Multiple charging of ultrafine particles in a corona charger

The charge distribution on ultrafine aerosol particles in the size range below 35 nm has been measured using a corona-based unipolar charger, in which ion generation and aerosol charging take place simultaneously in the region around a sharp-point discharge electrode. The mean number of charges per particle predicted by Fuchs’ diffusion charging theory is in relatively good agreement with the experimental results, and this implies that diffusion charging is the predominant mechanism in spite that the electric field in the charging region is very high. Since a steady state is unattainable in unipolar charging, the charge distribution depends on the geometry and operating conditions of each particular charger. When the present device operates under the conditions (nt-product) which yield the maximum charging efficiency, double charge appears on particles with diameter as small as 15 nm. At larger values of nt, 32 nm particles can acquire up to five charges. The critical particle diameter above which multiple charging occurs is about four times smaller than for bipolar radioactive chargers. In order to use corona charging in aerosol particle size measurement by electrical methods, the required mobility data inversion is thus straightforward for particle diameter below about 15 nm, but becomes quite complex for larger sizes.     

Estimating aerosol particle charging parameters using a Bayesian inversion technique

A Bayesian inversion routine is described in which data from tandem differential mobility analysis (TDMA) can be used to determine fundamental parameters for charging models as a function of particle size. The measurement and inversion techniques were verified using simulated data for particles in the 50–500 nm range undergoing unipolar diffusion charging as described by Fuchs’ limiting sphere theory, for which the fundamental charging parameter is the product of the unipolar ion concentration and residence time within the charger, the so-called nt product. Under conditions where the average particle charge is greater than one unit charge, the inversion routine is precisely and accurately able to determine the nt value. The inversion routine breaks down, however, when the average number of charges per particle is well below unity, i.e. for low nt values or for small particle sizes. Incorporation of charging efficiency data in addition to TDMA data can allow for use of the inversion routine when the average number of charges per particle is low. With its limitations known, the inversion routine was applied to determine the nt value for the unipolar charger used in the TSI electrical aerosol detector (EAD), model 3070A, for particles in the 50–200 nm size range. The effective nt value within the EAD charger decreased with decreasing particle size, implying that charged particle losses occur within the EAD charger. The described inversion routine is unique in its ability to determine size dependent charge model parameters, and can be utilized with any given charging model. It is expected that this technique will be of use in advancing the understanding of aerosol particle charging models and in future design of unipolar chargers.     

A Device for Generating Singly Charged Particles in the 0.1–1.0-μm Diameter Range

In this paper an aerosol charger that largely avoids the production of multiply charged particles in the 0.1–1.0 μm diameter range is described. The input aerosol is first passed through an electrostatic condenser to remove all charged particles and ions. The remaining neutral aerosol then flows into a 23-cm-long, 2.1-cm inner diameter cylindrical tube; the inner surface of this tube is uniformly coated with 0.09 μCi⁶³ Ni, a 0.067 MeV β-emitter with a half-life of 92 years. At typical airflow rates of 0.2–1.0 lpm, this low-activity source of ionizing radiation produces bipolar ion concentrations ranging from 1 × 10⁴ to 9 × 10⁴ ion/cm³, which is much lower than levels required to bring the aerosol to Boltzmann charge equilibrium. At a flow rate of 1.0 lpm, particles smaller than about 1.0 μm typically interact with no more than one ion en route through the charger. Therefore, particles at the charger exit are mostly either neutral or singly charged. Charge distributions of initially-neutral mono-disperse polystyrene latex particles were measured at the exit from the charger for particle diameters ranging in size from 0.09 to 1.09 μm. It was found that, at an airflow rate of 1.0 lpm and particle size 1.09 μm, the ratios of singly, doubly, and triply charged to total positively charged concentrations were 0.75, 0.19, and 0.06 respectively; particles with more than three charges were not detected. In contrast, the analogous charge ratio at Boltzmann equilibrium is 0.28 (+ 1), 0.24 (+ 2), 0.19 (+ 3), 0.13 (+ 4), 0.08 (+ 5), 0.05 (+ 6), and 0.7 (+ 02).     

