期刊
ACS CATALYSIS
卷 4, 期 11, 页码 3994-4003出版社
AMER CHEMICAL SOC
DOI: 10.1021/cs5009656
关键词
iron; catalysis; acceptorless dehydrogenation; hydrogenation; metal-ligand; cooperativity
资金
- Center for Electrocatalysis, Transport Phenomena, and Materials (CETM) for Innovative Energy Storage, an Energy Frontier Research Center - U.S. Department of Energy
- ESD NYSTAR program
- COST Action [1205]
- Alexander von Humboldt Foundation
- National Science Foundation through the Center for the Capture and Conversion of CO2 [CHE-1240020]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1240020] Funding Source: National Science Foundation
Acceptorless dehydrogenation of alcohols, an important organic transformation, was accomplished with well-defined and inexpensive iron-based catalysts supported by a cooperating PNP pincer ligand. Benzylic and aliphatic secondary alcohols were dehydrogenated to the corresponding ketones in good isolated yields upon release of dihydrogen. Primary alcohols were dehydrogenated to esters and lactones, respectively. Mixed primary/secondary diols were oxidized at the secondary alcohol moiety with good chemoselectivity. The mechanism of the reaction was investigated using both experiment and DFT calculations, and the crucial role of metalligand cooperativity in the reaction was elucidated. The iron complexes are also excellent catalysts for the hydrogenation of challenging ketone substrates at ambient temperature under mild H-2 pressure, the reverse of secondary alcohol dehydrogenation.
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