Cargando…
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...
Autores principales: | , |
---|---|
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 |
_version_ | 1783450057755852800 |
---|---|
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). |
format | Online Article Text |
id | pubmed-6733931 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2019 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
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 |
work_keys_str_mv | AT hezhitao palladiumcatalyzedaarylationfortheadditionofsmallringstoaromaticcompounds AT hartwigjohnf palladiumcatalyzedaarylationfortheadditionofsmallringstoaromaticcompounds |