Inherently aligned microfluidic electrodes composed of liquid metal

This paper describes the fabrication and characterization of microelectrodes that are inherently aligned with microfluidic channels and in direct contact with the fluid in the channels. Injecting low melting point alloys, such as eutectic gallium indium (EGaIn), into microchannels at room temperature (or just above room temperature) offers a simple way to fabricate microelectrodes. The channels that define the shape and position of the microelectrodes are fabricated simultaneously with other microfluidic channels (i.e., those used to manipulate fluids) in a single step; consequently, all of the components are inherently aligned. In contrast, conventional techniques require multiple fabrication steps and registration (i.e., alignment of the electrodes with the microfluidic channels), which are technically challenging. The distinguishing characteristic of this work is that the electrodes are in direct contact with the fluid in the microfluidic channel, which is useful for a number of applications such as electrophoresis. Periodic posts between the microelectrodes and the microfluidic channel prevent the liquid metal from entering the microfluidic channel during injection. A thin oxide skin that forms rapidly and spontaneously on the surface of the metal stabilizes mechanically the otherwise low viscosity, high surface tension fluid within the channel. Moreover, the injected electrodes vertically span the sidewalls of the channel, which allows for the application of uniform electric field lines throughout the height of the channel and perpendicular to the direction of flow. The electrodes are mechanically stable over operating conditions commonly used in microfluidic applications; the mechanical stability depends on the magnitude of the applied bias, the nature of the bias (DC vs. AC), and the conductivity of the solutions in the microfluidic channel. Electrodes formed using alloys with melting points above room temperature ensure mechanical stability over all of the conditions explored. As a demonstration of their utility, the fluidic electrodes are used for electrohydrodynamic mixing, which requires extremely high electric fields (~10(5) V m(-1)).     

Separation of erythrocytes and latex beads by dielectrophoretic levitation and hyperlayer field-flow fractionation.

A model system consisting of a mixture of latex beads and erythrocytes has been investigated to demonstrate the practical feasibility of particle separation by means of the combined application of negative dielectrophoresis and hyperlayer field-flow fractionation. The dielectrophoretic levitation of latex beads is demonstrated by energizing interdigitated electrodes, of widths and separation ranging from 5 to 40 μm, with AC signals of 0–10 V (rms) in the frequency range 1 kHz–10 MHz. Maximum levitation was attained at 1 MHz, at which frequency levitation is relatively independent of the suspending medium conductivity. Levitation was also independent of particle size, but dependent on particle density and dielectric properties. At 1 MHz the erythrocytes were attracted to the electrodes by positive dielectrophoresis, and so could be separated from the latex beads by fluid flow. The electric field and field gradient above the electrodes were also computer modelled, and this information was used to design the electrode and chamber geometries for optimum DEP-field-flow fractionation.     

AC electrokinetic immobilization of influenza virus

The use of alternating current (AC) electrokinetic forces, like dielectrophoresis and AC electroosmosis, as a simple and fast method to immobilize sub-micrometer objects onto nanoelectrode arrays is presented. Due to its medical relevance, the influenza virus is chosen as a model organism. One of the outstanding features is that the immobilization of viral material to the electrodes can be achieved permanently, allowing subsequent handling independently from the electrical setup. Thus, by using merely electric fields, we demonstrate that the need of prior chemical surface modification could become obsolete. The accumulation of viral material over time is observed by fluorescence microscopy. The influences of side effects like electrothermal fluid flow, causing a fluid motion above the electrodes and causing an intensity gradient within the electrode array, are discussed. Due to the improved resolution by combining fluorescence microscopy with deconvolution, it is shown that the viral material is mainly drawn to the electrode edge and to a lesser extent to the electrode surface. Finally, areas of application for this functionalization technique are presented.     

