Synthesis and Characterization of Iron-Nitrogen-Doped Graphene/Core-Shell Catalysts: Efficient Oxidative Dehydrogenation of N-Heterocycles

被引:281
作者
Cui, Xinjiang [1 ]
Li, Yuehui [1 ]
Bachmann, Stephan [2 ]
Scalone, Michelangelo [2 ]
Surkus, Annette-Enrica [1 ]
Junge, Kathrin [1 ]
Topf, Christoph [1 ]
Beller, Matthias [1 ]
机构
[1] Univ Rostock, Leibniz Inst Katalyse eV, D-18059 Rostock, Germany
[2] F Hoffmann La Roche Ltd, Proc Res & Dev, CH-4070 Basel, Switzerland
关键词
COBALT OXIDE CATALYSTS; CORE-SHELL; AEROBIC OXIDATION; SELECTIVE OXIDATION; ACCEPTORLESS DEHYDROGENATION; HYDROGEN STORAGE; SECONDARY-AMINES; NANOPARTICLES; REDUCTION; COMPOSITE;
D O I
10.1021/jacs.5b05674
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
An important goal for nanocatalysis is the development of flexible and efficient methods for preparing active and stable core-shell catalysts. In this respect, we present the synthesis and characterization of iron oxides surrounded by nitrogen-doped-graphene shells immobilized on carbon support (labeled FeOx@NGr-C). Active catalytic materials are obtained in a simple, scalable and two-step method via pyrolysis of iron acetate and phenanthroline and subsequent selective leaching. The optimized FeOx@NGr-C catalyst showed high activity in oxidative dehydrogenations of several N-heterocycles. The utility of this benign methodology is demonstrated by the synthesis of pharmaceutically relevant quinolines. In addition, mechanistic studies prove that the reaction progresses via superoxide radical anions (center dot O-2(-)).
引用
收藏
页码:10652 / 10658
页数:7
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