Affiliation:
1. School of Chemistry and Environmental Engineering Key Laboratory of Novel Biomass‐Based Environmental and Energy Materials in Petroleum and Chemical Industry Key Laboratory of Green Chemical Engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education Hubei Key Laboratory of Novel Reactor and Green Chemical Technology Wuhan Institute of Technology Wuhan 430073 P. R. China
2. State Key Laboratory of New Textile Materials & Advanced Processing Technologies Wuhan Textile University Wuhan 430200 P. R. China
3. DTU Nanolab. Technical University of Denmark Fysikvej, Building 307 Lyngby 2800 Kgs Denmark
4. Aramco Boston Research Center Cambridge MA 02139 USA
5. Nanyang Environment and Water Research Institute Nanyang Technological University 1 CleanTech Loop Singapore 637141 Singapore
6. School of Mechanical and Aerospace Engineering Nanyang Technological University 50 Nanyang Avenue Singapore 639798 Singapore
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.
Subject
Electrochemistry,Condensed Matter Physics,Biomaterials,Electronic, Optical and Magnetic Materials