Design and evaluation of a Dean vortex-based micromixer

A mixer, based on the Dean vortex, is fabricated and tested in an on-chip format. When fluid is directed around a curve under pressure driven flow, the high velocity streams in the center of the channel experience a greater centripetal force and so are deflected outward. This creates a pair of counter-rotating vortices moving fluid toward the inner wall at the top and bottom of the channel and toward the outer wall in the center. For the geometries studied, the vortices were first seen at Reynolds numbers between 1 and 10 and became stronger as the flow velocity is increased. Vortex formation was monitored in channels with depth/width ratios of 0.5, 1.0, and 2.0. The lowest aspect ratio strongly suppressed vortex formation. Increasing the aspect ratio above 1 appeared to provide improved mixing. This design has the advantages of easy fabrication and low surface area.     

Microfluidic flow transducer based on the measurement of electrical admittance

A new flow transducer for measuring the flow rate of a conducting fluid in a microchannel is reported. In this paper, the measure of flow of such fluid under laminar flow conditions based on the change of electrical admittance is established with the aid of a pair of electrodes parallel to the line of flow in a glass-PDMS microfluidic device. This flow sensor is simple in design and can be integrated to most of the microfluidic platforms. The effect of flow rate of the electrolyte, the frequency of the applied ac voltage, the voltage applied across the detector electrodes, and the conductivity of the electrolyte are varied to optimize for high sensitivity. The optimized values are then used to demonstrate the measurements of very low flow rates (<1 nL s(-1)). This flow sensor can be extended towards the measurement of chemical and biochemical buffers and reagents.     

Continuous concentration of bacteria in a microfluidic flow cell using electrokinetic techniques

A novel method for the concentration of bacterial solutions is presented that implements electrokinetic techniques, zone electrophoresis (ZE) and isoelectric focusing (IEF), in a microfluidic device. The method requires low power (< 3e-5 W) and can be performed continuously on a flowing stream. The device consists of two palladium electrodes held in a flow cell constructed from layers of polymeric film held together by a pressure-sensitive adhesive. Both ZE and IEF are performed with carrier-free solutions in devices in which the electrodes are in intimate contact with the sample fluid. IEF experiments were performed using natural pH gradients; no carrier ampholyte solution was required. Experiments performed in buffer alone resulted in significant electroosmotic flow. Pretreatment of the sample chamber with bleach followed by a concentrated solution of cationic detergent effectively suppressed electroosmotic flow.     

HBF4溶液中全铅液流电池

报道了一种HBF₄水溶液中的全铅液流电池,正、负电极电解液均采用Pb（BF₄）₂的HBF₄水溶液.在酸性的四氟硼酸铅电解液中考察了石墨电极和玻碳电极作为工作电极的循环伏安性能,石墨电极较适于用作全铅液流电池的正、负电极.采用石墨电极作为电池的正、负电极并在四氟硼酸铅酸性电解液中进行充放电实验,其中Pb（BF₄）₂浓度分别为0.5、1.0和1.5 mol·L^-1,且保持游离的HBF₄浓度为1.0 mol·L^-1.该电池为单液流电池,不需要隔膜分隔正、负极的电解液,电流密度为10、20和40 mA.cm^-2,当限定充电容量为7.0 mAh.cm^-2,放电电压截止到1.0 V时,平均库仑效率大于87%,平均能量效率大于68%;当电解液采用1.0或1.5 mol·L^-1 Pb（BF₄）₂+1.0 mol·L^-1HBF₄水溶液时,在10及20 mA.cm^-2电流下的能量效率最高可超过74%.     

A multifunctional micro-fluidic system for dielectrophoretic concentration coupled with immuno-capture of low numbers of Listeria monocytogenes

In this study, we demonstrated a micro-fluidic system with multiple functions, including concentration of bacteria using dielectrophoresis (DEP) and selective capture using antibody recognition, resulting in a high capture efficiency of bacterial cells. The device consisted of an array of oxide covered interdigitated electrodes on a flat silicon substrate and a approximately 16 microm high and approximately 260 microm wide micro-channel within a PDMS cover. For selective capture of Listeria monocytogenes from the samples, the channel surface was functionalized with a biotinylated BSA-streptavidin-biotinylated monoclonal antibody sandwich structure. Positive DEP (at 20 V(pp) and 1 MHz) was used to concentrate bacterial cells from the fluid flow. DEP could collect approximately 90% of the cells in a continuous flow at a flow rate of 0.2 microl min(-1) into the micro-channel with concentration factors between 10(2)-10(3), in sample volumes of 5-20 microl. A high flow rate of 0.6 microl min(-1) reduced the DEP capture efficiency to approximately 65%. Positive DEP attracts cells to the edges of the electrodes where the field gradient is the highest. Cells concentrated by DEP were captured by the antibodies immobilized on the channel surface with efficiencies of 18 to 27% with bacterial cell numbers ranging from 10(1) to 10(3) cells. It was found that DEP operation in our experiments did not cause any irreversible damage to bacterial cells in terms of cell viability. In addition, increased antigen expression (antigens to C11E9 monoclonal antibody) on cell membranes was observed following the exposure to DEP.     

