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     

Impact of power level and refill liquid composition on the aerosol output and particle size distribution generated by a new-generation e-cigarette device

The new high-power Electronic Nicotine Delivery System (ENDS) can generate aerosols with higher nicotine concentrations than older ENDS. Aerosol particle sizes affect deposition patterns and then plasma nicotine levels in vapers. Consequently, understanding the factors influencing particle size distribution of high-power ENDS is relevant to assess their performance in terms of nicotine delivery. The particle size distribution and the aerosol output (aerosol mass) were measured using cascade impactors. The effects of the refill liquid composition (80% PG/20% VG vs. 80% VG/20% PG; PG refers to propylene glycol and VG to vegetable glycerin) and the power level of the battery (from 7 W to 22 W) were investigated. The aerosol output increases significantly with the power level following a logarithmic law. The PG/VG ratio also has an impact on the aerosol output. The higher the VG content in the refill liquid, the higher is the aerosol output. Besides, particle size distribution is positively related to the power level, following linear correlations between the mass median aerodynamic diameter (MMAD) and the power level in the range of 7–22 W. A moderate impact of the PG/VG ratio on size distribution is equally observed. Changes in the power level allow the transition between a dominant mode with MMAD from 613 nm to 949 nm. We demonstrated that the power level can strongly change the aerodynamic properties of high-power ENDS, especially at high voltage. Associated with the aerosol nicotine level assessment, MMAD could be determined as a means for comparing ENDS devices and nicotine delivery.

Copyright © 2018 American Association for Aerosol Research     

In-situ characterization of e-cigarette aerosols by 90°-light scattering of polarized light

The polarization ratio method is used for fast in-situ characterization of unimodal condensed aerosols of e-cigarettes. The method is based on 90°-light scattering of polarized 680 nm laser light by the droplet ensemble inside an optically defined measuring volume. Mass median droplet diameter (MMD) is derived from the ratio of scattered light from horizontally and vertically polarized incident light beams assuming a fixed value of the geometric standard deviation of the aerosol mass distribution. MMD is used to correct for the size dependence of the mass-based scattering signal of vertically polarized light to obtain the mass concentration if the sensor is calibrated once with an aerosol with a fixed MMD. The sensor uses commercially available aerosol photometers, and its application to e-cigarette aerosols was validated with an impactor for MMD and with a filter measurement for mass concentration. Good correlation (r² > 0.97) for both parameters was observed. Application ranges are mass concentration range 0.5–50 mg/L, MMD 0.2–1.2 µm, 100 ms time resolution, and 0.2–3 L/min flow rate. The usefulness of this simple sensor for e-cigarette aerosol characterization is demonstrated by developing a scaling law between MMD and operating parameters of an e-cigarette, i.e., puff flow rate and mass concentration.

Copyright © 2018 American Association for Aerosol Research     

Aerosol Measurement by Induced Currents

We introduce a new electrical measurement technique for aerosol detection, based on pulsed unipolar charging followed by a non-contact measurement of the rate of change of the aerosol space charge in a Faraday cage. This technique, which we call “aerosol measurement with induced currents,” has some advantages compared to the traditional method of collecting the charged particles on either an electrode or with a particle filter. We describe the method and illustrate it with a simple and miniature (shirt-pocket-sized) instrument to measure lung-deposited surface area. Aerosol measurement by induced currents can also be applied to more complex devices.

Copyright 2014 American Association for Aerosol Research     

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     

The First Combined Thermal Desorption Aerosol Gas Chromatograph—Aerosol Mass Spectrometer (TAG-AMS)

To address the critical need for improving the chemical characterization of the organic composition of ambient particulate matter, we introduce a combined thermal desorption aerosol gas chromatograph—aerosol mass spectrometer (TAG-AMS). The TAG system provides in-situ speciation of organic chemicals in ambient aerosol particles with hourly time resolution for marker compounds indicative of sources and transformation processes. However, by itself the TAG cannot separate by particle size and it typically speciates and quantifies only a fraction of the organic aerosol (OA) mass. The AMS is a real-time, in-situ instrument that provides quantitative size distributions and mass loadings for ambient fine OA and major inorganic fractions; however, by itself the AMS has limited ability for identification of individual organic compounds due to the electron impact ionization detection scheme used without prior molecular separation.

