Search Results (30)

This research explores the utilization of chitosan, a naturally derived biopolymer, as an innovative additive in bitumen for road construction. The experimental procedure for incorporating chitosan into bitumen, in agreement with its thermal stability, is described. Four different types of chitosan (two different degrees of deacetylation: >75 and >90% in free amine groups; molecular weight ranging from 100 to 800 kD) have been considered. Each chitosan was added to a bitumen at 1, 3, 6 wt%, and the mechanical characteristics were tested by dynamic shear rheology with the aim of testing the thermal stability of modified bitumen. An increase in the gel-to-sol temperature transition was generally found in the presence of chitosan, suggesting enhanced resistance to deformation under traffic loads. The most marked effect was obtained for chitosan with a molecular weight of 310,000–375,000 kD and with a deacetylation degree ≥75% (free amine groups). In addition, it was found that chitosan can slow down the oxidative aging of bitumen, especially when chitosan with high molecular weight (600,000–800,000 kD) and with a deacetylation degree >90% (free amine groups) was used. This further finding suggests that chitosan can potentially extend the final road pavement life. Full article

Central composite design (CCD) is a statistical experimental design technique that utilizes a combination of factorial and axial points to study the effects of multiple variables on a response. This study focused on optimizing hydrogel formulations for 3D printing using CCD. Three biopolymers were selected: sodium alginate (SA), gelatin (GEL), and carboxymethyl cellulose (CMC). The maximum and minimum concentrations of each polymer were established using a Google Scholar search, and CCD was employed to generate various combinations for hydrogel preparation. The hydrogels were characterized in accordance with their swelling degree (SD) in phosphate-buffered saline (PBS) and Dulbecco’s Modified Eagle Medium (DMEM), as well as their printability in 2D and 3D assays. The formulation consisting of 7.5% SA, 7.5% GEL, and 2.5% CMC exhibited the best swelling properties and exceptional printability, surpassing all other tested formulations. This study highlights the effectiveness of design of experiment methodologies in accelerating the development of optimized hydrogel formulations for various applications in 3D printing and suggests avenues for future research to explore their performance in specific biological contexts. Full article

Inks based on soybean protein isolate (SPI) were developed and their formulations were optimized as a function of the ink heat treatment and the content of other biopolymers to assess the effects of protein–polysaccharides and protein–protein interactions. First, the rheological behavior of the inks was analyzed in relation to the polyvinyl alcohol (PVA) concentration employed (20, 25, and 30 wt%) and, as a result of the analysis, the ink with 25 wt% PVA was selected. Additionally, sodium alginate (SA) and gelatin (GEL) were added to the formulations to improve the viscoelastic properties of the inks and the effect of the SA or GEL concentrations (1, 2, and 3 wt%) was studied. All inks showed shear thinning behavior and self-supporting abilities. Among all the 3D printed scaffolds, those with higher SA (3 wt%) or GEL (2 and 3 wt%) content showed higher shape fidelity and were selected for further characterization. Texture profile analysis demonstrated that the scaffolds prepared with previously heat-treated inks containing 3 wt% GEL showed the highest strength. Additionally, these scaffolds showed a higher water-uptake capacity profile. Full article

