科研之友
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摘要
Generating FeIV=O on single‐atom catalysts by Fenton‐like reaction has been established for water treatment; however, the FeIV=O generation pathway and oxidation behavior remain obscure. Employing an Fe?N?C catalyst with a typical Fe?N4 moiety to activate peroxymonosulfate (PMS), we demonstrate that generating FeIV=O is mediated by an Fe?N?C?PMS* complex—a well‐recognized nonradical species for induction of electron‐transfer oxidation—and we determined that adjacent Fe sites with a specific Fe1?Fe1 distance are required. After the Fe atoms with an Fe1‐Fe1 distance 1‐Fe1 distance of 4–5?? can coordinate with the adjacent FeII?N4, forming an inter‐complex with enhanced charge transfer to produce FeIV=O. FeIV=O enables the Fenton‐like system to efficiently oxidize various pollutants in a substrate‐specific, pH‐tolerant, and sustainable manner, where its prominent contribution manifests for pollutants with higher one‐electron oxidation potential.(#br)Iron atoms with a Fe1‐Fe1 distance of 4?? are the real active sites for generating FeIV=O in Fenton‐like reactions, forming a complex through dual‐site adsorption of peroxymonosulfate (PMS) as the key step. The versatile FeIV=O species promotes the overall oxidizing capacity, pH tolerance, and stability of a Fenton‐like system for water treatment.
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