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Condensed ferric dimers for green photocatalytic synthesis of nylon precursors

机译:缩合铁二聚体用于绿色光催化合成尼龙前体

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摘要

Although iron oxides have been extensively studied as photocatalysts because of their abundance and environmental compatibility, their performance is notoriously low due to factors such as low photoinduced charge-separation efficiency. Iron oxides, thus, must be modified with expensive and/or toxic materials to attain higher performances, which devalues their appeal as sustainable materials. Here, we design an iron oxide exhibiting an unprecedentedly high photocatalytic performance unrealized by previous photocatalysts such as TiO2 for reactions including the selective oxidation of cyclohexane to industrial nylon precursors. The iron oxide photocatalyst consists of ferric dimers, otherwise extremely unstable, formed via etching of Fe and O sites from ferric oxide nanoparticles immobilized within porous silica. We demonstrate a remarkably high photoinduced charge-separation efficiency (long lifetime of active species) of the ferric dimers due to their electronic structure and the potential of this supported photocatalyst for many more reactions.
机译:尽管氧化铁由于其丰度和与环境的相容性而被广泛研究作为光催化剂,但是由于诸如低的光诱导电荷分离效率之类的因素,其性能仍然很差。因此,氧化铁必须用昂贵和/或有毒的材料改性才能获得更高的性能,这降低了它们作为可持续材料的吸引力。在这里,我们设计了一种氧化铁,该氧化铁具有前所未有的高光催化性能,而这种光催化性能是以前的光催化剂(如TiO2)无法实现的,该反应包括将环己烷选择性氧化为工业尼龙前体。氧化铁光催化剂由铁二聚体组成,否则极度不稳定,是通过固定化在多孔二氧化硅中的三氧化二铁纳米颗粒中的Fe和O位进行蚀刻而形成的。我们证明了由于三聚体的电子结构和这种负载型光催化剂的潜力,使其具有更多的反应,因此具有很高的光诱导电荷分离效率(活性物种的寿命长)。

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