Inertial Separation of Ultrafine Particles Using a Condensational Growth/Virtual Impaction System

ABSTRACT

A system for the separation of ultrafine particles (i.e., particles smaller than 0.1 μm) has been developed and evaluated. Ultrafine particles are first grown by means of supersaturation to a size that can be easily separated in a virtual impactor. Thus, inertial separation of ultrafine particles occurs without subjecting them to a high vacuum. The condensational growth/virtual impaction system has been evaluated using monodisperse 0.05 and 0.1 μm fluorescent PSL particles, as well as polydisperse ultrafine ammonium sulfate and potassium nitrate aerosols. The generated aerosols were first drawn over a pool of warm water (50°C) where they became saturated. Subsequently, the saturated aerosol was drawn through a cooling tube (8°C) where particles grew due to supersaturation to sizes in the range 1.0–4.0 μm. By placing a virtual impactor with a theoretical 50% cutpoint of 1.4 μm downstream of the condenser, ultrafine particles were separated from the majority (i.e., 90%) of the surrounding gas. The sampling flow rate of the virtual impactor was 8 L/min and its minor-to-total flow ratio was 0.1. For these operating conditions, the particle collection efficiency of the virtual impactor averaged to about 0.9 for particle concentrations in the range 7 × 10⁴-5 × 10⁵ particles/cm³. Particle losses through the system were found less than 5%. Increasing the particle concentration to levels in the range 106–107 particles/cm³ resulted in a decrease in the collection efficiency of the virtual impactor to about 50–70%, presumably due to the smaller final droplet size to which the ultrafine particles grew for the available supersaturation.     

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.     

Chemical Characterization of Flowing Polydisperse Aerosols by Raman Spectroscopy

We have applied Raman spectroscopy to the in-situ measurement of chemical composition of polydisperse flowing aerosols. Monodisperse and polydisperse aerosols in the size range 0.3 to 1.8 w m, composed of diethylsebacate (DES) and ammonium sulfate, were generated. The particles were irradiated with 514.5 nm laser light and Raman spectra were collected. The Raman intensities of DES at 2935 cm -1 and ammonium sulfate at 981 cm -1 , normalized by the nitrogen carrier gas Raman intensity at 2313 cm -1 , were approximately proportional to the aerosol mass loading over the particle size range studied. Calculations based on previous theoretical studies support this observation. The mass loading ranged from 0.17 to 12.8 g/m 3 for DES and 20 to 138 mg/m 3 for ammonium sulfate. The method was applied to mixing aerosol streams containing DES and ammonium sulfate in a turbulent jet. The Raman system, with a sensitive volume of 0.02 mm 3 , was used to measure radial and axial concentration profiles in the mixing region. The results compared well with turbulent mixing theory. The primary limitation for application of the method is the low signal to noise ratio.     

Analytic Solutions to Diffusional Deposition of Polydisperse Aerosols in Fibrous Filters

Deposition of polydisperse aerosols by Brownian diffusion was studied analytically using the penetration efficiency of monodisperse aerosols combined with the correlations among the moments of lognormal distribution functions. The analytic solutions, so obtained were validated using the exact solutions, which were applied to recalculate the filtration efficiencies of the existing experimental data for various filtration conditions. It was found that the collection efficiency of a fibrous filter should be corrected with respect to the position in the filter, if the particles are polydisperse. By considering the effect of the polydispersity of particle size, the analytic solutions showed good agreement with existing experimental data. It is believed that the present work makes it possible to determine the filtration efficiency of polydisperse aerosols in fibrous filters and to estimate errors associated with the degree of polydispersity of the particles quickly and accurately for the diffusion dominant regime.     

