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1.
This work explores the volatility of particles produced from two diesel low temperature combustion (LTC) modes proposed for high-efficiency compression ignition engines. It also explores mechanisms of particulate formation and growth upon dilution in the near-tailpipe environment. The number distribution of exhaust particles from low- and mid-load dual-fuel reactivity controlled compression ignition (RCCI) and single-fuel premixed charge compression ignition (PPCI) modes were experimentally studied over a gradient of dilution temperature. Particle volatility of select particle diameters was investigated using volatility tandem differential mobility analysis (V-TDMA). Evaporation rates for exhaust particles were compared with V-TDMA results for candidate pure n-alkanes to identify species with similar volatility characteristics. The results show that LTC particles are mostly comprised of material with volatility similar to engine oil alkanes. V-TDMA results were used as inputs to an aerosol condensation and evaporation model to support the finding that smaller particles in the distribution are comprised of lower volatility material than large particles under primary dilution conditions. Although our results show that saturation levels are high enough to drive condensation of alkanes onto existing particles under the dilution conditions investigated, they are not high enough to allow homogeneous nucleation of these same compounds in the primary exhaust plume. Therefore, we conclude that observed particles from LTC operation must grow from low concentrations of highly nonvolatile compounds present in the exhaust.

Copyright © 2016 American Association for Aerosol Research  相似文献   


2.
The Aerodyne Aerosol Chemical Speciation Monitor (ACSM) is well suited for measuring non-refractory particulate matter up to approximately 1.0 µm in aerodynamic diameter (NR-sub-PM1). However, for larger particles the detection efficiency is limited by losses in the sampling inlet system and through the standard aerodynamic focusing lens. In addition, larger particles have reduced collection efficiency due to particle bounce at the vaporizer. These factors have limited the NR-sub-PM1 ACSM from meeting PM2.5 (particulate matter with aerodynamic diameter smaller than 2.5 µm) monitoring standards. To overcome these limitations, we have redesigned the sampling inlet, the aerodynamic lens, and particle vaporizer. Both the new lens and vaporizer are tested in the lab using a quadruple aerosol mass spectrometer (QAMS) system equipped with light scattering module. Our results show that the capture vaporizer introduces additional thermal decomposition of both inorganic and organic compounds, requiring modifications to the standard AMS fragmentation table, which is used to partition ion fragments to chemical classes. Experiments with mixed NH4NO3 and (NH4)2SO4 particles demonstrated linearity in the NH4+ ion balance, suggesting that there is no apparent matrix effect in the thermal vaporization-electron impact ionization detection scheme for mixed inorganic particles. Considering a typical ambient PM2.5 size distribution, we found that 89% of the non-refractory mass is detected with the new system, while only 65% with the old system. The NR-PM2.5 system described here can be adapted to existing Aerodyne Aerosol Mass Spectrometer (AMS) and ACSM systems.

Copyright © 2017 American Association for Aerosol Research  相似文献   


3.
Single-particle mass spectrometry (SPMS) has been widely used for characterizing the chemical mixing state of ambient aerosol particles. However, processes occurring during particle ablation and ionization can influence the mass spectra produced by these instruments. These effects remain poorly characterized for complex atmospheric particles. During the 2005 Study of Organic Aerosols in Riverside (SOAR), a thermodenuder was used to evaporate the more volatile aerosol species in sequential temperature steps up to 230°C; the residual aerosol particles were sampled by an aerosol mass spectrometer (AMS) and a single-particle aerosol time-of-flight mass spectrometer (ATOFMS). Removal of the secondary species (e.g., ammonium nitrate/sulfate) through heating permitted assessment of the change in ionization patterns as the composition changed for a given particle type. It was observed that a coating of secondary species can reduce the ionization efficiency by changing the degree of laser absorption or particle ablation, which significantly impacted the measured ion peak areas. Nonvolatile aerosol components were used as pseudo-internal standards (or “reference components”) to correct for this LDI effect. Such corrected ATOFMS ion peak areas correlated well with the AMS measurements of the same species up to 142°C. This work demonstrates the potential to accurately relate SPMS peak areas to the mass of specific aerosol components.