Electrically induced colloidal clusters for generating shear mixing and visualizing flow in microchannels

When aqueous suspensions of 1 μm, negatively charged polystyrene particles are subject to a 1 kHz alternating electric field of strength greater than 7 kV(rms) m(-1), dynamic elliptical clusters of particles spontaneously form. With potential applications in microchannel fluidics in mind, we characterize how cluster formation and particle circulation, driven by induced dipole-dipole interactions, is critically dependent on time, field strength, electrolyte concentration, and cell thickness. Logarithmic growth of cluster size is observed, and particle velocity within the clusters is found to be proportional to cluster length. Increasing cell thickness from 10 to 60 μm increases the projected cluster area but decreases cluster aspect ratio as the result of changing particle dispersal rates. Clusters are shown to generate significant fluid shear suitable for microchannel mixing applications. These clusters are observed to distort under transverse fluid flow and, above a critical flow rate, to undergo a transition to form regularly spaced particle streams, which may be suitable for two-dimensional visualization of fluid flow.     

Potentiometric batch and flow injection analysis of betaine hydrochloride

Novel PVC membrane electrodes for the determination of betaine ion based on the formation of betaine-tetraphenylborate (Be-TPB) and betaine-phosphotungstate (Be-PT) ion-exchangers as electroactive materials are described. The sensors show a fast, stable, near Nernstian response for 6.92 x 10(-6) to 7.94 x 10(-3) M and 1.0 x 10(-4) to 1.0 x 10(-2) M betaine hydrochloride (Be.Cl) in case of Be-TPB electrode applying batch and flow injection analysis (FIA), respectively, and 2.95 x 10(-5) to 2.26 x 10(-3) M and 3.16 x 10(-5) to 1.0 x 10(-2) M in case of Be-PT electrode for batch and FIA electrodes, respectively, at 25 degrees C over the pH range of 3.5-10 with a cationic slope of 60.2 and 59.1 mV decade(-1) and a fast potential response of < or =15 s. The lower detection limits are 7.94 x 10(-6) and 3.18 x 10(-5) M Be.Cl for Be-TPB and Be-PT electrodes, respectively. Selectivity coefficient data for some common inorganic cations, sugars, amino acids and the components other than betaine, of the mixed drug investigated show negligible interference. The electrodes have been applied to the direct potentiometric determination of betaine hydrochloride in water and in a pharmaceutical preparation under batch and FIA conditions. Potentiometric titrations of Be.Cl with NaTPB and PTA as titrants were monitored with the developed betaine electrodes as an end point indicator electrode. The determination of Be.Cl shows an average recovery of 100.8% with mean relative standard deviation of 0.61%. The effect of temperature on the electrodes was also studied.     

Modulation of electroosmotic flow by neutral polymers

Polymer coating is widely used to modulate the fluid flow in micro- and nanometer pores and flows that are sensitive to surface properties such as electroosmotic flow. Here we report on the dissipative particle dynamics simulations of the modulation of electroosmotic flow by neutral polymers. In these coarse-grained simulations, fluid and polymers are resolved at a scale comparable to polymer size and the two-way coupling between polymer conformation and fluid flow are explicitly accounted for. The simulations indicate that, in the parameter space explored, the screening of electroosmotic flow by polymers decreases nonlinearly as the external electric field increases. Such an observation is understood by analyzing the surface coverage by polymers, height and orientation of the grafted polymers, and the two different modes of flow screening by polymer segments as a function of the external electric field. Understanding the effects and interplay of these physical processes is crucial for the rational design of polymer coating for flow control in microfluidic and nanofluidic systems.     

