Effect of Electrode Pattern on the Column Structure and Yield Stress of Electrorheological Fluids

For electrorheological (ER) suspensions, the aggregate structures of particles were observed in electric fields by the use of transparent cells with different electrode patterns. Although the suspension is dispersed to noninteracting particles without electric fields, many aggregates are formed on the electrode surface in electric fields. Since the dipole–dipole interactions cause chain structures of particles and equilibrium conformations of chains are always aligned with electric field, the aggregates indicate the presence of columns spanning the electrode gap. The particle concentration in columns which are developed between parallel-plate electrodes is about 22 vol %. In striped electrodes, the particles construct striped aggregates along the electrodes and no particles remain in the insulating region. The particle concentration in striped aggregates is about 35 vol %. The nonuniformity of electric field is responsible for the high particle concentration. The increase in particle concentration of column lead to the high yield stress of electrified suspension. Therefore, the ER performance of suspension as an overall response can be improved by the electrode design.     

Electrically developed morphology of carbon nanoparticles in suspensions monitored by in situ optical observations under sinusoidal electric field

In situ optical observations were performed for suspensions composed of carbon nanoparticles under the sinusoidal electric field with an amplitude around 20 kV/mm (volt per micrometer) and various frequencies. For extremely diluted suspensions of mixed fullerenes or multiwalled carbon nanotubes (MWNTs) in a silicone oil, the dark-field optical microscopy was effective for the in situ observation of the particle behavior under the electric field. The nanoparticles in a fullerene suspension under the sinusoidal electric field with a frequency of 100 Hz (in short, 100 Hz electric field) were aggregated to form a rigid spherical microstructure around the halfway between the electrodes. On the other hand, the nanoparticles in an MWNT suspension under 100 Hz electric field were also aggregated but aligned to form a chain-like microstructure which spans the electrodes. Both of the aggregated particles were stable even after the removal of the electric field, and they were redispersed by application of 10 Hz electric field.     

Monodisperse conducting colloidal dipoles with symmetric dimer structure for enhancing electrorheology properties

This study introduces an electrorheological (ER) approach that allows us to obtain remarkably enhanced ER properties by using monodisperse colloidal dimer particles. Two sets of colloidal particles, which are spheres and symmetric dimers, were synthesized employing the seeded polymerization technique. The aspect ratio of dimer particles was ~1.43. Then, the surface of the particles was coated with polyaniline by using the chemically oxidative polymerization method. After preparation of the particle suspensions having the same particle volume and concentration, their ER behavior was investigated with changing the electric field strength. At the same experimental condition, both shear stress and shear yield stress of the dimer particle suspension remarkably increased, compared with those of the spherical particle suspension. This attributes to the fact that the shape anisotropy of suspending particles effectively led to increase in the dipole moment under the electric field, thus resulting in formation of a well-structured colloidal chains between the electrodes.     

In situ conductance measurements for alignments of silica particles under alternating electric fields

The alignments of silica particles formed in sinusoidal electrical fields of 1 kHz were assessed using an optical microscope with measuring the electric conductance of a silica dispersion between two Pt electrodes in a vitreous silica glass cell. We confirmed that the electric conductance of the silica dispersion between the two electrodes in the cell reflected the surface conductance of the silica particles settling at the bottom of the cell. More interestingly, we observed that the electric conductance of the silica dispersion in the cell increased when pearl chains of the silica particle were formed along the direction of the electric field. However, no clear change in the electric conductance of the dispersion was observed at higher electric field strengths where a transition from pearl chains to zigzag band patterns and circulating movements of the silica particles in the zigzag bands formed.     

Electric field processing to control the structure of poly(vinylidene fluoride) composite proton conducting membranes

A novel method is reported for controlling the structure of poly(vinylidene fluoride) (PVdF) composite proton conducting membranes. When proton conducting Nafion or zirconium phosphate sulfophenylenphosphonate (ZrPSPP) particles are dispersed in a mixed colloidal suspension with PVdF particles, the proton conducting particles selectively respond to an applied electric field. Under appropriate conditions, the proton conducting particles are induced to assemble into chains that rapidly grow to span the gap between electrodes as the electric field is applied. By removing the solvent and melting the PVdF phase while applying the electric field, composite membranes were formed that have field-induced structure. In comparison to randomly structured composites, the electric field-processed Nafion/PVdF or ZrPSPP/PVdF composite membranes showed improved proton conductivity, water sorption, selectivity for protons over methanol, and controlled surface area changes upon swelling with water. The transport and mechanical properties of the electric field-processed composite membranes suggest the potential for improved performance in direct methanol fuel cells.     

