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Article Dans Une Revue Chemistry of Materials Année : 2023

Highly Synergistic Properties of Multicomponent Hydrogels Thanks to Cooperative Nucleopeptide Assemblies

Résumé

Supramolecular materials have drawn much attention in the past years, particularly because of their great versatility in terms of structures, organization, and types of nano-objects they can form. Among them, amino acid and peptide derivatives are biomolecules extensively used thanks to their inherent properties and applicability for biological and health applications. Their exceptional abilities to self-assemble have been harnessed to create a myriad of objects and materials, including hydrogels. However, the use of one and only one molecule (i.e., monocomponent) is the widely reported approach which is of great interest in terms of simplicity of use, but it has numerous limitations in terms of properties. To tackle these issues, the multicomponent approach is a promising strategy, even if challenging, for designing lowmolecular-weight molecules able to interact with each other to create new assemblies and new properties not achievable with a single compound. In this context, we report herein on the design, synthesis, and multiscale analysis of an original series of nucleopeptides, i.e., comprising both peptide and DNA-nucleobase moieties linked covalently. Thanks to their dual nature, these nucleopeptides are able to co-assemble when complementary nucleobase moieties interact intermolecularly via hydrogen bonding and π-stacking interactions, leading to impressive synergistic effects, which result in mechanical properties improved by more than 270,000% (with stiffness up to >700 kPa) and self-assembly abilities by ∼280%. To decipher the structure/property relationships, a comprehensive multiscale analysis approach (including rheology, fluorescence, cryo-scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, circular dichroism, nuclear magnetic resonance, and high-resolution magic angle spinning) has been carried out to understand the impact of nucleobases on the supramolecular assembly process and the subsequent formation of nanoobjects, three-dimensional architectures of the hydrogel scaffold, and the resulting physicochemical and mechanical properties of these highly synergistic nucleopeptide assemblies.

Domaines

Chimie
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Dates et versions

hal-04281977 , version 1 (13-11-2023)

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Paul Hoschtettler, Guillaume Pickaert, Alain Carvalho, Marie-Christine Averlant-Petit, Loïc Stefan. Highly Synergistic Properties of Multicomponent Hydrogels Thanks to Cooperative Nucleopeptide Assemblies. Chemistry of Materials, 2023, 35 (11), pp.4259 - 4275. ⟨10.1021/acs.chemmater.3c00308⟩. ⟨hal-04281977⟩
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