Electrokinetic Mechanism Research Articles

Self-potential monitoring of a crude oil-contaminated site (Trecate, Italy)

We present a multidisciplinary approach for characterization of a crude oil-contaminated site (Trecate, Italy), integrating geophysical data, such as subsoil electrical potential (in millivolts) and electrical resistivity (in ohm meters) distribution, with hydrogeological and bio-chemical data. Self-potential measurements have been evaluated together with active geoelectrical measurements and hydrological information, to provide spatial and temporal information about the self-potential sources and their possible correlations with the contamination state of the subsoil. Three self-potential surveys (March 2010, October 2010, and March 2011) were conducted at the site, both in the contaminated and uncontaminated regions. The obtained self-potential maps show large time-lapse differences in correspondence of the contaminated area, with positive electrical potential values (up to 50mV) in spring surveys and an electrical potential dipolar distribution in October (2010) survey (amplitude from -15 to 25mV). To understand the origin of the measured self-potential signals, a model using vertical dipolar electrical sources was built, taking into account the electrical resistivity distribution deduced from electrical resistivity tomography. The self-potential source identification allows the Trecate contamination state to be better delineated. In particular, two self-potential contributions are superimposed: the electrokinetic mechanism is predominant in spring, while the redox mechanism represents the most important contribution in autumn.

Rapid (<5 min) Identification of Pathogen in Human Blood by Electrokinetic Concentration and Surface-Enhanced Raman Spectroscopy

This study reports a novel microfluidic platform for rapid and long-ranged concentration of rare-pathogen from human blood for subsequent on-chip surface-enhanced Raman spectroscopy (SERS) identification/discrimination of bacteria based on their detected fingerprints. Using a hybrid electrokinetic mechanism, bacteria can be concentrated at the stagnation area on the SERS-active roughened electrode, while blood cells were excluded away from this region at the center of concentric circular electrodes. This electrokinetic approach performs isolation and concentration of bacteria in about three minutes; the density factor is increased approximately a thousand fold in a local area of ~5000 μm2 from a low bacteria concentration of 5 × 103 CFU/ml. Besides, three genera of bacteria, S. aureus, E. coli, and P. aeruginosa that are found in most of the isolated infections in bacteremia were successfully identified in less than one minute on-chip without the use of any antibody/chemical immobilization and reaction processes.

Numerical analysis of seismoelectric wave propagation in spatially confined geological units

ABSTRACTUsing numerical modelling, we investigate the evolution of seismoelectric effects induced by seismic excitation in spatially confined lithological units. Typical geometries represent clay lenses embedded in an aquifer or petroleum deposits in a host rock. In fluid‐saturated rocks, seismic waves can generate electromagnetic fields due to electrokinetic coupling mechanisms associated with such processes in the vicinity of the fluid‐mineral interface. Two seismoelectric phenomena are investigated: (1) the co‐seismic field associated with the seismic displacement at each point in a subsurface and (2) the interface response generated at layer boundaries. Our modelling uses a simplified time‐domain formulation of the coupled problem and an efficient 2D finite‐element implementation. To gain insight into the morphogenetic field behaviour of the seismoelectric effects, several numerical simulations for various target geometries were treated. Accordingly, we varied both the thickness of the confined units and the value of the electrical bulk conductivity in porous media. Analysis of these effects shows differences between interface responses for electrically conductive versus resistive units. So the pertinent contrast in electrical bulk conductivity controls the shape and structure of these seismoelectric conversion patterns. Moreover, the seismoelectric interface response captures both the petrophysical and geometrical characteristics of the geological unit. These models demonstrate the value of using seismoelectric interface response for reservoir characterization in either hydrogeological or hydrocarbon exploration studies.