Experimental study of a new corona-based unipolar aerosol charger

A corona-based unipolar aerosol charger has been constructed, and its performance has been systematically evaluated. The prototype consists of completely separated corona ionization and charging chambers. With this configuration the electrostatic loss of charged particles is eliminated, and particle loss by diffusion and the space charge effect is minimized by the angular injection of the ionizer flow and the rapid exit of charged particles. The charger performance was optimized by varying different operational parameters, i.e., total and ionizer flowrates, and ion concentration. It was found that operation with one corona ionizer gave higher extrinsic charging efficiency than operation with two ionizers. The corona-discharge current has negligible effect on the charging performance. Operating the charger at a total flowrate of 5 lpm, with 1.0 lpm flow in each of the two ionizers, gave the highest extrinsic charging efficiency. Further, the performance of prototype charger was not compromised even at a total flowrate of 10 lpm. The charger provides higher extrinsic charging efficiency than other corona-based unipolar chargers. Extrinsic charge distributions for particles of different sizes were at last measured by the tandem-DMA technique.     

Monodisperse fine aerosol generation using fluidized bed

Monodisperse, fine aerosols are needed in many applications: filter testing, experiments for testing models, and aerosol instrument calibration, among others. Usually, monodisperse fine aerosols are generated in very low concentrations, or mass flow rates, in the laboratory scale. In this work, we needed to generate aerosols with higher mass flow rate than typically available by the laboratory-scale methods, such as atomizers, nebulizers, ultrasonic generators, vibrating orifice generators, and condensation generators. Therefore, we constructed a fluidized bed aerosol generator to achieve particle mass flow rates in the range of 15-100 g/h. Monodisperse, spherical SiO₂ particles of two sizes with geometrical diameters of 1.0 and 2.6 µm were used in the aerosol generator. The aerosol generator was used at both atmospheric pressure, and at high pressures up to 5 bar (abs).The particle size, mass concentration and the net average particle charge were measured after mixing the aerosol with nitrogen. The particle size distributions with both particle sizes were monodisperse, and no particle agglomerates were entrained from the fluidized bed. The behavior of the fluidized bed generator was found to be markedly different with the two particle sizes in regard to particle concentration, presumably due to different particle charging inside the generator. After determining the net average charge of the particles, an ion source Kr-85 was used to reduce the charge of the particles. This was found to be effective in neutralizing the particles.     

Determination of the adhesion force between particles and a flat surface, using the centrifuge technique

By using a centrifuge technique, the influence of powdery material particle size on the adhesion force particle-surface was determined. In order to achieve this, the adhesion of phosphatic rock (ρ_p = 3.090 kg m^− 3) and of manioc starch particles (ρ_p = 1.480 kg m^− 3) on a steel surface were studied. A microcentrifuge that reached a maximum speed rotation of 14000 rpm and which contained specially designed centrifuge tubes was used. There tubes contained the flat surface where the test particles were deposited. The powder particles were dispersed on these disks and the particles detachment were performed using diverse centrifugal speeds. The graphics of particle percentages still adhering on the surface of the disks as a function of the applied detachment force showed that the profile of adhesion force followed a log-normal distribution. The adhesion force increased with particle size. The manioc starch particles presented adhesion forces greater than those for the phosphatic rock particles for all particle sizes studied. The results obtained were compared with the theory proposed by Derjaguin, Muller and Toporov whose theoretical adhesion presented values close to the experimental data for the phosphatic rock particles adhesion on the stainless steel surface. On the contrary, the theoretical values were lower than the experimental ones for the manioc starch particles maybe due to the small roughness of these particles, their physical properties (softer and deformable material) and/or specific chemical interactions since the organic composition of the manioc starch particles that can dominate the adhesion force. Finally, the separation distance among the surfaces in contact (Z₀) was estimated in approximately 1.0 × 10^− 9 m for the phosphatic rock and 5.0 × 10^− 10 m for the manioc starch. These results were weakly dependent on the particle size range.     