The combined TAG-AMS system provides real-time detection by AMS followed by semicontinuous analysis of the TAG sample that was acquired during AMS operation, achieving simultaneous and complementary measurements of quantitative organic mass loading and detailed organic speciation. We have employed a high-resolution time-of-flight mass spectrometer (HR-ToF-MS) to enable elemental-level determination of OA oxidation state as measured on the AMS, and to allow improved compound identification and separation of unresolved complex mixtures (UCM) measured on the TAG. The TAG-AMS interface has been developed as an upgrade for existing AMS systems. Such measurements will improve the identification of organic constituents of ambient aerosol and contribute to the ability of atmospheric chemistry models to predict ambient aerosol composition and loadings.

Copyright 2014 American Association for Aerosol Research     

Opto-aerodynamic focusing of aerosol particles

We describe a new method for focusing and concentrating a stream of moving micron-sized aerosol particles in air. The focusing and concentrating process is carried out by the combined drag force and optical force that is generated by a double-layer co-axial nozzle and a focused doughnut-shaped hollow laser beam, respectively. This method should supply a new tool for aerosol science and related research.

Copyright © 2018 American Association for Aerosol Research     

Mathematical modeling and numerical simulation of surfactant delivery within a physical model of the neonatal trachea for different aerosol characteristics

Surfactant aerosol delivery in conjunction with a noninvasive respiratory support holds the potential to treat neonatal respiratory distress syndrome in a safe manner. The objective of the present study was to gain knowledge in order to optimize the geometry of an intracorporeal inhalation catheter and improve surfactant aerosol delivery effectiveness in neonates. Initially, a mathematical model capable of predicting the aerosol flow generated by this inhalation catheter within a physical model of the neonatal trachea was implemented and validated. Subsequently, a numerical study was performed to analyze the effect of the aerosol liquid droplet size and mass flow rate on surfactant delivery and on the required aerosolization time period. Experimental validation of the mathematical model showed a close prediction of the air axial velocity at the distal end of the physical model, with an absolute error between 0.01 and 0.15 m/s. Furthermore, an admissible absolute error between 0.2 and 2 µm was attained in the prediction of the aerosol mean aerodynamic diameter and mass median aerodynamic diameter in this region. The numerical study highlighted the beneficial effects of generating an intracorporeal aerosol with a mass median aerodynamic diameter higher than 4 µm and a surfactant mass flow rate above 8.93 mg/s in order to obtain effective surfactant delivery in neonates with minimal airway manipulation.

Copyright © 2017 American Association for Aerosol Research     

Development and Evaluation of a Nanoparticle Generator for Human Inhalation Studies with Airborne Zinc Oxide

In the EU there is an increasing need for regulatory agencies to derive health based threshold limits based on human inhalation studies with airborne particles. A necessary prerequisite for such projects is the development of a suitable generator system to produce nanoparticle test aerosols for human whole-body inhalation studies. We decided to use a generator with flame-based heating of aqueous precursor solutions. Validation of the test system was done by generating zinc oxide (ZnO) nanoparticles with minimal contamination of trace gases, i.e., nitric oxides or carbon monoxide that could confound the effects seen in exposed subjects. ZnO was selected based on the uncertainties surrounding its health effects after exposure at the workplace. The generation process of the developed flame generator yields ZnO nanoparticles with monomodal size distribution and very good temporal stability. The maximum target exposure mass concentration of 2 mg/m³ ZnO, with a resulting median particle diameter of 57 nm, is attainable in our human exposure laboratory. The morphological examination shows typical agglomerates and aggregates formed by high temperature processes. Overall, the performed experiments confirm that a constant exposure can be provided for all subjects at all times.

Copyright 2014 American Association for Aerosol Research     

Sensitivity of Aerosol Refractive Index Retrievals Using Optical Spectroscopy

Accurate refractive index values are required to determine the effects of aerosol particles on direct radiative forcing. Theoretical retrievals using extinction data alone or extinction plus absorption data have been simulated to determine the sensitivity of each retrieval. A range of aerosol types with a range of different refractive indices were considered. The simulations showed that the extinction-only retrieval was not able to accurately or precisely retrieve refractive index values, even for purely scattering compounds, but the addition of a simulated absorption measurement greatly improved the retrieval.

