Ternary blends of poly(lactic acid) (PLA), polycaprolactone (PCL) and cellulose acetate butyrate (CAB) were fabricated into the form of electrospun nanofibres targeted for skin tissue scaffolds. The effects of blend ratio and molecular mass of PCL (PCL1 and PCL2) on morphology, miscibility, crystallinity, thermal properties, surface hydrophilicity and cell culture of the nanofibres were investigated. Blends with high PLA loading (80/10/10 PLA/PCL/CAB) gave fibres with a smooth surface, owing to the enhanced miscibility between the polymer chains from the presence of CAB, which acts as compatibilizer. In contrast, blends with high PCL loading were immiscible, which led to beads during the electrospinning process. The increased molecular mass of PCL2 produced smoother fibres than low-molecular-mass PCL1. The XRD patterns of blends of PLA/PCL1/CAB and PLA/PCL2/CAB were similar to one another, in which the high-crystallinity peaks of PCL seen for 20/70/10 blends were very small for 50/40/10 blends and much less prevalent for 80/10/10 blends. Better fibre formation (80/10/10 > 50/40/10 > 20/70/10) with less crystallinity occurs in well-formed fibres. Selected blends of PLA/PCL/CAB promoted growth of NIH/3T3 fibroblast cells, demonstrating that our novel biocompatible ternary blend nanofibrous scaffolds have potential in skin tissue repair applications. In addition, this work helps in the design and understanding of the factors that control the properties of nanofibrous PLA/PCL/CAB scaffolds.
Silk sericin (SS) has been extensively used to fabricate scaffolds for tissue engineering. However, due to its inferior mechanical properties, it has been found to be a poor choice of material when being electrospun into nanofibrous scaffolds. Here, SS has been combined with poly(vinyl alcohol) (PVA) and electrospun to create scaffolds with enhanced physical properties. Crucially, these SS/PVA nanofibrous scaffolds were created using only distilled water as a solvent with no added crosslinker in an environmentally friendly process. Temperature has been shown to have a marked effect on the formation of the SS sol–gel transition and thus influence the final formation of fibers. Heating the spinning solutions to 70 °C delivered nanofibers with enhanced morphology, water stability and mechanical properties. This is due to the transition of SS from β‐sheets into random coils that enables enhanced molecular interactions between SS and PVA. The most applicable SS/PVA weight ratios for the formation of nanofibers with the desired properties were found to be 7.5/1.5 and 10.0/1.5. The fibers had diameters ranging from 60 to 500 nm, where higher PVA and SS concentrations promoted larger diameters. The crystallinity within the fibers could be controlled by manipulation of the balance between PVA and SS loadings. In vitro degradation (in phosphate buffer solution, pH 7.4 at 37 °C) was 30–50% within 42 days and fibers were shown to be nontoxic to skin fibroblast cells. This work demonstrates a new green route for incorporating SS into nanofibrous fabrics, with potential use in biomedical applications. © 2019 Society of Chemical Industry
Core–shell fibres (CSFs) offer a simple route to multifunctional hybrid materials for a wide range of applications. Herein, we report the design of a core–shell electrospun nanofibrous fabric containing a hydrophilic core and hydrophobic shell. CSFs were fabricated for the first time from poly(vinyl alcohol)/silk sericin (from silk cocoons) as the core and poly(lactide‐co‐glycolide) as the shell. The core serves as a potential carrier for water‐soluble bioactive agents, and the shell works as a barrier to prevent premature release of water‐soluble agents from the core. The effect of the molecular weight of poly(lactide‐co‐glycolide) and the loading of silk sericin on the morphology of fibres was studied. The parameters that significantly influence the core–shell electrospinning process were studied to elucidate the most effective conditions to create our multifunctional nanofibrous fabrics with smooth fibre morphology (diameters in the range 800–1300 nm) and low bead formation. Our CSFs were shown to degrade in saline buffer solution (pH 7.4) and were readily rendered with anti‐bacterial properties against Staphylococcus aureus and Escherichia coli by the post‐spinning deposition of silver nanoparticles (AgNPs, 40 nm diameter) or cinnamon essential oil (CEO). The fibres were non‐toxic to normal human dermal fibroblast cell lines, as the cells were shown to attach and proliferate on CSFs, CSF/AgNPs and CSF/CEO with good cell tolerance for 72 h of incubation. These smart multifunctional CSFs show great potential towards smart delivery fabrics/dressings capable of carrying water‐soluble bioactive agents surrounded by a protective, but degradable, antibacterial shell to guard the cargo for more effective controlled release. © 2021 Society of Industrial Chemistry.
This work was concerned with the fabrication of a porous hydrogel system suitable for medium to heavy-exudating wounds where traditional hydrogels cannot be used. The hydrogels were based on 2-acrylamido-2-methyl-1-propane sulfonic acid (AMPs). In order to produce the porous structure, additional components were added (acid, blowing agent, foam stabilizer). Manuka honey (MH) was also incorporated at concentrations of 1 and 10% w/w. The hydrogel samples were characterized for morphology via scanning electron microscopy, mechanical rheology, swelling using a gravimetric method, surface absorption, and cell cytotoxicity. The results confirmed the formation of porous hydrogels (PH) with pore sizes ranging from ~50–110 µm. The swelling performance showed that the non-porous hydrogel (NPH) swelled to ~2000%, while PH weight increased ~5000%. Additionally, the use of a surface absorption technique showed that the PH absorbed 10 μL in <3000 ms, and NPH absorbed <1 μL over the same time. Incorporating MH the enhanced gel appearance and mechanical properties, including smaller pores and linear swelling. In summary, the PH produced in this study had excellent swelling performance with rapid absorption of surface liquid. Therefore, these materials have the potential to expand the applicability of hydrogels to a range of wound types, as they can both donate and absorb fluid.
This study investigated the performance of novel hydrogels based on poly (N-vinylformamide) (PNVF), copolymers of NVF with N-hydroxyethyl acrylamide (HEA) (P(NVF-co-HEA)), and 2-carboxyethyl acrylate (CEA) (P(NVF-co-CEA)), which were synthesized by photopolymerization using a UVLED light source. The hydrogels were analyzed for important properties such as equilibrium water content (%EWC), contact angle, freezing and non-freezing water, and diffusion-based in vitro release. The results showed that PNVF had an extremely high %EWC of 94.57%, while a decreasing NVF content in the copolymer hydrogels led to a decrease in water content with a linear relationship with HEA or CEA content. Water structuring in the hydrogels showed appreciably more variance, with ratios of free to bound water differing from 16.7:1 (NVF) to 1.3:1 (CEA), corresponding to PNVF having ~67 water molecules per repeat unit. The release studies of different dye molecules followed Higuchi’s model, with the amount of dye released from the hydrogels depending on the amount of free water and the structural interactions between the polymer and the molecule being released. The results suggest that PNVF copolymer hydrogels have potential for controlled drug delivery by altering the polymer composition to govern the amount and ratio of free to bound water contained in the hydrogels.
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