Particle Manipulation in Insulator Based Dielectrophoretic Devices1

Microfluidic devices can make a significant impact in many fields where obtaining a rapid response is critical, particularly in analyses involving biological particles, from deoxyribonucleic acid (DNA) and proteins, to cells. Microfluidics has revolutionized the manner in which many different assessments/processes are carried out, since it offers attractive advantages over traditional bench-scale techniques. Some of the advantages are: small sample and reagent amounts, higher resolution and sensitivity, improved level of integration and automation, lower cost and much shorter processing times. There is a growing interest on the development of techniques that can be used in microfluidics devices. Among these, electrokinetic techniques have shown great potential due to their flexibility. Dielectrophoresis (DEP) is an electrokinetic mechanism that refers to the interaction of a dielectric particle with a spatially non-uniform electric field; this leads to particle movement due to polarization effects. DEP offers great potential since it can be carried out employing DC and AC electric fields, and neutral and charged particles can be manipulated. This work is focused on the use of insulator based dielectrophoresis (iDEP), a novel dielectrophoretic mode that employs arrays of insulating structures to generate dielectrophoretic forces. Successful micro and nanoparticles manipulation can be achieved employing iDEP, due to its unique characteristics that allow for great flexibility. In this work, microchannels containing arrays of cylindrical insulating posts were employed to concentrate, sort and separate microparticles. Mathematical modeling with COMSOL® was performed to identify optimal device configuration. Different sets of experiments were carried out employing DC and AC potentials. The results demonstrated that effective and fast particle manipulation is possible by fine tuning dielectrophoretic force and electroosmotic flow.

A mechanistic study of arsenate removal from artificially contaminated clay soils by electrokinetic remediation

Batch desorption experiments and bench-scale electrokinetic experiments were performed to elucidate the electrokinetic remediation mechanisms of arsenate from artificially contaminated kaolinite. The electrokinetic experiments in which a constant voltage was applied demonstrated that high soil pH favored arsenate remediation with respect to both the remediation time and electricity consumption. It was also demonstrated that applying a pulse voltage (1h ON, 1h OFF) significantly improved the electricity consumption efficiency when the soil pH was maintained at the initial value during the experiments; this trend was not observed when the soil pH was gradually increased from the cathode side. These electrokinetic experimental results, with the support of arsenate desorption data obtained from batch experiments, indicate that the remediation rate-limiting step varied with soil pH. When the soil pH was maintained at the initial value of 7.2 during the experiments, arsenate desorption was the remediation rate-limiting step rather than the migration of dissolved arsenate toward the anode. Conversely, when the cathode pH was not controlled and the soil pH was correspondingly increased gradually from the cathode side, the migration of hydroxyl and desorbed arsenate ions toward the anode played a more important role in the control of the overall remediation efficiency.

Electrokinetic properties of the mammalian tectorial membrane

The tectorial membrane (TM) clearly plays a mechanical role in stimulating cochlear sensory receptors, but the presence of fixed charge in TM constituents suggests that electromechanical properties also may be important. Here, we measure the fixed charge density of the TM and show that this density of fixed charge is sufficient to affect mechanical properties and to generate electrokinetic motions. In particular, alternating currents applied to the middle and marginal zones of isolated TM segments evoke motions at audio frequencies (1-1,000 Hz). Electrically evoked motions are nanometer scaled (∼5-900 nm), decrease with increasing stimulus frequency, and scale linearly over a broad range of electric field amplitudes (0.05-20 kV/m). These findings show that the mammalian TM is highly charged and suggest the importance of a unique TM electrokinetic mechanism.

Optoelectrofluidic behavior of metal–polymer hybrid colloidal particles

Behavior of metal–polymer hybrid colloidal particles in an optoelectrofluidic device has been investigated theoretically and experimentally. In the application of hundreds of kHz ac voltage, a variety of optically induced electrokinetic and electrostatic mechanisms affect the movement of gold-coated polystyrene microspheres. The particles repel from the light pattern, and their mobility increases as the amount of gold increases. We apply this model to develop an optoelectrofluidic immunoassay, in which the corresponding metal–polymer hybrid particles are formed by a reaction of antibody-coated gold nanoparticles, antigens, and antibody-coated polystyrene microspheres.

