High-Resolution Reconstruction Method for Presenting and Manipulating Particle Histogram Data

Modern electronic aerosol instruments such as the scanning mobility analyzer or the aerodynamic particle sizer provide size information at much higher resolution than older impactors or optical particle counters do. Whereas an impactor may span a decade of particle diameter with two or three stages, an aerodynamic instrument may do so with 25-30 channels and a scanning mobility spectrometer with 64 channels. Whether or not the channels represent real particle size discrimination, comparison of data between high- and low-resolution instruments would be made easier if the data resolution could be made comparable. Moreover, the problems of converting mass concentration measurements to number concentrations (and vice versa) would be facilitated if there were high resolution size bins to use for computations, rather than having to rely on some average size to represent all the particle sizes within a size band. We present here an interpolation method for redistributing coarse histogram data into finer size bins without compromising the original data and including information gleaned from experience with multiple aerosol measurements. It is based upon a simple smoothness criterion and can be implemented in many computer spreadsheet programs.     

Causes of Concentration Differences Between a Scanning Mobility Particle Sizer and a Condensation Particle Counter

Accurate aerosol concentration measurement is important in many applications of aerosol science. Here we compare aerosol concentration measurements of classified NaCl aerosol in the size range of 20 to 80 nm (diameter) between a scanning mobility particle sizer (SMPS) and a condensation particle counter (CPC). The SMPS systematically measured higher concentrations than the CPC, with the difference increasing with decreasing particle size. Experiments suggest several causes for the discrepancy. First, the factory calibration of the SMPS impactor flow was incorrect for the study site at 780 mbar. Second, the neutralizer used in the SMPS was inefficient in bringing the classified aerosol to charge equilibrium, and third, there were significant losses of charged aerosol within the CPC. The comparisons were improved with proper impactor flow calibration and proper charge neutralization of the classified aerosol before measurement by the SMPS and CPC. The results of this study point to the importance of proper conditioning of aerosol below about 100 nm for measurement with the SMPS and condensation-based particle counters.     

Design and performance of an optimized electrical diffusion battery

Standard aerosol instruments to measure particle size distributions in the ultrafine size range are large and heavy. We built a small electrical diffusion battery, which can be carried in a backpack and thus makes size-resolved short-term personal aerosol exposition measurements possible. The instrument was designed for maximal measurable particle size range and long maintenance intervals. The optimum number of stages for the diffusion battery was found with a Monte-Carlo simulation. To assess the instrument's performance, we compared size distributions measured with the electrical diffusion battery to those obtained with standard aerosol instruments (the scanning mobility particle sizer and the fast mobility particle sizer of TSI Inc.). In general, the readings of the electrical diffusion battery and those of standard instruments agree well (to within 10–20%).     

Coagulation of Mainstream Cigarette Smoke in the Mouth During Puffing and Inhalation

The effect of Brownian coagulation on the particle size distribution of mainstream cigarette smoke subjected to conditions encountered in the mouth during human smoking has been examined experimentally and simulated with a numerical coagulation model. Smoke puffed into an artificial mouth was subjected to variable aging times and exhausted to a fast electrical mobility analyzer for particle size distribution measurement. The experimental results agreed well with the predictions of a sectional-based model of Brownian coagulation that allowed for the modeling of various continuous feed and fixed volume coagulation environments. Due to the steady input of fresh, smaller particles, particle growth during the filling of the mouth with smoke, a process intrinsic to the puffing maneuver, was significant but slower than that during fixed volume, static aging. Mouth hold times and initial smoke mass concentration were found to be strong determinants of the average particle size of smoke exiting the mouth into the respiratory tract during inhalation. The results also suggest that the smallest particles present in fresh smoke, those less than 0.1 μm diameter, are greatly reduced in number during the unavoidable mouth coagulation during puffing and virtually eliminated after 1 s of mouth hold.     

