Atomic‐Layered Cu5 Nanoclusters on FeS2 with Dual Catalytic Sites for Efficient and Selective H2O2 Activation

Regulating the distribution of reactive oxygen species generated from H₂ O₂ activation is the prerequisite to ensuring the efficient and safe use of H₂ O₂ in the chemistry and life science fields. Herein, we demonstrate that constructing a dual Cu-Fe site through the self-assembly of single-atomic-layered Cu₅ nanoclusters onto a FeS₂ surface achieves selective H₂ O₂ activation with high efficiency. Unlike its unitary Cu or Fe counterpart, the dual Cu-Fe sites residing at the perimeter zone of the Cu₅ /FeS₂ interface facilitate H₂ O₂ adsorption and barrierless decomposition into ⋅OH via forming a bridging Cu-O-O-Fe complex. The robust in situ formation of ⋅OH governed by this atomic-layered catalyst enables the effective oxidation of several refractory toxic pollutants across a broad pH range, including alachlor, sulfadimidine, p-nitrobenzoic acid, p-chlorophenol, p-chloronitrobenzene. This work highlights the concept of building a dual catalytic site in manipulating selective H₂ O₂ activation on the surface molecular level towards efficient environmental control and beyond.