Interlayer synergistic reaction of radical precursors for ultraefficient 1O2 generation via quinone- based covalent organic framework
成果类型：
Article
署名作者：
Tao, Yuan; Hou, Yu; Yang, Huangsheng; Gong, Zeyu; Yu, Jiaxing; Zhong, Huajie; Fu, Qi; Wang, Junhui; Zhu, Fang; Ouyang, Gangfeng
署名单位：
Southern Marine Science & Engineering Guangdong Laboratory; Southern Marine Science & Engineering Guangdong Laboratory (Zhuhai); Sun Yat Sen University; Sun Yat Sen University; Zhengzhou University; Chinese Academy of Sciences; Guangdong Academy of Sciences; Institute of Analysis, Guangdong Academy of Sciences
刊物名称：
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
ISSN/ISSBN：
0027-9505
DOI：
10.1073/pnas.2401175121
发表日期：
2024-09-17
关键词：
activation
peroxymonosulfate
degradation
persulfate
摘要：
Singlet oxygen (1O2) is important in the environmental remediation field, however, its efficient production has been severely hindered by the ultrafast self- quenching of the as- generated radical precursors in the Fenton- like reactions. Herein, we elaborately designed lamellar anthraquinone- based covalent organic frameworks (DAQ- COF) with sequential localization of the active sites (C=O) at molecular levels for visible- light- assisted peroxymonosulfate (PMS) activation. Theoretical and experimental results revealed that the radical precursors (SO5-) were formed in the nearby layers with the migration distance less than 0.34 nm, via PMS donating electrons to the photogenerated holes. This interlayer synergistic effect eventually led to ultraefficient 1O2 production (14.8 mu M s-1), which is 12 times that of the highest reported catalyst. As an outcome, DAQ- COF enabled the complete degradation of bisphenol A in 5 min with PMS under natural sunlight irradiation. This interlayer synergistic concept represents an innovative and effective strategy to increase the utilization efficiency of ultrashort- lived radical precursors, providing inspirations for subtle structural construction of Fenton- like catalysts.