A low sample volume particle separation device with electrokinetic pumping based on circular travelling-wave electroosmosis

Particle separation is a crucial step in sample preparation processes. The preparation of low volume samples is especially important for clinical diagnosis and chemical analysis. The advantages of microfluidic techniques have lead them to become potential candidates for particle separation. However, existing microfluidic devices require external pumping sources and extensive geometric patterns to attain high separation efficiency, which is disadvantageous when handling low volume samples. This paper presents a low sample volume particle separation microfluidic device with low voltage electrokinetic pumping based on circular travelling-wave electroosmosis (TWEO). Computational numerical software was utilized to simulate two electrokinetic mechanisms: circular TWEO and dielectrophoresis (DEP). The circular TWEO shear flow generates a velocity gradient in the radial direction which causes a shear stress-induced force to drag particles into the center region of the device. In contrast, the non-parallel electrodes induce negative DEP forces which push polystyrene beads towards the peripheral regions; the magnitude of the DEP forces are dependent on the sizes of the polystyrene beads. We used particles of various sizes to experimentally prove the concept of particle separation. Our experiments show that 15 μm beads are dragged into the center region due to the shear stress-induced force, and 1 μm beads move towards the outer region because of the large negative DEP force. The results show a separation purity of 94.4% and 80.0% for 15 μm and 1 μm beads respectively. We further demonstrated particle isolation from a sample of containing a small proportion of 6 μm beads mixed with 1 μm beads at a concentration ratio of 1 : 300. Therefore, the innovative device developed in this paper provides a promising solution to allow particle separation in sample volumes as low as 50 nL.

Multiple electrokinetic actuators for feedback control of colloidal crystal size

We report a feedback control method to precisely target the number of colloidal particles in quasi-2D ensembles and their subsequent assembly into crystals in a quadrupole electrode. Our approach relies on tracking the number of particles within a quadrupole electrode, which is used in a real-time feedback control algorithm to dynamically actuate competing electrokinetic transport mechanisms. Particles are removed from the quadrupole using DC-field mediated electrophoretic-electroosmotic transport, while high-frequency AC-field mediated dielectrophoretic transport is used to concentrate and assemble colloidal crystals. Our results show successful control of the size of crystals containing 20 to 250 colloidal particles with less than 10% error. Assembled crystals are characterized by their radius of gyration, crystallinity, and number of edge particles, and demonstrate the expected size-dependent properties. Our findings demonstrate successful ensemble feedback control of the assembly of different sized colloidal crystals using multiple actuators, which has broad implications for control over nano- and micro- scale assembly processes involving colloidal components.

Numerical simulation of molecular uptake via electroporation

A numerical study of electroporation-mediated molecular delivery is presented. The model consists of the Nernst–Planck equations for species transport, coupled with an asymptotic Smoluchowski equation for membrane permeabilization. The transfer of calcium ions into a Chinese Hamster Ovary cell is simulated. The results reveal important physical insights. First, for this particular case, ion electrophoresis plays an important role, and is an order of magnitude faster than free diffusion on a comparable time scale. Second, the maximum achievable concentration within the cell is reciprocally correlated with the extracellular electrical conductivity. This behavior is mediated by an electrokinetic mechanism known as field-amplified sample stacking. Through this mechanism, the intracellular ion concentration can reach a level higher than the extracellular one provided that the intra-to-extracellular conductivity ratio is greater than unity. The results corroborate well with data in the literature, and offer a mechanistic interpretation to previous experimental observations. This work is a step toward the quantification of molecular delivery via electroporation.

Numerical Simulation of Molecular Delivery via Electroporation

A numerical simulation to study molecular delivery via electroporation is presented. The Nernst-Planck equations for species transport are solved in both the intra- and extra-cellular spaces, and are coupled at the cell membrane through an asymptotic Smoluchowski equation for membrane permeabilization. The delivery of calcium ions into a Chinese Hamster Ovary cell is simulated. To facilitate comparison with fluorescence measurement, the simulation includes three species (Ca2+, Fluo-3, and CaFluo) and their reactive kinetics. The results agree well with experimental data from the literature (Gabriel and Teissié, Biophys. J., 1999), and reveal that ion electrophoresis plays an important role in the process. Furthermore, the maximum achievable concentration within the cell is reciprocally correlated with the extracellular electrical conductivity. This observation corroborates well with both previous data (Djuzenova et al., Biochim. Biophys. Acta, 1996) and our own recent measurements. The root-cause of this behavior is an electrokinetic mechanism known as field-amplified sample stacking. Through this mechanism, the intracellular ion concentration can reach a level higher than the extracellular one provided that the intra-to-extra-cellular conductivity ratio is greater than unity. This work is a step toward the quantification of electroporation-mediated molecular delivery.

