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Synthesis and Characterization of a Novel Resveratrol Xylobioside Obtained Using a Mutagenic Variant of a GH10 Endoxylanase

Resveratrol is a natural polyphenol with antioxidant activity and numerous health benefits. However, in vivo application of this compound is still a challenge due to its poor aqueous solubility and rapid metabolism, which leads to an extremely low bioavailability in the target tissues. In this work,...

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Autores principales: Pozo-Rodríguez, Ana, Méndez-Líter, Juan A., García-Villalba, Rocío, Beltrán, David, Calviño, Eva, Santana, Andrés G., de Eugenio, Laura I., Cañada, Francisco Javier, Prieto, Alicia, Barriuso, Jorge, Tomás-Barberán, Francisco A., Martínez, María Jesús
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9855058/
https://www.ncbi.nlm.nih.gov/pubmed/36670947
http://dx.doi.org/10.3390/antiox12010085
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author Pozo-Rodríguez, Ana
Méndez-Líter, Juan A.
García-Villalba, Rocío
Beltrán, David
Calviño, Eva
Santana, Andrés G.
de Eugenio, Laura I.
Cañada, Francisco Javier
Prieto, Alicia
Barriuso, Jorge
Tomás-Barberán, Francisco A.
Martínez, María Jesús
author_facet Pozo-Rodríguez, Ana
Méndez-Líter, Juan A.
García-Villalba, Rocío
Beltrán, David
Calviño, Eva
Santana, Andrés G.
de Eugenio, Laura I.
Cañada, Francisco Javier
Prieto, Alicia
Barriuso, Jorge
Tomás-Barberán, Francisco A.
Martínez, María Jesús
author_sort Pozo-Rodríguez, Ana
collection PubMed
description Resveratrol is a natural polyphenol with antioxidant activity and numerous health benefits. However, in vivo application of this compound is still a challenge due to its poor aqueous solubility and rapid metabolism, which leads to an extremely low bioavailability in the target tissues. In this work, rXynSOS-E236G glycosynthase, designed from a GH10 endoxylanase of the fungus Talaromyces amestolkiae, was used to glycosylate resveratrol by using xylobiosyl-fluoride as a sugar donor. The major product from this reaction was identified by NMR as 3-O-ꞵ-d-xylobiosyl resveratrol, together with other glycosides produced in a lower amount as 4′-O-ꞵ-d-xylobiosyl resveratrol and 3-O-ꞵ-d-xylotetraosyl resveratrol. The application of response surface methodology made it possible to optimize the reaction, producing 35% of 3-O-ꞵ-d-xylobiosyl resveratrol. Since other minor glycosides are obtained in addition to this compound, the transformation of the phenolic substrate amounted to 70%. Xylobiosylation decreased the antioxidant capacity of resveratrol by 2.21-fold, but, in return, produced a staggering 4,866-fold improvement in solubility, facilitating the delivery of large amounts of the molecule and its transit to the colon. A preliminary study has also shown that the colonic microbiota is capable of releasing resveratrol from 3-O-ꞵ-d-xylobiosyl resveratrol. These results support the potential of mutagenic variants of glycosyl hydrolases to synthesize highly soluble resveratrol glycosides, which could, in turn, improve the bioavailability and bioactive properties of this polyphenol.
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spelling pubmed-98550582023-01-21 Synthesis and Characterization of a Novel Resveratrol Xylobioside Obtained Using a Mutagenic Variant of a GH10 Endoxylanase Pozo-Rodríguez, Ana Méndez-Líter, Juan A. García-Villalba, Rocío Beltrán, David Calviño, Eva Santana, Andrés G. de Eugenio, Laura I. Cañada, Francisco Javier Prieto, Alicia Barriuso, Jorge Tomás-Barberán, Francisco A. Martínez, María Jesús Antioxidants (Basel) Article Resveratrol is a natural polyphenol with antioxidant activity and numerous health benefits. However, in vivo application of this compound is still a challenge due to its poor aqueous solubility and rapid metabolism, which leads to an extremely low bioavailability in the target tissues. In this work, rXynSOS-E236G glycosynthase, designed from a GH10 endoxylanase of the fungus Talaromyces amestolkiae, was used to glycosylate resveratrol by using xylobiosyl-fluoride as a sugar donor. The major product from this reaction was identified by NMR as 3-O-ꞵ-d-xylobiosyl resveratrol, together with other glycosides produced in a lower amount as 4′-O-ꞵ-d-xylobiosyl resveratrol and 3-O-ꞵ-d-xylotetraosyl resveratrol. The application of response surface methodology made it possible to optimize the reaction, producing 35% of 3-O-ꞵ-d-xylobiosyl resveratrol. Since other minor glycosides are obtained in addition to this compound, the transformation of the phenolic substrate amounted to 70%. Xylobiosylation decreased the antioxidant capacity of resveratrol by 2.21-fold, but, in return, produced a staggering 4,866-fold improvement in solubility, facilitating the delivery of large amounts of the molecule and its transit to the colon. A preliminary study has also shown that the colonic microbiota is capable of releasing resveratrol from 3-O-ꞵ-d-xylobiosyl resveratrol. These results support the potential of mutagenic variants of glycosyl hydrolases to synthesize highly soluble resveratrol glycosides, which could, in turn, improve the bioavailability and bioactive properties of this polyphenol. MDPI 2022-12-30 /pmc/articles/PMC9855058/ /pubmed/36670947 http://dx.doi.org/10.3390/antiox12010085 Text en © 2022 by the authors. https://creativecommons.org/licenses/by/4.0/Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Article
Pozo-Rodríguez, Ana
Méndez-Líter, Juan A.
García-Villalba, Rocío
Beltrán, David
Calviño, Eva
Santana, Andrés G.
de Eugenio, Laura I.
Cañada, Francisco Javier
Prieto, Alicia
Barriuso, Jorge
Tomás-Barberán, Francisco A.
Martínez, María Jesús
Synthesis and Characterization of a Novel Resveratrol Xylobioside Obtained Using a Mutagenic Variant of a GH10 Endoxylanase
title Synthesis and Characterization of a Novel Resveratrol Xylobioside Obtained Using a Mutagenic Variant of a GH10 Endoxylanase
title_full Synthesis and Characterization of a Novel Resveratrol Xylobioside Obtained Using a Mutagenic Variant of a GH10 Endoxylanase
title_fullStr Synthesis and Characterization of a Novel Resveratrol Xylobioside Obtained Using a Mutagenic Variant of a GH10 Endoxylanase
title_full_unstemmed Synthesis and Characterization of a Novel Resveratrol Xylobioside Obtained Using a Mutagenic Variant of a GH10 Endoxylanase
title_short Synthesis and Characterization of a Novel Resveratrol Xylobioside Obtained Using a Mutagenic Variant of a GH10 Endoxylanase
title_sort synthesis and characterization of a novel resveratrol xylobioside obtained using a mutagenic variant of a gh10 endoxylanase
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9855058/
https://www.ncbi.nlm.nih.gov/pubmed/36670947
http://dx.doi.org/10.3390/antiox12010085
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