Substituent-induced oxidation-reduction molecular organic junction for interfacial hydrogen peroxide photosynthesis
2026-03-25
The distribution of catalytic active sites critically dictates photocatalytic efficiency, but existing catalyst design operate at the same or adjacent sites still remain limitations toward photocatalytic reaction. To address this, a kind of spatially separable oxidation-reduction assignment in fluorine substituted molecular organic junction catalyst (covalent triazine framework, CTF-TF-0.5) is constructed. By modulating the coordination of F-substituted benzene linkers, we controlled the redox nature of triazine ring in CTFs to obtain the separable oxidation-reduction assignment. It achieves a interfacial hydrogen peroxide (H 2 O 2 ) photosynthesis rate of 4664 µmol g −1 h −1 at triphasic interface with simulated sunlight and ultrasonic forces. With external forces, the photogenerated-holes allow to transfer to the oxidation site (triazine connected two benzene and a F-substituted benzene) and photogenerated-electrons to the reduction site (triazine connected a benzene and two F-substituted benzene) via benzene bridges for a dual-pathway of water oxidation and oxygen reduction reactions to synthesize H 2 O 2 . Additionally, this heterogeneous interfacial reaction system exhibits efficient purification capability for arsenic-containing mining wastewater. This study using the separable oxidation-reduction sites for addressing the coupling reaction at manipulable active sites to improve overall catalytic efficiency via molecular junction catalyst.