Experimental evaluation of miniature plate DMAs (mini-plate DMAs) for future ultrafine particle (UFP) sensor network

Two iPhone-sized differential mobility analyzers (DMAs) in the parallel-plate configuration (i.e., mini-plate DMAs) were designed and their performance was calibrated in this study in order to gain the instructive knowledge for the future mini-plate DMA design and to have a well-calibrated mini-plate DMA for the ultrafine particle (UFP) sensor network. The performance of mini-plate DMAs was calibrated using the tandem DMA (TDMA) technique. The experimental transfer functions of prototypes at different particle sizes and under various combinational conditions of aerosol and sheath flow rates were derived from the TDMA data. It is concluded that mini-plate DMAs performed reasonably well for UFP sizing. It was also found that the sizing resolution of mini-plate DMAs is closer to the aerosol-to-sheath flow rate ratio when the percentage of aerosol slit opening in length was increased (relative to the width of aerosol classification zone). A new concept of “effective sheath flow rate” was introduced to better interpret the experimental observation on the area and FWHM (full width at half maximum) data of measured DMA transfer functions. Based on the experimental data, we proposed a modified equation for mini-plate DMAs to better calculate the voltage required to size particles of a given electrical mobility.

Copyright © 2016 American Association for Aerosol Research     

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     

Assessment of a Cylindrical and a Rectangular Plate Differential Mobility Analyzer for Size Fractionation of Nanoparticles at High-Aerosol Flow Rates

An existing differential mobility analyzer (DMA) of cylindrical electrodes and a novel DMA of rectangular plate electrodes are demonstrated for size fractionation of nanoparticles at high-aerosol flow rates in this work. The two DMAs are capable of delivering monodisperse size selected nanoparticles (SMPS σ_g < 1.1) at gas flow rates ranging from 200 slm to 500 slm. At an aerosol flow rate of 200 slm, the maximum attainable particle mean size is of about 20 nm for the cylindrical DMA and of nearly 50 nm for the rectangular plate DMA. The number concentration of the monodisperse nanoparticles delivered by the high-flow DMAs spans from 10⁴ cm^?3 to 10⁶ cm^?3 depending upon the particle mean size and particle size dispersion.

Copyright 2014 American Association for Aerosol Research     

Determination of the Mean Mobility of Aerosol Nanoparticles Classified by Differential Mobility Analyzers

MonteCarlo simulations of diffusive particle trajectories, as well as Stolzenburg's model calculations, have shown that the mean mobility of the particles classified by a differential mobility analyzer (DMA) at a given applied voltage may differ from the theoretical one inferred from the Knutson–Whitby equation if the particles are withdrawn from the tails of the particle mobility distribution. In this case, the true mean mobility, defined as the mean mobility of the particles classified at the specified voltage, can be precisely measured by a second DMA operating in series with the first one (tandem DMA). However, if particles are extracted from the central part of the distribution, their mobility can be correctly measured with a single DMA. Besides showing the importance of the usage of the tandem DMA technique for accurate measurements of mobility, this article provides an analytical expression which, if the mobility distribution of the polydisperse aerosol fed to the DMA is known, allows an accurate estimation of the true (mean) mobility of the classified particles.

Copyright 2014 American Association for Aerosol Research     

Portable Planar DMA: Development and Tests

A novel high-resolution planar and portable differential mobility analyzer (DMA) has been designed and built (Nano-ID® PMC500, Naneum, Canterbury, UK). Finite element multi-physics numerical modeling was employed to optimize the geometry of the DMA and to find a regime for high resolution within the confines of a portable instrument. The numerical approach for solving the Navier–Stokes equation was verified by comparison of calculated data to experimental values. The PMC500 was calibrated and tested with different monodisperse aerosol challenges. The PMC500 portable DMA is shown to have good sizing accuracy and resolution, similar in performance to commercially available desktop instruments.

