Carbon nanotube incorporation and framework protonation-regulated energy band for enhanced photocatalytic hydrogen peroxide production of COF

Covalent organic frameworks (COFs) were the promising solar catalysts for producing hydrogen peroxide (H₂O₂). However, they remain suffered from poor light absorption, slow charge separation, and limited substrate accessibility. To address these issues, we synthesized an imine-linked triazine-based COF directly onto carbon nanotubes (CNTs) through an interface-mediated Schiff base reaction, creating a tubular nano-complex designated as CNT@COF. Protonation of the imine bonds in the resulting CNT@COF-H significantly enhanced its photocatalytic H₂O₂ production, achieving a rate of 790.5 μM·h⁻¹ under one sunlight irradiation. This performance outshines that of the unmodified COF and surpasses many other COF-based materials. Further studies revealed that protonation improved substrate accessibility, while the integrated CNTs acted as electron transporters to expand light absorption and reduce charge recombination, thereby enhancing photocatalytic activity. The efficacy of CNT@COF-H was demonstrated through its strong sterilization capability and clear dye degradation, offering a promising method for efficient and eco-friendly production of H₂O₂.