Real-Time Chemical Analysis of Organic Aerosols Using a Thermal Desorption Particle Beam Mass Spectrometer

An instrument has been developed for real-time, quantitative chemical analys is of organic particles in laboratory environments. In this apparatus, which we call a Thermal Desorption Particle Beam Mass Spectrometer (TDPBMS), particles are sampled into a differentially-pumped vacuum chamber, focused into a narrow, low-divergence particle beam using aerodynamic lenses, and then transported into a high-vacuum region where they impact on a heated surface, evaporate, and the vapor is mass analyzed in a quadrupole mass spectrometer. The average composition of a continuous stream of particles is thus measured in real time, and size-dependent composition can be obtained by passing the incoming aerosol through a differential mobility analyzer. The TDPBMS can analyze multi component organic particles in the 0.02-0.5mu m size range for compound concentrations 0.1-1mu g m3 without particle matrix effects. By using careful calibration techniques that account for particle shape and transport efficiency, the particulate organic components can be quantified with an estimated uncertainty of 20%. The utility of TDPBMS for laboratory studies of aerosol chemistry is demonstrated by monitoring the tridecanoic acid concentration in secondary organic aerosol formed during a smog chamber reaction of 1-tetradecene and ozone.     

An Intensive Study of the Size and Composition of Submicron Atmospheric Aerosols at a Rural Site in Ontario,Canada

Atmospheric sampling was conducted at a rural site near Egbert, about 70 km north of Toronto, Ontario, Canada from March 27 to May 8, 2003 to characterize the physical and chemical properties of the ambient aerosol in near real-time. The instrumentation included a tapered element oscillating microbalance (TEOM), an ultrafine condensation particle counter (UCPC), a scanning mobility particle sizer (SMPS), an aerodynamic particle sizer (APS), an aerosol mass spectrometer (AMS), and a particulate nitrate monitor (R&P 8400N) for aerosol measurements. Gas-phase non-methane hydrocarbon compounds (NMHCs) were measured by gas chromatograph-flame ionization detection (GC-FID). Filter samples were also collected for analysis of inorganic ions by ion chromatography (IC). Aerosol properties varied considerably depending upon meteorological conditions and airmass histories. For example, urban and industrial emissions advected from the south strongly influenced the site occasionally, resulting in higher particulate mass with the higher fractions of nitrate and organics. Cleaner northwesterly winds carried aerosols with relatively higher fractions of organics and sulfate. The AMS derived mass size distributions showed that the inorganic species in the particles with vacuum aerodynamic diameters between about 60 nm and 600 nm had mass modal vacuum aerodynamic diameters around 400–500 nm. The particulate organics often exhibited two modes at about 100 nm and 425 nm, more noticeable during fresh pollution events. The small organic mode was well correlated with gas-phase nonmethane hydrocarbons such as ethylbenzene, toluene, and propene, suggesting that the likely sources of small organic particles were combustion related emissions. The particulate nitrate exhibited a diurnal variation with higher concentrations during dark hours and minima in the afternoon. Particulate sulfate and organics showed evidence of photochemical processing with higher levels of sulfate and oxygenated organics in the afternoon. Reasonable agreement among all of the co-located measurements is found, provided the upper size limit of the AMS is considered.     

Deposition Uniformity and Particle Size Distribution of Ambient Aerosol Collected with a Rotating Drum Impactor

Rotating drum impactors (RDI) are cascade type impactors used for size and time resolved aerosol sampling, mostly followed by spectrometric analysis of the deposited material. They are characterized by one rectangular nozzle per stage and are equipped with an automated stepping mechanism for the impaction wheels. An existing three-stage rotating drum impactor was modified, to obtain new midpoint cutoff diameters at 2.5 μm, 1 μm, and 0.1 μm, respectively. For RDI samples collected under ambient air conditions, information on the size-segregation and the spatial uniformity of the deposited particles are key factors for a reliable spectrometric analysis of the RDI deposits. Two aerodynamic particle sizers (APS) were used for the determination of the RDI size fractionation characteristics, using polydisperse laboratory room air as quasi-stable proxy for urban ambient air. This experimental approach was suitable for the scope of this study, but was subject to numerous boundary conditions that limit a general use. Aerodynamic stage penetration midpoint diameters were estimated to be 2.4 and 1.0 μm for the first two RDI stages. Additionally, the spatial uniformity and geometrical size distribution of the deposited aerosol were investigated using micro-focus synchrotron radiation X-ray fluorescence spectrometry (micro-SR-XRF) and transmission electron microscopy (TEM), respectively. The size distribution of the particles found on the TEM samples agreed well with the results from the APS experiments. The RDI deposits showed sufficient uniformity for subsequent spectrometric analysis, but in the 2.5–10 μm size range the particle area density was very low. All of the applied methods confirmed the theoretical cutoff values of the modified RDI and showed that compared to other cascade impactors, the determined stage penetration sharpness was rather broad for the individual impactor stages.     

