Atomic‐Layered Cu 5 Nanoclusters on FeS 2 with Dual Catalytic Sites for Efficient and Selective H 2 O 2 Activation

Abstract Regulating the distribution of reactive oxygen species generated from H 2 O 2 activation is the prerequisite to ensuring the efficient and safe use of H 2 O 2 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 Cu 5 nanoclusters onto a FeS 2 surface achieves selective H 2 O 2 activation with high efficiency. Unlike its unitary Cu or Fe counterpart, the dual Cu−Fe sites residing at the perimeter zone of the Cu 5 /FeS 2 interface facilitate H 2 O 2 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 H 2 O 2 activation on the surface molecular level towards efficient environmental control and beyond.