Design and performance test of a multi-channel diffusion charger for real-time measurements of submicron aerosol particles having a unimodal log-normal size distribution

It is important to develop a simple and fast method for measuring the sizes of submicron particles in both laboratories and fields. In our previous studies, Park, An, and Hwang [(2007). Development and performance test of a unipolar diffusion charger for real-time measurements of submicron aerosol particles having a log-normal size distribution. Journal of Aerosol Science, 38, 420–430] and Park, Kim, An, and Hwang [(2007). Real-time measurement of submicron aerosol particles having a log-normal size distribution by simultaneously using unipolar diffusion charger and unipolar field charger. Journal of Aerosol Science, 38, 1240–245], we introduced methodologies that our lab made unipolar charger could lead to detection times of under 5 s in conjunction with an electrometer and a condensation particle counter (CPC), and under 3 s with two electrometers.However, both methodologies require an appropriate assumption of the geometric standard deviation of particle sizes. In this paper, we introduce a methodology for determining the geometric standard deviation of particle sizes as well as the geometric mean diameter and the total number concentration of particles. For this purpose, a diffusion charger that consisted of discharge zone, mixing and charging zone, and three flow channels for obtaining three different residence times and average charges of particles in the channels, was designed and tested. For determining the average particle charge, various methods including theoretical calculations and the tandem differential mobility analyzer (TDMA) method were used. The results obtained from the different methods agreed well with each other. To compare the size distribution with the data that were measured through a scanning mobility particle sizer (SMPS), sodium chloride (NaCl) particles were used. The estimated results by using a data inversion algorithm were less than those measured by SMPS by around 22% for the total number concentration and 10% for both the geometric mean diameter and the geometric standard deviation. Furthermore, the detection time was under 3 s.     

Unipolar Charging of Nanosized Aerosol Particles Using Soft X-ray Photoionization

A unipolar charging device based on a soft X-ray (<9.5 keV) photoionization was developed to investigate the charging efficiency of aerosol nanoparticles. Unipolar charging using a 241 Am charger was also evaluated as a comparison with the characteristics obtained by X-ray charging. The production rate and the concentration of ions generated by the X-ray and 241 Am unipolar chargers were estimated from ion current measurements. Theoretical calculations by the unipolar diffusion charging theory were also carried out and the calculated data were compared with the experimental results. For acquiring a high number of standard nanoparticles, the classification of monodisperse nanoparticles from polydisperse aerosol particles using the X-ray unipolar charger and a differential mobility analyzer (DMA) was also evaluated. The ion production rate of the X-ray unipolar charger was at least 5.5 times higher than that of the 241 Am unipolar charger and the ion concentration was about three times higher. Therefore, the X-ray unipolar charger showed a higher capability for charging aerosol particles of 10-40 nm size in diameter than the 241 Am charger. The charging state of particles produced by the X-ray unipolar charger was in good agreement with theoretical calculations. The X-ray unipolar charger developed herein has potential for use in charging a high number concentration of nanoparticles for use in nanotechnology investigations.     

Solids mixing behavior in a nano-agglomerate fluidized bed

The nano-particles mixing behavior in a nano-agglomerate fluidized bed (NAFB) using R972, a kind of nano-SiO₂ powder, was investigated by the nano-particle coated phosphors tracer method. The axial and radial solids dispersion coefficients in this system were two orders of magnitude lower than those in fluid catalytic cracking (FCC) catalyst systems. The axial solids dispersion coefficient increased with increasing superficial gas velocities, and ranged between 9.1 × 10^− 4 and 2.6 × 10^− 3 m²/s. There was a step increase in the axial solids dispersion coefficient between the particulate fluidization regime and bubbling and turbulent fluidization regimes. As the superficial gas velocity increased, the radial solids dispersion coefficient increased gradually, from 1.2 × 10^− 4 to 4.5 × 10^− 4 m²/s. The much smaller D_a and D_r, compared to regular fluidized systems, is mainly due to the reduced density difference between the fluidized particles and fluidizing medium. To validate this, the solids dispersion coefficients in the NABF were compared with literature values for liquid-solid particulate systems in the particulate fluidization regime and FCC systems in the bubbling and turbulent fluidization regimes. The density difference between the fluidized particles and fluidizing medium and kinetic viscosity of the fluidizing medium, and other hydrodynamic factors like the superficial velocity of the fluidizing medium and the average diameters of the fluidized particles, were the key factors in the solids mixing in the fluidized beds. Empirical correlations are given to describe the results.     

