| Affiliation: | 1. Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438 China School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081 China;2. Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438 China;3. School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081 China;4. College of Science, Huazhong Agricultural University, Wuhan, 430070 China |
| Abstract: | Herein, the exposure of highly-active nitrogen cation sites has been accomplished by photo-driven quasi-topological transformation of a 1,10-phenanthroline-5,6-dione-based covalent organic framework (COF), which contributes to hydrogen peroxide (H2O2) synthesis during the 2-electron O2 photoreduction. The exposed nitrogen cation sites with photo-enhanced Lewis acidity not only act as the electron-transfer motor to adjust the inherent charge distribution, powering continuous and stable charge separation, and broadening visible-light adsorption, but also providing a large number of active sites for O2 adsorption. The optimal catalyst shows a high H2O2 production rate of 11965 μmol g−1 h−1 under visible light irradiation and a remarkable apparent quantum yield of 12.9 % at 400 nm, better than most of the previously reported COF photocatalysts. This work provides new insights for designing photo-switchable nitrogen cation sites as catalytic centers toward efficient solar to chemical energy conversion. |
