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.     

Use of an aerodynamic particle sizer as a real-time monitor in generation of ideal solid aerosols

A method based on real-time responses of an aerodynamic particle sizer (APS) has been developed to monitor the formation of both ideal and nonideal solid aerosol particles. Preliminary studies demonstrated that, at various generating conditions, the morphology change of particles in photomicrographs can be identified from the channel shift in the APS outputs. With this method, the time-consuming conventional way of ensuring the dryness, sphericity and monodispersity of particles with scanning electron microscopic studies is not required. The technique has been used successfully to determine optimum conditions for the generation of monodisperse ammonium fluorescein particles (3–17 μm) with a vibrating orifice aerosol generator under certain operating conditions. The mean density of the particles that were generated was calculated to be 1.35 g cm⁻³.     

Coating of Silica and Titania Aerosol Nanoparticles by Silver Vapor Condensation

Silica and titania aerosol nanoparticles are coated with silver through a physical coating process. The silver is evaporated in a tubular furnace flow system and condensed on the ceramic carrier particles with diameters of approximately 100?nm. The temperature gradient in the furnace system is optimized in order to avoid homogeneous nucleation of the silver. The generated ceramic–silver composite nanoparticles are characterized with aerosol measurements and analytical transmission electron microscopy. Two completely different particle morphologies are clearly observed, silver-decoration and composite doublet, with amorphous silica and crystalline rutile titania as the carrier particles, respectively. The former morphology consists of multiple silver nanodots with diameters of 1–10?nm, while in the latter morphology the silver had formed a larger structure with a size comparable to that of the carrier particle. Different shapes are observed in these larger silver structures, such as triangular, rodlike, and hexagonal. Differences in the silver particle migration on the surface of the silica and titania particles is proposed to be the key factor resulting into the two distinct particle morphologies.

Copyright 2015 American Association for Aerosol Research     

Structural Property Effect of Nanoparticle Agglomerates on Particle Penetration through Fibrous Filter

Most filtration studies have been conducted with spherical particles; however, many aerosol particles are agglomerates of small primary spheres. Filtration efficiency tests were conducted with silver NP agglomerates, with the agglomerate structure controlled by altering the temperature of a sintering furnace. The mobility diameter and mass of the silver NP agglomerates were measured using a differential mobility analyzer together with an aerosol particle mass analyzer. From these measurements, it was found that the fractal-like dimension, D _fm, varied from 2.07 to 2.95 as the sintering temperatures was increased from ambient to 600°C. The agglomerates were essentially fully coalesced at 600°C allowing direct comparison of the filtration behavior of the agglomerate to that of a sphere with the same mobility diameter. Other agglomerate properties measured include the primary diameter, the agglomerate length and aspect ratio, and the dynamic shape factor.

Agglomerate filtration modeling with no adjustable parameters has been investigated in terms of diffusion, impaction, and interception. The model results agree qualitatively with the experimental results in the particle size range of 50 to 300 nm. The results indicated that the larger interception length of agglomerates is responsible for the smaller penetration through a fibrous filter in comparison to spherical particles with the same mobility diameters.     

Method to Determine the Number of Bacterial Spores Within Aerosol Particles

We describe methodology to reveal the number of microbial spores within aerosol particles. The procedure involves visualization under differential- interference-contrast microscopy enhanced by high-resolution photography and further analysis by computer-assisted imaging. The method was used to analyze spore of Bacillus globigii in aerosols generated by a small (pressured metered-dose inhaler type) generator. Particles consisting in 1 or 2 spores accounted for 85% of all generated particles. This percentage rose to 91% when the same aerosol was collected on an Andersen cascade impactor that collected particles larger than 0.65 μm and was even higher (96%) when particles larger than 3.3 μm were also eliminated. These results demonstrate that the imaging analysis of aerosol particles collected on glass slides is sensitive to even relatively small changes in aerosol particle composition. The accuracy of the enhanced microscopic method described herein (differences between visual and computer analysis were approximately 3% of the total particle counts) seems adequate to determine the spore composition of aerosols of interest in biodefense.     

The Effect of Inkjet Operating Parameters on the Size Control of Aerosol Particles

We investigated the effect of inkjet operating parameters on the size control of aerosol particles. Droplets with agglomerates of polystyrene latex particles were generated from an inkjet nozzle and continuously dried up at the temperature of 38°C. When droplets have the size range of 30 to 70 μm in diameter, aerosol particles with the size range of 3.5 to 7.1 μm were generated after the drying process. We controlled the particle size easily within a factor of two by adjusting rising/falling time and voltages of an actuating waveform. Generated particles were shown to have a narrow particle size distribution. Thus, the particle concentration of aqueous suspension does not need to be adjusted precisely in order to control the size of generated aerosol particles.