Copyright 2014 American Association for Aerosol Research  相似文献   


4.
The fraction of outdoor aerosol that penetrates into indoor environments plays an important role in determining the contribution of outdoor particles to the total lung dose of particles in human exposure. The objective of this study was to investigate the physical processes affecting migration of outdoor traffic particles into indoor environments. Particle number size distributions were measured by a fast mobility particle sizer system in both indoor and outdoor environments of a house located in close proximity to a busy street in Bologna (Italy) in the period February–April 2012. Indoor to outdoor (I/O) ratios for submicron particle number concentrations showed strong dependence on particle size and meteorological conditions. The loss rates of particles due to deposition, coagulation, and evaporation were determined using dynamic mass balance and coagulation models. Higher loss rates were found for small particles (nucleation and Aitken mode) indoors than for larger particles (accumulation mode). The coagulation and evaporation processes made a significant contribution to the loss of traffic nanoparticles indoors, especially during the day time. Application of positive matrix factorization to the indoor and outdoor particle size distributions showed a substantial loss of traffic-generated nucleation mode particles in the indoor environment, with evaporation playing a major role.

Copyright © 2017 American Association for Aerosol Research  相似文献   


5.
To address the critical need for improving the chemical characterization of the organic composition of ambient particulate matter, we introduce a combined thermal desorption aerosol gas chromatograph—aerosol mass spectrometer (TAG-AMS). The TAG system provides in-situ speciation of organic chemicals in ambient aerosol particles with hourly time resolution for marker compounds indicative of sources and transformation processes. However, by itself the TAG cannot separate by particle size and it typically speciates and quantifies only a fraction of the organic aerosol (OA) mass. The AMS is a real-time, in-situ instrument that provides quantitative size distributions and mass loadings for ambient fine OA and major inorganic fractions; however, by itself the AMS has limited ability for identification of individual organic compounds due to the electron impact ionization detection scheme used without prior molecular separation.

The combined TAG-AMS system provides real-time detection by AMS followed by semicontinuous analysis of the TAG sample that was acquired during AMS operation, achieving simultaneous and complementary measurements of quantitative organic mass loading and detailed organic speciation. We have employed a high-resolution time-of-flight mass spectrometer (HR-ToF-MS) to enable elemental-level determination of OA oxidation state as measured on the AMS, and to allow improved compound identification and separation of unresolved complex mixtures (UCM) measured on the TAG. The TAG-AMS interface has been developed as an upgrade for existing AMS systems. Such measurements will improve the identification of organic constituents of ambient aerosol and contribute to the ability of atmospheric chemistry models to predict ambient aerosol composition and loadings.

Copyright 2014 American Association for Aerosol Research  相似文献   


6.
A scanning mobility particle sizer was used to determine the size, number, and mass concentration of particle emissions from an ethanol-fueled homogeneous charge compression ignition (HCCI) engine. Semi-volatile particle composition was characterized using tandem differential mobility analysis (TDMA). Variable temperature thermal conditioning was used to gain insight into particle volatility and a catalytic stripper was used to determine the solid particle distribution. Four engine conditions were evaluated, including low to moderate range loads and motoring (deceleration, coasting). Results indicated that aerosol from a fully premixed HCCI engine under firing conditions is formed almost entirely via nucleation of semi-volatile material originating from the lubricating oil. TDMA analysis indicated 98% of total particle volume evaporated below 100°C. Results pointed towards homogeneous nucleation of precursors derived from the organic species in the lubricating oil, possibly in combination with a sulfur species. The motoring condition, with no fuel injected, exhibited the highest number and mass concentrations. During motoring, there was poor sealing leading to increased atomization of oil and associated ash emissions. Emissions were lower during firing with better sealing and much less atomization, but evaporation of the most volatile fractions of the lubricating oil still led to significant PM emissions consisting of nearly entirely semi-volatile particles containing very little ash.

