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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
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.
Rhodamine 6G and 800 intermolecular heteroaggregates embedded in PMMA for near-infrared wavelength shifting
The opto-electronic properties of small-molecules and functional dyes usually differ when incorporated into solid matrices with respect to their isolated form due to an aggregation phenomenon that alters their optical and fluorescent properties. These spectroscopic modifications are studied in the framework of the exciton theory of aggregates, which has been extensively applied in the literature for the study of molecular aggregates of the same type of molecules (homoaggregation). Despite the demonstrated potential of the control of the heteroaggregation process (aggregation of different types of molecules), most of the reported works are devoted to intramolecular aggregates, complex molecules formed by several chromophores attached by organic linkers. The intramolecular aggregates are specifically designed to hold a certain molecular structure that, on the basis of the exciton theory, modifies their optical and fluorescent properties with respect to the isolated chromophores that form the molecule. The present article describes in detail the incorporation of Rhodamine 6G (Rh6G) and 800 (Rh800) into polymeric matrices of poly-(methyl methacrylate), PMMA. The simultaneous incorporation of both dyes results in an enhanced fluorescent emission in the near-infrared (NIR), originating from the formation of ground-state Rh6G–Rh800 intermolecular heteroaggregates. The systematic control of the concentration of both rhodamines provides a model system for the elucidation of the heteroaggregate formation. The efficient energy transfer between Rh6G and Rh800 molecules can be used as wavelength shifters to convert effectively the light from visible to NIR, a very convenient wavelength range for many practical applications which make use of inexpensive commercial detectors and systems.
Ionophobicity of carbon sub-nanometer pores enables efficient desalination at high salinity
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.
Interacting particles in an activity landscape
We study interacting active Brownian particles (ABPs) with a space-dependent swim velocity via simulation and theory. We find that, although an equation of state exists, a mechanical equilibrium does not apply to ABPs in activity landscapes. The pressure imbalance originates in the flux of polar order and the gradient of swim velocity across the interface between regions of different activity. An active-passive patch system is mainly controlled by the smallest global density for which the passive patch can be close packed. Below this density a critical point does not exist and the system splits continuously into a dense passive and a dilute active phase with increasing activity. Above this density and for sufficiently high activity the active phase may start to phase separate into a gas and a liquid phase caused by the same mechanism as motility-induced phase separation of ABPs with a homogeneous swim velocity.
Design of high-performance antimony/MXene hybrid electrodes for sodium-ion batteries
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.
Analytical and numerical results for the elasticity and adhesion of elastic films with arbitrary Poisson’s ratio and confinement
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.