Simultaneous concentration and separation of microorganisms: insulator-based dielectrophoretic approach

Microanalytical methods offer attractive characteristics for rapid microbial detection and concentration. There is a growing interest in the development of microscale separation techniques. Dielectrophoresis (DEP), a nondestructive electrokinetic transport mechanism, is a technique with great potential for microbe manipulation, since it can achieve concentration and separation in a single step. DEP is the movement of particles due to polarization effects in nonuniform electric fields. The majority of the work on dielectrophoretic manipulation of microbes has employed alternating current fields in arrays of microelectrodes, an approach with some disadvantages. An alternative is to employ insulator-based DEP (iDEP), a dielectrophoretic mode where nonuniform fields are produced by employing arrays of insulating structures. This study presents the concentration and fractionation of a mixture of bacteria and yeast cells employing direct current-iDEP in a microchannel containing an array of cylindrical insulating structures. Negative dielectrophoretic trapping of both types of microorganisms was demonstrated, where yeast cells exhibited a stronger response, opening the possibility for dielectrophoretic differentiation. Simultaneous concentration and fractionation of a mixture of both types of cells was carried out analogous to a chromatographic separation, where a dielectropherogram was obtained in less than 2 min by applying an electric field gradient and achieving concentration factors in the order of 50 and 37 times the inlet concentration for Escherichia coli and Saccharomyces cerevisiae cells, respectively. Encouraging results were also obtained employing a sample of water taken from a pond. The findings demonstrated the great potential of iDEP as a rapid and effective technique for intact microorganism concentration and separation.

MuSET: A multiparameter and high precision sensor for downhole spontaneous electrical potential measurements

On the basis of an existing multiparameter borehole fluid sensor ( p, T, Cw, pH, Eh), a new downhole tool designed for 200 bars and 75 °C was developed to measure the spontaneous electrical potential in situ with great precision (better than a μV). To this end, the new sensor is based on the use of unpolarizable Pb/PbCl 2 electrodes either at the surface or downhole. In situ testing has demonstrated a capacity to identify several subsurface sources of natural electrical potential such as diffusion ones (membrane potential in the presence of clays, Fickian processes due to pore fluid salinity gradients), or else the electrokinetic mechanisms with gradients in pore fluid pressure. As a consequence, Multi-Sensors Electrical Tool (MuSET) might be used as an “electrical flowmeter” sensitive to both horizontal and vertical fluid flow in a vertical borehole.

Transient processes at the deposition of charged Langmuir monolayers

An electrokinetic mechanism is proposed to explain the slow meniscus relaxation that is observed in experiments of the deposition of charged Langmuir monolayers on a solid substrate using the LB technique. The major element of the proposed mechanism amounts to the formation the ion concentration and electric potential profiles in the subphase close to the three-phase contact line during the monolayer transfer. A mathematical model is developed to describe the transition processes which occur in the subphase when the imposed speed of substrate changes with time transiently. The calculations on the basis of the proposed model predict meniscus relaxation times of the same order of magnitude as those observed in experiments. The obtained results are important for analyzing meniscus oscillations which lead to formation of striped patterns within the deposited LB films.

Enhancement of charged macromolecule capture by nanopores in a salt gradient.

