Soot Aggregates Research Articles

Determining fractal properties of soot aggregates and primary particle size distribution in counterflow flames up to 10 atm

Abstract Experimental investigations of soot morphology are performed in counterflow flames of N2-diluted ethylene and air, up to 10 atm. A thermophoretic sampling device is attached to a pressure vessel containing a counterflow burner where flames with an ethylene mole fraction of 0.3 are stabilized at 3, 5, and 6 atm. To allow measurements at higher pressures, the fuel mole fraction is lowered to 0.2 to reduce the soot loading and flames are studied at 5, 7, and 10 atm. Thermophoretic sampling of the soot zone is performed using TEM grids. The sampling process causes minimal flame disturbances. Soot collected on TEM grids is analyzed under transmission electron microscope (TEM). Primary particle size distributions are inferred at each pressure by manually analyzing the primary particles from TEM images. Fractal properties of soot at each pressure are also obtained by analyzing the TEM images at comparatively low magnifications. Mean primary particle diameter increases from 17.5 to 47.1 nm as the pressure is increased from 3 to 10 atm, whereas the fractal dimension and prefactor do not change with pressure up to 10 atm. For the flames studied here, fractal dimension lies between 1.61 and 1.67 whereas fractal prefactor varies between 1.68 and 1.86 without following any apparent trend with pressure.

In-flame soot particle structure on the up- and down-swirl side of a wall-interacting jet in a small-bore diesel engine

This study shows how the structure of soot particles within the flame changes due to the relative direction of the swirl flow in a small-bore diesel engine in which significant flame–wall interactions cause about half of the flame travelling against the swirl flow while the other half penetrating in the same direction. The thermophoresis-based particle sampling method was used to collect soot from three different in-flame locations including the flame–wall impingement point near the jet axis and the two 60° off-axis locations on the up-swirl and down-swirl side of the wall-interacting jet. The sampled soot particle images were obtained using transmission electron microscopes and the image post-processing was conducted for statistical analysis of size distribution of soot primary particles and aggregates, fractal dimension, and sub-nanoscale parameters such as the carbon layer fringe length, tortuosity, and spacing. The results show that the jet-wall impingement region is dominated by many small immature particles with amorphous internal structure, which is very different to large, fractal-like soot aggregates sampled from 60° downstream location on the down-swirl side. This structure variation suggests that the small immature particles underwent surface growth, coagulation and aggregation as they travelled along the piston-bowl wall. During this soot growth, the particle internal structure exhibits the transformation from amorphous carbon segments to a typical core–shell structure. Compared to those on the down-swirl side, the soot particles sampled on the up-swirl side show much lower number counts and more compact aggregates composed of highly concentrated primary particles. This soot aggregate structure, together with much narrower carbon layer gap, indicates higher level of soot oxidation on the up-swirl side of the jet.

Impact of the primary particle polydispersity on the radiative properties of soot aggregates

Abstract Combustion generated soot appears as fractal aggregates formed by polydisperse nearly spherical primary particles. Knowledge of their radiative properties is a prerequisite for laser based diagnostics of soot. In this parametric study, the effect of primary particle polydispersity on soot aggregate absorption and scattering properties is investigated numerically. Two series of fractal aggregates formed by normal and lognormal distributed primary particles of different levels of standard deviation were numerically generated for typical flame soot with a fractal dimension and prefactor fixed to D f = 1.73 and kf ≈ 1.5, respectively. Three aggregate sizes consisting of N p = 15 , 50 and 150 monomers per aggregate were investigated. Due to the uncertainty in soot refractive index, radiative properties were calculated by considering two different refractive indices at λ ≈ 532 nm recommended in the literature using the Discrete Dipoles Approximation and the Generalized Multiparticle Mie method. The results are interpreted in terms of correction factors to the Rayleigh–Debye–Gans theory for fractal aggregates (RDG-FA) for the forward scattering cross section A and for the absorption cross section h. It is shown that differential cross section for vertically polarized incident light, total scattering and absorption cross sections are well predicted by the RDG-FA theory for all considered aggregates formed by normally ( σ / d p ¯ ≤ 30%) and lognormally (σgeo ≤ 1.6) distributed primary particles. The refractive index is found to be of greater impact than primary particle polydispersity on the importance of multiple scattering. The radiative force per unit laser power experienced by the soot aggregates was found primarily determined by the aggregate volume, regardless of the level of primary particle polydispersity.

