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This research focuses on the synthesis of hydrogels exhibiting enhanced antioxidant properties derived from hyaluronic acid (HA) and poly(ethylene brassylate-co-squaric acid) (PEBSA), a copolymacrolactone that have the ability to be used in drug delivery applications. Quercetin (Q), a bioflavonoid with strong antioxidant properties, is employed as a bioactive compound. The biomolecule is encapsulated in the polymeric network using different entrapment techniques, including the initial formation of a complex between PEBSA and Q, which is demonstrated through the dynamic light scattering technique. Fourier transform infrared spectroscopy (FT-IR) and rheological studies confirm the formation of the hydrogels, revealing the occurrence of physical interactions between the synthetic polymer and the polysaccharide. Moreover, the hydrogels demonstrate biocompatible properties after direct contact with the HDFa cell line and antioxidant properties, as revealed by DPPH tests.

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Eying the increasing impact of hyaluronic acid (HA) and its multifaceted applications, this study employs a non-toxic, one-pot strategy to develop injectable, self-healing hydrogels for biomedical applications. Phytic acid (PA), a plant-derived organic acid with high biocompatibility and numerous hydroxyl groups, can act as a cross-linking agent to form hydrogen-bonded networks with the HA chains. The study examined the optimal mass ratio of HA to PA to achieve superior hydrogel performance. Fourier transform infrared spectroscopy, rheological studies, and thermal analysis confirmed the successful formation of the hydrogels, which exhibited injectability, rapid self-healing, malleability, and elasticity. The investigation of different compositions revealed a sensitive influence of PA on the self-assembly phenomena of HA during flow. SEM cross-section images of the freeze-dried gels revealed a porous surface in the form of an interconnected network of microchannels. In addition, the hydrogel exhibits good tissue adhesion properties and promotes cell proliferation in biocompatibility tests on human gingival fibroblasts. The significance of this study lies in the ability of the proposed materials to be injected, to conform to the complex 3D structure of host tissues as well as their ability to recover after damage, indicating significant potential as scaffolds for wound healing.

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The implementation of personalized patches, tailored to individual genetic profiles and containing specific amounts of bioactive substances, has the potential to produce a transformative impact within the medical sector. There are several methods of designing scaffolds in the context of personalized medicine, with three-dimensional (3D) printing emerging as a pivotal technique. This innovative approach can be used to construct a wide variety of pharmaceutical dosage forms, characterized by variations in shape, release profile, and drug combinations, allowing precise dose individualization and the incorporation of multiple therapeutic agents. To expand the potential and applicability of personalized medicine, particularly with regards to indomethacin (IND), a drug necessitating individualized dosing, this study proposes the development of new transdermal delivery systems for IND based on hyaluronic acid and a polylactone synthesized within our research group, namely poly(ethylene brasilate-co-squaric acid) (PEBSA). The obtained systems were characterized in terms of their swelling capacity, rheological behavior, and morphological characteristics that highlighted the formation of stable three-dimensional networks. To impart specific shape and geometry to the structures, multi-component systems based on PEBSA, HA, and methacrylate gelatin were obtained. The scaffolds were loaded with IND and subsequently 3D printed. The release capacity of IND and its dependence on the relative ratios of the components comprising the scaffold composition were highlighted. The cytocompatibility studies revealed the successful development of biocompatible and noncytotoxic systems.

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Low-molecular-weight gelators (LMWGs) are compounds with an intrinsic tendency to self-assemble forming various supramolecular architectures via non-covalent interactions. Considering that the development of supramolecular assemblies through the synergy of molecules is not entirely understood at the molecular level, this study introduced a Fmoc-short peptide and four Fmoc-amino acids as building blocks for the self-assembly/co-assembly process. Hence, we investigated the formation of supramolecular gels starting from the molecular aggregation following two triggering approaches: solvent/co-solvent method and pH switch. The complex morphological analysis (POM, AFM, and STEM) offered an insight into the spontaneous formation of well-ordered nanoaggregates. Briefly, POM and AFM images demonstrated that self-assembled gels present various morphologies like dendrimer, spherulite, and vesicle, whereas all co-assembled supramolecular systems exhibit fibrillar morphologies as a result of the interaction between co-partners of each system. STEM study has confirmed that the molecules interact and join together, finally forming a fibrous network, an aspect seen in both self-assembled and co-assembled gels. XRD allowed the determination of the molecular arrangement. The study emphasized that the Fmoc motif protected the amino groups and facilitated gelation through additional π-π interactions.

