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Surface structure influences contact killing of bacteria by copper
Copper kills bacteria rapidly by a mechanism that is not yet fully resolved. The antibacterial property of copper has raised interest in its use in hospitals, in place of plastic or stainless steel. On the latter surfaces, bacteria can survive for days or even weeks. Copper surfaces could thus provide a powerful accessory measure to curb nosocomial infections. We here investigated the effect of the copper surface structure on the efficiency of contact killing of Escherichia coli, an aspect which so far has received very little attention. It was shown that electroplated copper surfaces killed bacteria more rapidly than either polished copper or native rolled copper. The release of ionic copper was also more rapid from electroplated copper compared to the other materials. Scanning electron microscopy revealed that the bacteria nudged into the grooves between the copper grains of deposited copper. The findings suggest that, in terms of contact killing, more efficient copper surfaces can be engineered.
A correlative analysis of gold nanoparticles internalized by A549 cells
Fluorescently labeled nanoparticles are widely used to investigate nanoparticle cell interactions by fluorescence microscopy. Owing to limited lateral and axial resolution, nanostructures (<100 nm) cannot be resolved by conventional light microscopy techniques. Especially after uptake into cells, a common fate of the fluorescence label and the particle core cannot be taken for granted. In this study, a correlative approach is presented to image fluorescently labeled gold nanoparticles inside whole cells by correlative light and electron microscopy (CLEM). This approach allows for detection of the fluorescently labeled particle shell as well as for the gold core in one sample. In this setup, A549 cells are exposed to 8 nm Atto 647N-labeled gold nanoparticles (3.3 × 109 particles mL−1, 0.02 μg Au mL−1) for 5 h and are subsequently imaged by confocal laser scanning microscopy (CLSM) and transmission electron microscopy (TEM). Eight fluorescence signals located at different intracellular positions are further analyzed by TEM. Five of the eight fluorescence spots are correlated with isolated or agglomerated gold nanoparticles. Three fluorescence signals could not be related to the presence of gold, indicating a loss of the particle shell.
Ageing of alkylthiol-stabilized gold nanoparticles
The ageing of spherical gold nanoparticles having 6-nm-diameter cores and a ligand shell of dodecanethiol is investigated under different storage conditions. Losses caused by agglomeration and changes in optical particle properties are quantified. Changes in colloidal stability are probed by analytical centrifugation in a polar solvent mixture. Chemical changes are detected by elementary analysis of particles and solvent. Fractionation occurs under all storage conditions. Ageing is not uniform but broadens the property distributions of the particles. Small-number statistics in the ligand shell density and the morphological heterogeneity of particles are possible explanations. Washing steps exacerbate ageing, a process that could not be fully reversed by excess ligands. Dry storage is not preferable to storage in solvent. Storage under inert argon atmosphere reduces losses more than all other conditions but could not prevent it entirely.
Contact Aging Enhances Adhesion of Micropatterned Silicone Adhesives to Glass Substrates
The transfer of biological concepts into synthetic micropatterned adhesives has recently enabled a new generation of switchable, reversible handling devices. Over the last two decades, many design principles have been explored that helped to understand the underlying mechanics and to optimize such adhesives for certain applications. An aspect that has been overlooked so far is the influence of longer hold times on the adhesive contacts. Exemplarily, the pull‐off stress and work of separation of a micropatterned adhesive specimen are enhanced by factors 3 and 6, respectively, after 1000 min in contact with a glass substrate. In addition to such global measures, the increase of adhesion of all individual micropillars is analyzed. It is found that contact aging varied across the microarray, as it drastically depends on local conditions. Despite great differences on the micropillar scale, the adhesion of entire specimens increased with very similar power laws, as this is determined by the mean contact ageing of the individual structures. Overall, contact aging must be critically evaluated before using micropatterned adhesives, especially for long‐term fixations and material combinations that are chemically attractive to each other.
A novel universal algorithm for filament network tracing and cytoskeleton analysis
The rapid development of advanced microscopy techniques over recent decades has significantly increased the quality of imaging and our understanding of subcellular structures, such as the organization of the filaments of the cytoskeleton using fluorescence and electron microscopy. However, these recent improvements in imaging techniques have not been matched by similar development of techniques for computational analysis of the images of filament networks that can now be obtained. Hence, for a wide range of applications, reliable computational analysis of such two-dimensional methods remains challenging. Here, we present a new algorithm for tracing of filament networks. This software can extract many important parameters from grayscale images of filament networks, including the mesh hole size, and filament length and connectivity (also known as Coordination Number). In addition, the method allows sub-networks to be distinguished in two-dimensional images using intensity thresholding. We show that the algorithm can be used to analyze images of cytoskeleton networks obtained using different advanced microscopy methods. We have thus developed a new improved method for computational analysis of two-dimensional images of filamentous networks that has wide applications for existing imaging techniques. The algorithm is available as open-source software.