Size Distribution Measurement of Carbonaceous Particulate Matter Using a Low Pressure Impactor with Quartz Fiber Substrates

The collection characteristics of a small deposit area low pressure impactor (SDI) were studied in order to employ the impactor for size distribution measurements of carbonaceous matter. In this work, the SDI was calibrated for soft and porous quartz substrate material in a series of laboratory experiments. The collection efficiency curves were measured by using monodisperse dioctyl sebacate particles and by applying two different detection methods. One method was based on the detection of current carried by charged test particles, and the other measured number concentrations of particles in bipolar charge equilibrium by two condensation particle counters. Concerning the particle size corresponding to a 50% collection efficiency (D ₅₀ ), significant shifts toward smaller particle sizes were found for the quartz fiber substrates compared with the flat plates. Also the shapes of the collection efficiency curves differed considerably: quartz substrate gave less steep curves than plain impaction plates. The new calibration was applied to field data from urban and rural sites. Compared with the original calibration of the SDI, the new calibration changed the measured size distributions of organic and elemental carbon. In addition, a reasonable size-segregated mass closure was achieved by combining data from thermal-optical analysis and ion-chromatography.     

Condensational Growth of Polydisperse Aerosol for the Entire Particle Size Range

The condensation problem of polydisperse aerosols is investigated theoretically. The single particle growth rate suggested by Kulmala (1993) is approximated and simplified by neglecting the Kelvin effect and by adopting the harmonic mean method for the transition correction, which is a good approximation of the representative flux-matching theories. An analytical solution to the particle size distribution change by condensation is derived in an explicit form using the modified growth rate. This study represents the first analytical solution to the condensation problem of polydisperse aerosols for the entire particle size range. The derived solution is compared with results of the previous study of Kulmala (1993) and is shown to be reasonably accurate, except for very small particles for which the Kelvin effect cannot be neglected.     

Single Charging of Nanoparticles by UV Photoionization at High Flow Rates

The feasibility of UV photoionization for single unipolar charging of nanoparticles at flow rates up to 100 l· min ^?1 is demonstrated. The charging level of the aerosol particles can be varied by adjusting the intensity of the UV radiation. The suitability of a UV photocharger followed by a DMA to deliver monodisperse nanoparticles at high aerosol flow rates has been assessed experimentally in comparison to a radioactive bipolar charger ( ⁸⁵ Kr, 10 mCi). Monodisperse aerosols with particle sizes in the range of 5 to 25 nm and number concentrations between 10 ⁴ and 10 ⁵ cm ^?3 have been obtained at flow rates up to 100 l· min ^?1 with the two aerosol chargers. In terms of output particle concentration, the UV photoionizer performs better than the radioactive ionizer with increasing aerosol flow rate. Aerosol charging in the UV photoionizer is described by means of a photoelectric charging model that relies on an empirical parameter and of a diffusion charging model based on the Fuchs theory. The UV photocharger behaved as a quasi-unipolar charger for polydisperse aerosols with particles sizes less than 30 nm and number concentrations ～10 ⁷ cm ^?3 . Much reduced diffusion charging was observed in the experiments, with respect to the calculations, likely due to ion losses onto the walls caused by unsteady electric fields in the irradiation region.     

Development of polydisperse aerosol generation and measurement procedures for wind tunnel evaluation of size-selective aerosol samplers

Accurate development and evaluation of inlets for representatively collecting ambient particulate matter typically involves the use of monodisperse particles in aerosol wind tunnels. However, the resource requirements of using monodisperse aerosols for inlet evaluation creates the need for more rapid and less-expensive techniques to enable determination of size-selective performance in aerosol wind tunnels. The goal of recent wind tunnel research at the U.S. EPA was to develop and validate the use of polydisperse aerosols, which provide more rapid, less resource-intensive test results, which still meet data quality requirements necessary for developing and evaluating ambient aerosol inlets. This goal was successfully achieved through comprehensive efforts regarding polydisperse aerosol generation, dispersion, collection, extraction, and analysis over a wide range of aerodynamic particle sizes. Using proper experimental techniques, a sampler’s complete size-selective efficiency curve can be estimated with polydisperse aerosols in a single test, as opposed to the use of monodisperse aerosols, which require conducting multiple tests using several different particle sizes. While this polydisperse aerosol technique is not proposed as a regulatory substitute for use of monodisperse aerosols, the use of polydisperse aerosols is advantageous during an inlet’s development where variables of sampling flow rate and inlet geometry are often iteratively evaluated before a final inlet design can be successfully achieved. Complete Standard Operating Procedures for the generation, collection, and analysis of polydisperse calibration aerosols are available from EPA as downloadable files. The described experimental methods will be of value to other researchers during the development of ambient sampling inlets and size-selective evaluation of the inlets in aerosol wind tunnels.

