Highly time-resolved urban aerosol characteristics during springtime in Yangtze River Delta, China: insights from soot particle aerosol mass spectrometry

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J. Wang

2016-07-01

Full Text Available In this work, the Aerodyne soot particle – aerosol mass spectrometer (SP-AMS was deployed for the first time during the spring of 2015 in urban Nanjing, a megacity in the Yangtze River Delta (YRD of China, for online characterization of the submicron aerosols (PM1. The SP-AMS enables real-time and fast quantification of refractory black carbon (rBC simultaneously with other non-refractory species (ammonium, sulfate, nitrate, chloride, and organics. The average PM1 concentration was found to be 28.2 µg m−3, with organics (45 % as the most abundant component, following by sulfate (19.3 %, nitrate (13.6 %, ammonium (11.1 %, rBC (9.7 %, and chloride (1.3 %. These PM1 species together can reconstruct ∼ 44 % of the light extinction during this campaign based on the IMPROVE method. Chemically resolved mass-based size distributions revealed that small particles especially ultrafine ones (< 100 nm vacuum aerodynamic diameter were dominated by organics and rBC, while large particles had significant contributions from secondary inorganic species. Source apportionment of organic aerosols (OA yielded four OA subcomponents, including hydrocarbon-like OA (HOA, cooking-related OA (COA, semi-volatile oxygenated OA (SV-OOA, and low-volatility oxygenated OA (LV-OOA. Overall, secondary organic aerosol (SOA, equal to the sum of SV-OOA and LV-OOA dominated the total OA mass (55.5 %, but primary organic aerosol (POA, equal to the sum of HOA and COA can outweigh SOA in the early morning and evening due to enhanced human activities. High OA concentrations were often associated with high mass fractions of POA and rBC, indicating the important role of anthropogenic emissions during heavy pollution events. The diurnal cycles of nitrate, chloride, and SV-OOA both showed good anti-correlations with air temperatures, suggesting their variations were likely driven by thermodynamic equilibria and gas-to-particle partitioning. On the other hand

Ice Nucleation of Soot Particles in the Cirrus Regime: Is Pore Condensation and Freezing Relevant for Soot?

Science.gov (United States)

Kanji, Z. A.; Mahrt, F.; David, R.; Marcolli, C.; Lohmann, U.; Fahrni, J.; Brühwiler, D.

2017-12-01

Heterogeneous ice nucleation (HIN) onto soot particles from previous studies have produced inconsistent results of temperature and relative humidity conditions required for freezing depending on the source of soot particle investigated. The ability of soot to act as HIN depended on the type of soot and size of particle. Often homogenous freezing conditions or water saturation conditions were required to freeze soot particles, rendering HIN irrelevant. Using synthesised mesoporous silica particles, we show pore condensation and freezing works with experiments performed in the Zurich Ice Nucleation Chamber (ZINC). By testing a variety of soot particles in parallel in the Horizontal Ice Nucleation Chamber (HINC), we suggest that previously observed HIN on soot particles is not the responsible mechanism for ice formation. Laboratory generated CAST brown and black soot, commercially available soot and acid treated soot were investigated for their ice nucleation abilities in the mixed-phase and cirrus cloud temperature regimes. No heterogeneous ice nucleation activity is inferred at T > -38 °C (mixed-phase cloud regime), however depending on particle size and soot type, HIN was observed for T nucleation of ice in the pores or cavities that are ubiquitous in soot particles between the primary spherules. The ability of some particles to freeze at lower relative humidity compared to others demonstrates why hydrophobicity plays a role in ice nucleation, i.e. controlling the conditions at which these cavities fill with water. Thus for more hydrophobic particles pore filling occurs at higher relative humidity, and therefore freezing of pore water and ice crystal growth. Future work focusses on testing the cloud processing ability of soot particles and water adsorption isotherms of the different soot samples to support the hydrophobicity inferences from the ice nucleation results.

Highly time-resolved urban aerosol characteristics during springtime in Yangtze River Delta, China: insights from soot particle aerosol mass spectrometry

Science.gov (United States)

Wang, Junfeng; Ge, Xinlei; Chen, Yanfang; Shen, Yafei; Zhang, Qi; Sun, Yele; Xu, Jianzhong; Ge, Shun; Yu, Huan; Chen, Mindong

2016-07-01

In this work, the Aerodyne soot particle - aerosol mass spectrometer (SP-AMS) was deployed for the first time during the spring of 2015 in urban Nanjing, a megacity in the Yangtze River Delta (YRD) of China, for online characterization of the submicron aerosols (PM1). The SP-AMS enables real-time and fast quantification of refractory black carbon (rBC) simultaneously with other non-refractory species (ammonium, sulfate, nitrate, chloride, and organics). The average PM1 concentration was found to be 28.2 µg m-3, with organics (45 %) as the most abundant component, following by sulfate (19.3 %), nitrate (13.6 %), ammonium (11.1 %), rBC (9.7 %), and chloride (1.3 %). These PM1 species together can reconstruct ˜ 44 % of the light extinction during this campaign based on the IMPROVE method. Chemically resolved mass-based size distributions revealed that small particles especially ultrafine ones (cooking-related OA (COA), semi-volatile oxygenated OA (SV-OOA), and low-volatility oxygenated OA (LV-OOA). Overall, secondary organic aerosol (SOA, equal to the sum of SV-OOA and LV-OOA) dominated the total OA mass (55.5 %), but primary organic aerosol (POA, equal to the sum of HOA and COA) can outweigh SOA in the early morning and evening due to enhanced human activities. High OA concentrations were often associated with high mass fractions of POA and rBC, indicating the important role of anthropogenic emissions during heavy pollution events. The diurnal cycles of nitrate, chloride, and SV-OOA both showed good anti-correlations with air temperatures, suggesting their variations were likely driven by thermodynamic equilibria and gas-to-particle partitioning. On the other hand, in contrast to other species, sulfate, and LV-OOA concentrations increased in the afternoon, and showed no positive correlations with relative humidity (RH), likely indicating the contribution from photochemical oxidation is dominant over that of aqueous-phase processing for their formations. The

T-matrix modeling of linear depolarization by morphologically complex soot and soot-containing aerosols

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Mishchenko, Michael I.; Liu, Li; Mackowski, Daniel W.

2013-07-01

We use state-of-the-art public-domain Fortran codes based on the T-matrix method to calculate orientation and ensemble averaged scattering matrix elements for a variety of morphologically complex black carbon (BC) and BC-containing aerosol particles, with a special emphasis on the linear depolarization ratio (LDR). We explain theoretically the quasi-Rayleigh LDR peak at side-scattering angles typical of low-density soot fractals and conclude that the measurement of this feature enables one to evaluate the compactness state of BC clusters and trace the evolution of low-density fluffy fractals into densely packed aggregates. We show that small backscattering LDRs measured with ground-based, airborne, and spaceborne lidars for fresh smoke generally agree with the values predicted theoretically for fluffy BC fractals and densely packed near-spheroidal BC aggregates. To reproduce higher lidar LDRs observed for aged smoke, one needs alternative particle models such as shape mixtures of BC spheroids or cylinders.

Fragmentation and bond strength of airborne diesel soot agglomerates

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Messerer Armin

2008-06-01

Full Text Available Abstract Background The potential of diesel soot aerosol particles to break up into smaller units under mechanical stress was investigated by a direct impaction technique which measures the degree of fragmentation of individual agglomerates vs. impact energy. Diesel aerosol was generated by an idling diesel engine used for passenger vehicles. Both the aerosol emitted directly and aerosol that had undergone additional growth by Brownian coagulation ("aging" was investigated. Optionally a thermo-desoption technique at 280°C was used to remove all high-volatility and the majority of low-volatility HC adsorbates from the aerosol before aging. Results It was found that the primary soot agglomerates emitted directly from the engine could not be fragmented at all. Soot agglomerates permitted to grow additionally by Brownian coagulation of the primary emitted particles could be fragmented to a maximum of 75% and 60% respectively, depending on whether adsorbates were removed from their surface prior to aging or not. At most, these aged agglomerates could be broken down to roughly the size of the agglomerates from the primary emission. The energy required for a 50% fragmentation probability of all bonds within an agglomerate was reduced by roughly a factor of 2 when aging "dry" agglomerates. Average bond energies derived from the data were 0.52*10-16 and 1.2*10-16 J, respectively. This is about 2 orders of magnitude higher than estimates for pure van-der-Waals agglomerates, but agrees quite well with other observations. Conclusion Although direct conclusions regarding the behavior of inhaled diesel aerosol in contact with body fluids cannot be drawn from such measurements, the results imply that highly agglomerated soot aerosol particles are unlikely to break up into units smaller than roughly the size distribution emitted as tail pipe soot.

