Ultrathin Crystalline Covalent‐Triazine‐Framework Nanosheets with Electron Donor Groups for Synergistically Enhanced Photocatalytic Water Splitting

Abstract Ultrathin nanosheets have great potential for photocatalytic applications, however, suffer from enlarged band gap and narrowed visible‐light‐responsive range due to the quantum confinement effect. Herein, we report a novel redox strategy for efficient preparation of ultrathin crystalline amide‐functionalized covalent‐triazine‐framework nanosheets (CTF NSs) with enhanced visible light absorption. The CTF NSs exhibited photocatalytic hydrogen (512.3 μmol h −1 ) and oxygen (12.37 μmol h −1 ) evolution rates much higher than that of pristine bulk CTF. Photocatalytic overall water splitting could be achieved with efficient stoichiometric H 2 (5.13 μmol h −1 ) and O 2 (2.53 μmol h −1 ) evolution rates under visible light irradiation. Experimental and theoretical analysis revealed that introduction of amide groups as electron donor optimized the band structure and improve its visible‐light absorption, hydrophilicity and carrier separation efficiency, thus resulting in the enhanced photocatalytic performance. The well‐dispersed CTF NSs could be easily cast onto a support as a thin film device and demonstrate excellent photocatalytic activity (25.7 mmol h −1 m −2 for hydrogen evolution).