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1.
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   


2.
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  相似文献   


3.
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   


4.
The climate-change and environmental literature, including that on aerosols, is replete with mention of black carbon (BC) and soot. The terms are used interchangeably in much of the literature, although BC and soot commonly have operational and source-based definitions, respectively, and reliable reference samples and aerosol standards do not exist for either one. The uncertainty about their exact chemical nature and properties can be decreased by materials-based measurement techniques and terminology. Here, we discuss ambiguities in common uses of BC and soot and propose the term ns-soot, where “ns” refers to carbon nanospheres, for a characteristic constituent of BC and soot. Based on its composition, morphology, and structure, we define ns-soot as particles that consist of nanospheres, typically with diameters <100 nm, that possess distinct structures of concentrically wrapped, graphene-like layers of carbon and with grape-like (aciniform) morphologies. We additionally propose that, because of their importance for climate modeling and health issues, distinctions are made among bare, coated, and embedded ns-soot particles.

Copyright 2014 American Association for Aerosol Research  相似文献   


5.
Aerosol instruments provide more informative engine exhaust particulate matter (PM) data than the gravimetric filter and solid particle number methods prescribed by regulations. Yet their lack of conformity to the regulatory methods can limit their acceptance for vehicle development. This article examines the ability of the Dekati Mass Monitor (DMM), Engine Exhaust Particle Sizer (EEPS), and Micro Soot Sensor (MSS) to measure PM2.5 mass and solid particle number relative to current motor vehicle PM emissions standards. Simultaneous PM measurements are made by these three instruments and the two regulatory methods for 50 tests of six gasoline direct injection and two port fuel injection vehicles over the U.S. Federal Test Procedure. DMM and EEPS determinations of PM mass correlate well to gravimetric values (regression slopes of 1.06 ± 0.04 and 0.98 ± 0.08) down to a few mg/mile, below which filter weighing variability becomes problematic. The MSS exhibits a lower slope of 0.79 ± 0.03 consistent with it measuring the soot fraction, rather than total PM. At emissions rates above ~1013 particles/mile, solid particle number determined from DMM and EEPS data correlates respectably with, but overestimates the regulatory method (regression slopes are 1.7 ± 0.1 and 1.4 ± 0.15, respectively). Below this emissions rate, the correlation degrades. EEPS estimates of PM mass are significantly improved with the recent soot optimized inversion algorithm (slope improves from 0.45 to 0.98). While they cannot replace filters and solid particle counting, the present study suggests that these instruments can be used as more informative surrogates during motor vehicle development.

© 2016 Ford Motor Company  相似文献   


6.
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   


7.
8.
The characteristics of fugitive dust emitted from vehicles traveling on unpaved dirt roads were measured using a suite of instruments including a real-time fugitive dust sampler. The fugitive dust sampler is formed from a combination of a large particle inlet and an optical particle spectrometer that reports particle sizes from 6 to 75 µm. The large particle inlet permits the sampling of particles up to 75 µm with only a moderate dependence of sampling efficiency on wind-speed. Measurements made with the sampler showed that particles as large as ~50 µm were suspended from vehicular movement on the dirt roads, with the mode of the fugitive dust particle number size distribution ~2 µm, while the mass distribution mode was ~7 µm. A comparison of the fugitive dust sampler measurements with those made using standard PM instruments showed that the conventional instruments have a wind-direction bias that can result in under-sampling of large particles. The current measurements suggest that particles suspended from dirt roadways are of importance for local air quality within the near-road environment.

Copyright © 2017 American Association for Aerosol Research  相似文献   


9.
Lab-scale soot nanoparticle generators are used by the aerosol research community to study the properties of soot over a broad range of particle size distributions, and number and mass concentrations. In this study, a novel miniature inverted-flame burner is presented and its emitted soot particles were characterized. The burner consisted of two co-annular tubes for fuel and co-flow air and the flame was enclosed by the latter. The fuel used was ethylene. A scanning mobility particle sizer (SMPS) and an aerodynamic aerosol classifier (AAC) were used to measure mobility and aerodynamic size distribution of soot particles, respectively. Particle morphology was studied using transmission electron microscopy (TEM). The elemental carbon (EC) and organic carbon (OC) content of the soot were measured using thermal-optical analysis (TOA). The burner produced soot particles with mobility diameter range of 66–270?nm, aerodynamic diameter range of 56–140?nm, and total concentration range of 2?×?105–1?×?107?cm?3. TEM images showed that most soot particles were sub-micron soot aggregates. Some soot superaggregates, typically larger than 2?µm in length, were observed and their abundance increased with ethylene flow rate. TOA showed that the concentration of EC in the generated soot increased with ethylene flow rate, and the soot was observed to have high EC fraction at high ethylene flow rates. The miniature inverted-flame burner was demonstrated to produce soot nanoparticles over a range of concentrations and sizes with high EC content, making it a practical device to study soot nanoparticle properties in different applications.

