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In this study, we report a simple one-pot synthesis of iron oxide nanoparticles (IONPs) modified with thermoresponsive polymers potentially applicable for nucleic acid capture. Ferrous (Fe2+) and ferric (Fe3+) ions were coprecipitated to a dispersion of previously prepared poly(N-isopropylacrylamide-co-2-aminoethyl methacrylate) P(NIPAAm-co-AEM) for in situ synthesis of magnetite (Fe3O4) and concurrent surface modification of Fe3O4 with the polymer to obtain magnetic nanocomposites. Fourier-transform infrared (FTIR) spectroscopy analysis reveals the surface modification of Fe3O4 with P(NIPAAm-co-AEM) and P(NIPAAm) as functional and control polymers, respectively. Fe3O4@P(NIPAAm-co-AEM) and Fe3O4@P(NIPAAm) nanocomposites’ surfaces contain 7.5 and 2.3 wt% of immobilized polymers, respectively. Vibrating sample magnetometry (VSM) result indicates a high saturation of magnetization value, 75 emu/g, for Fe3O4@P(NIPAAm-co-AEM) nanocomposites. The hydrodynamic diameter of Fe3O4@P(NIPAAm-co-AEM) in water changes depending on pH and temperature. A study for deoxyribonucleic acid (DNA) capture ability of Fe3O4@P(NIPAAm-co-AEM) nanocomposites shows a maximum 18.5 mg/g of DNA can be adsorbed on Fe3O4@P(NIPAAm-co-AEM).
In this paper, we use finite element analysis (FEA) to study the linear viscoelastic response of polyurea, a type of hard–soft block copolymer. A Niblack's algorithm-based technique employed on atomic force microscopy images provides geometry inputs for the FEA model, while the viscoelastic master curves of the soft matrix are obtained via a combination of dynamic mechanical analysis data and molecular dynamic (MD) estimations. In this microstructural image-based FEA framework, we introduce an interphase area of altered properties between the hard and soft domains. Both spatial and property distributions of this interphase area affect the viscoelastic response of the copolymer system. To quantitatively investigate the impact of structural and property features of the interphase on the energy storage and dissipation of a system during linear perturbation, we develop a statistical descriptor representation of the interphase region related to physical parameters. Utilizing decision-tree and random forest concepts from machine learning, we apply a ranking algorithm to identify the most significant features for four different mechanical response descriptors. Results show that the total interphase volume fraction and shifting factor distributions in the interphase area dominate the magnitude of the tan δ peak, whereas the magnitudes of the shifting factors primarily affect the tan δ peak location in frequency space. This method allows us to readily identify the dominant features impacting individual properties and paves the way for material design of hard–soft block copolymer systems.
We report on the synthesis, properties, and ion conductivity of a solid polymer electrolyte produced from polytetrahydrofuran (PTHF) photo-crosslinked with 3,4-epoxycyclohexylmethyl 3ʹ,4ʹ-epoxycyclohexane carboxylate (Epoxy), via an active monomer mechanism that facilitates the reaction of the native hydroxyl and epoxide end-groups. Crosslinked samples were loaded with different quantities of lithium tetrafluoroborate (LiBF4) and evaluated by electrochemical spectroscopy impedance (EIS) to determine their ionic conductivity. An increase in lithium salt loading led to an increase in ionic transport, reaching competitive conductivities of up to 10-3 S/cm at temperatures typical for battery operation. Thermal analysis confirms the amorphous structure and high thermal stability (30-90°). The mechanical analysis shows the materials possess suitable stiffness for applications. The results demonstrate a new synthetic route to tunable crosslinked networks for a broad range of chemical building blocks to achieve high lithium-ion conduction and attain desirable thermal and mechanical properties.
