Size Distributions of Motor Vehicle Exhaust PM: A Comparison Between ELPI and SMPS Measurements

Particle size measurements using the electrical low pressure impactor (ELPI) and scanning mobility particle sizer (SMPS) are compared from the perspective of characterizing the particulate matter in motor vehicle exhaust. Both steady state vehicle operation and transient drive cycles are considered, and both gasoline and diesel fueled vehicle emissions are compared. Although the ELPI and SMPS measure different physical properties, respectively, the aerodynamic diameter and mobility diameter, the steady state particle size distributions are in close agreement, except for the 37 nm impactor stage of the ELPI which may overestimate particle number by up to a factor of two relative to the SMPS. This has little effect on the volume, or mass, weighted distribution. These, too, are generally in good agreement, though discrepancies appear at large particle size due to multiple charging effects in the SMPS and to electrometer offsets and the small particle loss correction in the ELPI. Selecting particles based on their electrical mobility with the SMPS, and then measuring their aerodynamic diameter with the ELPI, reveals that diesel particulate matter with well-specified mobility diameter exhibits a wide range in aerodynamic diameter and, therefore, also in effective density. Over transient drive cycles, the ELPI provides second by second particle distributions, whereas the SMPS must be run in a fixed particle size mode and size distributions constructed from repeated tests. The ELPI registers higher instantaneous PM emission rates during transients than the SMPS due to the faster time responses of the ELPI. The time integrated ELPI and SMPS size distributions, however, remain in good agreement. The relative merits of the two instruments for steady state and transient tests are discussed.     

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.     

On the effective density of non-spherical particles as derived from combined measurements of aerodynamic and mobility equivalent size

Effective densities derived from combined mobility and aerodynamic sizing provide a valuable tool for the characterization of non-spherical particles. Different effective densities have been introduced depending on the primary measurement parameters (mass, mobility and/or aerodynamic size) and the flow regime (transition, free-molecular). Here we explore the relationship between these effective densities, their physical interpretation and their dependence on particle shape, density and various equivalent diameters. We also provide an overview over the wide range of practical implications of the effective density concept with a particular focus on the characterization of particles with irregular or even unknown shape using commercially available instruments such as DMA, SMPS, FMPS, ELPI, APS, TEOM and multi-stage impactors. Finally, we identify new perspectives for particle characterization by extending the effective density concept into the free-molecular regime and by suggesting a triple-instrument approach for on-line determination of both particle density and shape as well as the dynamic shape factor for different flow regimes.     

Tandem Measurements of Aerosol Properties—A Review of Mobility Techniques with Extensions

When multiple instruments are used in tandem it is possible to obtain more complete information on particle transport and physicochemical properties than can be obtained with a single instrument. This article discusses tandem measurements in which submicrometer particles classified according to electrical mobility are then characterized with one or more additional methods. Measurement combinations that are summarized here include mobility plus mass, aerodynamic (or vacuum aerodynamic) diameter, integrated or multiangle light scattering, composition by single particle mass spectrometry, electron microscopy, and so on. Such measurements enable intercomparisons of different measures of size including mobility diameter, optical size, aerodynamic diameter, volume (for agglomerates and nanowires), length (for nanowires), and mass, even for particles that are morphologically and chemically complex. In addition, the article summarizes the use of tandem techniques to measure various transport properties (e.g., dynamic shape factor, sedimentation speed, diffusion coefficient) and physicochemical properties (e.g., mixing state, shape, fractal dimension, density, vapor pressure, equilibrium water content, composition). In addition to providing an overview of such tandem measurements we describe previously unreported results from several novel tandem measurement methods.     