© 2017 American Association for Aerosol Research  相似文献   


7.
The Aerosol Mass Spectrometer (AMS) and Aerosol Chemical Speciation Monitor (ACSM) are widely used for quantifying submicron aerosol mass concentration and composition, in particular for organic aerosols (OA). Using the standard vaporizer (SV) installed in almost all commercial instruments, a collection efficiency (CE) correction, varying with aerosol phase and chemical composition, is needed to account for particle bounce losses. Recently, a new “capture vaporizer” (CV) has been shown to achieve CE~1 for ambient aerosols, but its chemical detection properties show some differences from the SV due to the increased residence time of particles and vaporized molecules inside the CV. This study reports on the properties and changes of mass spectra of OA in CV-AMS using both AMS and ACSM for the first time. Compared with SV spectra, larger molecular-weight fragments tend to shift toward smaller ions in the CV due to additional thermal decomposition arising from increased residence time and hot surface collisions. Artifact CO+ ions (and to a lesser extent, H2O+), when sampling long chain alkane/alkene-like OA (e.g., squalene) in the CV during the laboratory studies, are observed, probably caused by chemical reactions between sampled OA and molybdenum oxides on the vaporizer surfaces (with the carbon derived from the incident OA). No evidence for such CO+ enhancement is observed for ambient OA. Tracer ion marker fractions (fm/z =, i.e., the ratio of the organic signal at a given m/z to the total OA signal), which are used to characterize the impact of different sources are still present and usable in the CV. A public, web-based spectral database for mass spectra from CV-AMS has been established.

Copyright © 2018 American Association for Aerosol Research  相似文献   


8.
The aerosol mass spectrometer (AMS) and aerosol chemical speciation monitor (ACSM) are widely used for quantifying aerosol composition. The quantification uncertainty of these instruments is dominated by the collection efficiency (CE) due to particle bounce. A new “capture vaporizer” (CV) has been recently developed to achieve unit CE. In this study, we examine the performance of the CV while sampling ambient aerosols. AMS/ACSMs using the original standard vaporizer (SV) and CV were operated in parallel during three field studies. Concentrations measured with the CV (assuming CE = 1) and SV (using the composition-dependent CE of Middlebrook et al.), as well as SMPS and PILS-IC are compared. Agreement is good in all cases, verifying that CE ~ 1 in the CV when sampling ambient particles. Specific findings include: (a) The fragmentation pattern of ambient nitrate and sulfate species observed with the CV was shifted to smaller m/z, suggesting additional thermal decomposition. (b) The differences in fragmentation patterns of organic vs. inorganic nitrate and sulfur species are still distinguishable in the CV, however, with much lower signal-to-noise compared to the SV. (c) Size distribution broadening is significant, but its impact is limited in field studies since ambient distributions are typically quite broad. Consistent size distributions were measured with the SV and CV. (d) In biogenic areas, UMR nitrate is overestimated based on the default fragmentation table (~factor of 2–3 in SOAS) for both vaporizers, due to underestimation of the organic interferences. We also report a new type of small interference: artifact chloride signal can be observed in the AMS when high nitrate mass concentration is sampled with both the SV (~0.5% chloride/nitrate) or CV (~0.2% chloride/nitrate). Our results support the improved quantification with the CV AMS and characterize its chemical detection properties.

Copyright © 2017 American Association for Aerosol Research  相似文献   


9.
To reduce air pollution and the reliance on fossil fuel, biodiesel has been widely investigated as an alternative fuel for diesel engines. The purpose of this study is to investigate the influence of waste cooking oil (WCO) biodiesel on the physical properties and the oxidation reactivity of the particles emitted by a diesel engine operating on WCO biodiesel as the main fuel. Experiments were conducted on a direct-injection diesel engine fueled with biodiesel, B75 (75% biodiesel and 25% diesel on volume basis, v/v), B50, B20, and diesel fuel, at five engine loads and at an engine speed of 1920 rev/min. Particulate samples were collected to analyze the particulate nanostructure, volatility, and oxidation characteristics. Biodiesel or low-load operation leads to smaller primary particles and more disordered nanostructures having shorter and more curved graphene layers. It can be found that particles from biodiesel, blended fuels, or low-load operation have higher volatile mass fractions and faster oxidation reaction rates than particles from diesel or heavy-load operation. The higher oxidation reaction rates are due mainly to the smaller particle size, the more disordered nanostructure, and the higher volatile mass fraction. It is also found that changes in primary particle size and particulate nanostructure are not directly proportional to the biodiesel content, while changes in particulate volatility and particulate oxidation reactivity are proportional to the biodiesel content. The use of biodiesel can enhance particulate oxidation reactivity and the regeneration of soot particles in an after-treatment device.

