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Alkynyl triazenes enable divergent syntheses of 2-pyrones

The 2-pyrone motif occurs frequently in bioactive natural products and is appreciated as synthetic intermediates. However, only few methods allow for diversifying functional group modifications on this relevant heterocycle. The distinct properties of 1-alkynyl triazenes promote a smooth addition of...

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Autores principales: Tan, Jin-Fay, Bormann, Carl Thomas, Severin, Kay, Cramer, Nicolai
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8261734/
https://www.ncbi.nlm.nih.gov/pubmed/34276943
http://dx.doi.org/10.1039/d1sc02583j
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author Tan, Jin-Fay
Bormann, Carl Thomas
Severin, Kay
Cramer, Nicolai
author_facet Tan, Jin-Fay
Bormann, Carl Thomas
Severin, Kay
Cramer, Nicolai
author_sort Tan, Jin-Fay
collection PubMed
description The 2-pyrone motif occurs frequently in bioactive natural products and is appreciated as synthetic intermediates. However, only few methods allow for diversifying functional group modifications on this relevant heterocycle. The distinct properties of 1-alkynyl triazenes promote a smooth addition of propiolic acids across the triple bond. Addition of catalytic amounts of silver salt induces cyclization to 2-pyrones. Depending on the reaction temperature, either 6-triazenyl or 5-triazenyl 2-pyrones are selectively formed. The triazenyl unit is subsequently replaced by a variety of valuable groups in a one-pot process yielding for instance 2-fluoro pyrones. The substitution occurs with an intriguing 1,5-carbonyl transposition. Moreover, the triazenyl group serves as traceless activating group for subsequent Diels–Alder cycloadditions and as a constituting unit for rare fused aminopyrazole pyrone heterocycles.
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spelling pubmed-82617342021-07-16 Alkynyl triazenes enable divergent syntheses of 2-pyrones Tan, Jin-Fay Bormann, Carl Thomas Severin, Kay Cramer, Nicolai Chem Sci Chemistry The 2-pyrone motif occurs frequently in bioactive natural products and is appreciated as synthetic intermediates. However, only few methods allow for diversifying functional group modifications on this relevant heterocycle. The distinct properties of 1-alkynyl triazenes promote a smooth addition of propiolic acids across the triple bond. Addition of catalytic amounts of silver salt induces cyclization to 2-pyrones. Depending on the reaction temperature, either 6-triazenyl or 5-triazenyl 2-pyrones are selectively formed. The triazenyl unit is subsequently replaced by a variety of valuable groups in a one-pot process yielding for instance 2-fluoro pyrones. The substitution occurs with an intriguing 1,5-carbonyl transposition. Moreover, the triazenyl group serves as traceless activating group for subsequent Diels–Alder cycloadditions and as a constituting unit for rare fused aminopyrazole pyrone heterocycles. The Royal Society of Chemistry 2021-06-04 /pmc/articles/PMC8261734/ /pubmed/34276943 http://dx.doi.org/10.1039/d1sc02583j Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by-nc/3.0/
spellingShingle Chemistry
Tan, Jin-Fay
Bormann, Carl Thomas
Severin, Kay
Cramer, Nicolai
Alkynyl triazenes enable divergent syntheses of 2-pyrones
title Alkynyl triazenes enable divergent syntheses of 2-pyrones
title_full Alkynyl triazenes enable divergent syntheses of 2-pyrones
title_fullStr Alkynyl triazenes enable divergent syntheses of 2-pyrones
title_full_unstemmed Alkynyl triazenes enable divergent syntheses of 2-pyrones
title_short Alkynyl triazenes enable divergent syntheses of 2-pyrones
title_sort alkynyl triazenes enable divergent syntheses of 2-pyrones
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8261734/
https://www.ncbi.nlm.nih.gov/pubmed/34276943
http://dx.doi.org/10.1039/d1sc02583j
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AT cramernicolai alkynyltriazenesenabledivergentsynthesesof2pyrones