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Decoupling Interlayer Interactions Boosts Charge Separation in Covalent Organic Frameworks for High-Efficiency

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Summary

Interlayer coupling in covalent organic frameworks (COFs) significantly impacts charge transfer for photocatalysis. Weakening these interactions enhances COF performance in solar CO2 reduction.

Keywords:
charge transfercovalent organic frameworksdonor‐acceptor systemsinterlayer π–π interactionphotocatalytic CO2 reduction

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Area of Science:

  • Materials Science
  • Photocatalysis
  • Computational Chemistry

Background:

  • Covalent organic frameworks (COFs) show promise as photocatalysts due to their tunable properties.
  • Previous research focused on narrow bandgaps, overlooking interlayer coupling's role in charge transfer.
  • Monolayer models fail to capture essential interlayer effects on electron transport.

Purpose of the Study:

  • Investigate the influence of interlayer interactions on intralayer charge transfer in imine-based COFs using DFT.
  • Understand how interlayer coupling affects electron transport to catalytic sites.
  • Design COFs with optimized interlayer interactions for enhanced photocatalysis.

Main Methods:

  • Density functional theory (DFT) calculations.
  • Theoretical analysis of bilayer COF architectures.
  • Design and synthesis of isomeric pyrene-based COFs with varied interlayer coupling.

Main Results:

  • Bilayer COFs exhibit significant interlayer interference in charge transfer, unlike monolayer models.
  • Weakened interlayer interactions in pyrene-based COFs improved photocatalytic CO2 reduction.
  • Achieved a CO evolution rate of 553.3 µmol g⁻¹ h⁻¹ with 94% selectivity under visible light.

Conclusions:

  • Interlayer coupling is a critical factor in COF photocatalyst design.
  • Optimizing interlayer interactions enhances charge transfer dynamics.
  • This work provides a new principle for developing efficient COF-based solar energy conversion materials.