Singlet oxygen ( 1 O 2 ) 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 (SO 5 ·− ) 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 1 O 2 production (14.8 μM 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.

中文翻译：

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自由基前驱体的层间协同反应通过醌基共价有机骨架实现超高效 1 O 2 生成


单线态氧( 1 O 2 )在环境修复领域很重要，然而，类芬顿反应中生成的自由基前体的超快自猝灭严重阻碍了其高效生产。在此，我们精心设计了基于蒽醌的层状共价有机框架（DAQ-COF），其活性位点（C=O）在分子水平上顺序定位，用于可见光辅助的过一硫酸盐（PMS）活化。理论和实验结果表明，通过PMS向光生空穴提供电子，自由基前驱体(SO 5·− )在附近层中形成，迁移距离小于0.34 nm。这种层间协同效应最终导致超高效的 1 O 2 生产（14.8 μM s -1 ），是报道的最高催化剂的 12 倍。结果，DAQ-COF 能够在自然阳光照射下使用 PMS 在 5 分钟内完全降解双酚 A。这种层间协同概念代表了一种创新且有效的策略，可以提高超短寿命自由基前驱体的利用效率，为类芬顿催化剂的精细结构构建提供灵感。