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The cationic polymerization mechanism consists of three steps: initiation, propagation, and termination. In the initiation step of the polymerization process, the π bond of a monomer gets protonated by the Lewis acid catalyst, which is formed from boron trifluoride and water. The protonation of the π bond generates a carbocation stabilized by the electron‐donating group. In the propagation step, the π bond of the second monomer acts as a nucleophile and attacks the...
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Terminal-Group Engineering to Amplify Asymmetric Electronic Interactions in COFs for Enhanced Optoelectronic

Zhongping Li1, Yuqiang Huang1, Yucheng Jin2

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Terminal-group engineering enhances covalent organic frameworks (COFs) for optoelectronics. This method boosts charge mobility and photocatalytic performance, nearly quadrupling hydrogen peroxide production in COFs.

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Area of Science:

  • Materials Science
  • Chemistry

Background:

  • Covalent organic frameworks (COFs) are promising for optoelectronics due to tunable properties.
  • Asymmetric electronic structures enhance charge separation and photoelectric conversion efficiency.
  • Current methods to amplify asymmetry involve new monomers or linkage modifications.

Purpose of the Study:

  • To develop a terminal-group engineering strategy to amplify asymmetry in sp² carbon-conjugated COFs.
  • To precisely modulate electronic structure and photophysical behavior for improved performance.
  • To enhance charge mobility and photocatalytic efficiency in COFs.

Main Methods:

  • Engineered terminal groups on sp² carbon-conjugated COFs.
  • Investigated the impact on electronic structure and photophysical properties.
  • Evaluated photocatalytic performance, specifically hydrogen peroxide production.

Main Results:

  • Terminal-group engineering effectively amplified asymmetry in COFs.
  • Achieved enhanced charge mobility and significantly improved photocatalytic performance.
  • Engineered COFs showed a nearly 4-fold increase in hydrogen peroxide production compared to unmodified COFs.
  • Demonstrated excellent structural stability and long-term operational durability.

Conclusions:

  • Terminal-group engineering is a powerful and generalizable strategy for COF design.
  • This approach enables precise control over electronic and photophysical properties.
  • Developed high-performance COF-based materials for optoelectronic and photocatalytic applications.