Maximizing the singly charged fraction of sub-micrometer particles using a unipolar charger

Particle charging via the mixing of aerosols with unipolar ions typically results in multiple charges on particles. Particle classification and sizing, based on the electrical mobility, ideally requires all the particles being singly charged to the performance enhancement. In this study, we explored the feasibility of maximizing the singly charged fraction of particles via the control of the N_it product in a unipolar charger. The feasibility was first investigated by modeling unipolar diffusion charging. It was found that the singly charged fraction of monodisperse particles could be maximized by the control of the N_it product. A corona-based unipolar charger was also constructed to study the maximization of the singly charged fraction of monodisperse particles. It was found that a wider range of ion concentration in the charging zone could be obtained by the variation of ion-driving voltage compared to that by changing the corona-discharge current. The maximum singly charged fraction of monodisperse particles in various sizes was characterized when the charger was operated at the flow rates of 1.5 and 3.0 lpm. It was evidenced that the current charger could be conditioned to achieve a higher singly charged fraction of particles than that by bipolar chargers in the particle size range of 20–200?nm, particularly in the ultrafine particle size range. The control of N_it product in the charging zone of a unipolar charger offers a simple and effective means to enhance the singly charged fraction of particles in a given size range.

Copyright © 2019 American Association for Aerosol Research     

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.     

Unipolar Charging of Fine and Ultra-Fine Particles Using Carbon Fiber Ionizers

A simple and novel unipolar charger using carbon fiber ionizers was developed to effectively charge fine and ultra-fine aerosol particles without the generation of ozone. The particle penetration in the charger was investigated for non-charged, neutralized, and singly charged particles in the size range of 20–200 nm. Particle loss and the intrinsic, exit and extrinsic charging efficiencies of fine and ultra-fine particles were also investigated for non-charged particles at different applied voltages to the charger. Particle penetrations in the charger were nearly 100% for particles larger than 20 nm, irrespective of the initial particle charging state. Particle losses in the charger could be decreased by decreasing the applied voltage to the charger from 4.0 kV to 2.3 kV. The intrinsic charging efficiencies were proportionally increased with the applied voltage, whereas the exit charging efficiencies were almost independent of the applied voltage. Therefore, the extrinsic charging efficiency of the charger becomes higher for the lower applied voltage (2.3 kV), at which about 60% of 20 nm particles were charged. Little (less than 4 ppb) to no ozone was generated under all operation conditions. It can be concluded that the newly developed unipolar charger using carbon fiber ionizers can charge fine and ultra-fine particles at least as effectively as currently available unipolar chargers, but with the major advantage of negligible ozone generation, a highly desirable feature if the charged particles are to be used for chemical or biological analysis.     

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.     

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.     

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     

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.     

Unipolar Field and Diffusion Charging in the Transition Regime—Part II: Charging Experiments

Unipolar charging of narrowly distributed 30–100 nm DEHS aerosols in air is investigated, in order to determine the influence of the external electric field (E ₀ ≤ 5 kV/cm) and high charging intensities (n·t ≤ 5 · 10 ¹⁴ s/m ³ ) on the charging efficiency. The results are compared with a combined diffusion and field charging model based on the limiting-sphere concept described in Part I.

The experiments were carried out in a wire corona charger under conditions of complete radial turbulent mixing, which makes the determination of charging history straightforward and very accurate. The state of mixing was verified on the basis of the Deutsch model, by separate measurements of particle losses.

For positive charging, the agreement between measured and predicted mean charge was generally better than 5% for particles larger than 45 nm, which typically carried more than 4 unit charges; for 30 nm particles and relatively low charge levels the uncertainties in the model lead to deviations up to 30%.

In case of negative charging, the observed charge levels progressively exceeded those predicted on the basis of mean ion mobilities by factors up to 2 as the charging intensity increased, and there was evidence of additional charging by free electrons.     