Laser microprobe mass analysis of fog droplet residues

In order to investigate air particulate matter incorporated in the aqueous phase the residues resulting from evaporated fog droplets are compared to single particles of the interstitial aerosol. A counterflow virtual impactor (CVI) is used to separate the fog droplets from both the gaseous and the particulate aerosol components. The fog droplets sampled evaporate and the residues are collected on thin organic films by means of a cascade impactor. Simultaneously a second impactor device (size range about 0.1 to 10 μm) of the same type is exposed to collect the particles of the interstitial aerosol. A special impactor head rejects the larger fog droplets. Mainly the laser microprobe mass analysis (LAMMA -500, Leybold AG) is used to get informations about the chemical composition of both the fog droplet residues and the interstitial particles. Preliminary results indicate that the two particle types show significant differences in their chemical composition. E.g. sulfate and nitrate containing carbonaceous particles preferably appear in the fraction of the interstitial aerosol. In contrast the residues dominantly consist of sulfate species only. Due to the in-fog scavenging of gases the formation of hydroxy methane sulfonate is observed.     

Characterization of Mainstream Cigarette Smoke Particle Size Distributions from Commercial Cigarettes Using a DMS500 Fast Particulate Spectrometer and Smoking Cycle Simulator

Particle size distribution and number concentration measurements of mainstream cigarette smoke are reported for commercial cigarettes encompassing a broad range of design parameters. Measurements were made using a Cambustion DMS500 fast particulate spectrometer. Twenty-nine brand styles were evaluated using a 60-mL puff of 2-s duration taken once every 30 s. A subset of cigarettes was evaluated using additional smoking regimens to explore the influence of puff volume and filter ventilation blocking. The DMS500-derived particulate matter mass was compared with filter-collected mass to assess the reliability of the aerosol measurements. Under the 60-mL/2-s puffing condition, all puffs for all products were observed to exhibit count median diameters between 145 nm and 189 nm. Measured particle size was 12–22 nm smaller for a 60-mL puff relative to a 35-mL puff. Partial or complete filter ventilation blocking under the 60-mL/2-s puffing condition had a small effect on particle size. Some trends in particle size as a function of puff number and smoking regimen appear consistent with a tobacco-rod residence time/coagulation hypothesis; however, other observations suggest that smoke formation processes in addition to coagulation influence particle size. The DMS500 underestimates smoke particulate mass relative to gravimetric filter collection, indicating evaporation of cigarette smoke particulate matter within the instrument. Approximately 75% of the evaporated mass can be attributed to particulate phase water. Some data also suggest a possible underestimation of number concentration. This introduces a significant confounding bias in the measurements and limits the information on smoke formation that can be extracted.     

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     

Comparison and Combination of Aerosol Size Distributions Measured with a Low Pressure Impactor,Differential Mobility Particle Sizer,Electrical Aerosol Analyzer,and Aerodynamic Particle Sizer

Data from a different mobility particle sizer (DMPS) or an electrical aerosol analyzer (EAA) has been combined with data from an aerodynamic particle sizer (APS) and converted to obtain aerosol mass distribution parameters on a near real-time basis. A low pressure impactor (LPI), a direct and independent measure of this mass distribution, provided information for comparison.

The number distribution of particles within the electrical measurement range was obtained with the DMPS and EAA. Data from the APS for particles greater than that size were used to complete the number distribution. Two methods of obtaining mass distribution parameters from this number data were attempted. The first was to convert the number data, channel by channel, to mass data and then fit a log-normal function to this new mass distribution. The second method was to fit a log-normal function to the combined number distribution and then use the Hatch-Choate equations to obtain mass parameters.

