Aerosol Generation by a Spray-Drying Technique Under Coulomb Explosion and Rapid Evaporation for the Preparation of Aerosol Particles for Inhalation Tests

In this study, nanosized (<100 nm) aerosol particles with high mass concentrations for inhalation tests were generated by a spray-drying technique with combining Coulomb explosion and rapid evaporation of the droplets. Under typical spray-drying conditions, aerosol particles with average diameter of 50–150 nm were prepared from a suspension of NiO nanoparticles with a primary diameter of 15–30 nm. Under the Coulomb explosion method, the sprayed droplets were charged by being mixed with unipolar ions to break up the droplets, which resulted in the generation of smaller aerosol particles with diameters of 15–30 nm and high number concentrations. Under the rapid evaporation method, the droplets were heated immediately after being sprayed to avoid inertial impaction on the flow path due to shrinkage of the droplet, which increased the mass concentration of the aerosol particles. The combination of the Coulomb explosion and rapid evaporation of droplets resulted in the generation of aerosol particles with sizes less than 100 nm and mass concentrations greater than 1 mg/m³; these values are often necessary for inhalation tests. The aerosols generated under the combined method exhibited good long-term stability for inhalation tests. The techniques developed in this study were also applied to other metal oxide nanoparticle materials and to fibrous multiwalled carbon nanotubes.

Copyright 2014 American Association for Aerosol Research     

Aerosol Process for the In Situ Coating of Nanoparticles with a Polymer Shell

This article presents a novel method to encapsulate gas-borne nanoparticles with a polymeric shell. This method implies heterogeneous condensation of monomer vapor around the surface of nanoparticles as nuclei and polymerization is then subsequently started by addition of NH₃ as aerosol initiator. Ag and SiO₂ nanoparticles were generated as inorganic core by spark discharge and nebulization, respectively, and glycidyl methacrylate (GMA) was used as organic monomer. The effect of several parameters, including vapor pressure of monomer and properties of inorganic core such as morphology, material, particle size, and production method on the thickness of polymeric shell and morphology of resulting nanocomposites has been investigated. The particle size distribution and morphology of the resulting core-shell nanoparticles have been studied via scanning mobility particle sizer (SMPS) and transmission electron microscope (TEM). Finally, the coating efficiency was determined by aerosol photoemission (APE) and the results show that monomer and polymer coating efficiency are 99% and 60%, respectively.

Copyright 2014 American Association for Aerosol Research     

Using silver as a surrogate for plutonium: An experimental study of the explosive silver aerosol source term

An experimental method is developed for the purpose of simulating plutonium aerosol source terms with conventional metals in laboratory. In this method, metal samples are aerosolized by high explosive detonation in a containment vessel. Aerosols having aerodynamic diameter (AD) less than 10 µm are then collected by a cascade impactor and analyzed by atomic absorption spectroscopy. Two sets of experiments were conducted. In the first set, five candidate metal samples (Ag, W, Sn, Ce, and V) were tested. It is found that the cumulative mass distribution of silver under certain conditions was in good agreement with that of plutonium from the Operation Roller Coaster-Double Track experiment. Thus, silver is chosen as a surrogate to simulate the plutonium aerosol source term. In the second set, silver aerosol source term was studied in detail with different test configurations. The results demonstrate that the peak of the mass-size distribution of silver is in the AD range 1.1–3.3 µm. The amount and fraction of relatively small silver aerosols decrease significantly with time due to coagulation and deposition. Interestingly, the amount of silver in aerosols could be expressed as a quadratic function of the peak detonation pressure.

© 2016 American Association for Aerosol Research     

Observations of a Correlation Between Primary Particle and Aggregate Size for Soot Particles

For decades, soot has been modeled as fractal-like aggregates of nearly equiaxed spherules. Cluster–cluster aggregation simulations, starting from a population of primary particles, give rise to structures that closely match real aerosols of solid particles produced in flames. In such simulations, primary particle size is uncorrelated with aggregate size, as all aggregates contain primary particles drawn from the same population. Aerosol measurements have been interpreted with this geometric model. Examination of transmission electron micrographs of soot samples from various sources shows that primary particle sizes are not well mixed within an aerosol population. Larger aggregates tend to contain larger primary particles and the variation in size is much larger between aggregates than within aggregates. The soot sources considered here are all substantially not well-mixed (aircraft jet engine, inverted diffusion flame, gasoline direct injection engine, heavy-duty compression ignition engine). The observed variations in primary particle size can be explained if soot aggregates are formed and grew by coagulation in small zones of the combustion chamber, prior to dilution and transport (with minimal coagulation) to the sampling system.

