Effect of different crosslinking agents on hybrid chitosan/collagen hydrogels for potential tissue engineering applications.

Tissue engineering (TE) demands scaffolds that have the necessary resistance to withstand the mechanical stresses once implanted in our body, as well as excellent biocompatibility. Hydrogels are postulated as interesting materials for this purpose, especially those made from biopolymers. In this study, the microstructure and rheological performance, as well as functional and biological properties of chitosan and collagen hydrogels (CH/CG) crosslinked with different coupling agents, both natural such as d-Fructose (F), genipin (G) and transglutaminase (T) and synthetic, using a combination of 1-ethyl-3-(3-dimethylaminopropyl)carbodiimide hydrochloride with N-hydroxysuccinimide (EDC/NHS) will be assessed. FTIR tests were carried out to determine if the proposed crosslinking reactions for each crosslinking agent occurred as expected, obtaining positive results in this aspect. Regarding the characterization of the properties of each system, two main trends were observed, from which it could be established that crosslinking with G and EDC-NHS turned out to be more effective and beneficial than with the other two crosslinking agents, producing significant improvements with respect to the base CH/CG hydrogel. In addition, in vitro tests demonstrated the potential application in TE of these systems, especially for those crosslinked with G, T and EDC-NHS.

Biodegradable Fiber-Reinforced Gluten Biocomposites for Replacement of Fossil-Based Plastics.

Biocomposites based on wheat gluten and reinforced with carbon fibers were produced in line with the strive to replace fossil-based plastics with microplastic-free alternatives with competing mechanical properties. The materials were first extruded/compounded and then successfully injection molded, making the setup adequate for the current industrial processing of composite plastics. Furthermore, the materials were manufactured at very low extrusion and injection temperatures (70 and 140 °C, respectively), saving energy compared to the compounding of commodity plastics. The sole addition of 10 vol % fibers increased yield strength and stiffness by a factor of 2-4 with good adhesion to the protein. The biocomposites were also shown to be biodegradable, lixiviating into innocuous molecules for nature, which is the next step in the development of sustainable bioplastics. The results show that an industrial protein coproduct reinforced with strong fibers can be processed using common plastic processing techniques. The enhanced mechanical performance of the reinforced protein-based matrix herein also contributes to research addressing the production of safe materials with properties matching those of traditional fossil-based plastics.

Injectable Thermoresponsive Microparticle/Hydrogel System with Superparamagnetic Nanoparticles for Drug Release and Magnetic Hyperthermia Applications.

Cancer is a disease that continues to greatly impact our society. Developing new and more personalized treatment options is crucial to decreasing the cancer burden. In this study, we combined magnetic polysaccharide microparticles with a Pluronic thermoresponsive hydrogel to develop a multifunctional, injectable drug delivery system (DDS) for magnetic hyperthermia applications. Gellan gum and alginate microparticles were loaded with superparamagnetic iron oxide nanoparticles (SPIONs) with and without coating. The magnetic microparticles' registered temperature increases up to 4 °C upon the application of an alternating magnetic field. These magnetic microparticles were mixed with drug-loaded microparticles, and, subsequently, this mixture was embedded within a Pluronic thermoresponsive hydrogel that is capable of being in the gel state at 37 °C. The proposed DDS was capable of slowly releasing methylene blue, used as a model drug, for up to 9 days. The developed hydrogel/microparticle system had a smaller rate of drug release compared with microparticles alone. This system proved to be a potential thermoresponsive DDS suitable for magnetic hyperthermia applications, thus enabling a synergistic treatment for cancer.

Porous Thermoformed Protein Bioblends as Degradable Absorbent Alternatives in Sanitary Materials.

Protein-based porous absorbent structures can be processed and assembled into configurations suitable for single-use, biodegradable sanitary materials. In this work, a formulation based on a mixture of proteins available as industrial coproducts is processed into continuous porous structures using extrusion and assembled using conventional thermal methods. The experimental design led to formulations solely based on zein-gluten protein bioblends that could be manufactured as liquid absorbent pellets, compressed pads, and/or porous films. The processing versatility is attributed to the synergistic effect of zein as a low viscosity thermoformable protein with gluten as a readily cross-linkable high molecular weight protein. The capillary-driven sorption, the biodegradability of the materials, and the possibility to assemble the products as multilayer components provide excellent performance indicators for their use as microplastic-free absorbents. This work shows the potential of biopolymers for manufacturing sustainable alternatives to current nonbiodegradable and highly polluting disposable items such as pads and diapers.

Valorization of Honduran Agro-Food Waste to Produce Bioplastics.

