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Hydrogels supramoléculaires mono- et multi-composés formés d'hybrides peptides/acides nucléiques : synthèse, caractérisation et analyse multi-échelle

Abstract : At the tenuous frontier between the solid and the liquid states, soft matter is focusing intense research interest. In particular, gels draw scientists’ attention due to their ability to fix a large amount of solvent either organic (organogels) or aqueous (hydrogels). The latter are predominantly made of polymers and find dozens of applications from industry to daily life. However, over the last twenty years, a new kind of hydrogels has appeared: the peptide-based hydrogels. Indeed, depending on their amino acid sequences, peptides can self-assemble to form supramolecular assemblies which give rise to higher-level structures, namely fibrils, fibres and eventually complex tridimensional networks. Thanks to their inherent advantages in terms of biocompatibility and biodegradability, peptides are highly relevant to develop hydrogel materials for numerous applications, mainly in the biomedical domain. However, the rational design of such hydrogels remains difficult because of a lack of understanding of the relationships between the primary structure of peptides and the resulting properties. This limitation prevents researchers to develop new hydrogels with finely controlled physicochemical and mechanical properties.In this context, we report herein on the development of new series of bio-inspired peptide-based structures forming hydrogels and their multiscale analyses from the supramolecular scale to the mechanical characterisations. Thus, we first discuss the rational design, synthesis and characterisation of hybrid DNA-nucleobase-incorporating peptide derivatives, also termed nucleopeptides, comprised of an heptapeptide functionalized with one of the four DNA nucleobases (i.e., adenine, thymine, guanine or cytosine). Interestingly, the incorporation of a nucleobase induces significant modulations of their physical and structural gel properties, self-assembling kinetics and mechanical properties (e.g., with drastic enhancements of the elastic moduli or resistances to stress, and remarkable thermal reversibilities), depending on the nature of the nucleobase. To further understand the origins of such differences, all the mono-component hydrogels have been subsequently studied at the mesoscopic and then at lower scales, highlighting the impact of nucleic acids on the supramolecular organization.Then, to develop new hydrogel materials with more tuneable properties, we have focused our attention on the development of multicomponent nucleopeptide-based hydrogels. The multicomponent approach consists of the association of several constituents, which can interact in different ways, to obtain new hydrogels for which, in some instances, the resulting properties are greater than the sum of their parts. Thus, taking advantage of the presence of nucleobases and their inherent ability to self-assemble, we discuss the use of nucleopeptides to formulate multicomponent hydrogels and the impact of such mixtures on the structural, physicochemical and mechanical properties compared to the monocomponent approach. We show that mixing peptides and/or nucleopeptides bearing complementary nucleobases allows a control of the mechanical properties of the hydrogels. A multiscale analysis based on a large panel of techniques has provided new knowledge on the interaction behaviour of nucleopeptides and their subsequent consequences on the supramolecular assemblies, on the nanoobjects formed and on the physicochemical and mechanical properties of the resulting hydrogels.Thus, through a multiscale analysis approach of original series of nucleopeptide-based hydrogels, this work provides a better understanding of the relationships between structures and properties, highlighting the high potential of nucleopeptides to develop mono or multicomponent supramolecular hydrogels with optimized and well-controlled properties, thanks to a rational design.
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https://hal.univ-lorraine.fr/tel-03653170
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Submitted on : Wednesday, April 27, 2022 - 2:31:25 PM
Last modification on : Thursday, April 28, 2022 - 3:36:35 AM

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  • HAL Id : tel-03653170, version 1

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Tristan Giraud. Hydrogels supramoléculaires mono- et multi-composés formés d'hybrides peptides/acides nucléiques : synthèse, caractérisation et analyse multi-échelle. Génie des procédés. Université de Lorraine, 2021. Français. ⟨NNT : 2021LORR0226⟩. ⟨tel-03653170⟩

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