Origin of the Excellent Activity and Selectivity of a Single-Atom Copper Catalyst with Unsaturated Cu-N₂ Sites via Peroxydisulfate Activation: Cu(III) as a Dominant Oxidizing Species

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Abstract

As an efficient active oxidant for the selective degradation of pollutants in wastewater, the high-valent copper species Cu(III) with persulfate activation has attracted substantial attention in some Cu-based catalysts. However, the systematic study of a catalyst structure and mechanism about Cu(III) with peroxydisulfate (PDS) activation is challenging owing to the coexistence of multiple Cu species and the structural symmetry of PDS. Herein, we anchored a Cu atom with two pyridinic N atoms to synthesize a single-atom Cu catalyst (Cu_SA-NC). Experimental characterizations and theoretical calculations complemented each other well because of the uniform atomic active sites. The single-atom Cu was identified as the active site, and the unsaturated Cu-N₂ configuration was more conductive to PDS activation than the saturated Cu-N₄ configuration. Benefiting from the generation of Cu(III), Cu_SA-NC exhibited an obvious selective and anti-interference performance for pollutant degradation in a complex matrix. The superior catalytic activity of Cu_SA-NC compared with that of other reported Cu-based catalysts and good durability in a continuous-flow experiment further revealed the potential of Cu_SA-NC for practical applications. This work strongly deepens the understanding of the generation of Cu(III) in a single-atom Cu catalyst with unsaturated Cu-N₂ sites under PDS activation and develops an efficient approach for actual water purification.

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