The development of biodegradable plastics and eco-friendly biomaterials derived from renewable resources is crucial for reducing environmental damage. Agro-industrial waste and rejected food can be polymerized into bioplastics, offering a sustainable solution. Bioplastics find use in various industries, including for food, cosmetics, and the biomedical sector. This research investigated the fabrication and characterization of bioplastics using three types of Honduran agro-wastes: taro, yucca, and banana. The agro-wastes were stabilized and characterized (physicochemically and thermically). Taro flour presented the highest protein content (around 4.7%) and banana flour showed the highest moisture content (around 2%). Furthermore, bioplastics were produced and characterized (mechanically and functionally). Banana bioplastics had the best mechanical properties, with a Young's modulus around 300 MPa, while taro bioplastics had the highest water-uptake capacity (200%). In general, the results showed the potential of these Honduran agro-wastes for producing bioplastics with different characteristics that could add value to these wastes, promoting the circular economy.

Stabilization and Valorization of Beer Bagasse to Obtain Bioplastics.

Beer bagasse is a residue produced in large quantities, though it is undervalued in the industry. Its high protein and polysaccharide content make it attractive for use in sectors such as the manufacture of bioplastics. However, its high water content makes it necessary to stabilize it before being considered as a raw material. The main objective of this work was to evaluate the stabilization of beer bagasse and the production of bioplastics from it. In this sense, different drying methods (freeze-drying and heat treatment at 45 and 105 °C) were studied. The bagasse was also characterized physicochemically to evaluate its potential. In addition, bagasse was used in combination with glycerol (plasticizer) to make bioplastics by injection molding, analyzing their mechanical properties, water absorption capacity and biodegradability. The results showed the great potential of bagasse, presenting a high content of proteins (18-20%) and polysaccharides (60-67%) after its stabilization, with freeze-drying being the most suitable method to avoid its denaturation. Bioplastics present appropriate properties for use in applications such as horticulture and agriculture.

Effect of Calcination Temperature and Time on the Synthesis of Iron Oxide Nanoparticles: Green vs. Chemical Method.

Nowadays, antioxidants and antibacterial activity play an increasingly vital role in biosystems due to the biochemical and biological reactions that involve free radicals and pathogen growth, which occur in many systems. For this purpose, continuous efforts are being made to minimize these reactions, including the use of nanomaterials as antioxidants and bactericidal agents. Despite such advances, iron oxide nanoparticles still lack knowledge regarding their antioxidant and bactericidal capacities. This includes the investigation of biochemical reactions and their effects on nanoparticle functionality. In green synthesis, active phytochemicals give nanoparticles their maximum functional capacity and should not be destroyed during synthesis. Therefore, research is required to establish a correlation between the synthesis process and the nanoparticle properties. In this sense, the main objective of this work was to evaluate the most influential process stage: calcination. Thus, different calcination temperatures (200, 300, and 500 °C) and times (2, 4, and 5 h) were studied in the synthesis of iron oxide nanoparticles using either Phoenix dactylifera L. (PDL) extract (green method) or sodium hydroxide (chemical method) as the reducing agent. The results show that calcination temperatures and times had a significant influence on the degradation of the active substance (polyphenols) and the final structure of iron oxide nanoparticles. It was found that, at low calcination temperatures and times, the nanoparticles exhibited small sizes, fewer polycrystalline structures, and better antioxidant activities. In conclusion, this work highlights the importance of green synthesis of iron oxide nanoparticles due to their excellent antioxidant and antimicrobial activities.

Soy Protein Isolate as Emulsifier of Nanoemulsified Beverages: Rheological and Physical Evaluation.

The production of biologically active molecules or the addition of new bioactive ingredients in foods, thereby producing functional foods, has been improved with nanoemulsion technology. In this sense, the aim of this work was to develop nanoemulsified beverages as potential candidates for the encapsulation of bioactive compounds, whose integrity and release across the intestinal tract are controlled by the structure and stability of the interfaces. To achieve this, firstly, a by-product rich-in protein has been evaluated as a potential candidate to act as an emulsifier (chemical content, amino acid composition, solubility, ζ-potential and surface tension were evaluated). Later, emulsions with different soy protein isolate concentrations (0.5, 1.0, 1.5 and 2.0 wt%), pH values (2, 4, 6 and 8) and homogenization pressures (100, 120 and 140 PSI) were prepared using a high-pressure homogenizer after a pre-emulsion formation. Physical (stability via Backscattering and drop size evolution) and rheological (including interfacial analysis) characterizations of emulsions were carried out to characterize their potential as delivery emulsion systems. According to the results obtained, the nanoemulsions showed the best stability when the protein concentration was 2.0 wt%, pH 2.0 and 120 PSI was applied as homogenization pressure.