Fragmentation and bond strength of airborne diesel soot agglomerates

Science.gov (United States)

Rothenbacher, Sonja; Messerer, Armin; Kasper, Gerhard

2008-01-01

Background The potential of diesel soot aerosol particles to break up into smaller units under mechanical stress was investigated by a direct impaction technique which measures the degree of fragmentation of individual agglomerates vs. impact energy. Diesel aerosol was generated by an idling diesel engine used for passenger vehicles. Both the aerosol emitted directly and aerosol that had undergone additional growth by Brownian coagulation ("aging") was investigated. Optionally a thermo-desoption technique at 280°C was used to remove all high-volatility and the majority of low-volatility HC adsorbates from the aerosol before aging. Results It was found that the primary soot agglomerates emitted directly from the engine could not be fragmented at all. Soot agglomerates permitted to grow additionally by Brownian coagulation of the primary emitted particles could be fragmented to a maximum of 75% and 60% respectively, depending on whether adsorbates were removed from their surface prior to aging or not. At most, these aged agglomerates could be broken down to roughly the size of the agglomerates from the primary emission. The energy required for a 50% fragmentation probability of all bonds within an agglomerate was reduced by roughly a factor of 2 when aging "dry" agglomerates. Average bond energies derived from the data were 0.52*10-16 and 1.2*10-16 J, respectively. This is about 2 orders of magnitude higher than estimates for pure van-der-Waals agglomerates, but agrees quite well with other observations. Conclusion Although direct conclusions regarding the behavior of inhaled diesel aerosol in contact with body fluids cannot be drawn from such measurements, the results imply that highly agglomerated soot aerosol particles are unlikely to break up into units smaller than roughly the size distribution emitted as tail pipe soot. PMID:18533015

Evaluation of a Lagrangian Soot Tracking Method for the prediction of primary soot particle size under engine-like conditions

DEFF Research Database (Denmark)

Cai Ong, Jiun; Pang, Kar Mun; Walther, Jens Honore

2018-01-01

This paper reports the implementation and evaluation of a Lagrangian soot tracking (LST) method for the modeling of soot in diesel engines. The LST model employed here has the tracking capability of a Lagrangian method and the ability to predict primary soot particle sizing. The Moss-Brookes soot...... in predicting temporal soot cloud development, mean soot diameter and primary soot size distribution is evaluated using measurements of n-heptane and n-dodecane spray combustion obtained under diesel engine-like conditions. In addition, sensitivity studies are carried out to investigate the influence of soot....... A higher rate of soot oxidation due to OH causes the soot particles to be fully oxidized downstream of the flame. In general, the LST model performs better than the Eulerian method in terms of predicting soot sizing and accessing information of individual soot particles, both of which are shortcomings...

The competition between mineral dust and soot ice nuclei in mixed-phase clouds (Invited)

Science.gov (United States)

Murray, B. J.; Atkinson, J.; Umo, N.; Browse, J.; Woodhouse, M. T.; Whale, T.; Baustian, K. J.; Carslaw, K. S.; Dobbie, S.; O'Sullivan, D.; Malkin, T. L.

2013-12-01

The amount of ice present in mixed-phase clouds, which contain both supercooled liquid water droplets and ice particles, affects cloud extent, lifetime, particle size and radiative properties. The freezing of cloud droplets can be catalysed by the presence of aerosol particles known as ice nuclei. In this talk our recent laboratory and global aerosol modelling work on mineral dust and soot ice nuclei will be presented. We have performed immersion mode experiments to quantify ice nucleation by the individual minerals which make up desert mineral dusts and have shown that the feldspar component, rather than the clay component, is most important for ice nucleation (Atkinson et al. 2013). Experiments with well-characterised soot generated with eugenol, an intermediate in biomass burning, and n-decane show soot has a significant ice nucleation activity in mixed-phase cloud conditions. Our results for soot are in good agreement with previous results for acetylene soot (DeMott, 1990), but extend the efficiency to much higher temperatures. We then use a global aerosol model (GLOMAP) to map the distribution of soot and feldspar particles on a global basis. We show that below about -15oC that dust and soot together can explain most observed ice nuclei in the Earth's atmosphere, while at warmer temperatures other ice nuclei types are needed. We show that in some regions soot is the most important ice nuclei (below -15oC), while in others feldspar dust dominates. Our results suggest that there is a strong anthropogenic contribution to the ice nuclei population, since a large proportion of soot aerosol in the atmosphere results from human activities. Atkinson, J. D., Murray, B. J., Woodhouse, M. T., Carslaw, K. S., Whale, T. F., Baustian, K. J., Dobbie, S., O'Sullivan, D., and Malkin, T. L.: The importance of feldspar for ice nucleation by mineral dust in mixed-phase clouds, Nature, 10.1038/nature12278, (2013). Demott, P. J. 1990. An Exploratory-Study of Ice Nucleation by Soot

Combustion characteristics of water-insoluble elemental and organic carbon in size selected ambient aerosol particles

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K. Wittmaack

2005-01-01

Full Text Available Combustion of elemental carbon (EC and organic carbon (OC contained in ambient aerosol matter was explored using scanning electron microscopy (SEM in combination with energy dispersive X-ray analysis (EDX. To ease identification of the particles of interest and to avoid or at least reduce interaction with simultaneously sampled inorganic oxides and salts, the approach used in this work differed in two ways from commonly applied procedures. First, rather than using a mixture of particles of vastly different sizes, as in PM10 or PM2.5, aerosol matter was collected in a 5-stage impactor. Second, the water soluble fraction of the collected matter was removed prior to analysis. Diesel soot particles, which appeared in the well-known form of chain-type aggregates, constituted the major fraction of EC. In contrast, OC containing particles were observed in a variety of shapes, including a sizable amount of bioaerosol matter appearing mostly in the size range above about 1 µm. During heating in ambient air for 1h, diesel soot particles were found to be stable up to 470°C, but complete combustion occurred in a narrow temperature interval between about 480 and 510°C. After diesel soot combustion, minute quantities of 'ash' were observed in the form of aggregated tiny particles with sizes less than 10 nm. These particles could be due to elemental or oxidic contaminants of diesel soot. Combustion of OC was observed over a wide range of temperatures, from well below 200°C to at least 500°C. Incompletely burnt bioaerosol matter was still found after heating to 600°C. The results imply that the EC fraction in aerosol matter can be overestimated significantly if the contribution of OC to a thermogram is not well separated.

Thermal fragmentation and deactivation of combustion-generated soot particles

KAUST Repository

Raj, Abhijeet

2014-09-01

The effect of thermal treatment on diesel soot and on a commercial soot in an inert environment under isothermal conditions at intermediate temperatures (400-900°C) is studied. Two important phenomena are observed in both the soot samples: soot fragmentation leading to its mass loss, and loss of soot reactivity towards O2. Several experimental techniques such as high resolution transmission electron microscopy, electron energy loss spectroscopy, thermo-gravimetric analysis with mass spectrometry, elemental analysis, Fourier transform infrared spectroscopy and X-ray diffraction have been used to identify the changes in structures, functional groups such as oxygenates and aliphatics, σ and π bonding, O/C and H/C ratios, and crystallite parameters of soot particles, introduced by heat. A decrease in the size of primary particles and an increase in the average polycyclic aromatic hydrocarbon (PAH) size was observed in soots after thermal treatment. The activation energies of soot oxidation for thermally treated soot samples were found to be higher than those for the untreated ones at most conversion levels. The cyclic or acyclic aliphatics with sp3 hybridization were present in significant amounts in all the soot samples, but their concentration decreased with thermal treatment. Interestingly, the H/C and the O/C ratios of soot particles increased after thermal treatment, and thus, they do not support the decrease in soot reactivity. The increase in the concentration of oxygenates on soot surface indicate that their desorption from soot surface in the form of CO, CO2 and other oxygenated compounds may not be significant at the temperatures (400-900°C) studied in this work. © 2014 The Combustion Institute.