Copyright © 2015 American Association for Aerosol Research     

Experimental investigation on the particle capture by a single fiber using microscopic image technique

Four kinds of solid particles were captured by a single fiber. The particles included two kinds of fly ash particles and two kinds of ceramic particles under three different types of charging pretreatment. The single fiber was fixed across a square cross-section glass tube. A standard continuous aerosol generator was used to disperse particles to generate a uniform aerosol. The aerosol particles from the generator were tribocharged, polarized or charged, and then passed across the fiber. A microscope and a CCD camera were used to observe the capturing process and the shape distribution of dendrites. The results showed that the deposited particles developed in different ways. In the tribocharged case, dendrite formation can be classified into three distinct stages. In the prepolarized case, straight chains were formed at a uniform spacing interval, and had high binding intensity to support very long chains. Even though the long chains fell over they still had high capturing efficiency. In the precharged case, some straight chains with some branches were formed, but their binding intensity was low and they easily fell over and broke. The results also showed how the particle diameter and shape influenced the formation of dendrites and chains.     

Measurement of size-dependent dynamic shape factors of quartz particles in two flow regimes

Understanding and modeling the behavior of quartz dust particles, commonly found in the atmosphere, requires knowledge of many relevant particle properties, including particle shape. This study uses a single particle mass spectrometer, a differential mobility analyzer, and an aerosol particle mass analyzer to measure quartz aerosol particles mobility (d_m), vacuum aerodynamic, and volume equivalent diameters, mass, composition, effective density, and dynamic shape factor as a function of particle size, in both the free molecular and transition flow regimes. The results clearly demonstrate that dynamic shape factors can vary significantly as a function of particle size. For the quartz samples studied here, the dynamic shape factors increase with size, indicating that larger particles are significantly more aspherical than smaller particles. In addition, dynamic shape factors measured in the free-molecular (χ_v) and transition (χ_t) flow regimes can be significantly different, and these differences vary with the size of the quartz particles. For quartz, χ_v of small (d_m < 200 nm) particles is 1.25, while χ_v of larger particles (d_m ～ 440 nm) is 1.6, with a continuously increasing trend with particle size. In contrast, χ_t of small particles starts at 1.1 increasing slowly to 1.34 for 550 nm diameter particles. The multidimensional particle characterization approach used here goes beyond determination of average properties for each size, to provide additional information about how the particle dynamic shape factor may vary even for particles with the same mass and volume equivalent diameter.

© 2016 American Association for Aerosol Research     

Particle Morphology and Density Characterization by Combined Mobility and Aerodynamic Diameter Measurements. Part 2: Application to Combustion-Generated Soot Aerosols as a Function of Fuel Equivalence Ratio

Composition, shape factor, size, and fractal dimension of soot aerosol particles generated in a propane/O₂, flame were determined as a function of the fuel equivalence ratio (φ). Soot particles were first size-selected by a differential mobility analyzer (DMA) and then analyzed by an Aerodyne aerosol mass spectrometer (AMS). The DMA provides particles of known mobility diameter (d_m ). The AMS quantitatively measures the mass spectrum of the nonrefractory components of the particles and also provides the vacuum aerodynamic diam eter (d_va ) corresponding to the particles of known mobility diameter. The measured d_m, d_va , and nonrefractory composition are used in a system of equations based on the formulation presented in the companion article to estimate the particle dynamic shape factor, total mass, and black carbon (BC) content. Fractal dimension was estimated based on the mass-mobility relationship. Two types of soot particles were observed depending on the fuel equivalence ratio. Type 1: for φ < 4 (lower propane/O₂), d_va ; was nearly constant and independent of d_m . The value of d_va increased with increasing φ. Analysis of the governing equations showed that these particles were highly irregular (likely fractal aggregates), with a dynamic shape factor that increased with d_m and φ. The fractal dimension of these particles was approximately 1.7. These particles were composed mostly of BC, with the organic carbon content increasing as φ increased. At φ = 1.85, the particles were about 90% BC, 5% PAH, and 5% aliphatic hydrocarbon (particle density = 1.80 g/cm³). Type 2: for φ > 4 (high propane/O₂), d_va was linearly proportional to d_m . Analysis of the governing equations showed that these particles were nearly spherical (likely compact aggregates), with a dynamic shape factor of 1.1 (versus 1 for a sphere) and a fr actal dimension of 2.95 (3 for a sphere). These particles were composed of about 50% PAH, 45% BC, and 5% aliphatic hydrocarbons (particle density = 1.50 g/cm³). These results help interpret some measurement s obtained in recent field studies.     