Vast improvements have been made to the capabilities of advanced manufacturing (AM), yet there are still limitations on which materials can effectively be used in the technology. To this end, parts created using AM would benefit from the ability to be developed from feedstock materials incorporating additional functionality. A common three-dimensional (3D) printing polymer, acrylonitrile butadiene styrene, was combined with bismuth and polyvinylidene fluoride via a solvent treatment to fabricate multifunctional composite materials for AM. Composites of varying weight percent loadings were extruded into filaments, which were subsequently 3D printed into blocks via fused filament fabrication. Investigating the material properties demonstrated that in addition to the printed blocks successfully performing as radiation shields, the chemical, thermal, and mechanical properties are suitable for AM. Thus, this work demonstrates that it is possible to enhance AM components with augmented capabilities while not significantly altering the material properties which make AM possible.
Hydrogels have gained recent attention for biomedical applications because of their large water content, which imparts biocompatibility. However, their mechanical properties can be limiting. There has been significant recent interest in the strength and fracture toughness of hydrogel materials in addition to their stiffness and time-dependent behavior. Hydrogels can fail in a brittle manner, although they are extremely compliant. In this work, the failure and fracture of hydrogels are examined using a compression test of spherical hydrogel particles. Spheres of commercially available polyacrylamide–potassium polyacrylate were hydrated and tested to failure in compression as a function of loading rate. The spheres exhibited little relaxation when compressed to small fixed displacements. The distributions of strength values obtained were examined in a particle fracture framework previously used for brittle ceramics. There was loading rate dependence apparent in the measured peak force and calculated peak strength values, but the data fell on a single empirical distribution function of strength for the hydrogels regardless of loading rate. Strength values for these hydrogels were mostly in the range of 0.05–0.3 MPa, illustrating the challenges using hydrogels for mechanically demanding applications such as tissue engineering.
A growing interest in dielectric waveguides (DWGs) as an alternative to commonly used waveguides (like coaxial or twisted-pair cables) for high data rate interconnects could be observed in the last few years. Especially in the mm-wave frequency range (30–300 GHz) applications with these waveguides benefit from low losses and low dispersion. Moreover, using both polarizations of the fundamental mode in such waveguides could theoretically double the data rate without the need of higher bandwidth or additional fibers. The connection between DWGs and commonly available transceiver chips requires broadband transitions from planar waveguides like microstrip lines to DWGs. In this paper, an overview of the current developments of such transitions is given and a novel low-complexity design is presented that reduces the space consumption by 35% related to recently published works. This allows an easy integration into a printed circuit board layout or a chip package. Furthermore, an extensive sensitivity analysis is presented to prove the robustness toward manufacturing tolerances. The transition is realized at W-band frequencies (75–110 GHz) and achieves a relative 10 dB-bandwidth of more than 25% with a minimum insertion loss of 1.2 dB. It is shown that these properties even hold for manufacturing tolerances of nowadays manufacturing processes.
In this work, filament based on ɛ-polycaprolactone (PCL) and containing the bioactive ceramics nanohydroxyapatite (nHap) and Laponite® (Lap) was prepared by the extrusion process. To obtain the material, a mass ratio of 89:10:1 (PCL:nHap:Lap) was used, and structural and morphological characterization was realized. In addition, cytotoxicity (using Allium cepa bulbs) and viability tests on L929 cells also were performed. The results showed that filament (diameter of 1.79 ± 0.17 mm) presented a good dispersion of nHap and Lap into polymeric matrices. Fourier transform infrared spectroscopy identified typical bands at 1720, 1091, and 1045 cm−1 addressed to PCL and nHAp, In addition, Lap was identified through dispersive energy system and X-ray diffraction analyses. All filaments did not exhibit cytotoxic effects.
Areas of overlap between intensification in liquid–liquid systems and membrane technology intensification are highlighted. Liquid membrane systems, supported liquid membranes, pertraction, and application to liquid–liquid coalescence are discussed. Fundamentals of emulsion formation are reviewed, including thermodynamic aspects and the importance of emulsion properties for application. The role of surfactants in emulsion stability is discussed. Characterization of emulsions and predictive methods for emulsion drop size are described. The immobilization of solvents onto hollow fiber membranes is described and the advantages of low solvent inventory and ease of phase separation are highlighted. The basic principle of application of a liquid membrane system is described, showing the generic process steps: emulsification, contact with the feed phase, emulsion breakage, and product recovery. The role of facilitated transport is also described. Different configurations are compared, including hybrid liquid membranes, polymer inclusion membranes, and colloidal liquid aphrons. Selected examples of application of liquid membrane systems are described.
