Cargando…

Photochemical diazidation of alkenes enabled by ligand-to-metal charge transfer and radical ligand transfer

Vicinal diamines are privileged synthetic motifs in chemistry due to their prevalence and powerful applications in bioactive molecules, pharmaceuticals, and ligand design for transition metals. With organic diazides being regarded as modular precursors to vicinal diamines, enormous efforts have been...

Descripción completa

Detalles Bibliográficos
Autores principales: Bian, Kang-Jie, Kao, Shih-Chieh, Nemoto, David, Chen, Xiao-Wei, West, Julian G.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9789121/
https://www.ncbi.nlm.nih.gov/pubmed/36564375
http://dx.doi.org/10.1038/s41467-022-35560-3
_version_ 1784858907051556864
author Bian, Kang-Jie
Kao, Shih-Chieh
Nemoto, David
Chen, Xiao-Wei
West, Julian G.
author_facet Bian, Kang-Jie
Kao, Shih-Chieh
Nemoto, David
Chen, Xiao-Wei
West, Julian G.
author_sort Bian, Kang-Jie
collection PubMed
description Vicinal diamines are privileged synthetic motifs in chemistry due to their prevalence and powerful applications in bioactive molecules, pharmaceuticals, and ligand design for transition metals. With organic diazides being regarded as modular precursors to vicinal diamines, enormous efforts have been devoted to developing efficient strategies to access organic diazide generated from olefins, themselves common feedstock chemicals. However, state-of-the-art methods for alkene diazidation rely on the usage of corrosive and expensive oxidants or complicated electrochemical setups, significantly limiting the substrate tolerance and practicality of these methods on large scale. Toward overcoming these limitations, here we show a photochemical diazidation of alkenes via iron-mediated ligand-to-metal charge transfer (LMCT) and radical ligand transfer (RLT). Leveraging the merger of these two reaction manifolds, we utilize a stable, earth abundant, and inexpensive iron salt to function as both radical initiator and terminator. Mild conditions, broad alkene scope and amenability to continuous-flow chemistry rendering the transformation photocatalytic were demonstrated. Preliminary mechanistic studies support the radical nature of the cooperative process in the photochemical diazidation, revealing this approach to be a powerful means of olefin difunctionalization.
format Online
Article
Text
id pubmed-9789121
institution National Center for Biotechnology Information
language English
publishDate 2022
publisher Nature Publishing Group UK
record_format MEDLINE/PubMed
spelling pubmed-97891212022-12-25 Photochemical diazidation of alkenes enabled by ligand-to-metal charge transfer and radical ligand transfer Bian, Kang-Jie Kao, Shih-Chieh Nemoto, David Chen, Xiao-Wei West, Julian G. Nat Commun Article Vicinal diamines are privileged synthetic motifs in chemistry due to their prevalence and powerful applications in bioactive molecules, pharmaceuticals, and ligand design for transition metals. With organic diazides being regarded as modular precursors to vicinal diamines, enormous efforts have been devoted to developing efficient strategies to access organic diazide generated from olefins, themselves common feedstock chemicals. However, state-of-the-art methods for alkene diazidation rely on the usage of corrosive and expensive oxidants or complicated electrochemical setups, significantly limiting the substrate tolerance and practicality of these methods on large scale. Toward overcoming these limitations, here we show a photochemical diazidation of alkenes via iron-mediated ligand-to-metal charge transfer (LMCT) and radical ligand transfer (RLT). Leveraging the merger of these two reaction manifolds, we utilize a stable, earth abundant, and inexpensive iron salt to function as both radical initiator and terminator. Mild conditions, broad alkene scope and amenability to continuous-flow chemistry rendering the transformation photocatalytic were demonstrated. Preliminary mechanistic studies support the radical nature of the cooperative process in the photochemical diazidation, revealing this approach to be a powerful means of olefin difunctionalization. Nature Publishing Group UK 2022-12-23 /pmc/articles/PMC9789121/ /pubmed/36564375 http://dx.doi.org/10.1038/s41467-022-35560-3 Text en © The Author(s) 2022 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Bian, Kang-Jie
Kao, Shih-Chieh
Nemoto, David
Chen, Xiao-Wei
West, Julian G.
Photochemical diazidation of alkenes enabled by ligand-to-metal charge transfer and radical ligand transfer
title Photochemical diazidation of alkenes enabled by ligand-to-metal charge transfer and radical ligand transfer
title_full Photochemical diazidation of alkenes enabled by ligand-to-metal charge transfer and radical ligand transfer
title_fullStr Photochemical diazidation of alkenes enabled by ligand-to-metal charge transfer and radical ligand transfer
title_full_unstemmed Photochemical diazidation of alkenes enabled by ligand-to-metal charge transfer and radical ligand transfer
title_short Photochemical diazidation of alkenes enabled by ligand-to-metal charge transfer and radical ligand transfer
title_sort photochemical diazidation of alkenes enabled by ligand-to-metal charge transfer and radical ligand transfer
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9789121/
https://www.ncbi.nlm.nih.gov/pubmed/36564375
http://dx.doi.org/10.1038/s41467-022-35560-3
work_keys_str_mv AT biankangjie photochemicaldiazidationofalkenesenabledbyligandtometalchargetransferandradicalligandtransfer
AT kaoshihchieh photochemicaldiazidationofalkenesenabledbyligandtometalchargetransferandradicalligandtransfer
AT nemotodavid photochemicaldiazidationofalkenesenabledbyligandtometalchargetransferandradicalligandtransfer
AT chenxiaowei photochemicaldiazidationofalkenesenabledbyligandtometalchargetransferandradicalligandtransfer
AT westjuliang photochemicaldiazidationofalkenesenabledbyligandtometalchargetransferandradicalligandtransfer