate lithium‐ion storageorganic anode materials

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Nanotechnology

Background:

  • Covalent organic frameworks (COFs) show potential as anode materials for lithium-ion batteries (LIBs) due to their tunable structures and redox activity.
  • However, their practical application is hindered by poor electronic conductivity and slow ion kinetics, limiting rate capability and cycle life.

Purpose of the Study:

  • To develop a high-performance anode material for LIBs by engineering the electronic state of COFs.
  • To enhance ion transport and electrochemical kinetics in COF-based anodes through targeted structural modification.

Main Methods:

  • In situ construction of fluorinated COF nanocables on conductive carbon nanotube (CNT) scaffolds (F-COF@CNT).
  • Utilizing electronic-state polarization engineering via C─F bonds to modify the COF framework.
  • Employing Galvanostatic Intermittent Titration (GITT) and Density Functional Theory (DFT) calculations to study ion diffusion.

Main Results:

  • The F-COF@CNT anode exhibited enhanced Li+ attraction and accelerated ion transport due to localized electronic polarization.
  • Reduced Li+ diffusion barriers and sustained diffusion coefficients (10^-11 cm^2 s^-1) were observed.
  • The F-COF@CNT anode delivered a high capacity of 496.32 mAh g-1 at 0.1 A g-1 and maintained 281.21 mAh g-1 after 2000 cycles at 2.0 A g-1.
  • A full cell using NCM811||F-COF@CNT demonstrated excellent stability with 105.94 mAh g-1 after 500 cycles.

Conclusions:

  • Electronic-state polarization engineering is an effective strategy to overcome kinetic limitations in COF anodes.
  • The F-COF@CNT material offers a promising solution for high-performance and stable lithium-ion batteries.
  • This approach provides a general pathway for designing advanced organic framework-based energy storage materials.