Achieving control over the morphology of conjugated polymer (CP) blends at nanoscale is crucial for enhancing their performances in diverse organic optoelectronic devices, including thin film transistors, photovoltaics, and light emitting diodes. However, the complex CP chemical structures and intramolecular interactions often make such control difficult to implement. We demonstrate here that cooperative combination of non-covalent interactions, including hydrogen bonding, coordination interactions, and π-π interactions, etc., can be used to effectively define the morphology of CP blend films, in particular being able to achieve accurate spatial arrangement of nanoparticles within CP nanostructures. Through UV-vis absorption spectroscopy and transmission electron microscopy, we show strong attachment of fullerene molecules, CdSe quantum dots, and iron oxide nanoparticles, onto well-defined CP nanofibers. The resulting core/shell hybrid nanofibers exhibit well-defined donor/acceptor interface when employed in photovoltaic devices, which also contributes to enhanced charge separation and transport. These findings provide a facile new methodology of improving CP/nanoparticle interfacial properties and controlling blend morphology. The generality of this methodology demonstrated in current studies points to a new way of designing hybrid materials based on organic polymers and inorganic nanoparticles towards applications in modern electronic devices.
The quality of the polymer raw material used in plastic processing methods is an important characteristic because it is one of the main factors in producing quality products. Therefore, the characterization of polymeric pellets in the polymer processing industry is very important to avoid using inferior materials. In general, differences in the interiors of polymeric pellets reflect differences in their densities. In this study, a high-sensitivity magnetic levitation method was used to characterize the polymeric pellets in four different occasions. The device used has a high sensitivity that can distinguish minute differences as small as of 0.0041 g/cm3 in density between different samples. In addition, the method can obtain a sample's density without knowing the weight and volume of the sample. This method can be used to characterize materials by testing only a single pellet, which is very useful for polymeric pellet characterization.
Bioactive dressings which can treat any kind of chronic or acute wounds and can fully replace the conventional gauzes and superabsorbent dressings have proven to be a future market of wound care products in recent times. These dressings are multifunctional, which can effectively combat the wound infection, remove the exudate, promote angiogenesis, and protect the wound from external trauma. Proper selection of bioactive and polymer defines its efficiency. Current research unveils the therapeutic efficacy of curcumin–honey-loaded multilayered polyvinyl alcohol/cellulose acetate electrospun nanofibrous mats as an interactive bioactive wound dressing material. Scanning electron microscopy and Fourier transform infrared spectroscopy analysis infers uniform encapsulation and chemical compatibility of herbal actives and polymer, inside the nanofibrous layers. The as-spun mat shows potential resistance towards Escherichia coli and ∼90% antioxidant activity against diphenyl-picrylhydrazyl (DPPH)–free radical. Additionally, water absorbency, water vapor transmission rate, and wettability analysis show quick and excellent absorption with controlled transmission of wound exudate.
Ab initio design of polymer nanocomposite materials for high breakdown strength requires prediction of localized trap states at the polymer–filler interface. Systematic first-principles calculations of realistic interfaces can be challenging, particularly for amorphous polymers and fillers that necessitate the calculation of ensembles of large unit cells with hundreds of atoms. We present a computational approach for automatically generating reasonable structures for amorphous polymer–filler interfaces, combining classical molecular dynamics and Monte Carlo simulations. We identify trap states by analyzing the localization of electronic eigenstates calculated using density functional theory on ensembles of interface structures, clearly distinguishing shallow trap states from delocalized band-edge states. Applying this approach to silica–polyethylene interfaces as an initial example, we find under-coordination and distorted coordination structures at amorphous silica surfaces contribute a combination of deep and shallow traps at these interfaces, whereas polyethylene does not generate localized interfacial states.