Copyright 2014 American Association for Aerosol Research     

Methodology to quantify the ratio of multiple-to single-charged fractions acquired in aerosol neutralizers

A methodology for the quantification of the ratio of multiple- to single-charged fractions acquired in aerosol neutralizers is presented. These quantities are necessary for an accurate monodisperse calibration of aerosol instrumentation. A tandem Differential Mobility Analyzer (DMA) setup is required, with the second DMA scanning the electrical mobility spectra classified in the first DMA. In contrast to previous studies on the quantification of bipolar charge distribution utilizing tandem DMA schemes, the methodology targets at the direct determination of the multiple- to single-charge fractions and does so through the analysis of the raw signal instead of the inverted size distributions, thus circumventing errors associated with the assumptions in the DMA data inversion. The proposed methodology is employed for the characterization of different types of aerosols commonly employed for instrument calibration. Spherical liquid particles (emery oil and dioctyl sebacate) were found to acquire lower multiple charge fractions than those suggested by the commonly employed regression fits of Wiedensohler, which was published in the year 1988 in the Journal of Aerosol Science (vol. 19, pp. 387–389), but still within the range of values reported in the literature. Diffusion flame soot and spark generated graphite particles, produced by a miniCAST 6203C burner and a PALAS DNP 3000, respectively, exhibited higher fraction of multiple charges, in good agreement with previous work on agglomerates. The use of a soft X-ray bipolar charger (TSI 3088) yielded systematically higher multiple fractions of positive charges compared to a ⁸⁵Kr neutralizer (TSI 3077A), confirming the importance of direct photoionization charging on the former.

Copyright © 2016 American Association for Aerosol Research     

Accuracy of recovered moments for narrow mobility distributions obtained with commonly used inversion algorithms for mobility size spectrometers

Aerosol mobility size spectrometers are commonly used to measure size distributions of submicrometer aerosol particles. Commonly used data inversion algorithms for these instruments assume that the measured mobility distribution is broad relative to the DMA transfer function. This article theoretically examines errors that are incurred for input distributions of any width with an emphasis on those with mobility widths comparable to that of the DMA's transfer function. Our analysis is valid in the limit of slow scan rates, and is applicable to the interpretation of measurements such as those obtained with tandem differential mobility analyzers as well as broader distributions. The analysis leads to expressions that show the relationship between the inverted number concentration, mean size, and standard deviation and true values of those parameters. For narrow distributions (e.g., for a mobility distribution produced by a DMA with a 1:10 aerosol:sheath air flow ratio) under typical operating conditions, number concentrations and mean mobility obtained with inversion algorithms are accurate to within 0.5% and 1.0%, respectively. This corresponds to mean diameter retrieval errors of 1.0% for large particles and 0.5% for small (kinetic regime) particles. The widths (i.e., relative mobility variance) of the inverted distributions, however, significantly exceed the true values.

Copyright © 2018 American Association for Aerosol Research     

Modeling the thermodynamics and kinetics of sulfuric acid-dimethylamine-water nanoparticle growth in the CLOUD chamber

Dimethylamine (DMA) has a stabilizing effect on sulfuric acid (SA) clusters, and the SA and DMA molecules and clusters likely play important roles in both aerosol particle formation and growth in the atmosphere. We use the monodisperse particle growth model for acid-base chemistry in nanoparticle growth (MABNAG) together with direct and indirect observations from the CLOUD4 and CLOUD7 experiments in the cosmics leaving outdoor droplets (CLOUD) chamber at CERN to investigate the size and composition evolution of freshly formed particles consisting of SA, DMA, and water as they grow to 20 nm in dry diameter. Hygroscopic growth factors are measured using a nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA), which combined with simulations of particle water uptake using the thermodynamic extended-aerosol inorganics model (E-AIM) constrain the chemical composition. MABNAG predicts a particle-phase ratio between DMA and SA molecules of 1.1–1.3 for a 2 nm particle and DMA gas-phase mixing ratios between 3.5 and 80 pptv. These ratios agree well with observations by an atmospheric-pressure interface time-of-flight (APi-TOF) mass spectrometer. Simulations with MABNAG, direct observations of the composition of clusters <2 nm, and indirect observations of the particle composition indicate that the acidity of the nucleated particles decreases as they grow from ～1 to 20 nm. However, MABNAG predicts less acidic particles than suggested by the indirect estimates at 10 nm diameter using the nano-HTDMA measurements, and less acidic particles than observed by a thermal desorption chemical ionization mass spectrometer (TDCIMS) at 10–30 nm. Possible explanations for these discrepancies are discussed.

