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Introduction of a 7-aza-6-MeO-indoline auxiliary in Lewis-acid/photoredox cooperative catalysis: highly enantioselective aminomethylation of α,ß-unsaturated amides.
Pagire, Santosh K; Kumagai, Naoya; Shibasaki, Masakatsu.
Afiliación
  • Pagire SK; Institute of Microbial Chemistry (BIKAKEN) 3-14-23, Kamiosaki Shinagawa-ku Tokyo 141-0021 Japan mshibasa@bikaken.or.jp nkumagai@bikaken.or.jp.
  • Kumagai N; Institute of Microbial Chemistry (BIKAKEN) 3-14-23, Kamiosaki Shinagawa-ku Tokyo 141-0021 Japan mshibasa@bikaken.or.jp nkumagai@bikaken.or.jp.
  • Shibasaki M; Institute of Microbial Chemistry (BIKAKEN) 3-14-23, Kamiosaki Shinagawa-ku Tokyo 141-0021 Japan mshibasa@bikaken.or.jp nkumagai@bikaken.or.jp.
Chem Sci ; 11(20): 5168-5174, 2020 Apr 27.
Article en En | MEDLINE | ID: mdl-34122973
An efficient cooperative chiral Lewis acid/photoredox catalytic system for engaging highly reactive radicals in highly enantioselective conjugate addition to α,ß-unsaturated carbonyls is highly desirable. Direct photoexcitation of unbound substrates typically induces undesired background pathways for racemic products and remains a formidable challenge to be addressed in the area of enantioselective photocatalysis. Herein, we report a cooperative catalytic system comprising a chiral Cu(i) complex and an Ir(iii) photocatalyst fueled by visible-light irradiation that allows for seamless integration of the catalytic formation of α-amino alkyl radicals and subsequent enantioselective addition to α,ß-unsaturated amides. A 7-aza-6-MeO-indoline attachment on the amide substrates plays a pivotal role in suppressing the undesired pathways, resulting in excellent enantioselectivity and enabling expedited access to valuable γ-aminobutyramides. The indoline amide was readily diversified with full recovery of the azaindoline attachment, highlighting the synthetic utility of this cooperative catalytic system.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Chem Sci Año: 2020 Tipo del documento: Article Pais de publicación: Reino Unido

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Chem Sci Año: 2020 Tipo del documento: Article Pais de publicación: Reino Unido