Copyright 2014 American Association for Aerosol Research     

The Use of Nonlinear Acoustics as an Energy-Efficient Technique for Aerosol Removal

This article is a feasibility study on using nonlinear acoustic effects, acoustic streaming and acoustic radiation pressure, for aerosol removal in an air duct. Unlike previous research, which used acoustics solely to cause aerosol agglomeration prior to aerosol removal in traditional duct collection systems, this article considers the acoustic streaming effect, which is significant but was previously neglected. Monodispersed polystyrene spheres with diameters ranging from 0.3 to 6 μm were tested. The proposed system removed 12–20% of the submicron aerosols and 25–32% of the micron aerosols when the airflow rate was approximately 90 L/min. Acoustic streaming introduces stagnation points on the surface of the air duct and removes the aerosols by deposition. Acoustic radiation pressure causes aerosols to form agglomerates. This enhances inertial impaction and/or gravitational sedimentation, which further enhances the removal efficiency of micron aerosols. The particle-removal efficiency is proportional to the duration that the aerosols are exposed to the acoustic field. The pressure drop due to the nonlinear acoustic effects is negligible; thus, power consumption is minimal. This system has the potential to be developed into an energy-efficient technique for aerosol removal.

Copyright 2014 American Association for Aerosol Research     

A novel high-volume Photochemical Emission Aging flow tube Reactor (PEAR)

Aerosols emitted from various anthropogenic and natural sources undergo constant physicochemical transformations in the atmosphere, altering their impacts on health and climate. This article presents the design and characteristics of a novel Photochemical Emission Aging flow tube Reactor (PEAR). The PEAR was designed to provide sufficient aerosol mass and flow for simultaneous measurement of the physicochemical properties of aged aerosols and emission exposure studies (in vivo and in vitro). The performance of the PEAR was evaluated by using common precursors of secondary aerosols as well as combustion emissions from a wood stove and a gasoline engine. The PEAR was found to provide a near laminar flow profile, negligible particle losses for particle sizes above 40?nm, and a narrow residence time distribution. These characteristics enable resolution of temporal emission patterns from dynamic emission sources such as small-scale wood combustion. The formation of secondary organic aerosols (SOA) in the PEAR was found to be similar to SOA formation in a smog chamber when toluene and logwood combustion emissions were used as aerosol sources. The aerosol mass spectra obtained from the PEAR and smog-chamber were highly similar when wood combustion was used as the emission source. In conclusion, the PEAR was found to plausibly simulate the photochemical aging of organic aerosols with high flow rates, needed for studies to investigate the effects of aged aerosols on human health. The method also enables to study the aging of different emission phases in high time resolution, and with different OH-radical exposures up to conditions representing long-range transported aerosols.

Copyright © 2019 American Association for Aerosol Research     

Droplet-based microfluidics detector for bioaerosol detection

Detection of bioaerosols is important in fields ranging from environmental health monitoring to biosurveillance, and current detector weaknesses have motivated the development of new technologies. In this work, a detector was built, which applies the principles of droplet microfluidics to bioaerosol detection. Droplet microfluidics is a subfield of microfluidics based on the creation of monodisperse microdroplets with compartmentalized reagents and supports enhanced assays and fluidic manipulations. The bioaerosol detector operates by aerodynamically focusing aerosols directly into these droplets to harness the benefits of the microreactor environment. A breadboard detector system, which consisted of an aerodynamic focusing lens, aerosol-focusing capillary, microfluidic droplet chip, and optical microscope, was constructed. Computational fluid dynamic simulations and Lagrangian particle tracking modeling were conducted to identify the optimal conditions for focusing. Preliminary experiments, where aerosols were deposited onto a solid substrate, demonstrated sub 200-µm spot diameters for aerodynamic diameters of 2–5 µm. Test aerosols were then generated, and collected into the microfluidic liquid interface on the chip as verified by microscopy. Recovery efficiency of the aerosols was dependent on aerosol size and ranged from about 27% to nearly 100%. Finally, to prove bioaerosol collection and detection, a droplet propidium iodide (PI) assay was performed: the system distinguished between E. coli and non-biological aerosols within 20 s. Overall, this work established the technique of direct collection of bioaerosols into a convenient droplet microfluidic platform for detection.

