Exploring Multivalent Architectures for Binding and Stabilization of <i>N</i>-Acetylgalactosamine 6-Sulfatase

Morquio A syndrome is a lysosomal disorder caused by the deficiency of the lysosomal enzyme <i>N</i>-acetylgalactosamine 6-sulfatase (GALNS, EC 3.1.6.4). Currently, enzyme replacement therapy (ERT) is used to treat Morquio A through the infusion of the recombinant enzyme VIMIZIM<sup&g...

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Main Authors: Maria Giulia Davighi, Francesca Clemente, Giampiero D’Adamio, Macarena Martínez-Bailén, Alessio Morano, Andrea Goti, Amelia Morrone, Camilla Matassini, Francesca Cardona
Format: Article
Language:English
Published: MDPI AG 2025-05-01
Series:Molecules
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Online Access:https://www.mdpi.com/1420-3049/30/10/2222
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author Maria Giulia Davighi
Francesca Clemente
Giampiero D’Adamio
Macarena Martínez-Bailén
Alessio Morano
Andrea Goti
Amelia Morrone
Camilla Matassini
Francesca Cardona
author_facet Maria Giulia Davighi
Francesca Clemente
Giampiero D’Adamio
Macarena Martínez-Bailén
Alessio Morano
Andrea Goti
Amelia Morrone
Camilla Matassini
Francesca Cardona
author_sort Maria Giulia Davighi
collection DOAJ
description Morquio A syndrome is a lysosomal disorder caused by the deficiency of the lysosomal enzyme <i>N</i>-acetylgalactosamine 6-sulfatase (GALNS, EC 3.1.6.4). Currently, enzyme replacement therapy (ERT) is used to treat Morquio A through the infusion of the recombinant enzyme VIMIZIM<sup>®</sup> (elosulfase alfa, BioMarin). Unfortunately, the recombinant enzyme exhibits low conformational stability in vivo. A promising approach to address this issue is the coadministration of recombinant human GALNS (rhGALNS) with a pharmacological chaperone (PC), a molecule that selectively binds to the misfolded protein, stabilizes its conformation, and assists in the restoration of the impaired function. We report in this work the synthesis of a library of multivalent glycomimetics exploiting the copper(I)-catalyzed azide-alkyne cycloaddition (CuAAC) reaction between several dendrimeric scaffolds armed with terminal alkynes and azido ending iminosugars of different structures (pyrrolidines, piperidines, and pyrrolizidines) or simple azido ending carbohydrates as bioactive units. The biological evaluation identified pyrrolidine-based nonavalent dendrimers <b>1</b> and <b>36</b> as the most promising compounds, able both to bind the native enzyme with IC<sub>50</sub> in the micromolar range and to act as enzyme stabilizers toward rhGALNS in a thermal denaturation study, thus identifying promising compounds for a combined PC/ERT therapy.
