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The white pollution caused by unsustainable materials is a significant challenge around the globe. Here, a novel and fully biobased polybutyrolactam (PBY) nanofiber membrane was fabricated via the electrospinning method. As-spun PBY nanofiber membranes have good thermal stability, high porosity of up to 71.94%, and excellent wetting behavior. The biodegradability in soil, UV aging irradiation, and seawater was investigated. The PBY nanofiber membrane is almost completely degraded in the soil within 80 days, showing excellent degradability. More interestingly, γ-aminobutyric acid, as a healthcare agent with intrinsic hypotensive, tranquilizing, diuretic, and antidiabetic efficacy, can be detected in the degradation intermediates. In addition, the PBY nanofiber membrane also exhibits antibacterial ability against Escherichia coli. As a fully biomass-derived material, the PBY membrane has excellent biodegradable performance in various environments as well as negligible cytotoxicity and commendable cell proliferation. Our PBY nanofiber membrane shows great potential as biodegradable packaging and in vitro healthcare materials.

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Non-degradable plastic mulch films used in agriculture are polluting the environment by leaving residues and microplastics in the soil. They are also difficult to recycle due to contamination during their use. Biodegradable mulch films are needed as alternatives so that they can be used effectively during the growing season and later be ploughed to be degraded in soil. However, market-available so-called biodegradable mulch films are very slow to degrade in the natural environment and thus do not fit with crop rotation demands or annual cultivation. In this study, we have developed mulch films from cotton gin trash (CGT) and/or gin motes (GM) in combination with biodegradable polycaprolactone and demonstrated their effectiveness over 3 months in outdoor conditions. Both the stability and degradation behaviours of mulch film samples were observed when they were placed on top of the soil and buried in the soil, respectively. Pesticide residue analysis also was carried out on CGT powder to identify and quantify individual pesticides against a matrix of known pesticides. The mulch films prepared in this study showed comparable and stable mechanical properties compared to commercial biodegradable mulch film, though were much quicker to degrade when buried in the soil. No pesticides were detected in the CGT samples. The films produced were vapour-permeable and may be useful in practical agricultural settings by being able to maintain consistent soil moisture and allowing precipitation to penetrate gradually. The lab-scale production cost for the film was 98.8 AUD/kg, which could be lowered by integrating a continuous film line in large-scale production.

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It is challenging to recapitulate the natural extracellular matrix's hierarchical nano/microfibrous three-dimensional (3D) structure with multilevel pores, good mechanical and hydrophilic properties, and excellent bioactivity for designing and developing advanced biomimetic materials. This work reports a new facile strategy for the scalable manufacturing of such a 3D architecture. Natural polymers in an aqueous solution are interpenetrated into a 3D microfibrous matrix with arbitrary shapes and property characteristics to self-assemble in situ into a nanofibrous network. The collagen fiber-like hierarchical structure and interconnected multilevel pores are achieved by self-assembly of the formed nanofibers within the 3D matrix, triggered by a simple cross-linking treatment. The as-prepared alginate/polypropylene biomimetic matrices are bioactive and have a tunable mechanical property (compressive modulus from ∼17 to ∼24 kPa) and a tunable hydrophilicity (water contact angle from ∼94° to 63°). This facile and versatile strategy allows eco-friendly and scalable manufacturing of diverse biomimetic matrices or modification of any existing porous matrices using different polymers.

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Cotton gin trash (CGT), a lignocellulosic waste generated during cotton fibre processing, has recently received significant attention for production of composite bio-plastics. However, earlier studies were limited to either with biodegradable polymers, through small-scale solution-casting method, or using industrially adaptable extrusion route, but with non-biodegradable polymers. In this study, a scale-up production of completely biodegradable CGT composite plastic film with adjustable biodegradation rate is proposed. First using a twin screw extruder, the prepared CGT powder was combined with polycaprolactone (PCL) to form pellets, and then using the compressing moulding, the pellets were transformed into bio-plastic composite films. Hydrophilic polyethylene glycol (PEG) was used as a plasticiser in the mixture and its impact on the biodegradation rate was analysed. The morphology of CGT bio-plastic composite films showed even distribution of CGT powder within the PCL matrix. The CGT incorporation improved the UV resistance, thermal stability, and Young's modulus of PCL material. Further, the flexibility and mixing properties of the composites were improved by PEG. Overall, this study demonstrated a sustainable production method of CGT bio-plastic films using the whole CGT and without any waste residue produced, where the degradation of the produced composite films can be adjusted to minimise the environmental impact.