Morphological transformation of soot: investigation of microphysical processes during the condensation of sulfuric acid and limonene ozonolysis product vapors

Abstract. The morphological transformation of soot particles via condensation of low-volatility materials constitutes a dominant atmospheric process with serious implications for the optical and hygroscopic properties, as well as atmospheric lifetime of the soot. We consider the morphological transformation of soot aggregates under the influence of condensation of vapors of sulfuric acid, and/or limonene ozonolysis products. This influence was systematically investigated using a Differential Mobility Analyzer coupled with an Aerosol Particle Mass Analyzer (DMA–APM) and the Tandem DMA techniques integrated with a laminar flow-tube system. We hypothesize that the morphology transformation of soot results (in general) from a two-step process, i.e., (i) filling of void space within the aggregate and (ii) growth of the particle diameter. Initially, the transformation was dominated by the filling process followed by growth, which led to the accumulation of sufficient material that exerted surface forces, which eventually facilitated further filling. The filling of void space was constrained by the initial morphology of the fresh soot as well as the nature and the amount of condensed material. This process continued in several sequential steps until all void space within the soot aggregate was filled. And then “growth” of a spherical particle continued as long as vapors condensed on it. We developed a framework for quantifying the microphysical transformation of soot upon the condensation of various materials. This framework used experimental data and the hypothesis of “ideal sphere growth” and void filling to quantify the distribution of condensed materials in the complementary filling and growth processes. Using this framework, we quantified the percentage of material consumed by these processes at each step of the transformation. For the largest coating experiments, 6, 10, 24, and 58 % of condensed material went to filling process, while 94, 90, 76, and 42 % of condensed material went to growth process for 75, 100, 150, and 200 nm soot particles, respectively. We also used the framework to estimate the fraction of internal voids and open voids. This information was then used to estimate the volume-equivalent diameter of the soot aggregate containing internal voids and to calculate the dynamic shape factor, accounting for internal voids. The dynamic shape factor estimated based on the traditional assumption (of no internal voids) differed significantly from the value obtained in this study. Internal voids are accounted for in the experimentally derived dynamic shape factor determined in the present study. In fact, the dynamic shape factor adjusted for internal voids was close to 1 for the fresh soot particles considered in this study, indicating the particles were largely spherical. The effective density was strongly correlated with the morphological transformation responses to the condensed material on the soot particle, and the resultant effective density was determined by the (i) nature of the condensed material and (ii) morphology and size of the fresh soot. In this work we quantitatively tracked in situ microphysical changes in soot morphology, providing details of both fresh and coated soot particles at each step of the transformation. This framework can be applied to model development with significant implications for quantifying the morphological transformation (from the viewpoint of hygroscopic and optical properties) of soot in the atmosphere.

Experimental study on combustion characteristics of an n-butanol-biodiesel droplet

This work was aimed to study droplet combustion which was a foundation of spray combustion. Combustion characteristics of BUT00 (pure biodiesel) and BUT50 (50% n-butanol and 50% biodiesel by mass) were investigated using droplet suspension technology under 1 bar and 900 K. One flame was observed for BUT00 while two flames were observed for BUT50. The flame of BUT00 underwent successively faint luminosity, bright luminosity, soot aggregate and soot spread. The first flame of BUT50 was faint and the second one was similar to that of BUT00 because they were caused by n-butanol and biodiesel combustion respectively. Before the auto-ignition of BUT00, (D/D0)2 was approximately unchanged at 1.0 and similarity degree (SD) was higher than 97%. Temperature growth rate (TGR) decreased first quickly and then slowly. After the auto-ignition of BUT00, (D/D0)2 sharply decreased and SD was in the range of 90–97%. The flame heating led to the increase of TGR. For BUT50, obvious fluctuations were found in (D/D0)2, SD and TGD. The SD of BUT50 was generally lower than 97%. The (D/D0)2 of BUT50 included transient heating, fluctuation evaporation and equilibrium evaporation phases. Some characteristic parameters were deterministic although (D/D0)2 in fluctuation evaporation phase was a non-deterministic process.

