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Herein, we demonstrate digital microfluidics-like manipulations of preconcentrated biomolecule plugs within a continuous flow that is different from the commonly known digital microfluidics involving discrete ( i.e. droplets) media. This is realized using one- and two-dimensional arrays of individually addressable ion-permselective membranes with interconnecting microfluidic channels. The location of powered electrodes, dictates which of the membranes are active and generates either enrichment/depletion diffusion layers, which, in turn, control the location of the preconcentrated plug. An array of such powered membranes enables formation of multiple preconcentrated plugs of the same biosample as well as of preconcentrated plugs of multiple biosample types introduced via different inlets in a selective manner. Moreover, digital-microfluidics operations such as up-down and left-right translation, merging, and splitting, can be realized, but on preconcentrated biomolecule plugs instead of on discrete droplets. This technology, based on nanoscale electrokinetics of ion transport through permselective medium, opens future opportunities for smart and programmable digital-like manipulations of preconcentrated biological particle plugs for various on-chip biological applications.

Nanofluidic diodes are capable of rectifying the electrical current by several orders of magnitude. In the current state of affairs, determining the rectification factor is not possible as it depends on many system parameters. In this work, we systematically scan the effects of geometry and excess counterion concentrations (i.e., surface charge effects). We show that the current-voltage response varies between the two extreme behaviors of unipolar and bipolar responses. The exact behavior depends on the geometry and surface charge properties of the system. Here, we have gone beyond the typical setup that only considers the dynamics within the nanochannel itself and we have included the effects of the adjoining microchannels. Systems that include both nanochannels and microchannels exhibit the classical signatures of concentration polarization, such as ionic depletion and enrichment. Here, where we have scanned a wide range of parameters, we show that bipolar and semi-bipolar systems exhibit a wider range of phenomena that are intrinsically more complicated. Our system characterization is for both, the much more investigated case of steady state and the less investigated, but equally interesting, time-transient case. For example, it is common to characterize the system by its steady-state result (current-voltage response, rectification factor, and transport number). Here, we demonstrate that the time-transient behavior of the fluxes can also be used to characterize the system, and that the time-dependent rectification factors and transport numbers are meaningful. The systematic approach taken in this work, and the results presented herein, can be used to further elucidate the complicated behavior of the current-voltage response of nanofluidic diodes and to rationalize experimental results. The insights of this work can be used to enhance and improve the design of all nanofluidic diodes.

Ionic concentration-polarization (CP)-based biomolecule preconcentration is an established method for enhancing the detection sensitivity of target biomolecules. However, the formed preconcentrated biomolecule plug rapidly sweeps over the surface-immobilized antibodies, resulting in a short-term overlap between the capture agent and the analyte, and subsequently suboptimal binding. To overcome this, we designed a setup allowing for the periodic formation of a preconcentrated biomolecule plug by activating the CP for predetermined on/off intervals. This work demonstrated the feasibility of cyclic CP actuation and optimized the sweeping conditions required to obtain the maximum retention time of a preconcentrated plug over a desired sensing region and enhanced detection sensitivity. The ability of this method to efficiently preconcentrate different analytes and to successfully increase immunoassay sensitivity underscore its potential in immunoassays serving the clinical and food testing industries.

Presented is a novel flow sensor based on electrochemical sensing of the ionic concentration-polarization (CP) layer developed within a microchannel-ion permselective membrane device. To demonstrate the working principle of the electrochemical flow sensor, the effect of advection on the transient and steady-state ionic concentration-polarization (CP) phenomenon in microchannel-Nafion membrane systems is studied. In particular, we focused on the local impedance, measured using an array of electrode pairs embedded at the bottom of the microchannel, as well as the total current across the permselective medium, as two approaches for estimating the flow. We examined both a stepwise application of CP under steady-state flow and a stepwise application of flow under steady-state CP.

We investigate the development of electro-osmotic (Teorell) oscillations at a weakly charged microporous membrane without a preimposed transmembrane electrolyte concentration drop. This drop, necessary for the occurrence of oscillations, develops spontaneously as a result of concentration polarization in the solution layers adjacent to the membrane. A three-layer model comprising a membrane flanked by two diffusion layers is proposed and analyzed for galvano- and potentiostatic regimes of operation.

In this paper, the variation of permselectivity in the course of concentration polarization is systematically analyzed for a three-layer membrane system consisting of a nonperfectly permselective ion exchange membrane, homogeneous or heterogeneous, flanked by two diffusion layers of a binary univalent electrolyte. For a heterogeneous membrane, an ionic transport model is proposed, which is amenable to analytical treatment. In this model, assuming a constant fixed charge in the membrane and disregarding water splitting, the entire transport problem is reduced to solution of a single algebraic equation for the counterion transport number. It is concluded that for both types of membrane the concentration polarization may significantly affect the permselectivity of the system through the effects of the induced nonuniformity of the coion diffusion flux in the membrane (convexity of the coion concentration profile) and varying membrane-solution interface concentration. While the former is significant for low membrane fixed charge density, for a heterogeneous membrane, the latter might be considerably affected by the flux focusing effect at the permeable membrane segments.