Single Metal Atoms Anchored on N‐Doped Holey Graphene as Efficient Dual‐Active‐Component Catalysts for Nitroarene Reduction

Abstract

AbstractDeveloping efficient catalysts for facilitating organic synthesis processes is a popular but challenging topic in modern chemical industries. A combination of active metals and an active support structure is, in theory, an effective strategy for boosting catalytic activity but such combinations have been rarely explored. Herein, a strategy for fabricating highly efficient dual‐active‐component catalysts (DACCs) is presented by anchoring single‐atom metals (M1; e.g., Pd1, Ni1, Co1, and Zn1) or double‐atomic metals (e.g., Pd1‐Co1, Pd1‐Ru1, and Pd1‐Ni1) on nitrogen‐doped holey graphene (NHG). Among the resultant DACCs, Pd1/NHG, which combines atomically dispersed metal species and an active NHG carbocatalyst, has been shown to display enhanced catalytic performance toward nitroarene reduction . In particular, its catalytic efficiency in reducing 4‐nitrophenol corresponds to a turnover frequency of 2.0 min−1, which is 97 times higher than the benchmark set by commercial Pd/C catalysts (5.0 wt.%), and vastly superior to those of its counterparts (e.g., NHG carbocatalyst and NHG supported Pd clusters. Notably, four intermediates and two active components (i.e., NHG and single‐atom Pd) in the nitroarene reduction process have been identified. This study presents an effective and versatile synthetic strategy to prepare DACCs through the combination of metallic catalysts and a carbocatalyst substrate.