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Divergent synthesis of chiral cyclic azides via asymmetric cycloaddition reactions of vinyl azides

Vinyl azides, bearing conjugated azide and alkene functional groups, have been recognized as versatile building blocks in organic synthesis. In general vinyl azides act as 3-atom (CCN) synthons through the fast release of molecular nitrogen and have been extensively utilized in the construction of s...

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Autores principales: Thirupathi, Nuligonda, Wei, Fang, Tung, Chen-Ho, Xu, Zhenghu
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6639305/
https://www.ncbi.nlm.nih.gov/pubmed/31320649
http://dx.doi.org/10.1038/s41467-019-11134-8
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author Thirupathi, Nuligonda
Wei, Fang
Tung, Chen-Ho
Xu, Zhenghu
author_facet Thirupathi, Nuligonda
Wei, Fang
Tung, Chen-Ho
Xu, Zhenghu
author_sort Thirupathi, Nuligonda
collection PubMed
description Vinyl azides, bearing conjugated azide and alkene functional groups, have been recognized as versatile building blocks in organic synthesis. In general vinyl azides act as 3-atom (CCN) synthons through the fast release of molecular nitrogen and have been extensively utilized in the construction of structurally diverse N-heterocycles. Keeping the azide moiety intact in organic transformations to synthesis chiral azides is an important but challenging task. Herein, we report an enantioselective copper(II)/BOX-catalyzed cycloaddition of vinyl azides, generating diverse chiral cyclic azides. α-Aryl substituted vinyl azides react with unsaturated keto esters through an inverse-electron-demand hetero-Diels-Alder reaction to afford chiral azido dihydropyrans with excellent enatioselectivities. In contrast, cyclohexenyl azides undergo a diastereo- and enantio-selective Diels-Alder reaction giving important azido octahydronaphthalenes with three continuous stereogenic centers. Notable features of these reactions include a very broad scope, mild reaction conditions and 100% atom economy.
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spelling pubmed-66393052019-07-22 Divergent synthesis of chiral cyclic azides via asymmetric cycloaddition reactions of vinyl azides Thirupathi, Nuligonda Wei, Fang Tung, Chen-Ho Xu, Zhenghu Nat Commun Article Vinyl azides, bearing conjugated azide and alkene functional groups, have been recognized as versatile building blocks in organic synthesis. In general vinyl azides act as 3-atom (CCN) synthons through the fast release of molecular nitrogen and have been extensively utilized in the construction of structurally diverse N-heterocycles. Keeping the azide moiety intact in organic transformations to synthesis chiral azides is an important but challenging task. Herein, we report an enantioselective copper(II)/BOX-catalyzed cycloaddition of vinyl azides, generating diverse chiral cyclic azides. α-Aryl substituted vinyl azides react with unsaturated keto esters through an inverse-electron-demand hetero-Diels-Alder reaction to afford chiral azido dihydropyrans with excellent enatioselectivities. In contrast, cyclohexenyl azides undergo a diastereo- and enantio-selective Diels-Alder reaction giving important azido octahydronaphthalenes with three continuous stereogenic centers. Notable features of these reactions include a very broad scope, mild reaction conditions and 100% atom economy. Nature Publishing Group UK 2019-07-18 /pmc/articles/PMC6639305/ /pubmed/31320649 http://dx.doi.org/10.1038/s41467-019-11134-8 Text en © The Author(s) 2019 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/.
spellingShingle Article
Thirupathi, Nuligonda
Wei, Fang
Tung, Chen-Ho
Xu, Zhenghu
Divergent synthesis of chiral cyclic azides via asymmetric cycloaddition reactions of vinyl azides
title Divergent synthesis of chiral cyclic azides via asymmetric cycloaddition reactions of vinyl azides
title_full Divergent synthesis of chiral cyclic azides via asymmetric cycloaddition reactions of vinyl azides
title_fullStr Divergent synthesis of chiral cyclic azides via asymmetric cycloaddition reactions of vinyl azides
title_full_unstemmed Divergent synthesis of chiral cyclic azides via asymmetric cycloaddition reactions of vinyl azides
title_short Divergent synthesis of chiral cyclic azides via asymmetric cycloaddition reactions of vinyl azides
title_sort divergent synthesis of chiral cyclic azides via asymmetric cycloaddition reactions of vinyl azides
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6639305/
https://www.ncbi.nlm.nih.gov/pubmed/31320649
http://dx.doi.org/10.1038/s41467-019-11134-8
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