Constructing Donor-Acceptor Covalent Organic Frameworks for Highly Efficient H₂O₂ Photosynthesis Coupled with...

Area of Science:

• Materials Science
• Photocatalysis
• Organic Chemistry

Background:

• Simultaneous production of H2O2 and organic chemicals via photocatalysis offers dual benefits for solar energy utilization.
• Existing photocatalysts for dual functions are limited, necessitating new material development.

Purpose of the Study:

• To synthesize and evaluate donor-acceptor covalent organic frameworks (COFs) for the co-production of H2O2 and N-benzylbenzaldimine (BBAD).
• To identify the most efficient COF-based photocatalyst for this dual application.

Main Methods:

• Synthesis of a series of COFs (JUC-675 to JUC-677).
• Photocatalytic testing for H2O2 and BBAD co-production.
• Validation experiments and density functional theory (DFT) calculations to elucidate reaction mechanisms.

Main Results:

• JUC-675 demonstrated exceptional photocatalytic performance, achieving a H2O2 production rate of 22.8 mmol g-1 h-1 and 15.7% apparent quantum yield.
• Solar-to-chemical conversion efficiency reached 1.09% for JUC-675, the highest reported for COF-based photocatalysts.
• JUC-675 exhibited high selectivity (99.9%) and yield (96%) for BBAD synthesis via oxidative coupling of benzylamine.

Conclusions:

• JUC-675 is a highly effective COF-based photocatalyst for the simultaneous production of H2O2 and BBAD.
• This study advances the design of dual-function photocatalytic systems and enhances solar energy utilization strategies.