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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Summary: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%.
ISSN:1420-3049