Ultrathin Crystalline Covalent‐Triazine‐Framework Nanosheets with Electron Donor Groups for Synergistically Enhanced Photocatalytic Water Splitting. Issue 48 (27th October 2021)

• Record Type: Journal Article
• Authors: Wang, Congxu; Zhang, Hualei; Luo, Wenjia; Sun, Tian; Xu, Yuxi
• Is Part Of: Angewandte Chemie international edition. Volume 60:Issue 48(2021)
• Page Start: 25381
• Page End: 25390
• Publication Date: 2021-10-27
• Subjects: covalent triazine framework -- electron donor effect -- photocatalytic water splitting -- redox strategy -- ultrathin crystalline nanosheets; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.202109851
• Languages: English
• ISSNs: 1433-7851

Abstract

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 H2 (5.13 μmol h −1 ) and O2 (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). Abstract : Ultrathin crystalline 2D triazine polymer nanosheets with electron donor groups are prepared for the first time by a novel redox strategy. They demonstrate ultrahigh photocatalytic overall water splitting performance arising from the optimized band structure and improved light‐responsive range from the electron donor groups introduced into the 2D ordered molecular plane.