Nanopores spanning synthetic membranes have been used as key components in proof-of-principle nanofluidic applications, particularly those involving manipulation of biomolecules or sequencing of DNA. The only practical way of manipulating charged macromolecules near nanopores is through a voltage difference applied across the nanopore-spanning membrane. However, recent experiments have shown that salt concentration gradients applied across nanopores can also dramatically enhance charged particle capture from a low concentration reservoir of charged molecules at one end of the nanopore. This puzzling effect has hitherto eluded a physically consistent theoretical explanation. Here, we propose an electrokinetic mechanism of this enhanced capture that relies on the electrostatic potential near the pore mouth. For long pores with diameter much greater than the local screening length, we obtain accurate analytic expressions showing how salt gradients control the local conductivity which can lead to increased local electrostatic potentials and charged analyte capture rates. We also find that the attractive electrostatic potential may be balanced by an outward, repulsive electro-osmotic flow that can in certain cases conspire with the salt gradient to further enhance the analyte capture rate.

Relation between salt rejection and electrokinetic properties on Shirasu porous glass (SPG) membranes with nano-order uniform pores

The salt rejection by Shirasu porous glass (SPG) membranes having nano-order uniform pores was investigated for understanding the electrokinetic mechanism resulting from the surface charge developed on the membrane when in contact with salt solutions. Due to the dissociation of the hydroxyl groups such as silanol groups on the membrane surface, the membrane was negatively charged over a pH range of 3–10 from electrophoretic measurements. Cross-flow filtration experiments showed that up to 63% of NaCl was rejected by an SPG membrane having a mean pore diameters of 33 nm in a 1 mol m −3 NaCl solution at pH 7 under a transmembrane pressure of 74 kPa, even though the pore diameter is much larger than the ion diameter. This is a consequence of the electrostatic repulsive interaction between the co-ions (Cl − ions) and the membrane surface. At the same pH, the rejection factor of NaCl decreased with increasing salt concentration due to an increase in the ionic strength. More negative charge on the membrane surface at higher pH resulted in higher rejection factors of NaCl for a fixed salt concentration. Higher rejection factors of NaCl by SPG membranes with smaller pore sizes for a fixed concentration are due to the higher ratio of the thickness of the electric double layer (Debye length) to the pore radius. The SPG membrane showed a salt rejection sequence: Na 2SO 4, NaCl and CaCl 2 at the same pH. This is because divalent anions (SO 4 2−) are more strongly repelled by the negatively charged membrane, while divalent cations (Ca 2+) adsorb specifically onto the membrane surface than monovalent cations (Na +). The salt rejection factor increased with increasing permeate volume flux. Due to the stronger acidity of the membrane materials, SPG membranes had a higher rejection factor and a lower isoelectric point (IEP < 3) than ceramic membranes.

Nonlinear electrokinetic phenomena around nearly insulated sharp tips in microflows

This contribution seeks to provide for the first time a combined comprehensive theoretical prediction and quantitative experimental (microparticle imaging velocimetry – μ -PIV) measurements of the nonlinear electrokinetic flow around sharp tips in order to substantiate former theoretical and qualitative experimental flow visualization results [S.K. Thamida, H.C Chang, Phys. Fluids 14 (2002) 12; P. Takhistov, K. Duginova, H.C. Chang, J. Colloid Interface Sci. 263 (2003) 133; G. Yossifon, I. Frankel, T. Miloh, Phys. Fluids 18 (2006) 117108]. The study focuses on two microchannel designs: an L-shaped channel and two isolated tips in a straight channel, important in engineering for mixing and particle-trapping purposes. The new experimental results were explained in terms of an induced-charge electrokinetic mechanism alone, without the concentration polarization mechanism as suggested by earlier studies. The vortex generation phenomenon around corners was explained in terms of the varying ratio between the equilibrium and the induced-charge zeta-potentials, showing fair qualitative agreement between numerical and experimental results. Hence, a transition from an irrotational to nonlinear-dominated flow with a vortex pattern occurs beyond a certain electric-field threshold. In particular, for the L-shaped channel case, it is demonstrated that beyond a second field threshold an upstream vortex appears in addition to the downstream one.

