Sulfone-Modified Covalent Organic Frameworks Enabling Efficient Photocatalytic Hydrogen Peroxide Generation via One-Step Two-Electron O2 Reduction |
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| Authors: | Yu Luo Beiping Zhang Chenchen Liu Prof. Dehua Xia Dr. Xinwen Ou Yanpeng Cai Prof. Yang Zhou Prof. Jin Jiang Prof. Bin Han |
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| Affiliation: | 1. Key Laboratory for City Cluster Environmental Safety and Green Development of the Ministry of Education, School of Ecology, Environment and Resources, Guangdong University of Technology, Guangzhou, 510006 P. R. China;2. School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou, 510275 P. R. China;3. School of Physics, Zhejiang University, Zheda Road 38, Hangzhou, 310027 P. R. China |
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| Abstract: | Photocatalytic oxygen reduction reaction (ORR) offers a promising hydrogen peroxide (H2O2) synthetic strategy, especially the one-step two-electron (2e−) ORR route holds great potential in achieving highly efficient and selectivity. However, efficient one-step 2e− ORR is rarely harvested and the underlying mechanism for regulating the ORR pathways remains greatly obscure. Here, by loading sulfone units into covalent organic frameworks (FS-COFs), we present an efficient photocatalyst for H2O2 generation via one-step 2e− ORR from pure water and air. Under visible light irradiation, FS-COFs exert a superb H2O2 yield of 3904.2 μmol h−1 g−1, outperforming most reported metal-free catalysts under similar conditions. Experimental and theoretical investigation reveals that the sulfone units accelerate the separation of photoinduced electron-hole (e−-h+) pairs, enhance the protonation of COFs, and promote O2 adsorption in the Yeager-type, which jointly alters the reaction process from two-step 2e− ORR to the one-step one, thereby achieving efficient H2O2 generation with high selectivity. |
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| Keywords: | COFs H2O2 Generation Oxygen Reduction Reaction Photosynthesis Sulfone Units |
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