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In Situ Polymerization-Driven Exfoliation of COFs: A Universal Strategy Toward High-Performance Polymer Organic
Mengjia Yin1, Fei Shi1, Jing-Jing Yang2
1Key Laboratory of Material Chemistry For Energy Conversion and Storage, Ministry of Education, Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, China.
We developed a novel in situ composite strategy to create few-layer covalent organic framework (COF) nanosheets for advanced lithium-ion batteries. This method enhances ion and electron transport, significantly improving battery performance and energy density.
Area of Science:
- Materials Science
- Electrochemistry
- Nanotechnology
Background:
- Covalent organic frameworks (COFs) show potential as organic cathodes for lithium-ion batteries.
- However, their bulk structure hinders ion/electron transport, limiting performance.
Purpose of the Study:
- To develop an in situ composite strategy to overcome the limitations of bulk COFs.
- To create few-layer COF nanosheets integrated with polymers (COF@Polymer) for enhanced battery performance.
Main Methods:
- An in situ polymerization strategy was employed, growing polymers within COF pores.
- Polymerization stress and polymer-COF interactions were utilized to exfoliate bulk COFs into nanosheets.
- The resulting COF@Polymer composites were characterized for their electrochemical properties.
Main Results:
- The in situ method yielded high-quality COF nanosheets with improved yield and applicability compared to traditional exfoliation.
- COF@Polymer cathodes demonstrated enhanced active site utilization (up to 98%), superior rate capability (70% capacity retention at 10 A g-1), and improved cycle stability.
- One composite (BTCOF@FS-20) achieved a power density of 30.5 kW kg-1 with an energy density of 336 Wh kg-1.
Conclusions:
- The COF@Polymer composite strategy effectively addresses ion/electron transport limitations in COF cathodes.
- This approach offers a scalable method for producing high-performance organic cathode materials for next-generation lithium-ion batteries.