The Effect of Particle Pre-Existing Charge on Unipolar Charging and Its Implication on Electrical Aerosol Measurements

We investigated the effect of particle pre-existing charges on unipolar charging. Particles carrying a defined number and polarity of pre-existing charges were used to study the unipolar charging process in a unipolar diffusion charger with positive ions. It was found that the particles initially carrying negative charges have almost the same amount of positive charges as the initially uncharged particles after passing the test charger; and the particles initially carrying more positive charges have more final charges. An analytical solution of a model for particle charge distribution of initially charged particles was provided for unipolar charging based on Fuchs' theory and the birth-and-death theory. The N _ion t value used in this model was obtained by fitting the experimental data of average charge on particles for initially uncharged particles. The results from the analytical solution show very good agreements with experimental data regarding the relationship between the pre-existing charge and the final charge on particles (50–200 nm in this study). Experimental tests of the response of Nanoparticle Surface Area Monitor (NSAM) against initially charged particles demonstrated that NSAM could have a large response deviation (more than 20% in the tested charge level) depending on the particle size and the amount of pre-existing positive charges on particles. Modeling of NSAM response showed similar deviation and predicted that when pre-existing charge is high enough, the NSAM response can be as large as 5 and 9 times of the uncharged particle response for alveolar and tracheobronchial surface area concentration, respectively.     

An Ion Generator for Neutralizing Concentrated Aerosols

An ion generator was developed to neutralize concentrated streams of large, highly charged particles in a low-velocity wind tunnel. The aerosol stream tested consisted of 30 mu m aluminum oxide particles (aerodynamic diameter 52 mu m) at a flow rate of 9.6 m³/h (160 L min) and a mass concentration of 43 g/m³. The average number of excess charges per particle was 240,000 (positive), which corresponds to a neutralizing current requirement of 0.11 mu A. Neutralization to < +/- 10,000 charges per particle was necessary to prevent electrostatic sampling artifacts. Neutralization with radioactive sources would have required an impractically large source. The ion generator, constructed from 21 and 32 mm PVC pipe, has 4 peripheral radial electrodes of 0.5 mm tungsten wire and a 2.0 mm diameter central electrode. The aerosol flowed through the ion generator along its axis. The ion generator was powered by an adjustable (0-8.5 kV) power supply. Performance of the ion generator was monitored with an isokinetic Faraday-cup sampler connected to a Keithley Model 6512 electrometer capable of 0.1 fA resolution. The sampler used a stainless steel 47 mm filter holder as the Faraday cup. The cup was insulated with Teflon inside a 90 mm diameter stainless steel enclosure with a 21 mm diameter inlet. This setup gave near real-time measure ment of the charge state of the aerosol in the wind tunnel. By adjusting the ion generator power supply, particle charge could be reduced to < 2% of its original charge. Ion generator output was sufficiently stable to maintain the particle charge within +/- 2% of the original charge over a 1 h period. These reduced charge levels are comparable to charge levels found on workplace aerosols.     

A novel bipolar charger for submicron aerosol particles using carbon fiber ionizers

A simple and novel bipolar charging device using carbon fiber ionizers was developed to neutralize submicron aerosol particles without the generation of ozone. The ion currents of the positive and negative ions generated by carbon fiber ionizers were so chosen as to optimize particle neutralization. The particle penetration, charging probability and charge distribution resulting from the charger were investigated and compared to those from a Kr-85 radioactive neutralizer for the particles in the size range of 20–120 nm. Size distributions for various laboratory-generated aerosols (sodium chloride, ammonium nitrate, ammonium sulfate and glutaric acid) neutralized by the charger were also investigated and compared to those obtained without neutralization. Particle penetration in the charger was over 90% for particles larger than 20 nm. Charging probability and charge distribution for the charger were in good agreement with those from Kr-85 neutralizer and with theoretical estimations. Size distributions observed for the charger and Kr-85 neutralizer were also in good agreement for particles of different concentrations and various chemical compositions. The newly developed bipolar carbon fiber charger can neutralize submicron particles, at least as effectively as currently available radioactive neutralizers and with negligible ozone generation which is its major advantage.     

