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1.
Flame-generated soot from miniCAST burners is increasingly being used in academia and industry as engine exhaust soot surrogate for atmospheric studies and instrument calibration. Previous studies have found that elemental carbon (EC) content of miniCAST soot is proportional to the mean particle size. Here, the characterization of a prototype miniCAST generator (5201 Type BC), which was designed to decouple the soot composition from the particle size and produce soot particles with high EC and BC content in a large size range, is reported. This prototype may operate either in a diffusion-flame or a partially premixed-flame mode, an option that was not available in former models. It was confirmed that soot properties, such as EC content and Ångström absorption exponent (AAE), were linked to the overall flame composition. In particular, combustion under fuel-rich conditions provided particles with size coupled to the EC fraction and AAE, i.e. smaller particles exhibited a lower EC fraction and higher AAE. In contrast, with fuel-lean diffusion flames and especially with premixed flames under near overall stoichiometric conditions small particles (down to 30?nm) with high EC/TC ratios (>60%) and low AAE (≈1.4) could be generated even without any thermal after-treatment. This new source might thus serve in the future as a useful surrogate for engine exhaust emissions and help to improve calibration procedures of common aerosol instruments.

Copyright © 2018 The Author(s). Published with license by Taylor & Francis Group, LLC  相似文献   


2.
Steam collection devices collecting aerosol particles into liquid samples are frequently used to analyze water-soluble particulate material. The fate of water-insoluble components is often neglected. In this work, we show that fresh soot particles can be suspended into pure water using a steam collection device, the particle-into-liquid sampler (PILS, Weber et?al. 2001). The overall collection efficiency of freshly generated soot particles was found to be on the order of 20%. This shows that, depending on the analytic technique employed, the presence of insoluble, and/or hydrophobic particles in liquid samples from steam collection cannot be neglected.

Copyright © 2018 The Author(s). Published with license by Taylor & Francis Group, LLC  相似文献   


3.
In this study, we describe a newly developed three-wavelength differential photoacoustic spectrometer, which we denote RGB-DPAS, for aerosol absorption measurement in the visible spectral range: 671?nm (red), 532?nm (green), and 473?nm (blue). This instrument utilizes the differential photoacoustic spectrometric (DPAS) technique, which simultaneously measures light absorption signals due to total particulate matter?+?gaseous samples and those of gaseous samples alone. The difference between the photoacoustic signals recorded from the two nearly identical acoustic cells (<0.2% variability in physical dimensions) yields the aerosol photoacoustic signals at the three wavelengths. This measurement approach eliminates the interferences from light-absorbing gaseous species as well as low-frequency ambient acoustic noise. In this study, we demonstrate the linearity of the RGB-DPAS signal response to the number concentration of the synthetic carbon black particles at electrical mobility diameter (Dm) = 350?nm, which is used as a calibration surrogate. Based on the Allan variance analysis, detection limits (2σ) of 0.20?Mm?1 at 671?nm, 0.22?Mm?1 at 532?nm, and 0.90?Mm?1 at 473?nm have been achieved in 100?s data acquisition for the RGB-DPAS instrument.

Copyright © 2018 American Association for Aerosol Research  相似文献   


4.
Soot is a climate forcer and a dangerous air pollutant that has been increasingly regulated. In aviation, regulatory measurements of soot mass concentration in the exhaust of aircraft turbine engines are to be based on measurements of black carbon (BC) calibrated to elemental carbon (EC) content of diffusion flame soot. The calibration soot must currently meet only one criterion: minimum EC to total carbon (TC) ratio of 0.8. However, not including soot properties other than the EC/TC ratio may potentially lead to discrepancies between different BC measurements. We studied the response of two instruments, the AVL Micro-Soot Sensor (MSS) and the Artium Laser-Induced Incandescence 300 (LII), to soot from two miniature combustion aerosol standard (mini-CAST) burners. By changing the air-fuel ratio, premixing nitrogen into the fuel, and using a catalytic stripper to remove volatile compounds, we produced a wide range of particle morphologies and EC contents. As the EC content decreased, both the instruments underreported the EC mass, but the LII diverged more severely. Upon closer investigation of eight conditions with EC/TC > 0.8, the LII underreporting was found independent of primary particle size, but increased with decreasing geometric mean diameter of the soot agglomerates. As the geometric mean diameter decreased from 160 nm to 50 nm, the differences between the LII and MSS increased from 15% to 50%. The results suggest that in addition to EC content, calibration procedures for the regulatory BC measurements may need to take particle size distributions into account.