Controlled Generation of Nanoscale Organic Pigments by Adiabatic Expansion in Laval Nozzles and in Expanding Free Jets

As organic pigments are produced mainly in wet chemical processes, a novel gas to particle process for generating organic nanoscale pigments is introduced. This process is based on the expansion of a nearly saturated gas flow from an overpressure regime to ambient pressure conditions.

The expansion is achieved in a Laval nozzle and subsequently continues as an expanding free jet in an expansion chamber. This expansion chamber is equipped with an adjustable cooling system. Copper phthalocyanine and Paliogen Red, two organic pigments, were used as test materials. By controlling the temperature in the expansion chamber, particularly in the free jet, nanoscale pigments with high (needle shape) to low (grainy shape) aspect ratios are generated. Particle size distribution measurements as well as scanning electron microscopy and transmission electron microscopy analyses show that newly generated particles differ significantly in size and shape from the cubic-shaped bulk material. Particles with low aspect ratio are below 100 nm in all dimensions. Hence, specific control of temperatures in the expanding free jet offers a tool to produce nanoscale organic pigments with defined particle sizes.     

Experimental Study of Particle Deposition on Semiconductor Wafers

A sensitive method for detecting particle deposition on semiconductor wafers has been developed. The method consisted of generating a monodisperse fluorescent aerosol, depositing the known-size monodisperse aerosol on a wafer in a laminar flow chamber, and analyzing the deposited particles using a fluorometric technique. For aerosol particles in the size range of 0.1–1.0 μm, the mobility classification-inertial impaction technique developed by Romay-Novas and Pui (1988) was used to generate the monodisperse test aerosols. Above a particle diameter of 1.0 μm, monodisperse uranine-tagged oleic acid aerosols were generated by a vibrating-orifice generator. The test wafer was a 3.8-cm diameter silicon wafer placed horizontally in a vertical laminar flow chamber which was maintained at a free stream velocity of 20 cm/s. A condensation nucleus counter and an optical particle counter were used to obtain the particle concentration profile in the test cross section and to monitor the stability of aerosol concentration during the experiment. The results show that the measured particle deposition velocities on the wafers agree well with the theory of Liu and Ahn (1987) in the particle size range between 0.15 and 8.0 μm. The deposition velocity shows a minimum around 0.25 μm in particle diameter and increases with both smaller and larger particle size owing to diffusional deposition and gravitational settling, respectively.     

Generation of monodisperse aerosols by combining aerodynamic flow-focusing and mechanical perturbation

A novel instrument has been developed for generating highly monodisperse aerosol particles with a geometrical standard deviation of 1.05 or less. This aerosol generator applies a periodic mechanical excitation to a micro-liquid jet obtained by aerodynamic flow-focusing. The jet diameter and its fastest growth wavelength have been optimized as a function of the flow-focusing pressure drop and the liquid flow rate. The monodisperse aerosol generated by this instrument is also charge neutralized with bipolar ions produced by a non-radioactive, corona discharge device. Monodisperse droplet generation in the 15- to 72-μm diameter range from a single 100-micron nozzle has been demonstrated. Both liquid and solid monodisperse particles can be generated from 0.7- to 15-μm diameter by varying solution concentration, liquid flow rate, and excitation frequency. The calculated monodisperse particle diameter agrees well with independent measurements. The operation of this new monodisperse aerosol generator is stable and reliable without nozzle clogging, typical of other aerosol generators at the lower end of the operating particle size ranges.

Copyright © 2016 American Association for Aerosol Research     

Synthesis of Spherical β-Silicon Carbide Particles by Ultrasonic Spray Pyrolysis

Fine agglomerate-free spherical β-SiC powder was synthesized from a dispersion of colloidal silica, saccharose, and boric acid, by means of an ultrasonic spray pyrolysis method. Droplets of 2.2 μm were formed with an aerosol generator, operated at 2.5 MHz, and carried into a reaction furnace at 900°C with argon. Spherical X-ray amorphous gel particles of 1.1 μm were obtained. β-SiC particles with a mean diameter of 0.79 μm and spherical shape resulted when the SiC gel precursor particles were heated at 1500°C in argon.     

