Wet spinning and 3D printing of supramolecular hydrogels in acid-base and dynamic conditions
2023
Andriamiseza, Faniry | Peters, Salomé | Roux, Clément | Dietrich, Nicolas | Coudret, Christophe | Fitremann, Juliette | Interactions moléculaires et réactivité chimique et photochimique (IMRCP) ; Institut de Chimie de Toulouse (ICT) ; Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3) ; Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie - CNRS Chimie (INC-CNRS)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP) ; Université de Toulouse (UT)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3) ; Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie - CNRS Chimie (INC-CNRS)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP) ; Université de Toulouse (UT)-Institut Ecologie et Environnement - CNRS Ecologie et Environnement (INEE-CNRS) ; Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Fédération de Recherche Fluides, Energie, Réacteurs, Matériaux et Transferts (FERMAT) ; Institut National des Sciences Appliquées - Toulouse (INSA Toulouse) ; Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Université Toulouse III - Paul Sabatier (UT3) ; Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP) ; Université de Toulouse (UT)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse) ; Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS) | Université de Lille | Toulouse Biotechnology Institute (TBI) ; Institut National des Sciences Appliquées - Toulouse (INSA Toulouse) ; Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE) | This work was supported by the French Ministry of Higher Education, Research and Innovation (Ministere de l'Enseignement Superieur, de la Recherche et de l'Innovation) for F.A.'s grant, L'Ecole Nationale Ve'te'rinaire de Toulouse, ENVT for Salome & nbsp | ANR-15-CE07-0007,NEURAXE,Gels supramoléculaires orientés pour le guidage de cellules souches neurales(2015)
International audience
Mostrar más [+] Menos [-]Inglés. N-alkyl-D-galactonamides give biocompatible hydrogels that are very delicate and not injectable. To circumvent their mechanical fragility and the injectability issue, we have developed a method of injection based on solvent-water exchange. A solution of the gelator in a good solvent is injected vertically in a bath of water. The diffusion of water inside the solvent jet triggers the fast self-assembly of the N-alkyl-D-galactonamides into supramolecular fibers. It leads to the formation of well-defined gel filaments. We first used dimethylsulfoxide (DMSO) as the good solvent of N-alkyl-D-galactonamides. Then, we considered to get rid of this organic solvent by implementing an "all-aqueous method", paving the way to green chemistry methods. Despite the fact that these molecules do not have conventional acid-base functions in water, N-alkyl-D-galactonamides can be deprotonated and solubilized in highly concentrated NaOH aqueous solutions. As with DMSO, the basic solution is denser than the solution in the bath. Thus, a well-defined vertical jet falls down when the solution is injected in an acidic aqueous solution. The neutralization of the base at the acid-base interface triggers the gelation and leads to the formation of well-defined gel filaments as well. The acid-base reaction at the interface has been visualized by colored pH in-dicators. With phenol red (pKa = 7.9), a pink-to-yellow V-shaped "flame" transition is clearly observed. A similar transition from colorless-to-pink is observed with the pH indicator acid fuchsin, which pKa = 13 is close to the N-heptyl-D-galactonamide pKa. The distance from the nozzle of this transition zone is directly related to the injection rate, which is well-described by a model. We also applied this method to 3D printing, by a liquid-in liquid direct writing. It gives well-resolved patterns. The opportunity to get noodles or 3D printed patterns made of single small molecules by acid-base exchange opens new perspectives. Notably, the supramolecular fibers could be used to support and direct the formation of inorganic materials with original microstructures.
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