小提琴手
光化学
阳离子聚合
光催化
化学
Knoevenagel冷凝
单体
离子液体
高分子化学
聚合物
催化作用
有机化学
作者
Zixuan Xu,Ke Liu,Shijie Wang,Yanan Chang,Juan Chen,Shuo Wang,Chaoran Meng,Zhouyang Long,Qin Zheng-long,Guojian Chen
出处
期刊:ACS applied polymer materials
[American Chemical Society]
日期:2023-12-29
标识
DOI:10.1021/acsapm.3c02311
摘要
Rational design of radical porous organic polymers with redox functions for metal-free heterogeneous photocatalysis is a promising research topic. In this work, we reported a class of viologen-based cationic radical porous organic polymers (VCR-POPs), which were facilely constructed by the one-pot Knoevenagel condensation reaction between 1,3,5-tris(p-formylphenyl)benzene and an acetonitrile-functionalized viologen-based ionic monomer (VIL-CN). Interestingly, the stable viologen cationic radical was found in the obtained VCR-POPs, probably undergoing in situ single-electron reduction of the dicationic monomer VIL-CN during the base catalyst Cs2CO3-involved Knoevenagel condensation reaction. The radical character of the typical porous organic polymer VCR-POP-1 was confirmed by the electron paramagnetic resonance spectrum and X-ray photoelectron spectroscopy, and the chemical structures and porous textural properties were fully characterized. The optical and electrochemical properties of VCR-POP-1 manifest the semiconductor nature, excellent light-harvesting ability, and better charge separation and transfer efficiency of this well-designed cationic radical polymer compared with the ionic monomer VIL-CN. Therefore, the polymer VCR-POP-1 with viologen-based cationic radicals and π-conjugated structures could be regarded as a highly efficient metal-free heterogeneous photocatalyst for visible-light-driven oxidative coupling of amines in air by virtue of the dominant reactive oxygen species of singlet oxygen.
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