Engineering nanoscale glyco-zeolitic-imidazolate frameworks: Insights into the mechanism of formation

The efficient encapsulation of large carbohydrates into porous metal-organic frameworks (MOFs), and not simply attached to the MOF's surface, is still challenging and underexplored. In this work we have investigated the scope of an optimized synthetic procedure following a biomimetic mineraliza...

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Detalles Bibliográficos
Autores: Rodríguez-Marín, Rocío, Balestra, Salvador R. G., Hamad, Said, Sánchez-Fernández, Elena M., Carrillo-Carrión, Carolina
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2025
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/386150
Acceso en línea:http://hdl.handle.net/10261/386150
https://api.elsevier.com/content/abstract/scopus_id/85216315872
Access Level:acceso abierto
Palabra clave:Electronic structure calculations
De novo encapsulation
Glycolipids
Glycomimetics
Zeolitic-imidazolate frameworks
http://metadata.un.org/sdg/3
Ensure healthy lives and promote well-being for all at all ages
glycolipids
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spelling Engineering nanoscale glyco-zeolitic-imidazolate frameworks: Insights into the mechanism of formationRodríguez-Marín, RocíoBalestra, Salvador R. G.Hamad, SaidSánchez-Fernández, Elena M.Carrillo-Carrión, CarolinaElectronic structure calculationsDe novo encapsulationGlycolipidsGlycomimeticsZeolitic-imidazolate frameworkshttp://metadata.un.org/sdg/3Ensure healthy lives and promote well-being for all at all agesglycolipidsThe efficient encapsulation of large carbohydrates into porous metal-organic frameworks (MOFs), and not simply attached to the MOF's surface, is still challenging and underexplored. In this work we have investigated the scope of an optimized synthetic procedure following a biomimetic mineralization strategy for the encapsulation of a variety of therapeutic glycolipids within a Zeolitic-Imidazolate Framework-8 nanostructure (GlycoZIFs). In all cases, regardless of the glycosidic linkage nature of the glycolipid, we obtained uniform, crystalline and reproducible GlycoZIFs nanoparticles by using the same optimized experimental conditions, which demonstrate the versatility of our approach. Our experimental data revealed that the formation of glyco-micelles, by taking advantage of the surfactant-like character of these glycolipids, is key to promote the nucleation of ZIF-8 around, allowing thus a precise control of the spatial location and amount of glycodrug encapsulated in each ZIF-particle. In turn, the electronic structure calculations showed that there is a strong interaction between the hydroxyl groups in positions C3 and C4 of the glycone core of the glycolipid and the Zn atoms on the ZIF-8 surface, suggesting that those favourable glyco-ZIF interactions also played an important role to induce the ZIF-8 nucleation. Experimental control data and computational studies obtained with a protected glycolipid featuring O-acetyl groups supported that conclusion.This work was supported by grants funded by the Ministerio de Ciencia, Innovación y Universidades and the Agencia Estatal de Investigación MICIU/AEI/10.13039/501100011033 and “ERDF/EU” (PID2022-141034OB-C22 to C.C.-C. and PID2022-141034OB-C21 to E.M.S.-F.). Financial support was also provided from the University of Seville (VIIPPIT-2022-V.1 Modality A2 to E.M.S.-F. and C.C.-C.). R.R.-M. is a FPI fellow (Grant number, PREP2022-000217). Technical assistance from the research support services of the University of Seville Research, Technology and Innovation Centre (CITIUS) is also acknowledged.Peer reviewedElsevierMinisterio de Ciencia, Innovación y Universidades (España)Agencia Estatal de Investigación (España)Universidad de SevillaEuropean CommissionRodríguez-Marín, Rocío [0009-0005-1394-5120]Balestra, Salvador R.G [0000-0002-2163-2782]Hamad, Said [0000-0003-4148-2344]Sánchez-Fernández, Elena M. [0000-0002-8617-8234]Carrillo-Carrión, Carolina [0000-0002-5011-5936]Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202520252025info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Publisher's versioninfo:eu-repo/semantics/publishedVersionapplication/pdfhttp://hdl.handle.net/10261/386150https://api.elsevier.com/content/abstract/scopus_id/85216315872reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2022-141034OB-C22info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2022-141034OB-C21PREP2022-000217The underlying dataset has been published as supplementary material of the article in the publisher platform at DOI https://doi.org/10.1016/j.mtchem.2025.102546https://doi.org/10.1016/j.mtchem.2025.102546Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3861502026-05-22T06:33:51Z
dc.title.none.fl_str_mv Engineering nanoscale glyco-zeolitic-imidazolate frameworks: Insights into the mechanism of formation
title Engineering nanoscale glyco-zeolitic-imidazolate frameworks: Insights into the mechanism of formation
spellingShingle Engineering nanoscale glyco-zeolitic-imidazolate frameworks: Insights into the mechanism of formation
Rodríguez-Marín, Rocío
Electronic structure calculations
De novo encapsulation
Glycolipids
Glycomimetics
Zeolitic-imidazolate frameworks
http://metadata.un.org/sdg/3
Ensure healthy lives and promote well-being for all at all ages
glycolipids
title_short Engineering nanoscale glyco-zeolitic-imidazolate frameworks: Insights into the mechanism of formation
title_full Engineering nanoscale glyco-zeolitic-imidazolate frameworks: Insights into the mechanism of formation
title_fullStr Engineering nanoscale glyco-zeolitic-imidazolate frameworks: Insights into the mechanism of formation
title_full_unstemmed Engineering nanoscale glyco-zeolitic-imidazolate frameworks: Insights into the mechanism of formation
title_sort Engineering nanoscale glyco-zeolitic-imidazolate frameworks: Insights into the mechanism of formation
dc.creator.none.fl_str_mv Rodríguez-Marín, Rocío
Balestra, Salvador R. G.