Effective density of airborne particles in a railway tunnel from field measurements of mobility and aerodynamic size distributions

The objective of this study is to investigate the particle effective density of aerosol measurements in a railway tunnel environment. Effective density can serve as a parameter when comparing and calibrating different aerosol measurements. It can also be used as a proxy parameter reflecting the source of particles. Effective density was determined using two different methods. Method one defined it by the ratio of mass concentration to apparent volume size distribution. Method two relied on a comparison of aerodynamic and mobility diameter size distribution measurements. The aerodynamic size range for method one was 0.006–10?µm, and for method two, it was 10–660?nm. Using the first method, a diurnal average value of about 1.87?g/cm³ was observed for the measurements with tapered element oscillating microbalance (TEOM) in tandem with aerodynamic particle sizer?+?scanning mobility particle sizer (SMPS), and 1.2?g/cm³ for the combination of TEOM with electrical low pressure impactor plus (ELPI+) in the presence of traffic. With method two, the effective density was 1.45?g/cm³ estimated from the size distribution measurements with ELPI?+?and fast mobility particle sizer (FMPS), and 1.35?g/cm³ from ELPI?+?in tandem with SMPS. With both calculation methods, the effective density varied for conditions with and without traffic, indicating different sources of particles. The proportion of particles with small sizes (10–660?nm) had a significant effect on the value of the effective density when no traffic was operating. The responses of different instruments to the railway particle measurements were also compared.

Copyright © 2018 The Authors. Published with license by Taylor &; Francis Group, LLC     

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 TRANSMISSION EFFICIENCY THROUGH THE NOZZLE OF THE API AEROSIZERTM

This study has investigated the particle transmission efficiency through the nozzle of the API Aerosizer^TM numerically. Two-dimensional flow field in the nozzle was first simulated. Particle trajectories for both liquid and solid particles were then calculated to obtain the particle transmission efficiency under various conditions. This study shows that particle aerodynamic diameter, particle materials, particle density and laser beam diameter influence the transmission efficiency. The transmission efficiency is found to increase with increasing particle diameter when the particle aerodynamic diameter is less than several micrometers. The efficiency for liquid particles drops significantly when particle aerodynamic diameter increases from several micrometers because of particle impaction loss in the nozzle. For solid particles, the relationship of the efficiency with particle diameter is found to be more complicated. For particles less than several micrometers in aerodynamic diameter, solid particles behave similarly to the liquid particles. However, as particles are greater than several micrometers, the effect of solid particle bounce is to increase the transmission efficiency with increasing aerodynamic diameter until particles become large enough so that plastic deformation occurs in the particles. Then the transmission efficiency will decrease with increasing particle aerodynamic diameter.     

Aerosolisation behaviour of micronised and supercritically-processed powders

Comparative analysis of salmeterol xinafoate (SX) powders was carried out to define the aerodynamic properties and mechanism of particle dispersion relevant to the use of these materials in dry powder inhalation drug delivery. Particle sizing methodology was evaluated using laser diffraction, time-of-flight and Andersen cascade impactor measurements combined with electron microscopy and surface area determination. Particle interactions, assessed on the basis of powder bulk density and inverse gas chromatography surface energy measurements, were compared with the aerodynamic forces generated by a dry-powder dispersion device. The supercritically produced material showed by a factor of seven reduced tensile strength of the aggregates and indicated a two-fold increase of fine particle fraction deposited in a cascade impactor when blended with lactose. This effect was explained by the reduced particle aggregation at low differential air pressures and flow rates. A relatively small value of aerodynamic stress required to disperse supercritically produced particles in comparison to micronized material comes from: (a) lower bulk density (loose aggregate structure), (b) larger volume mean diameter, (c) larger aerodynamic shape factor and (d) smaller specific free energy of S-SX particles, in this order of priority. It is shown that aggregation between primary drug particles is important for SX/lactose formulations because such aggregates survive the pre-separation impactor stage.     

Modification of the ELPI to measure mean particle effective density in real-time

A new modification of electrical low pressure impactor (ELPI) for the particle effective density measurement is presented. The system is capable of real-time operation and it is based on the serial measurement of mobility and aerodynamic diameter. In the studied configuration, a zeroth order mobility analyser is installed inside of the ELPI-instrument. The system is feasible for single modal distributions. For several particle materials and varying size distributions, the measured average density values were within 15% of the values obtained with a reference method.     

