Charge Accumulation Engineering in Covalent Organic Frameworks for Enhancing Photocatalytic H₂O₂ Production

Area of Science:

• Materials Science
• Photocatalysis
• Green Chemistry

Background:

• Covalent organic frameworks (COFs) show promise for photocatalysis.
• Efficient charge separation and transport are critical for optimizing photocatalytic performance.
• Developing strategies to enhance these processes is key for advanced applications.

Purpose of the Study:

• To design and implement a charge accumulation strategy in multicomponent COFs.
• To maximize photocatalytic hydrogen peroxide (H₂O₂) production.
• To provide a rational design for high-performance photocatalysts.

Main Methods:

• Synthesized multicomponent COFs with a specific D-A-A omino-A-D configuration.
• Utilized electron-donating (D) and electron-accepting (A, A omino) building blocks.
• Investigated charge carrier dynamics and photocatalytic H₂O₂ evolution.

Main Results:

• The D-A-A omino-A-D configuration effectively funnels and confines photogenerated electrons.
• This leads to enhanced oxygen adsorption and activation at the A omino center.
• Achieved a H₂O₂ evolution rate of 6864.68 µmol·g⁻¹·h⁻¹, AQY of 14.13%, and SCC efficiency of 1.27%.

Conclusions:

• The charge accumulation strategy significantly enhances photocatalytic H₂O₂ production compared to conventional designs.
• The developed COF material demonstrates robust activity under natural sunlight in real water.
• This work offers insights into charge transport in COFs and a design principle for efficient photocatalysts.