Abstract Generally, the sulfate (SO 4 · − ) and hydroxyl (HO · ) radicals are the dominant active species in most catalytic oxidation processes with peroxymonosulfate (PMS). However, the existence of various natural organic and inorganic matters in aquatic environments might influence the oxidation efficiency of these radicals, and/or form more toxic and refractory intermediates than the parent, especially in chlorine-ion-containing conditions. Here, we constructed a novel visible-light catalytic system with PMS based on iron hexadecachlorophthalocyanine-poly (4-vinylpyridine)/polyacrylonitrile nanofibers through pyridine ligands to generate high-valent iron-oxo (Fe(IV)=O) species as the main active species. The coordination structure was characterized by UV–Vis diffuse reflection, X-ray photoelectron spectroscopy, etc. The high-valent iron-oxo generation from peroxysulfate O–O bond heterolytic cleavage was proved by high-definition electrospray ionization mass spectrometer. Ultra-performance liquid chromatography coupled with high-definition mass spectrometry showed that the photocatalytic system was efficient for the degradation of carbamazepine and the chlorinated intermediates by iron-oxo active species in chlorine-ion-containing conditions. Graphic Abstract

中文翻译：

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高价铁氧配合物作为主要物种通过在可见光照射下活化过硫酸盐来消除药物和含氯中间体

摘要 一般而言，硫酸盐(SO 4 · - ) 和羟基(HO · ) 自由基是大多数过氧单硫酸盐(PMS) 催化氧化过程中的主要活性物质。然而，水生环境中各种天然有机和无机物质的存在可能会影响这些自由基的氧化效率，和/或形成比母体更具毒性和难降解的中间体，尤其是在含氯离子的条件下。在这里，我们通过吡啶配体构建了一种基于十六氯酞菁铁-聚（4-乙烯基吡啶）/聚丙烯腈纳米纤维的新型可见光催化体系，以生成高价铁氧（Fe（IV）= O）物种为主要活性种。通过紫外-可见漫反射、X射线光电子能谱等表征配位结构。高清晰度电喷雾电离质谱仪证明了由过硫酸盐 O-O 键异裂裂解产生的高价铁氧。超高效液相色谱结合高清质谱表明，该光催化体系在含氯离子条件下可有效降解卡马西平和铁氧活性物质的氯化中间体。图形摘要