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- ItemCytocompatible, Injectable, and Electroconductive Soft Adhesives with Hybrid Covalent/Noncovalent Dynamic Network(Weinheim : Wiley-VCH, 2019) Xu, Yong; Patsis, Panagiotis A.; Hauser, Sandra; Voigt, Dagmar; Rothe, Rebecca; Günther, Markus; Cui, Meiying; Yang, Xuegeng; Wieduwild, Robert; Eckert, Kerstin; Neinhuis, Christoph; Akbar, Teuku Fawzul; Minev, Ivan R.; Pietzsch, Jens; Zhang, YixinSynthetic conductive biopolymers have gained increasing interest in tissue engineering, as they can provide a chemically defined electroconductive and biomimetic microenvironment for cells. In addition to low cytotoxicity and high biocompatibility, injectability and adhesiveness are important for many biomedical applications but have proven to be very challenging. Recent results show that fascinating material properties can be realized with a bioinspired hybrid network, especially through the synergy between irreversible covalent crosslinking and reversible noncovalent self-assembly. Herein, a polysaccharide-based conductive hydrogel crosslinked through noncovalent and reversible covalent reactions is reported. The hybrid material exhibits rheological properties associated with dynamic networks such as self-healing and stress relaxation. Moreover, through fine-tuning the network dynamics by varying covalent/noncovalent crosslinking content and incorporating electroconductive polymers, the resulting materials exhibit electroconductivity and reliable adhesive strength, at a similar range to that of clinically used fibrin glue. The conductive soft adhesives exhibit high cytocompatibility in 2D/3D cell cultures and can promote myogenic differentiation of myoblast cells. The heparin-containing electroconductive adhesive shows high biocompatibility in immunocompetent mice, both for topical application and as injectable materials. The materials could have utilities in many biomedical applications, especially in the area of cardiovascular diseases and wound dressing.
- ItemToward Functional Synthetic Cells: In-Depth Study of Nanoparticle and Enzyme Diffusion through a Cross-Linked Polymersome Membrane(Weinheim : Wiley-VCH, 2019) Gumz, Hannes; Boye, Susanne; Iyisan, Banu; Krönert, Vera; Formanek, Petr; Voit, Brigitte; Lederer, Albena; Appelhans, DietmarUnderstanding the diffusion of nanoparticles through permeable membranes in cell mimics paves the way for the construction of more sophisticated synthetic protocells with control over the exchange of nanoparticles or biomacromolecules between different compartments. Nanoparticles postloading by swollen pH switchable polymersomes is investigated and nanoparticles locations at or within polymersome membrane and polymersome lumen are precisely determined. Validation of transmembrane diffusion properties is performed based on nanoparticles of different origin—gold, glycopolymer protein mimics, and the enzymes myoglobin and esterase—with dimensions between 5 and 15 nm. This process is compared with the in situ loading of nanoparticles during polymersome formation and analyzed by advanced multiple-detector asymmetrical flow field-flow fractionation (AF4). These experiments are supported by complementary i) release studies of protein mimics from polymersomes, ii) stability and cyclic pH switches test for in polymersome encapsulated myoglobin, and iii) cryogenic transmission electron microscopy studies on nanoparticles loaded polymersomes. Different locations (e.g., membrane and/or lumen) are identified for the uptake of each protein. The protein locations are extracted from the increasing scaling parameters and the decreasing apparent density of enzyme-containing polymersomes as determined by AF4. Postloading demonstrates to be a valuable tool for the implementation of cell-like functions in polymersomes.
- ItemOrganic vapor sensing behavior of polycarbonate/polystyrene/multi-walled carbon nanotube blend composites with different microstructures(Amsterdam [u.a.] : Elsevier Science, 2019) Li, Yilong; Pionteck, Jürgen; Pötschke, Petra; Voit, BrigitteWith the focus on the use as leakage detectors, the vapor sensing behavior of conductive polymer composites (CPCs) based on polycarbonate/polystyrene/multi-walled carbon nanotube (PC/PS/MWCNT) blends with different blend ratios was studied as well as their morphological and electrical properties. In the melt mixed blend composites, the MWCNTs are preferentially localized in PC. At the PC/PS ratio of 70/30 wt%, the composites showed a sea-island structure, while for blends containing 40 wt% or 50 wt% PS co-continuous structures were developed resulting in a reduction in the MWCNT percolation threshold. The saturated vapors of the selected solvents have good interactions to PS but different interactions to PC. At 0.75 wt% MWCNT, sea-island CPCs showed high relative resistance change (Rrel) but poor reversibility towards moderate vapors like ethyl acetate and toluene, while CPCs with co-continuous structure exhibited lower Rrel and better reversibility. All CPCs showed poor reversibility towards vapor of the good solvent dichloromethane due to strong interactions between polymers and vapor. In the vapor of the poor solvent cyclohexane, CPCs with higher PS content showed increased Rrel. After extraction of the PS component by cyclohexane, the sensing response was decreased and the Rrel of the co-continuous blend even reached negative values.
