Bacterial Cellulose Electrospun Fiber Mesh Coated with Chitin Nanofibrils for Eardrum Repair.

In this study, we develop a bio-based and bioactive nanofibrous patch based on bacterial cellulose (BC) and chitin nanofibrils (CNs) using an ionic liquid as a solvent for BC, aimed at tympanic membrane (TM) repair. Electrospun BC nanofiber meshes were produced via electrospinning, and surface-modified with CNs using electrospray. The rheology of the BC/ionic liquid system was investigated. The obtained CN/BC meshes underwent comprehensive morphological, physicochemical, and mechanical characterization. Cytotoxicity tests were conducted using L929 mouse fibroblasts, revealing a cell viability of 97.8%. In vivo tests on rabbit skin demonstrated that the patches were nonirritating. Furthermore, the CN/BC fiber meshes were tested in vitro using human dermal keratinocytes (HaCaT cells) and human umbilical vein endothelial cells as model cells for TM perforation healing. Both cell types demonstrated successful growth on these scaffolds. The presence of CNs resulted in improved indirect antimicrobial activity of the electrospun fiber meshes. HaCaT cells exhibited an upregulated mRNA expression at 6 and 24 h of key proinflammatory cytokines crucial for the wound healing process, indicating the potential benefits of CNs in the healing response. Overall, this study presents a natural and eco-sustainable fiber mesh with great promise for applications in TM repair, leveraging the synergistic effects of BC and CNs to possibly enhance tissue regeneration and healing. Impact statement Repair of tympanic membrane perforations following chronic otitis media is a main clinical issue in otologic surgery, where the underlying infection obstacles self-healing. To address this challenge, our study proposes a bio-based patch made of nanoscale carbohydrate materials (i.e., bacterial cellulose electrospun fibers and chitin nanofibrils) processed via green solvents. The scaffold is nonirritating in vivo, and cytocompatible with fibroblasts, endothelial cells, and keratinocytes. In epithelial cells, it stimulates the expression of the antimicrobial peptide human beta defensin 2, with a pathway of cytokine expression compatible with the wound healing process. Therefore, it could be applied with unsolved infective pathology.

Innovative Biobased and Sustainable Polymer Packaging Solutions for Extending Bread Shelf Life: A Review.

Sustainable packaging has been steadily gaining prominence within the food industry, with biobased materials emerging as a promising substitute for conventional petroleum-derived plastics. This review is dedicated to the examination of innovative biobased materials in the context of bread packaging. It aims to furnish a comprehensive survey of recent discoveries, fundamental properties, and potential applications. Commencing with an examination of the challenges posed by various bread types and the imperative of extending shelf life, the review underscores the beneficial role of biopolymers as internal coatings or external layers in preserving product freshness while upholding structural integrity. Furthermore, the introduction of biocomposites, resulting from the amalgamation of biopolymers with active biomolecules, fortifies barrier properties, thus shielding bread from moisture, oxygen, and external influences. The review also addresses the associated challenges and opportunities in utilizing biobased materials for bread packaging, accentuating the ongoing requirement for research and innovation to create advanced materials that ensure product integrity while diminishing the environmental footprint.

Biopolymer- and Natural Fiber-Based Biomimetic Tissues to Realize Smart Cosmeceuticals and Nutraceuticals Using an Innovative Approach.

More sustainable and smart cosmeceuticals and nutraceuticals are necessary due to the ecological transition. In this study, a pullulan-based water solution containing chitin nanofibril-nano-lignin (CN-LG) complexes that encapsulate fish collagen polypeptide, allantoin and nicotinamide was electrospun onto a nonwoven substrate made of bamboo fibers to obtain a smart nanostructured bilayer system for releasing active molecules onto the skin or other body tissues. Infrared spectroscopy was used to characterize the composition of the bilayer system before and after rapid washing of the sample with distilled water and liquids mimicking physiological fluids. The viability of keratinocytes was studied as well as the antioxidant activity, protective activity towards UV light, metalloproteinase release of aged fibroblasts and the inhibitor activity against collagen degradation. Immunomodulatory tests were performed to investigate the anti-inflammatory activity of the bilayer system as well as its indirect antimicrobial activity. The results indicate that the bilayer system can be used in the production of innovative sustainable cosmeceuticals. In general, the adopted strategy can be extended to several smart treatments for fast release that can be commercialized as solid products, thus avoiding the use of preservatives and water.

