Search Results (34)

The enhancement of gel properties in chicken myofibrillar proteins (MPs) is a crucial objective in meat processing. In this experiment, we systematically investigated the effects of lentinan (LNT) on MP gel formation ability and three-dimensional network structure features through multi-scale structural characterization and molecular interactions analysis and elucidated the molecular pathways of their molecular actions in regulating gel properties. The addition of LNT (0–2%, w/v) significantly enhanced the water-holding capacity (WHC), textural, and rheological properties of LNT-MPs. As the concentration of LNT increased, the hydrophobic and electrostatic interactions became more pronounced. Conversely, the contribution from disulfide bonds exhibited an inverse relationship, with hydrogen bonds demonstrating the least impact. Subsequently, the α-helix content decreased from 23.75% to 22.64%, and the β-fold content increased from 28.03% to 29.22%, suggesting that the protein aggregates reorganized to form larger aggregates, which contributed to forming a more stable network structure of gels. This investigation establishes LNT’s capacity to modify the gelation mechanisms of MPs. These outcomes offer crucial insights for implementing fungal polysaccharides in processed meat product development. Full article

Glycerohydrogels based on silicon glycerolate, chitosan (CS) and polyvinyl alcohol (PVA) are widely studied for use in biomedical applications. In line with the general trend of replacing synthetic polymers with natural ones in such compositions, it would be of interest to replace PVA with the polysaccharide glucomannan (GM), as well as to introduce functional additives to impart the desired properties, including gelation time, to the final hydrogel. In this work, a comprehensive study of the preparation conditions and properties of glycerohydrogels based on silicon tetraglycerolate, chitosan hydrochloride (CS·HCl) and GM was carried out. Viscometry was used to assess the conformational state of CS·HCl and GM macromolecules, and their associates in solution before gelation. Gelation was studied using the vessel inversion method. The mucoadhesive and the dermoadhesive properties of the glycerohydrogels obtained were assessed using the tearing off method from the model substrates simulating mucous and dermal tissues. The conformational state of the individual polymers and their mixed associates in solution before gelation was estimated; the intrinsic viscosity and the hydrodynamic radius of the macromolecular coils were calculated. The influence of various factors (addition of ε-aminocaproic and hydrochloric acids, sodium chloride, hydroxide and tetraborate to vary the acidity and ionic strength of the medium, as well as temperature) and the molecular weight of chitosan on the gelation time was studied. The gelation time achieved was less than 2 min, which is promising in practical terms, i.e., for creating liquid plasters. Our best samples are not inferior to the commercial preparation “Metrogyl Denta”^® in terms of tearing force during mucoadhesion and dermoadhesion at short gelation times. Thus, the glycerohydrogels synthesized by us and based on silicon tetraglycerolate, CS·HCl and GM could find usage in new biopharmaceutical and biomedical applications. Full article

This study aimed to evaluate the influence of indirect-plasma-treated water (IPTW) in the preparation of hydrogels. Three commonly used natural, biodegradable polymers with the ability to form gels were selected: gelatin, carrageenan, and sodium alginate. The pH, gelling temperature, texture profile, swelling degree, and color of hydrogels were evaluated, and the polymers were subjected to Fourier-transform infrared (FTIR) spectroscopy. The morphology of the hydrogels was investigated using Scanning Electron Microscopy (SEM). Additionally, the physiochemical properties of the water media, which were distilled water (DW) and IPTW, were analyzed. The results indicated that the gels prepared using IPTW were characterized by a lower pH, higher hardness and lower gelation temperature. After 48 h of swelling ratio (SR) testing, gelatin and alginate hydrogels made with IPTW were characterized by lower SR, while an inverse relationship was found in the case of SR of carrageenan gels. The FTIR analysis confirmed changes in the water binding ability. The use of IPTW also significantly affected the microstructure of the tested materials. A statistically significant change in the color of IPTW gel samples was also noted. The results showed that IPTW induces physicochemical changes in hydrogels, which can lead to the enhancement of their practical applications. Full article