Copyright © 2016 American Association for Aerosol Research     

Performance Evaluation of the Brechtel Mfg. Humidified Tandem Differential Mobility Analyzer (BMI HTDMA) for Studying Hygroscopic Properties of Aerosol Particles

The Tandem Differential Mobility Analyzer (TDMA) technique coupled with aerosol humidification has been widely used for studying aerosol hygroscopicity. In this study, we evaluate the performance of a commercial Humidified TDMA (BMI HTDMA, Model 3002) with respect to DMA sizing, relative humidity (RH) control, and growth factor (GF) measurements. Unique features of this particular HTDMA include a diffusion-based particle humidifier, a DMA design allowing selection of particles up to 2 μm diameter at only 5600 volts, and the ability to study the complete deliquescence and efflorescence cycle. The sizing agreement between DMA 1 and 2 was within 2% over the 35 to 500 nm diameter range. The measured TDMA responses agreed well with theoretical calculations. The RH control and stability were tested at a suburban field site in Hong Kong. The system achieved RH equilibrium in less than 4 min when changing the RH set point. With indoor temperature changes of less than 1°C per hour, the RH control of the system was very stable at 90%, within 1% RH deviation, as confirmed by GF measurements on ammonium sulfate (AS) aerosols performed on separate days. The hygroscopic properties of various pure aerosols were examined and the results agreed well with model predictions. The application of the BMI HTDMA for field measurements was also demonstrated. Two modes were resolved from the GF distributions at 90% RH and variable hygroscopic growth with changing RH was observed.

Copyright 2014 American Association for Aerosol Research     

Effect of Aerosol Volatility on the Sizing Accuracy of Differential Mobility Analyzers

Differential mobility analyzers (DMAs) are widely used for calibrating other instruments and measuring aerosol size distributions. DMAs classify aerosol particles according to their electrical mobility, which is assumed to be constant during the classification process. However, particles containing semivolatile substances can change their size in the DMA, leading to sizing errors. In this article, the effect of particle size changes during the classification process on the sizing accuracy of DMAs is discussed. It is shown that DMAs select particles whose time-of-flight-averaged electrical mobility is equal to that of stable particles that are selected under given operating conditions. For evaporating particles, this implies that DMAs select particles that are originally larger than the reported size. At the exit of the DMA, selected particles are smaller than the reported size. Particle evaporation and growth inside DMAs was modeled to study the effect of particle size changes on the sizing accuracy and the transfer function of DMAs in constant- and scanning-voltage modes of operation. Modeling predictions were found to agree well with the results of experiments with ammonium nitrate aerosol. The model was used to estimate sizing errors when measuring hygroscopic and other volatile aerosols. Errors were found to be larger at smaller sizes and low sheath flow rates. Errors, however, are fairly small when saturation concentration is below 10 μg/m³, assuming an evaporation coefficient of 0.1. Particles size changes during classification lead to distortion of the DMA transfer function. In voltage scanning mode, errors are generally larger, especially at high scan rates.

Copyright 2014 American Association for Aerosol Research     

Measuring aerosol size distributions with the aerodynamic aerosol classifier

The Aerodynamic Aerosol Classifier (AAC) is a novel instrument that selects aerosol particles based on their relaxation time or aerodynamic diameter. Additional theory and characterization is required to allow the AAC to accurately measure an aerosol’s aerodynamic size distribution by stepping while connected to a particle counter (such as a Condensation Particle Counter, CPC). To achieve this goal, this study characterized the AAC transfer function (from 32 nm to 3 μm) using tandem AACs and comparing the experimental results to the theoretical tandem deconvolution. These results show that the AAC transmission efficiency is 2.6–5.1 times higher than a combined Krypton-85 radioactive neutralizer and Differential Mobility Analyzer (DMA), as the AAC classifies particles independent of their charge state. However, the AAC transfer function is 1.3–1.9 times broader than predicted by theory. Using this characterized transfer function, the theory to measure an aerosol’s aerodynamic size distribution using an AAC and particle counter was developed. The transfer function characterization and stepping deconvolution were validated by comparing the size distribution measured with an AAC-CPC system against parallel measurements taken with a Scanning Mobility Particle Sizer (SMPS), CPC, and Electrical Low Pressure Impactor (ELPI). The effects of changing AAC classifier conditions on the particle selected were also investigated and found to be small (<1.5%) within its operating range.