Individual particle SEM-EDS analysis of atmospheric aerosols in rural, urban, and industrial sites of Central Italy

PM10 samples were collected simultaneously at three representative areas (urban, industrial, and rural areas). Their morphology and elemental composition were determined by scanning electron microscopy coupled with energy-dispersive analysis (SEM-EDS). Twenty-four chemical parameters (C, O, Na, Mg, Al, Si, P, Cd, Cl, K, Ca, S, Sn, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, W, and Pb) were determined and three morphological parameters (area, roundness, and fractal dimension) were measured by Image Pro Analyzer 6.3. The particles were classified into ten groups based on morphology and elemental composition: Ca-rich and metal particles, soot aggregates, cenosphere, alumosilicates, sea salt, calcium sulfate, spherical particles of iron, biological carbonaceous particles, and various. Particles of natural origin were predominantly found in the coarse size fraction and particles of anthropogenic origin in the fine size fraction. The greatest contribution to particulate matter belonged to aluminum-silicates and calcium-rich particles. The cenosphere were recognized only in the coastal urban site, while all the other particles were present in each site. The coastal industrial site was characterized by the prevalence of alumosilicates and Ca-rich particles, due to construction activity in this site during the sampling period (movement of vehicles, transport of terrigenous materials, and use of construction products). The coastal urban site was characterized by a higher amount of soot and by the presence of cenosphere, due to the presence of vehicular traffic.

Joint-scalar transported PDF modelling of soot in a turbulent non-premixed natural gas flame

The focus of the present work is on the prediction of soot in the turbulent Delft III/Adelaide natural gas flame at a Reynolds number of 9700. A parabolic flow solver with the SSG (Speziale, Sarkar and Gatski) Reynolds stress transport model for turbulence is coupled to a joint-scalar transported PDF (probability density function) approach allowing exact treatment of the interactions of turbulence with the solid and gas phase chemistries. Scalar mixing is treated via the modified Curl's coalescence/dispersion model and two different closures for the scalar dissipation rate are explored. The gas phase chemistry is represented by a systematically reduced mechanism featuring 144 reactions, 15 solved and 14 steady-state species. The dynamics of soot particles, including coagulation and aggregation in the coalescent and fractal aggregate limits, is treated either via a simplified two-equation model or via the MOMIC (method of moments with interpolative closure). The inclusion of soot surface reactions based on a second ring PAH (polycyclic aromatic hydrocarbon) analogy is also investigated. Soot oxidation via O, OH and O is taken into account and the sensitivity to the applied rates is investigated. An updated acetylene-based soot nucleation rate is formulated based on consistency with detailed chemistry up to pyrene and combined with a sectional model to compute soot particle size distributions in the NIST well-stirred/plug flow reactor configuration. The derived rate is subsequently used in turbulent flame calculations and subjected to a sensitivity analysis. Radiative emission from soot and gas phase species is accounted for using the RADCAL method and by the inclusion of enthalpy as a solved scalar. Computed soot levels reproduce experimental data comparatively well and approximately match absolute values. The axial location of peak soot in the Delft III/Adelaide flame is consistent with previous large eddy simulations and possible causes for the discrepancy with experimental data are analysed.

Soot aggregate morphology in coflow laminar ethylene diffusion flames at elevated pressures

The effect of combustion pressure on soot aggregate morphology and on primary soot particle diameter was investigated by thermophoretic sampling in nitrogen-diluted ethylene flames. Soot aggregate samples were collected using a high-pressure thermophoretic sampling system installed inside the high-pressure combustion chamber. Collected samples were imaged by transmission electron microscopy followed by an automated image analysis process to yield aggregate morphology information. The experiments covered pressures from 3 to 6 bar, and samples were collected at heights of 2 and 5 mm above the burner exit in nitrogen-diluted ethylene (ethylene to nitrogen mole ratio 2:1) flames with nominal visible flame heights of about 20 mm. It was observed that average primary soot particle diameter increased with increasing pressure within the pressure range considered, at both measurement locations within the flame. Fractal parameters of the soot aggregates were inferred directly from the experimental data (as opposed to the usual practice of assuming a priori values for fractal dimension and pre-factor). Near to the soot nucleation and growth regions of the co-flow laminar diffusion flames, at 2 mm above the burner exit, the fractal dimension of the aggregates was not as high as the accepted universal value of about 1.9, in spite of the fact that number of primary particles per aggregate is quite high and pressure is well above atmospheric. At 5 mm above the burner exit, however, the fractal dimension of the soot aggregates approached the accepted universal value of 1.9, at high pressures; at relatively lower pressures, the fractal dimension was about 1.6 at the same location within the flame. In view of the inferred fractal results, caution should be exercised when applying fractal analysis to low heights in flames at lower pressures where soot inception and growth are relatively dominant.

