Single-atom Mn-N4 Sites Catalyzed Peroxone Reaction for Efficient Production of Hydroxyl Radicals under Acidic Solution.
Guo Z , Xie Y , Xiao J , Zhao ZJ , Wang Y , Xu Z , Zhang Y , Yin L , Cao H , Gong J
Journal of the American Chemical Society
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 super-active hydroxyl radicals (•OH), but it suffers greatly from extremely limited reaction rate con-stant under acidic conditions (ca. less than 0.1 M-1s-1 at pH 3). This paper describes a heterogeneous catalyst comprised of single Mn atoms anchored on graphitic carbon nitride, which effectively overcome such the 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 activation of H2O2 is found, which gets rid of the restriction of HO2- as the essential initiator in conventional peroxone reaction. This work offer 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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