Abstract
Currently, the nanoparticle functionalization effect on supramolecular peptide-based hydrogels remains undescribed, but is expected to affect the hydrogels’ self-assembly and final magnetic gel properties. Herein, two different functionalized nanoparticles: citrate-stabilized (14.4 ± 2.6 nm) and lipid-coated (8.9 ± 2.1 nm) magnetic nanoparticles, were used for the formation of dehydropeptide-based supramolecular magnetogels consisting of the ultra-short hydrogelator Cbz-L-Met-Z-ΔPhe-OH, with an assessment of their effect over gel properties. The lipid-coated nanoparticles were distributed along the hydrogel fibers, while citrate-stabilized nanoparticles were aggregated upon gelation, which resulted into a heating efficiency improvement and decrease, respectively. Further, the lipid-coated nanoparticles did not affect drug encapsulation and displayed improved drug release reproducibility compared to citrate-stabilized nanoparticles, despite the latter attaining a stronger AMF-trigger. This report points out that adsorption of nanoparticles to hydrogel fibers, which display domains that improve or do not affect drug encapsulation, can be explored as a means to optimize the development of supramolecular magnetogels to advance theranostic applications.
Highlights
Supramolecular magnetogels basically comprise two main components: the hydrogel and the magnetic nanoparticles
Pursuing the effect of citrate and lipid-functionalized nanoparticles in the development of supramolecular magnetogels, the gelation of the hydrogel Cbz-L-methionine thionine (Met)-Z-∆Phe-OH was systematically optimized by using kinetic models to prepare homogeneous magnetogels, while considering both the kinetics of gelation and sedimentation of nanoparticles
The magnetogels revealed similar doxorubicin release profiles and alternating magnetic field (AMF)-trigger was stronger in the citrate-stabilized nanoparticles, though the triggered release was more reproducible in the lipid-coated nanoparticle-containing gels
Summary
Supramolecular magnetogels basically comprise two main components: the hydrogel and the magnetic nanoparticles. The self-assembly of the supramolecular hydrogelators is driven towards a kinetically-trapped intertwined fibrillar structure, such that solvent pocket microdomains are formed. This process takes place through the cooperative effect of different non-covalent intermolecular interactions: hydrogen bonding, van der Waals, electrostatic, and/or hydrophobic and aromatic interactions [1,2,3,4,5,6,7]. Nanomaterials 2021, 11, 16 provides a means for π-π interactions (like the N-capping group) and conformational constraints in the peptide backbone, meaning that it promotes the self-assembly into fibers and provides resistance to enzymatic degradation [8,9,10]. As assessed in this work, the hydrogel displays a moderate gelation kinetics and elastic modulus, which allows following the impact of the nanoparticles, so that diverse parameters can be optimized
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