Copyright © 2018 American Association for Aerosol Research     

Size and volatility of particle emissions from an ethanol-fueled HCCI engine

A scanning mobility particle sizer was used to determine the size, number, and mass concentration of particle emissions from an ethanol-fueled homogeneous charge compression ignition (HCCI) engine. Semi-volatile particle composition was characterized using tandem differential mobility analysis (TDMA). Variable temperature thermal conditioning was used to gain insight into particle volatility and a catalytic stripper was used to determine the solid particle distribution. Four engine conditions were evaluated, including low to moderate range loads and motoring (deceleration, coasting). Results indicated that aerosol from a fully premixed HCCI engine under firing conditions is formed almost entirely via nucleation of semi-volatile material originating from the lubricating oil. TDMA analysis indicated 98% of total particle volume evaporated below 100°C. Results pointed towards homogeneous nucleation of precursors derived from the organic species in the lubricating oil, possibly in combination with a sulfur species. The motoring condition, with no fuel injected, exhibited the highest number and mass concentrations. During motoring, there was poor sealing leading to increased atomization of oil and associated ash emissions. Emissions were lower during firing with better sealing and much less atomization, but evaporation of the most volatile fractions of the lubricating oil still led to significant PM emissions consisting of nearly entirely semi-volatile particles containing very little ash.

© 2017 American Association for Aerosol Research     

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     

Assessment of indoor bioaerosols using a lab-made virtual impactor

To assess indoor bioaerosols, a virtual impactor having 1 µm cutoff diameter was designed, fabricated, and evaluated with computational fluid dynamics simulation and also with laboratory test using polystyrene latex particles. Two other cutoff diameters of 635 nm and 1.5 µm were obtained by changing the inlet flow rate and the ratio of minor channel-to-inlet flow rates. In field test, the virtual impactor was operated with varying cutoff diameter and field-emission scanning electron microscope (FE-SEM) analysis was performed for each cutoff diameter to observe morphologies of indoor aerosol particles sampled at the major and minor outlet channels. Particles were sampled at both outlet channels using the SKC Button Aerosol sampler and subsequently cultured. By colony counting, it was found that 56% of cultured fungal particles and 63% of cultured bacterial particles had aerodynamic sizes smaller than 1 µm. MALDI-TOF analysis and visual inspection of culture samples were used to identify indoor bacterial and fungal species, respectively. Nearly same species of bacteria and fungi were detected both in the major and minor flow channels.

© 2017 American Association for Aerosol Research     

Rectangular Slit Atmospheric Pressure Aerodynamic Lens Aerosol Concentrator

A rectangular slit micro-aerodynamic-lens (μADL) aerosol concentrator operating at atmospheric pressure has been developed. A single stage version has shown concentration ratios of up to 40:1 for 1 μm aerosol particles while particles larger than 2 μm can be concentrated by more than 100:1 in a single stage. The design of this device has been guided by unsteady 3D CFD modeling using detached eddy simulations (DES), and has been validated experimentally using polystyrene spheres and salt crystals of known aerodynamic diameters. The pressure drop in the device does not exceed 1.5 kPa in the major flow and 0.3 kPa in the minor flow at a total flow of 10 slpm.

Copyright 2014 American Association for Aerosol Research     

Spatial aerosol flow maldistribution: A design flaw confounding the proper calibration and data interpretation of stages “0” and “1” of the Andersen eight-stage nonviable cascade impactor

We introduced monodisperse calibrant particles into an eight-stage non-viable Andersen cascade impactor (ACI) operated at 28.3 L/min and separately quantified the particle mass captured under each of the four concentric rings of nozzles on stages 0 and 1, the entry and succeeding stages of this impactor. On both stages, we found that each ring of nozzles has a particle capture efficiency behavior that differs from the others, and the fraction of calibrant particles deposited under each of the individual rings of nozzles depended on the particle size. We believe this behavior derives primarily from a radial flow velocity non-uniformity associated with recirculation zones introduced by the 110° expansion angle of the inlet cone. Because of these recirculation zones, the inertia of particles larger than about 5 µm aerodynamic diameter will cause their point-wise local concentration to differ from the concentration at the inlet entry. This concentration maldistribution continues to stage 1 primarily because of the annular collection plate at stage 0. The influence of the inlet cone aerodynamics on the performance of both stages means that the size of particles deposited on these plates will be uncertain unless the aerosol transport entering the impactor associated with calibration using monodisperse particles exactly simulates the in-use aerosol flow conditions. The degree of realism necessary in the calibration method has heretofore not been discussed in published calibrations of the ACI, introducing uncertainty in the size interpretation of the particle mass collected on stages 0 and 1 in practical applications of this impactor.