Generation and Characterization of Ultrafine Chain Aggregate Aerosols

Continuously stable, well-characterized chain aggregate aerosol sources generated from a flame aerosol generator are described. To characterize the length of the chain aggregate, a new image processing software was developed to measure the length distribution of aggregates. This program measures the path length of the aggregate that has been skeletonized into one pixel in width while maintaining its length and shape. In order to generate monodisperse chain aggregate sources, a differential mobility analyzer was used to classify aggregates according to electrical mobility. A series of experiments were conducted to generate singly charged, monodisperse chain aggregate aerosol sources. The operational range of the system for generation of monodisperse chain aggregates is described. Single-mode chain aggregates with a geometric mean particle length between 1.50 and 3.20 μm and a length standard deviation around 1.3 were generated.     

Inkjet Aerosol Generator as Monodisperse Particle Number Standard

The AIST-inkjet aerosol generator (IAG) can generate highly monodisperse solid or liquid aerosol particles in the particle diameter range from 0.3 to 20 μm at precisely known particle generation rates. The device has been developed for evaluating the counting efficiencies of optical and condensation particle counters. Particle generation efficiency of the IAG is defined as the number of aerosol particles generated by one voltage pulse sent to an inkjet head. The 95% confidence interval of the efficiency were 0.998 ± 0.006 within the 0.4 to 10 μm particle diameter range. The efficiencies remained close to unity when the droplet generation rates were within 20–500 s^?1 and 100–900 s^?1 using ultrapure-water and isopropyl alcohol (IPA) as the solvent of the inkjet solution, respectively. The operating aerosol flowrate range of the IAG is currently 0.5 and 1.0 L/min. The coefficients of variations (C.V.) of the size distributions were 2 to 3% indicating the generated particles were highly monodisperse. The generated particle sizes were defined as the volume equivalent diameter, D_ve. The uncertainty analysis on the factors affecting D_ve indicated that 95% confidence interval of the D_ve is expected to be ±5%. The uncertainty of D_ve was entirely caused by the uncertainty of the average mass of a droplet. The reproducibility of particle sizes within 0.5 to 10 μm was evaluated using an aerodynamic particle sizer. The C.V. of the measured particle sizes were less than 6% and 4% when NaCl particles and ionic liquid droplets were generated, respectively.

Copyright 2014 American Association for Aerosol Research     

Hygroscopic properties of potassium-halide nanoparticles

The hygroscopic properties of KBr, KCl, and KI nanoparticles having diameters from 8 to 60 nm were measured using a tandem Differential Mobility Analyzer. In all cases, the deliquescence and efflorescence relative humidity values increased with decreasing particle diameter. The associated growth factors also decreased with decreasing particle diameter, in agreement with predictions by Köhler theory. Overall, the theoretically predicted growth factors agreed well with the measurements, i.e., within ±3% uncertainty. For KCl particles having sizes down to 15 nm, however, a dynamic shape factor of 1.08, corresponding to non-spherical crystalline particles prior deliquescence, was inferred for agreement between measurements and theory. By comparison, KBr and KI within the same size range warranted shape factors of unity, equivalent to a sphere. These results contribute to an understanding of nanosize behavior widely relevant to material sciences as well as atmospheric aerosol particles over the oceans.     

Measurements of Morphology Changes of Fractal Soot Particles using Coating and Denuding Experiments: Implications for Optical Absorption and Atmospheric Lifetime

Mobility-selected fractal and non-fractal soot particles (mobility diameters d _m = 135 to 310 nm) were produced at three controlled fuel equivalence ratios (φ = 2.1, 3.5, and 4.5) by an ethylene/oxygen flame. Oleic acid (liquid) and anthracene (solid) coatings were alternately applied to the particles and removed. Simultaneous measurements with an Aerodyne aerosol mass spectrometer and a scanning mobility particle sizer yielded the particle mass, volume, density, composition, dynamic shape factor, fractal dimension, surface area, and the size and number of the primary spherules forming the fractal aggregate. For a given φ, the diameters of the primary spherules are approximately the same, independent of d _m (15 nm, 35 nm, and 55 nm for φ = 2.1, 3.5, and 4.5, respectively). As the coating thickness on a particle increases, the dynamic shape factor decreases but d _m remains constant until the particle reaches a spherical (for oleic acid) or non-fractal but irregular (for anthracene) shape. Under some conditions, liquid oleic acid coating causes the internal BC framework to rearrange into a more compact configuration. The surface area of fractal particles is up to 2.4 times greater than that of a sphere with the same d _m . Using the surface area determinations, the time for a fractal particle to obtain a monolayer of coating material is compared to that of spheres. If it is assumed that the fractal particle is a sphere with the same d _m as the fractal particle, the monolayer coating time is underestimated by a factor of up to 1.7.     