The tensile yield strength of high-density polyethylene using instrumented indentation tests with a flat-ended cylindrical indenter was evaluated. The variation in the field expressed by stress and strain beneath the flat-ended cylindrical indenter is investigated using a new expanding cavity model to study the relation between tension and indentation. This model starts from the separation of forces into the compressive force on the material and the frictional one, which is generated during indentation on the sides of indenter. The authors propose a method to correct the frictional force based on the saturation of indentation hardening and obtain load–depth curve with compressive component only. For conversion of indentation force and displacement, our new representation model is applied. By modifying Johnson's model, the new assumption of conservation of indentation plastic volume is suggested. This model proves and supports conventional relations of the strain rates between indentation and tension theoretically. These are verified through the experiments: instrumented indentation and uniaxial tensile test. The authors find a good agreement between the tensile yield strengths at various strain rates.
Nanocomposites of polyvinylidene fluoride loaded with various amounts of γ-Fe2O nanoparticles, with an average size ranging between 20 and 40 nm, have been obtained by melt mixing and investigated using various experimental techniques [Superconducting Quantum Interference Device, Mössbauer, and Thermogravimetric Analysis]. Magnetic and Mössbauer measurements confirmed the presence of maghemite and a trace of a paramagnetic iron compound. Magnetic data are consistent with a blocking temperature close to room temperature (RT), showing a decrease in the coercive field as the temperature is increased. A weak exchange bias was noticed in all nanocomposites investigated at all temperatures and tentatively ascribed to surface spin disorder. The temperature dependence of the coercive field obeys the Kneller law. The nanocomposites exhibit superparamagnetic behavior near RT. Most magnetic measurements have been performed below the blocking temperature, revealing thus a complex behavior. The dependence of the mass loss derivative versus temperature, as obtained by thermogravimetric analysis, exhibits a single peak due to the thermal degradation of the polymeric matrix. A weak increase in the thermal stability of the polymeric matrix upon loading with maghemite is reported.
Polymer nanocomposites possess unique sets of properties that make them suitable for different applications, including structural and flame-retardant material, electromagnetic wave reflector, sensors, thin film transistor, flexible display, and many more. The properties of these nanocomposite are dependent on nanofiller dispersion and bonding with polymer matrix (i.e. particle-matrix interaction). Thermography is a non-destructive method that may be used to gain insight into dispersion and particle-matrix interaction. Infrared (IR) radiation emitted from these nanomaterial polymer composite depends on the emissivity of the individual components. In addition, during flash heating and cooling, different thermal conductivity of components in the nanocomposite can influence pixel intensity differently in the IR image or video being captured. We have used an economical mid wavelength IR camera Fluke RSE600 equipped with a close-up macro lens and algorithm based on MATLAB image processing toolbox to analyse dispersion, voids and thermal diffusivity of patented graphene polymer nanocomposite materials (G-PMC) in micro-scale. These G-PMCs can act as a standard material to determine the potential of our IR thermography technique due to their homogeneity and lack of impurity due to unique fabrication process. Thermal diffusivity and dispersion of nanoparticles in our G-PMCs was estimated after irradiation with a xenon flash lamp by spatially mapping transient IR radiations from different G-PMCs using the Fluke RSE600 thermal imager. Results from thermography experiments were compared with scanning electron microscope (SEM) and Raman spectroscopy results. Micro-scale thermography was able to detect millimetre scale thermal diffusivity variation in the injection molded G-PMC samples and relate it to change in dispersion of nanofillers, unlike SEM and Raman, where micro-scale measurements could not determine the reason behind millimetre scale property variation. We believe this low cost, fast, micro-scale, non-destructive technique will provide valuable insight into functional polymer nanocomposite fabrication and corresponding electrical and thermal properties.