Biopolymer-Based Films Reinforced with Green Synthesized Zinc Oxide Nanoparticles.

Nowadays, biopolymer-based films are being developed as an alternative to conventional plastic-based films, mainly because they are non-toxic, flexible, inexpensive, and widely available. However, they are restricted in their applications due to several deficiencies in their properties. Accordingly, the reinforcement of these materials with nanoparticles/nanofillers could overcome some of their shortcomings, especially those processed by green methods. Green synthesized zinc oxide nanoparticles (ZnO-NPs) are highly suggested to overcome these deficiencies. Therefore, the main aim of this work was to develop different biopolymer-based films from cellulose acetate (CA), chitosan (CH), and gelatin (GE) reinforced with ZnO-NPs prepared by casting, and to assess their different properties. The results show the improvements produced by the incorporation of ZnO-NPs (1% w/w) into the CA, CH, and GE systems. Thus, the water contact angles (WCAs) increased by about 12, 13, and 14%, while the water vapor permeability (WVP) decreased by about 14, 6, and 29%, the water solubility (WS) decreased by about 23, 6, and 5%, and the transparency (T) increased by about 19, 31, and 20% in the CA, CH, and GE systems, respectively. Furthermore, the mechanical properties were enhanced by increasing the ultimate tensile strength (UTS) (by about 39, 13, and 26%, respectively) and Young's modulus (E) (by about 70, 34, and 63%, respectively), thereby decreasing the elongation at the break (εmax) (by about 56, 23, and 49%, respectively) and the toughness (by about 50, 4, and 30%, respectively). Lastly, the antioxidant properties were enhanced by 34, 49, and 39%, respectively.

Biopolymer-Based Films Reinforced with FexOy-Nanoparticles.

Nowadays, natural polymer-based films are considered potentially environmentally friendly alternatives to conventional plastic films, due to many advantageous properties, including their easy processability, high flexibility, non-toxicity, low cost, high availability, and environmental safety. However, they are limited in their application by a number of shortcomings, including their high water solubility and vapor permeability as well as their poor opacity and low mechanical resistance. Thus, nanoparticles, such as green FexOy-NPs, can be used to overcome the drawbacks associated with these materials. Therefore, the aim of this study was to develop three different polymer-based films (gelatin-based, cellulose acetate-based and chitosan-based films) containing green synthesized FexOy-NPs (1.0% w/w of the initial polymer weight) as an additive to improve film properties. This was accomplished by preparing the different films using the casting method and examining their physicochemical, mechanical, microstructural, and functional characteristics. The results show that the incorporation of FexOy-NPs into the different films significantly enhanced their physicochemical, mechanical, and morphological properties as well as their antioxidant characteristics. Consequently, it was possible to produce suitable natural polymer-based films with potential applications across a wide range of industries, including functional packaging for food, antioxidants, and antimicrobial additives for pharmaceutical and biomedical materials as well as pesticides for agriculture.

Green Synthesis of FexOy Nanoparticles with Potential Antioxidant Properties.

Iron oxide nanoparticles (FexOy-NPs) are currently being applied in numerous high-tech sectors, such as in chemical sectors for catalysis and in the medical sector for drug delivery systems and antimicrobial purposes, due to their specific, unique and magnetic properties. Nevertheless, their synthesis is under continuous investigation, as physicochemical methods are considered expensive and require toxic solvents. Thus, green nanotechnology has shown considerable promise in the eco-biogenesis of nanoparticles. In the current study, FexOy-NPs were synthesized by two different methods: via green synthesis through the use of polyphenols, which were extracted from Phoenix dactylifera L.; and via chemical synthesis, in which the reducing agent was a chemical (NaOH), and iron chloride was used as a precursor. Thus, polyphenol extraction and its ability to produce nanoparticles were evaluated based on the drying temperature used during the Phoenix dactylifera L. recollection, as well as the extraction solvent used. The results highlight the potential of polyphenols present in Phoenix dactylifera L. for the sustainable manufacture of FexOy-NPs. Finally, green and chemical syntheses were compared on the basis of physicochemical characteristics and functional properties.

Novel Trends in Hydrogel Development for Biomedical Applications: A Review.

