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- ItemMechanochemistry-assisted synthesis of hierarchical porous carbons applied as supercapacitors(Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2017) Leistenschneider, Desirée; Jäckel, Nicolas; Hippauf, Felix; Presser, Volker; Borchardt, LarsA solvent-free synthesis of hierarchical porous carbons is conducted by a facile and fast mechanochemical reaction in a ball mill. By means of a mechanochemical ball-milling approach, we obtained titanium(IV) citrate-based polymers, which have been processed via high temperature chlorine treatment to hierarchical porous carbons with a high specific surface area of up to 1814 m2 g−1 and well-defined pore structures. The carbons are applied as electrode materials in electric double-layer capacitors showing high specific capacitances with 98 F g−1 in organic and 138 F g−1 in an ionic liquid electrolyte as well as good rate capabilities, maintaining 87% of the initial capacitance with 1 M TEA-BF4 in acetonitrile (ACN) and 81% at 10 A g−1 in EMIM-BF4.
- ItemMechanically reinforced catechol-containing hydrogels with improved tissue gluing performance(Basel : MDPI, 2017) Feng, Jun; Ton, Xuan-Anh; Zhao, Shifang; Paez, Julieta I.; del Campo, AránzazuIn situ forming hydrogels with catechol groups as tissue reactive functionalities are interesting bioinspired materials for tissue adhesion. Poly(ethylene glycol) (PEG)–catechol tissue glues have been intensively investigated for this purpose. Different cross-linking mechanisms (oxidative or metal complexation) and cross-linking conditions (pH, oxidant concentration, etc.) have been studied in order to optimize the curing kinetics and final cross-linking degree of the system. However, reported systems still show limited mechanical stability, as expected from a PEG network, and this fact limits their potential application to load bearing tissues. Here, we describe mechanically reinforced PEG–catechol adhesives showing excellent and tunable cohesive properties and adhesive performance to tissue in the presence of blood. We used collagen/PEG mixtures, eventually filled with hydroxyapatite nanoparticles. The composite hydrogels show far better mechanical performance than the individual components. It is noteworthy that the adhesion strength measured on skin covered with blood was >40 kPa, largely surpassing (>6 fold) the performance of cyanoacrylate, fibrin, and PEG–catechol systems. Moreover, the mechanical and interfacial properties could be easily tuned by slight changes in the composition of the glue to adapt them to the particular properties of the tissue. The reported adhesive compositions can tune and improve cohesive and adhesive properties of PEG–catechol-based tissue glues for load-bearing surgery applications.
- ItemBright fluorescent silica-nanoparticle probes for high-resolution STED and confocal microscopy(Frankfurt am Main : Beilstein-Institut, 2017) Tavernaro, Isabella; Cavelius, Christian; Peuschel, Henrike; Kraegeloh, AnnetteIn recent years, fluorescent nanomaterials have gained high relevance in biological applications as probes for various fluorescencebased spectroscopy and imaging techniques. Among these materials, dye-doped silica nanoparticles have demonstrated a high potential to overcome the limitations presented by conventional organic dyes such as high photobleaching, low stability and limited fluorescence intensity. In the present work we describe an effective approach for the preparation of fluorescent silica nanoparticles in the size range between 15 and 80 nm based on L-arginine-controlled hydrolysis of tetraethoxysilane in a biphasic cyclohexane–water system. Commercially available far-red fluorescent dyes (Atto647N, Abberior STAR 635, Dy-647, Dy-648 and Dy-649) were embedded covalently into the particle matrix, which was achieved by aminosilane coupling. The physical particle attributes (particle size, dispersion, degree of agglomeration and stability) and the fluorescence properties of the obtained particles were compared to particles from commonly known synthesis methods. As a result, the spectroscopic characteristics of the presented monodisperse dye-doped silica nanoparticles were similar to those of the free uncoupled dyes, but indicate a much higher photostability and brightness. As revealed by dynamic light scattering and ζ-potential measurements, all particle suspensions were stable in water and cell culture medium. In addition, uptake studies on A549 cells were performed, using confocal and stimulated emission depletion (STED) microscopy. Our approach allows for a step-by-step formation of dye-doped silica nanoparticles in the form of dye-incorporated spheres, which can be used as versatile fluorescent probes in confocal and STED imaging.
