Journal
TOPICS IN CATALYSIS
Volume 53, Issue 13-14, Pages 915-923Publisher
SPRINGER/PLENUM PUBLISHERS
DOI: 10.1007/s11244-010-9523-7
Keywords
Pincer complexes; Metal-ligand cooperation; Acohols; Amines; Amides; Imines; Dehydrogenative coupling; Hydrogen; Ruthenium; Iridium; Catalysis; O-H activation; C-H activation; PNP; PNN
Categories
Funding
- Israel Science Foundation
- DIP Program
- Helen and Martin Kimmel Center for Molecular Design
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We have developed a new mode of metal-ligand cooperation, based on aromatization-dearomatization of pyridine-based pincer-type ligands, and have demonstrated it in the activation of H-2 and C-H bonds by PNP Ir complexes. This type of metal-ligand cooperation plays a key role in the recently discovered environmentally benign reactions of alcohols, catalyzed by PNP and PNN pincer complexes of ruthenium, including (a) dehydrogenation of secondary alcohols to ketones (b) dehydrogenative coupling of primary alcohols to form esters and H-2 (c) hydrogenation of esters to alcohols under mild conditions (d) unprecedented amide synthesis: catalytic coupling of amines with alcohols, with liberation of H-2. Ligand modification in the latter reaction has led to unprecedented synthesis of imines with H-2 liberation. These reactions are very efficient, proceed under neutral conditions and produce no waste.
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