Seaweeds, rich in high-value polysaccharides with thickening/gelling properties (e.g., agar, carrageenan, and alginate), are extensively used in the food industry for texture customization and enhancement. However, conventional extraction methods for these hydrocolloids often involve potentially hazardous chemicals and long extraction times. In this study, three red seaweed species (Chondrus crispus, Gelidium Corneum, and Gracilaria gracilis) commercialized as food ingredients by local companies were chosen for their native gelling biopolymers, which were extracted using water-based methodologies (i.e., (1) hydration at room temperature; (2) stirring at 90 °C; and (3) centrifugation at 40 °C) for production of sustainable food gels. The potential use of these extracts as bioinks was assessed employing an extrusion-based 3D printer. The present work aimed to study the gelation process, taken place during printing, and assess the effectiveness of the selected green extraction method in producing gels. To improve the definition of the printed gel, two critical printing parameters were investigated: the addition of locust bean gum (LBG) at different concentrations (0, 0.5, 1, 1.5, 2, and 2.5%) and printing temperature (30, 40, 60, and 80 °C). Rheological results from a controlled-stress rheometer indicated that gels derived from G. corneum and G. gracilis exhibited a lower gel strength (lower G′ and G″) and excessive material spreading during deposition (lower viscosity) than C. crispus. Thus, G′ was around 5 and 70 times higher for C. crispus gels than for G. corneum and G. gracilis, respectively. When increasing LBG concentration (0.5 to 2.5% w/w) and lowering the printing temperature (80 to 30 °C), an enhanced gel matrix definition for G. corneum and G. gracilis gels was found. In contrast, gels from C. crispus demonstrated greater stability and were less influenced by these parameters, showcasing the potential of the seaweed to develop sustainable clean label food gels. Eventually, these results highlight the feasibility of using algal-based extracts obtained through a green procedure as bioinks where LBG was employed as a synergic ingredient. Full article

Background: Gelatin–xanthan gum (Gel–Xnt) hydrogel has been previously modified to improve its printability; now, to increase its ability for use as cell-laden 3D scaffolds (bioink), polydopamine (PDA), a biocompatible, antibacterial, adhesive, and antioxidant mussel-inspired biopolymer, has been added (1–3% v/v) to hydrogel. Methods: Control (CT) and PDA-blended hydrogels were used to print 1 cm² grids. The hydrogels’ printability, moisture, swelling, hydrolysis, and porosity were tested after glutaraldehyde (GTA) crosslinking, while biocompatibility was tested using primary human-derived skin fibroblasts and spontaneously immortalized human keratinocytes (HaCaT). Keratinocyte or fibroblast suspension (100 µL, 2.5 × 10⁵ cells) was combined with an uncrosslinked CT and PDA blended hydrogel to fabricate cylinders (0.5 cm high, 1 cm wide). These cylinders were then cross-linked and incubated for 1, 3, 7, 14, and 21 days. The presence of cells within various hydrogels was assessed using optical microscopy. Results and discussion: PDA blending did not modify the hydrogel printability or physiochemical characteristics, suggesting that PDA did not interfere with GTA crosslinking. On the other hand, PDA presence strongly accelerated and increased both fibroblast and keratinocyte growth inside. This effect seemed to be linked to the adhesive abilities of PDA, which improve cell adhesion and, in turn, proliferation. Conclusions: The simple PDA blending method described could help in obtaining a new bioink for the development of innovative 3D-printed wound dressings. Full article

Hyaluronan (HA) is a natural biodegradable biopolymer; its biological functions include cell adhesion, cell proliferation, and differentiation as well as decreasing inflammation, angiogenesis, and regeneration of damaged tissue. This makes it a suitable candidate for fabricating nanomaterials with potential use in tissue engineering. However, HA nanofiber production is restricted due to the high viscosity, low evaporation rate, and high surface tension of HA solutions. Here, hybrids in the form of continuous and randomly aligned polyvinyl alcohol (PVA)–(HA)–siloxane nanofibers were obtained using an electrospinning process. PVA–HA fibers were crosslinked by a 3D siloxane organic–inorganic matrix via sol-gel that restricts natural hydrophilicity and stiffens the structure. The hybrid nanofiber mats were characterized by FT-IR, micro-Raman spectroscopy, SEM, and biological properties. The PVA/HA ratio influenced the morphology of the hybrid nanofibers. Nanofibers with high PVA content (10PVA-8 and 10PVA-10) form mats with few beaded nanofibers, while those with high HA content (5PVA-8 and 5PVA-10) exhibit mats with mound patterns formed by “ribbon-like” nanofibers. The hybrid nanofibers were used as mats to support osteoblast growth, and they showed outstanding biological properties supporting cell adhesion, cell proliferation, and cell differentiation. Importantly, the 5PVA-8 mats show 3D spherical osteoblast morphology; this suggests the formation of tissue growth. These novel HA-based nanomaterials represent a relevant advance in designing nanofibers with unique properties for potential tissue regeneration. Full article