Effective Density and Mixing State of Aerosol Particles in a Near-Traffic Urban Environment

DEFF Research Database (Denmark)

Rissler, Jenny; Nordin, Erik Z; Eriksson, Axel C

2014-01-01

-range transport from polluted continental areas. The effective density of each group was relatively stable over time, especially of the soot aggregates, which had effective densities similar to those observed in laboratory studies of fresh diesel exhaust emissions. When heated to 300 °C, the soot aggregate......In urban environments, airborne particles are continuously emitted, followed by atmospheric aging. Also, particles emitted elsewhere, transported by winds, contribute to the urban aerosol. We studied the effective density (mass-mobility relationship) and mixing state with respect to the density...... and more dense particles. Both groups were present at each size in varying proportions. Two types of temporal variability in the relative number fraction of the two groups were found: soot correlated with intense traffic in a diel pattern and dense particles increased during episodes with long...

Soot in the air may have serious climatic consequences

International Nuclear Information System (INIS)

Seip, Hans Martin

2002-01-01

Emissions of soot in China and India may be an important cause of changed summer weather in China, with increasing floods in the south-east and increasing droughts in the north-east. In addition to the greenhouse gases, the particulate matter (aerosols) in the air has an important effect on the climate. Most particles have a cooling effect since they reflect solar radiation. However, some particles are dark as they contain soot ('black carbon'). Such particles, which are formed by incomplete combustion of coal, oil and biomass, absorb solar radiation and thus have a warming effect, even if they reduce the solar irradiation on the ground. Soot particles do not have quite the same effect as the greenhouse gases. The soot particles absorb solar radiation, while the greenhouse gases absorb terrestrial heat radiation. In addition, the residence time of the soot particles in the atmosphere is shorter than that of, say, carbon dioxide. The concentration is therefore much higher in areas close to emission sources than elsewhere

Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

Energy Technology Data Exchange (ETDEWEB)

Davidovits, Paul [Boston College, Chestnut Hill, MA (United States)

2015-10-20

) two well-characterized source of soot particles and (b) a flow reactor for controlled OH and/or O3 oxidation of relevant gas phase species to produce well-characterized SOA particles. After formation, the aerosol particles are subjected to physical and chemical processes that simulate aerosol growth and aging. A suite of instruments in our laboratory is used to characterize the physical and chemical properties of aerosol particles before and after processing. The Time of Flight Aerosol Mass Spectrometer (ToF-AMS) together with a Scanning Mobility Particle Sizer (SMPS) measures particle mass, volume, density, composition (including black carbon content), dynamic shape factor, and fractal dimension. The–ToF-AMS was developed at ARI with Boston College participation. About 120 AMS instruments are now in service (including 5 built for DOE laboratories) performing field and laboratory studies world-wide. Other major instruments include a thermal denuder, two Differential Mobility Analyzers (DMA), a Cloud Condensation Nuclei Counter (CCN), a Thermal desorption Aerosol GC/MS (TAG) and the new Soot Particle Aerosol Mass Spectrometer (SP-AMS). Optical instrumentation required for the studies have been brought to our laboratory as part of ongoing and planned collaborative projects with colleagues from DOE, NOAA and university laboratories. Optical instruments that will be utilized include a Photoacoustic Spectrometer (PAS), a Cavity Ring Down Aerosol Extinction Spectrometer (CRD-AES), a Photo Thermal Interferometer (PTI), a new 7-wavelength Aethalometer and a Cavity Attenuated Phase Shift Extinction Monitor (CAPS). These instruments are providing aerosol absorption, extinction and scattering coefficients at a range of atmospherically relevant wavelengths. During the past two years our work has continued along the lines of our original proposal. We report on 12 completed and/or continuing projects conducted during the period 08/14 to 0814/2015. These projects are described in

Aerosol particle mixing state, refractory particle number size distributions and emission factors in a polluted urban environment: Case study of Metro Manila, Philippines

Science.gov (United States)

Kecorius, Simonas; Madueño, Leizel; Vallar, Edgar; Alas, Honey; Betito, Grace; Birmili, Wolfram; Cambaliza, Maria Obiminda; Catipay, Grethyl; Gonzaga-Cayetano, Mylene; Galvez, Maria Cecilia; Lorenzo, Genie; Müller, Thomas; Simpas, James B.; Tamayo, Everlyn Gayle; Wiedensohler, Alfred

2017-12-01

Ultrafine soot particles (black carbon, BC) in urban environments are related to adverse respiratory and cardiovascular effects, increased cases of asthma and premature deaths. These problems are especially pronounced in developing megacities in South-East Asia, Latin America, and Africa, where unsustainable urbanization ant outdated environmental protection legislation resulted in severe degradation of urban air quality in terms of black carbon emission. Since ultrafine soot particles do often not lead to enhanced PM10 and PM2.5 mass concentration, the risks related to ultrafine particle pollution may therefore be significantly underestimated compared to the contribution of secondary aerosol constituents. To increase the awareness of the potential toxicological relevant problems of ultrafine black carbon particles, we conducted a case study in Metro Manila, the capital of the Philippines. Here, we present a part of the results from a detailed field campaign, called Manila Aerosol Characterization Experiment (MACE, 2015). Measurements took place from May to June 2015 with the focus on the state of mixing of aerosol particles. The results were alarming, showing the abundance of externally mixed refractory particles (soot proxy) at street site with a maximum daily number concentration of approximately 15000 #/cm3. That is up to 10 times higher than in cities of Western countries. We also found that the soot particle mass contributed from 55 to 75% of total street site PM2.5. The retrieved refractory particle number size distribution appeared to be a superposition of 2 ultrafine modes at 20 and 80 nm with a corresponding contribution to the total refractory particle number of 45 and 55%, respectively. The particles in the 20 nm mode were most likely ash from metallic additives in lubricating oil, tiny carbonaceous particles and/or nucleated and oxidized organic polymers, while bigger ones (80 nm) were soot agglomerates. To the best of the authors' knowledge, no other

Wintertime hygroscopicity and volatility of ambient urban aerosol particles

Science.gov (United States)

Enroth, Joonas; Mikkilä, Jyri; Németh, Zoltán; Kulmala, Markku; Salma, Imre

2018-04-01

Hygroscopic and volatile properties of atmospheric aerosol particles with dry diameters of (20), 50, 75, 110 and 145 nm were determined in situ by using a volatility-hygroscopicity tandem differential mobility analyser (VH-TDMA) system with a relative humidity of 90 % and denuding temperature of 270 °C in central Budapest during 2 months in winter 2014-2015. The probability density function of the hygroscopic growth factor (HGF) showed a distinct bimodal distribution. One of the modes was characterised by an overall mean HGF of approximately 1.07 (this corresponds to a hygroscopicity parameter κ of 0.033) independently of the particle size and was assigned to nearly hydrophobic (NH) particles. Its mean particle number fraction was large, and it decreased monotonically from 69 to 41 % with particle diameter. The other mode showed a mean HGF increasing slightly from 1.31 to 1.38 (κ values from 0.186 to 0.196) with particle diameter, and it was attributed to less hygroscopic (LH) particles. The mode with more hygroscopic particles was not identified. The probability density function of the volatility GF (VGF) also exhibited a distinct bimodal distribution with an overall mean VGF of approximately 0.96 independently of the particle size, and with another mean VGF increasing from 0.49 to 0.55 with particle diameter. The two modes were associated with less volatile (LV) and volatile (V) particles. The mean particle number fraction for the LV mode decreased from 34 to 21 % with particle diameter. The bimodal distributions indicated that the urban atmospheric aerosol contained an external mixture of particles with a diverse chemical composition. Particles corresponding to the NH and LV modes were assigned mainly to freshly emitted combustion particles, more specifically to vehicle emissions consisting of large mass fractions of soot likely coated with or containing some water-insoluble organic compounds such as non-hygroscopic hydrocarbon-like organics. The hygroscopic

Morphology, Composition, and Mixing State of Individual Aerosol Particles in Northeast China during Wintertime

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Liang Xu

2017-02-01

Full Text Available Northeast China is located in a high latitude area of the world and undergoes a cold season that lasts six months each year. Recently, regional haze episodes with high concentrations of fine particles (PM2.5 have frequently been occurring in Northeast China during the heating period, but little information has been available. Aerosol particles were collected in winter at a site in a suburban county town (T1 and a site in a background rural area (T2. Morphology, size, elemental composition, and mixing state of individual aerosol particles were characterized by transmission electron microscopy (TEM. Aerosol particles were mainly composed of organic matter (OM and S-rich and certain amounts of soot and K-rich. OM represented the most abundant particles, accounting for 60.7% and 53.5% at the T1 and T2 sites, respectively. Abundant spherical OM particles were likely emitted directly from coal-burning stoves. Soot decreased from 16.9% at the T1 site to 4.6% at the T2 site and sulfate particles decrease from 35.9% at the T2 site to 15.7% at the T1 site, suggesting that long-range transport air masses experienced more aging processes and produced more secondary particles. Based on our investigations, we proposed that emissions from coal-burning stoves in most rural areas of the west part of Northeast China can induce regional haze episodes.