Improvement of the Nanoparticle Charging Efficiency of a Single-Wire Corona Unipolar Charger by Using Radial Sheath Airflow: Numerical Study

A single-wire corona unipolar charger with radial sheath air was proposed to enhance the nanoparticle charging efficiency. The charger consists of an insulated Teflon tube (inner diameter = 6.35 mm) with a 6 mm-long grounded porous metal tube placed at its center from which radial sheath air is introduced, and a discharge gold wire of 50 μm in the outer diameter and 6 mm in the effective length. The performance of the charger was evaluated and optimized numerically. The effect of the position of the sheath air opening on reducing charged particle loss was found to be important and two designs were studied. In design 1, both ends of the 6 mm wide sheath air opening are aligned with the ends of the 6 mm-long discharge wire, while in design 2 the sheath air opening is shifted 2 mm toward the left of the leading edge of the wire. At the same operating condition, design 2 was found to have less electrostatic loss than design 1 because of its smaller deposition region for charged particles. Compared to two unipolar chargers with the highest extrinsic charging efficiency for particles smaller than 10 nm in diameter, design 2 operated at the applied voltage of +3.5 kV, aerosol flow rate of 0.5 L/min, and sheath airflow rate of 0.7 L/min has a comparable extrinsic charging efficiency of 17.2%–70.5% based on particle number for particles ranging from 2.5 to 10 nm in diameter.

Copyright 2013 American Association for Aerosol Research     

Induction Charging and Electrostatic Classification of Micrometer-Size Particles for Investigating the Electrobiological Properties of Airborne Microorganisms

Our earlier studies have shown that the electrostatic collection technique, a potentially "gentle" bioaerosol collection method, allows for efficient collection of airborne bacteria, but sensitive bacteria such as Pseudomonas fluorescens ( P. fluorescens ) lose their culturability during collection. We hypothesized that excessive stress was imposed on the sensitive bacteria by the sampler's conventional corona charging mechanism. In this research, we developed and built an experimental setup that allows us to analyze electrobiological properties of airborne microorganisms. In this experimental system, we imparted electric charges on airborne biological and nonbiological particles by aerosolizing them in the presence of an electric field. The charged P. fluorescens test bacteria and NaCl test particles were then channeled into a parallel plate mobility analyzer, which we have designed so that bacteria and inert particles carrying specific charge ranges can be extracted and made available for further analysis. When testing the experimental system, we related the extracted particle concentrations to the total particle concentration and obtained the charge distributions of these particles at different charging conditions. Our results have shown that even without charging, aerosolized P. fluorescens bacteria have a net negative charge and can carry up to 13,000 elementary charges per bacterium. In contrast, the NaCl particles were found to carry very few electric charges. We concluded that the electric charge carried by a bacterium consists of 2 components: its own natural charge, which can be high, and the charge imposed on it by the dispersion process. Our experiments have shown that the charge distributions on biological and nonbiological particles can be effectively manipulated by varying the external electric field during their aerosolization. Since airborne microorganisms may carry high internal electric charges, their collection by electrical field forces may be possible without first electrically charging them.     

Charging of Ultra-Fine Aerosol Particles by an Ozone-Free Indirect UV Photo-Charger

Particle charging by indirect photoemission may be an alternative to charging methods based on corona discharge or on bipolar charging by radioactive ion sources. An indirect charger using a low energy UV radiation is introduced and characterized in detail. Depending on the carrier gas, photoelectrons or ions formed by electron-attachment charge the particles by diffusion charging. The achieved charging efficiency is in the range of 20–70% for particle sizes of 20 to 100 nm. It can easily be modulated by a small voltage applied to the photoemitter. To achieve stable electron emission, glassy carbon with its very inert surface is used as photoemitter. Particle losses are very small. The charge distribution has been measured by a tandem DMA setup. The experimental results are compared with the theory of unipolar diffusion charging based on the Fuchs’ combination probability of ions with the particles. The charger characterization has been performed by carbon particles in a size range of 20–100 nm, produced by a spark discharge generator.

Copyright 2013 American Association for Aerosol Research     

The effect of the generation and handling in the acquired electrostatic charge in airborne particles

The measurement of the charge distribution in laboratory generated aerosols particles was carried out. Four cases of electrostatic charge acquisition by aerosol particles were evaluated. In two of these cases, the charges acquired by the particles were naturally derived from the aerosol generation procedure itself, without using any additional charging method. In the other two cases, a corona charger and an impact charger were utilized as supplementary methods for charge generation. Two types of aerosol generators were used in the dispersion of particles in the gas stream: the vibrating orifice generator TSI model 3450 and the rotating plate generator TSI model 3433. In the vibrating orifice generator, a solution of methylene blue was used and the generated particles were mono-dispersed. Different mono-aerosols were generated with particle diameters varying from 6.0 × 10^− 6 m to 1.4 × 10^− 5 m. In the rotating plate generator, a poly-dispersed phosphate rock concentrate with Stokes mean diameter of 1.30 × 10^− 6 m and size range between 1.5 × 10^− 7 m and 8.0 × 10^− 6 m was utilized as powder material in all tests. In the tests performed with the mono-dispersed particles, the median charges of the particles varied between − 3.0 × 10^− 16 C and − 5.0 × 10^− 18 °C and a weak dependence between particle size and charge was observed. The particles were predominantly negatively charged. In the tests with the poly-dispersed particles the median charges varied fairly linearly with the particle diameter and were negative. The order of magnitude of the results obtained is in accordance with data reported in the literature. The charge distribution, in this case, was wider, so that an appreciable amount of particles were positively charged. The relative spread of the distribution varied with the charging method. It was also noticed that the corona charger acted very effectively in charging the particles.     

