Electrochemically Driven, Ni-Catalyzed Aryl Amination: Scope, Mechanism, and Applications.


Journal

Journal of the American Chemical Society
ISSN: 1520-5126
Titre abrégé: J Am Chem Soc
Pays: United States
ID NLM: 7503056

Informations de publication

Date de publication:
17 04 2019
Historique:
pubmed: 25 3 2019
medline: 7 8 2020
entrez: 26 3 2019
Statut: ppublish

Résumé

C-N cross-coupling is one of the most valuable and widespread transformations in organic synthesis. Largely dominated by Pd- and Cu-based catalytic systems, it has proven to be a staple transformation for those in both academia and industry. The current study presents the development and mechanistic understanding of an electrochemically driven, Ni-catalyzed method for achieving this reaction of high strategic importance. Through a series of electrochemical, computational, kinetic, and empirical experiments, the key mechanistic features of this reaction have been unraveled, leading to a second generation set of conditions that is applicable to a broad range of aryl halides and amine nucleophiles including complex examples on oligopeptides, medicinally relevant heterocycles, natural products, and sugars. Full disclosure of the current limitations and procedures for both batch and flow scale-ups (100 g) are also described.

Identifiants

pubmed: 30905151
doi: 10.1021/jacs.9b01886
pmc: PMC6996791
mid: NIHMS1551057
doi:

Substances chimiques

Amines 0

Types de publication

Journal Article Research Support, N.I.H., Extramural Research Support, Non-U.S. Gov't Research Support, U.S. Gov't, Non-P.H.S.

Langues

eng

Sous-ensembles de citation

IM

Pagination

6392-6402

Subventions

Organisme : NIGMS NIH HHS
ID : R35 GM118176
Pays : United States

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Auteurs

Yu Kawamata (Y)

Department of Chemistry , The Scripps Research Institute , 10550 North Torrey Pines Road , La Jolla , California 92037 , United States.
Center for Synthetic Organic Electrochemistry , 315 South 1400 East , Salt Lake City , Utah 84112 , United States.

Julien C Vantourout (JC)

Department of Chemistry , The Scripps Research Institute , 10550 North Torrey Pines Road , La Jolla , California 92037 , United States.

David P Hickey (DP)

Department of Chemistry , University of Utah , 315 South 1400 East , Salt Lake City , Utah 84112 , United States.
Center for Synthetic Organic Electrochemistry , 315 South 1400 East , Salt Lake City , Utah 84112 , United States.

Peng Bai (P)

Department of Chemical Engineering and Materials Science , University of Minnesota , Minneapolis , Minnesota 55455 , United States.
Center for Synthetic Organic Electrochemistry , 315 South 1400 East , Salt Lake City , Utah 84112 , United States.

Longrui Chen (L)

Asymchem Life Science (Tianjin) , Tianjin Economic-Technological Development Zone, Tianjin 300457 , China.

Qinglong Hou (Q)

Asymchem Life Science (Tianjin) , Tianjin Economic-Technological Development Zone, Tianjin 300457 , China.

Wenhua Qiao (W)

Asymchem Life Science (Tianjin) , Tianjin Economic-Technological Development Zone, Tianjin 300457 , China.

Koushik Barman (K)

Department of Chemistry , University of Utah , 315 South 1400 East , Salt Lake City , Utah 84112 , United States.
Center for Synthetic Organic Electrochemistry , 315 South 1400 East , Salt Lake City , Utah 84112 , United States.

Martin A Edwards (MA)

Department of Chemistry , University of Utah , 315 South 1400 East , Salt Lake City , Utah 84112 , United States.
Center for Synthetic Organic Electrochemistry , 315 South 1400 East , Salt Lake City , Utah 84112 , United States.

Alberto F Garrido-Castro (AF)

Department of Chemistry , The Scripps Research Institute , 10550 North Torrey Pines Road , La Jolla , California 92037 , United States.

Justine N deGruyter (JN)

Department of Chemistry , The Scripps Research Institute , 10550 North Torrey Pines Road , La Jolla , California 92037 , United States.

Hugh Nakamura (H)

Department of Chemistry , The Scripps Research Institute , 10550 North Torrey Pines Road , La Jolla , California 92037 , United States.

Kyle Knouse (K)

Department of Chemistry , The Scripps Research Institute , 10550 North Torrey Pines Road , La Jolla , California 92037 , United States.

Chuanguang Qin (C)

Department of Chemistry , The Scripps Research Institute , 10550 North Torrey Pines Road , La Jolla , California 92037 , United States.

Khalyd J Clay (KJ)

Department of Chemistry , The Scripps Research Institute , 10550 North Torrey Pines Road , La Jolla , California 92037 , United States.

Denghui Bao (D)

Asymchem Life Science (Tianjin) , Tianjin Economic-Technological Development Zone, Tianjin 300457 , China.

Chao Li (C)

Department of Chemistry , The Scripps Research Institute , 10550 North Torrey Pines Road , La Jolla , California 92037 , United States.

Jeremy T Starr (JT)

Discovery Sciences, Medicine Design , Pfizer Global Research and Development , 445 Eastern Point Road , Groton , Connecticut 06340 , United States.

Carmen Garcia-Irizarry (C)

Discovery Sciences, Medicine Design , Pfizer Global Research and Development , 445 Eastern Point Road , Groton , Connecticut 06340 , United States.

Neal Sach (N)

Department of Chemistry , La Jolla Laboratories, Pfizer , 10770 Science Center Drive , San Diego , California 92121 , United States.

Henry S White (HS)

Department of Chemistry , University of Utah , 315 South 1400 East , Salt Lake City , Utah 84112 , United States.
Center for Synthetic Organic Electrochemistry , 315 South 1400 East , Salt Lake City , Utah 84112 , United States.

Matthew Neurock (M)

Department of Chemical Engineering and Materials Science , University of Minnesota , Minneapolis , Minnesota 55455 , United States.
Center for Synthetic Organic Electrochemistry , 315 South 1400 East , Salt Lake City , Utah 84112 , United States.

Shelley D Minteer (SD)

Department of Chemistry , University of Utah , 315 South 1400 East , Salt Lake City , Utah 84112 , United States.
Center for Synthetic Organic Electrochemistry , 315 South 1400 East , Salt Lake City , Utah 84112 , United States.

Phil S Baran (PS)

Department of Chemistry , The Scripps Research Institute , 10550 North Torrey Pines Road , La Jolla , California 92037 , United States.
Center for Synthetic Organic Electrochemistry , 315 South 1400 East , Salt Lake City , Utah 84112 , United States.

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Classifications MeSH