Sensitivity of the Single Particle Soot Photometer to different black carbon types

Science.gov (United States)

Laborde, M.; Mertes, P.; Zieger, P.; Dommen, J.; Baltensperger, U.; Gysel, M.

2012-05-01

Black carbon (BC) is now mainly of anthropogenic origin. It is the dominant light absorbing component of atmospheric aerosols, playing an important role in the earth's radiative balance and therefore relevant to climate change studies. In addition, BC is known to be harmful to human beings making it relevant to policy makers. Nevertheless, the measurement of BC remains biased by the instrument-based definition of BC. The Single Particle Soot Photometer (SP2), allows the measurement of the refractory BC (rBC) mass of individual particles using laser-induced incandescence. However, the SP2 needs an empirical calibration to retrieve the rBC mass from the incandescence signal and the sensitivity of the SP2 differs between different BC types. Ideally, for atmospheric studies, the SP2 should be calibrated using ambient particles containing a known mass of ambient rBC. However, such "ambient BC" calibration particles cannot easily be obtained and thus commercially available BC particles are commonly used for SP2 calibration instead. In this study we tested the sensitivity of the SP2 to different BC types in order to characterize the potential error introduced by using non-ambient BC for calibration. The sensitivity of the SP2 was determined, using an aerosol particle mass analyzer, for rBC from thermodenuded diesel exhaust, wood burning exhaust and ambient particles as well as for commercially available products: Aquadag® and fullerene soot. Thermodenuded, fresh diesel exhaust has been found to be ideal for SP2 calibration for two reasons. First, the small amount of non-BC matter upon emission reduces the risk of bias due to incomplete removal of non-BC matter and second, it is considered to represent atmospheric rBC in urban locations where diesel exhaust is the main source of BC. The SP2 was found to be up to 16% less sensitive to rBC from thermodenuded ambient particles (≤15 fg) than rBC from diesel exhaust, however, at least part of this difference can be explained

Sensitivity of the Single Particle Soot Photometer to different black carbon types

Directory of Open Access Journals (Sweden)

M. Laborde

2012-05-01

Full Text Available Black carbon (BC is now mainly of anthropogenic origin. It is the dominant light absorbing component of atmospheric aerosols, playing an important role in the earth's radiative balance and therefore relevant to climate change studies. In addition, BC is known to be harmful to human beings making it relevant to policy makers. Nevertheless, the measurement of BC remains biased by the instrument-based definition of BC. The Single Particle Soot Photometer (SP2, allows the measurement of the refractory BC (rBC mass of individual particles using laser-induced incandescence. However, the SP2 needs an empirical calibration to retrieve the rBC mass from the incandescence signal and the sensitivity of the SP2 differs between different BC types. Ideally, for atmospheric studies, the SP2 should be calibrated using ambient particles containing a known mass of ambient rBC. However, such "ambient BC" calibration particles cannot easily be obtained and thus commercially available BC particles are commonly used for SP2 calibration instead. In this study we tested the sensitivity of the SP2 to different BC types in order to characterize the potential error introduced by using non-ambient BC for calibration. The sensitivity of the SP2 was determined, using an aerosol particle mass analyzer, for rBC from thermodenuded diesel exhaust, wood burning exhaust and ambient particles as well as for commercially available products: Aquadag^® and fullerene soot.

Thermodenuded, fresh diesel exhaust has been found to be ideal for SP2 calibration for two reasons. First, the small amount of non-BC matter upon emission reduces the risk of bias due to incomplete removal of non-BC matter and second, it is considered to represent atmospheric rBC in urban locations where diesel exhaust is the main source of BC. The SP2 was found to be up to 16% less sensitive to rBC from thermodenuded ambient particles (≤15 fg than rBC from diesel exhaust, however, at least part

Nanoparticle production by UV irradiation of combustion generated soot particles

International Nuclear Information System (INIS)

Stipe, Christopher B.; Choi, Jong Hyun; Lucas, Donald; Koshland, Catherine P.; Sawyer, Robert F.

2004-01-01

Laser ablation of surfaces normally produce high temperature plasmas that are difficult to control. By irradiating small particles in the gas phase, we can better control the size and concentration of the resulting particles when different materials are photofragmented. Here, we irradiate soot with 193 nm light from an ArF excimer laser. Irradiating the original agglomerated particles at fluences ranging from 0.07 to 0.26 J/cm 2 with repetition rates of 20 and 100 Hz produces a large number of small, unagglomerated particles, and a smaller number of spherical agglomerated particles. Mean particle diameters from 20 to 50 nm are produced from soot originally having a mean electric mobility diameter of 265nm. We use a non-dimensional parameter, called the photon/atom ratio (PAR), to aid in understanding the photofragmentation process. This parameter is the ratio of the number of photons striking the soot particles to the number of the carbon atoms contained in the soot particles, and is a better metric than the laser fluence for analyzing laser-particle interactions. These results suggest that UV photofragmentation can be effective in controlling particle size and morphology, and can be a useful diagnostic for studying elements of the laser ablation process

Buildup of aerosol precursor gases and sulfur-induced activation of soot in nascent jet aircraft exhaust plumes

Energy Technology Data Exchange (ETDEWEB)

Kaercher, B.; Hirschberg, M.M.; Fabian, P. [Muenchen Univ. (Germany). Lehrstuhl fuer Bioklimatologie und Immissionsforschung; Gerz, T. [Deutsche Forschungsanstalt fuer Luft- und Raumfahrt e.V. (DLR), Oberpfaffenhofen (Germany). Inst. fuer Physik der Atmosphaere

1997-12-31

Research issues concerning the chemical transformation of exhaust trace gases are summarized. The photochemical evolution of NO{sub x} early in the plume is strongly coupled to plume mixing. Substantial amounts of HNO{sub 3} are generated in nascent plumes even if no NO{sub 2} is emitted. The production of H{sub 2}SO{sub 4} becomes very efficient if part of the fuel sulfur is emitted as SO{sub 3}. Each emitted soot particle can acquire 1-10% by mass fully oxidized sulfur molecules prior to binary homogeneous nucleation, if a few percent of the exhaust SO{sub x} are emitted as SO{sub 3}, indicating an important activation pathway for soot, and leading to a marked enhancement of new aerosol formation and growth rates. (author) 11 refs.

Buildup of aerosol precursor gases and sulfur-induced activation of soot in nascent jet aircraft exhaust plumes

Energy Technology Data Exchange (ETDEWEB)

Kaercher, B; Hirschberg, M M; Fabian, P [Muenchen Univ. (Germany). Lehrstuhl fuer Bioklimatologie und Immissionsforschung; Gerz, T [Deutsche Forschungsanstalt fuer Luft- und Raumfahrt e.V. (DLR), Oberpfaffenhofen (Germany). Inst. fuer Physik der Atmosphaere

1998-12-31

Research issues concerning the chemical transformation of exhaust trace gases are summarized. The photochemical evolution of NO{sub x} early in the plume is strongly coupled to plume mixing. Substantial amounts of HNO{sub 3} are generated in nascent plumes even if no NO{sub 2} is emitted. The production of H{sub 2}SO{sub 4} becomes very efficient if part of the fuel sulfur is emitted as SO{sub 3}. Each emitted soot particle can acquire 1-10% by mass fully oxidized sulfur molecules prior to binary homogeneous nucleation, if a few percent of the exhaust SO{sub x} are emitted as SO{sub 3}, indicating an important activation pathway for soot, and leading to a marked enhancement of new aerosol formation and growth rates. (author) 11 refs.

