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- ItemA New Family of Layered Metal-Organic Semiconductors: Cu/V-Organophosphonates(Weinheim : Wiley-VCH, 2023) Tholen, Patrik; Wagner, Lukas; Ruthes, Jean G. A.; Siemensmeyer, Konrad; Beglau, Thi Hai Yen; Muth, Dominik; Zorlu, Yunus; Okutan, Mustafa; Goldschmidt, Jan Christoph; Janiak, Christoph; Presser, Volker; Yavuzçetin, Özgür; Yücesan, GündoğHerein, we report the design and synthesis of a layered redox-active, antiferromagnetic metal organic semiconductor crystals with the chemical formula [Cu(H2O)2V(µ-O)(PPA)2] (where PPA is phenylphosphonate). The crystal structure of [Cu(H2O)2V(µ-O)(PPA)2] shows that the metal phosphonate layers are separated by phenyl groups of the phenyl phosphonate linker. Tauc plotting of diffuse reflectance spectra indicates that [Cu(H2O)2V(µ-O)(PPA)2] has an indirect band gap of 2.19 eV. Photoluminescence (PL) spectra indicate a complex landscape of energy states with PL peaks at 1.8 and 2.2 eV. [Cu(H2O)2V(µ-O)(PPA)2] has estimated hybrid ionic and electronic conductivity values between 0.13 and 0.6 S m−1. Temperature-dependent magnetization measurements show that [Cu(H2O)2V(µ-O)(PPA)2] exhibits short range antiferromagnetic order between Cu(II) and V(IV) ions. [Cu(H2O)2V(µ-O)(PPA)2] is also photoluminescent with photoluminescence quantum yield of 0.02%. [Cu(H2O)2V(µ-O)(PPA)2] shows high electrochemical, and thermal stability.
- ItemHigh temporal-resolution scanning transmission electron microscopy using sparse-serpentine scan pathways([London] : Macmillan Publishers Limited, part of Springer Nature, 2021) Ortega, Eduardo; Nicholls, Daniel; Browning, Nigel D.; de Jonge, NielsScanning transmission electron microscopy (STEM) provides structural analysis with sub-angstrom resolution. But the pixel-by-pixel scanning process is a limiting factor in acquiring high-speed data. Different strategies have been implemented to increase scanning speeds while at the same time minimizing beam damage via optimizing the scanning strategy. Here, we achieve the highest possible scanning speed by eliminating the image acquisition dead time induced by the beam flyback time combined with reducing the amount of scanning pixels via sparse imaging. A calibration procedure was developed to compensate for the hysteresis of the magnetic scan coils. A combination of sparse and serpentine scanning routines was tested for a crystalline thin film, gold nanoparticles, and in an in-situ liquid phase STEM experiment. Frame rates of 92, 23 and 5.8 s-1 were achieved for images of a width of 128, 256, and 512 pixels, respectively. The methods described here can be applied to single-particle tracking and analysis of radiation sensitive materials.
- ItemReversible Conductive Inkjet Printing of Healable and Recyclable Electrodes on Cardboard and Paper(Weinheim : Wiley-VCH Verlag, 2020) Kang, D.J.; Jüttke, Y.; González-García, L.; Escudero, A.; Haft, M.; Kraus, T.Conductive inkjet printing with metal nanoparticles is irreversible because the particles are sintered into a continuous metal film. The resulting structures are difficult to remove or repair and prone to cracking. Here, a hybrid ink is used to obviate the sintering step and print interconnected particle networks that become highly conductive immediately after drying. It is shown that reversible conductive printing is possible on low-cost cardboard samples after applying standard paper industry coats that are adapted in terms of surface energy and porosity. The conductivity of the printed films approaches that of sintered standard inks on the same substrate, but the mobility of the hybrid particle film makes them less sensitive to cracks during bending and folding of the substrate. Damages that occur can be partially repaired by wetting the film such that particle mobility is increased and particles move to bridge insulating gaps in the film. It is demonstrated that the conductive material can be recovered from the cardboard at the end of its life time and be redispersed to recycle the particles and reuse them in conductive inks.
