Single-Atom Mn–N₄ Site-Catalyzed Peroxone Reaction for the Efficient Production of Hydroxyl Radicals in an Acidic Solution

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Abstract

The peroxone reaction between O₃ and H₂O₂ has been deemed a promising technology to resolve the increasingly serious water pollution problem by virtue of the generation of superactive hydroxyl radicals (•OH), but it suffers greatly from an extremely limited reaction rate constant under acidic conditions (ca. less than 0.1 M-1 s-1 at pH 3). This article describes a heterogeneous catalyst composed of single Mn atoms anchored on graphitic carbon nitride, which effectively overcomes such a drawback by altering the reaction pathway and thus dramatically promotes •OH generation in acid solution. Combined experimental and theoretical studies demonstrate Mn-N₄ as the catalytically active sites. A distinctive catalytic pathway involving HO₂• formation by the activation of H₂O₂ is found, which gets rid of the restriction of HO₂- as the essential initiator in the conventional peroxone reaction. This work offers a new pathway of using a low-cost and easily accessible single-atom catalyst (SAC) and could inspire more catalytic oxidation strategies.

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