Characterization of electrokinetic mobility of microparticles in order to improve dielectrophoretic concentration

Insulator-based dielectrophoresis (iDEP), an efficient technique with great potential for miniaturization, has been successfully applied for the manipulation of a wide variety of bioparticles. When iDEP is applied employing direct current (DC) electric fields, other electrokinetic transport mechanisms are present: electrophoresis and electroosmotic flow. In order to concentrate particles, iDEP has to overcome electrokinetics. This study presents the characterization of electrokinetic flow under the operating conditions employed with iDEP; in order to identify the optimal conditions for particle concentration employing DC-iDEP, microparticle image velocimetry (microPIV) was employed to measure the velocity of 1-microm-diameter inert polystyrene particles suspended inside a microchannel made from glass. Experiments were carried out by varying the properties of the suspending medium (conductivity from 25 to 100 microS/cm and pH from 6 to 9) and the strength of the applied electric field (50-300 V/cm); the velocities values obtained ranged from 100 to 700 microm/s. These showed that higher conductivity and lower pH values for the suspending medium produced the lowest electrokinetic flow, improving iDEP concentration of particles, which decreases voltage requirements. These ideal conditions for iDEP trapping (pH = 6 and sigma(m) = 100 microS/cm) were tested experimentally and with the aid of mathematical modeling. The microPIV measurements allowed obtaining values for the electrokinetic mobilities of the particles and the zeta potential of the glass surface; these values were used with a mathematical model built with COMSOL Multiphysics software in order to predict the dielectrophoretic and electrokinetic forces exerted on the particles; the modeling results confirmed the microPIV findings. Experiments with iDEP were carried out employing the same microparticles and a glass microchannel that contained an array of cylindrical insulating structures. By applying DC electric fields across the insulating structures array, it was seen that the dielectrophoretic trapping was improved when the electrokinetic force was the lowest; as predicted by microPIV measurements and the mathematical model. The results of this study provide guidelines for the selection of optimal operating conditions for improving insulator-based dielectrophoretic separations and have the potential to be extended to bioparticle applications.

The mechanism of the appearance of luminescence and electrification in liquid flows through narrow channels

The mechanism of the effects observed in hydrodynamic unit throttles was studied. These effects included luminescence in the visible range localized in a microscopic toroidal volume and electric pulses when a dielectric liquid flew through a narrow passage orifice. Equations for charging and conduction currents were obtained. The stationary electric charge, potential, and field strength on the internal surface of a passage orifice were calculated. It was shown theoretically that the appearance of luminescence most probably occurred in electrical breakdowns in cavitation bubbles in the initial flow section inside the passage orifice. Electric charge formed not only during hydrodynamic cavitation but also in a laminar throttle in the absence of cavitation in the liquid; the electrokinetic mechanism applied to this phenomenon too. It was shown experimentally that electric charges appeared not only in plastic but also in metallic throttles. The suggested mechanism of light emission and electric charge appearance was in agreement with the experimental results.

Performance characterization of an insulator‐based dielectrophoretic microdevice

Dielectrophoresis (DEP), the motion of particles in nonuniform electric fields, is a nondestructive electrokinetic (EK) transport mechanism can be used to concentrate and separate bioparticles. Traditionally, DEP has been performed employing microelectrodes, an approach that is expensive due to the cost of microelectrode fabrication. An alternative is insulator-based DEP (iDEP), an inexpensive method where nonuniform electric fields are created with arrays of insulating structures. This study presents the effects of operating conditions on the dielectrophoretic behavior of polystyrene microparticles under iDEP. Experiments were performed employing microchannels containing insulating structures that worked as insulators. The parameters varied were pH (8-9) and conductivity (25-100 microS/cm) of the bulk medium, and the magnitude of the applied field (200-850 V/cm). Optimal operating conditions in terms of pH and conductivity were obtained, and the microdevice performance was characterized in terms of concentration factor and minimum electric field required (minimum energy consumption). This is the first report on improving iDEP processes when EOF is present. DEP and EOF have been studied extensively, however, this study integrates the effect of suspending medium characteristics on both EK phenomena. These findings will allow improving the performance of iDEP microdevices achieving the highest concentration fold with the lowest energy consumption.