Fused deposition modelling (FDM) type of 3D printing is widely used for manufacturing complex shaped polymer products. Recently, the metal/polymer composite products can be made by 3D printer using metal/polymer composite filament. Now, we are planning to develop a new manufacturing process of the thermoelectric (TE) elements or modules by combining the FDM-type 3D printing and the degreasing-sintering process. In this work, we focused on the degreasing-sintering process of the mixture of Mg2Si and polylactic acid (PLA) powders. Mg2Si compound powder was synthesized by a liquid-solid phase reaction (LSPR) method. The powder mixtures of Mg2Si, Al and PLA were pressed and heated in a pulse discharge sintering (PDS) chamber under a vacuum in various degreasing conditions. Following the degreasing, the sintering of Mg2Si was carried out in the same PDS chamber at various starting sintering temperatures. Sintered density, Seebeck coefficient and electrical resistivity of the consolidated Mg2Si were measured and the power factor as a TE performance was estimated from the TE properties. The optimum conditions of degreasing-sintering process maximizing the sintered density and the TE performance of Al-doped Mg2Si were investigated. Furthermore, the influences of the additive amount of Al on the sintered density and the TE performance of Mg2Si fabricated via the optimized degreasing-sintering process were investigated.
Nature is ripe with biological organisms that can interact with its surroundings to continuously morph their surface texture. Many attempts have been made to optimize artificial surfaces depending on operational needs; however, most of these architected materials only focus on enhancing a specific material property or functionality. This study introduces a new class of instability-induced morphable structures, herein referred to as “Active Skins”, which enables on-demand, reversible, surface morphing through buckling-induced feature deployment. By taking advantage of a preconceived auxetic unit cell geometrical design, mechanical instabilities were introduced to facilitate rapid out-of-plane deformations when in-plane strains are applied. Here, these notches were introduced at judiciously chosen locations in an array of unit cells to elicit unique patterns of out-of-plane deformations to pave way for controlling bulk Active Skin behavior. These purposefully designed imperfections were employed for selectively actuating them for applications ranging from camouflage to surface morphing to soft robotic grippers.
Controlled degradation of hydrogels enables several applications of these materials, including controlled drug and cell release applications and directed growth of neural networks. These applications motivate the need of a simulation framework for modeling controlled degradation in hydrogels. We develop a Dissipative Particle Dynamics (DPD) framework for hydrogel degradation. As a model hydrogel, we prepare a network formed by end-linking tetra-arm polyethylene glycol precursors. We model bond breaking during degradation of this hydrogel as a stochastic process. The fraction of degradable bonds follows first order degradation kinetics. We characterize the rate of mass loss during degradation process.
Selective laser sintering methods are workhorses for additively manufacturing polymer-based components. The ease of rapid prototyping also means it is easy to produce illicit components. It is necessary to have a data-calibrated in-situ physical model of the build process in order to predict expected and defective microstructure characteristics that inform component provenance. Toward this end, sintering models are calibrated and characteristics such as component defects are explored. This is accomplished by assimilating multiple data streams, imaging analysis, and computational model predictions in an adaptive Bayesian parameter estimation algorithm. From these data sources, along with a phase-field model, bulk porosity distributions are inferred. Model parameters are constrained to physically-relevant search directions by sensitivity analysis, and then matched to predictions using adaptive sampling. Using this feedback loop, data-constrained estimates of sintering model parameters along with uncertainty bounds are obtained.
We continue to investigate the design, synthesis, and characterization of electrically and ionically active conjugated polythiophene copolymers for integrating a variety of biomedical devices with living tissue. This paper will describe some of our most recent results, including the development of several new monomers that can tailor the surface chemistry, adhesion, and biointegration of these materials with neural cells. Our efforts have focused on copolymers of 3,4 ethylenedioxythiophene (EDOT), functionalized variants of EDOT (including EDOT-acid and the trifunctional EPh), and dopamine (DOPA). The resulting PEDOT-based copolymers have electrical, optical, mechanical, and adhesive properties that can be precisely tailored by fine tuning the chemical composition and structure. Here we present results on EDOT-dopamine bifunctional monomers and their corresponding polymers. We discuss the design and synthesis of an EDOT-cholesterol that combines the thiophene with a biological moiety known to exhibit surface-active behaviour. We will also introduce EDOT-aldehyde and EDOT-maleimide monomers and show how they can be used as the starting point for a wide variety of functionalized monomers and polymers.