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Three-dimensional electro-Fenton oxidation of N-heterocyclic compounds with a novel catalytic particle electrode: high activity, wide pH range and?catalytic mechanism

机译:具有新型催化粒子电极的N-杂环化合物的三维Fenton电氧化:高活性,宽pH范围和催化机理

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A novel three-dimensional (3D) heterogeneous electro-Fenton (EF) system with sludge deserved activated carbon from sewage and iron sludge (SAC-Fe) as catalytic particle electrodes (CPEs) was constructed in this study. Its application in degrading nitrogen-heterocyclic compounds (NHCs) exhibited high catalytic efficiency over a wide applicable pH range from 3.0 to 9.0. SAC-Fe worked as both CPEs and a heterogeneous catalyst in this 3D EF system, enhancing oxidation activity. Degradation pathways of the NHCs (indole, quinoline and pyridine) and reasonable reaction mechanisms involved in this 3D EF were proposed. At pH 3.0, hydroxyl radicals were the dominant participant oxidants, following a Haber–Weiss mechanism. The FeII sites catalyzed the decomposition of electro-generated H2O2 to yield ˙OH. At pH 9.0, the oxidants generated from the decomposition of H2O2 were mainly ˙O2?/HO2˙ and to lesser extent were ˙OH. The formation and decomposition of H2O2 complex with catalytic sites (FeII and FeIII) as well as the catalytic decomposition of H2O2 were involved in the catalytic reactions to generate ˙O2?/HO2˙ and ˙OH. A quantitative structure–activity relationship analysis (QSAR) model was developed to describe the relationship between degradation properties of NHCs and their structures by involving quantum descriptors.
机译:本研究构建了一种新颖的三维(3D)异质电Fenton(EF)系统,该系统以污泥中应得的污水和铁污泥(SAC-Fe)中的活性炭为催化颗粒电极(CPE)。它在降解氮杂环化合物(NHCs)中的应用在3.0至9.0的广泛适用pH范围内均显示出高催化效率。 SAC-Fe在此3D EF系统中既充当CPE,又充当非均相催化剂,从而增强了氧化活性。提出了该3D EF涉及的NHC(吲哚,喹啉和吡啶)的降解途径和合理的反应机理。在pH 3.0时,遵循Haber-Weiss机制,羟基自由基是主要的参与氧化剂。 Fe II 位点催化电生成的H 2 O 2 < / sub> 生成OH。在pH 9.0时,H 2 O 2 分解产生的氧化剂主要为˙O 2 / HO 2 ˙,程度较小哦。 H 2 O 2 具有催化位点的配合物(Fe II 和Fe III )以及H 2 O的催化分解 2 参与催化反应生成˙O 2 / HO 2 ˙和˙OH。建立了定量构效关系分析(QSAR)模型,通过涉及量子描述符来描述NHC的降解特性与其结构之间的关系。

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