Copyright © 2017 The Johns Hopkins University Applied Physics Laboratory     

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     

Using Raman Microspectroscopy to Determine Chemical Composition and Mixing State of Airborne Marine Aerosols over the Pacific Ocean

Chemical composition and mixing state of aerosols collected over an 11,000 km latitudinal cruise in the Pacific Ocean are reported here as determined by a new application of Raman spectroscopy. The Raman microspectroscopy technique employs a Raman spectrometer coupled to an optical microscope to identify the chemical composition and internal mixing state of single particles. By analyzing multiple particles in a collected ensemble, the degree of external mixing of particles was also determined. To lend context to the Pacific aerosol population sampled, atmospheric aerosol concentration, and the critical supersaturation required for the aerosols to activate as cloud condensation nuclei, and chlorophyll a concentration in the underlying water (a metric for phytoplankton biomass in the ocean) were also obtained. Our results indicate that long chain organic molecules were prevalent in the marine aerosol samples throughout the cruise, including during coastal and open ocean locations, in both hemispheres, and in the seasons of autumn and spring. Long chain organic compounds tended to be present in internal mixtures with other organic and inorganic components. Although variations in the fraction of aerosols activated as CCN were observed, no simple correlation between organics and CCN activation was found. According to our measurements, marine aerosol in the Pacific Ocean may be generally characterized as multicomponent aerosol containing and often dominated by a high organic fraction. Our results suggest that the prevalence of organics and the high degree of internal mixing of aerosol must be accounted for in accurate modeling of the role of marine aerosols in cloud formation and climate.

Copyright 2014 American Association for Aerosol Research     

A numerical aerosol model Fractal Aggregate Moment Model (FAMM) to simulate simultaneous nucleation,coagulation, surface growth,and sintering of fractal aggregates

Particles generated from high-temperature processes often attain an aggregate structure, with physical and chemical properties and health impacts dependent on the particles’ size and morphology. A numerical aggregate model is a useful tool to produce well-controlled ceramic particles and to predict the production of particulate air contaminants. Although extensive efforts have been directed at developing accurate and fast-running numerical aerosol codes that can model the formation and growth of aerosol aggregates using the framework of the log-normal (LN) moment method, none developed thus far can account for the bimodal particle size distribution and aggregate morphology simultaneously. In this study, two previous models, a bimodal LN model for spherical particles and a unimodal LN model for fractal aggregates, are extended to fabricate a bimodal LN model for fractal aggregates. By tracing five time-dependent variables for the particle phase, the present model can predict the formation of nucleus particles from a gas precursor and the change in the particle size distribution and morphology. Nucleation, surface growth, intramodal and intermodal coagulation, sintering, and condensational obliteration are taken into account. Numerical experiments performed for validating the new model showed that it is a robust and efficient tool for predicting both aggregate particle size distribution and morphology. The proposed model is expected to be a useful tool for simulating the formation and growth of fractal aggregate particles in multidimensional spatial domains requiring a fast-running aerosol model.

Copyright © 2019 American Association for Aerosol Research     

Extension of the Smoluchowski Theory to Transitions from Dilute to Dense Regime of Brownian Coagulation: Triple Collisions

In order to study the transition from dilute (controlled by binary collisions) to dense (controlled by multiple collisions) regime of coagulation of colloidal or aerosol suspensions, the Smoluchowski equation is generalized by consideration of triple collisions in the kinetic approach, recently proposed by the authors for coagulation of comparable size particles. A good agreement of the new model predictions with more general results of the direct numerical simulations by Langevin dynamics (from the literature) is attained in a relatively wide range of the fractional volume, corresponding to the transition from dilute to dense regime of coagulation dynamics, in which multiple collisions among more than three particles can be neglected.

Copyright 2014 American Association for Aerosol Research     

A coupled CFD-Monte Carlo method for simulating complex aerosol dynamics in turbulent flows

A coupled computational fluid dynamics (CFD)-Monte Carlo method is presented to simulate complex aerosol dynamics in turbulent flows. A Lagrangian particle method-based probability density function (PDF) transport equation is formulated to solve the population balance equation (PBE) of aerosol particles. The formulated CFD-Monte Carlo method allows investigating the interaction between turbulence and aerosol dynamics and incorporating individual aerosol dynamic kernels as well as obtaining full particle size distribution (PSD). Several typical cases of aerosol dynamic processes including turbulent coagulation, nucleation and growth are studied and compared to the sectional method with excellent agreement. Coagulation in both laminar and turbulent flows is simulated and compared to demonstrate the effect of turbulence on aerosol dynamics. The effect of jet Reynolds (Re_j) number on aerosol dynamics in turbulent flows is fully investigated for each of the studied cases. The results demonstrate that Re_j number has significant impact on a single aerosol dynamic process (e.g., coagulation) and the simultaneous competitive aerosol dynamic processes in turbulent flows. This newly modified CFD-Monte Carlo/PDF method renders an efficient method for simulating complex aerosol dynamics in turbulent flows and provides a better insight into the interactions between turbulence and the full PSD of aerosol particles.