- ItemA new way of toughening of thermoset by dual-cured thermoplastic/thermosetting blend(Basel : MDPI, 2019) Khatiwada, Shankar P.; Gohs, Uwe; Lach, Ralf; Heinrich, Gert; Adhikari, RameshwarThe work aims at establishing the optimum conditions for dual thermal and electron beam curing of thermosetting systems modified by styrene/butadiene (SB)-based triblock copolymers in order to develop transparent and toughened materials. The work also investigates the effects of curing procedures on the ultimate phase morphology and mechanical properties of these thermoset-SB copolymer blends. It was found that at least 46 mol% of the epoxidation degree of the SB copolymer was needed to enable the miscibility of the modified block copolymer into the epoxy resin. Hence, an electron beam curing dose of ~50 kGy was needed to ensure the formation of micro- and nanostructured transparent blends. The micro- and nanophase-separated thermosets obtained were analyzed by optical as well as scanning and transmission electron microscopy. The mechanical properties of the blends were enhanced as shown by their impact strengths, indentation, hardness, and fracture toughness analyses, whereby the toughness values were found to mainly depend on the dose. Thus, we have developed a new route for designing dual-cured toughened micro- and nanostructured transparent epoxy thermosets with enhanced fracture toughness. © 2019 by the authors.
- ItemSurface Treatment of Carbon Fibers by Oxy-Fluorination(Basel : MDPI, 2019) Kruppke, Iris; Scheffler, Christina; Simon, Frank; Hund, Rolf-Dieter; Cherif, ChokriIn this paper, the oxy-fluorination process and the influence of different concentrations of fluorine and oxygen in the gas phase on the physicochemical properties of polyacrylonitrile(PAN)-based carbon fibers are described. The properties of the treated carbon structures are determined by zeta potential and tensiometry measurements. In addition, changes in surface composition and morphology are investigated by X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM). Adhesion properties are characterized by the single fiber pull-out (SFPO) test. Furthermore, changes in intrinsic properties are described by means of tensile and density measurements. After a primary desizing effect by oxy-fluorination, an increased number of oxygen-containing surface functional groups could be detected, which led to more debonding work in SFPOs with an epoxy-based matrix. It was also shown that the polar surface energy grows with rising fluorine concentration in the reaction gas mixture. In addition, a minor increase of ~10% in the maximum strength of PAN-based carbon fibers is detected by single fiber tensile measurements after oxy-fluorination with a fluorine content of 5% in the reaction mixture.
- ItemSERS and plasmonic heating efficiency from anisotropic core/satellite superstructures(Cambridge : RSC Publ., 2019) Kuttner, Christian; Höller, Roland P. M.; Quintanilla, Marta; Schnepf, Max J.; Dulle, Martin; Fery, Andreas; Liz-Marzán, Luis M.The optical properties of nanoparticle assemblies can be tailored via hybridization of plasmon modes. Isotropic core/satellite superstructures made of spherical nanoparticles are known to exhibit coupled modes with a strongly scattering (radiative) character, and provide hot spots yielding high activity in surface-enhanced Raman scattering (SERS). However, to complement this functionality with plasmonic heating, additional absorbing (non-radiative) modes are required. We introduce herein anisotropic superstructures formed by decorating a central nanorod with spherical satellite nanoparticles, which feature two coupled modes that allow application for both SERS and heating. On the basis of diffuse reflectance spectroscopy, small-angle X-ray scattering (SAXS), and electromagnetic simulations, the origin of the coupled modes is disclosed and thus serves as a basis toward alternative designs of functional superstructures. This work represents a proof-of-principle for the combination of high SERS efficiency with efficient plasmonic heating by near-infrared irradiation.
- ItemPEGylation-Dependent Metabolic Rewiring of Macrophages with Silk Fibroin Nanoparticles(Washington, DC : ACS Publications, 2019) Totten, John D.; Wongpinyochit, Thidarat; Carrola, Joana; Duarte, Iola F.; Seib, F. PhilippSilk fibroin nanoparticles are emerging as promising nanomedicines, but their full therapeutic potential is yet to be realized. These nanoparticles can be readily PEGylated to improve colloidal stability and to tune degradation and drug release profiles; however, the relationship between silk fibroin nanoparticle PEGylation and macrophage activation still requires elucidation. Here, we used in vitro assays and nuclear magnetic resonance based metabolomics to examine the inflammatory phenotype and metabolic profiles of macrophages following their exposure to unmodified or PEGylated silk fibroin nanoparticles. The macrophages internalized both types of nanoparticles, but they showed different phenotypic and metabolic responses to each nanoparticle type. Unmodified silk fibroin nanoparticles induced the upregulation of several processes, including production of proinflammatory mediators (e.g., cytokines), release of nitric oxide, and promotion of antioxidant activity. These responses were accompanied by changes in the macrophage metabolomic profiles that were consistent with a proinflammatory state and that indicated an increase in glycolysis and reprogramming of the tricarboxylic acid cycle and the creatine kinase/phosphocreatine pathway. By contrast, PEGylated silk fibroin nanoparticles induced milder changes to both inflammatory and metabolic profiles, suggesting that immunomodulation of macrophages with silk fibroin nanoparticles is PEGylation-dependent. Overall, PEGylation of silk fibroin nanoparticles reduced the inflammatory and metabolic responses initiated by macrophages, and this observation could be used to guide the therapeutic applications of these nanoparticles. © 2019 American Chemical Society.