Copyright © 2019 American Association for Aerosol Research  相似文献   


10.
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   


11.
For decades, soot has been modeled as fractal-like aggregates of nearly equiaxed spherules. Cluster–cluster aggregation simulations, starting from a population of primary particles, give rise to structures that closely match real aerosols of solid particles produced in flames. In such simulations, primary particle size is uncorrelated with aggregate size, as all aggregates contain primary particles drawn from the same population. Aerosol measurements have been interpreted with this geometric model. Examination of transmission electron micrographs of soot samples from various sources shows that primary particle sizes are not well mixed within an aerosol population. Larger aggregates tend to contain larger primary particles and the variation in size is much larger between aggregates than within aggregates. The soot sources considered here are all substantially not well-mixed (aircraft jet engine, inverted diffusion flame, gasoline direct injection engine, heavy-duty compression ignition engine). The observed variations in primary particle size can be explained if soot aggregates are formed and grew by coagulation in small zones of the combustion chamber, prior to dilution and transport (with minimal coagulation) to the sampling system.

Copyright 2014 American Association for Aerosol Research  相似文献   


12.
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   


13.
Cookstoves are a major source of black carbon (BC) particles and associated organic compounds, which influence the atmospheric radiative balance. We present results from experiments that characterize BC emissions from a rocket stove coated with secondary organic aerosol. Optical properties, namely, BC mass absorption cross-section (MACBC) and mass scattering cross-section (MSC), as a function of the organic-to-black carbon ratio (OA:BC) of fresh and aged cookstove emissions were compared with Mie and Rayleigh–Debye–Gans (RDG) calculations. Mie theory reproduced the measured MACBC across the entire OA:BC range. However, Mie theory failed to capture the MSC at low OA:BC, where the data agreed better with RDG, consistent with a fractal morphology of fresh BC aggregates. As the OA:BC increased, the MSC approached Mie predictions indicating that BC-containing particles approach a core–shell structure as BC cores become heavily coated. To gain insight into the implications of our findings, we calculated the spectral simple forcing efficiency (dSFE) using measured and modeled optical properties as inputs. Good agreement between dSFE estimates calculated from measurements and Mie-modeled dSFE across the entire OA:BC range suggests that Mie theory can be used to simulate the optical properties of aged cookstove emissions.

Copyright © 2016 American Association for Aerosol Research  相似文献   


14.
In this work, a mini-CAST soot generator was used to produce soot with different optical and physicochemical characteristics. Absorption Ångström exponents (AAE) expressing the absorption wavelength dependence were assessed by multiwavelength in-situ and filter-based (aethalometer) laser extinction. The two optical techniques showed good agreement. For the chosen mini-CAST operating conditions, AAEs between 1 and 3.5 were found. Soot with high mass-fractions of organic carbon (OC) and pyrolytic carbon (PC) determined with thermal optical analysis were associated with AAEs significantly higher than 1. Heating to 250 and 500°C removed the majority of polycyclic aromatic hydrocarbons. However, the thermal-optical analysis revealed that OC and PC were abundant in the soot with AAE > 2 also after heating the aerosol. Analysis of mass absorption cross section ratios for elemental carbon and OC indicated that elevated AAEs also after heating to 500°C could be related to persistent OC and PC components and/or the refractory soot. By comparing the mini-CAST soot optical properties with soot properties derived from in-situ extinction measurements in a premixed flame, mini-CAST soot with a higher AAE could be identified as less mature soot.

Copyright © 2018 The Authors  相似文献   


15.
The effects of injection pressure on diesel particle physical and chemical properties were investigated on a heavy-duty diesel engine. Three injection pressures (600 bar, 800 bar, and 1000 bar) were selected at two engine loads (0.3 MPa BMEP and 0.9 MPa BMEP). The exhaust particle size distribution was measured by a scanning mobility particle sizer (SMPS). Consistent with previous studies, increasing injection pressure effectively removes accumulation mode particles, which results in a significant decrease in particle total mass concentration. The elemental carbon emission factors were then tested through organic carbon/element carbon (OC/EC) analysis. The emitted EC is decreased by 64% and 50% with increasing injection pressure from 600 bar to 1000 bar at the low and high engine loads, respectively. Particle morphology and oxidation reactivity were investigated by means of transmission electron microscope (TEM) imaging and thermogravimetric analysis (TGA) technology, respectively. Smaller primary particles with shorter and flatter graphene layer segments are observed at higher injection pressure conditions, and the particle oxidation reactivity is increased with injection pressure.