- ItemFunnel-shaped microstructures for strong reversible adhesion(Hoboken, NJ : Wiley, 2017) Fischer, Sarah C.L.; Groß, Katja; Abad, Oscar Torrents; Becker, MIchael M.; Park, Euiyoung; Hensel, René; Arzt, EduardThe potential of a new design of adhesive microstructures in the micrometer range for enhanced dry adhesion is investigated. Using a two-photon lithography system, complex 3D master structures of funnel-shaped microstructures are fabricated for replication into poly(ethylene glycol) dimethacrylate polymer. The diameter, the flap thickness, and the opening angle of the structures are varied systematically. The adhesion of single structures is characterized using a triboindenter system equipped with a flat diamond punch. The pull-off stresses obtained reaches values up to 5.6 MPa, which is higher than any values reported in literature for artificial dry adhesives. Experimental and numerical results suggest a characteristic attachment mechanism that leads to intimate contact formation from the edges toward the center of the structures. van der Waals interactions most likely dominate the adhesion, while contributions by suction or capillarity play only a minor role. Funnel-shaped microstructures are a promising concept for strong and reversible adhesives, applicable in novel pick and place handling systems or wall-walking robots.
- ItemComposite pillars with a tunable interface for adhesion to rough substrates(Washington D.C. : American Chemical Society, 2017) Fischer, Sarah C.L.; Arzt, Eduard; Hensel, RenéThe benefits of synthetic fibrillar dry adhesives for temporary and reversible attachment to hard objects with smooth surfaces have been successfully demonstrated in previous studies. However, surface roughness induces a dramatic reduction in pull-off stresses and necessarily requires revised design concepts. Toward this aim, we introduce cylindrical two-phase single pillars, which are composed of a mechanically stiff stalk and a soft tip layer. Adhesion to smooth and rough substrates is shown to exceed that of conventional pillar structures. The adhesion characteristics can be tuned by varying the thickness of the soft tip layer, the ratio of the Young’s moduli and the curvature of the interface between the two phases. For rough substrates, adhesion values similar to those obtained on smooth substrates were achieved. Our concept of composite pillars overcomes current practical limitations caused by surface roughness and opens up fields of application where roughness is omnipresent.
- ItemVimentin levels and serine 71 phosphorylation in the control of cell-matrix adhesions, migration speed, and shape of transformed human fibroblasts(Basel : MDPI, 2017) Terriac, Emmanuel; Coceano, Giovanna; Mavajian, Zahra; Hageman, Tijmen A.G.; Christ, Andreas F.; Testa, Ilaria; Lautenschläger, Franziska; Gad, Annica K.G.Metastasizing tumor cells show increased expression of the intermediate filament (IF) protein vimentin, which has been used to diagnose invasive tumors for decades. Recent observations indicate that vimentin is not only a passive marker for carcinoma, but may also induce tumor cell invasion. To clarify how vimentin IFs control cell adhesions and migration, we analyzed the nanoscale (30–50 nm) spatial organization of vimentin IFs and cell-matrix adhesions in metastatic fibroblast cells, using three-color stimulated emission depletion (STED) microscopy. We also studied whether wild-type and phospho-deficient or -mimicking mutants of vimentin changed the size and lifetime of focal adhesions (FAs), cell shape, and cell migration, using live-cell total internal reflection imaging and confocal microscopy. We observed that vimentin exists in fragments of different lengths. Short fragments were mostly the size of a unit-length filament and were mainly localized close to small cell-matrix adhesions. Long vimentin filaments were found in the proximity of large FAs. Vimentin expression in these cells caused a reduction in FAs size and an elongated cell shape, but did not affect FA lifetime, or the speed or directionality of cell migration. Expression of a phospho-mimicking mutant (S71D) of vimentin increased the speed of cell migration. Taken together, our results suggest that in highly migratory, transformed mesenchymal cells, vimentin levels control the cell shape and FA size, but not cell migration, which instead is linked to the phosphorylation status of S71 vimentin. These observations are consistent with the possibility that not only levels, but also the assembly status of vimentin control cell migration.
- ItemInteractions between shape-persistent macromolecules as probed by AFM(Frankfurt am Main : Beilstein-Institut, 2017) Blas, Johannes; Brunke, Jessica; Emmerich, Franziska; Cédric, Przybylski; Garamus, Vasil M.; Feoktystov, Artem; Bennewitz, Roland; Wenz, Gerhard; Albrecht, MarcelWater-soluble shape-persistent cyclodextrin (CD) polymers with amino-functionalized end groups were prepared starting from diacetylene-modified cyclodextrin monomers by a combined Glaser coupling/click chemistry approach. Structural perfection of the neutral CD polymers and inclusion complex formation with ditopic and monotopic guest molecules were proven by MALDI–TOF and UV–vis measurements. Small-angle neutron and X-ray (SANS/SAXS) scattering experiments confirm the stiffness of the polymer chains with an apparent contour length of about 130 Å. Surface modification of planar silicon wafers as well as AFM tips was realized by covalent bound formation between the terminal amino groups of the CD polymer and a reactive isothiocyanate–silane monolayer. Atomic force measurements of CD polymer decorated surfaces show enhanced supramolecular interaction energies which can be attributed to multiple inclusion complexes based on the rigidity of the polymer backbone and the regular configuration of the CD moieties. Depending on the geometrical configuration of attachment anisotropic adhesion characteristics of the polymer system can be distinguished between a peeling and a shearing mechanism.