Bipolar charging and neutralization of nanometer-sized aerosol particles

An experimental study of charging and neutralization of 2.5–10 nm aerosol particles by bipolar air ions has been carried out. The time required to attain the charge equilibrium state, both for charging of initially uncharged particles and for neutralization of charged particles, has been previously determined using different-sized diffusive type chargers. To avoid sizing errors caused by space charge field and Brownian diffusion effects, a tandem DMA (differential mobility analyzer) system has been used. The first DMA classifies a certain fraction of particles, and the second one allows precise determination of their size. The experimental charging probabilities at equilibrium are in relatively good agreement with calculations based on Fuchs' theory, except in the particle size range below 3 nm where large deviations have been observed.     

Bench-scale tests to determine mechanisms of charge generation due to particle-particle and particle-wall contact in binary systems of fine and coarse particles

Bench-scale methods were utilized to determine changes in electrostatic charges and their mechanisms for various coarse and fine particles as they came into contact with each other and/or their containing vessel walls. Techniques included shaking tests and particle-copper plate contacting experiments. Electrostatic behaviour of coarse particles (glass beads and polyethylene) and fine particles (Larostat 519, glass beads and silver-coated glass beads) were investigated. Shaking tests resulted in charge separation in which the fine particles acquired significant positive charges, opposite to those carried by the large particles. In copper-plate contacting tests, charge transfer occurred between the fines and the copper plate with fines carrying away almost all of the initial charges on the plate followed by further charge separation. Charge separation was found to be the dominant charging mechanism between the coarse particle and copper plate, with the particles becoming negatively charged.     

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.     

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).     

Enhancement of Extrinsic Charging Efficiency of a Nanoparticle Charger with Multiple Discharging Wires

A unipolar charger with multiple discharging wires has been developed and investigated to enhance the extrinsic charging efficiency of nanoparticles by using sheath air near the wall of the charger. The applied voltage of the charger ranged from +4.0 to +10 kV, corresponding to corona current from 0.02 to 119.63 μA. Monodisperse NaCl particles of 10 ～ 50 nm and Ag particles of 2.5 ～ 10 nm in diameter were produced to test the performance of the charger with multiple discharging wires and to investigate the particle loss at different sheath flow rates, corona voltages and sheath air velocities. Results showed that the optimal efficiency in the charger was obtained at +9 kV applied voltage, 10 L/min aerosol flow rate and 20 L/min sheath air flow rate. The extrinsic charging efficiency increased from 2.86% to 86.3% in the charger as the particle diameter increasing from 2.5 to 50 nm. The TDMA (tandem-differential mobility analyzer) technique was used to investigate the charge distribution, and the charge distributions in the exit were obtained at the optimal operating condition.     

Particle charge-size distribution measurement using a differential mobility analyzer and an electrical low pressure impactor

We introduce a particle charge-size distribution measurement method using a differential mobility analyzer and an electrical low pressure impactor in tandem configuration. The main advantage of this type of measurement is that it is suitable for a wide range of particle sizes, from approximately 30 nm up to a micrometer, and for high charge levels, which have been problematic for previously used methods. The developed charge measurement method requires information on the particle effective density, and the accuracy of the measurement is dependent on how well the particle effective density is known or estimated. We introduce the measurement and calculation procedures and test these in laboratory conditions. The developed method has been tested using narrow and wide particle size distributions of a known density and well-defined particle charging states. The particles have been produced by the Singly Charged Aerosol Reference (SCAR) and an atomizer and charged with the previously well-characterized unipolar diffusion chargers used in the Nanoparticle Surface Area Monitor (NSAM) and in the Electrical Low Pressure Impactor (ELPI+). The acquired charge-size distributions are in good agreement with the reference values in terms of the median charge levels and widths of the charge distributions.

Copyright © 2017 American Association for Aerosol Research