AC electric field‐assisted assembly and alignment of cellulose nanocrystals

In this article, we describe an efficient physical electric‐field‐assisted method to study self‐assembly and orientation of cellulose nanocrystals. When applying an alternating voltage to a cellulose nanocrystals suspension deposited onto a thin gap of coplanar lithographically patterned metallic electrodes, a highly homogeneous orientation of cellulose nanocrystals is obtained. Parameters such as strength and frequency of the applied electric field and cellulose nanocrystals aspect ratios were studied to determine how they affect cellulose nanocrystals assembly and orientation. The prepared films were analyzed by atomic force microscopy, and the results suggest that the alignment of cellulose nanocrystals generated films is greatly influenced by the frequency and the strength of the applied electric field. The orientation of cellulose nanocrystals becomes more homogeneous with increasing electric field higher than 2000 V/cm with a frequency ranging between 10⁴ and 10⁶ Hz. © 2008 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 46: 1430–1436, 2008     

New SFA techniques for studying surface forces and thin film patterns induced by electric fields

We describe two ways to measure normal and/or lateral forces between two surfaces in a surface forces apparatus (SFA) while an electric field is applied between the surfaces. The first method involves depositing thin conductive layers on the exposed substrate (usually mica) sheets; the second involves using the optically reflecting silver layers on the back surfaces of the sheets as the electrodes. Two types of experiments were performed using these new techniques: (1) measuring the effects of an electric field on the rheology of an approximately 40-microm-thick film of zeolite particles suspended in silicone oil and (2) a dynamic study of electric field-induced pattern formation of a thin polymer film. In the first study, under an electric field of strength approximately 106 V/m the shear force or effective viscosity of the colloid suspension was found to be two orders of magnitude higher than in the absence of the field, when the expected bulk value was measured. In the dynamic study, the initially uniform film transformed into a 2-D honeycombed network of depressed cells bounded by elevated ridges that grew slowly with time in a way consistent with previously derived theories. The new techniques should be applicable to studies of other systems and interactions, such as double-layer forces, micro- and nanoelectrorheology, electric field-induced ordering of particles, and the effects of electric fields on adhesion, friction, and lubrication.     

Control of particle alignment in water by an alternating electric field

We attempted to align a large number of silica particles dispersed in aqueous solution by controlling the alternating electric field between the two electrodes (400 microm apart). Relatively large particles (9.9 microm) were found to align forming strings in the direction parallel to the electric field while relatively small particles (2.0 and 4.9 microm) were observed to align making stripes in the direction perpendicular to the field. The number of stripes formed by particles between the electrodes increased with increasing frequency of the alternating field. This peculiar perpendicular particle alignment appeared when the contribution to particle alignment of electroosmotic flow exceeded that of dielectric polarization and the osmotic flow was found to be stronger around the particles than in the vicinity of the electrode surface.     

Synthesis and electrorheological characteristics of sea urchin-like TiO<Subscript>2</Subscript> hollow spheres

TiO₂ hollow microspheres with sea urchin-like hierarchical architectures were synthesized by a simple hydrothermal method. The as-synthesized hollow microspheres with hierarchical architectures consisting of many rhombic building units exhibit high specific surface area. Electrorheological (ER) properties of hierarchical hollow TiO₂-based suspension were investigated under steady and oscillatory shear. The hollow TiO₂-based suspensions show much higher yield stress and elasticity than pure TiO₂ suspension at the same electric field strength. This phenomenon was elucidated well in view of their dielectric spectra analysis. The sea urchin-like architectures result in stronger interfacial polarization of hollow TiO₂ suspension upon an electric field, showing higher ER activity. Also, hollow interiors of TiO₂ particles increase the long-term stability of suspensions and further merit the ER effect.     

Control and modeling of the dielectrophoretic assembly of on-chip nanoparticle wires

Suspensions of metallic nanoparticles in water were assembled via the action of an alternating electric field (dielectrophoresis) into wires of micrometer thickness. Two modes of microwire assembly, one through the bulk of the suspension and one as half-cylinders on the glass surface between the electrodes, were identified. The operating conditions responsible for the two assembly modes were recognized. The control of the process parameters allows making, for example, straight single connectors or massively parallel arrays of microwires on the surface of the chip, which can be extracted in dry form. The microwire assembly process was modeled using finite element electrostatic calculations. The direction of growth can be guided by introducing conductive islands or particles in the suspension. The experiments, supported by electrostatic calculations, show that the wires grow in the direction of highest field intensity, "automatically" making electrical connections to the objects between the electrodes. The results point the way to controlled dielectrophoretic assembly of nanoparticles into on-chip electrical connectors, switches, and networks.     

