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Type 2 diabetes mellitus (T2DM) is a chronic metabolic disease that is increasingly common all over the world with a high risk of progressive hyperglycemia and high microvascular and macrovascular complications. The currently used drugs in the treatment of T2DM have insufficient glucose control and can carry detrimental side effects. Several drug delivery systems have been investigated to decrease the side effects and frequency of dosage, and also to increase the effect of oral antidiabetic drugs. In recent years, the use of microbubbles in biomedical applications has greatly increased, and research into microactive carrier bubbles continues to generate more and more clinical interest. In this study, various monodisperse polymer nanoparticles at different concentrations were produced by bursting microbubbles generated using a T-junction microfluidic device. Morphological analysis by scanning electron microscopy, molecular interactions between the components by FTIR, drug release by UV spectroscopy, and physical analysis such as surface tension and viscosity measurement were carried out for the particles generated and solutions used. The microbubbles and nanoparticles had a smooth outer surface. When the microbubbles/nanoparticles were compared, it was observed that they were optimized with 0.3 wt % poly(vinyl alcohol) (PVA) solution, 40 kPa pressure, and a 110 μL/min flow rate, thus the diameters of the bubbles and particles were 100 ± 10 μm and 70 ± 5 nm, respectively. Metformin was successfully loaded into the nanoparticles in these optimized concentrations and characteristics, and no drug crystals and clusters were seen on the surface. Metformin was released in a controlled manner at pH 1.2 for 60 min and at pH 7.4 for 240 min. The process and structures generated offer great potential for the treatment of T2DM.

Renewable polymers with excellent stretchability and self-healing ability are interesting for a wide range of applications. A novel type of wholly biobased, self-healing, polyamide-based thermoplastic elastomer was synthesized using a fatty dimer acid and a fatty dimer amine, both containing multiple alkyl chains, through facile one-pot condensation polymerization under different polymerization times. The resulting elastomer shows superior stretchability (up to 2286%), high toughness, and excellent shape recovery after being stretched to different strains. This elastomer also displays high room-temperature autonomous self-healing efficiency after fracture and zero water uptake during water immersion. The highly entangled main chain, the multiple dangling chains, the abundant reversible physical bonds, the intermolecular diffusion, and the low ratio of amide to methylene group within the elastomer are responsible for these extraordinary properties. The polymerization time influences the properties of the elastomer. The use of the optimal self-healing thermoplastic elastomer in anticorrosion coating, piezoresistive sensing, and highly stretchable fibers is also demonstrated. The elastomer coating prevents stainless-steel products from corrosion in a salty environment due to its superhydrophobicity. The elastomer serves as a robust flexible substrate for creating self-healing piezoresistive sensors with excellent repeatability and self-healing efficiency. The elastomer fiber yarn can be stretched to 950% of its original length confirming its outstanding stretchability.

Forming polymeric core–sheath nanofibers is gaining prominence owing to their numerous potential applications, most notably in functional scenarios such as antiviral filtration, which is attracting significant attention due to the current COVID pandemic. This study has successfully designed and constructed a novel pressurized gyration vessel to fabricate core–sheath polymer nanofibers. Several water-soluble and water-insoluble polymer combinations are investigated. Both polyethylene oxide and polyvinyl alcohol were used as the core while both poly(lactic acid) (PLA) and poly(caprolactone) (PCL) were used as the sheath; PLA and PCL were used as core and sheath, in different instances; respectively. The fluid behavior of the core–sheath within the vessel was studied with and without applied pressure using computational fluid dynamics to simulate the core–sheath flow within the chamber. A high-speed camera was used to observe the behavior of jetted solutions at core–sheath openings, and the best scenario was achieved using 6000 rpm spinning speed with 0.2 MPa (twice atmospheric) applied pressure. The surface morphology of core–sheath fibers was studied using a scanning electron microscope, and focused ion beam milling assisted scanning electron microscopy was used to investigate the cross-sectional features of the produced fibers. Laser confocal scanning microscopy was also used to verify the core–sheath structure of the fibers, which were further characterized by Fourier transform infrared spectroscopy and differential scanning calorimetry. Thus, using a variety of polymer combinations, we show, both theoretically and experimentally, how core–sheath fibers evolve in a vessel that can serve as a scalable manufacturing pressurized gyration production process.

The present study describes the use of two taste-masking polymers to fabricate a formulation of chlorpheniramine maleate for paediatric administration. Co-axial electrospinning was utilized to create layered nanofibres, the two polymers, Eudragit® E PO and Kollicoat® Smartseal, were alternated between the core and the shell of the system in order to identify the optimum taste-masked formulation. The drug was loaded in the core on all occasions. It was found that the formulation with Kollicoat® Smartseal in the core with the drug, and Eudragit® E PO in the shell showed the most effective taste-masking compared to the other formulations. These fibres were in the nano-range and had smooth morphology as verified by scanning electron microscopy. Solid-state characterization and thermal analysis confirmed that amorphous solid dispersions were formed upon electrospinning. The Insent E-tongue was used to assess the taste-masking efficiency of the samples, and it was found that this formulation was undetectable by the bitter sensor, indicating successful taste-masking compared to the raw version of the drug. The E-tongue also confirmed the drug’s bitterness threshold as compared to quinine HCl dihydrate, a parameter that is useful for formulation design and taste-masking planning.

Suspensions containing 8 and 10 wt% polyacrylonitrile (PAN) and 1, 2, 3, 5, 7 and 10 wt% graphene oxide (GO) were prepared using a special mixing routine and fibres were generated from these mixtures by pressurised gyration. The combination of pressure and gyration speed was effective in controlling the fibre morphology and fibre diameter which ranged from 1 to 20 μm. Fibres were pyrolysed to remove the polymer and only the 10 wt% PAN fibres survived. The microstructure of the pre- and post-pyrolysis products were characterised by scanning electron microscopy, both with and without focussed ion beam etching, Fourier-transformed infrared and Raman spectroscopies. Pyrolysed fibre electrical conductivities were measured and only those containing 1 and 2 wt% GO were conductive.