- ItemHybridized Guided-Mode Resonances via Colloidal Plasmonic Self-Assembled Grating(Washington, DC : Soc., 2019) Sarkar, Swagato; Gupta, Vaibhav; Kumar, Mohit; Schubert, Jonas; Probst, Patrick T.; Joseph, Joby; König, Tobias A.F.For many photonic applications, it is important to confine light of a specific wavelength at a certain volume of interest at low losses. So far, it is only possible to use the polarized light perpendicular to the solid grid lines to excite waveguide-plasmon polaritons in a waveguide-supported hybrid structure. In our work, we use a plasmonic grating fabricated by colloidal self-assembly and an ultrathin injection layer to guide the resonant modes selectively. We use gold nanoparticles self-assembled in a linear template on a titanium dioxide (TiO 2 ) layer to study the dispersion relation with conventional ultraviolet-visible-near-infrared spectroscopic methods. Supported with finite-difference in time-domain simulations, we identify the optical band gaps as hybridized modes: plasmonic and photonic resonances. Compared to metallic grids, the observation range of hybridized guided modes can now be extended to modes along the nanoparticle chain lines. With future applications in energy conversion and optical filters employing these cost-efficient and upscalable directed self-assembly methods, we discuss also the application in refractive index sensing of the particle-based hybridized guided modes. Copyright © 2019 American Chemical Society.
- ItemPolyacrylamide Bead Sensors for in vivo Quantification of Cell-Scale Stress in Zebrafish Development([London] : Macmillan Publishers Limited, part of Springer Nature, 2019) Träber, N.; Uhlmann, K.; Girardo, S.; Kesavan, G.; Wagner, K.; Friedrichs, J.; Goswami, R.; Bai, K.; Brand, M.; Werner, C.; Balzani, D.; Guck, J.Mechanical stress exerted and experienced by cells during tissue morphogenesis and organ formation plays an important role in embryonic development. While techniques to quantify mechanical stresses in vitro are available, few methods exist for studying stresses in living organisms. Here, we describe and characterize cell-like polyacrylamide (PAAm) bead sensors with well-defined elastic properties and size for in vivo quantification of cell-scale stresses. The beads were injected into developing zebrafish embryos and their deformations were computationally analyzed to delineate spatio-temporal local acting stresses. With this computational analysis-based cell-scale stress sensing (COMPAX) we are able to detect pulsatile pressure propagation in the developing neural rod potentially originating from polarized midline cell divisions and continuous tissue flow. COMPAX is expected to provide novel spatio-temporal insight into developmental processes at the local tissue level and to facilitate quantitative investigation and a better understanding of morphogenetic processes. © 2019, The Author(s).
- ItemExtruded polycarbonate/Di-Allyl phthalate composites with ternary conductive filler system for bipolar plates of polymer electrolyte membrane fuel cells(Bristol : IOP Publ., 2019) Naji, Ahmed; Krause, Beate; Pötschke, Petra; Ameli, AmirHere, we report multifunctional polycarbonate (PC)-based conductive polymer composites (CPCs) with outstanding performance manufactured by a simple extrusion process and intended for use in bipolar plate (BPP) applications in polymer electrolyte membrane (PEM) fuel cells. CPCs were developed using a ternary conductive filler system containing carbon nanotube (CNT), carbon fiber (CF), and graphite (G) and by introducing di-allyl phthalate (DAP) as a plasticizer to PC matrix. The samples were fabricated using twin-screw extrusion followed by compression molding and the microstructure, electrical conductivity, thermal conductivity, and mechanical properties were investigated. The results showed a good dispersion of the fillers with some degree of interconnection between dissimilar fillers. The addition of DAP enhanced the electrical conductivity and tensile strength of the CPCs. Due to its plasticizing effect, DAP reduced the processing temperature by 75 °C and facilitated the extrusion of CPCs with filler loads as high as 63 wt% (3 wt% CNT, 30 wt% CF, 30 wt% G). Consequently, CPCs with the through-plane electrical, in-plane electrical and thermal conductivities and tensile strength of 4.2 S cm-1, 34.3 S cm-1, 2.9 W m-1 K-1, and 75.4 MPa, respectively, were achieved. This combination of properties indicates the potential of PC-based composites enriched with hybrid fillers and plasticizers as an alternative material for BPP application.