Effect of Organogelator Concentration on Gelation Kinetics and Drug Release Behaviour of Paracetamol-Loaded Soybean Oleogels

Organogelators induce 3-D networked structures in apolar solvent molecules via cross-linking of non-covalent self-assembled aggregates below the gelation temperature. The objective of the present investigation was to evaluate the effects of different Span 40 concentrations on gelation kinetics and drug release behaviour of topical soybean oleogels. An inversely proportional relationship was observed between gelation time, melt flow index and concentration of Span 40 in soybean oleogels. Gompertz model was employed on gelation kinetics data to determine organogelator and oil parameters which are assumed to be associated with thermal stability and gel flexibility respectively. Formulation OGS2 (18% W/V Span 40) formed less viscous, thermally stable and presumably more flexible oleogel compared to other formulations. Nearly ideal zero-order release of paracetamol was achieved from OGS*2 following Fickian diffusion. However, slow drug release profiles, higher t50 values were observed with oleogels having 20-24% w/v Span 40 which followed Korsmeyer-Peppas kinetics with non-Fickian diffusion.

Role of Sodium Dodecyl Sulfate in Tailoring the Rheological Properties of High-Strength Gelatin Hydrogels

Gelatin hydrogels are widely used materials that may require surfactants to adjust their solution’s surface tension for cell attachment, surface adsorption enhancement, or foaming. However, gelatin is a highly surface-active polymer, and its concentrated solutions usually do not require surfactants to achieve low surface tension. However, anionic surfactants, such as sodium dodecyl sulfate (SDS), interact strongly with gelatin to form complexes that impact its hydrogels’ rheological properties, influencing processability and functionality. Nevertheless, there is a lack of systematic research on the impact of these complexes on high gelatin content (i.e., high strength) hydrogels’ rheological properties. In this work, the SDS/gelatin ratio-dependent viscoelastic properties (e.g., gel strength, gelation kinetics, and melting/gelling temperature) of high-strength gelatin hydrogels were investigated using rheology and correlated to surface tension, viscometry, FTIR, and UV-Vis spectrophotometry. SDS–gelatin ratio was proved to be an important factor in tailoring the rheological properties of gelatin hydrogels. The gel strength, gelation kinetics, and melting/gelling temperature of the gelatin hydrogels linearly increased with SDS incorporation up to a maximum value, from which they started to decline. The findings of this work have wide applicability in tailoring the properties of gelatin–SDS solutions and hydrogels during their processing.

Chemically Fueled Self-sorted Hydrogels

Narcissistic self-sorting in supramolecular assemblies can help to construct materials with more complex hierarchies. Whereas controlled changes in pH or temperature have been used to this extent for two-component self-sorted gels, here we show that a chemically fueled approach can provide three-component materials with high precision. The latter materials have interesting mechanical properties, such as enhanced or suppressed stiffness, and intricate multi-step gelation kinetics. In addition, we show that we can achieve supramolecular templating, where pre-existing supramolecular fibers first act as a templates for growth of a second gelator, after which they can selectively be removed.

Regulating the Homogeneity of Thiol-Maleimide Michael-Type Addition-Based Hydrogels Using Amino Biomolecules

Poly(ethylene glycol) (PEG)-based synthetic hydrogels based on Michael-type addition reaction have been widely used for cell culture and tissue engineering. However, recent studies showed that these types of hydrogels were not homogenous as expected since micro domains generated due to the fast reaction kinetics. Here, we demonstrated a new kind of method to prepare homogenous poly(ethylene glycol) hydrogels based on Michael-type addition using the side chain amine-contained short peptides. By introducing such a kind of short peptides, the homogeneity of crosslinking and mechanical property of the hydrogels has been also significantly enhanced. The compressive mechanical and recovery properties of the homogeneous hydrogels prepared in the presence of side chain amine-contained short peptides were more reliable than those of inhomogeneous hydrogels while the excellent biocompatibility remained unchanged. Furthermore, the reaction rate and gelation kinetics of maleimide- and thiol-terminated PEG were proved to be significantly slowed down in the presence of the side chain amine-contained short peptides, thus leading to the improved homogeneity of the hydrogels. We anticipate that this new method can be widely applied to hydrogel preparation and modification based on Michael-type addition gelation.

Strongly Adhesive and Antimicrobial Peptide-Loaded, Alginate–Catechol-Based Gels for Application against Periimplantitis