Investigation of Novel Flax Fiber/Epoxy Composites with Increased Biobased Content.

Currently, biobased epoxy resins derived from plant oils and natural fibers are available on the market and are a promising substitute for fossil-based products. The purpose of this work is to investigate novel lightweight thermoset fiber-reinforced composites with extremely high biobased content. Paying attention to the biobased content, following a cascade pathway, many trials were carried out with different types of resins and hardeners to select the best ones. The most promising formulations were then used to produce flax fiber reinforced composites by vacuum bagging process. The main biocomposite properties such as tensile, bending, and impact properties as well as the individuation of their glass transition temperatures (by DSC) were assessed. Three biocomposite systems were investigated with biobased content ranging from 60 to 91%, obtaining an elastic modulus that varied from 2.7 to 6.3 GPa, a flexural strength from 23 to 108.5 MPa, and Charpy impact strength from 11.9 to 12.2 kJ/m2. The properties reached by the new biocomposites are very encouraging; in fact, their stiffness vs. lightweight (calculated by the E/ρ3 ratio) is comparable to some typical epoxy-glass composites.

A Straightforward Method to Produce Multi-Nanodrug Delivery Systems for Transdermal/Tympanic Patches Using Electrospinning and Electrospray.

The delivery of drugs through the skin barrier at a predetermined rate is the aim of transdermal drug delivery systems (TDDSs). However, so far, TDDS has not fully attained its potential as an alternative to hypodermic injections and oral delivery. In this study, we presented a proof of concept of a dual drug-loaded patch made of nanoparticles (NPs) and ultrafine fibers fabricated by using one equipment, i.e., the electrospinning apparatus. Such NP/fiber systems can be useful to release drugs locally through the skin and the tympanic membrane. Briefly, dexamethasone (DEX)-loaded poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBHV) fiber meshes were decorated with rhodamine (RHO)-loaded poly(lactic-co-glycolic acid) (PLGA) NPs, with RHO representing as a second drug model. By properly tuning the working parameters of electrospinning, DEX-loaded PHBHV fibers (i.e., by electrospinning mode) and RHO-loaded PLGA NPs (i.e., by electrospray mode) were successfully prepared and straightforwardly assembled to form a TDDS patch, which was characterized via Fourier transform infrared spectroscopy and dynamometry. The patch was then tested in vitro using human dermal fibroblasts (HDFs). The incorporation of DEX significantly reduced the fiber mesh stiffness. In vitro tests showed that HDFs were viable for 8 days in contact with drug-loaded samples, and significant signs of cytotoxicity were not highlighted. Finally, thanks to a beaded structure of the fibers, a controlled release of DEX from the electrospun patch was obtained over 4 weeks, which may accomplish the therapeutic objective of a local, sustained and prolonged anti-inflammatory action of a TDDS, as is requested in chronic inflammatory conditions, and other pathological conditions, such as in sudden sensorineural hearing loss treatment.

Assessment of Electrospun Poly(ε-caprolactone) and Poly(lactic acid) Fiber Scaffolds to Generate 3D In Vitro Models of Colorectal Adenocarcinoma: A Preliminary Study.