Application of a robust and efficient Lagrangian particle scheme to soot transport in turbulent flames

KAUST Repository

Attili, Antonio

2013-09-01

A Lagrangian particle scheme is applied to the solution of soot dynamics in turbulent nonpremixed flames. Soot particulate is described using a method of moments and the resulting set of continuum advection-reaction equations is solved using the Lagrangian particle scheme. The key property of the approach is the independence between advection, described by the movement of Lagrangian notional particles along pathlines, and internal aerosol processes, evolving on each notional particle via source terms. Consequently, the method overcomes the issues in Eulerian grid-based schemes for the advection of moments: errors in the advective fluxes pollute the moments compromising their realizability and the stiffness of source terms weakens the stability of the method. The proposed scheme exhibits superior properties with respect to conventional Eulerian schemes in terms of stability, accuracy, and grid convergence. Taking into account the quality of the solution, the Lagrangian approach can be computationally more economical than commonly used Eulerian schemes as it allows the resolution requirements dictated by the different physical phenomena to be independently optimized. Finally, the scheme posseses excellent scalability on massively parallel computers. © 2013 Elsevier Ltd.

Fractal-like dimension of nanometer Diesel soot particles

Energy Technology Data Exchange (ETDEWEB)

Skillas, G.; Baltensperger, U. [Paul Scherrer Inst. (PSI), Villigen (Switzerland); Siegmann, K. [Eidgenoessische Technische Hochschule, Zurich (Switzerland)

1997-11-01

Measurements with a low-pressure impactor and a differential mobility analyser were conducted for Diesel soot at various engine loads. By means of these measurements a fractal-like dimension of Diesel soot particles, with diameters ranging from 55 up to 260 nm, was established. (author) 2 figs., 7 refs.

Soot particle size measurements in ethylene diffusion flames at elevated pressures

KAUST Repository

Steinmetz, Scott

2016-05-07

Soot particle size is investigated in laminar nitrogen-diluted ethylene coflow diffusion flames at 4, 8, 12 and 16 atm. Line of sight attenuation and scattering are used to measure two-dimensional soot volume fraction and particle size fields for the first time at elevated pressures. Soot volume fraction dependence on pressure is consistent with the observations of similar studies, scaling approximately with the square of pressure. Scattering intensity is analyzed through Rayleigh and Rayleigh-Debye-Gans polydisperse fractal aggregate theories to provide two estimates of particle size. An increase in overall particle sizes with pressure is found, consistent with similar one-dimensional studies. Particle diameters in the annulus of the flame increase faster with pressure than those on centerline. Contrary to previous studies, the dependence of particle size on pressure was found to taper off between 8 and 12 atm, with little observed growth beyond 12 atm. The measurements provide additional data for one of the International Sooting Flame (ISF) workshop\\'s target pressurized flames.

An in situ cell to study phase transitions in individual aerosol particles on a substrate using scanning transmission x-ray microspectroscopy

International Nuclear Information System (INIS)

Huthwelker, T.; Zelenay, V.; Birrer, M.; Krepelova, A.; Raabe, J.; Ammann, M.; Tzvetkov, G.; Vernooij, M. G. C.

2010-01-01

A new in situ cell to study phase transitions and chemical processes on individual aerosol particles in the x-ray transmission microscope at the PolLux beamline of the Swiss light source has been built. The cell is machined from stainless steel and aluminum components and is designed to be used in the standard mount of the microscope without need of complicated rearrangements of the microscope. The cell consists of two parts, a back part which contains connections for the gas supply, heating, cooling devices, and temperature measurement. The second part is a removable clip, which hosts the sample. This clip can be easily exchanged and brought into a sampling unit for aerosol particles. Currently, the cell can be operated at temperatures ranging from -40 to +50 deg. C. The function of the cell is demonstrated using two systems of submicron size: inorganic sodium bromide aerosols and soot originating from a diesel passenger car. For the sodium bromide we demonstrate how phase transitions can be studied in these systems and that O1s spectra from aqueous sodium bromide solution can be taken from submicron sized particles. For the case of soot, we demonstrate that the uptake of water onto individual soot particles can be studied.

Wintertime hygroscopicity and volatility of ambient urban aerosol particles

Directory of Open Access Journals (Sweden)

J. Enroth

2018-04-01

Full Text Available Hygroscopic and volatile properties of atmospheric aerosol particles with dry diameters of (20, 50, 75, 110 and 145 nm were determined in situ by using a volatility–hygroscopicity tandem differential mobility analyser (VH-TDMA system with a relative humidity of 90 % and denuding temperature of 270 °C in central Budapest during 2 months in winter 2014–2015. The probability density function of the hygroscopic growth factor (HGF showed a distinct bimodal distribution. One of the modes was characterised by an overall mean HGF of approximately 1.07 (this corresponds to a hygroscopicity parameter κ of 0.033 independently of the particle size and was assigned to nearly hydrophobic (NH particles. Its mean particle number fraction was large, and it decreased monotonically from 69 to 41 % with particle diameter. The other mode showed a mean HGF increasing slightly from 1.31 to 1.38 (κ values from 0.186 to 0.196 with particle diameter, and it was attributed to less hygroscopic (LH particles. The mode with more hygroscopic particles was not identified. The probability density function of the volatility GF (VGF also exhibited a distinct bimodal distribution with an overall mean VGF of approximately 0.96 independently of the particle size, and with another mean VGF increasing from 0.49 to 0.55 with particle diameter. The two modes were associated with less volatile (LV and volatile (V particles. The mean particle number fraction for the LV mode decreased from 34 to 21 % with particle diameter. The bimodal distributions indicated that the urban atmospheric aerosol contained an external mixture of particles with a diverse chemical composition. Particles corresponding to the NH and LV modes were assigned mainly to freshly emitted combustion particles, more specifically to vehicle emissions consisting of large mass fractions of soot likely coated with or containing some water-insoluble organic compounds such as non

Laboratory Experiments and Instrument Development for the Study of Atmospheric Aerosols

Energy Technology Data Exchange (ETDEWEB)

Davidovits, Paul

2011-12-10

Soot particles are generated by incomplete combustion of fossil and biomass fuels. Through direct effects clear air aerosols containing black carbon (BC) such as soot aerosols, absorb incoming light heating the atmosphere, while most other aerosols scatter light and produce cooling. Even though BC represents only 1-2% of the total annual emissions of particulate mass to the atmosphere, it has been estimated that the direct radiative effect of BC is the second-most important contributor to global warming after absorption by CO2. Ongoing studies continue to underscore the climate forcing importance of black carbon. However, estimates of the radiative effects of black carbon on climate remain highly uncertain due to the complexity of particles containing black carbon. Quantitative measurement of BC is challenging because BC often occurs in highly non-spherical soot particles of complex morphology. Freshly emitted soot particles are typically fractal hydrophobic aggregates. The aggregates consist of black carbon spherules with diameters typically in the range of about 15-40 nm, and they are usually coated by adsorbed polyaromatic hydrocarbons (PAHs) produced during combustion. Diesel-generated soot particles are often emitted with an organic coating composed primarily of lubricating oil and unburned fuel, as well as well as PAH compounds. Sulfuric acid has also been detected in diesel and aircraft-emitted soot particles. In the course of aging, these particle coatings may be substantially altered by chemical reactions and/or the deposition of other materials. Such processes transform the optical and CCN properties of the soot aerosols in ways that are not yet well understood. Our work over the past seven years consisted of laboratory research, instrument development and characterization, and field studies with the central focus of improving our understanding of the black carbon aerosol climate impacts. During the sixth year as well as during this seventh year (no

Phototransformation rate constants of PAHs associated with soot particles

International Nuclear Information System (INIS)