用电容平面图研究金／十八硫醇单分子膜的自组装过程和缺陷情况

推导了电化学体系中理想极化电极、电化学极化电极的复数电容表达式。根据这些表达式分析了上述体系的电容平面图 (Capacitance Plane Plot,CPP) ,利用 CPP可以方便地监测体系的电容值。用电子元件组成了上述体系的等效电路 ,测定了交流阻抗谱 ,得到了 CPP与理论推导一致。研究了金 /十八硫醇自组装膜的 CPP,根据 CPP讨论了金 /硫醇膜的组装过程及缺陷和组装时间的关系。     

Simple lab-on-chip approach with time-based detection

A simple lab-on-chip approach with time-based detection is proposed. A platform is made from a piece of acrylic differently shaped channels for introducing sample and reagent(s) using flow manipulation. Time-based changes involving migration of the reaction zone are monitored. The changes can be visually monitored by using a stop-watch with naked eyes observation. Some applications for the determination of ascorbic acid, acetic acid and iron in real samples with different chemistries were demonstrated.     

Electrohydrodynamic flow and colloidal patterning near inhomogeneities on electrodes

Current density inhomogeneities on electrodes (of physical, chemical, or optical origin) induce long-range electrohydrodynamic fluid motion directed toward the regions of higher current density. Here, we analyze the flow and its implications for the orderly arrangement of colloidal particles as effected by this flow on patterned electrodes. A scaling analysis indicates that the flow velocity is proportional to the product of the applied voltage and the difference in current density between adjacent regions on the electrode. Exact analytical solutions for the streamlines are derived for the case of a spatially periodic perturbation in current density along the electrode. Particularly simple asymptotic expressions are obtained in the limits of thin double layers and either large or small perturbation wavelengths. Calculations of the streamlines are in good agreement with particle velocimetry experiments near a mechanically generated inhomogeneity (a "scratch") that generates a current density larger than that of the unmodified electrode. We demonstrate that proper placement of scratches on an electrode yields desired patterns of colloidal particles.     

Experimental investigation of the flow induced by artificial cilia

The fluid transport produced by rectangular shaped, magnetically actuated artificial cilia of 70 μm length and 20 μm width was determined by means of phase-locked Micro Particle Image Velocimetry (μPIV) measurements in a closed microfluidic chamber. The phase-averaged flow produced by the artificial cilia reached up to 130 μm s(-1) with an actuation cycle frequency of 10 Hz. Analysis of the measured flow data indicate that the present system is capable of achieving volume flow rates of V[combining dot above](cilia) = 14 ± 4 μl min(-1) in a micro channel of 0.5 × 5 mm(2) cross-sectional area when no back pressure is built up. This corresponds to an effective pressure gradient of 6 ± 1 Pa m(-1), which equals a pressure difference of 0.6 ± 0.1 mPa over a distance of 100 μm between two rows of cilia. These results were derived analytically from the measured velocity profile by treating the cilia as a thin boundary layer. While the cilia produce phase-averaged velocities of the order of O(10(2)μm s(-1)), time-resolved measurements showed that the flow field reverses two times during one actuation cycle inducing instantaneous velocities of up to approximately 2 mm s(-1). This shows that the flow field is dominated by fluid oscillations and flow rates are expected to increase if the beating motion of the cilia is further improved.     

Mapping alternating current electroosmotic flow at the dielectrophoresis crossover frequency of a colloidal probe

AC electroosmotic (ACEO) flow above the gap between coplanar electrodes is mapped by the measurement of Stokes forces on an optically trapped polystyrene colloidal particle. E²‐dependent forces on the probe particle are selected by amplitude modulation (AM) of the ACEO electric field (E) and lock‐in detection at twice the AM frequency. E²‐dependent DEP of the probe is eliminated by driving the ACEO at the probe's DEP crossover frequency. The location‐independent DEP crossover frequency is determined, in a separate experiment, as the limiting frequency of zero horizontal force as the probe is moved toward the midpoint between the electrodes. The ACEO velocity field, uncoupled from probe DEP effects, was mapped in the region 1–9 μm above a 28 μm gap between the electrodes. By use of variously sized probes, each at its DEP crossover frequency, the frequency dependence of the ACEO flow was determined at a point 3 μm above the electrode gap and 4 μm from an electrode tip. At this location the ACEO flow was maximal at ～117 kHz for a low salt solution. This optical trapping method, by eliminating DEP forces on the probe, provides unambiguous mapping of the ACEO velocity field.     