Copyright © 2017 American Association for Aerosol Research     

A New Laser Induced Incandescence–Mass Spectrometric Analyzer (LII-MS) for Online Measurement of Aerosol Composition Classified by Black Carbon Mixing State

We developed a laser induced incandescence–mass spectrometric analyzer (LII-MS) for online measurements quantifying the aerosol chemical compositions with respect to the mixing state of black carbon (BC). The LII-MS is developed as a tandem series comprising an LII chamber to detect and vaporize BC-containing particles and a particle trap laser desorption mass spectrometer (PT-LDMS: Takegawa et al. 2012). The PT-LDMS collects aerosol particles transferred from the LII chamber and quantifies the chemical compositions. A newly designed collection probe, coupled with the sheath-air inlet nozzle of the LII chamber, enables a high throughput of aerosol particles without significant dilution. Total aerosol particles can be analyzed in the PT-LDMS by turning off the laser (MS mode), and the aerosol particles externally mixed with BC can be analyzed by turning on the laser (LII-MS mode). The difference in the PT-LDMS signals between the MS and LII-MS modes yields the chemical composition of materials internally mixed with BC. Performance of the developed instrument was evaluated in the laboratory by generating BC particles internally-mixed with oleic acid (OL) and BC particles externally mixed with ammonium sulfate particles. Preliminary results from ambient measurements are also presented and discussed.

Copyright 2014 American Association for Aerosol Research     

Eliminating the main source of instability and turbulence in TSI's 3071 DMA

The transfer function of TSI's widely used 3071 Differential Mobility Analyzer (DMA) widens drastically when the flow rate Q of sheath gas exceeds 30–40 lit/min, limiting its ability to resolve very small particles. This flow instability is unexpected at the prevailing relatively small Reynolds number (Re < 400). Here, we note that the rings holding the laminarization screens penetrate into the flow channel, generating unsteady vortices. A screen step exists not only on the outer screen region, but also on the inner screen region. Using a new step-free screen, no critical transition is observed up to the highest flow rate achieved of Q = 103 lit/min. The original DMA widens the flow cross-section in the mixing region where the aerosol joins the sheath gas. The flow deceleration then arising at small aerosol input flow rates introduces another source of transfer function broadening, which, however, has negative resolution effects only at Q > 60 lit/min. This feature is suppressed here by modifying a single inlet piece. Although the two flow improvements implemented increase the resolving power in the analysis of very small particles, a substantial non-ideality of unclear origin remains: the best resolving power R found with electrosprayed ions of the protein Immunoglobulin is R = 13.9 for the trimer (IgG)₃, and 12 for the monomer, even at a sheath/aerosol flow ratio of 100.

© 2017 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     

An integrative model for the filtration efficiencies in realistic tests with consideration of the filtration velocity profile and challenging particle size distribution

Many well-established models can be applied to calculate the filtration efficiencies. In these models the filtration velocity and challenging particle size are assumed to be known accurately. However, in realistic filtration tests, the filtration velocity has profiles dependent on the filter holder geometry and experimental conditions; the challenging particles have size distributions dependent on the instruments and operation conditions. These factors can potentially affect the measured filtration efficiency and lead to discrepancies with the models.

This study aims to develop an integrative model to predict the filtration efficiencies in realistic tests by incorporating the effects of the filtration velocity profile and challenging particle size distribution classified by a differential mobility analyzer (DMA) into the existing filtration models. Face velocity profile is modeled with fluid mechanics simulations; the initial generated particle size distribution, the particle charging status and the DMA transfer function are modeled to obtain the challenging particle size distribution. These results are then fed into the filtration models. Simulated results are compared with experimental ones to verify the model accuracy. This model can be used to reduce filtration test artifacts and to improve the experimental procedure.

The results reveal that the face velocity upstream the filter exhibits high degree of homogeneity not affecting the filtration efficiency if the filter pressure drop is not very low. The generated particle size distribution and the DMA selection size window could influence the challenging particle size distribution and therefore the measured filtration efficiency.

Copyright © 2017 American Association for Aerosol Research