Kim, Daekyun; Young, Thomas M.; Anastasio, Cort

2013-01-01

Photodegradation is a key process governing the residence time and fate of polycyclic aromatic hydrocarbons (PAHs) in particles, both in the atmosphere and after deposition. We have measured photodegradation rate constants of PAHs in bulk deposits of soot particles illuminated with simulated sunlight. The photodegradation rate constants at the surface (k p 0 ), the effective diffusion coefficients (D eff ), and the light penetration depths (z 0.5 ) for PAHs on soot layers of variable thickness were determined by fitting experimental data with a model of coupled photolysis and diffusion. The overall disappearance rates of irradiated low molecular weight PAHs (with 2–3 rings) on soot particles were influenced by fast photodegradation and fast diffusion kinetics, while those of high molecular weight PAHs (with 4 or more rings) were apparently controlled by either the combination of slow photodegradation and slow diffusion kinetics or by very slow diffusion kinetics alone. The value of z 0.5 is more sensitive to the soot layer thickness than the k p 0 value. As the thickness of the soot layer increases, the z 0.5 values increase, but the k p 0 values are almost constant. The effective diffusion coefficients calculated from dark experiments are generally higher than those from the model fitting method for illumination experiments. Due to the correlation between k p 0 and z 0.5 in thinner layers, D eff should be estimated by an independent method for better accuracy. Despite some limitations of the model used in this study, the fitted parameters were useful for describing empirical results of photodegradation of soot-associated PAHs. - Highlights: ► PAHs on soot were evaluated by a model of coupled photolysis and diffusion. ► Photodegradation rate at the surface, diffusion coefficient, and light penetration path were determined. ► Low MW PAHs were influenced by fast photodegradation and fast diffusion. ► High MW PAHs were controlled either by slow

Effects of Large Polycyclic Aromatic Hydrocarbons on the Soot Formation in Ethylene-Air Nonpremixed Flames

KAUST Repository

Prabhu, S.; Arias, P.G.; Wang, Y.; Gao, Y.; Park, S.; Im, Hong G.; Sarathy, Mani; Chung, Suk-Ho; Lu, T.

2015-01-01

This study presents updated comprehensive gas-phase kinetic mechanism and aerosol models to predict soot formation characteristics in ethylene-air nonpremixed flames. A main objective is to investigate the sensitivity of the soot formation rate to various chemical pathways for large polycyclic aromatic hydrocarbons (PAH). In this study, the detailed chemical mechanism was reduced from 397 to 99 species using directed relation graph (DRG) and sensitivity analysis. The method of moments with interpolative closure (MOMIC) was employed for the soot aerosol model. Counterflow nonpremixed flames of pure ethylene at low strain rate sooting conditions are considered, for which the sensitivity of soot formation characteristics with respect to hetrogeneous nucleation is investigated. Results show that higher PAH concentrations result in higher soot nucleation rate, and that the average size of the particles are in good agreement with experimental results. It is found that the nucleation processes (i.e., soot inception) from higher PAH precursors, coronene in particular, is critical for accurate prediction of the overall soot formation.

Effects of Large Polycyclic Aromatic Hydrocarbons on the Soot Formation in Ethylene-Air Nonpremixed Flames

KAUST Repository

Prabhu, S.

2015-03-30

This study presents updated comprehensive gas-phase kinetic mechanism and aerosol models to predict soot formation characteristics in ethylene-air nonpremixed flames. A main objective is to investigate the sensitivity of the soot formation rate to various chemical pathways for large polycyclic aromatic hydrocarbons (PAH). In this study, the detailed chemical mechanism was reduced from 397 to 99 species using directed relation graph (DRG) and sensitivity analysis. The method of moments with interpolative closure (MOMIC) was employed for the soot aerosol model. Counterflow nonpremixed flames of pure ethylene at low strain rate sooting conditions are considered, for which the sensitivity of soot formation characteristics with respect to hetrogeneous nucleation is investigated. Results show that higher PAH concentrations result in higher soot nucleation rate, and that the average size of the particles are in good agreement with experimental results. It is found that the nucleation processes (i.e., soot inception) from higher PAH precursors, coronene in particular, is critical for accurate prediction of the overall soot formation.

Absorbing Aerosols: Field and Laboratory Studies of Black Carbon and Dust

Science.gov (United States)

Aiken, A. C.; Flowers, B. A.; Dubey, M. K.

2011-12-01

Currently, absorbing aerosols are thought to be the most uncertain factor in atmospheric climate models (~0.4-1.2 W/m2), and the 2nd most important factor after CO2 in global warming (1.6 W/m2; Ramanathan and Carmichael, Nature Geoscience, 2008; Myhre, Science, 2009). While most well-recognized atmospheric aerosols, e.g., sulfate from power-plants, have a cooling effect on the atmosphere by scattering solar radiation, black carbon (BC or soot) absorbs sunlight strongly which results in a warming of the atmosphere. Dust particles are also present globally and can absorb radiation, contributing to a warmer and drier atmosphere. Direct on-line measurements of BC and hematite, an absorbing dust aerosol, can be made with the Single Particle Soot Photometer (SP2), which measures the mass of the particles by incandescence on an individual particle basis. Measurements from the SP2 are combined with absorption measurements from the three-wavelength photoacoustic soot spectrometer (PASS-3) at 405, 532, and 781 nm and the ultraviolet photoacoustic soot spectrometer (PASS-UV) at 375 nm to determine wavelength-dependent mass absorption coefficients (MACs). Laboratory aerosol samples include flame-generated soot, fullerene soot, Aquadag, hematite, and hematite-containing dusts. Measured BC MAC's compare well with published values, and hematite MAC's are an order of magnitude less than BC. Absorbing aerosols measured in the laboratory are compared with those from ambient aerosols measured during the Las Conchas fire and BEACHON-RoMBAS. The Las Conchas fire was a wildfire in the Jemez Mountains of New Mexico that burned over 100,000 acres during the Summer of 2011, and BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen - Rocky Mountain Biogenic Aerosol Study) is a field campaign focusing on biogenic aerosols at the Manitou Forest Observatory near Colorado Springs, CO in Summer 2011. Optical properties and size

Single Particle Soot Photometer intercomparison at the AIDA chamber

Directory of Open Access Journals (Sweden)

M. Laborde

2012-12-01

Full Text Available Soot particles, consisting of black carbon (BC, organic carbon (OC, inorganic salts, and trace elements, are emitted into the atmosphere during incomplete combustion. Accurate measurements of atmospheric BC are important as BC particles cause adverse health effects and impact the climate.

Unfortunately, the accurate measurement of the properties and mass concentrations of BC particles remains difficult. The Single Particle Soot Photometer (SP2 can contribute to improving this situation by measuring the mass of refractory BC in individual particles as well as its mixing state.

Here, the results of the first detailed SP2 intercomparison, involving 6 SP2s from 6 different research groups, are presented, including the most evolved data products that can presently be calculated from SP2 measurements.

It was shown that a detection efficiency of almost 100% down to 1 fg BC per particle can readily be achieved, and that this limit can be pushed down to ∼0.2 fg BC with optimal SP2 setup. Number and mass size distributions of BC cores agreed within ±5% and ±10%, respectively, in between the SP2s, with larger deviations in the range below 1 fg BC.

The accuracy of the SP2's mass concentration measurement depends on the calibration material chosen. The SP2 has previously been shown to be equally sensitive to fullerene soot and ambient BC from sources where fossil fuel was dominant and less sensitive to fullerene soot than to Aquadag. Fullerene soot was therefore chosen as the standard calibration material by the SP2 user community; however, many data sets rely solely on Aquadag calibration measurements. The difference in SP2 sensitivity was found to be almost equal (fullerene soot to Aquadag response ratio of ∼0.75 at 8.9 fg BC for all SP2s. This allows the calculation of a fullerene soot equivalent calibration curve from a measured Aquadag calibration, when no fullerene soot calibration is available. It could be

Soot particles at an elevated site in eastern China during the passage of a strong cyclone

Energy Technology Data Exchange (ETDEWEB)

Niu, Hongya [State Key Laboratory of Coal Resources and Safe Mining, School of Geoscience and Surveying Engineering, China University of Mining and Technology, Beijing 100083 (China); Faculty of Environmental and Symbiotic Sciences, Prefectural University of Kumamoto, Kumamoto 862-8502 (Japan); Shao, Longyi [State Key Laboratory of Coal Resources and Safe Mining, School of Geoscience and Surveying Engineering, China University of Mining and Technology, Beijing 100083 (China); Zhang, Daizhou, E-mail: dzzhang@pu-kumamoto.ac.jp [Faculty of Environmental and Symbiotic Sciences, Prefectural University of Kumamoto, Kumamoto 862-8502 (Japan)

2012-07-15

Atmospheric particles larger than 0.2 {mu}m were collected at the top of Mt. Tai (36.25 Degree-Sign N, 117.10 Degree-Sign E, 1534 m a.s.l.) in eastern China in May 2008 during the passage of a strong cyclone. The particles were analyzed with electron microscopes and characterized by morphology, equivalent diameter and elemental composition. Soot particles with coating (coated soot particles) and those without apparent coating (naked soot particles) were predominant in the diameter range smaller than 0.6 {mu}m in all samples. The number-size distribution of the relative abundance of naked soot particles in the prefrontal air was similar to that in the postfrontal air and their size modes were around 0.2-0.3 {mu}m. However, the distribution of inclusions of coated soot particles showed a mode in the range of 0.1-0.3 {mu}m. The coating degree of coated soot particles, which was defined by the ratio of the diameter of inclusion to the diameter of particle body, showed a mode around 0.5 with the range of 0.3-0.6. These results indicate that the status of soot particles in the prefrontal and postfrontal air was similar although air pollution levels were dramatically different. In addition, the relative abundance of accumulation mode particles increased with the decrease of soot particles after the front passage. - Highlights: Black-Right-Pointing-Pointer Particles at an elevated site in eastern China in a strong cyclone were studied. Black-Right-Pointing-Pointer Aged status of soot particles in the prefrontal and postfrontal air was similar. Black-Right-Pointing-Pointer Soot particles in elevated layers could be considered as aged ones.