Movement of colloidal particles in two-dimensional electric fields

We characterize the movement of carbon black particles in inhomogeneous, two-dimensional dc electric fields. Motivated by display applications, the particles are suspended in a nonpolar solvent doped with a charge control agent. The two-dimensional fields are generated between strip electrodes on a glass slide spaced 120 microm apart with field strengths up to 10(4) V/m. Such fields are insufficient to drive either electrohydrodynamic instabilities or natural convection due to ohmic heating, but they move the particles between the electrodes in about 30 s. In the center region between the strip electrodes, the particles move by electrophoresis; that is, the particle velocity is proportional to the electric field. However, when imposing a constant-potential or constant-current boundary condition at the electrodes to derive the electrical field, the electrophoretic mobility calculated from the measured particle velocities is outside the range of mobilities predicted from the theory of O'Brien and White. Near the electrodes the particles either speed up or slow down, depending on the polarity of the electrode, and these changes in velocity cannot be explained simply by electrophoresis in a spatially varying electric field. We suggest that this anomalous motion arises from electrohydrodynamic flows originating from the interaction between the space charge of the polarized layers above the electrodes and the electric field. Approximate calculations indicate such flows could be sufficiently strong to explain the anomalous trajectories near the edges of the electrodes.     

An automatic and quantitative on-chip cell migration assay using self-assembled monolayers combined with real-time cellular impedance sensing

Cell migration is crucial in many physiological and pathological processes including embryonic development, immune response and cancer metastasis. Traditional methods for cell migration detection such as wound healing assay usually involve physical scraping of a cell monolayer followed by an optical observation of cell movement. However, these methods require hand-operation with low repeatability. Moreover, it's a qualitative observation not a quantitative measurement, which is hard to scale up to a high-throughput manner. In this article, a novel and reliable on-chip cell migration detection method integrating surface chemical modification of gold electrodes using self-assembled monolayers (SAMs) and real-time cellular impedance sensing is presented. The SAMs are used to inhibit cell adherence forming an area devoid of cells, which could effectively mimic wounds in a cell monolayer. After a DC electrical signal was applied, the SAMs were desorbed from the electrodes and cells started to migrate. The process of cell migration was monitored by real-time impedance sensing. This demonstrates the first occurrence of integrating cellular impedance sensing and wound-forming with SAMs, which makes cell migration assay being real-time, quantitative and fully automatic. We believe this method could be used for high-throughput anti-migratory drug screening and drug discovery.     

A flow‐through column electrolytic cell for supercritical fluid chromatography*

A novel flow‐through column electrolytic cell was proposed as a detector to obtain current signals for supercritical fluid chromatography. The electrochemical cell consisted of two electrodes and its holder, and a working and a counter electrode were fabricated from 192 carbon strings, which were composed of 400 carbon fibers of 10 μm in diameter filled into a heat‐shrinkable tube. These electrodes were placed in the center of a holder made from polyether ether ketone blocks and they were separated by polytetrafluoroethylene membrane filters. To evaluate the sensitivity of this cell, a standard solution of ferrocene was injected into the supercritical fluid chromatography system connected to the electrolytic cell. The ferrocene was eluted through a silica gel column using a mixture of a mobile phase of supercritical CO₂ and a modifier of methanol containing ammonium acetate. The current peak area of ferrocene correlated to the ferrocene concentration in the range of 10–400 μmol/L (r  = 0.999). Moreover, the limit of detection on the column estimated from a signal‐to‐noise ratio of 3 was 9.8  × 10⁻¹³ mol.