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Construction of C-B axial chirality via dynamic kinetic asymmetric cross-coupling mediated by tetracoordinate boron

Catalytic dynamic kinetic asymmetric transformation (DyKAT) provides a powerful tool to access chiral stereoisomers from racemic substrates. Such transformation has been widely employed on the construction of central chirality, however, the application in axial chirality remains underexplored becaus...

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Autores principales: Yang, Kai, Mao, Yanfei, Zhang, Zhihan, Xu, Jie, Wang, Hao, He, Yong, Yu, Peiyuan, Song, Qiuling
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10366327/
https://www.ncbi.nlm.nih.gov/pubmed/37488114
http://dx.doi.org/10.1038/s41467-023-40164-6
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author Yang, Kai
Mao, Yanfei
Zhang, Zhihan
Xu, Jie
Wang, Hao
He, Yong
Yu, Peiyuan
Song, Qiuling
author_facet Yang, Kai
Mao, Yanfei
Zhang, Zhihan
Xu, Jie
Wang, Hao
He, Yong
Yu, Peiyuan
Song, Qiuling
author_sort Yang, Kai
collection PubMed
description Catalytic dynamic kinetic asymmetric transformation (DyKAT) provides a powerful tool to access chiral stereoisomers from racemic substrates. Such transformation has been widely employed on the construction of central chirality, however, the application in axial chirality remains underexplored because its equilibrium of substrate enantiomers is limited to five-membered metalacyclic intermediate. Here we report a tetracoordinate boron-directed dynamic kinetic asymmetric cross-coupling of racemic, configurationally stable 3-bromo-2,1-azaborines with boronic acid derivatives. A series of challenging C-B axially chiral compounds were prepared with generally good to excellent enantioselectivities. Moreover, this transformation can also be extended to prepare atropisomers bearing adjacent C-B and C-C diaxes with excellent diastereo- and enantio-control. The key to the success relies on the rational design of a reversible tetracoordinate boron intermediate, which is supported by theoretical calculations that dramatically reduces the rotational barrier of the original C-B axis and achieves the goal of DyKAT.
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spelling pubmed-103663272023-07-26 Construction of C-B axial chirality via dynamic kinetic asymmetric cross-coupling mediated by tetracoordinate boron Yang, Kai Mao, Yanfei Zhang, Zhihan Xu, Jie Wang, Hao He, Yong Yu, Peiyuan Song, Qiuling Nat Commun Article Catalytic dynamic kinetic asymmetric transformation (DyKAT) provides a powerful tool to access chiral stereoisomers from racemic substrates. Such transformation has been widely employed on the construction of central chirality, however, the application in axial chirality remains underexplored because its equilibrium of substrate enantiomers is limited to five-membered metalacyclic intermediate. Here we report a tetracoordinate boron-directed dynamic kinetic asymmetric cross-coupling of racemic, configurationally stable 3-bromo-2,1-azaborines with boronic acid derivatives. A series of challenging C-B axially chiral compounds were prepared with generally good to excellent enantioselectivities. Moreover, this transformation can also be extended to prepare atropisomers bearing adjacent C-B and C-C diaxes with excellent diastereo- and enantio-control. The key to the success relies on the rational design of a reversible tetracoordinate boron intermediate, which is supported by theoretical calculations that dramatically reduces the rotational barrier of the original C-B axis and achieves the goal of DyKAT. Nature Publishing Group UK 2023-07-24 /pmc/articles/PMC10366327/ /pubmed/37488114 http://dx.doi.org/10.1038/s41467-023-40164-6 Text en © The Author(s) 2023 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
Yang, Kai
Mao, Yanfei
Zhang, Zhihan
Xu, Jie
Wang, Hao
He, Yong
Yu, Peiyuan
Song, Qiuling
Construction of C-B axial chirality via dynamic kinetic asymmetric cross-coupling mediated by tetracoordinate boron
title Construction of C-B axial chirality via dynamic kinetic asymmetric cross-coupling mediated by tetracoordinate boron
title_full Construction of C-B axial chirality via dynamic kinetic asymmetric cross-coupling mediated by tetracoordinate boron
title_fullStr Construction of C-B axial chirality via dynamic kinetic asymmetric cross-coupling mediated by tetracoordinate boron
title_full_unstemmed Construction of C-B axial chirality via dynamic kinetic asymmetric cross-coupling mediated by tetracoordinate boron
title_short Construction of C-B axial chirality via dynamic kinetic asymmetric cross-coupling mediated by tetracoordinate boron
title_sort construction of c-b axial chirality via dynamic kinetic asymmetric cross-coupling mediated by tetracoordinate boron
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10366327/
https://www.ncbi.nlm.nih.gov/pubmed/37488114
http://dx.doi.org/10.1038/s41467-023-40164-6
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