The aim of this work was to develop sustainable patches for wound application, using the biopolymer starch, created using a low-cost 3D printing PAM device. The composition of a starch gel was optimized for PAM extrusion: corn starch 10% w/w, β-glucan water suspension (filler, 1% w/w), glycerol (plasticizer, 29% w/w), and water 60% w/w. The most suitable 3D printing parameters were optimized as well (nozzle size 0.8 mm, layer height 0.2 mm, infill 100%, volumetric flow rate 3.02 mm³/s, and print speed 15 mm/s). The suitable conditions for post-printing drying were set at 37 °C for 24 h. The obtained patch was homogenous but with low mechanical resistance. To solve this problem, the starch gel was extruded over an alginate support, which, after drying, becomes an integral part of the product, constituting the backing layer of the final formulation. This approach significantly improved the physicochemical and post-printing properties of the final bilayer patch, showing suitable mechanical properties such as elastic modulus (3.80 ± 0.82 MPa), strength (0.92 ± 0.08 MPa), and deformation at break (50 ± 1%). The obtained results suggest the possibility of low-cost production of patches for wound treatment by additive manufacturing technology. Full article

Pectin hydrogels have garnered significant attention in the food industry due to their remarkable versatility and promising properties. As a naturally occurring polysaccharide, pectin forms three-dimensional (3D) hydrophilic polymer networks, endowing these hydrogels with softness, flexibility, and biocompatibility. Their exceptional attributes surpass those of other biopolymer gels, exhibiting rapid gelation, higher melting points, and efficient carrier capabilities for flavoring and fat barriers. This review provides an overview of the current state of pectin gelling mechanisms and the classification of hydrogels, as well as their crosslinking types, as investigated through diverse research endeavors worldwide. The preparation of pectin hydrogels is categorized into specific gel types, including hydrogels, cryogels, aerogels, xerogels, and oleogels. Each preparation process is thoroughly discussed, shedding light on how it impacts the properties of pectin gels. Furthermore, the review delves into the various crosslinking methods used to form hydrogels, with a focus on physical, chemical, and interpenetrating polymer network (IPN) approaches. Understanding these crosslinking mechanisms is crucial to harnessing the full potential of pectin hydrogels for food-related applications. The review aims to provide valuable insights into the diverse applications of pectin hydrogels in the food industry, motivating further exploration to cater to consumer demands and advance food technology. By exploiting the unique properties of pectin hydrogels, food formulations can be enhanced with encapsulated bioactive substances, improved stability, and controlled release. Additionally, the exploration of different crosslinking methods expands the horizons of potential applications. Full article

Innovative materials are needed to produce scaffolds for various tissue engineering and regenerative medicine (TERM) applications, including tissue models. Materials derived from natural sources that offer low production costs, easy availability, and high bioactivity are highly preferred. Chicken egg white (EW) is an overlooked protein-based material. Whilst its combination with the biopolymer gelatin has been investigated in the food technology industry, mixed hydrocolloids of EW and gelatin have not been reported in TERM. This paper investigates these hydrocolloids as a suitable platform for hydrogel-based tissue engineering, including 2D coating films, miniaturized 3D hydrogels in microfluidic devices, and 3D hydrogel scaffolds. Rheological assessment of the hydrocolloid solutions suggested that temperature and EW concentration can be used to fine-tune the viscosity of the ensuing gels. Fabricated thin 2D hydrocolloid films presented globular nano-topography and in vitro cell work showed that the mixed hydrocolloids had increased cell growth compared with EW films. Results showed that hydrocolloids of EW and gelatin can be used for creating a 3D hydrogel environment for cell studies inside microfluidic devices. Finally, 3D hydrogel scaffolds were fabricated by sequential temperature-dependent gelation followed by chemical cross-linking of the polymeric network of the hydrogel for added mechanical strength and stability. These 3D hydrogel scaffolds displayed pores, lamellae, globular nano-topography, tunable mechanical properties, high affinity for water, and cell proliferation and penetration properties. In conclusion, the large range of properties and characteristics of these materials provide a strong potential for a large variety of TERM applications, including cancer models, organoid growth, compatibility with bioprinting, or implantable devices. Full article