Ambient Observations of Aerosols, Novel Aerosol Structures, And Their Engineering Applications

Science.gov (United States)

Beres, Nicholas D.

The role of atmospheric aerosols remains a crucial issue in understanding and mitigating climate change in our world today. These particles influence the Earth by altering the Earth's delicate radiation balance, human health, and visibility. In particular, black carbon particulate matter remains the key driver in positive radiative forcing (i.e., warming) due to aerosols. Produced from the incomplete combustion of hydrocarbons, these compounds can be found in many different forms around the globe. This thesis provides an overview of three research topics: (1) the ambient characterization of aerosols in the Northern Indian Ocean, measurement techniques used, and how these aerosols influence local, regional, and global climate; (2) the exploration of novel soot superaggregate particles collected in the Northern Indian Ocean and around the globe and how the properties of these particles relate to human health and climate forcing; and (3) how aerogelated soot can be produced in a novel, one-step method utilizing an inverted flame reactor and how this material could be used in industrial settings.

Cloud condensation nuclei and ice nucleation activity of hydrophobic and hydrophilic soot particles.

Science.gov (United States)

Koehler, Kirsten A; DeMott, Paul J; Kreidenweis, Sonia M; Popovicheva, Olga B; Petters, Markus D; Carrico, Christian M; Kireeva, Elena D; Khokhlova, Tatiana D; Shonija, Natalia K

2009-09-28

Cloud condensation nuclei (CCN) activity and ice nucleation behavior (for temperaturesnucleation experiments below -40 degrees C, AEC particles nucleated ice near the expected condition for homogeneous freezing of water from aqueous solutions. In contrast, GTS, TS, and TC1 required relative humidity well in excess of water saturation at -40 degrees C for ice formation. GTS particles required water supersaturation conditions for ice activation even at -51 degrees C. At -51 to -57 degrees C, ice formation in particles with electrical mobility diameter of 200 nm occurred in up to 1 in 1000 TS and TC1 particles, and 1 in 100 TOS particles, at relative humidities below those required for homogeneous freezing in aqueous solutions. Our results suggest that heterogeneous ice nucleation is favored in cirrus conditions on oxidized hydrophilic soot of intermediate polarity. Simple considerations suggest that the impact of hydrophilic soot particles on cirrus cloud formation would be most likely in regions of elevated atmospheric soot number concentrations. The ice formation properties of AEC soot are reasonably consistent with present understanding of the conditions required for aircraft contrail formation and the proportion of soot expected to nucleate under such conditions.

Ion chemistry and individual particle analysis of atmospheric aerosols over Mt. Bogda of eastern Tianshan Mountains, Central Asia.

Science.gov (United States)

Zhao, Shuhui; Li, Zhongqin; Zhou, Ping

2011-09-01

Aerosol samples were collected during the scientific expedition to Mt. Bogda in July-August, 2009. The major inorganic ions (Na( + ), NH⁺₄, K( + ), Mg(2 + ), Ca(2 + ), Cl( - ), SO²⁻₄, and NO⁻₃) of the aerosols were determined by ion chromatography. SO²⁻₄, NO⁻₃, and Ca(2 + ) were the dominate ions, with the mean concentrations of 0.86, 0.56, and 0.28 μg m⁻³, respectively. These mean ion concentrations were generally comparable with the background conditions in remote site of Xinjiang, while much lower than those in Ürümqi. Morphology and elemental compositions of 1,500 particles were determined by field emission scanning electron microscopy equipped with an energy dispersive X-ray spectrometer. Based on the morphology and elemental compositions, particles were classed into four major groups: soot (15.1%), fly ash (4.7%), mineral particles (78.9%), and little other matters (0.8% Fe-rich particles and 0.5% unrecognized particles). Presence of soot and fly ash particles indicated the influence of anthropogenic pollutions, while abundance mineral particles suggested that natural processes were the primary source of aerosols over this region, coinciding with the ionic analysis. Backward air mass trajectory analysis suggested that Ürümqi may contribute some anthropogenic pollution to this region, while the arid and semi-arid regions of Central Asia were the primary source.

Photoacoustic Soot Spectrometer (PASS) Instrument Handbook

Energy Technology Data Exchange (ETDEWEB)

Dubey, M [Los Alamos National Laboratory; Springston, S [Brookhaven National Laboratory; Koontz, A [Pacific Northwest National Laboratory; Aiken, A [Los Alamos National Laboratory

2013-01-17

The photoacoustic soot spectrometer (PASS) measures light absorption by aerosol particles. As the particles pass through a laser beam, the absorbed energy heats the particles and in turn the surrounding air, which sets off a pressure wave that can be detected by a microphone. The PASS instruments deployed by ARM can also simultaneously measure the scattered laser light at three wavelengths and therefore provide a direct measure of the single-scattering albedo. The Operator Manual for the PASS-3100 is included here with the permission of Droplet Measurement Technologies, the instrument’s manufacturer.

Seasonal features of aerosol particles recorded in snow from Mt. Qomolangma (Everest) and their environmental implications

Institute of Scientific and Technical Information of China (English)

CONG Zhiyuan; KANG Shichang; QIN Dahe

2009-01-01

To assess the seasonality of aerosol deposition and anthropogenic effects on central Himalayas, a 1.85-m deep snow pit was dug on the northern slope of Mr. Qomolangma (Everest). Based on the morphology and energy dispersive X-ray (EDX) signal, totally 1500 particles were classed into 7 groups: soot; aluminosilicates; fly ash; calcium sulfates; Ca/Mg carbonates; metal oxides; and biological particles and carbon fragments. The size distribution and number fractions of different particle groups exhibited distinct seasonal variations between non-monsoon and monsoon periods, which are clearly related to the differences in air mass pathways. Specifically, the relative abundance of soot in non-monsoon period (25%) was much higher than that in monsoon period (14%), indicating Mr. Qomolangma region received more anthropogenic influence in non-monsoon than monsoon period.

Application of the direct simulation Monte Carlo method to nanoscale heat transfer between a soot particle and the surrounding gas

International Nuclear Information System (INIS)

Yang, M.; Liu, F.; Smallwood, G.J.