Background: Periimplantitis is a disease linked to oral virulent bacteria such as P. gingivalis that grow in dental implants surrounding tissues and between implants and abutments. Antimicrobial gels previously described to fill these sites lose their effectiveness and resorb over time. Objective: Characterization of biophysical and antimicrobial properties of an original hydrogel, Alginate–Catechol (Alg–Cat), combined to D-Cateslytin (D-CTL). Methods: Gelation kinetics, frequency and strain sweep measurements were performed by rheology. Antibacterial activity of the gels was tested against P. gingivalis, and the MIC was determined. Peptides released from the gels were purified by HPLC and characterized by MALDI–TOF mass spectrometry. The behavior of bacteria in contact with the gel was observed using optical and electronic microscopy (SEM and TEM). Results: Gelation was fast and was achieved in 2 min with a storage modulus between 25 and 30 Pa. The gels were stable under strain and showed an adhesive potential reinforced with aging at 18 h (5.4 kPa) under a slow retraction speed (4 J·m−2 at 10 µm/s) with a mixed rupture profile (adhesive/cohesive). The MIC of D-CTL inside the Alg–Cat gel against P. gingivalis was equal to 470 µg·mL−1 after 24 h. Peptides recovered in the supernatant and inside the gel were fragmented, most of them conserving the ⍺-helix active site. No bacteria were visualized at the surface and inside the gel after 24 h. This gel is promising for clinical application for the prevention of periimplantitis.

Chemically Fueled Self-sorted Hydrogels

Narcissistic self-sorting in supramolecular assemblies can help to construct materials with more complex hierarchies. Whereas controlled changes in pH or temperature have been used to this extent for two-component self-sorted gels, here we show that a chemically fueled approach can provide three-component materials with high precision. The latter materials have interesting mechanical properties, such as enhanced or suppressed stiffness, and intricate multi-step gelation kinetics. In addition, we show that we can achieve supramolecular templating, where pre-existing supramolecular fibers first act as a templates for growth of a second gelator, after which they can selectively be removed.

Ex Vivo and In Vivo Properties of an Injectable Hydrogel Derived From Acellular Ear Cartilage Extracellular Matrix

Extracellular matrix (ECM) hydrogels provide advantages such as injectability, the ability to fill an irregularly shaped space, and the adequate bioactivity of native matrix. In this study, we developed decellularized cartilage ECM (dcECM) hydrogels from porcine ears innovatively via the main method of enzymatic digestion and verified good biocompatible properties of dcECM hydrogels to deliver chondrocytes and form subcutaneous cartilage in vivo. The scanning electron microscopy and turbidimetric gelation kinetics were used to characterize the material properties and gelation kinetics of the dcECM hydrogels. Then we evaluated the biocompatibility of hydrogels via the culture of chondrocytes in vitro. To further explore the dcECM hydrogels in vivo, grafts made from the mixture of dcECM hydrogels and chondrocytes were injected subcutaneously in nude mice for the gross and histological analysis. The structural and gelation kinetics of the dcECM hydrogels altered according to the variation in the ECM concentrations. The 10 mg/ml dcECM hydrogels could support the adhesion and proliferation of chondrocytes in vitro. In vivo, at 4 weeks after transplantation, cartilage-like tissues were detected in all groups with positive staining of toluidine blue, Safranin O, and collagen II, indicating the good gelation of dcECM hydrogels. While with the increasing concentration, the tissue engineering cartilages formed by 10 mg/ml dcECM hydrogel grafts were superior in weights, volumes, collagen, and glycosaminoglycan (GAG) content compared to the dcECM hydrogels of 1 mg/ml and 5 mg/ml. At 8 weeks after grafting, dcECM hydrogel grafts at 10 mg/ml showed very similar qualities to the control, collagen I grafts. After 12 weeks of in vivo culture, the histological analysis indicated that 10 mg/ml dcECM hydrogel grafts were similar to the normal cartilage from pig ears, which was the source tissue. In conclusion, dcECM hydrogel showed the promising potential as a tissue engineering biomaterial to improve the regeneration and heal injuries of ear cartilage.

Effect of Biodegradable Hydrophilic and Hydrophobic Emulsifiers on the Oleogels Containing Sunflower Wax and Sunflower Oil

The use of an appropriate oleogelator in the structuring of vegetable oil is a crucial point of consideration. Sunflower wax (SFW) is used as an oleogelator and displays an excellent potential to bind vegetable oils. The current study aimed to look for the effects of hydrophobic (SPAN-80) and hydrophilic (TWEEN-80) emulsifiers on the oleogels prepared using SFW and sunflower oil (SO). The biodegradability and all formulations showed globular crystals on their surface that varied in size and number. Wax ester, being the most abundant component of SFW, was found to produce fibrous and needle-like entanglements capable of binding more than 99% of SO. The formulations containing 3 mg of liquid emulsifiers in 20 g of oleogels showed better mechanical properties such as spreadability and lower firmness than the other tested concentrations. Although the FTIR spectra of all the formulations were similar, which indicated not much variation in the molecular interactions, XRD diffractograms confirmed the presence of β′ form of fat crystals. Further, the mentioned formulations also showed larger average crystallite sizes, which was supported by slow gelation kinetics. A characteristic melting point (Tm~60 °C) of triglyceride was visualized through DSC thermograms. However, a higher melting point in the case of few formulations suggests the possibility of even a stable β polymorph. The formed oleogels indicated the significant contribution of diffusion for curcumin release. Altogether, the use of SFW and SO oleogels with modified properties using biodegradable emulsifiers can be beneficial in replacing saturated fats and fat-derived products.