Impact of Humidity on Silica Nanoparticle Agglomerate Morphology and Size Distribution.

The effect of humidity on flame-made metal oxide agglomerate morphology and size distribution is investigated, for the first time to our knowledge, and compared to that on soot, which has been widely studied. Understanding the impact of humidity on such characteristics is essential for storage, handling, processing, and eventual performance of nanomaterials. More specifically, broadly used agglomerates of flame-made silica nanoparticles are humidified at various saturation ratios, S = 0.2-1.5, and dried before characterization with a differential mobility analyzer (DMA), an aerosol particle mass (APM) analyzer, and transmission electron microscopy. At high humidity, the constituent single and/or aggregated (chemically bonded) primary particles (PPs) rearrange to balance the capillary forces induced by condensation-evaporation of liquid bridges between PPs. Larger agglomerates restructure more than smaller ones, narrowing their mobility size distribution. After humidification at S = 1.5 and drying, agglomerates collapse into compact structures that follow a fractal scaling law with mass-mobility exponent Dfm = 3.02 ± 0.11 and prefactor km = 0.27 ± 0.07. This critical S = 1.5 for silica agglomerates is larger than the 1.26 obtained for soot because of the hydrophilic surface of silica that delays water evaporation. The relative effective density, ρeff/ρ, of collapsed agglomerates becomes invariant of mobility diameter, dm, similar to that of fluidized and spray-dried granules. The average silica ρeff/ρ = 0.28 ± 0.02 is smaller than the 0.36 ± 0.04 measured for the humidified-dried soot because of the larger size of silica aggregates, dm/ dp, and number of constituent primary particles, np, of diameter dp. This is verified by tandem-DMA (TDMA) measurements, yielding maximum dm = 3 dpor 5 dp and np = 13 or 36 for the soot or silica aggregates studied here, in good agreement with those reported from microscopy and high-pressure agglomerate dispersion. A scaling law relating the initial dm,o to dm, Dfm, and km after condensation-drying is developed. The mass-mobility relationship of collapsed silica and soot agglomerates obtained by combining this law with fast TDMA measurements is in excellent agreement with that measured by the direct, but tedious, DMA-APM analysis.

Soot production modeling in a laminar coflow ethylene diffusion flame at different Oxygen Indices using a PAH-based sectional model

A numerical study is carried out to, first of all, investigate the capability of a Polycyclic Aromatic Hydrocarbon (PAH)-based sectional particle dynamics soot model in the prediction of soot production in laminar coflow ethylene diffusion flames. The effects of different oxygen mole fractions in the oxidizer stream, called Oxygen Index (OI), ranging from 17% to oxygen-enriched conditions up to 33% are investigated. Secondly, the relative importance of species responsible for the increase in both soot formation and oxidation rates with increasing the OI is analyzed. The soot production model considers a detailed description of nucleation via collisions among heavy PAHs, particle aggregation, PAH condensation, surface growth and oxidation through the hydrogen abstraction acetylene addition (HACA) mechanism, and fragmentation of soot aggregates. Model predictions are compared with previously-published experimental data and numerical predictions obtained with a semi-empirical acetylene-based soot production model [Comb. Flame 160: 786–795 (2013)]. Results indicate that the flame structure, soot volume fraction and flame cross-section integrated soot volume fraction predicted by the PAH-based sectional soot model are in good agreement with the experimental data over the entire range of OI considered. The temperature and the concentrations of soot precursors increase with the OI, leading to higher soot nucleation, condensation, surface growth, and oxidation rates. Results show that the PAH-based sectional soot model represents a significant improvement over the semi-empirical acetylene based two-equation soot model studied earlier, especially in conditions far from the normal air conditions (21% of O2). With increasing the OI, the non-dimensional zone of influence does not change for the flame cross-section integrated soot formation rates but increases for the integrated soot oxidation rate. Nucleation occurs just above the burner rim and displays the largest increase in its rate with increasing the OI. Nucleation and condensation are mainly dependent on the concentrations of BGHIF and BAPYR. Condensation is also affected by the increase in the number of aggregates available for collision. Soot formation is mainly dominated by surface growth, through HACA, with a significant influence of soot condensation closer to the burner surface, regardless of the level of OI. The surface growth through HACA is mainly controlled not only by the acetylene concentration and the associated kinetic rate, but also by the specific soot surface area. Oxidation by O2 is found to dominate at the top of the flame, while oxidation by OH is dominant at the middle height of the flame. The oxidation rate by O2 increases more rapidly with increasing the OI than that by OH.