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Short aromatic peptide derivatives, i.e., peptides or amino acids modified with aromatic groups, such as 9-fluorenylmethoxycarbonyl (Fmoc), can self-assemble into extracellular matrix-like hydrogels due to their nanofibrillar architecture. Among different types of amino acids, lysine (Lys) and glycine (Gly) are involved in multiple physiological processes, being key factors in the proper growth of cells, carnitine production, and collagen formation. The authors have previously successfully presented the possibility of obtaining supramolecular gels based on Fmoc-Lys-Fmoc and short peptides such as Fmoc-Gly-Gly-Gly in order to use them as a substrate for cell cultures. This paper investigates how the introduction of a gelling polymer can influence the properties of the network as well as the compatibility of the resulting materials with different cell types. A series of hydrogel compositions consisting of combinations of Fmoc-Lys-Fmoc and Fmoc-Gly-Gly-Gly with Agarose and Phytagel are thus obtained. All compositions form structured gels as shown by rheological studies and scanning electron microscopy. Fourier transform infrared spectroscopy analysis evidences the formation of H-bonds between the polysaccharides and amino acids or short peptides. Moreover, all gels exhibit good cell viability on fibroblasts as demonstrated by a live-dead staining test and good in vivo biocompatibility, which highlights the great potential of these biomaterials for biomedical applications.

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In the last years, physical hydrogels have been widely studied due to the characteristics of these structures, respectively the non-covalent interactions and the absence of other necessary components for the cross-linking processes. Low molecular weight gelators are a class of small molecules which form higher ordered structures through hydrogen bonding and π-π interactions. In this context it is known that the formation of hydrogels based on FMOC-amino acids is determined by the primary structures of amino acids and the secondary structure arrangement (alpha-helix or beta-sheet motifs). The present study aimed to obtain supramolecular gels through co-assembly phenomenon using FMOC-amino acids as low molecular weight gelators. The stability of the new structures was evaluated by the vial inversion test, while FTIR spectra put into evidence the interaction between the compounds. The gel-like structure is evidenced by viscoelastic parameters in oscillatory shear conditions. SEM microscopy was used to obtain the visual insight into the morphology of the physical hydrogel network while DLS measurements highlighted the sol-gel transition. The molecular arrangement of gels was determined by circular dichroism, fluorescence and UV-Vis spectroscopy.

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The article reviews the possibilities of encapsulating essential oils EOs, due to their multiple benefits, controlled release, and in order to protect them from environmental conditions. Thus, we present the natural polymers and the synthetic macromolecular chains that are commonly used as networks for embedding EOs, owing to their biodegradability and biocompatibility, interdependent encapsulation methods, and potential applicability of bioactive blend structures. The possibilities of using artificial intelligence to evaluate the bioactivity of EOs-in direct correlation with their chemical constitutions and structures, in order to avoid complex laboratory analyses, to save money and time, and to enhance the final consistency of the products-are also presented.

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(Nano)gels from macromolecular compounds-natural, synthetic, or a combination thereof, suitable crosslinkers-and conferred characteristics-such as degradability, size, charge, amphiphilicity, responsiveness, and softness-are capable of responding to the challenges imposed by bioengineering applications. Polysaccharide-based gels have received particular attention in this field. This review addresses recent advancement in the use of (nano)gel structures prepared only from compounds based on gellan gum, heparin, chondroitin sulfate, carrageenan, guar gum, galactose, or agarose, which represent an important part of the special class of natural polymers, the polysaccharides. Also, future trends are taken into discussion regarding the (nano)gels' use in biomedical applications such as biomimetics, biosensors, artificial muscles, and chemical separations in relation with their ability to be used as a vehicle for various biomolecules due to their physicochemical properties, biocompatibility, and biodegradability.

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