Supramolecular Hydrogel Induced by Electrostatic Interactions between Polycation and Phosphorylated-Fmoc-Tripeptide
- Miryam Criado-GonzalezMiryam Criado-GonzalezUniversité de Strasbourg, CNRS, Institut Charles Sadron UPR 22, 67034 Strasbourg, FranceInstitut National de la Santé et de la Recherche Médicale, UMR-S 1121, “Biomatériaux et Bioingénierie”, 67087 Strasbourg, FranceUniversité de Strasbourg, Faculté de Chirurgie Dentaire, Fédération de Médecine Translationnelle de Strasbourg and Fédération des Matériaux et Nanoscience d’Alsace, 67000 Strasbourg, FranceMore by Miryam Criado-Gonzalez
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- Déborah WagnerDéborah WagnerUniversité de Strasbourg, CNRS, Institut Charles Sadron UPR 22, 67034 Strasbourg, FranceMore by Déborah Wagner
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- Jennifer Rodon ForesJennifer Rodon ForesUniversité de Strasbourg, CNRS, Institut Charles Sadron UPR 22, 67034 Strasbourg, FranceMore by Jennifer Rodon Fores
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- Christian BlanckChristian BlanckUniversité de Strasbourg, CNRS, Institut Charles Sadron UPR 22, 67034 Strasbourg, FranceMore by Christian Blanck
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- Marc SchmutzMarc SchmutzUniversité de Strasbourg, CNRS, Institut Charles Sadron UPR 22, 67034 Strasbourg, FranceMore by Marc Schmutz
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- Alain ChaumontAlain ChaumontUniversité de Strasbourg, Faculté de Chimie, UMR7140, 67000 Strasbourg, FranceMore by Alain Chaumont
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- Morgane RabineauMorgane RabineauInstitut National de la Santé et de la Recherche Médicale, UMR-S 1121, “Biomatériaux et Bioingénierie”, 67087 Strasbourg, FranceUniversité de Strasbourg, Faculté de Chirurgie Dentaire, Fédération de Médecine Translationnelle de Strasbourg and Fédération des Matériaux et Nanoscience d’Alsace, 67000 Strasbourg, FranceMore by Morgane Rabineau
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- Joseph B. SchlenoffJoseph B. SchlenoffDepartment of Chemistry and Biochemistry, Florida State University, Tallahassee, Florida 32306, United StatesMore by Joseph B. Schlenoff
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- Guillaume FleithGuillaume FleithUniversité de Strasbourg, CNRS, Institut Charles Sadron UPR 22, 67034 Strasbourg, FranceMore by Guillaume Fleith
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- Jérôme CombetJérôme CombetUniversité de Strasbourg, CNRS, Institut Charles Sadron UPR 22, 67034 Strasbourg, FranceMore by Jérôme Combet
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- Pierre Schaaf*Pierre Schaaf*E-mail: [email protected]. Phone: +33-3-68-85-33-87 (P.S.).Université de Strasbourg, CNRS, Institut Charles Sadron UPR 22, 67034 Strasbourg, FranceInstitut National de la Santé et de la Recherche Médicale, UMR-S 1121, “Biomatériaux et Bioingénierie”, 67087 Strasbourg, FranceUniversité de Strasbourg, Faculté de Chirurgie Dentaire, Fédération de Médecine Translationnelle de Strasbourg and Fédération des Matériaux et Nanoscience d’Alsace, 67000 Strasbourg, FranceEcole de Chimie, Polymères et Matériaux, Université de Strasbourg, 67087 Strasbourg, FranceMore by Pierre Schaaf
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- Loïc JierryLoïc JierryUniversité de Strasbourg, CNRS, Institut Charles Sadron UPR 22, 67034 Strasbourg, FranceEcole de Chimie, Polymères et Matériaux, Université de Strasbourg, 67087 Strasbourg, FranceMore by Loïc Jierry
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- Fouzia Boulmedais*Fouzia Boulmedais*E-mail: [email protected]. Phone: +33-3-88-41-41-60 (F.B.).Université de Strasbourg, CNRS, Institut Charles Sadron UPR 22, 67034 Strasbourg, FranceMore by Fouzia Boulmedais
Abstract
Supramolecular hydrogels formed through noncovalent interactions of low-molecular-weight hydrogelators (LMWHs) show great potential applications in different fields, such as delivery of therapeutics, injectable biomaterials, catalysis, or materials chemistry. Generally, the self-assembly of LMWHs is triggered by a sol–gel process through an external stimulus able to switch their solubility, such as temperature, pH, or solvent change and chemical or enzymatic reactions. In this work, we introduced a new strategy to trigger and control the self-assembly of Fmoc-FFpY peptides by direct electrostatic interactions with a polycation without dephosphorylation of the peptides. The resulting hydrogels show enhanced mechanical properties in comparison to gels of Fmoc-FFpY induced by enzymatic dephosphorylation. Peptide self-assembly yields β-sheets, revealed by circular dichroism and infrared spectroscopy. Characteristic distances predicted by geometry optimization in the gas phase are in agreement with X-ray scattering data and transmission electron microscopy observations. It is proposed that core–shell cylinders are formed in which polycation chains decorate the micellar structures of Fmoc-FFpY peptides through electrostatic interactions between the charged amine groups of the polycations and the phosphate groups of the peptides. Because the gels form quickly and have superior mechanical properties, applications as injectable biomaterials are foreseen. This work opens a route toward a new class of self-assembled hydrogels, where Fmoc tripeptides can be self-assembled with specific polycations to obtain, for example, antimicrobial hydrogels.
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