The production of customized polymeric hydrogels in the form of 3D scaffolds with application in bone tissue engineering is currently a topic of great interest. Based on gelatin methacryloyl (GelMa) as one of the most popular used biomaterials, GelMa with two different methacryloylation degrees (DM) was obtained, to achieve crosslinked polymer networks by photoinitiated radical polymerization. In this work, we present the obtention of new 3D foamed scaffolds based on ternary copolymers of GelMa with vinylpyrrolidone (VP) and 2-hydroxyethylmethacrylate (HEMA). All biopolymers obtained in this work were characterized by infrared spectroscopy (FTIR) and thermogravimetric analysis (TGA), whose results confirm the presence of all copolymers in the crosslinked biomaterial. In addition, scanning electron microscopy (SEM) pictures were obtained verifying the presence of the porosity created by freeze-drying process. In addition, the variation in its swelling degree and its enzymatic degradation in vitro was analyzed as a function of the different copolymers obtained. This has allowed us to observe good control of the variation in these properties described above in a simple way by varying the composition of the different comonomers used. Finally, with these concepts in mind, biopolymers obtained were tested through assessment of several biological parameters such as cell viability and differentiation with MC3T3-E1 pre-osteoblastic cell line. Results obtained show that these biopolymers maintain good results in terms of cell viability and differentiation, along with tunable properties in terms of hydrophilic character, mechanical properties and enzymatic degradation. Full article

The aim of this work was to study the influence of water as a co-solvent on the interaction between a polymerizable ionic liquid—choline acrylate (ChA)—and bacterial cellulose. Bacterial cellulose dispersed in ChA is a new type of UV-curable biopolymer-based ink that is a prospective material for the 3D printing of green composite ion-gels. Higher cellulose content in inks is beneficial for the ecological and mechanical properties of materials, and leads to increased viscosity and the yield stress of such systems and hampers printability. It was found that the addition of water results in (1) a decrease in the solvent viscosity and yield stress; and (2) a decrease in the stability of dispersion toward phase separation under stress. In this work, an optimal composition in the range of 30–40 wt% water content demonstrating 97–160 Pa of yield stress was found that ensures the printability and stability of inks. The rheological properties of inks and mechanical characteristics (0.7–0.8 MPa strength and 1.1–1.2 MPa Young’s modulus) were obtained. The mechanism of influence of the ratio ChA/water on the properties of ink was revealed with atomic force microscopy, wide-angle X-ray diffraction studies of bacterial cellulose after regeneration from solvent, and computer simulation of ChA/water mixtures and their interaction with the cellulose surface. Full article

Hydrocolloids are long-chain biopolymers that can form viscous solutions or gels when dissolved in water. They are employed as rheological modifiers in various manufacturing processes or finished products. Due to its unique gelation properties, animal gelatin is one of the most widely used hydrocolloids, finding applications in several fields such as food, pharmaceutical, and photographic. Nowadays, the challenge of finding valid alternatives to animal products has become a crucial issue, for both ethical and environmental reasons. The aim of this work, is to propose a green hydrocolloidal network, able to reproduce the gelation features of animal gelatin gels. κ-carrageenan gels may be an interesting alternative to gelatin, due to their attractive gelling features. We investigate the thermorheological behavior of κ-carrageenan aqueous solutions at various concentrations, focusing on gel features such as transition temperature and gel strength. To improve the viscoelastic response of such gels, we add a viscosity-enhancing hydrocolloid, i.e., xanthan gum. The results show that the gel strength increases exponentially with xanthan concentration, thus suggesting a synergistic interaction between the two networks. We also study the effect of sucrose on the thermal and mechanical properties of modified gels, finding a marked increase in transition temperatures and gel elasticity. In recent years, three-dimensional (3D) food printing has been extensively studied in the food industry, due to its many advantages, such as customized food design, personalized nutrition, simplified supply chain, and the expansion of available food materials. In view of this growing interest for additive manufacturing, we also study the printability of the complete formulation composed of κ-carrageenan, xanthan gum and sucrose. Full article

