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
Abstract
AbstractPhotocatalytic 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.
Subject
General Chemistry,Catalysis
Cited by
44 articles.
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