Characterization of coal burning-derived individual particles emitted from an experimental domestic stove

Coal combustion in the domestic stoves, which is common in most parts of the Chinese countryside, can release harmful substances into the air and cause health issues. In this study, particles emitted from laboratory stove combustion of the raw powder coals were analyzed for morphologies and chemical compositions by using transmission electron microscopy (TEM) coupled with energy-dispersive X-ray spectrometry (EDX). The coal burning-derived individual particles were classified into two groups: carbonaceous particles (including soot aggregates and organic particles) and non-carbonaceous particles (including sulfate, mineral and metal particles). The non-carbonaceous particles, which constituted a majority of the coal burning-derived emissions, were subdivided into Si-rich, S-rich, K-rich, Ca-rich, and Fe-rich particles according to the elemental compositions. The Si-rich, S-rich and K-rich particles are commonly observed in the coal burning emission. The proportions for particles of different types exhibit obvious coal-issue dependence. Burning of coal with high ash yield could emit more non-carbonaceous particles, and burning of coal with high sulfur content can emit more S-rich particles. By comparing the S-rich particles from this coal burning experiment with those in the atmosphere, we draw a conclusion that some S-rich particles in the atmosphere in China could be mainly sourced from coal combustion.

Optical characterization limits of nanoparticle aggregates at different wavelengths using approximate Bayesian computation

Optical characterization of nanoparticle aggregates is a complex inverse problem that can be solved by deterministic or statistical methods. Previous studies showed that there exists a different lower size limit of reliable characterization, corresponding to the wavelength of light source used. In this study, these characterization limits are determined considering a light source wavelength range changing from ultraviolet to near infrared (266–1064 nm) relying on numerical light scattering experiments. Two different measurement ensembles are considered. Collection of well separated aggregates made up of same sized particles and that of having particle size distribution. Filippov's cluster-cluster algorithm is used to generate the aggregates and the light scattering behavior is calculated by discrete dipole approximation. A likelihood-free Approximate Bayesian Computation, relying on Adaptive Population Monte Carlo method, is used for characterization. It is found that when the wavelength range of 266–1064 nm is used, successful characterization limit changes from 21–62 nm effective radius for monodisperse and polydisperse soot aggregates.

Sensitivity analysis of morphology on radiative properties of soot aerosols.

Absorption cross section (Cabs), scattering cross section (Csca) and asymmetry parameter (ASY) of soot particles in different atmospheric aging status were investigated under fixed equivalent volume radius (RV) using the numerically exact multiple-sphere T-matrix method. The radiative properties of soot particles would be largely diverse in different aging status even RV is fixed. However, there are many insensitive parameters under different aging status. The Cabs and ASY is insensitive to monomers number (Ns) when Ns is larger than a threshold value. For bare and thinly coated soot aggregates, Cabs is insensitive to fractal dimension (Df) when the RV is small, where the relative errors of Cabs for different Df are within 2.5%. However, the effects of Df is obvious for large soot due to the shielding effects of large monomers, and the relative errors for different Df can reach to 18% for bare soot. For thinly coated soot, the changes of ASY with soot volume fraction (fsoot) is small due to the little changes of the fractal structure when the RV is fixed. In addition, for thickly coated soot, ASY is insensitive to Ns due to the unchanged overall spherical structure. Our results give a further understanding of the influences of morphology on radiative properties. It may be helpful for model selection and model simplification.

Morphology and nano-structure analysis of soot particles sampled from high pressure diesel jet flames under diesel-like conditions

Soot particles emitted from diesel engines have a significant impact on the atmospheric environment. Detailed understanding of soot formation and oxidation processes is helpful for reducing the pollution of soot particles, which requires information such as the size and nano-structure parameters of the soot primary particles sampled in a high-temperature and high-pressure diesel jet flame. Based on the thermophoretic principle, a novel sampling probe minimally disturbing the diesel jet flame in a constant volume combustion vessel is developed for analysing soot particles. The injected quantity of diesel fuel is less than 10 mg, and the soot particles sampled by carriers with a transmission electron microscope (TEM) grid and lacey TEM grid can be used to analyse the morphologies of soot aggregates and the nano-structure of the soot primary particles, respectively. When the quantity of diesel fuel is more than 10 mg, in order to avoid burning-off of the carriers in higher temperature and pressure conditions, single-crystal silicon chips are employed. Ultrasonic oscillations and alcohol extraction are then implemented to obtain high quality soot samples for observation using a high-resolution transmission electron microscope. An in-house Matlab-based code is developed to extract the nano-structure parameters of the soot particles. A complete sampling and analysis procedure of the soot particles is provided to study the formation and oxidation mechanism of soot.