Silica-based ceramics doped with calcium and magnesium have been proposed as suitable materials for scaffold fabrication. Akermanite (Ca₂MgSi₂O₇) has attracted interest for bone regeneration due to its controllable biodegradation rate, improved mechanical properties, and high apatite-forming ability. Despite the profound advantages, ceramic scaffolds provide weak fracture resistance. The use of synthetic biopolymers such as poly(lactic-co-glycolic acid) (PLGA) as coating materials improves the mechanical performance of ceramic scaffolds and tailors their degradation rate. Moxifloxacin (MOX) is an antibiotic with antimicrobial activity against numerous aerobic and anaerobic bacteria. In this study, silica-based nanoparticles (NPs) enriched with calcium and magnesium, as well as copper and strontium ions that induce angiogenesis and osteogenesis, respectively, were incorporated into the PLGA coating. The aim was to produce composite akermanite/PLGA/NPs/MOX-loaded scaffolds through the foam replica technique combined with the sol–gel method to improve the overall effectiveness towards bone regeneration. The structural and physicochemical characterizations were evaluated. Their mechanical properties, apatite forming ability, degradation, pharmacokinetics, and hemocompatibility were also investigated. The addition of NPs improved the compressive strength, hemocompatibility, and in vitro degradation of the composite scaffolds, resulting in them keeping a 3D porous structure and a more prolonged release profile of MOX that makes them promising for bone regeneration applications. Full article

Biopolymers based on the amniotic membrane compare favorably with synthetic materials in that, along with a specific 2D structure, they have biologically active properties. However, in recent years, there has been a tendency to perform decellularization of the biomaterial during the preparation of the scaffold. In this study, we studied the microstructure of 157 samples and identified individual biological components in the manufacture of a medical biopolymer from an amniotic membrane using various methods. Group 1 had 55 samples, and the amniotic membrane was impregnated with glycerol and dried over silica gel. Group 2 had 48 samples, and the decellularized amniotic membrane was impregnated with glycerol followed by lyophilization, Group 3 had 44 samples, and the decellularized amniotic membrane without pre-impregnation with glycerol was subjected to lyophilization. Decellularization was performed by treatment with a low-frequency ultrasound at a frequency of 24–40 kHz in an ultrasonic bath. A morphological study using a light microscope and a scanning electron microscope showed the preservation of the structure of the biomaterial and more complete decellularization in samples subjected to lyophilization without prior impregnation with glycerol. The study of the Raman spectroscopy lines of a biopolymer made from a lyophilized amniotic membrane without preliminary impregnation with glycerin showed significant differences in the intensity of the spectral lines of amides, glycogen, and proline. Additionally, in these samples, the spectral lines of Raman scattering the characteristic of glycerol were not visualized; therefore, only biological substances characteristic of the native amniotic membrane have been preserved. Full article

The aim of the study was to characterize raw aqueous extracts from Plantago ovata husk in terms of molecular chain mass, osmotic, hydrodynamic, and rheological properties. The raw extracts used in this study have not been yet investigated in the indicated research area. Determination of the molecular weight of the chains present in the extract was performed by gel permeation chromatography (GPC). Osmotic properties were characterized using membrane osmometry. Rheological properties were investigated via classical rotational rheology with normal force measurements, as well as less common but equally important measurements of extensional viscosity. Two types of chains with an average molecular mass of 200 and 1780 kDa were found. The values of the first virial coefficient (B₂) indicate the predominance of biopolymer-biopolymer interactions. The hydrodynamic radius established at 25 and 30 °C was 74 and 67 nm, respectively, and lower than at 40 °C (>600 nm). The first critical concentration was determined: $c^{*}=0.11 \mathrm{g}·{\mathrm{dL}}^{-1}$. The dominance of negative normal force values resulting from the formation of a pseudo-gel structure of the heteroxylates was demonstrated. Extensional viscosity measurement results revealed that the studied extracts cannot be treated as simple shear-thinning fluids, as indicated by shear flow, but should be considered as viscoelastic fluids. Full article