Thiophene-Containing Covalent Organic Frameworks for Overall Photocatalytic H2O2 Synthesis in Water and Seawater |
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Authors: | Dr Jie-Yu Yue Li-Ping Song Yan-Fei Fan Zi-Xian Pan Dr Peng Yang Dr Yu Ma Dr Qing Xu Dr Bo Tang |
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Institution: | 1. College of Chemistry, Chemical Engineering and Materials Science, Collaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of Shandong, Key Laboratory of Molecular and Nano Probes, Ministry of Education, Institutes of Biomedical Sciences, Shandong Normal University, 250014 Jinan, P. R. China;2. College of Chemistry, Chemical Engineering and Materials Science, Collaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of Shandong, Key Laboratory of Molecular and Nano Probes, Ministry of Education, Institutes of Biomedical Sciences, Shandong Normal University, 250014 Jinan, P. R. China
These authors contributed equally to this work.;3. CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute (SARI), Chinese Academy of Sciences (CAS), 201210 Shanghai, P. R. China |
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Abstract: | H2O2 is a significant chemical widely utilized in the environmental and industrial fields, with growing global demand. Without sacrificial agents, simultaneous photocatalyzed H2O2 synthesis through the oxygen reduction reaction (ORR) and water oxidation reaction (WOR) dual channels from seawater is green and sustainable but still challenging. Herein, two novel thiophene-containing covalent organic frameworks (TD-COF and TT-COF) were first constructed and served as catalysts for H2O2 synthesis via indirect 2e− ORR and direct 2e− WOR channels. The photocatalytic H2O2 production performance can be regulated by adjusting the N-heterocycle modules (pyridine and triazine) in COFs. Notably, with no sacrificial agents, just using air and water as raw materials, TD-COF exhibited high H2O2 production yields of 4060 μmol h−1 g−1 and 3364 μmol h−1 g−1 in deionized water and natural seawater, respectively. Further computational mechanism studies revealed that the thiophene was the primary photoreduction unit for ORR, while the benzene ring (linked to the thiophene by the imine bond) was the central photooxidation unit for WOR. The current work exploits thiophene-containing COFs for overall photocatalytic H2O2 synthesis via ORR and WOR dual channels and provides fresh insight into creating innovative catalysts for photocatalyzing H2O2 synthesis. |
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Keywords: | H2O2 Oxygen Reduction Reaction Photocatalysis Thiophene Units Water Oxidation Reaction |
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