The ability to generate core&ndash, sheath bicomponent polymer nanofibers in a single-step with scale-up possibilities is demonstrated using pressurised gyration manufacturing. This is the first time that nanofiber containing more than one polymer having a core&ndash, sheath configuration has been generated in this way. Water-soluble polymers polyethylene oxide (PEO) and polyvinyl pyrrolidone (PVP) are used as the core and sheath layers, respectively. Core&ndash, sheath nanofibers with a diameter in the range of 331 to 998 nm were spun using 15 wt % PEO and 15 wt % PVP polymer solutions. The forming parameters, working pressure and rotating speed, had a significant influence on the size, size distribution and the surface morphology of the nanofibers generated. Overall, fibre size decreased with increasing working pressure and rotating speed. The fibre size was normally distributed in all cases, with 0.2 MPa working pressure in particular showing narrower distribution. The fibre size distributions for 0.1 and 0.3 MPa working pressure were broader and a mean fibre size of 331 nm was obtained in the latter case. The fibre size was evenly distributed and narrower for rotating speeds of 2000 and 4000 RPMs. The distribution was broader for rotating speed of 6000 RPM with a mean value obtained at 430 nm. Continuous, smooth and bead-free fibre morphologies were obtained in each case. The fibre cross-section analysis using a focused ion beam machine showed a solid core surrounded by a sheath layer. Our findings demonstrate that the pressurised gyration could be used to produce core&ndash, sheath polymer nanofibers reliably and cost-effectively with scale-up possibilities (~4 kg h&minus, 1).

Amphiphilic block copolymers are widely used in science owing to their versatile properties. In this study, amphiphilic block copolymer poly(lactic- co-glycolic acid)- block-poly(ethylene glycol) (PLGA- b-PEG) was used to create microdroplets in a T-junction microfluidic device with a well-defined geometry. To compare interfacial characteristics of microdroplets, dichloromethane (DCM) and chloroform were used to prepare PLGA- b-PEG solution as an oil phase. In the T-junction device, water and oil phases were manipulated at variable flow rates from 50 to 300 μL/min by increments of 50 μL/min. Fabricated microdroplets were directly collected on a glass slide. After a drying period, porous two-dimensional and three-dimensional structures were obtained as honeycomb-like structure. Pore sizes were increased according to increased water/oil flow rate for both DCM and chloroform solutions. Also, it was shown that increasing polymer concentration decreased the pore size of honeycomb-like structures at a constant water/oil flow rate (50:50 μL/min). Additionally, PLGA- b-PEG nanoparticles were also obtained on the struts of honeycomb-like structures according to the water solubility, volatility, and viscosity properties of oil phases, by the aid of Marangoni flow. The resulting structures have a great potential to be used in biomedical applications, especially in drug delivery-related studies, with nanoparticle forming ability and cellular responses in different surface morphologies.

Several new spinning methods have been developed recently to mass produce polymeric fibers. Pressure-coupled infusion gyration is one of them. Because the fiber diameter plays a pivotal role for the mechanical, electrical, and optical properties of the produced fiber mats, in this work, polyethylene oxide is used as a model polymer, and the processing parameters including polymer concentration, infusion (flow) rate, working pressure, and rotational speed are chosen as variables to control fiber diameters spanning the micro- to nanoscale. The experimental process is modeled using response surface methodology, both in linear and nonlinear fitting formats, to allow optimization of processing parameters. The successes of the fitted models are evaluated using adjusted R2 and Akaike information criterion. A systematic description of the experimental process could be obtained according to the model in this study. From the analysis of variance, it is concluded that the polymer concentration of the solution and the working pressure affected the fiber diameters more strongly than other parameters.

Cellulose derivatives are an attractive sustainable material used frequently in biomaterials, however their solubility in safe, green solvents is not widely exploited. In this work three cellulose derivatives; ethyl cellulose, cellulose acetate and carboxymethyl cellulose were subjected to electrohydrodynamic processing. All were processed with safe, environmentally friendly solvents; ethanol, acetone and water. Ethyl cellulose was electrospun and an interesting transitional region was identified. The morphological changes from particles with tails to thick fibres were charted from 17 to 25 wt% solutions. The concentration and solvent composition of cellulose acetate (CA) solutions were then changed; increasing the concentration also increased fibre size. At 10 wt% CA, with acetone only, fibres with heavy beading were produced. In an attempt to incorporate water in the binary solvent system to reduce the acetone content, 80:20 acetone/water solvent system was used. It was noted that for the same concentration of CA (10 wt%), the beading was reduced. Finally, carboxymethyl cellulose was electrospun with poly(ethylene oxide), with the molecular weight and polymer compositions changed and the morphology observed.

Cardiac tissue engineering (CTE) is currently a prime focus of research due to an enormous clinical need. In this work, a novel functional material, Poly(3-hydroxyoctanoate), P(3HO), a medium chain length polyhydroxyalkanoate (PHA), produced using bacterial fermentation, was studied as a new potential material for CTE. Engineered constructs with improved mechanical properties, crucial for supporting the organ during new tissue regeneration, and enhanced surface topography, to allow efficient cell adhesion and proliferation, were fabricated. Our results showed that the mechanical properties of the final patches were close to that of cardiac muscle. Biocompatibility of the P(3HO) neat patches, assessed using Neonatal ventricular rat myocytes (NVRM), showed that the polymer was as good as collagen in terms of cell viability, proliferation and adhesion. Enhanced cell adhesion and proliferation properties were observed when porous and fibrous structures were incorporated to the patches. Also, no deleterious effect was observed on the adults cardiomyocytes’ contraction when cardiomyocytes were seeded on the P(3HO) patches. Hence, P(3HO) based multifunctional cardiac patches are promising constructs for efficient CTE. This work will provide a positive impact on the development of P(3HO) and other PHAs as a novel new family of biodegradable functional materials with huge potential in a range of different biomedical applications, particularly CTE, leading to further interest and exploitation of these materials.