Both the DMPS / APS and the EAA / APS systems were shown to successfully measure aerosol mass distribution as a function of aerodynamic diameter. Careful operation of the measurement equipment and proper data manipulation are necessary to achieve reliable results. A channel-by-channel conversion from number to mass distribution provided the best comparison to the LPI measurement. The DMPS / APS combination furnishes higher-size resolution and accuracy than the EAA / APS system. A small gap was observed in the EAA / APS combined data; however, this did not seem to adversely affect the determination of mass distribution parameters.     

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.     

A novel quartz crystal cascade impactor for real-time aerosol mass distribution measurement

A quartz crystal microbalance (QCM) based instrument has been developed for real-time aerosol mass distribution measurement. It includes two key components: a six-stage QCM micro-orifice cascade impactor and a novel relative humidity (RH) conditioner. This instrument operates at a flow rate of 10 L·min^?1 and measures the mass of the collected particles in six aerodynamic diameter channels between 45 nm and 2.5 μm. The RH conditioner ensures that the aerosol particles are collected at an RH between 40% and 65%, which is critical for eliminating particle bounce and for ensuring optimal particle coupling with the QCM. The nozzles of the impactors are clustered in the center of the nozzle plates. Therefore, particles are deposited on the central electrode of the QCM, where the mass calculated from first principles (i.e., Sauerbrey equation) agrees with the actual collected mass. The QCM response is linear up to around 130 μg for solid particles and up to around 2 μg for liquid particles. The collection efficiency curves of the QCM impactor stages were measured experimentally with monodisperse aerosols, and the results agree with the predictions of established impactor theory. This QCM-based instrument has also been tested with ambient aerosols with varying temperature and relative humidity. The aerosol distributions measured by this new instrument are in good agreement with simultaneous independent measurements carried out with a wide-range particle spectrometer (MSP Model 1000XP WPS).

Copyright © 2016 American Association for Aerosol Research     

Direct Transfer of Gas-Borne Nanoparticles into Liquid Suspensions by Means of a Wet Electrostatic Precipitator

The direct transfer of flame-synthesized aerosols of silica nanoparticles into aqueous suspensions is investigated. Silica nanoparticle aerosols with production rates of 0.5 g/h and different mean diameters and degrees of agglomeration are transferred into liquid suspensions by means of a novel wet electrostatic precipitator. Particle collection efficiencies above 99.999% were measured. The influence of the transfer on the particle size distribution was investigated by comparison of aerosol and suspensions size measurements. Aerosol sizes were measured with the scanning mobility particle sizer (SMPS), and suspension size measurements were conducted by dynamic light scattering (DLS) and by SMPS measurements of the aerosolized suspension employing a novel nebulizer. Depending on the aerosol and stabilization conditions, particle transfer with nearly no influence on the particle size distribution is possible. Suspensions generated from the same particle aerosol by direct transfer and by sonication of the respective powder were compared. In contrast to the direct transfer, the aerosol particle size distribution could not be restored by ultrasonication.

Copyright © 2015 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     

Evaluation of thermal denuder and catalytic stripper methods for solid particle measurements

The objective of this study was to compare two methods that are used to separate the solid and volatile components of an aerosol: the thermal denuder (TD) and catalytic stripper (CS). We challenged the TD and CS with atmospheric and laboratory generated aerosols. Laboratory generated particles were composed of tetracosane, tetracosane and sulfuric acid, and dioctyl sebacate and sulfuric acid. These compositions were chosen because they roughly simulate the composition of nanoparticles found in Diesel exhaust. The TD method produced semi-volatile particle artifacts due to the incomplete removal of evaporated compounds that nucleated and formed particles and solid particle artifacts that formed during treatment of the aerosol by the TD. Our results suggest that the differences in these methods will lead to different conclusions regarding the presence or absence, size, and concentration of solid particles in Diesel exhaust.     