Copyright © 2016 American Association for Aerosol Research  相似文献   


10.
11.
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   


12.
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   


13.
Understanding the links between aerosol and cloud and radiative properties remains a large uncertainty in predicting Earth's changing energy budget. Surfactants are observed in ambient atmospheric aerosol particles, and their effect on cloud droplet growth is a mechanism that was, until recently, neglected in model calculations of particle activation and droplet growth. In this study, coarse mode aqueous aerosol particles were created containing the surfactant Igepal CA-630 and NaCl. The evaporation and condensation of these individual aqueous particles were investigated using an aerosol optical trap combined with Raman spectroscopy. For a relative humidity (RH) change from 70% to 80%, droplets containing both Igepal and NaCl at atmospheric concentrations exhibited on average more than 4% larger changes in droplet radii, compared to droplets containing NaCl only. This indicates enhanced water uptake in the presence of surfactants, but this result is unexpected based on the standard calculation of the effect of surfactants, using surface tension reduction and/or hygroscopicity changes, for particles of this size. One implication of these results is that in periods with increasing RH, surfactant-containing aqueous particles may grow larger than similarly sized aqueous NaCl particles without surfactants, thus shifting atmospheric particle size distributions, influencing particle growth, and affecting aerosol loading, visibility, and radiative forcing.

Copyright © 2018 American Association for Aerosol Research  相似文献   


14.
The aerodynamic lens system of the Aerodyne Aerosol Mass Spectrometer (AMS) was analyzed using the Aerodynamic Lens Calculator. Using this tool, key loss mechanisms were identified, and a new lens design that can extend the transmission of particulate matter up to 2.5 μm in diameter (PM2.5) was proposed. The new lens was fabricated and experimentally characterized. Test results indicate that this modification to the AMS lens can significantly improve the transmission of large sized particles, successfully achieving a high transmission efficiency up to PM2.5 range.

© 2016 American Association for Aerosol Research  相似文献   


15.
Differential mobility analyzers (DMAs) are widely used for calibrating other instruments and measuring aerosol size distributions. DMAs classify aerosol particles according to their electrical mobility, which is assumed to be constant during the classification process. However, particles containing semivolatile substances can change their size in the DMA, leading to sizing errors. In this article, the effect of particle size changes during the classification process on the sizing accuracy of DMAs is discussed. It is shown that DMAs select particles whose time-of-flight-averaged electrical mobility is equal to that of stable particles that are selected under given operating conditions. For evaporating particles, this implies that DMAs select particles that are originally larger than the reported size. At the exit of the DMA, selected particles are smaller than the reported size. Particle evaporation and growth inside DMAs was modeled to study the effect of particle size changes on the sizing accuracy and the transfer function of DMAs in constant- and scanning-voltage modes of operation. Modeling predictions were found to agree well with the results of experiments with ammonium nitrate aerosol. The model was used to estimate sizing errors when measuring hygroscopic and other volatile aerosols. Errors were found to be larger at smaller sizes and low sheath flow rates. Errors, however, are fairly small when saturation concentration is below 10 μg/m3, assuming an evaporation coefficient of 0.1. Particles size changes during classification lead to distortion of the DMA transfer function. In voltage scanning mode, errors are generally larger, especially at high scan rates.