Effect of after injections on late cycle soot oxidation in a small-bore diesel engine

After injection, for which a short fuel injection follows the main injection, is proved to be effective in reducing soot emissions in diesel engines. The present study aims to better understand this in-cylinder soot reduction mechanism of after injection with a particular emphasis on its efficacy in a small-bore diesel engine in which more significant flame-wall interactions could cause different behaviour compared with extensively studied heavy-duty diesel engines in the literature. With the main injection only case as a baseline, two after-injection cases of close-coupled and long-dwell timings have been investigated in a single-cylinder common-rail optical engine. Various optical/laser-based imaging diagnostics have been performed including line-of-sight integrated chemiluminescence imaging of OH*, planar laser-induced florescence of hydroxyl (OH-PLIF), planar laser-induced incandescence of soot (PLII) and transmission electron microscope (TEM) imaging of thermophoretically sampled in-flame soot particles to visualise the spatial and temporal evolution of high temperature reaction and soot as well as particle structure. The results indicate that both after-injection strategies introduce a secondary heat release that leads to additional bulk gas temperature rise and thereby promoting the late-cycle soot oxidation. However, the efficacy is found to be dependent upon the after-injection timing. The OH-PLIF and PLII images show that the close-coupled after-injection induces additional high-temperature reaction and soot formation due to high ambient gas temperature. The new reaction occurs near the jet–wall impingement point, which is well separated from the main combustion zone as the main fuel jet travelled along the bowl wall due to significant jet–wall interactions. Although the main and after-injection soot are decoupled, soot morphology analysis based on TEM images suggests that the close-coupled after-injection does enhance the oxidation of main combustion-generated soot particles through the breakdown of large soot aggregates at elevated temperatures and with increased OH radicals. In comparison, both OH-PLIF and PLII images show no visual evidences of decoupled after-injection combustion for the long-dwell case due to insufficient temperature as the additional reaction occurs later in the expansion stroke. However, the increased OH radicals and breakdown of soot aggregates in the main combustion region are evident in OH-PLIF and TEM images. Overall, the close-coupled after-injection adds more soot but induces a higher degree of oxidation for the main combustion-generated soot particles. By contrast, the promotion of soot oxidation is less significant for the long-dwell after-injection but it produces no extra soot.

Morphologies and elemental compositions of local biomass burning particles at urban and glacier sites in southeastern Tibetan Plateau: Results from an expedition in 2010

Many studies indicate that the atmospheric environment over the southern part of the Tibetan Plateau is influenced by aged biomass burning particles that are transported over long distances from South Asia. However, our knowledge of the particles emitted locally (within the plateau region) is poor. We collected aerosol particles at four urban sites and one remote glacier site during a scientific expedition to the southeastern Tibetan Plateau in spring 2010. Weather and backward trajectory analyses indicated that the particles we collected were more likely dominated by particles emitted within the plateau. The particles were examined using an electron microscope and identified according to their sizes, shapes and elemental compositions. At three urban sites where the anthropogenic particles were produced mainly by the burning of firewood, soot aggregates were in the majority and made up >40% of the particles by number. At Lhasa, the largest city on the Tibetan Plateau, tar balls and mineral particles were also frequently observed because of the use of coal and natural gas, in addition to biofuel. In contrast, at the glacier site, large numbers of chain-like soot aggregates (~25% by number) were noted. The morphologies of these aggregates were similar to those of freshly emitted ones at the urban sites; moreover, physically or chemically processed ageing was rarely confirmed. These limited observations suggest that the biomass burning particles age slowly in the cold, dry plateau air. Anthropogenic particles emitted locally within the elevated plateau region may thus affect the environment within glaciated areas in Tibet differently than anthropogenic particles transported from South Asia.