Application of fractal theory to estimation of equivalent diameters of airborne carbon nanotube and nanofiber agglomerates

Understanding transport characteristics of airborne nanotubes and nanofibers is important for assessing their fate in the respiratory system. Typically, diffusion and aerodynamic diameters capture key deposition mechanisms of near-spherical particles such as diffusion and impaction in the submicrometer size range. For nonspherical particles with high aspect ratios, such as aerosolized carbon nanotubes, these diameters can vary widely, requiring their independent measurement. The objective of this study was to develop an approach to provide approximate estimates of aerodynamic- and diffusion-equivalent diameters of airborne carbon nanotubes (CNTs) and carbon nanofibers (CNFs) using their morphological characteristics obtained from electron micrographs. The as-received CNT and CNF materials were aerosolized using different techniques such as dry dispersion and nebulization. Mobility and aerodynamic diameters of test aerosol were directly deduced from tandem measurement of particle mobility and mass. The same test aerosol was mobility-classified and subsequently collected on a microscopy grid for transmission electron microscopy (TEM) analysis. TEM micrographs were used to obtain projected area, maximum projected length, and two-dimensional (2-D) radius of gyration of test particles. Estimates of the aerodynamic diameter and the diffusion diameter were obtained by applying the fractal theory developed for aerosol agglomerates of primary spherical particles. After accounting for the particle dynamic shape factor, estimated aerodynamic diameters agreed with those from the direct measurements (using tandem mobility-mass technique) within 30–40% for the agglomerates with relatively open structures while the diffusion diameters agreed within 40–50%. The uncertainty of these estimates mainly depends on degree of overlapping structures in the microscopy image and nonuniformity in tube diameter. The approach could be useful in calculating approximate airborne properties from microscopy images of CNT and CNF agglomerates with relatively open structures.

This article not subject to US copyright law     

Extending the Capabilities of Single Particle Mass Spectrometry: II. Measurements of Aerosol Particle Density without DMA

Particle density is an important and useful property that is difficult to measure because it usually requires two separate instruments to measure two particle attributes. As density measurements are often performed on size-classified particles, they are hampered by low particle numbers, and hence poor temporal resolution. We present here a new method for measuring particle densities using our single particle mass spectrometer, SPLAT. This method takes advantage of the fact that the detection efficiency in our single particle mass spectrometer drops off very rapidly as the particle size decreases below 100 nm creating a distinct sharp feature on the small particle side of the vacuum aerodynamic size distribution. Thus, the two quantities needed to determine particle density, the particle diameter and vacuum aerodynamic diameter, are known. We first test this method on particles of known compositions and densities to find that the densities it yields are accurate. We then apply the method to obtain the densities of particles that were characterized during instrument field deployments. We illustrate how the method can also be used to measure the density of chemically resolved particles. In addition, we present a new method to characterize the instrument detection efficiency as a function of particle size that relies on measuring the mobility and vacuum aerodynamic size distributions of polydisperse spherical particles of known density. We show that a new aerodynamic lens used in SPLAT II improves instrument performance, making it possible to detect 83 nm particles with 50% efficiency.     

A Novel Particle Trap Impactor for Use with the Gas-Quenching Probe Sampling System

A novel particle trap impactor has been developed for use with the gas-quenching probe in order to exclude solid particles from entering into the probe during sampling of gaseous metallic species in fluidized bed combustion conditions. The impactor must be small in size (Ø_impactor ≤ Ø_probe = 45 mm) but capable of collecting a relatively large amount of particles at elevated temperatures. As the first step, the impactor was designed, constructed, and tested at room temperature for KCI aerosol particles. The impactor with a nozzle of 0.95 mm in diameter, in combination with the orifice-to-jet diameter ratio of 1.5 and the ratio of the jet-to-plate spacing to jet diameter at 1.4 yielded a sharp cutoff curve with a maximum collection efficiency of about 0.9 and a √Stk₅₀ value of about 0.22. In addition, the collection efficiency of the impactor was compared with the particle removal efficiency of a filter of the same type as the filter previously used with the gas-quenching probe. The difference from the comparison is very small, indicating that the impactor can be used to replace the filter to prevent fly ash particles from entering the gas-quenching probe in fluidized bed combustion conditions.     