Copyright 2014 American Association for Aerosol Research     

Transport phenomena governing nicotine emissions from electronic cigarettes: Model formulation and experimental investigation

Electronic cigarettes (ECIGs) electrically heat and aerosolize a liquid-containing propylene glycol (PG), vegetable glycerin (VG), flavorants, water, and nicotine. ECIG effects and proposed methods to regulate them are controversial. One regulatory focal point involves nicotine emissions. We describe a mathematical model that predicts ECIG nicotine emissions. The model computes the vaporization rate of individual species by numerically solving the unsteady species and energy conservation equations. To validate model predictions, yields of nicotine, total particulate matter, PG, and VG were measured while manipulating puff topography, electrical power, and liquid composition across 100 conditions. Nicotine flux, the rate at which nicotine is emitted per unit time, was the primary outcome. Across conditions, the measured and computed nicotine flux were highly correlated (r = 0.85, p < .0001). As predicted, device power, nicotine concentration, PG/VG ratio, and puff duration influenced nicotine flux (p < .05), while water content and puff velocity did not. Additional empirical investigation revealed that PG/VG liquids act as ideal solutions, that liquid vaporization accounts for more than 95% of ECIG aerosol mass emissions, and that as device power increases the aerosol composition shifts towards the less volatile components of the parent liquid. To the extent that ECIG regulations focus on nicotine emissions, mathematical models like this one can be used to predict ECIG nicotine emissions and to test the effects of proposed regulation of factors that influence nicotine flux.

Copyright © 2017 American Association for Aerosol Research     

A practical set of miniaturized instruments for vertical profiling of aerosol physical properties

In situ atmospheric aerosol measurements have been performed from a Manta unmanned aircraft system (UAS) using recently developed miniaturized aerosol instruments. Flights were conducted up to an altitude of 3000 m (AMSL) during spring 2015 in Ny-Ålesund, Svalbard, Norway. We use these flights to demonstrate a practical set of miniaturized instruments that can be deployed onboard small UASs and can provide valuable information on ambient aerosol. Measured properties include size-resolved particle number concentrations, aerosol absorption coefficient, relative humidity, and direct sun intensity. From these parameters, it is possible to derive a comprehensive set of aerosol optical properties: aerosol optical depth, single scattering albedo, and asymmetry parameter. The combination of instruments also allows us to determine the aerosol hygroscopicity.

Copyright © 2017 American Association for Aerosol Research     

Size-dependent deposition of inhaled nanoparticles in the rat respiratory tract using a new nose-only exposure system

Concerns about the potential health effects of exposure to nanomaterials have led to a growing number of in vivo inhalation toxicity studies using nanoparticle aerosols. Estimates of aerosol deposition within the respiratory tract are important for these studies to enable: (a) the interpretation of the results, in particular, the evaluation of dose–response relationships; (b) comparison with the results of other related studies; and (c) the extrapolation of results from animal models to human. Unfortunately, only a limited number of studies have been undertaken to investigate respiratory tract deposition efficiencies for nano-sized aerosol particles. This is of particular importance as deposition efficiencies are predicted to vary significantly over the nano-size range for some elements of the respiratory tract. In this study, female Wistar-Kyoto rats were exposed in a new design nose-only inhalation exposure system to spark generated radioactive iridium-192 nanoparticle aerosols of four particle sizes chosen to cover the majority of the nano-size range (nominal sizes: 10, 15, 35, and 75 nm). The content of iridium-192 in the lung, head, gastrointestinal tract, and various other organs and tissues was measured. Aerosol deposition efficiencies in the whole respiratory tract and components (head airways, lung, alveolar region, and tracheobronchial region) were estimated and compared with the predictions of the Multiple Path Particle Dosimetry (MPPD) model (v2.11). The experimentally derived deposition efficiencies were broadly consistent with, but typically higher than, model predictions and the results of comparable studies in the literature.