A one step approach to prepare hybrid nanoparticle embedded polymer fibres using pressurised gyration is presented. Two types of novel antimicrobial nanoparticles and poly(methylmethacrylate) polymer were used in this work. X-ray diffraction analysis of the nanoparticles revealed Ag, Cu and W are the main elements present in them. The concentration of the polymer solution and the nanoparticle concentration had a significant influence on the fibre diameter, pore size and morphology. Fibres with a diameter in the range of 6-20μm were spun using 20wt% polymer solutions containing 0.1, 0.25 and 0.5 wt% nanoparticles under 0.3MPa working pressure and a rotational speed of 36,000rpm. Continuous, bead-free fibre morphologies were obtained for each case. The pore size in the fibres varied between 36 and 300nm. Successful incorporation of the nanoparticles in polymer fibres was confirmed by energy dispersive x-ray analysis. The fibres were also gyrospun on to metallic discs to prepare filters which were tested for their antibacterial activity on a suspension of Pseudomonas aeruginosa. Nanoparticle loaded fibres showed higher antibacterial efficacy than pure poly(methylmethacrylate) fibres.

Poly(glycerol sebacate) (PGS) was discovered in the previous decade and is a promising bioelastomer with tuneable mechanical, biodegradable and biocompatible properties. Despite of these superiorities, PGS possesses solubility and processability disadvantages. To overcome these drawbacks of PGS, blends could be formed with a polymer which is soluble in a common solvent with PGS prepolymer, having a melting temperature above the crosslinking temperature and which can be removed from the structure after crosslinking. In this study, PGS fibers were fabricated for the first time using pressurized gyration as scaffolds. Fibers were obtained through blending the synthesized PGS prepolymer with poly(vinyl alcohol) (PVA) to overcome solubility/melting drawbacks of crosslinked PGS polymer. Obtained fiber diameters have a narrow size distribution which did not change after thermal crosslinking. After the washing procedure, ∼25% decrease in the average fiber diameter was observed due to the PVA removal. Resulting PGS fibers were characterized in terms of chemical structure, morphology, and cell viability. Fibroblast cell adhesion and spreading on three-dimensional fiber networks were determined by microscopy. PGS fibers supported cell adhesion and proliferation. After 7 days of cell-PGS fiber interactions, cell proliferation and spreading increased without any toxicity.

Bacterial Cellulose (BC) has over recent decades shown great versatility in wound healing dressings, but is difficult to spin fibers with at high concentrations. An investigation into the preparation of bandage-like fibrous meshes is carried out to determine the optimal blend of polycaprolactone (PCL) and polylactic acid (PLA) as a suitable carrier for BC. Using a simple centrifugal spinning setup, polymer blends of PCL, PLA and BC are investigated as a ternary system to determine the most suitable composition with a focus on achieving maximal BC concentration. It is found that BC content in the fibers above 10 wt % reduced product yield. By creating blends of PLA-PCL fibers, we can create a more suitable system in terms of yield and mechanical properties. The fibrous samples are examined for yield, fiber morphology using scanning electron microscopy, mechanical properties using tensile testing and chemical characteristics using Fourier-transform infrared spectroscopy. A fibrous scaffold with &gt, 30 wt % BC was produced with enhanced mechanical properties owing to the blending of PLA and PCL.

[Image: see text] Electrospinning is increasingly becoming a viable means of producing drug delivery vehicles for oral delivery, particularly as issues of manufacturing scalability are being addressed. In this study, electrospinning is explored as a taste-masking manufacturing technology for bitter drugs. The taste-masking polymer Eudragit E PO (E-EPO) was electrospun, guided by a quality by design approach. Using a design of experiment, factors influencing the production of smooth fibers were investigated. Polymer concentration, solvent composition, applied voltage, flow rate, and gap distance were the parameters examined. Of these, polymer concentration was shown to be the only statistically significant factor within the ranges studied (p-value = 0.0042). As the concentration increased, smoother fibers were formed, coupled with an increase in fiber diameter. E-EPO (35% w/v) was identified as the optimum concentration for smooth fiber production. The optimized processing conditions identified were a gap distance of 175 mm, an applied voltage of between 15 and 20 kV, and a flow rate of 1 mL/h. Using this knowledge, the production optimization of electrospun E-EPO with chlorpheniramine maleate (CPM), a bitter antihistamine drug, was explored. The addition of CPM in drug loads of 1:6 up to 1:10 CPM/E-EPO yielded smooth fibers that were electrospun under conditions similar to placebo fibers. Solid-state characterization showed CPM to be molecularly dispersed in E-EPO. An electronic tasting system, or E-tongue, indicated good taste-masking performance as compared to the equivalent physical mixtures. This study therefore describes a means of producing, optimizing, and assessing the performance of electrospun taste-masked fibers as a novel approach to the formulation of CPM and potentially other bitter drug substances.

In this work, a simple microfluidic junction with a T geometry and coarse (200 μm diameter) capillaries was used to generate monodisperse microbubbles with an alginate polymer shell. Subsequently, these bubbles were used to prepare porous alginate films with good control over the pore structure. The lack of pore size, shape, and surface control in scalable forming of polymeric films is a major application-limiting drawback at present. Controlling the thinning process of the shell of the bubbles to tune the surface of the resulting structures was also explored. Films were prepared with nanopatterned surfaces by controlling the thinning of the bubble shell, with the aid of surfactants, to induce efficient bursting (fragmentation) of bubbles to generate nanodroplets, which become embedded within the film surface. This novel feature greatly expands and enhances the use of hydrophilic polymers in a wide range of biomedical applications, particularly in drug delivery and tissue engineering, such as studying cellular responses to different morphological surfaces.