Pullulan is a polysaccharide that has attracted the attention of scientists in recent times as a former of edible films. On the other hand, its use for the preparation of hydrogels needs more study, as well as the formation of pullulan microcapsules as active ingredient release systems for the food industry. Due to the slow gelation kinetics of pullulan with sodium trimetaphosphate (STMP), capsules cannot be formed through the conventional method of dropping into a solution of the gelling agent, as with other polysaccharides, since the pullulan chains migrate to the medium before the capsules can form by gelation. Pullulan microcapsules have been obtained by using inverse water-in-oil emulsions as templates. The emulsion that acts as a template has been characterized by monitoring its stability and by optical microscopy, and the size of the emulsion droplets has been correlated with the size of the microcapsules obtained, demonstrating that it is a good technique for their production. Although some flocs of droplets form, these remain dispersed during the gelation process and two capsule size distributions are obtained: those of the non-flocculated droplets and the flocculated droplets. The microcapsules have been evaluated as vitamin C release systems, showing zero-order release kinetics for acidic pH and Fickian mechanism for neutral pH. On the other hand, the microcapsules offer good protection of vitamin C against oxidation during an evaluation period of 14 days. Full article

The gelation kinetics of agar aqueous solutions were studied by means of the viscosity flow curves using a coaxial Couette cylinder viscometer. The viscosity curves show an unusual sigmoidal trend or an exponential decay to a viscous steady state. An original theory of gelation kinetics was developed considering the coarsening of increasingly larger and more stable clusters due to Ostwald ripening and the breakup of clusters that were too large due to the instability of rotating large particles induced by the shear rate. The developed Bounded Ripening Growth model takes into account the trend of the viscosity curves by means of an autocatalytic process with negative feedback on aggregation according to the logistic kinetic equation, in which the constants $k_1(\gamma )$ and $k_{-}(\nu )$ are governed by the surface tension and shear rate, respectively. A dimensionless equation based on the difference between the Weber number and the ratio of the inverse kinetic constant to forward constant, accounts for the behavior of the dispersed phase in equilibrium conditions or far from the hydrostatic equilibrium. Full article

Polysilsesquioxane (PSQ) microspheres have shown promise in many fields, but previous studies about porous PSQ microspheres are scarce. Herein, we fabricated novel micron-sized thiol-functional polysilsesquioxane (TMPSQ) microspheres with open and interconnected macropores by combining inverse suspension polymerization with two-step sol–gel and polymerization-induced phase separation processes, without using phase-separation-promoting additives or sacrificial templates. The chemical composition of the TMPSQ microspheres was confirmed using FTIR and Raman spectroscopy. The morphology of the TMPSQ microspheres was characterized using SEM and TEM. TGA was employed to test the thermal stability of the TMPSQ microspheres. Mercury intrusion porosimetry and nitrogen adsorption–desorption tests were performed to investigate the pore structure of the TMPSQ microspheres. The results showed that the TMPSQ microspheres had open and interconnected macropores with a pore size of 839 nm, and the total porosity and intraparticle porosity reached 70.54% and 43.21%, respectively. The mechanism of porous generation was proposed based on the morphological evolution observed using optical microscopy. The macropores were formed through the following four steps: phase separation (spinodal decomposition), coarsening, gelation, and evaporation of the solvent. The macropores can facilitate the rapid mass transfer between the outer and inner spaces of the TMPSQ microspheres. The TMPSQ microspheres are promising in various fields, such as catalyst supports and adsorbents. Full article

During the preparation of cotton cellulose hydrogels using the phase inversion gelation method of N,N-dimethylacetamide/LiCl solution under ethanol vapor, acetone (AC), methyl ethyl ketone (MEK), or diethyl ketone (DEK) were added as additives, and their gelation state and the properties of the resulting hydrogels were evaluated. Adding the ketones to the cellulose solution caused an increase in the gelation time, but the solution viscosity decreased, indicating that the cellulose tended to aggregate in the solution. Among the hydrogels prepared by adding ketones, the water content was as high as 2050%, especially for AC and MEK. In these hydrogels, cellulose formed an agglomerated fibrous network of a few micron widths, forming a tuft-like entrapment space of about 10 to 100 μm size. The structure surrounded water and held it in the hydrogels. The FTIR results showed that the water, which formed hydrogen bonds, was retained within the hydrogel network. This structural configuration was determined to be conducive to maintaining the gel state against external deformation forces, especially in the case of the addition of MEK. Full article

