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Now showing 1 - 10 of 24
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    Revealing the co-action of viscous and multistability hysteresis in an adhesive, nominally flat punch: A combined numerical and experimental study
    ([Erscheinungsort nicht ermittelbar] : arXiv, 2022) Christian Müller, Manar Samri, René Hensel, Eduard Arzt, Martin H. Müser
    Viscoelasticity is well known to cause a significant hysteresis of crack closure and opening when an elastomer is brought in and out of contact with a flat, rigid counterface. In contrast, the idea that adhesive hysteresis can also result under quasi-static driving due to small-scale, elastic multistability is relatively new. Here, we study a system in which both mechanisms act concurrently. Specifically, we compare the simulated and experimentally measured time evolution of the interfacial force and the real contact area between a soft elastomer and a rigid, flat punch, to which small-scale, single-sinusoidal roughness is added. To this end, we further the Green's function molecular dynamics method and extend recently developed imaging techniques to elucidate the rate- and preload-dependence of the pull-off process. Our results reveal that hysteresis is much enhanced when the saddle points of the topography come into contact, which, however, is impeded by viscoelastic forces and may require sufficiently large preloads. A similar coaction of viscous- and multistability effects is expected to occur in macroscopic polymer contacts and be relevant, e.g., for pressure-sensitive adhesives and modern adhesive gripping devices.
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    Engineering Micropatterned Dry Adhesives: From Contact Theory to Handling Applications
    (Weinheim : Wiley-VCH, 2018) Hensel, René; Moh, Karsten; Arzt, Eduard
    Reversible adhesion is the key functionality to grip, place, and release objects nondestructively. Inspired by nature, micropatterned dry adhesives are promising candidates for this purpose and have attracted the attention of research groups worldwide. Their enhanced adhesion compared to nonpatterned surfaces is frequently demonstrated. An important conclusion is that the contact mechanics involved is at least as important as the surface energy and chemistry. In this paper, the roles of the contact geometry and mechanical properties are reviewed. With a focus on applications, the effects of substrate roughness and of temperature variations, and the long-term performance of micropatterned adhesives are discussed. The paper provides a link between the current, detailed understanding of micropatterned adhesives and emerging applications.
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    Lighting the Path: Light Delivery Strategies to Activate Photoresponsive Biomaterials In Vivo
    (Weinheim : Wiley-VCH, 2021) Pearson, Samuel; Feng, Jun; del Campo, Aránzazu
    Photoresponsive biomaterials are experiencing a transition from in vitro models to in vivo demonstrations that point toward clinical translation. Dynamic hydrogels for cell encapsulation, light-responsive carriers for controlled drug delivery, and nanomaterials containing photosensitizers for photodynamic therapy are relevant examples. Nonetheless, the step to the clinic largely depends on their combination with technologies to bring light into the body. This review highlights the challenge of photoactivation in vivo, and presents strategies for light management that can be adopted for this purpose. The authors’ focus is on technologies that are materials-driven, particularly upconversion nanoparticles that assist in “direct path” light delivery through tissue, and optical waveguides that “clear the path” between external light source and in vivo target. The authors’ intention is to assist the photoresponsive biomaterials community transition toward medical technologies by presenting light delivery concepts that can be integrated with the photoresponsive targets. The authors also aim to stimulate further innovation in materials-based light delivery platforms by highlighting needs and opportunities for in vivo photoactivation of biomaterials. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH.
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    Electrocatalytic fuel cell desalination for continuous energy and freshwater generation
    (Maryland Heights, MO : Cell Press, 2021) Zhang, Yuan; Wang, Lei; Presser, Volker
    Advanced hydrogen technologies contribute essentially to the decarbonization of our industrialized world. Large-scale hydrogen production would benefit from using the abundantly available water reservoir of our planet’s oceans. Current seawater-desalination technologies suffer from high energy consumption, high cost, or low performance. Here, we report technology for water desalination at seawater molarity, based on a polymer ion-exchange membrane fuel cell. By continuously supplying hydrogen and oxygen to the cell, a 160-mM concentration decrease from an initial value of 600 mM is accomplished within 40 h for a 55-mL reservoir. This device’s desalination rate in 600 mM NaCl and substitute ocean water are 18 g/m2/h and 16 g/m2/h, respectively. In addition, by removing 1 g of NaCl, 67 mWh of electric energy is generated. This proof-of-concept work shows the high application potential for sustainable fuel-cell desalination (FCD) using hydrogen as an energy carrier.