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With an increase in environmental pollution and microplastic problems, it is more urgent now to replace non-biodegradable films with biodegradable films that are low-cost and from renewable resources. Cotton gin motes (GM), a type of cellulosic waste that is generated from cotton ginning, is an excellent candidate for fabricating biodegradable films due to its properties and abundance. In this study, GM was first mechanically milled into a fine powder, followed by compounding with polycaprolactone (PCL) and extruded to produce composite pellets which were then compress-moulded into composite films. This environmentally friendly process used physical processing and all the materials were consumed in the process without generating any waste residue. To improve the compatibility and mixing properties between GM and PCL, the use of a plasticiser (polyethylene glycol) was considered. A high content of GM powder (up to 50%) was successfully compounded with the polymer. The SEM images of the composite films showed smooth surface morphology and well-distributed GM powder in the PCL matrix. The added advantage of compounding GM with the polymer matrix was that the composite film developed UV-shielding properties due to the presence of lignin in the GM powder. This property will be critical for films used in UV-resistance applications. Furthermore, the composite even with high GM content (50%), showed good mechanical properties, with 9.5 MPa yield strength and 442% elongation, which was only a 50% decrease in elongation when compared with clear PCL film. The soil biodegradation of GM composite films under controlled temperature (20 °C) and humidity (50%) for 1 month showed around 41% weight loss. Overall, this study demonstrates the potential of GM to be used as a biodegradable and UV-protective composite film for a wide array of applications, such as packaging and UV-protective coverings.

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Globally, automotive manufacturers are looking for ways to produce environmentally sustainable and recyclable materials for automobiles to meet new regulations and customer desires. To enable the needs for rapid response, this study investigated the feasibility of using waste and virgin wool fibres as cost-effective and sustainable alternatives for automotive sound and heat insulation using a chemical-free approach. Several properties of the currently available commercial automotive insulators were investigated in order to facilitate the designing of green wool-based needle-punched nonwoven materials. The effect of fibre diameter, nonwoven surface, layer structure, thickness, and area density on sound absorption and thermal resistance was investigated. The results suggested that the wool nonwoven materials, fabricated using waste and virgin wool fibres, possessed extremely efficient acoustic and thermal insulating properties comparable with the currently used commercial synthetic insulating materials. Besides, the wool nonwoven materials showed identical antibacterial and antifungal properties with a greater biodegradation rate (50%) than that of the commercial synthetic insulating materials. Hence, this study showed that natural wool fibres have the potential to be used as green, lightweight, and sustainable materials in the automobiles, while they qualify for Reuse-Recycle and Reuse-Recover purposes at the end-of-life of vehicles.

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Three-dimensional (3D) microfibrous scaffolds hold great promise for biomedical applications due to their good mechanical properties and biomimetic structure similar to that of the fibrous natural extracellular matrix. However, the large diameter and smooth surface of microfibers provide limited cues for regulating cell activity and behaviors. In this work, we report a facile heat-welding-and-embossing strategy to develop 3D macroporous microfibrous scaffolds with a featured surface topography. Here, solid monosodium glutamate (MSG) particles with crystalline ridge-like surface features play a key role as templates in both the formation of scaffold pores and the surface embossing of scaffold fibers when short thermoplastic polypropylene microfibers were heat-welded. The embossing process can be programmed by adjusting heating temperatures and MSG/fiber ratios. Compared to traditional 3D microfibrous scaffolds, the as-welded 3D scaffolds show higher compressive strength and modulus. Taking mouse C2C12 myoblasts as a model cell line, the scaffolds with embossed surface features significantly promoted the growth of cells, interactions of cells and scaffolds, and formation of myotubes. The findings indicate that the as-prepared 3D scaffolds are a good platform for cell culture study. The facile strategy can be applied to fabricate different fibrous scaffolds by changing the combination of templates and thermoplastic polymer fibers with a melting temperature lower than that of the template. The obtained insights in this work could provide a guide and inspiration for the design and fabrication of functional 3D fibrous scaffolds.

