Synthesis of New DltA Inhibitors and Their Application as Adjuvant Antibiotics to Re-Sensitize Methicillin-Resistant <i>Staphylococcus aureus</i>

The synthesis of a new acyclic and cyclic series of D-Ala-AMP analogues was reported. Chemical modifications were introduced on the carbohydrate, the sulfamate linker, and/or the amino-acid <i>N</i>-terminal moiety in order to increase <i>in vivo</i> stability and cell permea...

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Main Authors: David Leparfait, Alexandre Mahé, Xiao Feng, Delphine Coupri, Fabien Le Cavelier, Nicolas Verneuil, Emmanuel Pfund, Aurélie Budin-Verneuil, Thierry Lequeux
Format: Article
Language:English
Published: MDPI AG 2025-06-01
Series:Molecules
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Online Access:https://www.mdpi.com/1420-3049/30/12/2569
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author David Leparfait
Alexandre Mahé
Xiao Feng
Delphine Coupri
Fabien Le Cavelier
Nicolas Verneuil
Emmanuel Pfund
Aurélie Budin-Verneuil
Thierry Lequeux
author_facet David Leparfait
Alexandre Mahé
Xiao Feng
Delphine Coupri
Fabien Le Cavelier
Nicolas Verneuil
Emmanuel Pfund
Aurélie Budin-Verneuil
Thierry Lequeux
author_sort David Leparfait
collection DOAJ
description The synthesis of a new acyclic and cyclic series of D-Ala-AMP analogues was reported. Chemical modifications were introduced on the carbohydrate, the sulfamate linker, and/or the amino-acid <i>N</i>-terminal moiety in order to increase <i>in vivo</i> stability and cell permeability. These new compounds were evaluated <i>in vitro</i> as DltA inhibitors and also <i>in vivo</i> as adjuvant antibiotics to re-sensitize methicillin-resistant <i>Staphylococcus aureus</i>. Indeed, we showed that seven nucleosides containing either a fluorine atom, an azido group, a difluorophosphonylated allylic ether moiety onto the 2′-position, or a sulfamate and a triazole as the sulfamate linker had moderate to excellent IC<sub>50</sub> values. Among all these new DltA inhibitors, two molecules functionalized by the fluorinated ether or the sulfamide linker were able to efficiently re-sensitize MRSA to imipenem. Quantification of D-alanyl esters confirmed that these two compounds reduced the level of bacterial cell wall D-alanyl residues by 50% and 80%.
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publishDate 2025-06-01
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spelling doaj-art-d379ade698fc484fbf3927263d8c12302025-08-20T03:29:48ZengMDPI AGMolecules1420-30492025-06-013012256910.3390/molecules30122569Synthesis of New DltA Inhibitors and Their Application as Adjuvant Antibiotics to Re-Sensitize Methicillin-Resistant <i>Staphylococcus aureus</i>David Leparfait0Alexandre Mahé1Xiao Feng2Delphine Coupri3Fabien Le Cavelier4Nicolas Verneuil5Emmanuel Pfund6Aurélie Budin-Verneuil7Thierry Lequeux8ENSICAEN, Université de Caen Normandie, Université de Rouen Normandie, INSA Rouen Normandie, CNRS, Institut CARMeN UMR 6064, 14050 Caen, FranceCBSA UR 4312, Université de Caen Normandie, 14000 Caen, FranceENSICAEN, Université de Caen Normandie, Université de Rouen Normandie, INSA Rouen Normandie, CNRS, Institut CARMeN UMR 6064, 14050 Caen, FranceCBSA UR 4312, Université de Caen Normandie, 14000 Caen, FranceENSICAEN, Université de Caen Normandie, Université de Rouen Normandie, INSA Rouen Normandie, CNRS, Institut CARMeN UMR 6064, 14050 Caen, FranceCBSA UR 4312, Université de Caen Normandie, 14000 Caen, FranceENSICAEN, Université de Caen Normandie, Université de Rouen Normandie, INSA Rouen Normandie, CNRS, Institut CARMeN UMR 6064, 14050 Caen, FranceCBSA UR 4312, Université de Caen Normandie, 14000 Caen, FranceENSICAEN, Université de Caen Normandie, Université de Rouen Normandie, INSA Rouen Normandie, CNRS, Institut CARMeN UMR 6064, 14050 Caen, FranceThe synthesis of a new acyclic and cyclic series of D-Ala-AMP analogues was reported. Chemical modifications were introduced on the carbohydrate, the sulfamate linker, and/or the amino-acid <i>N</i>-terminal moiety in order to increase <i>in vivo</i> stability and cell permeability. These new compounds were evaluated <i>in vitro</i> as DltA inhibitors and also <i>in vivo</i> as adjuvant antibiotics to re-sensitize methicillin-resistant <i>Staphylococcus aureus</i>. Indeed, we showed that seven nucleosides containing either a fluorine atom, an azido group, a difluorophosphonylated allylic ether moiety onto the 2′-position, or a sulfamate and a triazole as the sulfamate linker had moderate to excellent IC<sub>50</sub> values. Among all these new DltA inhibitors, two molecules functionalized by the fluorinated ether or the sulfamide linker were able to efficiently re-sensitize MRSA to imipenem. Quantification of D-alanyl esters confirmed that these two compounds reduced the level of bacterial cell wall D-alanyl residues by 50% and 80%.https://www.mdpi.com/1420-3049/30/12/2569nucleoside analogsDltA inhibitorantibiotic resistance
spellingShingle David Leparfait
Alexandre Mahé
Xiao Feng
Delphine Coupri
Fabien Le Cavelier
Nicolas Verneuil
Emmanuel Pfund
Aurélie Budin-Verneuil
Thierry Lequeux
Synthesis of New DltA Inhibitors and Their Application as Adjuvant Antibiotics to Re-Sensitize Methicillin-Resistant <i>Staphylococcus aureus</i>
Molecules
nucleoside analogs
DltA inhibitor
antibiotic resistance
title Synthesis of New DltA Inhibitors and Their Application as Adjuvant Antibiotics to Re-Sensitize Methicillin-Resistant <i>Staphylococcus aureus</i>
title_full Synthesis of New DltA Inhibitors and Their Application as Adjuvant Antibiotics to Re-Sensitize Methicillin-Resistant <i>Staphylococcus aureus</i>
title_fullStr Synthesis of New DltA Inhibitors and Their Application as Adjuvant Antibiotics to Re-Sensitize Methicillin-Resistant <i>Staphylococcus aureus</i>
title_full_unstemmed Synthesis of New DltA Inhibitors and Their Application as Adjuvant Antibiotics to Re-Sensitize Methicillin-Resistant <i>Staphylococcus aureus</i>
title_short Synthesis of New DltA Inhibitors and Their Application as Adjuvant Antibiotics to Re-Sensitize Methicillin-Resistant <i>Staphylococcus aureus</i>
title_sort synthesis of new dlta inhibitors and their application as adjuvant antibiotics to re sensitize methicillin resistant i staphylococcus aureus i
topic nucleoside analogs
DltA inhibitor
antibiotic resistance
url https://www.mdpi.com/1420-3049/30/12/2569
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