Copyright 2014 American Association for Aerosol Research  相似文献   


16.
This work presents the development and characterization of a thermodenuder for the study and interpretation of aerosol volatility. Thermodenuder measurements are further combined with a continuous-flow streamwise thermal gradient CCN counter to obtain the corresponding aerosol hygroscopicity. The thermodenuder response function is characterized with monodisperse aerosol of variable volatility and hygroscopicity. The measurements are then interpreted with a comprehensive instrument model embedded within an optimization framework to retrieve aerosol properties with constrained uncertainty. Special attention is given to the interpretation of the size distribution of the thermodenuded aerosol, deconvoluting the effects of impurities and multiple charging, and to simplifications on the treatment of thermodenuder geometry, temperature, the cooling section, and the effects of curvature and accommodation coefficient on inferred particle volatility. Retrieved vapor pressures are consistent with published literature and shown to be most sensitive to uncertainty in the accommodation coefficient.

Copyright 2014 American Association for Aerosol Research  相似文献   


17.
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   


18.
Many well-established models can be applied to calculate the filtration efficiencies. In these models the filtration velocity and challenging particle size are assumed to be known accurately. However, in realistic filtration tests, the filtration velocity has profiles dependent on the filter holder geometry and experimental conditions; the challenging particles have size distributions dependent on the instruments and operation conditions. These factors can potentially affect the measured filtration efficiency and lead to discrepancies with the models.

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

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

Copyright © 2017 American Association for Aerosol Research  相似文献   


19.
The performance of a thermal denuder (thermodenuder—TD) and a fresh catalytic stripper (CS) was assessed by sampling laboratory aerosol, produced by different combinations of sulfuric acid, octacosane, and soot particles, and marine exhaust aerosol produced by a medium-speed marine engine using high sulfur fuels. The intention was to study the efficiency in separating non-volatile particles. No particles could be detected downstream of either device when challenged with neat octacosane particles at high concentration. Both laboratory and marine exhaust aerosol measurements showed that sub-23 nm semi-volatile particles are formed downstream of the thermodenuder when upstream sulfuric acid approached 100 ppbv. Charge measurements revealed that these are formed by re-nucleation rather than incomplete evaporation of upstream aerosol. Sufficient dilution to control upstream sulfates concentration and moderate TD operation temperature (250°C) are both required to eliminate their formation. Use of the CS following an evaporation tube seemed to eliminate the risk for particle re-nucleation, even at a ten-fold higher concentration of semi-volatiles than in case of the TD. Particles detected downstream of the CS due to incomplete evaporation of sulfuric acid and octacosane aerosol, did not exceed 0.01% of upstream concentration. Despite the superior performance of CS in separating non-volatile particles, the TD may still be useful in cases where increased sensitivity over the traditional evaporation tube method is needed and where high sulfur exhaust concentration may fast deplete the catalytic stripper adsorption capacity.

Copyright © 2018 American Association for Aerosol Research  相似文献   


20.
Predicting indoor exposures to ambient organic aerosol (OA) is complicated by shifts in the gas-particle partitioning of ambient organics with outdoor-to-indoor transport. This analysis aims to quantify the effect of changes in temperature and OA loading on the gas-particle partitioning of ambient organics transported indoors and explores whether accounting for shifts in partitioning closes the gap between measured indoor ambient OA concentrations and indoor concentrations calculated in a previous analysis using a model that accounts for only physical losses. Changes in the gas-particle partitioning of ambient organics with outdoor-to-indoor transport were calculated for 167 homes using measured temperatures and OA concentrations and published OA volatility distributions. Initially, it was assumed that ambient OA could be represented with a single volatility distribution. We then repeated the analysis treating ambient OA as the sum of distinct components, each with a distinct volatility distribution, derived from factor analysis of aerosol mass spectra (e.g., hydrocarbon-like OA [HOA], oxygenated OA [OOA]). We also evaluated the sensitivity of our calculations to uncertainty in the thermodynamic properties of ambient OA by varying the enthalpy of vaporization. Partitioning shifts were sensitive to enthalpy-of-vaporization assumptions and resulted in changes in indoor ambient OA concentrations of 13–27%. Our calculations indicate that phase changes are important determinants of residential exposure to ambient OA and are of sufficient magnitude to close the gap between measured and modeled indoor concentrations of ambient OA.

Copyright 2014 American Association for Aerosol Research  相似文献   


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