This work focuses on forming bead on string poly(caprolactone) (PCL) by using gyration under pressure. The fibre morphology of bead on string is an interesting feature that falls between bead-free fibres and droplets, and it could be effectively controlled by the rheological properties of spinning dopes and the major processing parameters of the pressurised gyration system which are working pressure and rotating speed. Bead products were not always spherical in shape and tended to be more elliptical, therefore both their width and length were measured. The average bead width and length produced spanned a range 145-660μm and 140-1060μm, respectively. The average distance between two adjacent beads (i.e. inter-bead distance) and the bead size (width and length) are shown to be a function of processing parameters and polymer concentration. An interesting morphology i.e. beads with short fibre was observed when using a high polymer concentration. Bead on string structure agglomeration was promoted by a low polymer concentration. Formation of droplets or agglomerated bead on string is promoted below 5wt% polymer concentration, and beads with short fibre were present in the microstructure beyond a polymer concentration of 20wt%.

A simple and effective process combining pressure and gyration has been developed and used to jet-out composite fibres containing graphene nanoplatelets. Thermoplastic polyurethane and phenolic resin polymers were used as matrices. Processing parameters such as rotation speed, pressure and polymer concentration had a marked influence on the composite fibre diameter. Focussed ion beam milling and etching verified the effective incorporation of the graphene nanoplatelets into the composite fibres. Morphological, rheological, physico-chemical and thermal properties of the composite fibres were evaluated to identify possible applications for them.

A pressurized melt gyration process has been used for the first time to generate poly(e-caprolactone) (PCL) fibers. Gyration speed, working pressure, and melt temperature are varied and these parameters influence the fiber diameter and the temperature enabled changing the surface morphology of the fibers. Two types of nonwoven PCL fiber constructs are prepared. First, Ag-doped PCL is studied for antibacterial activity using Gram-negative Escherichia coli and Pseudomonas aeruginosa microorganisms. The melt temperature used to make these constructs significantly influences antibacterial activity. Neat PCL nonwoven scaffolds are also prepared and their potential for application in muscular tissue engineering is studied with myoblast cells. Results show significant cell attachment, growth, and proliferation of cells on the scaffolds.

A novel fabrication of polymer composite fibers using polycaprolactone (PCL), montmorillonite nanoclay (MMT-Clay), and nano-hydroxyapatite-clay (HAP MMT-Clay) is reported for bone tissue engineering applications. Using a pressurized gyration (PG) setup, polycaprolactone (PCL) fibers incorporated with in situ mineralized HAP MMT-Clay and MMT-Clay were investigated. Using the novel fabrication method, we were able to successfully manufacture HAP-nanoclay-PCL fibers. Further, 3D scaffolds made using the prepared fibers were able to enhance bone growth, cell viability, and proliferation. The results demonstrated that the polymer fiber scaffolds are biocompatible, and the cells were able to thrive and differentiate on the fiber scaffolds. A significant increase in cell viability, osteogenic differentiation, ECM formation, and collagen formation was observed with PCL HAP MMT-Clay fibers scaffolds compared to the behaviors in PCL fibers. Further, the intracellular ALP levels increased with PCL HAP MMT-Clay fiber scaffold, indicating enhanced osteogenic differentiation of MSCs. This work shows a promising outlook for the future of manufacturable composite nanoclay polymer fibers incorporated as scaffolds for bone tissue engineering applications.

The application of polymer fibers has rocketed to unimaginable heights in recent years and occupies every corner of our day-to-day life, from knitted protective textile clothes to buzzing smartphone electronics. Polymer fibers could be obtained from natural and synthetic polymers at a length scale from the nanometer to micrometer range. These fibers could be formed into different configurations such as single, core–sheath, hollow, blended, or composite according to human needs. Of these several conformations of fibers, core–sheath polymer fibers are an interesting class of materials, which shows superior physical, chemical, and biological properties. In core–sheath fiber structures, one of the components called a core is fully surrounded by the second component known as a sheath. In this format, different polymers can be applied as a sheath over a solid core of another polymer, thus resulting in a variety of modified properties while maintaining the major fiber property. After a brief introduction to core–sheath fibers, this review paper focuses on the development of the electrospinning process to manufacture core–sheath fibers followed by illustrating the current methodology and approaches to form them on a larger scale, suitable for industrial manufacturing and exploitation. Finally, the paper reviews the applications of the core–sheath fibers, in particular, recent studies of core–sheath polymer fibers in tissue engineering (nerve, vascular grafts, cardiomyocytes, bone, tendons, sutures, and wound healing), growth factors and other bioactive component release, and drug delivery. Therefore, core–sheath structures are a revolutionary development in the field of science and technology, becoming a backbone to many emerging technologies and novel opportunities.

An electrohydrodynamic printer designed and constructed in our laboratory was used to fabricate polycaprolactone nasal septal scaffolds. Three different polymer concentrations (15 wt.%, 18 wt.% and 23 wt.%) were used. The generated scaffolds, each with a unique architecture, were evaluated using PeakForce Quantitative Nanomechanical Mapping (QNM) Atomic Force Microscopy (AFM) to measure Young's modulus using the Dejaguin–Müller–Toporov (DMT) model. In addition, this allowed estimation of adhesion forces, deformation and dissipation energy of the scaffolds. The degree of crystallinity and purity of the polymer in the scaffolds were characterized by differential scanning calorimetry and Fourier transform infrared spectroscopy. Keywords: Electrohydrodynamic, Direct-write, Polymer, Polycaprolactone, Scaffold, Nasal, Septal

Co-axial electrospraying and electrospinning are versatile electrohydrodynamic (EHD) techniques that can be used to encapsulate a variety of materials in the form of polymeric particles and fibres via a one step process. The successful production of uniform encapsulated products in co-axial EHD (CEHD) processing depends on multiple parameters including solution concentration, applied voltage and needle capillary diameter. Although many studies have been conducted to investigate the effects of these parameters, there has been very limited research on how the axial displacement between the two needle tips affects the final products formed. Hence the purpose of this study was to adjust the positioning of the inner needle such that its tip extends beyond, is level with or resides inside that of the outer needle and to thus determine the most effective arrangement for controlling product size, uniformity and/or yield. Core–shell particles were prepared using two polymers, poly(lactic-co-glycolic)acid (PLGA) as the shell and polymethylsilsesquioxane (PMSQ) as the core and core–shell fibres using PMSQ as the shell and a volatile liquid, perfluorohexane (PFH) as the core. The products formed were analyzed by optical microscopy, scanning electron microscopy (SEM) and transmission electron microscopy (TEM). After analysis, it was concluded that the most effective arrangement for generating both particles and fibres with the optimal combination of size, uniformity and yield was to have the inner needle 2 mm inside the outer needle. This allows for formation of a stable cone–jet and successful encapsulation of the inner liquid within the outer liquid, before the outer stable cone–jet forms. The corresponding collected product diameter and percentage of products in which material was successfully encapsulated were found to be 0.6 ± 0.1 μm and 85 ± 3% respectively for particles and 9 ± 1 μm and 92 ± 2% for fibres.