© 2016 American Association for Aerosol Research  相似文献   


5.
Due to the exponential increase in aircraft traffic in recent decades, the role of soot particles emitted by aircraft engines on the radiative forcing needs to be addressed, and especially their interaction with clouds has to be better understood and quantified. In this work, we investigate the hygroscopic properties of fresh and aged soot sampled on line in a kerosene flame. The activated fraction (Fa) of size selected soot is measured by means of a variable supersaturation condensation nucleus counter at several heights above the burner (HAB), thereby probing soot particles with different residence times in the flame, i.e., different degrees of maturity. In order to simulate atmospheric aging, the activity of soot as cloud condensation nuclei is measured as a function of ozone exposure. We show that fresh soot is hydrophobic (Fa~0), while Fa increases when soot is exposed to ozone. The measurements depend on the HAB at which soot particles are sampled showing that activation of soot particles is related to their chemical composition. This study brings new results on the link between atmospheric aging of soot and its hygroscopic properties, which is of great interest for understanding the role of soot in the cloud formation.

Copyright © 2018 American Association for Aerosol Research  相似文献   


6.
A new primary standard method for calibrating optical particle counters (OPC) has been developed based on quantitative gravitational deposition on a silicon wafer and accurate counting of the particles by a wafer surface scanner (WSS). The test aerosol consists of 3-μm diameter monodisperse polystyrene latex (PSL) spheres at concentrations in the range of 0.1 cm?3 to 1 cm?3. A key element to the calibration is the ability to generate monodisperse PSL spheres without residue particles by use of a virtual impactor and differential mobility analyzer. The use of these devices reduced the percentage of residue particles from more than 99.98% to about 5%. The expanded relative uncertainty (95% confidence level) in the number concentration determined with a WSS for a deposition of 200 particles is 17.8%. The major uncertainty component arises from the Poisson fluctuations in the aerosol concentration because of the low concentration. This methodology has advantages of a fast scanning time by the WSS of minutes compared to hours or days by microscopy and of counting every particle deposited compared to often only a small fraction via microscopy.

The WSS was used in the calibration of an OPC based on 12 depositions with concentrations ranging from 0.1 cm?3 to 1 cm?3 for each deposition. Make-up air was added to the aerosol entering the OPC so that the lowest achievable concentration for the OPC measurement is about 0.01 cm?3 in this study. The detection efficiency of the OPC was measured to be 0.984 with an expanded uncertainty of 13.4%.

Copyright 2014 American Association for Aerosol Research  相似文献   


7.
Nascent soot particles with mobility diameters ≤10 nm were measured in an ethylene/air premixed flame to shed light on the challenges and potential artifacts affecting studies on soot inception by differential mobility analysis (DMA) techniques. The size distribution functions (SDFs) of particles with charge acquired either naturally or diffusively upon ion seeding were measured at several positions in the flame using rapid-dilution probing and a high-resolution DMA for different values of the ratio of dilution ratio to residence time (DR/Δt). The SDFs are roughly bimodal with a sub-3 nm mode and a larger one that appears either downstream in the flame or for low DR/Δts. Soot nuclei smaller than 3 nm preferentially acquire positive charge, which brings into question the assumption of steady-state charging probability of flame sampled soot nuclei in the bipolar diffusion neutralizer. The approximately polarity-symmetric lognormal SDF of larger particles is attributed to nuclei coagulation. Naturally charged particles increase in number when lowering DR/Δt, suggesting either their collisional charging by flame chemi-ions or particle nucleation by condensation of neutral molecules on ions or both. The critical conditions for suppressing particle coagulation and charge redistribution in the sampling system were not achieved under most conditions, despite the fact that values of DR/Δts were more favorable to such a suppression in the present experiment as compared to other studies in the literature. As a result, the identification of this “asymptotic” regime, which is critical to determine the parent SDFs and the charge state of nascent soot in the flame, is still elusive.