The use of nanoemulsions as encapsulation systems for active ingredients, such as cinnamon oil, has been studied. A surfactant based on polyoxyethylene glycerol esters from coconut/palm kernel oil has been used. The nanoemulsions were obtained by the two most commonly low-energy emulsification methods, the composition inversion phase (PIC) and the temperature inversion phase (PIT) methods. Nanoemulsions were successfully obtained by both methods, with very small droplet sizes (5–14 nm) in both cases, but a greater stability was observed when the PIT method was used. Nanoemulsions were encapsulated by external gelation using two different polysaccharides, alginate or chitosan, dissolved in the continuous phase of the nanoemulsion. Then, the nanoemulsion was dropped into a bath with a gelling agent. To improve the release control of cinnamon oil and avoid the burst effect, beads prepared with one of the polysaccharides were coated with the second polysaccharide and then gelled again. Double gelled beads were successfully obtained, the core with chitosan and the outer layer (shell) with alginate. SEM images showed the morphology of the single beads presenting high porosity. When the beads were coated, the porosity decreased because the second polysaccharide molecules covered the pre-existing pores. The smoother surface was obtained when this second layer was, in turn, gelled. The release patterns at pH = 2 and pH = 7 were studied. It was observed that the double gelled bead provided a more gradual release, but maintained approximately the same amount of final released oil. The release patterns were fitted to the Korsmeyer-Peppas model. The fitting parameters reflected the effect of the different coating layers, correlating with different diffusion mechanisms according to the bead core and shell materials. Full article

Molecular gels, which are soft and flexible materials, are candidates for healthcare, cosmetic base, and electronic applications as new materials. In this study, a new polymeric organogelator bearing a polyrotaxane (PR) structure was developed and could induce the gelation of N′,N″-dimethylformamide (DMF), a known solvent for dissolving polymeric materials and salts. Furthermore, the resulting DMF molecular gels exhibited thixotropic properties, observed by the inversion method using vials, which are essential for gel spreading. The scanning electron microscopy of the xerogels suggested that the gel-forming ability and thixotropic property of gels were imparted by the network of the laminated aggregates of thin layer material similar to those of other gels made of clay materials. This thin layer material would be formed by the aggregation of polymeric organogelators. The dynamic viscoelasticity measurements of the obtained gels revealed the stability and pseudo-thixotropic behaviors of the obtained gels, as well as a specific concentration effect on the mechanical behavior of the gels attributed to the introduction of the PR structure. Additionally, the preparation of the polymer organogelator/polymer composites was investigated to improve the mechanical properties via the filler effect induced by the agglomerates of organogelator. Moreover, the tensile tests confirmed that the introduction of the gelator enhanced the mechanical properties of the composites. Full article

The production of aerogels for different applications has been widely known, but the use of polysaccharide-based aerogels for pharmaceutical applications, specifically as drug carriers for wound healing, is being recently explored. The main focus of this work is the production and characterization of drug-loaded aerogel capsules through prilling in tandem with supercritical extraction. In particular, drug-loaded particles were produced by a recently developed inverse gelation method through prilling in a coaxial configuration. Particles were loaded with ketoprofen lysinate, which was used as a model drug. The core-shell particles manufactured by prilling were subjected to a supercritical drying process with CO₂ that led to capsules formed by a wide hollow cavity and a tunable thin aerogel layer (40 μm) made of alginate, which presented good textural properties in terms of porosity (89.9% and 95.3%) and a surface area up to 417.0 m²/g. Such properties allowed the hollow aerogel particles to absorb a high amount of wound fluid moving very quickly (less than 30 s) into a conformable hydrogel in the wound cavity, prolonging drug release (till 72 h) due to the in situ formed hydrogel that acted as a barrier to drug diffusion. Full article

Selective delivery of anticancer drug molecules to the tumor site enhances local drug dosages, which leads to the death of cancer cells while simultaneously minimizing the negative effects of chemotherapy on other tissues, thereby improving the patient’s quality of life. To address this need, we developed reduction-responsive chitosan-based injectable hydrogels via the inverse electron demand Diels–Alder reaction between tetrazine groups of disulfide-based cross-linkers and norbornene groups of chitosan derivatives, which were applied to the controlled delivery of doxorubicin (DOX). The swelling ratio, gelation time (90–500 s), mechanical strength (G’~350–850 Pa), network morphology, and drug-loading efficiency (≥92%) of developed hydrogels were investigated. The in vitro release studies of the DOX-loaded hydrogels were performed at pH 7.4 and 5.0 with and without DTT (10 mM). The biocompatibility of pure hydrogel and the in vitro anticancer activity of DOX-loaded hydrogels were demonstrated via MTT assay on HEK-293 and HT-29 cancer cell lines, respectively. Full article

