Journal
JOURNAL OF CATALYSIS
Volume 342, Issue -, Pages 151-157Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2016.07.021
Keywords
Pd nanoparticles; MIL-100(Fe); Double-solvent impregnation; Multifunctional catalyst; Light-induced N-alkylation reaction
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Funding
- 973 Program [2014CB239303]
- NSFC [21273035]
- Specialized Research Fund for the Doctoral Program of Higher Education [20123514110002]
- Independent Research Project of State Key Laboratory of Photo catalysis on Energy and Environment [2014A03]
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Pd nanoparticles with an average size of 1.7 nm confined inside a MIL-100(Fe) cavity (Pd@MIL-100(Fe)) were prepared via double-solvent impregnation combined with a photoreduction process. Due to efficient coupling of photocatalytic dehydrogenation and Pd-based hydrogenation, the resultant Pd@MIL-100(Fe) showed significantly superior performance in light-induced N-alkylation of amines with alcohols over Pd/MIL-100(Fe), in which larger Pd nanoparticles (6-12 nm) deposited on the external surface of MIL-100(Fe) were prepared via a conventional single-solvent impregnation followed by a similar photoreduction process. Kinetic studies and controlled experiments revealed that the whole N-alkylation reaction is limited by the photocatalytic alcohol-to-aldehyde dehydrogenation reaction. This is the first demonstration of light-induced N-alkylation of amines by alcohols over M/MOFs nanocomposites and also highlights the great potential of using M/MOFs nanocomposites as multifunctional catalysts for light-induced organic syntheses. (C) 2016 Elsevier Inc. All rights reserved.
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