© 2018 American Association for Aerosol Research     

Evaluation of a High Volume Aerosol Concentrator

A virtual impactor sampler, which is designed to concentrate aerosols from a 1000 L/min ambient air sample into a 1 L/min exhaust airflow stream, was tested with near monodisperse aerosols in aerosol wind tunnels to characterize sampling performance. New methodology is introduced to correct results for the presence of doublet and satellite aerosol particles that can be present in the particle size distribution from a vibrating jet atomizer. Aerosol penetration from the free stream near the sampler inlet to the outlet of the device has a peak value of 78% at a particle size of 3.9 w m AD. Sampling effectiveness, which is the mean penetration over the size range of 2.5 to 10 w m AD, is 48%. There are 4 virtual impaction stages in the sampler, and examination of the regional losses shows that most of the aerosol deposition occurs on surfaces of the last 2 stages. The ideal power expenditure of the sampler (excluding electrical and frictional losses in the motor and bearing losses in the blower) is 58 watts as compared to the actual power consumption of 320 watts.     

The effect of polydispersity on dust lifting behind shock waves

Knowledge-based modeling of dust lifting behind shock waves is a prerequisite for realistic simulation of dust explosions. Mostly numerical simulations of this process focus on dusts consisting of monodisperse particles, while real dusts are polydisperse. This article investigates the effect on the lifting process of the dust being polydisperse with a log–normal distribution of particle sizes. The spatial distribution of the various sizes in the rising layer is studied, and statistical results for the rise, the collision frequency and the particle kinetic energy are compared for polydisperse and monodisperse dusts. It is shown that a layer consisting of polydisperse particles rises significantly faster than a one consisting of monodisperse particles, all other parameters being the same.     

Particle Bounce During Filtration of Particles on Wet and Dry Filters

This paper experimentally examines the bounce and immediate re-entrainment of liquid and solid monodisperse aerosols under a stable filtration regime (precake formation) by wet and dry fibrous filters. PSL and DEHS were the solid and liquid aerosols, respectively, used in four monodisperse sizes of 0.52, 0.83, 1.50, and 3.00 w m. Three different fibrous filters were used to filter the aerosol streams, and the efficiency of the filtration process for each aerosol type under dry and wet regimes was measured. It was found that the solid particles generally exhibited a lower fractional filtration efficiency than liquid particles, although this difference decreased in the smaller size fractions. The difference between solid and liquid efficiencies was found to be greatest in the 1.5 w m size range. As particle sizes of liquid/solid aerosols and filtration parameters were similar, this difference is most likely to be due to the effect of particle bounce and or immediate re-entrainment occurring inside the filter, with the greater efficiency of filtration of the liquid particles being due to their greater capacity to plastically/elastically deform in order to absorb the impact forces. However, for the wet filtration regime (each fibre of the filter was coated by a film of water), no significant difference in filtration efficiency was detectable between solid and liquid aerosols. Therefore, the conclusion can be drawn that the either the bounce effect of the particles is inhibited by the liquid film, or the filtration conditions in the wet filter are so different that the aerosol properties are less significant with respect to capture.     

Continuous Measurements of Ambient Particle Deposition in Human Subjects

The total deposition fraction (TDF) of fine and ultrafine aerosols was measured in a group of six healthy adults exposed to polydisperse ambient aerosols in Boston. Fifteen repeated inhalation-exhalation cycles were conducted during a given exposure session. Deposition efficiency for particles with aerodynamic diameter ranging from 63.5 to 2045 nm was determined using the average concentration of inhaled and exhaled particles measured during these cycles. Deposition efficiencies ranged from 7.3±18.7%(240-275 nm) to 98.6±28.1%(1545-2045 nm). Subjects exhibited similar deposition patterns with minimum efficiencies between 200-400 nm. Results from ANOVA and mixed-model regression analyses showed significant differences (p < 0.05) in particle deposition efficiency by particle size as well as among the subjects. Deposition efficiencies varied most among the subjects for particles between 100 and 1000 nm in size. A comparison with the ICRP model showed good agreement, with best agreement for male subjects and particle sizes <400 nm.     

