Cargando…

Highly selective nickel-catalyzed gem-difluoropropargylation of unactivated alkylzinc reagents

In spite of the important applications of difluoroalkylated molecules in medicinal chemistry, to date, the reaction of difluoroalkylating reagents with unactivated, aliphatic substrates through a controllable manner remains challenging and has not been reported. Here we describe an efficient nickel-...

Descripción completa

Detalles Bibliográficos
Autores principales: An, Lun, Xu, Chang, Zhang, Xingang
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2017
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5684216/
https://www.ncbi.nlm.nih.gov/pubmed/29133781
http://dx.doi.org/10.1038/s41467-017-01540-1
_version_ 1783278428056715264
author An, Lun
Xu, Chang
Zhang, Xingang
author_facet An, Lun
Xu, Chang
Zhang, Xingang
author_sort An, Lun
collection PubMed
description In spite of the important applications of difluoroalkylated molecules in medicinal chemistry, to date, the reaction of difluoroalkylating reagents with unactivated, aliphatic substrates through a controllable manner remains challenging and has not been reported. Here we describe an efficient nickel-catalyzed cross-coupling of unactivated alkylzinc reagen\ts with gem-difluoropropargyl bromides. The reaction proceeds under mild reaction conditions with high efficiency and excellent regiochemical selectivity. Transformations of the resulting difluoroalkylated alkanes lead to a variety of biologically active molecules, providing a facile route for applications in drug discovery and development. Preliminary mechanistic studies reveal that an alkyl nickel intermediate [Ni(tpy)alkyl] (tpy, terpyridine) is involved in the catalytic cycle.
format Online
Article
Text
id pubmed-5684216
institution National Center for Biotechnology Information
language English
publishDate 2017
publisher Nature Publishing Group UK
record_format MEDLINE/PubMed
spelling pubmed-56842162017-11-17 Highly selective nickel-catalyzed gem-difluoropropargylation of unactivated alkylzinc reagents An, Lun Xu, Chang Zhang, Xingang Nat Commun Article In spite of the important applications of difluoroalkylated molecules in medicinal chemistry, to date, the reaction of difluoroalkylating reagents with unactivated, aliphatic substrates through a controllable manner remains challenging and has not been reported. Here we describe an efficient nickel-catalyzed cross-coupling of unactivated alkylzinc reagen\ts with gem-difluoropropargyl bromides. The reaction proceeds under mild reaction conditions with high efficiency and excellent regiochemical selectivity. Transformations of the resulting difluoroalkylated alkanes lead to a variety of biologically active molecules, providing a facile route for applications in drug discovery and development. Preliminary mechanistic studies reveal that an alkyl nickel intermediate [Ni(tpy)alkyl] (tpy, terpyridine) is involved in the catalytic cycle. Nature Publishing Group UK 2017-11-13 /pmc/articles/PMC5684216/ /pubmed/29133781 http://dx.doi.org/10.1038/s41467-017-01540-1 Text en © The Author(s) 2017 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
An, Lun
Xu, Chang
Zhang, Xingang
Highly selective nickel-catalyzed gem-difluoropropargylation of unactivated alkylzinc reagents
title Highly selective nickel-catalyzed gem-difluoropropargylation of unactivated alkylzinc reagents
title_full Highly selective nickel-catalyzed gem-difluoropropargylation of unactivated alkylzinc reagents
title_fullStr Highly selective nickel-catalyzed gem-difluoropropargylation of unactivated alkylzinc reagents
title_full_unstemmed Highly selective nickel-catalyzed gem-difluoropropargylation of unactivated alkylzinc reagents
title_short Highly selective nickel-catalyzed gem-difluoropropargylation of unactivated alkylzinc reagents
title_sort highly selective nickel-catalyzed gem-difluoropropargylation of unactivated alkylzinc reagents
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5684216/
https://www.ncbi.nlm.nih.gov/pubmed/29133781
http://dx.doi.org/10.1038/s41467-017-01540-1
work_keys_str_mv AT anlun highlyselectivenickelcatalyzedgemdifluoropropargylationofunactivatedalkylzincreagents
AT xuchang highlyselectivenickelcatalyzedgemdifluoropropargylationofunactivatedalkylzincreagents
AT zhangxingang highlyselectivenickelcatalyzedgemdifluoropropargylationofunactivatedalkylzincreagents