Copyright © 2016 American Association for Aerosol Research     

Dihydroxyacetone levels in electronic cigarettes: Wick temperature and toxin formation

Recently, we reported the presence of dihydroxyacetone (DHA), the active ingredient in sunless tanners, in the aerosol of an electronic cigarette. DHA has been shown to react with DNA in vitro. The FDA restricts the use of DHA to external application only. It states that it should not be inhaled, ingested, or come into contact with any areas containing mucous membranes, due to unknown risk. Herein, the quantification of DHA in the aerosols of three brands of e-cigarettes has been carried out. These included two devices with horizontal heating coil configurations as well as one with a sub-ohm resistance vertical heating coil. In order to understand and begin to address the origin of DHA and related aerosol products, the wicking properties of the three e-cigarettes were compared. DHA levels were analyzed by a combination of GS/MS and ¹H NMR. DHA was found in all three e-cigarettes, with substantially less in the sub-ohm, vertical coil device as compared to the horizontal coil devices (e.g., 0.088 µg/puff vs. 2.29 µg/puff, respectively). Correspondingly, the temperature of the wet layer of the wick for the vertical coil was relatively stable, compared to the wicks for the horizontal coils, upon increasing battery power output. This result is in agreement with prior studies of e-cigarette wicking efficiency and aerosol toxin formation. The temperature measurements reported are a simple means for comparing devices with different design properties during operation.

Copyright © 2018 American Association for Aerosol Research     

Clouds and “throat hit”: Effects of liquid composition on nicotine emissions and physical characteristics of electronic cigarette aerosols

Electronic cigarettes (ECIGs) heat and vaporize a liquid mixture to produce an inhalable aerosol that can deliver nicotine to the user. The liquid mixture is typically composed of propylene glycol (PG) and vegetable glycerin (VG), in which are dissolved trace quantities of flavorants and, usually, nicotine. Due to their different chemical and thermodynamic properties, the proportions of PG and VG in the liquid solution may affect nicotine delivery and user sensory experience. In social media and popular culture, greater PG fraction is associated with greater “throat-hit,” a sensation that has been attributed in cigarette smokers to increased presence of vapor-phase nicotine. VG, on the other hand, is associated with thicker and larger exhaled “clouds.” In this study, we aim to investigate how PG/VG ratio influences variables that relate to nicotine delivery and plume visibility. Aerosols from varying PG/VG liquids were generated using a digitally controlled vaping instrument and a commercially available ECIG, and analyzed for nicotine content by GC-MS. Particle mass and number distribution were determined using a six-stage cascade impactor and a fast particle spectrometer (TSI EEPS), with tightly controlled dilution and sampling biases. A Mie theory model was used to compute the aerosol scattering coefficients in the visible spectrum. Decreasing the PG/VG ratio resulted in a decrease in total particulate matter (TPM) and nicotine yield (R² > 0.9, p < .0001). Measured particle count median diameter ranged between 44 and 97nm, and was significantly smaller for PG liquids. Although the particle mass concentration was lower, aerosols produced using liquids that contained VG had an order of magnitude greater light scattering coefficients. These findings indicate that PG/VG ratio is a strong determinant of both nicotine delivery and user sensory experience.

Copyright © 2017 American Association for Aerosol Research     

Toward the Determination of Joint Volatility-Hygroscopicity Distributions: Development and Response Characterization for Single-Component Aerosol

This work presents the development and characterization of a thermodenuder for the study and interpretation of aerosol volatility. Thermodenuder measurements are further combined with a continuous-flow streamwise thermal gradient CCN counter to obtain the corresponding aerosol hygroscopicity. The thermodenuder response function is characterized with monodisperse aerosol of variable volatility and hygroscopicity. The measurements are then interpreted with a comprehensive instrument model embedded within an optimization framework to retrieve aerosol properties with constrained uncertainty. Special attention is given to the interpretation of the size distribution of the thermodenuded aerosol, deconvoluting the effects of impurities and multiple charging, and to simplifications on the treatment of thermodenuder geometry, temperature, the cooling section, and the effects of curvature and accommodation coefficient on inferred particle volatility. Retrieved vapor pressures are consistent with published literature and shown to be most sensitive to uncertainty in the accommodation coefficient.