A cell electro‐rotation micro‐device using polarized cells as electrodes

Cell rotation is widely required in various fields as an important technique for single cell manipulation. Usually, the electro‐rotational manipulation of single cells by dielectrophoresis technologies requires at least three electrodes to generate rotating electric fields which induce cells to rotate. Here, we present a novel microfluidic chip capable of rotating single cell using only two planar electrodes by taking polarized cells as the extra electrodes with phase‐shifted signal. To demonstrate this idea, we configured two parallel and planar electrodes as basic dielectrophoresis elements and placed trenches above these electrodes to attract cells, which were in turn polarized to be electrodes. Through simulation, we confirmed the functional structure of the device works well to generate proper rotating electric fields for cell rotation. Through experiment, we successfully demonstrated controlled electro‐rotation of HeLa and HepaRG cells. The novel electro‐rotation mechanism not only simplifies the micro‐device structure but also reduces the complexity of single cell rotation operation which will be a benefit to the potential users.     

Electrical breakdown of human erythrocytes: a technique for the study of electro-haemolysis

This paper describes a technique suitable for investigating the electromechanical breakdown properties of erythrocyte cells. The cells were exposed to square wave electric pulses of precise duration and voltage. The erythrocytes were suspended in normal isotonic saline between two opposing platinum electrodes. A red LED light source and photodiode detector system were positioned orthogonally to the electrodes to record changes in the light transmission that occur immediately after applying an electric pulse. The light transmitted through the electrically treated erythrocyte suspension could be monitored continuously. Experiments were conducted to explore the inter-relationship between the critical voltage and pulse length for haemolysis. Human blood taken from "healthy" donors underwent haemolysis at a critical field strength of 304 kV/m for a 5 micros pulse and 292 kV/m for a 50 micros pulse. The relationship of critical pulse length and critical voltage for the blood samples was found to be inversely linear.     

Linear viscoelastic properties of electro-rheological nano-suspension confined to narrow gap between electrodes

The linear viscoelastic properties of a suspension composed of titanium dioxide nanoparticles were measured under the direct current (dc) electric field with narrow gap distances between the electrodes. The yielding behavior under no external electric fields was also discussed. The wall slip at the interface between the parallel plates and the nano-suspension was briefly discussed. Under the dc electric field, a fine chain-like microstructure was optically found within a narrow gap of 50 μm between the electrodes in the quiescent state. The nano-suspension confined to a narrow gap of 65 μm between the parallel plates was rather viscoelastic even at the highest strength of the electric field of 16 kV·mm⁻¹. Furthermore, fast and slow relaxations of the dynamic moduli were found after removal of the electric field. It was pointed out that the linear viscoelasticity was an appropriate measure of the microstructure before yielding.     

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.     

Aligned carbon cones in free‐standing UV‐Curable polymer composite

A concept where an alternating electric field (dielectrophoresis) is used to assemble and align carbon nanocone particles (CNCs) into microscopic wires in self‐supporting polymer films is demonstrated. The particle fraction is kept low (one‐tenth of the percolation threshold of isotropic mixture), which allows uniform dispersion and efficient UV curing. The alignment leads to the conductivity enhancement of three to four orders of magnitude (from ～10^?7 to ～10^?3 S/m) in the alignment direction. It does not require passing current so the material can be isolated from the alignment electrodes. This prevents electrodes attaching to the film, if the film is adhesive in nature. The alignment can be done using either in‐plane or out‐of‐plane geometries. It is proposed that this concept could be applied in areas such as electrostatic discharge applications where inexpensive conductive or dissipative materials and macroscopic uniformity are prerequisites. © 2011 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys, 2011     

Particle interactions in electrophoresis due to inertia

The inertial forces acting on two cylinders and two spheres have been calculated. The cylinders or spheres are of the same radius and zeta potential, and arbitrarily oriented in an electric field. It is found that when two particles are aligned perpendicular to the direction of the electric field, the force between them along the line of the centers is attractive. When they are along the direction of the electric field, the force between them along the line of the centers is repulsive. On a pair of arbitrarily oriented particles, the force perpendicular to the line of the centers tends to rotate the particles around the midpoint between the particle centers such that the pair is aligned normal to the applied electric field. The stable equilibrium orientation of a pair of particles and the attractive interaction forces between the particles when they are stably orientated may give rise to aggregation of particles during electrophoretic motion of a suspension.     

