Tailoring β-ketoenamine covalent organic framework with azo for blue light-driven selective oxidation of amines with oxygen
Journal of Colloid and Interface Science(2024)
摘要
Covalent organic frameworks (COFs) present bright prospects as visible light photocatalysis with abundant active sites and exceptional stability. Tailoring an established COF with a photoactive group is a prudent means to extend visible light absorption. Here, a β-ketoenamine COF, TpBD-COF, constructed with 1,3,5-triformylphloroglucinol (Tp) and 4,4′-biphenyldiamine (BD), is tailored with azo to validate this tactic. By the insertion of azo into BD, TpAzo-COF is successfully constructed with Tp and 4,4′-azodianiline (Azo). Intriguingly, the insertion of azo enhances π-conjugation, thereby facilitating visible light absorption and intramolecular electron transfer. Moreover, TpAzo-COF, characterized by an appropriate electronic structure and an impressive specific surface area of 1855 m2/g, offers substantial active sites conducive to the reduction of oxygen (O2) to superoxide. Compared with TpBD-COF, TpAzo-COF exhibits superior performance for the blue light-driven oxidation of amines with O2. Superoxide, the critical reactive oxygen species, controls the selective formation of product imines. This work foreshadows the remarkable capacity of tailoring COFs with a photoactive group toward broad visible light photocatalysis.
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关键词
Azo,Visible light,Covalent organic frameworks,Oxidation of amines,Photocatalysis
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