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Palladium-catalyzed α-arylation for the addition of small rings to aromatic compounds

Small, strained rings have rigid, defined conformations and unique electronic properties. For these reasons, many groups seek to use these subunits to form biologically active molecules. We report a generally applicable approach to attach small rings to a wide range of aromatic compounds by palladiu...

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Autores principales: He, Zhi-Tao, Hartwig, John F.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6733931/
https://www.ncbi.nlm.nih.gov/pubmed/31501444
http://dx.doi.org/10.1038/s41467-019-12090-z
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author He, Zhi-Tao
Hartwig, John F.
author_facet He, Zhi-Tao
Hartwig, John F.
author_sort He, Zhi-Tao
collection PubMed
description Small, strained rings have rigid, defined conformations and unique electronic properties. For these reasons, many groups seek to use these subunits to form biologically active molecules. We report a generally applicable approach to attach small rings to a wide range of aromatic compounds by palladium-catalyzed α-arylation of cyclopropyl, cyclobutyl and azetidinyl esters. The direct α-arylation of cyclopropyl esters and cyclobutyl esters is achieved in high yield by ensuring that the rate of coupling exceeds the rate of Claisen condensation. The α-arylation of azetidines is achieved without ring opening of the strained saturated heterocycle by conducting the reactions with an azetidine derivative bearing a benzyl protecting group on nitrogen. Mechanistic studies show that the α-arylation of small rings is challenging because of the weak acidity of α C-H bond (cyclopropanes), strong sensitivity of the strained esters to Claisen condensation (cyclobutatanes), or facile decomposition of the enolates (azetidinyl esters).
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spelling pubmed-67339312019-09-11 Palladium-catalyzed α-arylation for the addition of small rings to aromatic compounds He, Zhi-Tao Hartwig, John F. Nat Commun Article Small, strained rings have rigid, defined conformations and unique electronic properties. For these reasons, many groups seek to use these subunits to form biologically active molecules. We report a generally applicable approach to attach small rings to a wide range of aromatic compounds by palladium-catalyzed α-arylation of cyclopropyl, cyclobutyl and azetidinyl esters. The direct α-arylation of cyclopropyl esters and cyclobutyl esters is achieved in high yield by ensuring that the rate of coupling exceeds the rate of Claisen condensation. The α-arylation of azetidines is achieved without ring opening of the strained saturated heterocycle by conducting the reactions with an azetidine derivative bearing a benzyl protecting group on nitrogen. Mechanistic studies show that the α-arylation of small rings is challenging because of the weak acidity of α C-H bond (cyclopropanes), strong sensitivity of the strained esters to Claisen condensation (cyclobutatanes), or facile decomposition of the enolates (azetidinyl esters). Nature Publishing Group UK 2019-09-09 /pmc/articles/PMC6733931/ /pubmed/31501444 http://dx.doi.org/10.1038/s41467-019-12090-z 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
He, Zhi-Tao
Hartwig, John F.
Palladium-catalyzed α-arylation for the addition of small rings to aromatic compounds
title Palladium-catalyzed α-arylation for the addition of small rings to aromatic compounds
title_full Palladium-catalyzed α-arylation for the addition of small rings to aromatic compounds
title_fullStr Palladium-catalyzed α-arylation for the addition of small rings to aromatic compounds
title_full_unstemmed Palladium-catalyzed α-arylation for the addition of small rings to aromatic compounds
title_short Palladium-catalyzed α-arylation for the addition of small rings to aromatic compounds
title_sort palladium-catalyzed α-arylation for the addition of small rings to aromatic compounds
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6733931/
https://www.ncbi.nlm.nih.gov/pubmed/31501444
http://dx.doi.org/10.1038/s41467-019-12090-z
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