Regulating Benzothiadiazole-Based Covalent-Organic Frameworks to Boost Hydrogen Peroxide Photosynthesis and Pathogenic Bacterial Elimination

Benzothiadiazole offers an effective charge transfer channel and serves as a suitable unit for constructing donor-acceptor (D-A) covalent-organic frameworks (COFs), yet systematic investigation on benzothiadiazole-containing COFs is still rare. Herein, we construct four highly crystalline COFs and carefully explore their H2O2 photosynthetic efficiency. Changing the donor unit from phenyl to naphthalenyl group effectively enhances the H2O2 yield rate by nearly 3-fold, highlighting the importance of regulating D-A configuration. The optimized COF (BTpaNda) presents a high H2O2 yield rate of 10,122 mu mol g-1 h-1. Theoretical calculations reveal that BTpaNda COF has the lowest Gibbs free energy in rate-determining oxygen-containing intermediate formation, corroborating the superb H2O2 photosynthesis. Furthermore, the BTpaNda COF demonstrates good stability and excellent bacterial elimination effects with the involvement of oxygen-containing intermediates. Thus, the structural regulation of benzothiadiazole-containing COFs on photocatalytic H2O2 generation and cascade bacterial elimination with oxygen-containing intermediate generation is demonstrated.