On the Effect of Particle Alignment in the DMA

The Differential Mobility Analyzer (DMA) is designed to measure particle mobility diameter, which for spherical particles is equal to particle volume equivalent diameter. In contrast, the mobility diameter of aspherical particles is a function of the particle shape and orientation. The magnitude of the DMA electric fields is such that it can cause aspherical particles to align preferentially in a specific orientation. The same electric field and the sheath flow rate ( q _sh ) define the particle mobility diameter. But, the fact that particle orientation depends on the electric field makes the dynamic shape factor and hence the mobility diameter depend on q _sh . Here, we describe an operating procedure that relies on a tandem DMA system, in which the second DMA is operated at a number of q _sh , to obtain information about particle shape by measuring the effect of particle alignment on the particle mobility diameter. We show how the relationship between the mobility diameter and q _sh can even be used to physically separate particles according to their shapes. In addition we explore the use of simultaneous measurements of particle alignment and particle vacuum aerodynamic diameters to gain further information on particle shape and account for particle alignment in the calculations of dynamic shape factor. We first test this approach on doublets and compact triplets of PSL spheres, for which the orientation dependent dynamic shape factors are known. We then investigate applications on a number of polydisperse particle systems of various shapes.     

Design of a Glass Impactor for an Annular Denuder/Filter Pack System

A glass impactor for an annular denuder/filter pack system was developed, to further the application of denuder technology in sampling atmospheric gases and particles. The glass impactor consists of an entrance section containing the inlet tube, the acceleration jet, and the impaction plate, which is mounted at the entrance to the annular denuder. The impaction plate is a removable porous glass disk which can be impregnated with mineral oil to minimize bounce-off of the collected particles during sampling. Calibration tests showed that the impactor has a 50% aerodynamic particle cutoff size of 2.1 μm, at a flow of 10 L min^?1. Particle loss experiments were conducted. Total losses on surfaces inside the impactor, annular denuder, and filter pack, determined for particle sizes ranging between 1.50 and 2.77 μm, were lower than 3%. Co-located air sampling was conducted using the glass impactor and the Harvard impactor. Mass concentrations determined using the Harvard impactor were about 10% higher than for the glass impactor because the glass impactor has a slightly lower aerodynamic particle cutoff point, while sulfate concentrations obtained from the two systems were in excellent agreement.     

High Precision Density Measurements of Single Particles: The Density of Metastable Phases

We describe a system designed to measure the size, composition, and density of individual spherical particles in real time. It uses a Differential Mobility Analyzer (DMA) to select a monodisperse particle population and the single particle mass spectrometer to measure individual particle aerodynamic diameter. Together the mobility and aerodynamic diameters yield particle density. The mass spectrometer aerodynamic sizing resolution d _{ν a} /Δ d _{ν a} is ～ 50 and > 100 for 200 nm and 800 nm particles respectively and together with the DMA the overall system resolution is 20. We demonstrate that the line shape of the aerodynamic size distribution can be used to identify asphericity. We present results from two operational schemes: one suitable for most applications, yielding particle density with a precision of ± 2.5%, and a high precision variant, that uses an internal calibrant to remove any of the systematic errors and significantly improves the measurement quality. The high precision scheme is most suitable for laboratory studies, making it possible to follow slight changes in particle density. An application of the system to measure the density of hygroscopic particles in deep metastable phases near zero relative humidity is presented. The density data presented here are consistent with conclusions reached in a number of other studies, namely, that some particle systems, once deliquesced, persist as droplets down to near zero relative humidity.     