Three-dimensional scaffold-based culture has been increasingly gaining influence in oncology as a therapeutic strategy for tumors with a high relapse percentage. This study aims to evaluate electrospun poly(ε-caprolactone) (PCL) and poly(lactic acid) (PLA) scaffolds to create a 3D model of colorectal adenocarcinoma. Specifically, the physico-mechanical and morphological properties of PCL and PLA electrospun fiber meshes collected at different drum velocities, i.e., 500 rpm, 1000 rpm and 2500 rpm, were assessed. Fiber size, mesh porosity, pore size distribution, water contact angle and tensile mechanical properties were investigated. Caco-2 cells were cultured on the produced PCL and PLA scaffolds for 7 days, demonstrating good cell viability and metabolic activity in all the scaffolds. A cross-analysis of the cell-scaffold interactions with morphological, mechanical and surface characterizations of the different electrospun fiber meshes was carried out, showing an opposite trend of cell metabolic activity in PLA and PCL scaffolds regardless of the fiber alignment, which increased in PLA and decreased in PCL. The best samples for Caco-2 cell culture were PCL500 (randomly oriented fibers) and PLA2500 (aligned fibers). Caco-2 cells had the highest metabolic activity in these scaffolds, with Young's moduli in the range of 8.6-21.9 MPa. PCL500 showed Young's modulus and strain at break close to those of the large intestine. Advancements in 3D in vitro models of colorectal adenocarcinoma could move forward the development of therapies for this cancer.

Chitin nanofibrils modulate mechanical response in tympanic membrane replacements.

The tympanic membrane (TM), is a thin tissue lying at the intersection of the outer and the middle ear. TM perforations caused by traumas and infections often result in a conductive hearing loss. Tissue engineering has emerged as a promising approach for reconstructing the damaged TM by replicating the native material characteristics. In this regard, chitin nanofibrils (CN), a polysaccharide-derived nanomaterial, is known to exhibit excellent biocompatibility, immunomodulation and antimicrobial activity, thereby imparting essential qualities for an optimal TM regeneration. This work investigates the application of CN as a nanofiller for poly(ethylene oxide terephthalate)/poly(butylene terephthalate) (PEOT/PBT) copolymer to manufacture clinically suitable TM scaffolds using electrospinning and fused deposition modelling. The inclusion of CN within the PEOT/PBT matrix showed a three-fold reduction in the corresponding electrospun fiber diameters and demonstrated a significant improvement in the mechanical properties required for TM repair. Furthermore, in vitro biodegradation assay highlighted a favorable influence of CN in accelerating the scaffold degradation over a period of one year. Finally, the oto- and cytocompatibility response of the nanocomposite substrates corroborated their biological relevance for the reconstruction of perforated eardrums.

Upcycling of Poly(Lactic Acid) by Reactive Extrusion with Recycled Polycarbonate: Morphological and Mechanical Properties of Blends.

Poly(lactic acid) (PLA) is one of the most promising renewable polymers to be employed to foster ecological and renewable materials in many fields of application. To develop high-performance products, however, the thermal resistance and the impact properties should be improved. At the same time, it is also necessary to consider the end of life through the exploration of property assessment, following reprocessing. In this context the aim of the paper is to develop PLA/PC blends, obtained from recycled materials, in particular scraps from secondary processing, to close the recycling loop. Indeed, the blending of PLA with polycarbonate (PC) was demonstrated to be a successful strategy to improve thermomechanical properties that happens after several work cycles. The correlation between the compositions and properties was then investigated by considering the morphology of the blends; in addition, the reactive extrusions resulting in the formation of a PLA-PC co-polymer were investigated. The materials obtained are then examined by means of a dynamic-mechanical analysis (DMTA) to study the relaxations and transitions.

Antimicrobial and Gas Barrier Crustaceans and Fungal Chitin-Based Coatings on Biodegradable Bioplastic Films.

Chitin nanofibrils (CN) can be obtained from crustaceans and fungal sources and can be used for preparing coatings for bioplastic films, that are fundamental for developing a safe and sustainable biodegradable food packaging. Coatings with different concentrations of CN from shrimps were applied on different bioplastic substrates, like Poly (butylene succinate-co-adipate)/Poly(3-hydroxybutyrate-co-3-hydroxyvalerate (PBSA/PHBV) blend, Polybutylene succinate (PBS), and Polybutylene adipate terephthalate/Poly(lactic acid) (PBAT/PLA) blend, but the adhesion to the substrates was scarce. On the contrary, the fungal-based CN showed a better adhesion. Additionally, it was found that the use of an additive based on oligomeric lactic acid was useful to prepare a coating with an improved adhesion to bioplastics. The gas barrier properties to oxygen and water vapour of coated and un-coated films were measured, revealing an improvement of these properties thanks to applied coatings, especially towards the oxygen. Antimicrobial properties and biodegradation capacity were also evaluated revealing an antibacterial effect of the coatings that did not significantly interfere with their biodegradability. The results are discussed and interpreted considering the correlation between composition and macromolecular structures with the observed functional properties.

