期刊
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
卷 -, 期 5, 页码 754-760出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/ejic.201500900
关键词
Ligand effects; N,P ligands; Iridium; Alkylation; Amines
资金
- Japanese Ministry of Education, Culture, Sports, Science and Technology (MEXT) [24109010]
- KAKENHI from Japan Society for the Promotion of Science (JSPS) [26288050]
- Grants-in-Aid for Scientific Research [26288050, 24109010] Funding Source: KAKEN
A series of Ir-I complexes [Ir(L)(PPEP*)] [L = Cl- (3), CO (4), tBuNC (5), PMe3 (6), PPh3 (7)], coordinated with a PNP-pincer-type phosphaalkene ligand bearing a dearomatized pyridine ring (PPEP*), have been prepared and their catalytic properties for the dehydration/condensation of amines with alcohols has been examined. The catalytic reactions successfully proceed under base-free conditions to give N-alkylated amines and their dehydrogenation derivatives (imines). The product selectivity is dependent on L coordinated with Ir(PPEP*). Complexes 4 and 5 that contain p-accepting ligands (CO, tBuNC) form N-alkylated amines as the major products in a closed system using a nitrogen-gas-filled Schlenk tube. In contrast, complex 7 that contain PPh3 as L produces imines as the major products under a nitrogen-gas flow. The reason for the selectivity change depending on L is discussed based on stoichiometric reactions using model compounds of presumed catalytic intermediates.
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