Particle Charge Distribution Measurement for Commonly Generated Laboratory Aerosols

ABSTRACT

An improved particle charge analyzer system has been developed to measure the absolute charge distribution of common generated laboratory aerosols. The charge analyzer system consists of an integral cylindrical mobility analyzer used in conjunction with an optical aerosol spectrometer, with computer assisted operation and data reduction. The charge analyzer collects aerosol particles over an absolute electrical mobility range from 4.2*10^?4 to 400 cm²/(stat · Volt second) and flow rates that can vary from 0.3 to 30 liters per minute. The charge analyzer has been used to investigate the nature of spray and contact electrification during aerosol generation by measuring the residual charge distribution on the liquid and solid generated particles. In addition, the neutralization of charged particles by bipolar ions also was studied using conventional neutralizers that use ionizing radiation from alpha and beta sources. Charge distribution measurements were performed on alumina dust (Al), Arizona road dust (ARD), potassium chloride (KCl), sodium chloride (NaCl) and di-octyl sebacate (DOS) liquid particles. Aerosol generation devices include a Collison atomizer, a condensation aerosol generator and a fluidized bed dust generator. Our work provides experimental charge distribution data for comparison with simple models of electrification theory. Experimental results showed that charge levels of atomized KCl and NaCl particles were high and decreased as the dissolved ion concentration increased. DOS particles generated by evaporation-condensation were both neutral and moderately charged. These conclusions support the existence of a dipole layer at the liquid-gas interface that interacts with dissolved particles and changes their charge state. Alumina and ARD generated by the fluidized bed disperser are highly charged due to strong contact electrification during dispersion. In most cases, the charge on generated aerosols could be reduced to Boltzmann charge equilibrium conditions by commonly used radioactive neutralizers.     

Differences in estimates of size distribution of beryllium powder materials using phase contrast microscopy, scanning electron microscopy, and liquid suspension counter techniques

Accurate characterization of the physicochemical properties of aerosols generated for inhalation toxicology studies is essential for obtaining meaningful results. Great emphasis must also be placed on characterizing particle properties of materials as administered in inhalation studies. Thus, research is needed to identify a suite of techniques capable of characterizing the multiple particle properties (i.e., size, mass, surface area, number) of a material that may influence toxicity. The purpose of this study was to characterize the morphology and investigate the size distribution of a model toxicant, beryllium. Beryllium metal, oxides, and alloy particles were aerodynamically size-separated using an aerosol cyclone, imaged dry using scanning electron microscopy (SEM), then characterized using phase contrast microscopy (PCM), a liquid suspension particle counter (LPC), and computer-controlled SEM (CCSEM). Beryllium metal powder was compact with smaller sub-micrometer size particles attached to the surface of larger particles, whereas the beryllium oxides and alloy particles were clusters of primary particles. As expected, the geometric mean (GM) diameter of metal powder determined using PCM decreased with aerodynamic size, but when suspended in liquid for LPC or CCSEM analysis, the GM diameter decreased by a factor of two (p < 0.001). This observation suggested that the smaller submicrometer size particles attached to the surface of larger particles and/or particle agglomerates detach in liquid, thereby shifting the particle size distribution downward. The GM diameters of the oxide materials were similar regardless of sizing technique, but observed differences were generally significant (p < 0.001). For oxides, aerodynamic cluster size will dictate deposition in the lung, but primary particle size may influence biological activity. The GM diameter of alloy particles determined using PCM became smaller with decreasing aerodynamic size fraction; however, when suspended in liquid for CCSEM and LPC analyses, GM particle size decreased by a factor of two (p < 0.001) suggesting that alloy particles detach in liquid. Detachment of particles in liquid could have significance for the expected versus actual size (and number) distribution of aerosol delivered to an exposure subject. Thus, a suite of complimentary analytical techniques may be necessary for estimating size distribution. Consideration should be given to thoroughly understanding the influence of any liquid vehicle which may alter the expected aerosol size distribution.     

A note on the aerodynamic diameter and the mobility of non-spherical aerosol particles

The aerodynamic diameter of a non-spherical aerosol particle is primarily related to the final settling velocity of the particle. The aerodynamic diameter is not obtained directly from mobility measurements by formally calculating a sphere diameter from the mobility equation for a spherical particle. Instead, a correction factor involving the dynamic shape factor of the non-spherical particle must be applied.