Nowadays, there are still numerous challenges for well-known biomedical applications, such as tissue engineering (TE), wound healing and controlled drug delivery, which must be faced and solved. Hydrogels have been proposed as excellent candidates for these applications, as they have promising properties for the mentioned applications, including biocompatibility, biodegradability, great absorption capacity and tunable mechanical properties. However, depending on the material or the manufacturing method, the resulting hydrogel may not be up to the specific task for which it is designed, thus there are different approaches proposed to enhance hydrogel performance for the requirements of the application in question. The main purpose of this review article was to summarize the most recent trends of hydrogel technology, going through the most used polymeric materials and the most popular hydrogel synthesis methods in recent years, including different strategies of enhancing hydrogels' properties, such as cross-linking and the manufacture of composite hydrogels. In addition, the secondary objective of this review was to briefly discuss other novel applications of hydrogels that have been proposed in the past few years which have drawn a lot of attention.

Gelatin-Based Biofilms with FexOy-NPs Incorporated for Antioxidant and Antimicrobial Applications.

Currently, gelatin-based films are regarded as promising alternatives to non-environmentally friendly plastic films for food packaging. Nevertheless, although they have great biodegradability, their weak mechanical properties and high solubility limit their applications. In this way, the use of nanoparticles, such as FexOy-NPs, could improve the properties of gelatin-based biofilms. Thus, the main objective of this work was to include different concentrations of FexOy-NPs (0.25 and 1.0%) manufactured by green synthesis (GS) and chemical synthesis (CS) into gelatin-based biofilms in order to improve their properties. The results show that FexOy-NPs can be distributed throughout the biofilm, although with a greater concentration on the upper surface. In addition, the incorporation of FexOy-NPs into the biofilms improves their physicochemical, mechanical, morphological, and biological properties. Thus, it is possible to achieve suitable gelatin-based biofilms, which can be used in several applications, such as functional packaging in the food industry, antioxidant and antimicrobial additives in biomedical and pharmaceutical biomaterials, and in agricultural pesticides.

Effect of Solution Properties in the Development of Cellulose Derivative Nanostructures Processed via Electrospinning.

In the last few years, electrospinning has proved to be one of the best methods for obtaining membranes of a micro and nanometric fiber size. This method mainly consists in the spinning of a polymeric or biopolymeric solution in solvents, promoted by the difference in the electric field between the needle and collector, which is finally deposited as a conjunction of randomly oriented fibers. The present work focuses on using cellulose derivatives (namely cellulose acetate and ethylcellulose), based on the revaluation of these byproducts and waste products of biorefinery, to produce nanostructured nanofiber through electrospinning with the objective of establishing a relation between the initial solutions and the nanostructures obtained. In this sense, a complete characterization of the biopolymeric solutions (physicochemical and rheological properties) and the resulting nanostructures (microstructural and thermal properties) was carried out. Therefore, solutions with different concentrations (5, 10, 15, and 20 wt%) of the two cellulose derivatives and different solvents with several proportions between them were used to establish their influence on the properties of the resulting nanostructures. The results show that the solutions with 10 wt% in acetic acid/H2O and 15 wt% in acetone/N,N-dimethylformamide of cellulose acetate and 5 wt% of ethylcellulose in acetone/N,N-dimethylformamide, exhibited the best properties, both in the solution and nanostructure state.

Biocompatible and Thermoresistant Hydrogels Based on Collagen and Chitosan.

Hydrogels are considered good biomaterials for soft tissue regeneration. In this sense, collagen is the most used raw material to develop hydrogels, due to its high biocompatibility. However, its low mechanical resistance, thermal stability and pH instability have generated the need to look for alternatives to its use. In this sense, the combination of collagen with another raw material (i.e., polysaccharides) can improve the final properties of hydrogels. For this reason, the main objective of this work was the development of hydrogels based on collagen and chitosan. The mechanical, thermal and microstructural properties of the hydrogels formed with different ratios of collagen/chitosan (100/0, 75/25, 50/50, 25/75 and 0/100) were evaluated after being processed by two variants of a protocol consisting in two stages: a pH change towards pH 7 and a temperature drop towards 4 °C. The main results showed that depending on the protocol, the physicochemical and microstructural properties of the hybrid hydrogels were similar to the unitary system depending on the stage carried out in first place, obtaining FTIR peaks with similar intensity or a more porous structure when chitosan was first gelled, instead of collagen. As a conclusion, the synergy between collagen and chitosan improved the properties of the hydrogels, showing good thermomechanical properties and cell viability to be used as potential biomaterials for Tissue Engineering.

Applied Rheology as Tool for the Assessment of Chitosan Hydrogels for Regenerative Medicine.