Micromechanical Deformation Processes and Failure of PBS Based Composites Containing Ultra-Short Cellulosic Fibers for Injection Molding Applications.

The use of biobased thermoplastic polymers has gained great attention in the last years as a potential alternative to fossil-based thermoplastic polymers. Biobased polymers in fact offer advantages not only in terms of reduced dependence on fossil resources but they also lower the CO2 footprint in accordance with sustainability and climate protection goals. To improve the properties of these materials, reinforcement with biobased fibers is a promising solution; however, it must be kept in mind that the fibers aspect ratio and the interfacial adhesion between the reinforcement and the matrix plays an important role influencing both physical and mechanical properties of the biocomposites. In this paper, the possibility of producing composites by injection molding, based on polybutylene succinate and ultra-short cellulosic fibers has been explored as a potential biobased solution. Thermo-mechanical properties of the composites were investigated, paying particular attention to the local micromechanical deformation processes, investigated by dilatometric tests, and failure mechanisms. Analytical models were also applied to predict the elastic and flexural modulus and the interfacial properties of the biocomposites. Good results were achieved, demonstrating the that this class of biocomposite can be exploited. Compared to pure PBS, the composites with 30 wt.% of cellulose fibers increased the Young's modulus by 154%, the flexural modulus by 130% and the heat deflection temperature by 9%.

Electrospun Poly(3-Hydroxybutyrate-Co-3-Hydroxyvalerate)/Olive Leaf Extract Fiber Mesh as Prospective Bio-Based Scaffold for Wound Healing.

Polyhydroxyalkanoates (PHAs) are a family of biopolyesters synthesized by various microorganisms. Due to their biocompatibility and biodegradation, PHAs have been proposed for biomedical applications, including tissue engineering scaffolds. Olive leaf extract (OLE) can be obtained from agri-food biowaste and is a source of polyphenols with remarkable antioxidant properties. This study aimed at incorporating OLE inside poly(hydroxybutyrate-co-hydroxyvalerate) (PHBHV) fibers via electrospinning to obtain bioactive bio-based blends that are useful in wound healing. PHBHV/OLE electrospun fibers with a size of 1.29 ± 0.34 µm were obtained. Fourier transform infrared chemical analysis showed a uniform surface distribution of hydrophilic -OH groups, confirming the presence of OLE in the electrospun fibers. The main OLE phenols were released from the fibers within 6 days. The biodegradation of the scaffolds in phosphate buffered saline was investigated, demonstrating an adequate stability in the presence of metalloproteinase 9 (MMP-9), an enzyme produced in chronic wounds. The scaffolds were preliminarily tested in vitro with HFFF2 fibroblasts and HaCaT keratinocytes, suggesting adequate cytocompatibility. PHBHV/OLE fiber meshes hold promising features for wound healing, including the treatment of ulcers, due to the long period of durability in an inflamed tissue environment and adequate cytocompatibility.

Sensing Devices for Detecting and Processing Acoustic Signals in Healthcare.

Acoustic signals are important markers to monitor physiological and pathological conditions, e.g., heart and respiratory sounds. The employment of traditional devices, such as stethoscopes, has been progressively superseded by new miniaturized devices, usually identified as microelectromechanical systems (MEMS). These tools are able to better detect the vibrational content of acoustic signals in order to provide a more reliable description of their features (e.g., amplitude, frequency bandwidth). Starting from the description of the structure and working principles of MEMS, we provide a review of their emerging applications in the healthcare field, discussing the advantages and limitations of each framework. Finally, we deliver a discussion on the lessons learned from the literature, and the open questions and challenges in the field that the scientific community must address in the near future.