- ItemAdhesion and Cellular Compatibility of Silicone-Based Skin Adhesives(Weinheim : Wiley-VCH, 2017) Fischer, Sarah C. L.; Kruttwig, Klaus; Bandmann, Vera; Hensel, René; Arzt, EduardPressure-sensitive adhesives based on silicone materials have emerging potential as adhesives in healthcare products, in particular for gentle skin adhesives. To this end, adhesion to rough skin and biocompatibility are crucial factors for a successful implementation. In this study, the mechanical, adhesive, and biological properties of the two-component poly(dimethylsiloxane) Soft Skin Adhesive MG 7-9800 (SSA, Dow Corning) have been investigated and compared to Sylgard 184. Different mixing ratios of SSA's components allow for tuning of the shear modulus, thereby modifying the adhesive properties of the polymer. To give a comprehensive insight, the authors have analyzed the interplay between pull-off stress, adhesion energy, and stretch of the adhesive films on smooth and rough surfaces. The focus is placed on the effects of substrate roughness and on low pressure oxygen plasma treatment of the adhesive films. SSA shows superior biocompatibility in in vitro cell culture experiments. High pull-off stresses in the range of 3 N cm−2 on a rough surface are achieved, promising broad application spectra for SSA-based healthcare products.
- ItemLow friction and high solid-solid contact ratio—A contradiction for laser-patterned surfaces?(Basel : MDPI, 2017) Bettscheider, Simon; Grützmacher, Philipp G.; Rosenkrantz, AndreasRecording of Stribeck-like curves is a common way to study the effect of laser-patterned surfaces on the frictional efficiency. However, solely relying on the coefficient of friction when identifying the lubrication regime and the underlying working principles can be misleading. Consequently, a ball-on-disc tribometer was combined with an electrical resistivity circuit to simultaneously measure Stribeck-like curves and solid-solid contact ratios for polished and laser-patterned samples. Line-like surface patterns with different periodicities were produced by direct laser interference patterning on steel substrates (AISI304). The reference shows a Stribeck-like behavior well correlating with the contact ratios. The behavior deviates for high sliding velocities (high contact ratios) due to a loss of lubricant induced by centrifugal forces pulling the lubricant out of the contact zone. In contrast, the solid–solid contact ratio of the laser-patterned samples is around 80% for all sliding velocities. Those values can be explained by higher contact pressures and the structural depth induced by the surface topography which make a full separation of the surfaces unlikely. Despite those high values for the contact ratio, laser-patterning significantly reduces friction, which can be traced back to a reduced real contact area and the ability to store oil in the contact zone.
- ItemLiquid-phase electron microscopy of molecular drug response in breast cancer cells reveals irresponsive cell subpopulations related to lack of HER2 homodimers(Bethesda, Md. : American Society for Cell Biology, 2017) Peckys, Diana B.; Korf, Ulrike; Wiemann, Stefan; de Jonge, NielsThe development of drug resistance in cancer poses a major clinical problem. An example is human epidermal growth factor receptor 2 (HER2) overexpressing breast cancer often treated with anti-HER2 antibody therapies, such as trastuzumab. Because drug resistance is rooted mainly in tumor cell heterogeneity, we examined the drug effect in different subpopulations of SKBR3 breast cancer cells and compared the results with those of a drugresistant cell line, HCC1954. Correlative light microscopy and liquid-phase scanning transmission electron microscopy were used to quantitatively analyze HER2 responses upon drug binding, whereby many tens of whole cells were imaged. Trastuzumab was found to selectively cross-link and down-regulate HER2 homodimers from the plasma membranes of bulk cancer cells. In contrast, HER2 resided mainly as monomers in rare subpopulations of resting and cancer stem cells (CSCs), and these monomers were not internalized after drug binding. The HER2 distribution was hardly influenced by trastuzumab for the HCC1954 cells. These findings show that resting cells and CSCs are irresponsive to the drug and thus point toward a molecular explanation behind the origin of drug resistance. This analytical method is broadly applicable to study membrane protein interactions in the intact plasma membrane, while accounting for cell heterogeneity.