© 2016 American Association for Aerosol Research  相似文献   


8.
A new polar nephelometer (PN) has been developed to measure simultaneously the scattering angular distributions from 11.7° to 168.3° for individual particles in planes parallel and perpendicular to the polarization of the incident laser beam. Each detection plane had 21 silicon photodiode detectors to detect scattered light at a rate of 100 Hz. Laboratory experiments to validate the performance of the instrument were conducted using nearly mono-disperse spherical particles (polystyrene latex [PSL] and nigrosine) and nonspherical particles (sodium chloride [NaCl] and soot). The observed scattering angular distributions for individual PSL particles were in good agreement with the results of simulations based on Mie theory. Complex refractive index values for nigrosine particles were determined by comparing the observed scattering angular distributions with the results of simulations. Clear differences between the measured scattering angular distributions and the results of simulations based on Mie theory assuming spherical particles were observed for NaCl particles (mobility diameters of 500 and 700 nm) and propane soot particles (mobility diameters of 300, 500, and 700 nm). These results are reasonably explained by theoretical predictions. We also conducted initial observations of ambient particles in Nagoya city, Japan. Scattering angular distributions for particles with a mobility diameter of 500 nm and an average effective density of 1.4 or 0.3 g/cm3, which were selected with a combination of differential mobility analyzer and aerosol mass particle analyzer, were measured using the PN. As results, scattering angular distributions for nearly spherical inorganic and organic particles with an average effective density of around 1.4 g/cm3 were found to be distinguishable from nonspherical particles with an average effective density of around 0.3 g/cm3. This study has demonstrated that our PN has the potential to distinguish between spherical and nonspherical particles.

Copyright © 2016 American Association for Aerosol Research  相似文献   


9.
Mixing state refers to the relative proportions of chemical species in an aerosol, and the way these species are combined; either as a population where each particle consists of a single species (‘externally mixed’) or where all particles individually consist of two or more species (‘internally mixed’) or the case where some particles are pure and some particles consist of multiple species. The mixing state affects optical and hygroscopic properties, and quantifying it is therefore important for studying an aerosol's climate impact. In this article, we describe a method to quantify the volatile mixing state of an aerosol using a differential mobility analyzer, centrifugal particle mass analyzer, catalytic denuder, and condensation particle counter by measuring the mass distributions of the volatile and non-volatile components of an aerosol and determining how the material is mixed within and between particles as a function of mobility diameter. The method is demonstrated using two aerosol samples from a miniCAST soot generator, one with a high elemental carbon (EC) content, and one with a high organic carbon (OC) content. The measurements are presented in terms of the mass distribution of the volatile and non-volatile material, as well as measures of diversity and mixing state parameter. It was found that the high-EC soot nearly consisted of only pure particles where 86% of the total mass was non-volatile. The high-OC soot consisted of either pure volatile particles or particles that contained a mixture of volatile and non-volatile material where 8% of the total mass was pure volatile particles and 70% was non-volatile material (with the remaining 22% being volatile material condensed on non-volatile particles).

© 2016 American Association for Aerosol Research  相似文献   


10.
During occupational exposure studies, the use of conventional scanning mobility particle sizers (SMPS) provides high quality data but may convey transport and application limitations. New instruments aiming to overcome these limitations are being currently developed. The purpose of the present study was to compare the performance of the novel portable NanoScan SMPS TSI 3910 with that of two stationary SMPS instruments and one ultrafine condensation particle counter (UCPC) in a controlled atmosphere and for different particle types and concentrations.

