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Version: publishedVersion × Subject: Polymers ×

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    Segregated Network Polymer Composites with High Electrical Conductivity and Well Mechanical Properties based on PVC, P(VDFTFE), UHMWPE, and rGO
    (Washington, DC : ACS Publications, 2020) Shiyanova, Kseniya A.; Gudkov, Maksim V.; Gorenberg, Arkady Ya; Rabchinskii, Maxim K.; Smirnov, Dmitry A.; Shapetina, Maria A.; Gurinovich, Tatiana D.; Goncharuk, Galina P.; Kirilenko, Demid A.; Bazhenov, Sergey L.; Melnikov, Valery P.
    The formation of a segregated network structure (wittingly uneven distribution of a filler) is one of the most promising strategies for the fabrication of electrically conductive polymer composites at present. However, the simultaneous achievement of high values of electrical conductivity with the retention of well mechanical properties within this approach remains a great challenge. Here, by means of X-ray photoelectron spectra (XPS), near-edge X-ray absorption fine structure (NEXAFS) spectra, scanning electron microscopy (SEM), dielectric spectroscopy, and compression engineering stress-strain curve analysis, we have studied the effect of a segregated network structure on the electrical conductivity and mechanical properties of a set of polymer composites. The composites were prepared by applying graphene oxide (GO) with ultralarge basal plane size (up to 150 μm) onto the surface of polymer powder particles, namely, poly(vinyl chloride) (PVC), poly(vinylidene fluoride-co-tetrafluoroethylene) (P(VDF-TFE)), and ultrahigh-molecular-weight poly(ethylene) (UHMWPE) with the subsequent GO reduction and composite hot pressing. A strong dependence of the segregated network polymer composites' physical properties on the polymer matrix was demonstrated. Particularly, 12 orders of magnitude rise of the polymers' electrical conductivity up to 0.7 S/m was found upon the incorporation of the reduced GO (rGO). A 17% increase in the P(VDF-TFE) elastic modulus filled by 1 wt % of rGO was observed. Fracture strength of PVC/rGO at 0.5 wt % content of the filler was demonstrated to decrease by fourfold. At the same time, the change in strength was not significant for P(VDF-TFE) and UHMWPE composites in comparison with pure polymers. Our results show a promise to accelerate the development of new composites for energy applications, such as metal-free supercapacitor plates and current collectors of lithium-ion batteries, bipolar plates of proton-exchange membrane fuel cells, antistatic elements of various electronic devices, etc. © 2020 American Chemical Society.
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    Secondary Structure and Glycosylation of Mucus Glycoproteins by Raman Spectroscopies
    (Columbus, Ohio : American Chemical Society, 2016) Davies, Heather S.; Singh, Prabha; Deckert-Gaudig, Tanja; Deckert, Volker; Rousseau, Karine; Ridley, Caroline E.; Dowd, Sarah E.; Doig, Andrew J.; Pudney, Paul D. A.; Thornton, David J.; Blanch, Ewan W.
    The major structural components of protective mucus hydrogels on mucosal surfaces are the secreted polymeric gel-forming mucins. The very high molecular weight and extensive O-glycosylation of gel-forming mucins, which are key to their viscoelastic properties, create problems when studying mucins using conventional biochemical/structural techniques. Thus, key structural information, such as the secondary structure of the various mucin subdomains, and glycosylation patterns along individual molecules, remains to be elucidated. Here, we utilized Raman spectroscopy, Raman optical activity (ROA), circular dichroism (CD), and tip-enhanced Raman spectroscopy (TERS) to study the structure of the secreted polymeric gel-forming mucin MUC5B. ROA indicated that the protein backbone of MUC5B is dominated by unordered conformation, which was found to originate from the heavily glycosylated central mucin domain by isolation of MUC5B O-glycan-rich regions. In sharp contrast, recombinant proteins of the N-terminal region of MUC5B (D1-D2-D′-D3 domains, NT5B), C-terminal region of MUC5B (D4-B-C-CK domains, CT5B) and the Cys-domain (within the central mucin domain of MUC5B) were found to be dominated by the β-sheet. Using these findings, we employed TERS, which combines the chemical specificity of Raman spectroscopy with the spatial resolution of atomic force microscopy to study the secondary structure along 90 nm of an individual MUC5B molecule. Interestingly, the molecule was found to contain a large amount of α-helix/unordered structures and many signatures of glycosylation, pointing to a highly O-glycosylated region on the mucin.