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spelling doaj-art-9c39481b8e1e47fca223a3cacc92ac902025-08-20T03:48:02ZengMDPI AGMolecules1420-30492025-05-013010222210.3390/molecules30102222Exploring Multivalent Architectures for Binding and Stabilization of <i>N</i>-Acetylgalactosamine 6-SulfataseMaria Giulia Davighi0Francesca Clemente1Giampiero D’Adamio2Macarena Martínez-Bailén3Alessio Morano4Andrea Goti5Amelia Morrone6Camilla Matassini7Francesca Cardona8Department of Chemistry “U. Schiff” (DICUS), University of Florence, Via della Lastruccia 3-13, 50019 Sesto Fiorentino, ItalyDepartment of Chemistry “U. Schiff” (DICUS), University of Florence, Via della Lastruccia 3-13, 50019 Sesto Fiorentino, ItalyDepartment of Chemistry “U. Schiff” (DICUS), University of Florence, Via della Lastruccia 3-13, 50019 Sesto Fiorentino, ItalyDepartment of Chemistry “U. Schiff” (DICUS), University of Florence, Via della Lastruccia 3-13, 50019 Sesto Fiorentino, ItalyDepartment of Chemistry “U. Schiff” (DICUS), University of Florence, Via della Lastruccia 3-13, 50019 Sesto Fiorentino, ItalyDepartment of Chemistry “U. Schiff” (DICUS), University of Florence, Via della Lastruccia 3-13, 50019 Sesto Fiorentino, ItalyLaboratory of Molecular Biology of Neurometabolic Diseases, Neuroscience Department, Meyer Children’s Hospital IRCCS, Viale Pieraccini 24, 50139 Firenze, ItalyDepartment of Chemistry “U. Schiff” (DICUS), University of Florence, Via della Lastruccia 3-13, 50019 Sesto Fiorentino, ItalyDepartment of Chemistry “U. Schiff” (DICUS), University of Florence, Via della Lastruccia 3-13, 50019 Sesto Fiorentino, ItalyMorquio A syndrome is a lysosomal disorder caused by the deficiency of the lysosomal enzyme <i>N</i>-acetylgalactosamine 6-sulfatase (GALNS, EC 3.1.6.4). Currently, enzyme replacement therapy (ERT) is used to treat Morquio A through the infusion of the recombinant enzyme VIMIZIM<sup>®</sup> (elosulfase alfa, BioMarin). Unfortunately, the recombinant enzyme exhibits low conformational stability in vivo. A promising approach to address this issue is the coadministration of recombinant human GALNS (rhGALNS) with a pharmacological chaperone (PC), a molecule that selectively binds to the misfolded protein, stabilizes its conformation, and assists in the restoration of the impaired function. We report in this work the synthesis of a library of multivalent glycomimetics exploiting the copper(I)-catalyzed azide-alkyne cycloaddition (CuAAC) reaction between several dendrimeric scaffolds armed with terminal alkynes and azido ending iminosugars of different structures (pyrrolidines, piperidines, and pyrrolizidines) or simple azido ending carbohydrates as bioactive units. The biological evaluation identified pyrrolidine-based nonavalent dendrimers <b>1</b> and <b>36</b> as the most promising compounds, able both to bind the native enzyme with IC<sub>50</sub> in the micromolar range and to act as enzyme stabilizers toward rhGALNS in a thermal denaturation study, thus identifying promising compounds for a combined PC/ERT therapy.https://www.mdpi.com/1420-3049/30/10/2222Morquio A<i>N</i>-acetylgalactosamine 6-sulfataseenzyme stabilizersiminosugarsdendrimersmultivalent glycomimetics
spellingShingle Maria Giulia Davighi
Francesca Clemente
Giampiero D’Adamio
Macarena Martínez-Bailén
Alessio Morano
Andrea Goti
Amelia Morrone
Camilla Matassini
Francesca Cardona
Exploring Multivalent Architectures for Binding and Stabilization of <i>N</i>-Acetylgalactosamine 6-Sulfatase
Molecules
Morquio A
<i>N</i>-acetylgalactosamine 6-sulfatase
enzyme stabilizers
iminosugars
dendrimers
multivalent glycomimetics
title Exploring Multivalent Architectures for Binding and Stabilization of <i>N</i>-Acetylgalactosamine 6-Sulfatase
title_full Exploring Multivalent Architectures for Binding and Stabilization of <i>N</i>-Acetylgalactosamine 6-Sulfatase
title_fullStr Exploring Multivalent Architectures for Binding and Stabilization of <i>N</i>-Acetylgalactosamine 6-Sulfatase
title_full_unstemmed Exploring Multivalent Architectures for Binding and Stabilization of <i>N</i>-Acetylgalactosamine 6-Sulfatase
title_short Exploring Multivalent Architectures for Binding and Stabilization of <i>N</i>-Acetylgalactosamine 6-Sulfatase
title_sort exploring multivalent architectures for binding and stabilization of i n i acetylgalactosamine 6 sulfatase
topic Morquio A
<i>N</i>-acetylgalactosamine 6-sulfatase
enzyme stabilizers
iminosugars
dendrimers
multivalent glycomimetics
url https://www.mdpi.com/1420-3049/30/10/2222
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