Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 137, Issue 14, Pages 4851-4859Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.5b01750
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Funding
- European Research Council (ERC) [246837]
- Israel Science Foundation
- Kimmel Center for Molecular Design
- Feinberg Graduated School
- DAAD
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The mechanism of the unique lactam formation from amines and water with concomitant H-2 liberation with no added oxidant, catalyzed by a well-defined acridine-based ruthenium pincer complex was investigated in detail by both experiment and DFT calculations. The results show that a dearomatized form of the initial complex is the active catalyst. Furthermore, reversible imine formation was shown to be part of the catalytic cycle. Water is not only the oxygen atom source but also acts as a cocatalyst for the H-2 liberation, enabled by conformational flexibility of the acridine-based pincer ligand.
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