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    Bioinspired Polydopamine Coating as an Adhesion Enhancer Between Paraffin Microcapsules and an Epoxy Matrix
    (Washington, DC : ACS Publications, 2020) Fredi, Giulia; Simon, Frank; Sychev, Dmitrii; Melnyk, Inga; Janke, Andreas; Scheffler, Christina; Zimmerer, Cordelia
    Microencapsulated phase change materials (PCMs) are attracting increasing attention as functional fillers in polymer matrices, to produce smart thermoregulating composites for applications in thermal energy storage (TES) and thermal management. In a polymer composite, the filler–matrix interfacial adhesion plays a fundamental role in the thermomechanical properties. Hence, this work aims to modify the surface of commercial PCM microcapsules through the formation of a layer of polydopamine (PDA), a bioinspired polymer that is emerging as a powerful tool to functionalize chemically inert surfaces due to its versatility and great adhesive potential in many different materials. Scanning electron microscopy (SEM) and atomic force microscopy (AFM) evidenced that after PDA coating, the surface roughness increased from 9 to 86 nm, which is beneficial, as it allows a further increase in the interfacial interaction by mechanical interlocking. Spectroscopic techniques allowed investigating the surface chemistry and identifying reactive functional groups of the PDA layer and highlighted that, unlike the uncoated microcapsules, the PDA layer is able to react with oxirane groups, thereby forming a covalent bond with the epoxy matrix. Hot-stage optical microscopy and differential scanning calorimetry (DSC) highlighted that the PDA modification does not hinder the melting/crystallization process of the paraffinic core. Finally, SEM micrographs of the cryofracture surface of epoxy composites containing neat or PDA-modified microcapsules clearly evidenced improved adhesion between the capsule shell and the epoxy matrix. These results showed that PDA is a suitable coating material with considerable potential for increasing the interfacial adhesion between an epoxy matrix and polymer microcapsules with low surface reactivity. This is remarkably important not only for this specific application but also for other classes of composite materials. Future studies will investigate how the deposition parameters affect the morphology, roughness, and thickness of the PDA layer and how the layer properties influence the capsule–matrix adhesion.
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    Surface, interphase and tensile properties of unsized, sized and heat treated basalt fibres
    (London [u.a.] : Institute of Physics, 2016) Förster, T.; Sommer, G.S.; Mäder, E.; Scheffler, C.
    Recycling of fibre reinforced polymers is in the focus of several investigations. Chemical and thermal treatments of composites are the common ways to separate the reinforcing fibres from the polymer matrices. However, most sizings on glass and basalt fibre are not designed to resist high temperatures. Hence, a heat treatment might also lead to a sizing removal, a decrease of mechanical performance and deterioration in fibre-matrix adhesion. Different basalt fibres were investigated using surface analysis methods as well as single fibre tensile tests and single fibre pull-out tests in order to reveal the possible causes of these issues. Heat treatment in air reduced the fibre tensile strength in the same level like heat treatment in nitrogen atmosphere, but it influenced the wetting capability. Re-sizing by a coupling agent slightly increased the adhesion strength and reflected a decreased post-debonding friction.
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    Local delivery to malignant brain tumors: potential biomaterial-based therapeutic/adjuvant strategies
    (Cambridge : RSC, 2021) Alghamdi, Majed; Gumbleton, Mark; Newland, Ben
    Glioblastoma (GBM) is the most aggressive malignant brain tumor and is associated with a very poor prognosis. The standard treatment for newly diagnosed patients involves total tumor surgical resection (if possible), plus irradiation and adjuvant chemotherapy. Despite treatment, the prognosis is still poor, and the tumor often recurs within two centimeters of the original tumor. A promising approach to improving the efficacy of GBM therapeutics is to utilize biomaterials to deliver them locally at the tumor site. Local delivery to GBM offers several advantages over systemic administration, such as bypassing the blood-brain barrier and increasing the bioavailability of the therapeutic at the tumor site without causing systemic toxicity. Local delivery may also combat tumor recurrence by maintaining sufficient drug concentrations at and surrounding the original tumor area. Herein, we critically appraised the literature on local delivery systems based within the following categories: polymer-based implantable devices, polymeric injectable systems, and hydrogel drug delivery systems. We also discussed the negative effect of hypoxia on treatment strategies and how one might utilize local implantation of oxygen-generating biomaterials as an adjuvant to enhance current therapeutic strategies. © 2021 The Royal Society of Chemistry.