Toward light‐regulated living biomaterials
Living materials are an emergent material class, infused with the productive,adaptive, and regenerative properties of living organisms. Property regulation in living materials requires encoding responsive units in the living components to allow external manipulation of their function. Here, an optoregulated Escherichia coli (E. coli)-based living biomaterial that can be externally addressed using light to interact with mammalian cells is demonstrated. This is achieved by using a photoactivatable inducer of gene expression and bacterial surface display technology to present an integrin-specific miniprotein on the outer membrane of an endotoxin-free E. coli strain. Hydrogel surfaces functionalized with the bacteria can expose cell adhesive molecules upon in situ light-activation, and trigger cell adhesion. Surface immobilized bacteria are able to deliver a fluorescent protein to the mammalian cells with which they are interacting, indicating the potential of such a bacterial material to deliver molecules to cells in a targeted manner.
Carbons and electrolytes for advanced supercapacitors
Electrical energy storage (EES) is one of the most critical areas of technological research around the world. Storing and efficiently using electricity generated by intermittent sources and the transition of our transportation fleet to electric drive depend fundamentally on the development of EES systems with high energy and power densities. Supercapacitors are promising devices for highly efficient energy storage and power management, yet they still suffer from moderate energy densities compared to batteries. To establish a detailed understanding of the science and technology of carbon/carbon supercapacitors, this review discusses the basic principles of the electrical double-layer (EDL), especially regarding the correlation between ion size/ion solvation and the pore size of porous carbon electrodes. We summarize the key aspects of various carbon materials synthesized for use in supercapacitors. With the objective of improving the energy density, the last two sections are dedicated to strategies to increase the capacitance by either introducing pseudocapacitive materials or by using novel electrolytes that allow to increasing the cell voltage. In particular, advances in ionic liquids, but also in the field of organic electrolytes, are discussed and electrode mass balancing is expanded because of its importance to create higher performance asymmetric electrochemical capacitors.
Acid‐Base Interactions of Pyrazine, Ethyl Acetate, Di‐alcohols, and Lysine with the cyclic Alumosiloxane (Ph2SiO)8[Al(O)OH]4 in View of Mimicking Al2O3(H2O) Surface Reactions
The etherate of (Ph2SiO)8[Al(O)OH]4 can be transformed into the pyrazine adduct (Ph2SiO)8[Al(O)OH]4·3N(C2H2)2N (1), the ethyl acetate adduct (Ph2SiO)8[Al(O)OH]4·3H3C‐C(O)OC2H5 (2), the 1,6‐hexane diol adduct (Ph2SiO)8[Al(O)OH]4·2HO–CH2(CH2)4CH2–OH (3) and the 1,4‐cyclohexane diol adduct (Ph2SiO)8[Al(O)OH]4·4HO–CH(CH2CH2)2CH–OH (4). In all compounds the OH groups of the starting material bind to the bases through O–H···N (1) or O–H···O hydrogen bonds (2, 3, 4) as found from single‐crystal X‐ray diffraction analyses. Whereas in 1 only three of the central OH groups bind to the pyrazines, in 2 two of them bind to the same carbonyl oxygen atom of the ethyl acetate resulting in an unprecedented O–H···O···H–O double hydrogen bridge. The hexane diol adduct 3 in the crystal forms a one‐dimensional coordination polymer with an intramolecularly to two OH groups grafted hexane diol loop, while the second hexane diol is connecting intermolecularly. In the cyclohexane diol adduct 4 all OH groups of the central Al4(OH)4 ring bind to different diols, leaving one alcohol group per diol uncoordinated. These “free” OH groups form an (O‐H···)4 assembly creating a three‐dimensional overall structure. When reacting with (Ph2SiO)8[Al(O)OH]4 lysine loses water, turns into the cyclic 3‐amino‐2‐azepanone, and transforms through chelation of one of the aluminum atoms the starting material into a new polycycle. The isolated compound has the composition (Ph2SiO)12[Al(O)OH]4[Al2O3]2·4 C6H12N2O·6(CH2)4O (5).
Combining Battery‐Type and Pseudocapacitive Charge Storage in Ag/Ti3C2Tx MXene Electrode for Capturing Chloride Ions with High Capacitance and Fast Ion Transport
The recent advances in chloride‐ion capturing electrodes for capacitive deionization (CDI) are limited by the capacity, rate, and stability of desalination. This work introduces Ti3C2Tx/Ag synthesized via a facile oxidation‐reduction method and then uses it as an anode for chloride‐ion capture in CDI. Silver nanoparticles are formed successfully and uniformly distributed with the layered‐structure of Ti3C2Tx. All Ti3C2Tx/Ag samples are hydrophilic, which is beneficial for water desalination. Ti3C2Tx/Ag samples with a low charge transfer resistance exhibit both pseudocapacitive and battery behaviors. Herein, the Ti3C2Tx/Ag electrode with a reaction time of 3 h exhibits excellent desalination performance with a capacity of 135 mg Cl− g−1 at 20 mA g−1 in a 10 × 10−3 m NaCl solution. Furthermore, low energy consumption of 0.42 kWh kg−1 Cl− and a desalination rate of 1.5 mg Cl− g−1 min−1 at 50 mA g−1 is achieved. The Ti3C2Tx/Ag system exhibits fast rate capability, high desalination capacity, low energy consumption, and excellent cyclability, which can be ascribed to the synergistic effect between the battery and pseudocapacitive behaviors of the Ti3C2Tx/Ag hybrid material. This work provides fundamental insight into the coupling of battery and pseudocapacitive behaviors during Cl− capture for electrochemical desalination.
Funnel-shaped microstructures for strong reversible adhesion
The 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.