Electronic Tuning of Covalent Triazine Framework Nanoshells for Highly Efficient Photocatalytic H2O2 Production

Abstract Photocatalytic H 2 O 2 production is a prospective alternative to the traditional anthraquinone oxidation method for H 2 O 2 production. Compared to well‐established inorganic counterparts, organic photocatalysts show greater promise owing to their structural diversity and functional tunability, but unfortunately suffer from limited activity at present. Here, a comonomer doping strategy is reported to tune the electronic structures of covalent triazine framework nanoshells by introducing strong electron‐withdrawing benzothiadiazole units into the conjugated networks. The product exhibits much enhanced charge separation as evidenced by multiple spectroscopic analyses. When investigated as the photocatalyst in aqueous solution, the best sample can enable an impressive H 2 O 2 production rate of 1630 µmol g −1 h −1 , which is approximately three times higher than that of the undoped sample and superior to most other inorganic and organic competitors.