On‐chip technology for single‐cell arraying,electrorotation‐based analysis and selective release

This paper reports a method for label‐free single‐cell biophysical analysis of multiple cells trapped in suspension by electrokinetic forces. Tri‐dimensional pillar electrodes arranged along the width of a microfluidic chamber define actuators for single cell trapping and selective release by electrokinetic force. Moreover, a rotation can be induced on the cell in combination with a negative DEP force to retain the cell against the flow. The measurement of the rotation speed of the cell as a function of the electric field frequency define an electrorotation spectrum that allows to study the dielectric properties of the cell. The system presented here shows for the first time the simultaneous electrorotation analysis of multiple single cells in separate micro cages that can be selectively addressed to trap and/or release the cells. Chips with 39 micro‐actuators of different interelectrode distance were fabricated to study cells with different sizes. The extracted dielectric properties of Henrietta Lacks, human embryonic kidney 293, and human immortalized T lymphocytes cells were found in agreements with previous findings. Moreover, the membrane capacitance of M17 neuroblastoma cells was investigated and found to fall in in the range of 7.49 ± 0.39 mF/m².     

Separation of mixtures of particles in a multipart microdevice employing insulator-based dielectrophoresis

Dielectrophoresis is the electrokinetic movement of particles due to polarization effects in the presence of non-uniform electric fields. In insulator-based dielectrophoresis (iDEP) regions of low and high electric field intensity, i.e. non-uniformity of electric field, are produced when the cross-sectional area of a microchannel is decreased by the presence of electrical insulating structures between two electrodes. This technique is increasingly being studied for the manipulation of a wide variety of particles, and novel designs are continuously developed. Despite significant advances in the area, complex mixture separation and sample fractionation continue to be the most important challenges. In this work, a microchannel design is presented for carrying out direct current (DC)-iDEP for the separation of a mixture of particles. The device comprises a main channel, two side channels and two sections of cylindrical posts with different diameters, which will generate different non-uniformities in the electric field on the main channel, designed for the discrimination and separation of particles of two different sizes. By applying an electric potential of 1000 V, a mixture of 1 and 4 μm polystyrene microspheres were dielectrophoretically separated and concentrated at the same time and then redirected to different outlets. The results obtained here demonstrate that, by carefully designing the device geometry and selecting operating conditions, effective sorting of particle mixtures can be achieved in this type of multi-section DC-iDEP devices.     

Electric‐Field Triggered Controlled Release of Bioactive Volatiles from Imine‐Based Liquid Crystalline Phases

Application of an electric field to liquid crystalline film forming imines with negative dielectric anisotropy, such as N‐(4‐methoxybenzylidene)‐4‐butylaniline (MBBA, 1 ), results in the expulsion of compounds that do not participate in the formation of the liquid crystalline phase. Furthermore, amines and aromatic aldehydes undergo component exchange with the imine by generating constitutional dynamic libraries. The strength of the electric field and the duration of its application to the liquid crystalline film influence the release rate of the expelled compounds and, at the same time, modulate the equilibration of the dynamic libraries. The controlled release of volatile organic molecules with different chemical functionalities from the film was quantified by dynamic headspace analysis. In all cases, higher headspace concentrations were detected in the presence of an electric field. These results point to the possibility of using imine‐based liquid crystalline films to build devices for the controlled release of a broad variety of bioactive volatiles as a direct response to an external electric signal.     

Front Cover: Enhancement of dielectrophoresis-based particle collection from high conducting fluids due to partial electrode insulation

Dielectrophoresis (DEP) is a successful method to recover nanoparticles from different types of fluid. The DEP force acting on these particles is created by an electrode microarray that produces a nonuniform electric field. To apply DEP to a highly conducting biological fluid, a protective hydrogel coating over the metal electrodes is required to create a barrier between the electrode and the fluid. This protects the electrodes, reduces the electrolysis of water, and allows the electric field to penetrate into the fluid sample. We observed that the protective hydrogel layer can separate from the electrode and form a closed domed structure and that collection of 100 nm polystyrene beads increased when this occurred. To better understand this collection increase, we used COMSOL Multiphysics software to model the electric field in the presence of the dome filled with different materials ranging from low-conducting gas to high conducting phosphate-buffered saline fluids. The results suggest that as the electrical conductivity of the material inside the dome is reduced, the whole dome acts as an insulator which increases electric field intensity at the electrode edge. This increased intensity widens the high-intensity electric field factor zone resulting in increased collection. This informs how dome formation results in increased particle collection and provides insight into how the electric field can be intensified to the increase collection of particles. These results have important applications for increasing the recovery of biologically-derived nanoparticles from undiluted physiological fluids that have high conductance, including the collection of cancer-derived extracellular vesicles from plasma for liquid biopsy applications.