Improvement of Interfacial Adhesion and Thermomechanical Properties of PLA Based Composites with Wheat/Rice Bran.

The present work aims to enhance the use of agricultural byproducts for the production of bio-composites by melt extrusion. It is well known that in the production of such bio-composites, the weak point is the filler-matrix interface, for this reason the adhesion between a polylactic acid (PLA)/poly(butylene succinate)(PBSA) blend and rice and wheat bran platelets was enhanced by a treatment method applied on the fillers using a suitable beeswax. Moreover, the coupling action of beeswax and inorganic fillers (such as talc and calcium carbonate) were investigated to improve the thermo-mechanical properties of the final composites. Through rheological (MFI), morphological (SEM), thermal (TGA, DSC), mechanical (Tensile, Impact), thermomechanical (HDT) characterizations and the application of analytical models, the optimum among the tested formulations was then selected.

Analytical Modeling of Stress Relaxation and Evaluation of the Activation Volume Variation: Effect of Temperature and Plasticizer Content for Poly(3-hydroxybutyrate-3-hydroxyvalerate).

In this study, stress-relaxation tests that have been carried out at different temperatures (quite below the heat deflection temperature) on a poly(3-hydroxybutyrate-3hydroxyvalerate) (PHB-HV) matrix containing different amounts of the acetyl tributyl citrate plasticizer (added at 5 and 10 wt %) are investigated. The analytical modeling of the stress relaxation behavior by the coupling of Eyring's approach and the Guiu and Pratt model is successful. The activation volume results achieved are very interesting; in fact, not only the dependence of the activation volume from temperature is confirmed (and it resulted in dependence from the α' relaxation temperature) but also, for the first time, the dependence of the activation volume from the plasticizer content is shown. In particular, the presence of a linear relationship between the activation volume and the plasticizer volume content is observed.

Influence of Functional Bio-Based Coatings Including Chitin Nanofibrils or Polyphenols on Mechanical Properties of Paper Tissues.

The paper tissue industry is a constantly evolving sector that supplies markets that require products with different specific properties. In order to meet the demand of functional properties, ensuring a green approach at the same time, research on bio-coatings has been very active in recent decades. The attention dedicated to research on functional properties has not been given to the study of the morphological and mechanical properties of the final products. This paper studied the effect of two representative bio-based coatings on paper tissue. Coatings based on chitin nanofibrils or polyphenols were sprayed on paper tissues to provide them, respectively, with antibacterial and antioxidant activity. The chemical structure of the obtained samples was preliminarily compared by ATR-FTIR before and after their application. Coatings were applied on paper tissues and, after drying, their homogeneity was investigated by ATR-FTIR on different surface areas. Antimicrobial and antioxidant properties were found for chitin nanofibrils- and polyphenols-treated paper tissues, respectively. The mechanical properties of treated and untreated paper tissues were studied, considering as a reference the same tissue paper sample treated only with water. Different mechanical tests were performed on tissues, including penetration, tensile, and tearing tests in two perpendicular directions, to consider the anisotropy of the produced tissues for industrial applications. The morphology of uncoated and coated paper tissues was analysed by field emission scanning electron microscopy. Results from mechanical properties evidenced a correlation between morphological and mechanical changes. The addition of polyphenols resulted in a reduction in mechanical resistance, while the addition of chitin enhanced this property. This study evidenced the different effects produced by two novel coatings on paper tissues for personal care in terms of properties and structure.

Chitin Nanofibril-Nanolignin Complexes as Carriers of Functional Molecules for Skin Contact Applications.

