TY - JOUR
T1 - Direct Catalytic Asymmetric Aldol Reaction of α-Alkoxyamides to α-Fluorinated Ketones
AU - Pluta, Roman
AU - Kumagai, Naoya
AU - Shibasaki, Masakatsu
N1 - Funding Information:
This work was financially supported by ACT-C (JPMJCR12YO) from JST and KAKENHI (17H03025 and JP16H01043 in Precisely Designed Catalysts with Customized Scaffolding) from the JSPS. R.P. thanks the JSPS for a Postdoctoral Fellowship. Dr. Ryuichi Sawa, Yumiko Kubota, Dr. Kiyoko Iijima, and Yuko Takahashi are gratefully acknowledged for their assistance with the spectroscopic analysis. We thank Dr. Tomoyuki Kimura for assistance with the X-ray crystallography.
Publisher Copyright:
© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
PY - 2019/2/18
Y1 - 2019/2/18
N2 - α-Oxygen-functionalized amides found particular utility as enolate surrogates for direct aldol couplings with α-fluorinated ketones in a catalytic manner. Because of the likely involvement of open transition states, both syn- and anti-aldol adducts can be accessed with high enantioselectivity by judicious choice of the chiral ligands. A broad variety of alkoxy substituents on the amides and aryl and fluoroalkyl groups on the ketone were tolerated, and the corresponding substrates delivered a range of enantioenriched fluorinated 1,2-dihydroxycarboxylic acid derivatives with divergent diastereoselectivity depending on the ligand used. The amide moiety of the aldol adduct was transformed into a variety of functional groups without protection of the tertiary alcohol, showcasing the synthetic utility of the present asymmetric aldol process.
AB - α-Oxygen-functionalized amides found particular utility as enolate surrogates for direct aldol couplings with α-fluorinated ketones in a catalytic manner. Because of the likely involvement of open transition states, both syn- and anti-aldol adducts can be accessed with high enantioselectivity by judicious choice of the chiral ligands. A broad variety of alkoxy substituents on the amides and aryl and fluoroalkyl groups on the ketone were tolerated, and the corresponding substrates delivered a range of enantioenriched fluorinated 1,2-dihydroxycarboxylic acid derivatives with divergent diastereoselectivity depending on the ligand used. The amide moiety of the aldol adduct was transformed into a variety of functional groups without protection of the tertiary alcohol, showcasing the synthetic utility of the present asymmetric aldol process.
KW - 7-azaindolines
KW - C−C bond formation
KW - aldol reaction
KW - asymmetric catalysis
KW - fluorine
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U2 - 10.1002/anie.201814607
DO - 10.1002/anie.201814607
M3 - Article
C2 - 30652398
AN - SCOPUS:85061051052
SN - 1433-7851
VL - 58
SP - 2459
EP - 2463
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 8
ER -