Nanofibers featuring functional nanoassemblies show great promise as enabling constituents for a diverse range of applications in areas such as tissue engineering, sensing, optoelectronics, and nanophotonics due to their controlled organization and architecture. An infusion gyration method is reported that enables the production of nanofibers with inherent biological functions by simply adjusting the flow rate of a polymer solution. Sufficient polymer chain entanglement is obtained at Berry number > 1.6 to make bead-free fibers integrated with gold nanoparticles and proteins, in the diameter range of 117-216 nm. Integration of gold nanoparticles into the nanofiber assembly is followed using a gold-binding peptide tag genetically conjugated to red fluorescence protein (DsRed). Fluorescence microscopy analysis corroborated with Fourier transform infrared spectroscopy (FTIR) data confirms the integration of the engineered red fluorescence protein with the nanofibers. The gold nanoparticle decorated nanofibers having red fluorescence protein as an integral part keep their biological functionality including copper-induced fluorescence quenching of the DsRed protein due to its selective Cu+2 binding. Thus, coupling the infusion gyration method in this way offers a simple nanoscale assembly approach to integrate a diverse repertoire of protein functionalities into nanofibers to generate biohybrid materials for imaging, sensing, and biomaterial applications.

This paper reports for the very first time a facile and simple method, consisting of simultaneous centrifugal spinning and solution blowing, to mass produce ceramic fibres from preceramic polymers. Solutions of two different commercially available silicone resins and a mixture of a silicone resin and graphene were used, and a polymer (polyvynilpyrolidone) was added to aid the fibre generation process. The fibre diameter and the morphology of the spun and the pyrolysed fibres were shown to be influenced by rotating speed, working pressure and the polymer concentration. Non-porous fibres were obtained using a low volatility binary solvent system and, after pyrolysis at high temperature, dense SiOC ceramic fibre bundles were produced. This fabrication method based on pressurised gyration shows great promise in the mass production of ceramic fibre bundles.

Solid polymer nanospheres with contrasting size and surface roughness were prepared using a V-shaped microfluidic junction device. Polymethysilsesquioxane (PMSQ) polymer dissolved separately in either methanol, or ethanol, or propanol or butanol was used, and the nanospheres produced were collected in distilled water at two different temperatures (23°C and 100°C). Each polymer solution together with a volatile liquid, perfluorohexane, was fed into the inlet channels of the microfluidic device. The process of nanosphere generation was recorded by high-speed camera imaging. Only PMSQ solutions of ethanol and propanol generated well-defined nanospheres. The influence of the solvents and the nanosphere collection temperature on nanosphere size distribution and surface roughness was assessed using scanning electron microscopy, which showed that solvent selection was crucial in tailoring the size distribution of the nanospheres and that the nanospheres collected at 100°C had a noticeably rougher surface. The temperature also helped to vary the size distribution of the nanospheres. Nanospheres containing Evans blue dye were also prepared, and those with a rough surface exhibited a very different dye release profile compared with those having a smooth surface. In fact, the release profile changes due to a size differential can be largely compensated for by having a rough surface.

The selection of a solvent or solvent system and the ensuing polymer–solvent interactions are crucial factors affecting the preparation of fibers with multiple morphologies. A range of poly(methylmethacrylate) fibers were prepared by pressurised gyration using acetone, chloroform, N,N-dimethylformamide (DMF), ethyl acetate and dichloromethane as solvents. It was found that microscale fibers with surface nanopores were formed when using chloroform, ethyl acetate and dichloromethane and poreless fibers were formed when using acetone and DMF as the solvent. These observations are explained on the basis of the physical properties of the solvents and mechanisms of pore formation. The formation of porous fibers is caused by many solvent properties such as volatility, solubility parameters, vapour pressure and surface tension. Cross-sectional images show that the nanopores are only on the surface of the fibers and they were not inter-connected. Further, the results show that fibers with desired nanopores (40–400 nm) can be prepared by carefully selecting the solvent and applied pressure in the gyration process.

Honeycomb-like 3D polymeric structures are useful to grow cells inside pores or in between nanofibres in cellular containment but their generation and morphology control involves different processing and forming procedures. In this work, using high speed camera footage, we show the dramatic effect of relative humidity (RH) has on the deposition of honeycomb structures using a hydrophilic water-soluble polymer. Approximately 35 mm diameter deposits were generated under several conditions of humidity while all other process parameters were kept constant. The morphology of the structures, i.e., their porosity and nanofibres, were studied and are related to the jet behaviour characteristics to explain why 3D honeycomb structures are obtained under selected optimum humidity conditions. 3D honeycomb structures were obtained only at an optimised 73% RH.

Polymeric nanoparticles have important applications in drug delivery, biotechnology, diagnostics and energy harvesting. We report a new technique named electrospray nanoprecipitation, which combines electrospray with agitated solvent displacement. The process enables one-step formation of polymeric nanoparticles

The ability to generate nanofibres useful for biomedical applications at bench and at a larger scale is a significant manufacturing challenge. In this study, we demonstrate that it is possible to generate nanofibre meshes of poly(N-vinylpyrrolidone) (PVP) using pressurised gyration. The effects of altering polymer molecular weight and concentration on fibre morphology and size have been investigated, with identification of minimum values for both parameters for successful fibre fabrication. In addition, we note that changing the molecular weight may result in changes to the Fourier Transform Infrared (FTIR) spectra associated with changes in fibre intramolecular bond strength and arrangement. Overall the study has demonstrated that pressure gyration represents a feasible means of producing nanofibres (470–970 nm) on a scale commensurate with commercial viability and have identified key parameters that influence mesh structure.

