Copper(I) Photocatalyzed Bromonitroalkylation of Olefins: Evidence for Highly Efficient Inner-Sphere Pathways.

Copper Homogeneous Catalysis Photocatalysis Radicals Reaction Mechanism

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:
11 Apr 2023
Historique:
received: 25 12 2022
medline: 3 2 2023
pubmed: 3 2 2023
entrez: 2 2 2023
Statut: ppublish

Résumé

We report the visible light-mediated copper-catalyzed vicinal difunctionalization of olefins utilizing bromonitroalkanes as ATRA reagents. This protocol is characterized by high yields and fast reaction times under environmentally benign reaction conditions with exceptional scope, allowing the rapid functionalization of both activated and unactivated olefins. Moreover, late-stage functionnalization of biologically active molecules and upscaling to gram quantities is demonstrated, which offers manifold possibilities for further transformations, e.g. access to nitro- and aminocyclopropanes. Besides the synthetic utility of the title transformation, this study undergirds the exclusive role of copper in photoredox catalysis showing its ability to stabilize and interact with radical intermediates in its coordination sphere. EPR studies suggest that such interactions can even outperform a highly favorable cyclization of transient to persistent radicals contrasting iridium-based photocatalysts.

Identifiants

pubmed: 36732299
doi: 10.1002/anie.202219086
doi:

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

e202219086

Subventions

Organisme : DFG
ID : TRR 325444632635-A1
Organisme : DFG
ID : RE3630/5
Organisme : Fonds der Chemischen Industrie
ID : Ph.D. fellowship
Organisme : Deutsche Forschungsgemeinschaft
ID : RE 948/18

Informations de copyright

© 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.

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Auteurs

Alexander Reichle (A)

Fakultät Chemie & Pharmazie, Universität Regensburg, Universitätsstr. 31, 93053, Regensburg, Germany.

Magdalena Koch (M)

Fakultät Chemie & Pharmazie, Universität Regensburg, Universitätsstr. 31, 93053, Regensburg, Germany.

Hannes Sterzel (H)

Fakultät Chemie & Pharmazie, Universität Regensburg, Universitätsstr. 31, 93053, Regensburg, Germany.

Lea-Joy Großkopf (LJ)

Fakultät Chemie & Pharmazie, Universität Regensburg, Universitätsstr. 31, 93053, Regensburg, Germany.

Johannes Floss (J)

Fakultät Chemie & Pharmazie, Universität Regensburg, Universitätsstr. 31, 93053, Regensburg, Germany.

Julia Rehbein (J)

Fakultät Chemie & Pharmazie, Universität Regensburg, Universitätsstr. 31, 93053, Regensburg, Germany.

Oliver Reiser (O)

Fakultät Chemie & Pharmazie, Universität Regensburg, Universitätsstr. 31, 93053, Regensburg, Germany.

Classifications MeSH