Macroscopic spatial patterns were formed in calcium alginate gels when a drop of a calcium nitrate solution was placed on the center of a sodium alginate solution on a petri dish. These patterns have been classified into two groups. One is multi-concentric rings consisting of alternating cloudy and transparent areas observed around the center of petri dishes. The other is streaks extending to the edge of the petri dish, which are formed to surround the concentric bands between the concentric bands and the petri dish edge. We have attempted to understand the origins of the pattern formations using the properties of phase separation and gelation. The distance between two adjacent concentric rings was roughly proportional to the distance from where the calcium nitrate solution was dropped. The proportional factor p increased exponentially for the inverse of the absolute temperature of the preparation. The p also depended on the concentration of alginate. The pattern characteristics in the concentric pattern agreed with those in the Liesegang pattern. The paths of radial streaks were disturbed at high temperatures. The length of these streaks shortened with increasing alginate concentration. The characteristics of the streaks were similar to those of crack patterns resulting from inhomogeneous shrinkage during drying. Full article

As the market for plant-based meat analogs grows, the development of plant-based animal fat analogs has become increasingly important. In this study, we propose an approach by developing a gelled emulsion based on sodium alginate, soybean oil (SO), and pea protein isolate. Formulations containing 15% to 70% (w/w) SO were successfully produced without phase inversion. The addition of more SO resulted in pre-gelled emulsions with a more elastic behavior. After the emulsion was gelled in the presence of calcium, the color of the gelled emulsion changed to light yellow, and the formulation containing 70% SO exhibited a color most similar to actual beef fat trimming. The lightness and yellowness values were greatly influenced by the concentrations of both SO and pea protein. Microscopic images revealed that pea protein formed an interfacial film around the oil droplets, and the oil was more tightly packed at higher oil concentrations. Differential scanning calorimetry showed that lipid crystallization of the gelled SO was influenced by the confinement of the alginate gelation, but the melting behavior was like that of free SO. FTIR spectrum analysis indicated a potential interaction between alginate and pea protein, but the functional groups of SO were unchanged. Under mild heating conditions, gelled SO exhibited an oil loss similar to that observed in actual beef trims. The developed product has the potential to mimic the appearance and slow-rendering melting attribute of real animal fat. Full article

Nanoemulsions have been widely studied as lipophilic compound loading systems. A low-energy emulsification method, phase inversion composition (PIC), was used to prepare oil-in-water nanoemulsions in a carvacrol–coconut oil/Tween 80^®–(linoleic acid–potassium linoleate)/water system. The phase behaviour of several emulsification paths was studied and related to the composition range in which small-sized stable nanoemulsions could be obtained. An experimental design was carried out to determine the best formulation in terms of size and stability. Nanoemulsions with a very small mean droplet diameter (16–20 nm) were obtained and successfully encapsulated to add carvacrol to foods as a natural antimicrobial and antioxidant agent. They were encapsulated into alginate beads by external gelation. In order to improve the carvacrol kinetics release, the beads were coated with two different biopolymers: chitosan and pullulan. All formulations were analysed with scanning electron microscopy to investigate the surface morphology. The release patterns at different pHs were evaluated. Different kinetics release models were fitted in order to study the release mechanisms affecting each formulation. Chitosan-coated beads avoided the initial release burst effect, improving the beads’ structure and producing a Fickian release. At basic pH, the chitosan-coated beads collapsed and the pullulan-coated beads moderately improved the release pattern of the alginate beads. For acid and neutral pHs, the chitosan-coated beads presented more sustained release patterns. Full article

The weak point of ionic liquids is their high viscosity, limiting the maximum polymer concentration in the forming solutions. A low-viscous co-solvent can reduce viscosity, but cellulose has none. This study demonstrates that dimethyl sulfoxide (DMSO), being non-solvent for cellulose, can act as a nominal co-solvent to improve its processing into a nanofiltration membrane by phase inversion. A study of the rheology of cellulose solutions in diluted ionic liquids ([EMIM]Ac, [EMIM]Cl, and [BMIM]Ac) containing up to 75% DMSO showed the possibility of decreasing the viscosity by up to 50 times while keeping the same cellulose concentration. Surprisingly, typical cellulose non-solvents (water, methanol, ethanol, and isopropanol) behave similarly, reducing the viscosity at low doses but causing structuring of the cellulose solution and its phase separation at high concentrations. According to laser interferometry, the nature of these non-solvents affects the mass transfer direction relative to the forming membrane and the substance interdiffusion rate, which increases by four-fold when passing from isopropanol to methanol or water. Examination of the nanofiltration characteristics of the obtained membranes showed that the dilution of ionic liquid enhances the rejection without changing the permeability, while the transition to alcohols increases the permeability while maintaining the rejection. Full article