The results show that NanoScan tends to overestimate particle number concentrations with regard to the UCPC, particularly for agglomerated particles (ZnO, spark generated soot and diesel soot particles) with relative differences >20%. The best agreements between the internal reference values and measured number concentrations were obtained when measuring compact and spherical particles (NaCl and DEHS particles). With regard to particle diameter (modal size), results from NanoScan were comparable < [± 20%] to those measured by SMPSs for most of the aerosols measured.

The findings of this study show that mobility particle sizers using unipolar and bipolar charging may be affected differently by particle size, morphologies, particle composition and concentration. While the sizing accuracy of the NanoScan SMPS was mostly within ±25%, it may miscount total particle number concentration by more than 50% (especially for agglomerated particles), thus making it unsuitable for occupational exposure assessments where high degree of accuracy is required (e.g., in tier 3). However, can be a useful instrument to obtain an estimate of the aerosol size distribution in indoor and workplace air, e.g., in tier 2.  相似文献   


11.
Laser-induced incandescence (LII) measurements were conducted to explore the ability of LII to detect small soot particles of less than 10 nm in two sooting flat premixed flames of n-butane: a so-called nucleation flame obtained at a threshold equivalence ratio Φ = 1.75, in which the incipient soot particles undergo only minor soot surface growth along the flame, and a more sooting flame at Φ = 1.95. Size measurements were obtained by modeling the time-resolved LII signals detected using 1064 nm laser excitation. Spectrally-resolved LII signals collected in the nucleation flame display a similar blackbody-like behavior as mature soot. Soot particle temperature was determined from spectrally-resolved detection. LII modeling was conducted using parameters either relevant to those of mature soot or derived from fitting the modeled results to the experimental LII data. Particle size measurements were also carried out using (1) ex situ analysis by helium-ion microscopy (HIM) of particles sampled thermophoretically and (2) online size distribution analysis of microprobe-sampled particles using a 1 nm-SMPS. The size distributions of the incipient soot particles, found in the nucleation flame and in the early soot region of the Φ = 1.95 flame, derived from time-resolved LII signals are in good agreement with HIM and 1 nm-SMPS measurements and are in the range of 2–4 nm. The thermal and optical properties of incipient soot were found to be not radically different from those of mature soot commonly used in LII modeling. This explains the ability of incipient soot particles to produce continuous thermal emissions in the visible spectrum. This study demonstrates that LII is a promising in situ optical particle sizing technique that is capable of detecting incipient soot as small as about 2.5 nm and potentially 2 nm and resolving small changes in soot sizes below 10 nm.

© 2017 American Association for Aerosol Research  相似文献   


12.
Indoor air microbial pollution may be responsible for various human allergies and diseases. To reduce exposure, airborne bacteria can be directly controlled through devices that employ ultraviolet-C (UV-C) radiation. In this study, a continuous annular photo-reactor was used to evaluate the inactivation dose for two species: Gram-negative Escherichia coli and Pseudomonas aeruginosa. In order to provide meaningful results, a comprehensive kinetic modeling was performed, which included the evaluation of optical properties of the microorganisms and the calculation of radiation field inside the reactor. In this way, intrinsic inactivation rates could be obtained. From the reactor modeling and the experimental data sets, the first order inactivation rate or UV susceptibility for E. coli was 0.1055?m2 J?1, while for P. aeruginosa the obtained value was 0.2579?m2 J?1. The approach used allows a straightforward scaling-up of the process for real applications and microorganism species involved.