The electrohydrodynamic (EHD) technique has traditionally been confined to the bench-top. Recently, a portable EHD device was constructed that allows the process to be applied in a much more flexible and versatile manner. In this article, the effect of electrode and collector height on the fibers generated by EHD and wound-dressing forming capabilities of the device tested on different types of simulated wound morphologies were investigated. Dressings were also fabricated on living tissue to investigate jet behavior and product morphology. The EHD device was found to be capable of controlled deposition of micrometer-sized poly(D,L-lactide-co-glycolide) acid fibers that can form an opaque, waterproof wound dressing on human skin within a few minutes with excellent adherence.

Core-sheath fibres of two polymers were generated using a novel set-up where rotating speed and pressure can be varied at ambient temperature. The specially designed spinneret consists of inner and outer chambers which can accommodate two polymers and other additives. The new methodology was demonstrated using poly(ethylene oxide) and poly(methylmethacrylate) (PMMA). Dyes were used as colouring agents for the polymers to verify core-sheath formation, and optical, scanning and fluorescent microscopy of the formed fibres confirmed the presence of a core-sheath combination. The core diameter obtained was in the range 5–10 μm and the sheath fibre diameter was 20–30 μm. The core/sheath diameter can be pre-set by selecting the forming conditions. To show the flexibility of the new method, nanoparticle containing PMMA fibres were also produced using the new device and incorporation of the nanoparticles in the sheath and core of the fibres was verified by electron microscopy and energy-dispersive X-ray spectroscopy analysis. A high yield of fibre was obtained and with more severe forming conditions the size of core-sheath fibres generated can be reduced to the nanoscale. Thus, the new process has a real capability of manufacturing a wide variety of novel functional materials and structures in a single scalable set-up. Keywords: Core-sheath, Polymer, Gyration, Pressure, Fibre, Device

This paper presents the development of the novel deposition of biodegradable polycaprolactone (PCL) polymer patterns on a metallic substrate using a jet spraying technique, template-assisted electrohydrodynamic atomization (TAEA), at ambient temperature. The structure of patterns was controlled by systematically varying the polymer concentration (2-15 wt.%) and the flow rate (1-25 μl min(-1)). Polymer deposition was carried out in the stable cone-jet mode to precisely control the surface structure and morphology. The patterns were studied by optical microscopy, scanning electron microscopy and profilometry, and a high degree of control over the pattern geometry and thickness was achieved by varying the spraying time. The hardness and the effective elastic modulus of the polymer patterns were estimated using nanoindentation. The effect of load, loading rate and the holding time on the hardness and effective elastic modulus was derived. Optimal results were obtained with 5 wt.% PCL in DMAC solution sprayed within the stable cone-jet mode operating window at a flow rate of 15 μl min(-1) for 300 s at 11.1 kV with a working distance of 60mm. Hexagonal patterns were well-defined and repeatable with thickness of ~34 μm. The hardness is 1.6 MPa at a loading rate of 0.1 μN/s and nearly halved when the load rate was increased to 1 μN/s. The effective elastic modulus of ~12 MPa is obtained for a load rate of 0.1 μN/s.

Ultrasound-responsive drug delivery systems have great potential for applications requiring stimulated release in vivo with a high degree of control over spatial and temporal location. In this study, systematic investigations were carried out to determine the effect of various ultrasound exposure parameters, in particular, output power, duty cycle and exposure time, on the release rate of a model drug (estradiol), encapsulated in poly DL-lactide-co-glycolide particles of different sizes prepared using electrohydrodynamic processing. The effect of ultrasound exposure on the degradation and surface morphology of the particles was also studied through optical and electron microscopy. There was found to be a positive correlation between drug release and each of the ultrasound parameters investigated, with output power having the most significant effect on both release rate and the morphology of the particles. The increase in surface porosity observed indicates that degradation may be attributed to cavitation phenomena.

Ultra fine short fibres have a variety of applications. Short aligned fibres or a mixture of short and long fibres can reinforce brittle materials, alter the appearance, texture and durability of synthetic fibres, and adjust the strength, toughness and stiffness of a composite material. Among electrospun products, short fibres are usually produced by secondary processing of continuous as-spun fibres. However, this is not entirely straightforward or cost-effective due to the efficiency of the secondary process and the relatively low tensile strength of the electrospun ultrafine fibres. Besides, sub-micrometre size fibres with an average aspect ratio (AR) 3000 under the same spinning conditions.

The preparation of capsules for medical and industrial use can be achieved via several conventional routes, yielding either hard or soft receptacles, depending on the type and the content of the material to be encapsulated. Together with tablets, capsules are amongst the most commonly used means of administering medication and this makes progress in capsule preparation technology a key area of drug delivery research. Here we uncover new technology for the preparation of capsules with porous chambers. The novelty is signified in the use of an electrohydrodynamic process engineering route and its potential is elucidated using a polymeric material; polymethylsilsesquioxane, which can be converted into an identical ceramic form by means of simple pyrolysis. Thus, both polymeric and ceramic capsules have been prepared. The effects of process control parameters such as the applied voltage and flow rate, on the characteristics of the capsules prepared are discussed.

The feasibility of producing a hollow microsphere with a single hole in its shell by coaxial electrohydrodynamic atomization (CEHDA) is demonstrated. Polymethylsilsesquioxane (PMSQ) was used as a model shell material encapsulating a core of a volatile liquid, perfluorohexane (PFH), which was subsequently evaporated to produce the hollow microspheres. The diameters of the microspheres and of the single surface pore were controlled by varying the flow rate of the components, the concentration of the PMSQ solution, and the applied voltage in the CEHDA process. The particles were characterized by scanning electron microscopy, and the ranges obtained were 275-860 nm for the microsphere diameter and 35-135 nm for the pore size. The process overcomes several of the key problems associated with existing methods of monoporous microsphere formation including removing the need for elevated temperatures, multiple processing steps, and the use of surfactants and other additives.