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Artificial recapitulation of the hierarchy of natural protein fibers is crucial to providing strategies for developing advanced fibrous materials. However, it is challenging due to the complexity of the natural environment. Inspired by the liquid crystalline spinning of spiders, we report the development of natural silk-like hierarchical fibers, with bundles of nanofibrils aligned in their long-axis direction, by self-assembly of crystallized silk fibroin (SF) droplets. The formation of self-assembled SF fibers is a process of coalesced droplets sprouting to form a branched fibrous network, which is similar to the development of capillaries in our body. The as-assembled hierarchical SF fibers are highly bioactive and can significantly enhance the spreading and growth of human umbilical vein endothelial cells compared to the natural SF fibers. This work could help to understand the natural silk spinning process of spiders and provides a strategy for design and development of advanced fibrous biomaterials for various applications.

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Dye wastewater has attracted much attention due to its severe environmental and health problems. The main challenge of separating dyes from wastewater, using adsorption, is developing a functional adsorbent that is cost-effective and sustainable. In this work, we have fabricated a novel low-cost membrane with antibacterial properties from naturally sustainable lemongrass (LG). Lemongrass was cut and milled into powder, then dissolved to prepare a lemongrass membrane. Graphene oxide (GO) was also included to prepare a LG/GO composite membrane. The physiochemical and antibacterial properties of membranes were evaluated and their dye adsorption capability was examined using methylene blue (MB) dye at different concentrations. The kinetic study revealed that the MB adsorption process complied with the pseudo second-order model. The lemongrass membrane showed a rough surface morphology, high reduced modulus and hardness, yet comparable dye adsorption to the LG/GO composite membrane. Considering the natural sustainability of lemongrass as an abundant cellulosic resource, its excellent dye adsorption, antibacterial properties and low cost as well as the facile fabrication technology, the lemongrass membrane could be a promising candidate for dye removal from wastewater with easy separation after use.

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The continuous evolution of tissue engineering scaffolds has been driven by the desire to recapitulate structural features and functions of the natural extracellular matrix (ECM). However, it is still an extreme challenge to create a three-dimensional (3D) scaffold with both aligned nanofibers and aligned interconnected macrochannels to mimic the ECM of anisotropic tissues. Here, we develop a facile strategy to create such a scaffold composed of oriented nanofibers and interconnected macrochannels in the same direction, with various natural polymers typically used for tissue regeneration. The orientation of nanofibers and interconnected macrochannels can be easily tuned by manipulating ice crystallization. The scaffold demonstrates both structural and functional features similar to the natural ECM of anisotropic tissues. Taking silk fibroin as an example, the scaffold with radially oriented nanofibers and interconnected macrochannels is more efficient for capturing cells and promoting the growth of both nonadherent embryonic dorsal root ganglion neurons (DRGs) and adherent human umbilical vein endothelial cells (HUVECs) compared to the widely used scaffold types. Interestingly, DRGs and neurites on the SF scaffold demonstrate a 3D growth mode similar to that of natural nerve tissues. Furthermore, the coaligned nanofibers and macrochannels of the scaffold can direct HUVECs to assemble into blood vessel-like structures and their collagen deposition in their arrangement direction. The strategy could inspire the design and development of multifunctional 3D scaffolds with desirable structural features for engineering different tissues.

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Herein, we report the phase inversion of ionomer-stabilized emulsions to form high internal phase emulsions (HIPEs) induced by salt concentration and pH changes. The ionomers are sulfonated polystyrenes (SPSs) with different sulfonation degrees. The emulsion types were determined by conductivity measurements, confocal microscopy and optical microscopy, and the formation of HIPE organogels was verified by the tube-inversion method and rheological measurements. SPSs with high sulfonation degrees (water-soluble) and low sulfonation degrees (water-insoluble) can stabilize oil-in-water emulsions; these emulsions were transformed into water-in-oil HIPEs by varying salt concentrations and/or changing the pH. SPS, with a sulfonation degree of 11.6%, is the most efficient, and as low as 0.2 (w/v)% of the organic phase is enough to stabilize the HIPEs. Phase inversion of the oil-in-water emulsions occurred to form water-in-oil HIPEs by increasing the salt concentration in the aqueous phase. Two phase inversion points from oil-in-water emulsions to water-in-oil HIPEs were observed at pH 1 and 13. Moreover, synergetic effects between the salt concentration and pH changes occurred upon the inversion of the emulsion type. The organic phase can be a variety of organic solvents, including toluene, xylene, chloroform, dichloroethane, dichloromethane and anisole, as well as monomers such as styrene, butyl acrylate, methyl methacrylate and ethylene glycol dimethacrylate. Poly(HIPEs) were successfully prepared by the polymerization of monomers as the continuous phase in the ionomer-stabilized HIPEs.