Copyright 2014 American Association for Aerosol Research  相似文献   


16.
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   


17.
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   


18.
Entrained flow gasification is a promising technique where biomass is converted to a synthesis gas (syngas) under fuel-rich conditions. In contrast to combustion, where the fuel is converted to heat, CO2, and H2O, the syngas from gasification is rich in energetic gases such as CO and H2. These compounds (CO and H2) represent the building blocks for further catalytic synthesis to chemicals or biofuels. Impurities in the syngas, such as particulates, need to be reduced to different levels depending on the syngas application. The objective of this work was to evaluate the amount of particulates; the particle size distribution and the particle composition from entrained flow gasification of pine stem wood at different operating conditions of the gasifier. For this purpose, online time resolved measurements were performed with a soot particle aerosol mass spectrometer (SP-AMS) and a scanning mobility particle sizer (SMPS). The main advantage of SP-AMS compared to other techniques is that the particle composition (soot, PAH, organics, and ash forming elements) can be obtained with high time resolution and thus studied as a direct effect of the gasifier-operating conditions. The results suggest that syngas particulates were essentially composed of soot at these tested process temperatures in the reactor (1200–1400°C). Furthermore, the AMS analysis showed a clear correlation between the amounts of polycyclic aromatic hydrocarbons (PAH) and soot in the raw syngas. Minimization of soot and PAH yields from entrained flow gasification of wood proved to be possible by further increasing the O2 addition.

Copyright 2014 American Association for Aerosol Research  相似文献   


19.
The effective density and size-resolved volatility of particles emitted from a Rolls-Royce Gnome helicopter turboshaft engine are measured at two engine speed settings (13,000 and 22,000 RPM). The effective density of denuded and undenuded particles was measured. The denuded effective densities are similar to the effective densities of particles from a gas turbine with a double annular combustor as well as a wide variety of internal combustion engines. The denuded effective density measurements were also used to estimate the size and number of primary particles in the soot aggregates. The primary particle size estimates show that the primary particle size was smaller at lower engine speed (in agreement with transmission electron microscopy analysis). As a demonstration, the size-resolved volatility of particles emitted from the engine is measured with a system consisting of a differential mobility analyzer, centrifugal particle mass analyzer, condensation particle counter, and catalytic stripper. This system determines the number distributions of particles that contain or do not contain non-volatile material, and the mass distributions of non-volatile material, volatile material condensed onto the surface of non-volatile particles, and volatile material forming independent particles (e.g., nucleated volatile material). It was found that the particulate at 13,000 RPM contained a measurable fraction of purely volatile material with diameters below ~25 nm and had a higher mass fraction of volatile material condensed on the surface of the soot (6%–12%) compared to the 22,000 RPM condition (1%–5%). This study demonstrates the potential to quantify the distribution of volatile particulate matter and gives additional information to characterize sampling effects with regulatory measurement procedures.

Copyright © 2017 American Association for Aerosol Research  相似文献   


20.
Accurate exposure assessments are needed to evaluate health hazards caused by airborne microorganisms and require air samplers that efficiently capture representative samples. This highlights the need for samplers with well-defined performance characteristics. While generic aerosol performance measurements are fundamental to evaluate/compare samplers, the added complexity caused by the diversity of microorganisms, especially in combination with cultivation-based analysis methods, may render such measurements inadequate to assess suitability for bioaerosols. Specific performance measurements that take into account the end-to-end sampling process, targeted bioaerosol and analysis method could help guide selection of air samplers.

Nine different samplers (impactors/impingers/cyclones/ electrostatic precipitators/filtration samplers) were subjected to comparative performance testing in this work. Their end-to-end cultivation-based biological sampling efficiencies (BSEs) and PCR-/microscopy-based physical sampling efficiencies (PSEs) relative to a reference sampler (BioSampler) were determined for gram-negative and gram-positive vegetative bacteria, bacterial spores, and viruses.

Significant differences were revealed among the samplers and shown to depend on the bioaerosol's stress–sensitivity and particle size. Samplers employing dry collection had lower BSEs for stress-sensitive bioaerosols than wet collection methods, while nonfilter-based samplers showed reduced PSEs for 1 μm compared to 4 μm bioaerosols. Several samplers were shown to underestimate bioaerosol concentration levels relative to the BioSampler due to having lower sampling efficiencies, although they generally obtained samples that were more concentrated due to having higher concentration factors.

Our work may help increase user awareness about important performance criteria for bioaerosol sampling, which could contribute to methodological harmonization/standardization and result in more reliable exposure assessments for airborne pathogens and other bioaerosols of interest.

Copyright 2014 American Association for Aerosol Research  相似文献   


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