Drug-delivery systems with a unique capability to respond to a given stimulus can improve therapeutic efficacy. However, development of such systems is currently heavily reliant on responsive polymeric materials and pursuing this singular strategy limits the potential for clinical translation. In this report, with a model system used for drug-release studies, we demonstrate a new strategy: how a temperature-responsive non-toxic, volatile liquid can be encapsulated and stored under ambient conditions and subsequently programmed for controlled drug release without relying on a smart polymer. When the stimulus temperature is reached, controlled encapsulation of different amounts of dye in the capsules is achieved and facilitates subsequent sustained release. With different ratios of the liquid (perfluorohexane): dye in the capsules, enhanced controlled release with real-time response is provided. Hence, our findings offer great potential for drug-delivery applications and provide new generic insights into the development of stimuli drug-release systems.

A method for generating poly(lactic-co-glycolic acid) and polycaprolactone biodegradable particles of different size and shape using a jet generated in an electric field is elucidated. These particles are suitable for use as drug carriers and the method can be developed into a mass production route. The effect of different parameters such as applied voltage, collecting distance, flow rate and polymer concentration on inducing size and shape differences in these particles was studied. It was found that the flow rate, polymer concentration and collecting distance have a significant impact on the size of the generated particles and by changing the collecting distance a systematic reduction in the particle size by at least an order of magnitude (10microm-100nm) can be achieved. By using a high polymer concentration (30 wt. %) the shape and surface morphology of these particles can also be controlled from spherical to fibrous, and smooth to irregular, respectively, which presently is an interesting strategy and concept in drug delivery. This method is very useful as a one-step generator of different sizes of drug carriers with morphological variations.

Folates are a group of vitamins vital for the growth and development of the central nervous system. Most of these natural derivatives of folic acid are prone to oxidation and are very sensitive towards heat, temperature, oxygen, and light. Encapsulation of folic acid within inert matrices of a polymer can improve its stability and stop its degradation by light and oxygen. Electrohydrodynamic (EHD) technology is capable of generating fine droplets ranging from micrometers to nanometers in diameter from the breakup of a jet depending on the flow rate and applied electrical potential difference. The aims of this study were to generate nano-sized particles of folic acid encapsulated in sodium alginate (Na alginate) using EHD technology and to study the effect of voltage and flow rate on particle size as well as the structure of the prepared particles. It was established that 40 mg/ml (Na alginate) concentration can be used in single jet EHD technology. However, only 10 mg/ml concentration furnished stable jetting at any applied voltage and flow rate. So, this concentration was utilized and used to encapsulate higher dosages of folic acid. It was observed that the optimum flow rate for obtaining spherical particles of uniform diameter (4.2 ± 1.2 μm) was 10 μl/min at a voltage of 12 kV. Upon drying, these particles acquired a diameter in the range of 50-200 nm and became less spherical in shape. As the folic acid concentration is increased from 1 to 10 mg/ml, the percentage yield of particles at a constant Na alginate concentration increased by over 10 % and the corresponding encapsulation efficiency doubled. FTIR spectroscopic studies revealed the presence of folic acid within Na alginate matrices and also no characteristic chemical interaction between them. It can be concluded from the above research findings that, at 10 mg/ml Na alginate concentration, 10 μl/min flow rate, and 12 kV voltage, a high amount of folic acid (5 mg/ml) can be encapsulated within Na alginate matrices, with high percentage yield (70 %) and loading capacity (96 %), generating non-spherical dried beads/particles of 90-150 nm in diameter. © 2012 Springer Science+Business Media, LLC.

Porous polymeric near-spherical capsules, ~ 3.6 mm in diameter, were prepared using an electrodydrodynamic process. These capsules were pyrolysed to porous ceramics, ~ 3 mm in diameter. The ceramic capsules had interconnected pores of ~ 1.3 μm in size, and large cells with a mean size of 28 μm. The larger pores resemble the cells in a typical ceramic foam and were evenly distributed throughout the structure. A large proportion of the ceramic capsules contained 65-70% porosity, and their compressive strength was 0.2-0.4 MPa. © 2008 Elsevier B.V. All rights reserved.

In this study, the ability to control the shell thickness of hollow polymeric microspheres prepared using electrohydrodynamic processing at ambient temperature was investigated. Polymethylsilsesquioxane (PMSQ) was used as a model material for the microsphere shell encapsulating a core of liquid perfluorohexane (PFH). The microspheres were characterized by Fourier transform infrared spectroscopy and optical and electron microscopy, and the effects of the processing parameters (flow-rate ratio, polymer concentration and applied voltage) on the mean microsphere diameter ( D ) and shell thickness ( t ) were determined. It was found that the mean diameters of the hollow microspheres could be controlled in the range from 310 to 1000 nm while the corresponding mean shell thickness varied from 40 to 95 nm. The results indicate that the ratio D : t varied with polymer concentration, with the largest value of approximately 10 achieved with a solution containing 18 wt% of the polymer, while the smallest value (6.6) was obtained at 36 wt%. For polymer concentrations above 63 wt%, hollow microspheres could not be generated, but instead PMSQ fibres encapsulating PFH liquid were obtained.

Naturally derived biopolymers have been widely used for biomedical applications such as drug carriers, wound dressings, and tissue engineering scaffolds. Chitosan is a typical polysaccharide of great interest due to its biocompatibility and film-formability. Chitosan membranes with controllable porous structures also have significant potential in membrane chromatography. Thus, the processing of membranes with porous nanoscale structures is of great importance, but it is also challenging and this has limited the application of these membranes to date. In this study, with the aid of a carefully selected surfactant, polyethyleneglycol stearate-40, chitosan membranes with a well controlled nanoscale structure were successfully prepared. Additional control over the membrane structure was obtained by exposing the suspension to high intensity, low frequency ultrasound. It was found that the concentration of chitosan/surfactant ratio and the ultrasound exposure conditions affect the structural features of the membranes. The stability of nanopores in the membrane was improved by intensive ultrasonication. Furthermore, the stability of the blended suspensions and the intermolecular interactions between chitosan and the surfactant were investigated using scanning electron microscope and Fourier transform infrared spectroscopy (FTIR) analysis, respectively. Hydrogen bonds and possible reaction sites for molecular interactions in the two polymers were also confirmed by FTIR analysis. © 2010 World Scientific Publishing Company.

