An ion-exchange-resin-based microfluidic pump is introduced that utilizes trace amounts of ions to generate fluid flows. We show experimentally that our pump operates in almost deionized water for periods exceeding 24 h and induces fluid flows of μm s over hundreds of μm. This flow displays a far-field, power-law decay which is characteristic of two-dimensional (2D) flow when the system is strongly confined and of three-dimensional (3D) flow when it is not. Using theory and numerical calculations we demonstrate that our observations are consistent with electroosmotic pumping driven by μmol L ion concentrations in the sample cell that serve as 'fuel' to the pump. Our study thus reveals that trace amounts of charge carriers can produce surprisingly strong fluid flows; an insight that should benefit the design of a new class of microfluidic pumps that operate at very low fuel concentrations.

We develop a double mean-field theory for charged macrogels immersed in electrolyte solutions in the spirit of the cell model approach.We first demonstrate that the equilibrium sampling of a single explicit coarse-grained charged polymer in a cell yields accurate predictions of the swelling equilibrium if the geometry is suitably chosen and all pressure contributions have been incorporated accurately. We then replace the explicit flexible chain by a suitably modeled penetrable charged rod that allows to compute all pressure terms within the Poisson-Boltzmann approximation. This model, albeit computationally cheap, yields excellent predictions of swelling equilibria under varying chain length, polymer charge fraction, and external reservoir salt concentrations when compared to coarse-grained molecular dynamics simulations of charged macrogels. We present an extension of the model to the experimentally relevant cases of pH-sensitive gels. arXiv:1905.04960v1 [cond-mat.soft]Polyelectrolyte gels consist of crosslinked charged polymers (polyelectrolytes) that can be synthesized with various topologies and are produced in sizes ranging from nanometers (nanogels) up to centimeters (macrogels) [1,2]. They show a large, reversible uptake of water that is exploited in numerous dailylife products, such as in superabsorbers, cosmetics, pharmaceuticals [3,4,5], agriculture [6,7], or quite recently water desalination [8,9]. Tailoring polyelectrolyte gels to their applications requires a sufficiently accurate prediction of their swelling capabilities and elastic responses, a task that still goes beyond analytical approaches [10,11,12,13,14,15,16,17,18]. So far only all-atom simulations of short single chains in the bulk (not of whole hydrogels) with explicit water have been performed [19,20,21,22]. On the other hand, coarse-grained polyelectrolyte network models have demonstrated their ability to amend analytical approaches, showing that structural microscopic details can have noticeable effects on the macroscopic properties such as the swelling [23,24,25,26,27,28,29,30,31,32]. Macroscopic gels with monodisperse chain length can be simulated with microscopic detail using molecular dynamics (MD) simulations with periodic boundary conditions (PBCs) (cf. periodic gel model ) where a unit gel section is connected periodically to yield an infinite gel without boundaries. However, even MD simulations of periodic gels remain computationally very expensive due to the many particles and the slow relaxation times of the involved polymers. Thus, the development of computationally efficient mean-field models capable of predicting swelling equilibria have been of scientific interest in the last years [33,15,31,32]. First ideas of using a Poisson-Boltzmann (PB) cell model under tension were put forward by Mann for salt-free gels, with moderate success [33].About sixty years ago Katchalsky and Michaeli [11] suggested a free energy model that has recently been shown to predict swelling equilibria reasonably well [31] when compared to MD simulat...

We consider the efficiency of self-phoretic colloidal particles (swimmers) as a function of the heterogeneity in the surface reaction rate. The set of fluid, species, and electrostatic continuity equations is solved analytically using a linearization and numerically using a finite-element method. To compare spherical swimmers of different size and with heterogeneous catalytic conversion rates, a 'swimmer efficiency' functional η is introduced. It is proven, that in order to obtain maximum swimmer efficiency the reactivity has to be localized at the pole(s). Our results also shed light on the sensitivity of the propulsion speed to details of the surface reactivity, a property that is notoriously hard to measure. This insight can be utilized in the design of new self-phoretic swimmers.