Narrow size distribution nanoparticle production by electrospray processing of ferritin

Electrospraying and in-flight heating of ferritin, the iron-storage protein, was used to produce controlled size, monodisperse aerosol particles which can be used as size standards for instrument calibration. As aerosol particles can be collected in liquids or on a substrate, standard size aerosol nanoparticles can be used for the calibration and development of not only aerosol instrumentation, but also colloid instrumentation and electron microscopes. Differences in the sizes of apoferritin and ferritin were detectable using scanning mobility particle spectrometry. Apoferritin has a mobility diameter of 11.8 nm, while iron-rich ferritin had a mobility diameter of 13.1 nm and the size distribution function of both apoferritin and ferritin had geometric standard deviations of 1.05. In-flight heating in a furnace aerosol reactor was used to remove the ferritin protein coat and produce monodisperse iron oxide particles 7.9 nm in diameter and a size distribution function geometric standard deviation of 1.07. Ferritin dimers and higher order n-mers, produced from multiple ferritin complexes being present in a single electrospray droplet, remained bound to each other after in-flight heating. Monte Carlo simulations of the electrospray process showed that as long as the electrospray droplets are sufficiently monodisperse, monodisperse standard size nanoparticles can also be produced from ferritin n-mers.     

Rapid Check of Cascade Impactor Cut-Sizes using a Polydisperse Challenge Aerosol Calibration Method

A method has been developed to check the 50% cut-size values of cascade impactor stages. The method involves generating a broad-size, log-normally distributed aerosol that covers the range of 50% cut-sizes for the impactor being tested. The amount of deposit on each impaction plate is analyzed and a histogram of the resulting aerosol size distribution plotted, using the amount of aerosol collected on each impaction plate and the published values for the cut-sizes of the impactor in question. If the particle size distribution indicated by the histogram does not result in a log-normal distribution, one or more of the assumed cut-sizes of the impactor are in error. The incorrect cut-sizes of the impactor can then be adjusted until the curve is log-normal, and these adjusted cut-sizes are the correct values for the impactor stages.     

Electrical Agglomeration of Aerosol Particles in an Alternating Electric Field

A laboratory scale test system has been designed and constructed to study the electrical agglomeration of charged aerosol particles as a method to increase the fine particle collection efficiency of electrostatic precipitators. The system consists of test aerosol generator, aerosol charger, agglomerator chambers, and aerosol measurement equipment. Air atomizing nozzles and the TSI six-jet atomizer have been used as the test particle generators. The test particles have been charged by a corona discharge. Two types of agglomerator chambers have been investigated. In one agglomerator the gas flows between two parallel plates, across which the alternating high voltage is applied. The other agglomerator is a quadrupole structure with cylindrical electrodes positioned between the grounded plates. Particle concentration and size distribution measurements have been carried out downstream of the agglomerator with agglomerator voltage on and off. Particle concentrations and size distributions have been measured with differential mobility analyzer (DMA) and a Berner low pressure impactor. These measurements show that agglomeration causes about a 4%-8% decrease in the fine particle concentration when the total mass concentration is between 1 and 2 g/m³. There was no difference between the results measured with the parallel plate and the quadrupole agglomerator.     

Evaluation of a High Volume Aerosol Concentrator

A virtual impactor sampler, which is designed to concentrate aerosols from a 1000 L/min ambient air sample into a 1 L/min exhaust airflow stream, was tested with near monodisperse aerosols in aerosol wind tunnels to characterize sampling performance. New methodology is introduced to correct results for the presence of doublet and satellite aerosol particles that can be present in the particle size distribution from a vibrating jet atomizer. Aerosol penetration from the free stream near the sampler inlet to the outlet of the device has a peak value of 78% at a particle size of 3.9 w m AD. Sampling effectiveness, which is the mean penetration over the size range of 2.5 to 10 w m AD, is 48%. There are 4 virtual impaction stages in the sampler, and examination of the regional losses shows that most of the aerosol deposition occurs on surfaces of the last 2 stages. The ideal power expenditure of the sampler (excluding electrical and frictional losses in the motor and bearing losses in the blower) is 58 watts as compared to the actual power consumption of 320 watts.