Chitin nanofibrils (CN) and nanolignin (NL) were used to embed active molecules, such as vitamin E, sodium ascorbyl phosphate, lutein, nicotinamide and glycyrrhetinic acid (derived from licorice), in the design of antimicrobial, anti-inflammatory and antioxidant nanostructured chitin nanofibrils-nanolignin (CN-NL) complexes for skin contact products, thus forming CN-NL/M complexes, where M indicates the embedded functional molecule. Nano-silver was also embedded in CN-NL complexes or on chitin nanofibrils to exploit its well-known antimicrobial activity. A powdery product suitable for application was finally obtained by spray-drying the complexes co-formulated with poly(ethylene glycol). The structure and morphology of the complexes was studied using infrared spectroscopy and field emission scanning electron microscopy, while their thermal stability was investigated via thermo-gravimetry. The latter provided criteria for evaluating the suitability of the obtained complexes for subsequent demanding industrial processing, such as, for instance, incorporation into bio-based thermoplastic polymers through conventional melt extrusion. In vitro tests were carried out at different concentrations to assess skin compatibility. The obtained results provided a physical-chemical, morphological and cytocompatibility knowledge platform for the correct selection and further development of such nanomaterials, allowing them to be applied in different products. In particular, chitin nanofibrils and the CN-NL complex containing glycyrrhetinic acid can combine excellent thermal stability and skin compatibility to provide a nanostructured system potentially suitable for industrial applications.

Improvement of the PLA Crystallinity and Heat Distortion Temperature Optimizing the Content of Nucleating Agents and the Injection Molding Cycle Time.

Three different commercial nucleating agents (LAK, talc, and calcium carbonate) were added at different weight percentages into poly (lactic acid) (PLA) in order to investigate the mechanical and thermo-mechanical behavior of blends in correlation to injection molding parameters. After as-sessing the best content of each nucleating agent, analyzing isothermal and non-isothermal crys-tallization, two cycle times that can be industrially adopted were selected. Crystallinity highly impacts the flexural modulus, while it improves the heat deflection temperature only when the crystallinity percentage is above 50%; nevertheless, an excessive crystallinity content leads to a decrement of impact resistance. LAK does not appear to be sensitive to cycle time while talc and calcium carbonate proved to be effective if a cycle time of 60 s is adopted. Since the choice of nu-cleating agent is not univocal, the identification of the best nucleating agents is subject to the technical specifications required by the application, accotuing for the most important commercial requirements (productivity, temperature, and impact resistance).

A Brief Review of Poly (Butylene Succinate) (PBS) and Its Main Copolymers: Synthesis, Blends, Composites, Biodegradability, and Applications.

PBS, an acronym for poly (butylene succinate), is an aliphatic polyester that is attracting increasing attention due to the possibility of bio-based production, as well as its balanced properties, enhanced processability, and excellent biodegradability. This brief review has the aim to provide the status concerning the synthesis, production, thermal, morphological and mechanical properties underlying biodegradation ability, and major applications of PBS and its principal copolymers.

Essential Work of Fracture and Evaluation of the Interfacial Adhesion of Plasticized PLA/PBSA Blends with the Addition of Wheat Bran By-Product.

In this work biocomposites based on plasticized poly(lactic acid) (PLA)-poly(butylene succinate-co-adipate) (PBSA) matrix containing wheat bran fiber (a low value by-product of food industry) were investigated. The effect of the bran addition on the mechanical properties is strictly correlated to the fiber-matrix adhesion and several analytical models, based on static and dynamic tests, were applied in order to estimate the interfacial shear strength of the biocomposites. Finally, the essential work of fracture approach was carried out to investigate the effect of the bran addition on composite fracture toughness.

Analysis, Development, and Scaling-Up of Poly(lactic acid) (PLA) Biocomposites with Hazelnuts Shell Powder (HSP).

In this work, two different typologies of hazelnuts shell powders (HSPs) having different granulometric distributions were melt-compounded into poly(lactic acid) (PLA) matrix. Different HSPs concentration (from 20 up to 40 wt.%) were investigated with the aim to obtain final biocomposites with a high filler quantity, acceptable mechanical properties, and good melt fluidity in order to be processable. For the best composition, the scale-up in a semi-industrial extruder was then explored. Good results were achieved for the scaled-up composites; in fact, thanks to the extruder venting system, the residual moisture is efficiently removed, guaranteeing to the final composites improved mechanical and melt fluidity properties, when compared to the lab-scaled composites. Analytical models were also adopted to predict the trend of mechanical properties (in particular, tensile strength), also considering the effect of HSPs sizes and the role of the interfacial adhesion between the fillers and the matrix.