- ItemAnalytical and numerical results for the elasticity and adhesion of elastic films with arbitrary Poisson’s ratio and confinement(London [u.a.] : Taylor & Francis, 2022) Müller, Christian; Müser, Martin H.We present an approximate, analytical treatment for the linearly elastic response of a film with arbitrary Poisson's ratio (Formula presented.), which is indented by a flat cylindrical punch while resting on a rigid foundation. Our approach is based on a simple scaling argument allowing the vast changes of the elastomer’s effective modulus (Formula presented.) with the ratio of film height (Formula presented.) and indenter radius (Formula presented.) to be described with a compact, analytical expression. This yields exact asymptotics for large and small reduced film heights (Formula presented.), whereby it also reproduces the observation that (Formula presented.) has a pronounced minimum for (Formula presented.) at (Formula presented.). Using Green’s function molecular dynamics (GFMD), we demonstrate that the predictions for (Formula presented.) are reasonably correct and generate accurate reference data for effective modulus and pull-off force. GFMD also reveals that the nature of surface instabilities occurring during stable crack growth as well as the crack initiation itself depend sensitively on the way how continuum mechanics is terminated at small scales, that is, on parameters beyond the two dimensionless numbers (Formula presented.) and (Formula presented.) defining the continuum problem.
- ItemReal-time monitoring of cell surface protein arrival with split luciferases(Oxford : Wiley-Blackwell, 2023) Fischer, Alexandra A. M.; Schatz, Larissa; Baaske, Julia; Römer, Winfried; Weber, Wilfried; Thuenauer, RolandEach cell in a multicellular organism permanently adjusts the concentration of its cell surface proteins. In particular, epithelial cells tightly control the number of carriers, transporters and cell adhesion proteins at their plasma membrane. However, sensitively measuring the cell surface concentration of a particular protein of interest in live cells and in real time represents a considerable challenge. Here, we introduce a novel approach based on split luciferases, which uses one luciferase fragment as a tag on the protein of interest and the second fragment as a supplement to the extracellular medium. Once the protein of interest arrives at the cell surface, the luciferase fragments complement and generate luminescence. We compared the performance of split Gaussia luciferase and split Nanoluciferase by using a system to synchronize biosynthetic trafficking with conditional aggregation domains. The best results were achieved with split Nanoluciferase, for which luminescence increased more than 6000-fold upon recombination. Furthermore, we showed that our approach can separately detect and quantify the arrival of membrane proteins at the apical and basolateral plasma membrane in single polarized epithelial cells by detecting the luminescence signals with a microscope, thus opening novel avenues for characterizing the variations in trafficking in individual epithelial cells.
- ItemSurfactant stabilization of vanadium iron oxide derived from Prussian blue analog for lithium-ion battery electrodes(Cambridge : Royal Society of Chemistry, 2023) Bornamehr, Behnoosh; El Gaidi, Hiba; Arnold, Stefanie; Pameté, Emmanuel; Presser, VolkerDue to their high energy density, Li-ion batteries have become indispensable for energy storage in many technical devices. Prussian blue and its analogs are a versatile family of materials. Apart from their direct use as an alkali-ion battery electrode, they are a promising source for templating other compounds due to the presence of carbon, nitrogen, and metallic elements in their structure, ease of synthesis, and high tunability. In this study, homogeneous iron vanadate derivatization from iron vanadium Prussian blue was successfully carried out using an energy efficient infrared furnace utilizing CO2 gas. Iron-vanadate is an inherently unstable electrode material if cycled at low potentials vs. Li/Li+. Several parameters were optimized to achieve a stable electrochemical performance of this derivative, and the effect of surfactants, such as tannic acid, sodium dodecylbenzene sulfonate, and polyvinylpyrrolidone were shown with their role in the morphology and electrochemical performance. While stabilizing the performance, we demonstrate that the type and order of addition of these surfactants are fundamental for a successful coating formation, otherwise they can hinder the formation of PBA, which has not been reported previously. Step-by-step, we illustrate how to prepare self-standing electrodes for Li-ion battery cells without using an organic solvent or a fluorine-containing binder while stabilizing the electrochemical performance. A 400 mA h g−1 capacity at the specific current of 250 mA g−1 was achieved after 150 cycles while maintaining a Coulombic efficiency of 99.2% over an extended potential range of 0.01–3.50 V vs. Li/Li+.