Effects of specific adsorption of copper (II) ion on charge transfer reaction at the thin film LiMn2O4 electrode/aqueous electrolyte interface

This study investigated the effect of a specific adsorption ion, copper (II) ion, on the kinetics of the charge transfer reaction at a LiMn₂O₄ thin film electrode/aqueous solution (1 mol dm⁻³ LiNO₃) interface. The zeta potential of LiMn₂O₄ particles showed a negative value in 1 × 10⁻² mol dm⁻³ LiNO₃ aqueous solution, while it was measured as positive in the presence of 1 × 10⁻² mol dm⁻³ Cu(NO₃)₂ in the solution. The presence of copper (II) ions in the solution increased the charge transfer resistance, and CV measurement revealed that the lithium insertion/extraction reaction was retarded by the presence of small amount of copper (II) ions. The activation energy for the charge transfer reaction in the solution with Cu(NO₃)₂ was estimated to be 35 kJ mol⁻¹, which was ca. 10 kJ mol⁻¹ larger than that observed in the solution without Cu(NO₃)₂. These results suggest that the interaction between the lithium ion and electrode surface is a factor in the kinetics of charge transfer reaction.     

Study of a Nanoparticle Charger Containing Multiple Discharging Wires in a Tube

Abstract

A unipolar charger containing multiple discharging wires in a tube (inner diameter: 50 mm) was developed and tested in order to increase the aerosol flow rate and the charging efficiency of nanoparticles. Four gold wires of 25 µm in diameter and 15 mm in length were used as the discharging electrodes to generate positive ions (N_i) from 2.72 × 10⁸ ions/cc to 3.87 × 10⁹ ions/cc in concentration at the discharging voltage of + 4.0 ～ + 10 KV. Monodisperse NaCl particles of 10 ～ 50 nm in diameter were used to test the charging efficiency and the particle loss of charged particles with different aerosol flow rates, corona voltages and sheath flow rates. The sheath air near the tube wall was found to increase the extrinsic charging efficiency, and the highest efficiency was obtained at + 6.0 KV discharging voltage, 10 L/min aerosol flow rate and 9 L/min sheath flow rate. The extrinsic charging efficiency increased from 10.6% to 74.2% when the particle diameter was increased from 10 to 50 nm. The TDMA (tandem differential mobility analyzer) method was used to determine the charge distribution and the mean charge per particle and it was found that the Fuchs charging theory corrected for the extrinsic charging efficiency matched with the experimental data very well.     

Mathematical Description of Experimentally Determined Charge Distributions of a Unipolar Diffusion Charger

The charge distributions of an improved opposed flow unipolar diffusion charger were measured using a tandem differential mobility analyzer (DMA) set up in a size range of approximately 20–400 nm. The charger is intended to be used in a portable aerosol sizer to measure particle size distributions. The determined charge distributions were represented by lognormal distributions, and a set of equations and coefficients was developed to calculate the charge distributions. These equations can be easily implemented in software for size distribution measurements. The agreement between the mathematically derived and measured charge distributions is very good, with regression coefficients R ² > 0.96. The investigations showed that approximately 55% of 20-nm particles remain uncharged, while up to 25 elementary charges need to be considered for multiple charge correction of 400-nm particles. Comparison with the Fuchs theory delivered satisfying agreement with the measured average charge levels, but charge distributions cannot be described by the Fuchs theory, likely caused by the charger geometry.

Copyright 2012 American Association for Aerosol Research     

Processing and properties of aligned multi-walled carbon nanotube/aluminoborosilicate glass composites made by sol-gel processing

We describe a novel sol-gel based approach for producing aluminoborosilicate glass composites containing continuous, aligned carbon nanotubes. The process involves the production of aligned carbon nanotubes (ACNT) via aerosol chemical vapour deposition (CVD), followed by infiltration of the ACNT with aluminoborosilicate sol. The advantages of this process are three fold: (1) aerosol CVD is an efficient method of producing clean, aligned arrays of CNTs, (2) sol-gel chemistry provides a simple route to infiltration of the ACNTs, and (3) carbon nanotube (CNT) agglomeration problems associated with CNT composites are circumvented. ACNTs (carpets) with heights of up to 4.4 mm were grown with areas of 10 mm × 20 mm for composite fabrication. The composite showed extensive pullout of the CNTs on a fracture surface and improved thermal and electrical conductivities of 16 Wm⁻¹ K⁻¹ and 5-8 × 10² S m⁻¹ respectively compared with only 1.2 W m⁻¹ K⁻¹ and 10⁻¹³ S m⁻¹ for the monolithic glass.     