Copyright © 2018 American Association for Aerosol Research  相似文献   


13.
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  相似文献   


14.
A combination of high-repetition rate imaging, laser extinction measurements, two-color soot pyrometry imaging, and high-resolution transmission electron microscopy of thermophoretically sampled soot is used to investigate the long-term and permanent effects of rapid heating of in-flame soot during laser-induced incandescence (LII). Experiments are carried out on a laminar non-premixed co-annular ethylene/air flame with various laser fluences. The high-repetition rate images clearly show that the heated and the neighboring laser-border zones undergo a permanent transformation after the laser pulse, and advect vertically with the flow while the permanent marking is preserved. The soot volume fraction at the heated zone reduces due to the sublimation of soot and the subsequent enhanced oxidation. At the laser-border zones, however, optical thickness increases that may be due to thermophoretic forces drawing hot particles towards relatively cooler zones and the rapid compression of the bath gas induced by the pressure waves created by the expansion of the desorbed carbon clusters. Additionally sublimed carbon clusters can condense onto existing particles and contribute to increase of the optical thickness. Time-resolved two-color pyrometry imaging show that the increased temperature of soot both in the heated and neighboring laser-border zones persists for several milliseconds. This can be associated to the increase in the bath-gas temperature, and a change in the wavelength-dependent emissivity of soot particles induced by the thermal annealing of soot. Ex-situ analysis show that the lattice structure of the soot sampled at the laser-border zones tend to change and soot becomes more graphitic. This may be attributed to thermal annealing induced by elevated temperature.

Copyright © 2017 American Association for Aerosol Research  相似文献   


15.
We performed controlled combustion experiments to investigate the dependence of the mass absorption cross-section (MAC) and absorption Ångström exponent (AAE) of combustion carbonaceous aerosol emissions on combustion conditions. Using benzene and toluene as fuels, we obtained a wide range of combustion conditions by varying the combustion temperature and equivalence ratio. We also used nitrogen as a passive diluent to tune the combustion conditions. We calculated MAC and AAE from multi-wavelength light-absorption measurements using a photoacoustic spectrophotometer and aerosol mass loadings estimated from thermal-optical analysis. Starting with relatively low-temperature and fuel-rich combustion conditions and progressively increasing the temperature and/or decreasing the equivalence ratio, we produced emissions with progressive change from weakly absorbing brown carbon (BrC) (MAC at 532?nm (MAC532) = 0.24?m2/g and AAE = 8.6) to strongly absorbing BrC (MAC532 = 2.1?m2/g and AAE = 3.1) to mixtures of black carbon (BC) and strongly absorbing BrC (MAC532 = 7.7?m2/g and AAE = 1.5). These findings indicate that combustion conditions are important in dictating the light-absorption properties of the emitted aerosols. Furthermore, regardless of fuel type and combustion conditions, the emitted aerosols exhibit a unified continuum of light-absorption properties that can be characterized by MAC532 and AAE pairs. The MAC532 and AAE pairs are well-correlated with the elemental carbon-to-organic carbon ratio (EC/OC), which is a proxy of combustion conditions, confirming previous findings that EC/OC is a practical basis for parameterizing the light-absorption properties of combustion carbonaceous aerosols.

Copyright © 2019 American Association for Aerosol Research  相似文献   


16.
With the microdroplets of water serving as light scattering particles, the mist flow patterns of round micro-jets can be visualized using the Aerosol Jet® direct-write system. The visualization images show that the laminar mist jet (with sheath-to-mist ratio Y?=?1:1) appears to extend to more than 20 times the diameter of nozzle orifice D for jet Reynolds number Re?<?600, especially with D?=?0.3?mm and less. For smaller jets (e.g., with D?=?0.15?mm), laminar collimated mist flow might be retained to 40×D for Re?<?600 and for Re ~1500 within 20×D from the nozzle. The laminar part of mist flow associated with larger jets (e.g., with D?=?1.0?mm for Re?<?600) tends to exhibit noticeable gradual widening due to viscous diffusion. For free jets, their breakdown length—the distance from nozzle where transition from laminar to turbulent mist flow takes place as signaled by a rapid widening of mist stream—is shown to decrease with increasing Re. The presence of impingement wall tends to prevent turbulence development, even when the wall is placed further downstream of the free-jet breakdown length for a given Re. The critical Re for an impinging jet to develop turbulence increases as the standoff S is reduced. The mist flow of impinging jet of D?=?1.0?mm seems to remain laminar even for Re?>?4000 at S?=?12?mm.