Generation of Submicron Mass/Volume-Monodisperse Aerosols with a Nebulizer-Impactor-Electrostatic Classifier System

A study was undertaken to investigate the mass size dispersion of particles classified according to their electrical mobilities. This is of primary concern in experiments that measure a concentration dependent property of the classified particles. Initially, the mass size distribution of particles produced by the 3-jet Collison, 6-jet Collison, and Misty-Ox nebulizers was measured. A 0–2 stage impactor was placed after the nebulizers and the size mass distribution was measured again. The polydisperse particle stream was then used to generate “size classified” aerosol and the mass size distribution of the equal mobility particles was calculated and measured. It was found that without an impactor in line, the aerosol stream contained a significant mass fraction of multiply charged particles. When an impactor was inserted directly after the nebulizers, the multiply charged particles were effectively removed and the particles were nearly monodisperse.     

Detection and Analysis of Aerosol Particles by Laser-Induced Breakdown Spectroscopy

Laser-induced breakdown spectroscopy (LIBS) was evaluated as a means for quantitative analysis of the size, mass, and composition of individual micron-to submicron-sized aerosol particles over a range of well-characterized experimental conditions. Conditional data analysis was used to identify LIBS spectra that correspond to discrete aerosol particles under low aerosol particle loadings. The size distributions of monodisperse particle source flows were measured using the LIBS technique for calcium- and magnesium-based aerosols. The resulting size distributions were in good agreement with independently measured size distribution data. A lower size detection limit of 175 nm was determined for the calcium- and magnesium-based particles, which corresponds to a detectable mass of approximately 3 femtograms. In addition, the accuracy of the LIBS technique for the interference-free analysis of different particle types was verified using a binary aerosol system of calcium-based and chromium particles.     

A coupled DEM/CFD analysis of the effect of air on powder flow during die filling

Die filling from a stationary shoe in a vacuum and in the presence of air was numerically analyzed using an Eulerian‐Lagrangian model, which employs a discrete element method (DEM) for the particles and computational fluid dynamics (CFD) for the air with a two‐way air‐particle interaction coupling term. Monodisperse and polydisperse powder systems have been simulated to explore the effect of the presence of air on the die filling process. For die filling with monodisperse powders, the influences of particle size and density on the flow behavior were explored. The numerical simulations revealed that the presence of air has a significant impact on the powder flow behavior, especially for systems with smaller and/or lighter particles. Flow has been characterized in terms of a dimensionless mass flow rate, and it has been shown that for die filling in a vacuum this is constant. The flow characteristics for die filling in air can be classified into two regimes. There is an air‐inert regime in which the particle size and density are sufficiently large that the effect of air flow becomes negligible, and the dimensionless mass flow rate is essentially identical to that obtained for die filling in a vacuum. There is also an air‐sensitive regime, for smaller particle sizes and lower particle densities, in which the dimensionless mass flow rate increases as the particle size and density increase. The effects of particle‐size distribution and adhesion on the flow behavior have also been investigated. It was found that, in a vacuum, the dimensionless mass flow rate for polydisperse systems is nearly identical to that for monodisperse systems. In the presence of air, a lower dimensionless mass flow rate is obtained for polydisperse systems compared to monodisperse systems, demonstrating that air effects become more significant. Furthermore, it has been shown that, as expected, the dimensionless mass flow rate decreases as the surface energy increases (i.e., for more cohesive powders). © 2008 American Institute of Chemical Engineers AIChE J, 2009     