Ozone-free post-DBD aerosol bipolar diffusion charger: Evaluation as neutralizer for SMPS size distribution measurements

A postplasma neutralizer for submicron particles size measurements by mobility analysis has been evaluated. Bipolar ion currents have been measured downstream a dielectric barrier discharge (DBD) to estimate the ion fluxes at the inlet of charging volume and the n_i·τ product that define the theoretical maximal concentration that can be neutralized. Charge distributions were measured versus DBD voltage, aerosol diameter and concentration for monodisperse aerosols. It is confirmed that the charge distribution of particles depends on the ratio of initial positive and negative ion currents controlled by the DBD voltage leading to a tuneable mean charge of aerosol in this post-DBD bipolar charger. As expected from Gunn's law, the mean charge and the variance are proportional to particle diameter above 50 nm and independent of the aerosol concentration. The size distributions measured with ⁸⁵Kr and post-DBD neutralizer present the same modal diameters and a maximal overestimation of the total concentration of 10%, for aerosol from 15 to 730 nm with concentrations up to 6 × 10¹² m^?3. This post-DBD bipolar charger can be used for submicron aerosol neutralization and thus for scanning mobility particle sizer size distribution measurements in air as well as in nitrogen to suppress ozone downstream DBD.

Copyright © 2017 American Association for Aerosol Research     

Electrochemically instantaneous reduction of conducting polyaniline-coated latex particles dispersed in acidic solution

A cathodic voltammetric wave was observed in an aqueous suspension of mono-dispersed, spherical polyaniline-coated polystyrene particles, whereas no anodic wave was detected. This irreversibility was common to particles with eight different diameters ranging from 0.2 to 7.5 μm. Such irreversibility cannot be found at polyaniline-coated electrodes, and thus is a property of the dispersion of polyaniline latex. The reduction current was controlled by diffusion of dispersed particles. The reduction, being the conversion from the electrical conducting state to the resistive one, should begin at a point of contact between the conducting particle and the electrode in order to be propagated to the whole particle rapidly. In contrast, the oxidation proceeds slowly with the propagation of conducting zone, during which Brownian motion lets the particle detach from the electrode. The number of loaded aniline units per particle, determined by weight analysis, ranged from 6 × 10⁶ (Ø 0.2 μm) to 3 × 10¹¹ (Ø 7.5 μm) and was proportional to 2.9 powers of the particle diameter. The diffusion-controlled current of the cathodic wave was proportional to 2.4 powers of the diameter. The difference in these powers, 0.5, agreed with a theoretical estimation of the diffusion-controlled current, the diffusion coefficient for which was given by the Stokes-Einstein equation.     

An Improved Method for Charging Submicron and Nano Particles with Uniform Charging Performance

An improved method for charging submicron and nano silver particles with uniform charging performance was developed. Monodisperse silver particles were grown into microdroplets through condensation. The aerodynamic diameter and GSD of the condensed droplets were the same regardless of their original diameter. The diameter of the droplets increased from 1.7μm to 2.5 μm as the temperature of the saturator increased from 45°C to 55°C. They were charged by an indirect corona-based charger, in which the ion-generation zone is followed by a particle-charging zone through which the condensed droplets pass. The charges of the droplets were controlled by varying the droplet size, ion concentration, and strength of electric field in the charger. The solvent of the charged droplets was evaporated in an evaporator. The size distribution of the evaporated particles was measured by SMPS spectrometer and compared with their original size distribution. The particles after evaporation were slightly larger than their original particles, due to recondensation. The total charge and number concentration of the particles were measured by aerosol electrometer and CPC, to calculate the average charge. Their electrical mobility distribution was measured by SMPS spectrometer without a neutralizer, to calculate the charge distribution and average charge of the evaporated particles. The results showed the average charges of the particles were similar, regardless of initial diameter and manner of calculation. The charge distributions of the evaporated particles were identical, except for 16.9 nm particles. Ion evaporation phenomenon of particles smaller than 40 nm in diameter was not detected.