The regeneration of soft tissues that connect, support or surround other tissues is of great interest. In this sense, hydrogels have great potential as scaffolds for their regeneration. Among the different raw materials, chitosan stands out for being highly biocompatible, which, together with its biodegradability and structure, makes it a great alternative for the manufacture of hydrogels. Therefore, the aim of this work was to develop and characterize chitosan hydrogels. To this end, the most important parameters of their processing, i.e., agitation time, pH, gelation temperature and concentration of the biopolymer used were rheologically evaluated. The results show that the agitation time does not have a significant influence on hydrogels, whereas a change in pH (from 3.2 to 7) is a key factor for their formation. Furthermore, a low gelation temperature (4 °C) favors the formation of the hydrogel, showing better mechanical properties. Finally, there is a percentage of biopolymer saturation, from which the properties of the hydrogels are not further improved (1.5 wt.%). This work addresses the development of hydrogels with high thermal resistance, which allows their use as scaffolds without damaging their mechanical properties.

Incorporation of Elastin to Improve Polycaprolactone-Based Scaffolds for Skeletal Muscle via Electrospinning.

Skeletal muscle regeneration is increasingly necessary, which is reflected in the increasing number of studies that are focused on improving the scaffolds used for such regeneration, as well as the incubation protocol. The main objective of this work was to improve the characteristics of polycaprolactone (PCL) scaffolds by incorporating elastin to achieve better cell proliferation and biocompatibility. In addition, two cell incubation protocols (with and without dynamic mechanical stimulation) were evaluated to improve the activity and functionality yields of the regenerated cells. The results indicate that the incorporation of elastin generates aligned and more hydrophilic scaffolds with smaller fiber size. In addition, the mechanical properties of the resulting scaffolds make them adequate for use in both bioreactors and patients. All these characteristics increase the biocompatibility of these systems, generating a better interconnection with the tissue. However, due to the low maturation achieved in biological tests, no differences could be found between the incubation with and without dynamic mechanical stimulation.

Rheological and Microstructural Evaluation of Collagen-Based Scaffolds Crosslinked with Fructose.

In recent years, tissue engineering research has led to the development of this field by designing scaffolds with better properties that can fulfill its purpose of better and faster tissue regeneration, consequently improving people's quality of life. Scaffolds are matrices, predominantly composed of polymeric materials, whose main function is to offer support for cell adhesion and subsequent growth, leading to the regeneration of the damaged tissue. The widely used biopolymer in tissue engineering is collagen, which is the most abundant protein in animals. Its use is due to its structure, biocompatibility, ease of modification, and processability. In this work, collagen-based scaffolds were developed with different concentrations and processing techniques, by obtaining hydrogels and aerogels that were characterized with an emphasis on their morphology and mechanical properties. Moreover, fructose was added in some cases as a chemical crosslinking agent to study its influence on the scaffolds' properties. The obtained results revealed that the scaffolds with higher collagen concentrations were more rigid and deformable. Comparing both systems, the aerogels were more rigid, although the hydrogels were more deformable and had higher pore size homogeneity. Fructose addition produced a slight increase in the critical strain, together with an increase in the elastic modulus.

Incorporation of ZnO Nanoparticles into Soy Protein-Based Bioplastics to Improve Their Functional Properties.

The union of nanoscience (nanofertilization) with controlled release bioplastic systems could be a key factor for the improvement of fertilization in horticulture, avoiding excessive contamination and reducing the price of the products found in the current market. In this context, the objective of this work was to incorporate ZnO nanoparticles in soy protein-based bioplastic processed using injection moulding. Thus, the concentration of ZnO nanoparticles (0 wt%, 1.0 wt%, 2.0 wt%, 4.5 wt%) and mould temperature (70 °C, 90 °C and 110 °C) were evaluated through a mechanical (flexural and tensile properties), morphological (microstructure and nanoparticle distribution) and functional (water uptake capacity, micronutrient release and biodegradability) characterization. The results indicate that these parameters play an important role in the final characteristics of the bioplastics, being able to modify them. Ultimately, this study increases the versatility and functionality of the use of bioplastics and nanofertilization in horticulture, helping to prevent the greatest environmental impact caused.

Polymer-Based Scaffolds for Soft-Tissue Engineering.

Biomaterials have been used since ancient times. However, it was not until the late 1960s when their development prospered, increasing the research on them. In recent years, the study of biomaterials has focused mainly on tissue regeneration, requiring a biomaterial that can support cells during their growth and fulfill the function of the replaced tissue until its regeneration. These materials, called scaffolds, have been developed with a wide variety of materials and processes, with the polymer ones being the most advanced. For this reason, the need arises for a review that compiles the techniques most used in the development of polymer-based scaffolds. This review has focused on three of the most used techniques: freeze-drying, electrospinning and 3D printing, focusing on current and future trends. In addition, the advantages and disadvantages of each of them have been compared.