dc.contributor.author | Criado González, Miryam | |
dc.contributor.author | Peñas Núñez, Mario Iván | |
dc.contributor.author | Barbault, Florent | |
dc.contributor.author | Müller Sánchez, Alejandro Jesús ![ORCID](/themes/Mirage2//images/orcid_16x16.png) | |
dc.contributor.author | Boulmedais, Fouzia | |
dc.contributor.author | Hernández Velasco, Rebeca | |
dc.date.accessioned | 2024-07-05T15:10:34Z | |
dc.date.available | 2024-07-05T15:10:34Z | |
dc.date.issued | 2024-05 | |
dc.identifier.citation | Nanoscale 16(20) : 9887-9898 (2024) | es_ES |
dc.identifier.issn | 2040-3364 | |
dc.identifier.issn | 2040-3372 | |
dc.identifier.uri | http://hdl.handle.net/10810/68793 | |
dc.description.abstract | Delving into the mechanism behind the molecular interactions at the atomic level of short-sequence peptides plays a key role in the development of nanomaterials with specific structure–property–function relationships from a bottom-up perspective. Due to their poor water solubility, the self-assembly of Fmoc-bearing peptides is usually induced by dissolution in an organic solvent, followed by a dilution step in water, pH changes, and/or a heating–cooling process. Herein, we report a straightforward methodology for the gelation of Fmoc-FFpY (F: phenylalanine; Y: tyrosine; and p: PO42−), a negatively charged tripeptide, in NaCl solution. The electrostatic interactions between Fmoc-FFpY and Na+ ions give rise to different nanofibrillar hydrogels with rheological properties and nanofiber sizes modulated by the NaCl concentration in pure aqueous media. Initiated by the electrostatic interactions between the peptide phosphate groups and the Na+ ions, the peptide self-assembly is stabilized thanks to hydrogen bonds between the peptide backbones and the π–π stacking of aromatic Fmoc and phenyl units. The hydrogels showed self-healing and thermo-responsive properties for potential biomedical applications. Molecular dynamics simulations from systems devoid of prior training not only confirm the aggregation of peptides at a critical salt concentration and the different interactions involved, but also corroborate the secondary structure of the hydrogels at the microsecond timescale. It is worth highlighting the remarkable achievement of reproducing the morphological behavior of the hydrogels using atomistic simulations. To our knowledge, this study is the first to report such a correspondence. | es_ES |
dc.description.sponsorship | Financial support from the Spanish Research Council (CSIC) and the French Research Council (CNRS) for the International Emerging Actions 2018 HYDROPRINT project is gratefully acknowledged. The authors also acknowledge the funding from the projects MAT2017-83014-C2-2-P and PID2020-113045GB-C22 by MCIN/AEI/10.13039/501100011033 and the ALBA Synchrotron (Proposal number 2021095380). R. H. is a member of the SUSPLAST+ platform of CSIC.
The authors thank Dr Rafael Nuñez from CIB-CSIC for TEM and Cryo-TEM measurements and the technical and human support provided by SGIker (UPV/EHU/ERDF, EU). SAXS experiments were performed at the BL 11 NCD-SWEET beamline at ALBA Synchrotron with the collaboration of ALBA staff. ANR (Agence Nationale de la Recherche) and CGI (Commissariat à l'Investissement d'Avenir) are gratefully acknowledged for their financial support of this work through Labex SEAM (Science and Engineering for Advanced Materials and Devices) ANR 11 LABX 086, and ANR 11 IDEX 05 02. This work benefited from the access to the supercomputing facilities of the GENCI (Grand Equipement National pour le Calcul Informatique) and the access to the ITODYS P3MB facility (Université Paris Cité, CNRS UMR 7086, Paris, France). | es_ES |
dc.language.iso | eng | es_ES |
dc.publisher | RSC | es_ES |
dc.relation | info:eu-repo/grantAgreement/MICIU/MAT2017-83014-C2-2-P | es_ES |
dc.relation | info:eu-repo/grantAgreement/MICINN/PID2020-113045GB-C22 | es_ES |
dc.rights | info:eu-repo/semantics/openAccess | es_ES |
dc.rights.uri | http://creativecommons.org/licenses/by-nc/3.0/es/ | * |
dc.title | Salt-induced Fmoc-tripeptide supramolecular hydrogels: a combined experimental and computational study of the self-assembly | es_ES |
dc.type | info:eu-repo/semantics/article | es_ES |
dc.rights.holder | This article is licensed under a Creative Commons Attribution-Non Commercial 3.0 Unported Licence. | es_ES |
dc.rights.holder | Atribución-NoComercial 3.0 España | * |
dc.relation.publisherversion | https://pubs.rsc.org/en/content/articlelanding/2024/nr/d4nr00335g | es_ES |
dc.identifier.doi | 10.1039/d4nr00335g | |
dc.departamentoes | Polímeros y Materiales Avanzados: Física, Química y Tecnología | es_ES |
dc.departamentoeu | Polimero eta Material Aurreratuak: Fisika, Kimika eta Teknologia | es_ES |