烯胺
光催化
共价键
催化作用
制氢
合理设计
化学工程
氢
量子效率
带隙
吸收(声学)
光化学
化学
组合化学
纳米技术
材料科学
有机化学
复合材料
光电子学
工程类
作者
Liying Yin,Yaohua Zhao,Yanmei Xing,Huaqiao Tan,Zhongling Lang,Wingkei Ho,Yonghui Wang,Yangguang Li
标识
DOI:10.1016/j.cej.2021.129984
摘要
Covalent organic frameworks (COFs), as new promising photocatalysts, have aroused great interests, but the systematic study on the structure–property relationship of COF-photocatalysts is scarcely reported. Herein, six β-keto-enamine-based COFs with different backbones and substituents have been prepared. Through systematic experiments and DFT calculation, the structure–property relationships of the composition, structure and substituents of COFs on their spectra, specific surface area, hydrophobicity, electronic structures, carrier separation and photocatalytic hydrogen production have been studied. We explore that the backbone of COFs has important influence on their band gap, spectral absorption and carrier separation. While the substituents affect the band positions, surface area and hydrophobicity of COFs. Comprehensively, TpPa-Cl2 (constructed by 1,3,5-triformylphloroglucinol and 2,5-dichloro-1,4-phenylenediamine) exhibits the best area-normalised photocatalytic performance for hydrogen production, which is about 11.73 µmol·m−2·h−1 (0.01 g catalysts) with apparent quantum efficiency of 17% at 400 nm. This work provides a new perspective for the rational design and construction of efficient COF-photocatalysts.
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