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Silk fibroin (SF) from Bombyx mori has many established excellent properties and has found various applications in the biomedical field. However, some abilities or capacities of SF still need improving to meet the need for using practically. Indeed, diverse SF-based composite biomaterials have been developed. Here we report the feasibility of fabricating pantothenic acid (vitamin B5, VB5)-reinforcing SF nanofibrous matrices for biomedical applications through green electrospinning. Results demonstrated the successful loading of D-pantothenic acid hemicalcium salt (VB5-hs) into resulting composite nanofibers. The introduction of VB5-hs did not alter the smooth ribbon-like morphology and the silk I structure of SF, but significantly decreased the mean width of SF fibers. SF conformation transformed into ß-sheet from random coil when composite nanofibrous matrices were exposed to 75% (v/v) ethanol vapor. Furthermore, nanofibers still remained good morphology after being soaked in water environment for five days. Interestingly, as-prepared composite nanofibrous matrices supported a higher level of cell viability, especially in a long culture period and significantly assisted skin cells to survive under oxidative stress compared with pure SF nanofibrous matrices. These findings provide a basis for further extending the application of SF in the biomedical field, especially in the personal skin-care field.

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As an excellent biocompatible and biodegradable protein polymer, silk fibroin (SF) has found wide applications, particularly serving as therapeutic agent for tissue-engineering applications, on which both post-spin treatment and sterilization processing are crucial to drug-loaded matrices. To find a safe, effective and appropriate post-spin treatment and sterilization approach for drug-loaded biomaterial matrices is one of the major problems in the field of tissue engineering at present. In this work, a simple, safe and effective approach skillfully integrating post-spin treatment with sterilization processing was developed to drug-loaded SF nanofibrous matrices. Electrospun SF nanofibrous matrices from its aqueous solution were post-treated with 75% ethanol vapor. (13)C-NMR and WAXD analysis demonstrated that such post-spin treatment rendered the structure of SF nanofibrous matrices transform from the silk I form to the silk II form. Furthermore, biological assays suggested that as-treated SF nanofibrous matrices significantly promoted the development of murine connective tissue fibroblasts. Skillfully integrated with novel sterilization processing, 75% ethanol vapor treatment could be a potential approach to designing and fabricating diverse drug-loaded SF nanofibrous matrices serving as therapeutic agents for tissue-engineering applications in that it can effectively protect the drug from losing compared with traditional post-spin treatment and sterilization processing.

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Chitosan, a naturally occurring polysaccharide with abundant resources, has been extensively exploited for various biomedical applications, typically as wound dressings owing to its unique biocompatibility, good biodegradability and excellent antibacterial properties. In this work, composite nanofibrous membranes of chitosan (CS) and silk fibroin (SF) were successfully fabricated by electrospinning. The morphology of electrospun blend nanofibers was observed by scanning electron microscopy (SEM) and the fiber diameters decreased with the increasing percentage of chitosan. Further, the mechanical test illustrated that the addition of silk fibroin enhanced the mechanical properties of CS/SF nanofibers. The antibacterial activities against Escherichia coli (Gram negative) and Staphylococcus aureus (Gram positive) were evaluated by the turbidity measurement method; and results suggest that the antibacterial effect of composite nanofibers varied on the type of bacteria. Furthermore, the biocompatibility of murine fibroblast on as-prepared nanofibrous membranes was investigated by hematoxylin and eosin (H&E) staining and MTT assays in vitro, and the membranes were found to promote the cell attachment and proliferation. These results suggest that as-prepared chitosan/silk fibroin (CS/SF) composite nanofibrous membranes could be a promising candidate for wound healing applications.

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