- ItemMicrogravity Removes Reaction Limits from Nonpolar Nanoparticle Agglomeration(Weinheim : Wiley-VCH, 2022) Pyttlik, Andrea; Kuttich, Björn; Kraus, TobiasGravity can affect the agglomeration of nanoparticles by changing convection and sedimentation. The temperature-induced agglomeration of hexadecanethiol-capped gold nanoparticles in microgravity (µ g) is studied at the ZARM (Center of Applied Space Technology and Microgravity) drop tower and compared to their agglomeration on the ground (1 g). Nonpolar nanoparticles with a hydrodynamic diameter of 13 nm are dispersed in tetradecane, rapidly cooled from 70 to 10 °C to induce agglomeration, and observed by dynamic light scattering at a time resolution of 1 s. The mean hydrodynamic diameters of the agglomerates formed after 8 s in microgravity are 3 times (for low initial concentrations) to 5 times (at high initial concentrations) larger than on the ground. The observations are consistent with an agglomeration process that is closer to the reaction limit on thground and closer to the diffusion limit in microgravity.
- ItemRole of Hair Coverage and Sweating for Textile Friction on the Forearm(Berlin : Springer, 2020) Lyu, Jingchun; Özgün, Novaf; Kondziela, David J.; Bennewitz, RolandFriction of textiles on the human forearm is an important factor in comfort sensations of garments. We built an experiment to measure friction for textiles sliding on the forearm under loading conditions which are characteristic for wearing shirts or jackets. The hair coverage of the participants’ forearm was quantified by image analysis of photographs of the arm in the region of contact. Friction results for five standard textiles suggest to treat hair coverage in two classes. Sweating after physical activity leads to an increase of friction by factors of 2 to 5 for participants with less hairy forearms, while an increase by a factor of 1 to 1.7 only was found for participants with more hairy forearms. We introduce a method of wetting the forearm of study participants in a controlled way with water, which results in similar friction as for the sweating forearm after physical activity. The method allows for efficient studies of the role of skin moisture for friction including varying hair coverage of the skin.
- ItemRelaxation Times of Ionic Liquids under Electrochemical Conditions Probed by Friction Force Microscopy(Weinheim : WILEY-VCH Verlag GmbH & Co. KGaA, 2023) Hausen, FlorianIonic liquids (ILs) represent an important class of liquids considered for a broad range of applications such as lubrication, catalysis, or as electrolytes in batteries. It is well-known that in the case of charged surfaces, ILs form a pronounced layer structure that can be easily triggered by an externally applied electrode potential. Information about the time required to form a stable interface under varying electrode potentials is of utmost importance in many applications. For the first time, probing of relaxation times of ILs by friction force microscopy is demonstrated. The friction force is extremely sensitive to even subtle changes in the interfacial configuration of ILs. Various relaxation processes with different time scales are observed. A significant difference dependent on the direction of switching the applied potential, i.e., from a more cation-rich to a more anion-rich interface or vice versa, is found. Furthermore, variations in height immediately after the potential step and the presence of trace amounts of water are discussed as well.
- ItemProbiomimetics - Novel Lactobacillus‐Mimicking Microparticles Show Anti‐Inflammatory and Barrier‐Protecting Effects in Gastrointestinal Models(Weinheim : Wiley-VCH, 2020) Kuhn, Thomas; Koch, Marcus; Fuhrmann, GregorThere is a lack of efficient therapies to treat increasingly prevalent autoimmune diseases, such as inflammatory bowel disease and celiac disease. Membrane vesicles (MVs) isolated from probiotic bacteria have shown tremendous potential for treating intestinal inflammatory diseases. However, possible dilution effects and rapid elimination in the gastrointestinal tract may impair their application. A cell‐free and anti‐inflammatory therapeutic system—probiomimetics—based on MVs of probiotic bacteria (Lactobacillus casei and Lactobacillus plantarum) coupled to the surface of microparticles is developed. The MVs are isolated and characterized for size and protein content. MV morphology is determined using cryoelectron microscopy and is reported for the first time in this study. MVs are nontoxic against macrophage‐like dTHP‐1 and enterocyte‐like Caco‐2 cell lines. Subsequently, the MVs are coupled onto the surface of microparticles according to facile aldehyde‐group functionalization to obtain probiomimetics. A significant reduction in proinflammatory TNF‐α level (by 86%) is observed with probiomimetics but not with native MVs. Moreover, it is demonstrated that probiomimetics have the ability to ameliorate inflammation‐induced loss of intestinal barrier function, indicating their potential for further development into an anti‐inflammatory formulation. These engineered simple probiomimetics that elicit striking anti‐inflammatory effects are a key step toward therapeutic MV translation.