Physicochemical Characteristics of Individual Aerosol Particles during the 2015 China Victory Day Parade in Beijing

During the 2015 China Victory Day parade control periods, the air quality in Beijing hit the best record, leading to 15 continuous good days with an average PM2.5 mass concentration 18 μg/m3, which provided a unique opportunity to study the ambient aerosols in megacity Beijing. The morphology and elemental composition of aerosol particles were investigated by transmission electron microscopy coupled with energy dispersive X-ray spectrometry (TEM-EDX). Five types of individual particles were identified, including homogeneous mixed S-rich particles (HS; 44.9%), organic coated S-rich particles (CS; 34.3%), mineral particles (10.5%), soot aggregates (7.21%) and organic particles (3.2%). The number percentage of secondary particles (including HS and CS) accounted for a large proportion with 79.2% during the control periods. The average diameter of secondary particles increased with relative humidity (RH), being 323 nm, 358 nm and 397 nm at the RH 34%, 43% and 53%, respectively, suggesting that the high RH might favor the growth of secondary particles. The higher proportion of CS particles may show great atmospheric implications and the CS particles may be formed by the condensation of secondary organic aerosols on pre-existing S-rich particles.

Physico-Chemical Characterization of Fine and Ultrafine Particles Emitted during Diesel Particulate Filter Active Regeneration of Euro5 Diesel Vehicles.

Diesel particulate filters (DPFs) are commonly employed in modern passenger cars to comply with current particulate matter (PM) emission standards. DPFs requires periodic regeneration to remove the accumulated matter. During the process, high-concentration particles, in both nucleation and accumulation modes, are emitted. Here, we report new information on particle morphology and chemical composition of fine (FPs) and ultrafine particles (UFPs) measured downstream of the DPF during active regeneration of two Euro 5 passenger cars. The first vehicle was equipped with a close-coupled diesel oxidation catalyst (DOC) and noncatalyzed DPF combined with fuel borne catalyst and the second one with DOC and a catalyzed-diesel particle filter (CDPF). Differences in PM emission profiles of the two vehicles were related to different after treatment design, regeneration strategies, and vehicle characteristics and mileage. Particles in the nucleation mode consisted of ammonium bisulfate, sulfate and sulfuric acid, suggesting that the catalyst desulfation is the key process in the formation of UFPs. Larger particles and agglomerates, ranging from 90 to 600 nm, consisted of carbonaceous material (soot and soot aggregates) coated by condensable material including organics, ammonium bisulfate and sulfuric acid. Particle emission in the accumulation mode was due to the reduced filtration efficiency (soot cake oxidation) throughout the regeneration process.

Investigation of soot oxidation by coupling LII, SAXS and scattering measurements

This work presents an in-situ characterization of the oxidation of soot particles in flames by coupling three different techniques. Small Angle X-ray Scattering and Static Light Scattering were used in order to provide information on the size of the primary spheres and the aggregates respectively. Laser Induced Incandescence was also used to determine the soot volume fraction in the flame. Flame temperatures and soot residence time were also determined. These techniques were combined to provide a complete description of the impact of the oxidation process on soot aggregates (aggregate and primary sphere densities, size distributions). In order to limit the phenomena to oxidation, soot was generated upstream by a miniCAST generator and injected into a non-sooting flame. Amongst other results, it is shown that primary sphere diameter reduction is accompanied by an increase of the geometric standard deviation. This effect can be modeled by considering the transition from a volume (diffusion) to a surface (reaction) oxidation process.

Characteristics of individual particles in Beijing before, during and after the 2014 APEC meeting

To understand the characteristics of individual aerosol particles as well as the effects of emission control measures on the air quality in Beijing before, during and after the 2014 APEC meeting, aerosol samples collected in Beijing from Oct. 8 to Nov. 24 were investigated by a scanning electron microscopy (SEM) coupled with an energy-dispersive X-ray (EDX). Individual particles were classified into fly ash, ammonium sulfate, carbonaceous particle, tar ball, soot aggregates, Fe/Ti oxide, Ca/Mg carbonate, calcium sulfate and aluminosilicates/quartz. The results showed that PM0.5–1.0 was predominant in aerosol particles while PM2.5–10 was the fewest in aerosol particles. Soot aggregates and carbonaceous particles mainly located in the size range of 0.5–2.5μm and mineral particles were dominant in the size range of 2.5–10μm. The tough emission control measures taken by the local government greatly improved the air quality. Reducing vehicles on the roads substantially decreased the amount of soot aggregates, and restricting coal combustion decreased the amount of tar ball during the APEC meeting. The concentrations of carbonaceous and mineral particles abated probably owing to the control on VOCs emission, and water spray and demolition layoff, respectively, during the APEC meeting.