Generation of Airborne Multi-Walled Carbon Nanotubes for Inhalation Studies

Recent studies suggest that inhaled or intratracheally instilled multi-walled carbon nanotubes (MWCNTs) cause adverse health effects depending on the fiber length. In the present study a simple batch particle generation system was developed to generate airborne MWCNTs for inhalational toxicology studies. The generation rate can be controlled by the amplitude of sieve shaker. Maximum concentration of respirable airborne MWCNTs was 1.2 mg m^–3 at a nose-exposure chamber supplied with air at flow rate of 30 L min^–1. We examined the performance of airborne MWCNT generation system and characterized properties of generated fibrous particles at mass concentrations of 0.4 mg m^–3 (particle number; ca. 1700 cm^–3). Monomodal shaped size distributions with peak located at electrical mobility diameter of 300 nm (in number) and aerodynamic diameter of 1–2 μm (in mass) were measured with a scanning mobility particle sizer and with a low-pressure impactor, respectively. Two hour particle generation reproducibility tests were conducted five times, in which stability and repeatability of particle size and total number concentration were within an acceptable range. Aerodynamically classified particle morphology was studied by TEM, dissociated fiber-like and agglomerated MWCNT particles were observed. The former contributes up to 38% to counted particles, and the average width and length of fiber were 80 nm and 3.7 μm, respectively, with an aerodynamic size for particle of 260–381 nm.     

Design and Test of 2.5 μ m Cutoff Size Inlet Based on a Particle Cup Impactor Configuration

Based on the particle cup impactor configuration, an inlet for sampling fine particles smaller than 2.5 w m in diameter was designed for operation at a flow rate of 25 l/min. To determine the optimal dimensions of the particle cup impactor applicable to the PM 2.5 inlet, calibration experiments were carried out at wind velocities of 2 and 24 km/h in a wind tunnel. It was noted that the particle cup impactor having an impaction nozzle diameter of 3.2 mm and the nozzle-to-cup spacing of 3.6 mm yielded a sharp size cutoff. Supplementary experiments were conducted on sampling performance with the inlet having the optimally selected configuration at a near-zero wind speed in the test chamber. Results of the tests showed the inlet had a cutoff size of 2.43 w m in aerodynamic diameter, at 25 l/min, and that particles larger than 2.5 w m were trapped in the cup. Additional experiments covering a flow rate between 10 and 40 l/min with particle sizes between 0.8 and 4.3 w m were conducted in the test chamber. A field test was performed to examine the PM 2.5 inlet in real situations. The performance indicated that the inlet design met the basic requirements of fine-particle sampling.     

Depositional arrangement of non-spherical atmospheric particles on impaction plate of a multi-nozzle impactor

Abstract

Aerosols and dust particles as a main component of atmospheric composition are of different shapes and sizes and affect the human health. Over the recent decades, the sampling, analysis and characterization of aerosol and dust particles have been a significant challenge. Finding a relationship between the location of particle deposition on impaction plate and its size and shape is very important for mineralogical and geochemical analysis. Hence, in this investigation, a common multi-nozzle impactor was taken and the arrangement of collected particles with different shapes and diameters on impaction plate was analyzed. Because of the highly priced geochemical and mineralogical analysis of atmospheric particles collected by the impactor, the results of this study can be used as a preliminary classifier for analyzing the accumulated atmospheric particles. In this study, a multi-nozzle impactor was three-dimensionally simulated. The simulation was carried out by applying Eulerian-Lagrangian approach. The experimental tests were also accomplished for sampling of the atmospheric particles. As the results of this study, the collection efficiency curve for the atmospheric particles with different shape factors was numerically obtained. As the most important result of this study, the location of particles deposited with diameters 2.5?µm and 5?µm and with shape factor of 1, 0.5 and 0.3 on impaction plate was numerically calculated. Due to these results, on one hand the central/outer parts of primary deposits mostly contain relatively coarse/fine-sized particles with high sphericity. On the other hand, the linear/low-cumulative deposits between adjacent jets mostly contain relatively fine/coarse-sized particles with low sphericity and angular shapes. Three-dimensional simulation results matched well with experimental sampling data.

Copyright © 2019 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     

Visualization of Defect Particle Transmission to the Major Flow of a Slit Virtual Impactor

Convective transport behavior of monodisperse supermicron particles has been analyzed in a slit virtual impactor. Particle trajectories were visualized using video imaging of scattered light and fluorescence from particles traversing the separation region of the impactor. The collection efficiency of the major flow was measured on an individual-particle basis for bulk Stokes numbers ranging from 0.42 to 25. We present an analysis based upon the local Stokes number to explain the transmission frequency of particles significantly larger than the 50% cutoff diameter into the major flow. The transmission efficiency calculated from the local Stokes number exhibits good agreement with the measured collection efficiencies.