Asymmetric Synthesis of Vicinal Tetrasubstituted Diamines via Reductive Coupling of Ketimines Templated by Chiral Diborons.

Asymmetric Homocoupling Asymmetric α-Bromination Chiral Diborons Chiral Tetrasubstituted Diamines Halogen Bonding

Journal

Angewandte Chemie (International ed. in English)
ISSN: 1521-3773
Titre abrégé: Angew Chem Int Ed Engl
Pays: Germany
ID NLM: 0370543

Informations de publication

Date de publication:
17 Apr 2023
Historique:
received: 09 01 2023
medline: 2 3 2023
pubmed: 2 3 2023
entrez: 1 3 2023
Statut: ppublish

Résumé

We herein describe the chiral diboron-templated asymmetric homocoupling of aryl alkyl ketimines, providing for the first time a series of chiral vicinal tetrasubstituted diamines with excellent ee values and good to high yields. The powerful and efficient diboron-participated [3,3]-sigmatropic rearrangement is successfully demonstrated by the homocoupling of a variety of ketimines thanks to the rational design and engineering of chiral diborons. Systematic DFT studies suggest that two chiral diborons adopt different conformational assembling strategies to couple the diboron template with ketimine substrates in their tight concerted transition states to ensure the excellent enantioselectivities. The synthetic value of chiral vicinal tetrasubstituted diamines is demonstrated by the asymmetric α-bromination of aliphatic aldehydes by employing a chiral vicinal tetrasubstituted diamine-based organocatalyst.

Identifiants

pubmed: 36859620
doi: 10.1002/anie.202300334
doi:

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

e202300334

Subventions

Organisme : National Key R&D Program of China
ID : 2022YFA1503702
Organisme : National Key R&D Program of China
ID : 2021YFF0701601
Organisme : National Natural Science Foundation of China
ID : 82188101
Organisme : National Natural Science Foundation of China
ID : 21725205
Organisme : National Natural Science Foundation of China
ID : 21432007
Organisme : National Natural Science Foundation of China
ID : 22071261
Organisme : National Natural Science Foundation of China
ID : 21572246
Organisme : National Natural Science Foundation of China
ID : 21702223
Organisme : National Natural Science Foundation of China
ID : 21933003
Organisme : National Natural Science Foundation of China
ID : 22193020
Organisme : National Natural Science Foundation of China
ID : 22193023
Organisme : Shenzhen Nobel Prize Scientists Laboratory Project
ID : C17783101
Organisme : Guangdong Provincial Key Laboratory of Catalytic Chemistry
ID : 2020B121201002
Organisme : Youth Innovation Promotion Association

Informations de copyright

© 2023 Wiley-VCH GmbH.

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Auteurs

Mingkang Zhou (M)

State Key Laboratory of Bio-Organic and Natural Products Chemistry, Shanghai Institute of Organic Chemistry, University of Chinese Academy of Sciences, 345 Ling Ling Road, Shanghai, 200032, China.

Yaodong Lin (Y)

State Key Laboratory of Bio-Organic and Natural Products Chemistry, Shanghai Institute of Organic Chemistry, University of Chinese Academy of Sciences, 345 Ling Ling Road, Shanghai, 200032, China.

Xiao-Xuan Chen (XX)

Shenzhen Grubbs Institute, Department of Chemistry and Guangdong Provincial Key Laboratory of Catalysis, Southern University of Science and Technology, Shenzhen, 518055, China.

Guangqing Xu (G)

State Key Laboratory of Bio-Organic and Natural Products Chemistry, Shanghai Institute of Organic Chemistry, University of Chinese Academy of Sciences, 345 Ling Ling Road, Shanghai, 200032, China.

Lung Wa Chung (LW)

Shenzhen Grubbs Institute, Department of Chemistry and Guangdong Provincial Key Laboratory of Catalysis, Southern University of Science and Technology, Shenzhen, 518055, China.

Wenjun Tang (W)

State Key Laboratory of Bio-Organic and Natural Products Chemistry, Shanghai Institute of Organic Chemistry, University of Chinese Academy of Sciences, 345 Ling Ling Road, Shanghai, 200032, China.
School of Chemistry and Materials Science, Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences, 1 Sub-lane Xiangshan, Hangzhou, 310024, China.

Classifications MeSH