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<p>Chemical warfare agents (CWAs) pose great threats to human life and require efficient remediation methods. Photocatalytic degradation by covalent-organic frameworks (COFs) provides an environmentally friendly disposal method for CWAs, but it is challenging to precisely regulate the electronic effects of COFs to enhance their photocatalytic degradation performance. Here, a series of phenylquinoline-based COFs were constructed via a one-pot, three-component self-assembly strategy using 1,3,5-tris(<i>p</i>-formylphenyl)benzene (TFPB), 1,3,5-tris(4-aminophenyl)benzene (TAPB), and phenylacetylene as building blocks. Functionalizing the phenylquinoline group at the <i>para</i> (<i>p</i>) position using −OCH<sub>3</sub>, −CH<sub>3</sub>, and −NO<sub>2</sub> regulated the electron distribution of the resulting COFs. The experimental results showed that the phenylquinoline-based COF with −OCH<sub>3</sub> group, TFPB-TAPB-<i>p</i>-OCH<sub>3</sub>-QL, in the oxidation of mustard gas simulant 2-chloroethyl ethyl sulfide under visible light demonstrated the best photocatalytic performance, followed by TFPB-TAPB-<i>p</i>-CH<sub>3</sub>-QL, while TFPB-TAPB-<i>p</i>-NO<sub>2</sub>-QL did not react. Theoretical calculations indicated that TFPB-TAPB-<i>p</i>-OCH<sub>3</sub>-QL with an electron-donating substituent had the smallest positive conduction band minimum of 0.24 eV and a moderate band gap. Excited electrons readily transferred to O<sub>2</sub> to form <sup>1</sup>O<sub>2</sub>, leading to superior photocatalytic oxidation activity. This study offers a new method to control the electronic effects and photocatalytic activity of COFs, providing a reference for improving COF-based photocatalysts for the decomposition of toxic chemicals.</p>

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Regulating the electronic effects of phenylquinoline-functionalized COFs for effective photocatalytic destruction of chemical warfare agent simulants

  • 期刊论文

  • 发表日期：

    2025年9月25日

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  • Tianhang Huang,
  • Kun Yuan,
  • Shuwen Li,
  • Shuai Han,
  • Yong Yan,
  • Zhengping Dong

摘要

Chemical warfare agents (CWAs) pose great threats to human life and require efficient remediation methods. Photocatalytic degradation by covalent-organic frameworks (COFs) provides an environmentally friendly disposal method for CWAs, but it is challenging to precisely regulate the electronic effects of COFs to enhance their photocatalytic degradation performance. Here, a series of phenylquinoline-based COFs were constructed via a one-pot, three-component self-assembly strategy using 1,3,5-tris(p-formylphenyl)benzene (TFPB), 1,3,5-tris(4-aminophenyl)benzene (TAPB), and phenylacetylene as building blocks. Functionalizing the phenylquinoline group at the para (p) position using −OCH3, −CH3, and −NO2 regulated the electron distribution of the resulting COFs. The experimental results showed that the phenylquinoline-based COF with −OCH3 group, TFPB-TAPB-p-OCH3-QL, in the oxidation of mustard gas simulant 2-chloroethyl ethyl sulfide under visible light demonstrated the best photocatalytic performance, followed by TFPB-TAPB-p-CH3-QL, while TFPB-TAPB-p-NO2-QL did not react. Theoretical calculations indicated that TFPB-TAPB-p-OCH3-QL with an electron-donating substituent had the smallest positive conduction band minimum of 0.24 eV and a moderate band gap. Excited electrons readily transferred to O2 to form 1O2, leading to superior photocatalytic oxidation activity. This study offers a new method to control the electronic effects and photocatalytic activity of COFs, providing a reference for improving COF-based photocatalysts for the decomposition of toxic chemicals.