Copyright © 2018 American Association for Aerosol Research  相似文献   


17.
Inhalation of aerosols containing pathogenic viruses can result in morbidity, in some cases leading to mortality. The objective of this study was to develop a model for assessing how infectious viruses might distribute in airborne particles using bacteriophage MS2 as a surrogate for human viruses. Particle deposition in the respiratory system is size-dependent, and small virus-containing particles can be inhaled deeply into the lower lungs, potentially leading to more severe respiratory disease manifestations. Laboratory-generated virus-containing particles were size-selected by a differential mobility analyzer and then collected by the newly introduced Super-Efficient Sampler for Influenza Virus. The number of infectious and total viruses per particle as a function of particle size varied with the spraying medium: it approximated a cubic exponential value scaling for deionized (DI) water, a quartic exponential value for artificial saliva (AS), and between quadratic and cubic exponential value for beef extract solution (BES). The survivability of MS2 did not change significantly with particle size for DI water and BES, while that for AS was maximum at 120?nm. Viruses could be homogeneously distributed or aggregated inside or on the surface of the particles, depending on the composition of the spraying medium.

Copyright © 2019 American Association for Aerosol Research  相似文献   


18.
We study the effects of electric field strength on the mobility of soot-like fractal aggregates (fractal dimension of 1.78). The probability distribution for the particle orientation is governed by the ratio of the interaction energy between the electric field and the induced dipole in the particle to the energy associated with Brownian forces in the surrounding medium. We use our extended Kirkwood–Riseman method to calculate the friction tensor for aggregates of up to 2000 spheres, with primary sphere sizes in the transition and near-free molecule regimes. Our results for electrical mobility versus field strength are in good agreement with published experimental data for soot, which show an increase in mobility on the order of 8% from random to aligned orientations. Our calculations show that particles become aligned at decreasing field strength as particle size increases because particle polarizability increases with volume. Large aggregates are at least partially aligned at field strengths below 1000 V/cm, though a small change in mobility means that alignment is not an issue in many practical applications. However, improved differential mobility analyzers would be required to take advantage of small changes in mobility to provide shape characterization.

Copyright © 2018 American Association for Aerosol Research  相似文献   


19.
Combustion produced soot is highly variable in its composition and nanostructure, both of which are dependent upon combustion conditions. Quantification of high-resolution transmission electron microscopy (HRTEM) images for nanostructure parameters shows that soot nanostructure is dependent upon its source. In principle, this permits identification of the soot and its contribution to any pollution monitoring receptor site. Many structural and chemical aspects are subtle, unaccounted for in direct nanostructure quantification. The process of pulsed laser annealing is demonstrated to enhance slight differences in nanostructure and chemical composition. Chemistry-based limitations imposed due to nanosecond heating and microsecond cooling timescales highlight these initial compositional and structural differences—as dependent upon source-specific formation conditions. This study demonstrates laser-based heating as an analytical tool for soot differentiation by formation conditions/source by identifying operational parameters for optimal derivatization. Nanostructure changes are qualitatively shown using HRTEM and quantified using image-based fringe analysis for real and model soots.

Copyright © 2019 American Association for Aerosol Research  相似文献   


20.
The effect of potassium on the oxidation of a model carbonaceous material (Printex U, namely, soot for brevity) has been investigated under isothermal conditions. For this purpose, Raman spectroscopy, Transmission Electron Microscopy (TEM), and Brunaure, Emmet, Teller surface area characterization have been applied to investigate structural changes occurring during soot oxidation both in the presence and in the absence of potassium. The Raman spectra of the model soot during combustion showed that oxidation preferentially involves the amorphous carbon fraction of the soot and only subsequently it affects the more ordered sp2 domains. However, in the K-doped Printex U the oxidation of both the amorphous and more ordered sp2 structures occurs concurrently. These findings have been confirmed by TEM analysis and explain the observed higher combustion activity of K-containing sample.

Copyright © 2016 American Association for Aerosol Research  相似文献   


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