Electrospraying and electrospinning are amongst the common methods of forming polymeric micro- and nano-scaled structures using electrically driven polymer processing. Utilising a co-axial flow of materials has been successful in enabling encapsulated structures to be generated by these techniques. However, with both of these methods, including their respective co-axial forms, there is limited control over the deposition of the resultant structures. Recently, an electrically driven direct-writing method has been developed which is based upon the same fundamental principles, but with the ability to deposit and form structures in an ordered manner, which has previously been restricted largely to single needle flow processing. In this paper, using selected polymeric materials, we demonstrate two novel methods of this direct-write system. The first method shows how the shape of formed structures can be varied in-situ using a single needle flow direct-write process. Secondly, we demonstrate how co-axial flows can be utilised to write and form encapsulated structures. We envisage that while the use of electrospinning and electrospraying methods will continue to expand, these novel areas will offer much greater control over the forming of a plethora of micro- and nano-scaled structures and will be essential for topographic studies (e. g. of living cells), novel particle preparation methods, coatings and direct writing of polymeric biomaterials. © 2011 Springer-Verlag France.

A novel V-junction microfluidic (VJM) device has been used to generate several types of particles from the break-up of bubbles. The flow rates of selected solutions and the gas pressure were adjusted in order to successfully generate monodisperse polymer coated microbubbles, which serve as a platform for particle generation. Uniform particles in both the nano and micro size ranges with different shapes were spontaneously generated from bubbles and have the potential to be used in several advanced technological applications. © 2012 Elsevier B.V. All rights reserved.

Microparticles were fabricated for pharmaceutical purposes using electrospraying with the aim to determine the effect of the solvent(s) used. Particles of poly(lactic-co-glycolic acid) (PLGA) and the drug Celecoxib were prepared from acetone, acetonitrile and acetone:methanol with different polymer and drug concentrations. The solvent power, evaporation rate and electrical conductivity of the solvents all had a significant effect on the particle formation process as well as the particle characteristics and drug release profile. Particles were near-spherical and between 2 and 7 μm in diameter with smooth or corrugated surfaces. The drug release rate was mainly dependent on particle size, with larger particles showing slower release. The solvent in which PLGA was poorly soluble resulted in small grainy particles that disintegrated instantaneously with full drug release. It may be concluded that the selection of an appropriate solvent may be a useful way to control particle characteristics and drug release profiles when using electrospraying. © 2012 Elsevier Ltd. All rights reserved.

Encapsulation of materials in fibres with a well-controlled size distribution is an important application of the electrospinning technique. This study investigates the effect of key parameters of the coaxial electrospinning process including flow rate, applied voltage and polymer concentration on the efficient encapsulation and size distribution of perfluorohexane (PFH) in polymethylsilsesquioxane (PMSQ) microfibres. Perfluorohexane can be exchanged for a drug via a simple diffusion-controlled process. By altering the polymer concentration and processing parameters, PMSQ microfibres with different diameters, PFH core size and core-to-core distance were obtained. It was found that PFH-encapsulated fibres with a diameter between 8 and 15 μm can be prepared when the PMSQ concentration is kept between 55–70 wt%. The PFH regions (cores) encapsulated in the fibre are uniformly distributed and of size 5–14 μm. The core-to-core distance significantly increased from 4 μm to 22 μm when the applied voltage was increased from 8 kV to 11 kV. These results indicate a potential strategy for controlling fibre diameter, core size and core-to-core distance by using coaxial electrospinning as the forming procedure and thus this work will help to advance biomedical engineering applications, for example, drug delivery, scaffolding for tissue engineering and wound dressing.

Micro- and nanoparticle formulations are widely used to improve the bioavailability of low solubility drugs. In this study, electrospraying is introduced as a method for producing drug-loaded microspheres at ambient conditions. PLGA microspheres containing celecoxib, a low solubility drug, were prepared with the objective of producing near-monodisperse microspheres with the drug in a stable amorphous form. We found that it is possible to produce near-monodisperse celecoxib-loaded PLGA microspheres at different polymer:drug ratios. The microspheres produced were in the size range 1-5 μm depending on the polymer:drug ratio and had smooth surfaces. Thermal analysis further indicates that celecoxib is present in an amorphous form inside the microspheres. Drug dissolution studies showed an initial burst release followed by a period of sustained release with the dissolution curve depending on the polymer:drug ratio. Electrospraying is thus a promising method for producing amorphous microspheres of low solubility drugs such as celecoxib. The microsphere properties may be further optimized to achieve an appropriate dissolution profile with the aim of increasing oral bioavailability of low solubility drugs.

Submicrometre size spheres prepared from biocompatible polymers are becoming increasingly popular in drug and gene delivery. This paper describes the preparation of polymeric spheres with a mean diameter of 0.4 μm with a polydispersivity index of 8%, using coaxial electrohydrodynamic atomization (CEHDA) microbubbling. An 18 wt.% solution of polymethylsilsesquioxane, a hydrophobic biocompatible polymer, was subjected to CEHDA microbubbling by passing air through the inner needle and polymer solution through the outer needle of a twin needle co-axial device, under the influence of an electric field. A parametric plot of the flow rate of air and the flow rate of polymer solution was constructed and used for systematic process control to reduce the diameter of the microspheres from micrometre size to submicrometre size. CEHDA is an excellent method for obtaining polymer microspheres. By studying the process in detail and mapping it, we can now demonstrate it can also be used to prepare submicrometre sized particles with the ability to control size and polydispersivity.