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    Ionophobicity of carbon sub-nanometer pores enables efficient desalination at high salinity
    (Maryland Heights, MO : Cell Press, 2022) Zhang, Yuan; Prehal, Christian; Jiang, Huili; Liu, Yang; Feng, Guang; Presser, Volker
    Electrochemical seawater desalination has drawn significant attention as an energy-efficient technique to address the global issue of water remediation. Microporous carbons, that is, carbons with pore sizes smaller than 2 nm, are commonly used for capacitive deionization. However, micropores are ineffective for capacitive deionization at high molar strength because of their inability to permselectively uptake ions. In our work, we combine experimental work with molecular dynamics simulation and reveal the ability of sub-nanometer pores (ultramicropores) to effectively desalinate aqueous media at seawater-like molar strength. This is done without any ion-exchange membrane. The desalination capacity in 600 mM reaches 12 mg/g, with a charge efficiency of 94% and high cycling stability over 200 cycles (97% of charge efficiency retention). Using molecular dynamic simulations and providing experimental data, our work makes it possible both to understand and to calculate desalination capacity and charge efficiency at high molar strength as a function of pore size.
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    Percolation of rigid fractal carbon black aggregates
    (Melville, NY : American Institute of Physics, 2021) Coupette, Fabian; Zhang, Long; Kuttich, Björn; Chumakov, Andrei; Roth, Stephan V.; González-García, Lola; Kraus, Tobias; Schilling, Tanja
    We examine network formation and percolation of carbon black by means of Monte Carlo simulations and experiments. In the simulation, we model carbon black by rigid aggregates of impenetrable spheres, which we obtain by diffusion-limited aggregation. To determine the input parameters for the simulation, we experimentally characterize the micro-structure and size distribution of carbon black aggregates. We then simulate suspensions of aggregates and determine the percolation threshold as a function of the aggregate size distribution. We observe a quasi-universal relation between the percolation threshold and a weighted average radius of gyration of the aggregate ensemble. Higher order moments of the size distribution do not have an effect on the percolation threshold. We conclude further that the concentration of large carbon black aggregates has a stronger influence on the percolation threshold than the concentration of small aggregates. In the experiment, we disperse the carbon black in a polymer matrix and measure the conductivity of the composite. We successfully test the hypotheses drawn from simulation by comparing composites prepared with the same type of carbon black before and after ball milling, i.e., on changing only the distribution of aggregate sizes in the composites.
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    Spot profile analysis and lifetime mapping in ultrafast electron diffraction: Lattice excitation of self-organized Ge nanostructures on Si(001)
    (Melville, NY : AIP Publishing LLC, 2015) Frigge, T.; Hafke, B.; Tinnemann, V.; Witte, T.; Horn-von Hoegen, M.
    Ultrafast high energy electron diffraction in reflection geometry is employed to study the structural dynamics of self-organized Germanium hut-, dome-, and relaxed clusters on Si(001) upon femtosecond laser excitation. Utilizing the difference in size and strain state the response of hut- and dome clusters can be distinguished by a transient spot profile analysis. Surface diffraction from {105}-type facets provide exclusive information on hut clusters. A pixel-by-pixel analysis of the dynamics of the entire diffraction pattern gives time constants of 40, 160, and 390 ps, which are assigned to the cooling time constants for hut-, dome-, and relaxed clusters.