Effect of solid monodisperse particles on the pressure drop of fibrous filters

The increase in pressure drop across glass HEPA filters has been measured as a function of particle mass loading using polystyrene latex particles (PSL). PSL particles in several different sizes were generated as challenge aerosols. For each particle size distribution, the specific resistance (K₂) was calculated by measuring the mass of PSL particles loaded per unit area of filter and the pressure drop across the filters at a given filtration velocity. In all cases, the specific resistance of the filter cake increased as the aerodynamic mean particle diameter decreased at the same mass loading. This correlation equation was modified by using the lognormal conversion method suggested by Raabe [1971] for a polydisperse particle size distribution; then the modified equation was expressed as a function of geometric mean particle diameter and standard deviation which could be obtained by the measuring instruments (PDS 3603; TSI Inc.). The advantage of this approach over other methods is the use of a more convenient prediction of pressure drop, if we know the geometric mean particle diameter and standard deviation, which could be easily measured. The values of porosities, obtained from the pressure drop responses of loading in the filters using the Rundnick and First equation, were compared with other researches.     

Penetration measurements for tube and screen-type diffusion batteries in the ultrafine particle size range

Experimental calibrations of tube and screen-type diffusion batteries are made by means of monodisperse particles of diameters ranging from 3.5 to 130 nm. Ultrafine Ag-aerosols are generated by means of a constant-temperature tube furnace. Electrostatic classification of the polydisperse primary aerosol yields monodisperse fractions with electric mobility particle diameters in the size range 3–200 nm. The monodispersity of the test aerosols and the accuracy of the calculated mean particle diameters are confirmed by a particle size analysis by means of the transmission-electron microscopy. The results for the tube diffusion batteries are in good agreement with the theory, if entrance effects and front face deposition are considered. The results for the screen-type diffusion batteries are in agreement with a theory developed by Y. S. Cheng in 1980, which is based on the filtration theory of a fan model filter.     

Virtual Impactor as an Accessory to Optical Particle Counters

A method to improve the sensitivity of optical particle counters for large particles is presented. The basic idea is to increase the concentration in the sample air by connecting a virtual impactor to the sample inlet of an optical particle counter. For particles with D _p > 3 μm, the number concentration is increased by a factor of 20. The improvement in statistical accuracy is particularly useful in Alter testing and clean room measurements. The differences in the size distributions measured with and without the virtual impactor are used in estimating the relationship between the aerodynamic and optical sizes of different aerosols.     

Application of rayleigh spectroscopy to the study of emulsion and dispersion polymerization and polymers

Application of Rayleigh spectroscopy for characterization of particle size in nonaqueous dispersion and water-based emulsion paint resins is described. The technique allows a straightforward and rapid estimation of particle size; the measurement does not require exact determination of scatterer concentration. For monodisperse samples, unambiguous results are obtained for particles at least up to 50 μm in diameter; for polydisperse samples, an average size heavily weighted by large particles is obtained. Typical experimental results on monodisperse and polydisperse water-based latexes and on polydisperse nonaqueous dispersion resins are described. In the latter case, comparison of electron micrograph and light scattering size determinations indicates that the light scattering experiment yields approximately a z-average radius. Observations on particle formation and growth during polymerization are also described.     

Mixing selectivity in bicomponent,bipolar aggregation

The selectivity of aggregation in mixtures of two charged aerosols containing chemically dissimilar nanoparticles is studied by means of a newly developed direct simulation Monte Carlo method. This method allows to trace changes in complex multidimensional systems, in this case describing particle size, charge and aggregate composition. A new procedure was developed for estimating the effective collision diameter of an aggregate composed of primary particles of any size. Three model systems were studied: polydisperse aerosols with initially bipolar charge distribution, unipolarly charged polydisperse aerosols and quasi-monodisperse oppositely charged aerosols. The study is focused on the aggregate composition's dependence on the initial size and charge distribution. It was found that the use of bipolarly charged aerosols does not increase the selectivity of mixing whereas unipolarly, oppositely charged aerosols reach more rapidly a more homogeneous distribution of components within the aggregates. In the last case, the addition of one more elementary charge to the particles roughly doubles the fraction of bicomponent, $\text{1}\text{:}\text{1}$ mixed nanoaggregates and accelerates the process.