Conspectus Active matter concerns itself with the study of particles that convert energy into work, typically motion of the particle itself. This field saw a surge of interest over the past decade, after the first micrometer-sized, man-made chemical motors were created. These particles served as a simple model system for studying in a well-controlled manner complex motion and cooperative behavior as known from biology. In addition, they have stimulated new efforts in understanding out-of-equilibrium statistical physics and started a revolution in microtechnology and robotics. Concentrated effort has gone into realizing these ambitions, and yet much remains unknown about the chemical motors themselves. The original designs for self-propelled particles relied on the conversion of the chemical energy of hydrogen peroxide into motion via catalytic decomposition taking place heterogeneously over the surface of the motor. This sets up gradients of chemical fields around the particle, which allow it to autophorese. That is, the interaction between the motor and the heterogeneously distributed solute species can drive fluid flow and the motor itself. There are two basic designs: the first relies on redox reactions taking place between the two sides of a bimetal, for example, a gold–platinum Janus sphere or nanorod. The second uses a catalytic layer of platinum inhomogeneously vapor-deposited onto a nonreactive particle. For convenience’s sake, these can be referred to as redox motors and monometallic half-coated motors, respectively. To date, most researchers continue to rely on variations of these simple, yet elegant designs for their experiments. However, there is ongoing debate on the exact way chemical energy is transduced into motion in these motors. Many of the experimental observations on redox motors were successfully modeled via self-electrophoresis, while for half-coated motors there has been a strong focus on self-diffusiophoresis. Currently, there is mounting evidence that self-electrophoresis provides the dominant contribution to the observed speeds of half-coated motors, even if the vast majority of the reaction products are electroneutral. In this Account, we will summarize the most common electrophoretic propulsion model and discuss its strengths and weaknesses in relation to recent experiments. We will comment on the possible need to go beyond surface reactions and consider the entire medium as an “active fluid” that can create and annihilate charged species. This, together with confinement and collective effects, makes it difficult to gain a detailed understanding of these swimmers. The potentially dominant effect of confinement is highlighted on the basis of a recent study of an electro-osmotic pump that drives fluid along a substrate. Detailed analysis of this system allows for identification of the electro-osmotic driving mechanism, which is powered by micromolar salt concentrations. We will discuss how our latest numerical solver developments, based on the lattice Boltzmann method, should enable us ...

Magnetic composite materials i.e. elastomers, polymer gels, or polymer solutions with embedded magnetic nanoparticles are useful for many technical and bio-medical applications. However, the microscopic details of the coupling mechanisms...

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This contribution provides an overview of the study of soft magnetic materials using particle-based simulation models. We focus in particular on systems where thermal fluctuations are important. As a basis for further discussion, we first describe two-dimensional models which demonstrate two deformation mechanisms of magnetic gels in a homogeneous field. One is based on the change of magnetic interactions between magnetic particles as a response to an external field; the other is the result of magnetically blocked particles acting as cross-linkers. Based on the qualitative behavior directly observable in the two-dimensional models, we extend our description to three-dimensions. We begin with particle-cross-linked gels, as for those, our three-dimensional model also includes explicitly resolved polymer chains. Here, the polymer chains are represented by entropic springs, and the deformation of the gel is the result of the interaction between magnetic particles. We use this model to examine the influence of the magnetic spatial configuration of magnetic particles (uniaxial or isotropic) on the gel’s magnetomechanical behavior. A further part of the article will be dedicated to scale-bridging approaches such as systematic coarse-graining and models located at the boundary between particle-based and continuum modeling. We will conclude our article with a discussion of recent results for modeling time-dependent phenomena in magnetic-polymer composites. The discussion will be focused on a simulation model suitable for obtaining AC-susceptibility spectra for dilute ferrofluids including hydrodynamic interactions. This model will be the basis for studying the signature of particle–polymer coupling in magnetic hybrid materials. In the long run, we aim to compare material properties probed locally via the AC-susceptibility spectra to elastic moduli obtained for the system at a global level.