Copyright © 2017 American Association for Aerosol Research     

Application of centrifugal filter to aerosol size distribution measurement

In the present work, the centrifugal filter proposed by the authors was applied to classify aerosol particles followed by the detection of total mass or number concentrations so as to measure the size distribution of aerosol particles. The structure and operating condition of the centrifugal filter were optimized in order to attain sharp separation curves with various cut-off sizes between 0.3 and 10 μm. The aerosol penetrating the centrifugal filter at various rotation speeds was measured with a photometer to determine the total mass concentration. The virtue of this system is that the cut-off size is varied just by scanning the rotation speed of filter and that it can be applied to the measurement of high concentration aerosols without dilution by choosing an appropriate filter medium. As a result, the centrifugal filter was successfully applied to measure the size distribution of solid particles in size ranging from 0.3 to 10 μm.

Copyright © 2017 American Association for Aerosol Research     

Numerical,wind-tunnel,and atmospheric evaluation of a turbulent ground-based inlet sampling system

The use of inlets for transferring aerosols from the environment to instrumentation can introduce uncertainty in the measurement of aerosol properties. Aerosol loss during this process is a non-negligible issue that may bias the subsequent measurements. These loss mechanisms include aspiration at the inlet head and deposition/evaporation/condensation during transport through the sampling lines. Coarse-mode aerosol is significantly impacted by the aspiration and inertial loss mechanisms within an inlet system. This work uses wind tunnel experiments to investigate aerosol losses through the Storm Peak Laboratory’s (SPL) new aerosol inlet system. The inlet is used extensively for both intensive field campaigns and long-term aerosol monitoring. The results of numerical simulations of the SPL aerosol inlet sampling efficiency are provided at several wind speeds, and experimental results demonstrate the system has a 50% cut off for the coarse-mode at an aerodynamic diameter of approximately 13?μm and wind speed of 0.5?m s^?1. This investigation will lead to improved accuracy of in situ aerosol measurements at SPL and this system can be replicated at other atmospheric stations.

Copyright © 2019 American Association for Aerosol Research     

Approximate analytical solutions to the condensation-coagulation equation of aerosols

We present analytical solutions to the steady state nucleation-condensation-coagulation equation of aerosols in the atmosphere. These solutions are appropriate under different limits but more general than previously derived analytical solutions. For example, we provide an analytic solution to the coagulation limit plus a condensation correction. Our solutions are then compared with numerical results. We show that the solutions can be used to estimate the sensitivity of the cloud condensation nuclei number density to the nucleation rate of small condensation nuclei and to changes in the formation rate of sulfuric acid.

© 2016 American Association for Aerosol Research     

Seasonal Variability of Particle-Associated Organic Compounds Near a Heavily Traveled Secondary Road

Size-resolved aerosol samples were collected both upwind and downwind of a large secondary road in the winter and spring of 2007 to assess contributions of on-road emissions to ambient aerosols. The aerosol samples were extracted and analyzed for a wide variety of organic compounds including polycyclic aromatic hydrocarbons (PAHs), alkanes, sugars, and organic acids. The results showed a strong seasonal pattern where the concentrations of most compounds were higher in winter than in spring. Some of the biogenic sugars were the exception, which might be the result of a “spring blooming season.” The surprising result was that the upwind site located in a residential neighborhood had very similar concentrations of most organic compounds compared to the near-roadway site. Possible reasons for the lack of differences in organic chemical concentrations between the near-road and control sites include: a large urban background concentration of aerosols superimposed on any local source; shifting wind directions that make the “downwind” site upwind during the night; and additional local sources in the residential neighborhood such as wood burning in winter.