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    High temperature reactive ion etching of iridium thin films with aluminum mask in CF4/O2/Ar plasma
    (New York : American Institute of Physics, 2016) Yeh, Chia-Pin; Lisker, Marco; Kalkofen, Bodo; Burte, Edmund P.
    Reactive ion etching (RIE) technology for iridium with CF4/O2/Ar gas mixtures and aluminum mask at high temperatures up to 350 °C was developed. The influence of various process parameters such as gas mixing ratio and substrate temperature on the etch rate was studied in order to find optimal process conditions. The surface of the samples after etching was found to be clean under SEM inspection. It was also shown that the etch rate of iridium could be enhanced at higher process temperature and, at the same time, very high etching selectivity between aluminum etching mask and iridium could be achieved.
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    Mechanochemical activation of disulfide-based multifunctional polymers for theranostic drug release
    (Cambridge : RSC, 2021) Shi, Zhiyuan; Song, Qingchuan; Göstl, Robert; Herrmann, Andreas
    Drug delivery systems responsive to physicochemical stimuli allow spatiotemporal control over drug activity to overcome limitations of systemic drug administration. Alongside, the non-invasive real-time tracking of drug release and uptake remains challenging as pharmacophore and reporter function are rarely unified within one molecule. Here, we present an ultrasound-responsive release system based on the mechanochemically induced 5-exo-trigcyclization upon scission of disulfides bearing cargo molecules attachedviaβ-carbonate linker within the center of a water soluble polymer. In this bifunctional theranostic approach, we release one reporter molecule per drug molecule to quantitatively track drug release and distribution within the cell in real-time. We useN-butyl-4-hydroxy-1,8-naphthalimide and umbelliferone as fluorescent reporter molecules to accompany the release of camptothecin and gemcitabine as clinically employed anticancer agents. The generality of this approach paves the way for the theranostic release of a variety of probes and drugs by ultrasound. © The Royal Society of Chemistry 2020.
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    Correction: Mechanochemical activation of disulfide-based multifunctional polymers for theranostic drug release
    (Cambridge : RSC, 2021) Shi, Zhiyuan; Song, Qingchuan; Göstl, Robert; Herrmann, Andreas
    Correction for ‘Mechanochemical activation of disulfide-based multifunctional polymers for theranostic drug release’ by Zhiyuan Shi et al., Chem. Sci., 2021, 12, 1668–1674, DOI: 10.1039/D0SC06054B.
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    Charged polymers transport under applied electric fields in periodic channels
    (Basel : MDPI AG, 2013) Nedelcu, S.; Sommer, J.-U.
    By molecular dynamics simulations, we investigated the transport of charged polymers in applied electric fields in confining environments, which were straight cylinders of uniform or non-uniform diameter. In the simulations, the solvent was modeled explicitly and, also, the counterions and coions of added salt. The electrophoretic velocities of charged chains in relation to electrolyte friction, hydrodynamic effects due to the solvent, and surface friction were calculated. We found that the velocities were higher if counterions were moved away from the polymeric domain, which led to a decrease in hydrodynamic friction. The topology of the surface played a key role in retarding the motion of the polyelectrolyte and, even more so, in the presence of transverse electric fields. The present study showed that a possible way of improving separation resolution is by controlling the motion of counterions or electrolyte friction effects.
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    Liquid sensing: Smart polymer/CNT composites
    (Amsterdam [u.a.] : Elsevier, 2011) Villmow, T.; Pegel, S.; John, A.; Rentenberger, R.; Pötschke, P.
    Today polymer/carbon nanotube (CNT) composites can be found in sports equipment, cars, and electronic devices. The growth of old and new markets in this area has been stimulated by our increased understanding of relevant production and processing methods, as well as the considerable price reduction of industrial CNT grades. In particular, CNT based electrically conductive polymer composites (CPCs) offer a range of opportunities because of their unique property profile; they demonstrate low specific gravity in combination with relatively good mechanical properties and processability. The electrical conductivity of polymer/CNT composites results from a continuous filler network that can be affected by various external stimuli, such as temperature shifts, mechanical deformations, and the presence of gases and vapors or solvents. Accordingly, CNT based CPCs represent promising candidates for the design of smart components capable of integrated monitoring. In this article we focus on their use as leakage detectors for organic solvents.