Hamad, Said
Sánchez-Fernández, Elena M.
Carrillo-Carrión, Carolina
author Rodríguez-Marín, Rocío
author_facet Rodríguez-Marín, Rocío
Balestra, Salvador R. G.
Hamad, Said
Sánchez-Fernández, Elena M.
Carrillo-Carrión, Carolina
author_role author
author2 Balestra, Salvador R. G.
Hamad, Said
Sánchez-Fernández, Elena M.
Carrillo-Carrión, Carolina
author2_role author
author
author
author
dc.contributor.none.fl_str_mv Ministerio de Ciencia, Innovación y Universidades (España)
Agencia Estatal de Investigación (España)
Universidad de Sevilla
European Commission
Rodríguez-Marín, Rocío [0009-0005-1394-5120]
Balestra, Salvador R.G [0000-0002-2163-2782]
Hamad, Said [0000-0003-4148-2344]
Sánchez-Fernández, Elena M. [0000-0002-8617-8234]
Carrillo-Carrión, Carolina [0000-0002-5011-5936]
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv Electronic structure calculations
De novo encapsulation
Glycolipids
Glycomimetics
Zeolitic-imidazolate frameworks
http://metadata.un.org/sdg/3
Ensure healthy lives and promote well-being for all at all ages
glycolipids
topic Electronic structure calculations
De novo encapsulation
Glycolipids
Glycomimetics
Zeolitic-imidazolate frameworks
http://metadata.un.org/sdg/3
Ensure healthy lives and promote well-being for all at all ages
glycolipids
description The efficient encapsulation of large carbohydrates into porous metal-organic frameworks (MOFs), and not simply attached to the MOF's surface, is still challenging and underexplored. In this work we have investigated the scope of an optimized synthetic procedure following a biomimetic mineralization strategy for the encapsulation of a variety of therapeutic glycolipids within a Zeolitic-Imidazolate Framework-8 nanostructure (GlycoZIFs). In all cases, regardless of the glycosidic linkage nature of the glycolipid, we obtained uniform, crystalline and reproducible GlycoZIFs nanoparticles by using the same optimized experimental conditions, which demonstrate the versatility of our approach. Our experimental data revealed that the formation of glyco-micelles, by taking advantage of the surfactant-like character of these glycolipids, is key to promote the nucleation of ZIF-8 around, allowing thus a precise control of the spatial location and amount of glycodrug encapsulated in each ZIF-particle. In turn, the electronic structure calculations showed that there is a strong interaction between the hydroxyl groups in positions C3 and C4 of the glycone core of the glycolipid and the Zn atoms on the ZIF-8 surface, suggesting that those favourable glyco-ZIF interactions also played an important role to induce the ZIF-8 nucleation. Experimental control data and computational studies obtained with a protected glycolipid featuring O-acetyl groups supported that conclusion.
publishDate 2025
dc.date.none.fl_str_mv 2025
2025
2025
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Publisher's version
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/386150
https://api.elsevier.com/content/abstract/scopus_id/85216315872
url http://hdl.handle.net/10261/386150
https://api.elsevier.com/content/abstract/scopus_id/85216315872
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv #PLACEHOLDER_PARENT_METADATA_VALUE#
#PLACEHOLDER_PARENT_METADATA_VALUE#
#PLACEHOLDER_PARENT_METADATA_VALUE#
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2022-141034OB-C22
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2022-141034OB-C21
PREP2022-000217
The underlying dataset has been published as supplementary material of the article in the publisher platform at DOI https://doi.org/10.1016/j.mtchem.2025.102546
https://doi.org/10.1016/j.mtchem.2025.102546
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Elsevier
publisher.none.fl_str_mv Elsevier
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
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