Copyright 2014 American Association for Aerosol Research     

Factors affecting the formation of alpha and beta polymorphs in glutaric acid aerosols

Dicarboxylic acids are prevalent in the atmosphere and frequently investigated by aerosol and atmospheric scientists. Glutaric acid, being a water-soluble dicarboxylic acid, is commonly used to model water activity in dicarboxylic acid aerosols. Different values associated with glutaric acid aerosols, specifically DRH and hygroscopic data, have been reported by several groups. We hypothesize that this variability is caused by its polymorphism. Glutaric acid exhibits dimorphism, meaning the molecule can form into two different types of crystal structures, an alpha and a beta polymorph. Glutaric acid naturally forms the beta polymorph, which is more stable. The alpha polymorph is the metastable phase. These polymorphs manifest themselves as a bimodal aerosol size distribution when analyzed by Scanning Mobility Particle Sizers or other aerosol mobility sizing methods. In this article, we discuss the formation of the nanoscale alpha glutaric acid polymorph generated from an aqueous glutaric acid solution. The formation of both polymorphs from an aqueous solution has not been documented elsewhere. We have found that the alpha polymorph forms at faster crystallization speeds, with a lower aqueous solution concentration and a lower solution flow rate into the atomizer. This identification of the presence of polymorphism in glutaric acid aerosols under common laboratory generation conditions could explain the variability present in studies associated with glutaric acid aerosols. Understanding the conditions at which the alpha polymorph is present will allow researchers to avoid it when using glutaric acid as a dicarboxylic acid standard and explain previously noted discrepancies.

Copyright © 2019 American Association for Aerosol Research     

Production of neutral molecular clusters by controlled neutralization of mobility standards

Measuring aerosols and molecular clusters below the 3 nm size limit is essential to increase our understanding of new particle formation. Instruments for the detection of sub-3 nm aerosols and clusters exist and need to be carefully calibrated and characterized. So far calibrations and laboratory tests have been carried out using mainly electrically charged aerosols, as they are easier to handle experimentally. However, the charging state of the cluster is an important variable to take into account. Furthermore, instrument characterization performed with charged aerosols could be biased, preventing a correct interpretation of data when electrically neutral sub-3 nm aerosols are involved. This article presents the first steps to generate electrically neutral molecular clusters as standards for calibration. We show two methods: One based on the neutralization of well-known molecular clusters (mobility standards) by ions generated in a switchable aerosol neutralizer. The second is based on the controlled neutralization of mobility standards with mobility standards of opposite polarity in a recombination cell. We highlight the challenges of these two techniques and, where possible, point out solutions. In addition, we give an outlook on the next steps toward generating well-defined neutral molecular clusters with a known chemical composition and concentration.

Published with license by American Association for Aerosol Research     

Characterization and Response Model of the PPS-M Aerosol Sensor

The Pegasor PPS-M sensor is an electrical aerosol sensor based on diffusion charging and current measurement without particle collection. In this study, the role and effect of each component in the instrument is discussed shortly and the results from a thorough calibration measurements are presented. A comprehensive response model for the operation of the PPS-M sensor was developed based on the calibration results and computational fluid dynamics (CFD) modeling results. The obtained response model, covering the effects of the particle charger, the mobility analyzer, and both diffusion and inertial losses, was tested in the laboratory measurements with polydisperse test aerosols, where a good correlation between the model and the measured results was found.

Copyright 2014 American Association for Aerosol Research     

Influence of surfactants on growth of individual aqueous coarse mode aerosol particles

Understanding the links between aerosol and cloud and radiative properties remains a large uncertainty in predicting Earth's changing energy budget. Surfactants are observed in ambient atmospheric aerosol particles, and their effect on cloud droplet growth is a mechanism that was, until recently, neglected in model calculations of particle activation and droplet growth. In this study, coarse mode aqueous aerosol particles were created containing the surfactant Igepal CA-630 and NaCl. The evaporation and condensation of these individual aqueous particles were investigated using an aerosol optical trap combined with Raman spectroscopy. For a relative humidity (RH) change from 70% to 80%, droplets containing both Igepal and NaCl at atmospheric concentrations exhibited on average more than 4% larger changes in droplet radii, compared to droplets containing NaCl only. This indicates enhanced water uptake in the presence of surfactants, but this result is unexpected based on the standard calculation of the effect of surfactants, using surface tension reduction and/or hygroscopicity changes, for particles of this size. One implication of these results is that in periods with increasing RH, surfactant-containing aqueous particles may grow larger than similarly sized aqueous NaCl particles without surfactants, thus shifting atmospheric particle size distributions, influencing particle growth, and affecting aerosol loading, visibility, and radiative forcing.

Copyright © 2018 American Association for Aerosol Research