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    Design of high-performance antimony/MXene hybrid electrodes for sodium-ion batteries
    (London [u.a.] : RSC, 2022) Arnold, Stefanie; Gentile, Antonio; Li, Yunjie; Wang, Qingsong; Marchionna, Stefano; Ruffo, Riccardo; Presser, Volker
    Due to their versatile properties and excellent electrical conductivity, MXenes have become attractive materials for alkali metal-ion batteries. However, as the capacity is limited to lower values due to the intercalation mechanism, these materials can hardly keep up in the ever-fast-growing community of battery research. Antimony has a promisingly high theoretical sodiation capacity characterized by an alloying reaction. The main drawback of this type of battery material is related to the high volume changes during cycling, often leading to electrode cracking and pulverization, resulting in poor electrochemical performance. A synergistic effect of combing antimony and MXene can be expected to obtain an optimized electrochemical system to overcome capacity fading of antimony while taking advantage of MXene charge storage ability. In this work, variation of the synthesis parameters and material design strategy have been dedicated to achieving the optimized antimony/MXene hybrid electrodes for high-performance sodium-ion batteries. The optimized performance does not align with the highest amount of antimony, the smallest nanoparticles, or the largest interlayer distance of MXene but with the most homogeneous distribution of antimony and MXene while both components remain electrochemically addressable. As a result, the electrode with 40 mass% MXene, not previously expanded, etched with 5 mass% HF and 60% antimony synthesized on the surfaces of MXene emerged as the best electrode. We obtained a high reversible capacity of 450 mA h g−1 at 0.1 A g−1 with a capacity retention of around 96% after 100 cycles with this hybrid material. Besides the successful cycling stability, this material also exhibits high rate capability with a capacity of 365 mA h g−1 at 4 A g−1. In situ XRD measurements and post mortem analysis were used to investigate the reaction mechanism.
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    On the geometric stability of an inorganic nanowire and an organic ligand shell
    (Amsterdam [u.a.] : Elsevier Science, 2019) Bettscheider, Simon; Kraus, Tobias; Fleck, NormanA.
    The break-up of a nanowire with an organic ligand shell into discrete droplets is analysed in terms of the Rayleigh-Plateau instability. Explicit account is taken of the effect of the organic ligand shell upon the energetics and kinetics of surface diffusion in the wire. Both an initial perturbation analysis and a full numerical analysis of the evolution in wire morphology are conducted, and the governing non-dimensional groups are identified. The perturbation analysis is remarkably accurate in obtaining the main features of the instability, including the pinch-off time and the resulting diameter of the droplets. It is conjectured that the surface energy of the wire and surrounding organic shell depends upon both the mean and deviatoric invariants of the curvature tensor. Such a behaviour allows for the possibility of a stable nanowire such that the Rayleigh-Plateau instability is not energetically favourable. A stability map illustrates this. Maps are also constructed for the final droplet size and pinch-off time as a function of two non-dimensional groups that characterise the energetics and kinetics of diffusion in the presence of the organic shell. These maps can guide future experimental activity on the stabilisation of nanowires by organic ligand shells. © 2018 The Authors
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    Niobium carbide nanofibers as a versatile precursor for high power supercapacitor and high energy battery electrodes
    (London [u.a.] : RSC, 2016) Tolosa, Aura; Krüner, Benjamin; Fleischmann, Simon; Jäckel, Nicolas; Zeiger, Marco; Aslan, Mesut; Grobelsek, Ingrid; Presser, Volker
    This study presents electrospun niobium carbide/carbon (NbC/C) hybrid nanofibers, with an average diameter of 69 ± 30 nm, as a facile precursor to derive either highly nanoporous niobium carbide-derived carbon (NbC–CDC) fibers for supercapacitor applications or niobium pentoxide/carbon (Nb2O5/C) hybrid fibers for battery-like energy storage. In all cases, the electrodes consist of binder-free and free-standing nanofiber mats that can be used without further conductive additives. Chlorine gas treatment conformally transforms NbC nanofiber mats into NbC–CDC fibers with a specific surface area of 1508 m2 g−1. These nanofibers show a maximum specific energy of 19.5 W h kg−1 at low power and 7.6 W h kg−1 at a high specific power of 30 kW kg−1 in an organic electrolyte. CO2 treatment transforms NbC into T-Nb2O5/C hybrid nanofiber mats that provide a maximum capacity of 156 mA h g−1. The presence of graphitic carbon in the hybrid nanofibers enabled high power handling, maintaining 50% of the initial energy storage capacity at a high rate of 10 A g−1 (64 C-rate). When benchmarked for an asymmetric full-cell, a maximum specific energy of 86 W h kg−1 was obtained. The high specific power for both systems, NbC–CDC and T-Nb2O5/C, resulted from the excellent charge propagation in the continuous nanofiber network and the high graphitization of the carbon structure.