Copyright 2014 American Association for Aerosol Research     

Electronic cigarette-generated aldehydes: The contribution of e-liquid components to their formation and the use of urinary aldehyde metabolites as biomarkers of exposure

Electronic cigarettes (e-cigarette) have emerged as a popular electronic nicotine delivery system (ENDS) in the last decade. Despite the absence of combustion products and toxins such as carbon monoxide (CO) and tobacco-specific nitrosamines (TSNA), carbonyls including short-chain, toxic aldehydes have been detected in e-cigarette-derived aerosols up to levels found in tobacco smoke. Given the health concerns regarding exposures to toxic aldehydes, understanding both aldehyde generation in e-cigarette and e-cigarette exposure is critical. Thus, we measured aldehydes generated in aerosols derived from propylene glycol (PG): vegetable glycerin (VG) mixtures and from commercial e-liquids with flavorants using a state-of-the-art carbonyl trap and mass spectrometry. To track e-cigarette exposure in mice, we measured urinary metabolites of 4 aldehydes using ULPC-MS/MS or GC-MS. Aldehyde levels, regardless of abundance (saturated: formaldehyde, acetaldehyde???unsaturated: acrolein, crotonaldehyde), were dependent on the PG:VG ratio and the presence of flavorants. The metabolites of 3 aldehydes – formate, acetate, and 3-hydroxypropyl mercapturic acid (3-HPMA; acrolein metabolite) – were increased in urine after e-cigarette aerosol and mainstream cigarette smoke (MCS) exposures, but the crotonaldehyde metabolite (3-hydroxy-1-methylpropylmercapturic acid, HPMMA) was increased only after MCS exposure. Interestingly, exposure to menthol-flavored e-cigarette aerosol increased the levels of urinary 3-HPMA and sum of nicotine exposure (nicotine, cotinine, trans-3′-hydroxycotinine) relative to exposure to a Classic Tobacco-flavored e-cigarette aerosol. Comparing these findings with aerosols of other ENDS and by measuring aldehyde-derived metabolites in human urine following exposure to e-cigarette aerosols will further our understanding of the relationship between ENDS use, aldehyde exposure, and health risk.

© 2018 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     

Single Particle Measurements of the Optical Properties of Small Ice Crystals and Heterogeneous Ice Nuclei

Dust aerosol and ice crystals are two major types of nonspherical particles in the atmosphere which have significant roles in cloud-aerosol interactions and the radiative budget. The presence of dust and ice often coincide in the atmosphere because dust particles are efficient ice nuclei. The size and composition dependence of the scattering properties of dust and ice are needed to assess their individual contributions to the optical scattering of sunlight. Here we present a new measurement technique used to determine the single particle forward scattering, backscattering, and depolarization ratio (at a wavelength of 680 nm) for representative nonspherical atmospheric particles. The Texas A&M University Continuous Flow Diffusion Chamber (CFDC) was used as an ice crystal generator to produce ice crystals via both homogenous and heterogeneous nucleation mechanisms under well-controlled laboratory conditions. Optical scattering properties of mineral dusts and small ice crystals (0.6 μm to 50 μm optical diameter) were measured by the Droplet Measurement Technologies, Inc. (DMT) Cloud Aerosol Spectrometer with Polarization (CASPOL). Significant differences between the optical properties of single dusts and ice particles of the same size were observed. Differences between the optical signatures of homogeneously and heterogeneously nucleated ice crystals were not statistically significant. Our results suggest that atmospheric ice crystals can be identified and quantified independently from the dust particles on which they form based on analysis of their backscatter and depolarization signals.

Copyright 2014 American Association for Aerosol Research     

Effects of temperature on the formation of secondary organic aerosol from amine precursors

Aerosol formation is directly influenced by meteorological properties such as temperature and relative humidity. This study examines the influence of temperature on the physical properties and chemical composition of the aerosol produced from radical oxidation of aliphatic amines. Aerosol formation for temperatures ranging from 10 to 40°C was investigated in dual 90 m³ indoor atmospheric chambers. Further, chemical and physical responses of aerosol formed at one temperature and then raised/cooled to another were investigated in detail. Around two to three times more aerosol formation occurred at 10°C than at 40°C. This has important implications for locations influenced by amine emissions during the winter months. Significant aerosol formation occurred with the oxidation of amines with nitrate radical (100–600 μg/m³) and consisted largely of amine nitrate salts. These reactions are important contributors to aerosol formation during the nighttime hours, when nitrate radical is the dominant oxidant and temperatures tend to be cooler. Solid/gas partitioning of amine nitrate salt aerosol was consistent with literature results. A novel, temperature dependent, mechanism describing peroxy and hydroperoxy radical reactions was observed in the trimethylamine with hydroxyl radical oxidation experiments.

Copyright © 2016 American Association for Aerosol Research