Engineering Conjugated Tetrone‐Imide‐Linked Tubular Carbon Nitride for Boosting Kinetics of Overall Water Splitting

Abstract Photocatalytic water splitting (POW) into H ₂ and O ₂ using organic photocatalysts presents a promising avenue for sustainable and green H ₂ production. Yet it remains a huge challenge to tailor the inherent incompatibility between rapid charge dynamics and sluggish redox kinetics, which limits the POW efficiency. Herein, embedding conjugated tetrone‐imide‐linked electron‐deficient structures (CEDS) in hollow tubular polymeric carbon nitride (TCN) is proposed to induce the anchoring of Pt NPs, significantly boosting charge carrier shuttle to improve the kinetics of overall water splitting. Systematic analysis demonstrates that the synergy between Pt NPs and CEDS sites not only lowers exciton binding energy and strengthens driving force to accelerate free‐electron tandem transfer but also remarkably prolongs the holes' lifetime of TCN and the benzene ring of CEDS under visible‐light response. Mechanism investigations further verify that the benzene ring as active sites favors the single‐ or dual‐site process of O ₂ formation with a thermodynamically low energy barrier. The resultant photocatalysts achieve a record H ₂ and O ₂ yield rates of 1328.65 and 631.33 µmol g ⁻¹ h ⁻¹ under visible‐light and solar‐to‐hydrogen of 0.16% under AM 1.5G irradiation. This work sheds light on a promising avenue for reasonably designing visible‐light response organic photocatalysts to balance the dynamics of charge carriers and surface reactions.