2004-01-01

Laser-Induced Incandescence (LII) technique has been widely used to measure soot volume fraction and primary particle size in flames and engine exhaust. Currently there is lack of quantitative understanding of the shielding effect of aggregated soot particles on its conduction heat loss rate to the surrounding gas. The conventional approach for this problem would be the application of the Monte Carlo (MC) method. This method is based on simulation of the trajectories of individual molecules and calculation of the heat transfer at each of the molecule/molecule collisions and the molecule/particle collisions. As the first step toward calculating the heat transfer between a soot aggregate and the surrounding gas, the Direct Simulation Monte Carlo (DSMC) method was used in this study to calculate the heat transfer rate between a single spherical aerosol particle and its cooler surrounding gas under different conditions of temperature, pressure, and the accommodation coefficient. A well-defined and simple hard sphere model was adopted to describe molecule/molecule elastic collisions. A combination of the specular reflection and completely diffuse reflection model was used to consider molecule/particle collisions. The results obtained by DSMC are in good agreement with the known analytical solution of heat transfer rate for an isolated, motionless sphere in the free-molecular regime. Further the DSMC method was applied to calculate the heat transfer in the transition regime. Our present DSMC results agree very well with published DSMC data. (author)

Detection of Soot Using a Resistivity Sensor Device Employing Thermophoretic Particle Deposition

Directory of Open Access Journals (Sweden)

Doina Lutic

2010-01-01

Full Text Available Results are reported for thermophoretic deposition of soot particles on resistivity sensors as a monitoring technique for diesel exhaust particles with the potential of improved detection limit and sensitivity. Soot with similar characteristics as from diesel exhausts was generated by a propane flame and diluted in stages. The soot in a gas flow at 240–270C∘ was collected on an interdigitated electrode structure held at a considerably lower temperature, 105–125C∘. The time delay for reaching measurable resistance values, the subsequent rate, and magnitude of resistance decrease were a function of the distance between the fingers in the electrodes and the degree of dilution of the soot containing flow. Soot deposition and subsequent removal by heating the sensor support was also performed in a real diesel exhaust. Good similarities between the behavior in our laboratory system and the real diesel exhaust were noticed.

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

Science.gov (United States)

Jiang, Hao; Li, Tie; Wang, Yifeng; He, Pengfei

2018-04-01

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.

Quantitative effects of rapid heating on soot-particle sizing through analysis of two-pulse LII

KAUST Repository

Cenker, Emre

2017-02-27

During the rapid laser pulse heating and consecutive cooling in laser-induced incandescence (LII), soot particles may undergo thermal annealing and sublimation processes which lead to a permanent change in its optical properties and its primary particle size, respectively. Overall, effects of these two processes on soot and LII model-based particle sizing are investigated by measuring the two-color time-resolved (2C-TiRe) LII signal decay from in-flame soot after two consecutive laser pulses at 1064-nm wavelength. Experiments are carried out on a non-premixed laminar ethylene/air flame from a Santoro burner with both low and moderate laser fluences suitable for particle sizing. The probe volume is set to a radial position close to the flame axis where the soot particles are known to be immature or less graphitic. With the first pulse, soot is pre-heated, and the LII signal after the consecutive second pulse is used for analysis. The two-color incandescence emission technique is used for the pyrometric determination of the LII-heated peak soot temperature at the second pulse. A new LII simulation tool is developed which accounts for particle heating via absorption and annealing, and cooling via sublimation, conduction, and radiation with various existing sub-models from the literature. The same approach of using two laser pulses is implemented in the simulations. Measurements indicate that thermal annealing and associated absorption enhancement becomes important at laser fluences above 0.17 J/cm2 for the immature in-flame soot. After a heating pulse at 0.33 J/cm2, the increase of the soot absorption function is calculated as 35% using the temperature measured at the second pulse and an absorption model based on the Rayleigh approximation. Present annealing model, on the other hand, predicts graphitization of soot even in the absence of laser heating at typical flame temperatures. Recorded experimental LII signal decays and LII-heated peak soot temperature

Properties of Arctic Aerosol Particles and Residuals of Warm Clouds: Cloud Activation Efficiency and the Aerosol Indirect Effect

Science.gov (United States)

Zelenyuk, A.; Imre, D. G.; Leaitch, R.; Ovchinnikov, M.; Liu, P.; Macdonald, A.; Strapp, W.; Ghan, S. J.; Earle, M. E.

2012-12-01

Single particle mass spectrometer, SPLAT II, was used to characterize the size, composition, number concentration, density, and shape of individual Arctic spring aerosol. Background particles, particles above and below the cloud, cloud droplet residuals, and interstitial particles were characterized with goal to identify the properties that separate cloud condensation nuclei (CCN) from background aerosol particles. The analysis offers a comparison between warm clouds formed on clean and polluted days, with clean days having maximum particle concentrations (Na) lower than ~250 cm-3, as compared with polluted days, in which maximum concentration was tenfold higher. On clean days, particles were composed of organics, organics mixed with sulfates, biomass burning (BB), sea salt (SS), and few soot and dust particles. On polluted days, BB, organics associated with BB, and their mixtures with sulfate dominated particle compositions. Based on the measured compositions and size distributions of cloud droplet residuals, background aerosols, and interstitial particles, we conclude that these three particle types had virtually the same compositions, which means that cloud activation probabilities were surprisingly nearly composition independent. Moreover, these conclusions hold in cases in which less than 20% or more than 90% of background particles got activated. We concluded that for the warm clouds interrogated in this study particle size played a more important factor on aerosol CCN activity. Comparative analysis of all studied clouds reveals that aerosol activation efficiency strongly depends on the aerosol concentrations, such that at Na <200 cm-3, nearly all particles activate, and at higher concentrations the activation efficiency is lower. For example, when Na was greater than 1500 cm-3, less than ~30% of particles activated. The data suggest that as the number of nucleated droplets increases, condensation on existing droplets effectively competes with particle

Aerosol and NOx emission factors and submicron particle number size distributions in two road tunnels with different traffic regimes

Directory of Open Access Journals (Sweden)

D. Imhof

2006-01-01

Full Text Available Measurements of aerosol particle number size distributions (18–700 nm, mass concentrations (PM2.5 and PM10 and NOx were performed in the Plabutsch tunnel, Austria, and in the Kingsway tunnel, United Kingdom. These two tunnels show different characteristics regarding the roadway gradient, the composition of the vehicle fleet and the traffic frequency. The submicron particle size distributions contained a soot mode in the diameter range D=80–100 nm and a nucleation mode in the range of D=20–40 nm. In the Kingsway tunnel with a significantly lower particle number and volume concentration level than in the Plabutsch tunnel, a clear diurnal variation of nucleation and soot mode particles correlated to the traffic density was observed. In the Plabutsch tunnel, soot mode particles also revealed a diurnal variation, whereas no substantial variation was found for the nucleation mode particles. During the night a higher number concentration of nucleation mode particles were measured than soot mode particles and vice versa during the day. In this tunnel with very high soot emissions during daytime due to the heavy-duty vehicle (HDV share of 18% and another 40% of diesel driven light-duty vehicles (LDV semivolatile species condense on the pre-existing soot surface area rather than forming new particles by homogeneous nucleation. With the low concentration of soot mode particles in the Kingsway tunnel, also the nucleation mode particles exhibit a diurnal variation. From the measured parameters real-world traffic emission factors were estimated for the whole vehicle fleet as well as differentiated into the two categories LDV and HDV. In the particle size range D=18–700 nm, each vehicle of the mixed fleet emits (1.50±0.08×1014 particles km-1 (Plabutsch and (1.26±0.10×1014 particles km-1 (Kingsway, while particle volume emission factors of 0.209±0.008 cm3 km-1 and 0.036±0.004 cm3 km-1, respectively, were obtained. PM1 emission factors of 104±4 mg

Observations and Modeling of the Green Ocean Amazon 2014/15: Transmission Electron Microscopy Analysis of Aerosol Particles Field Campaign Report

Energy Technology Data Exchange (ETDEWEB)

Buseck, Peter [Arizona State Univ., Tempe, AZ (United States)

2016-03-01

During two Intensive Operational Periods (IOP), we collected samples at 3-hour intervals for transmission electron microscopy analysis. The resulting transmission electron microscopy images and compositions were analyzed for the samples of interest. Further analysis will be done especially for the plume of interest. We found solid spherical organic particles from rebounded samples collected with Professor Scot Martin’s group (Harvard University). Approximately 30% of the rebounded particles at 95% relative humidity were spherical organic particles. Their sources and formation process are not known, but such spherical particles could be solid and will have heterogeneous chemical reactions. We observed many organic particles that are internally mixed with inorganic elements such as potassium and nitrogen. They are either homogeneously mixed or have inorganic cores with organic aerosol coatings. Samples collected from the Manaus, Brazil, pollution plume included many nano-size soot particles mixed with organic material and sulfate. Aerosol particles from clean periods included organic aerosol particles, sulfate, sea salt, dust, and primary biogenic aerosol particles. There was more dust, primary biogenic aerosol, and tar balls in samples taken during IOP1 than those taken during IOP2. Many dust particles were found between March 2 and 3.

Spectral Signature of Radiative Forcing by East Asian Dust-Soot Mixture

Science.gov (United States)

Zhu, A.; Ramanathan, V.

2007-12-01

The Pacific Dust Experiment (PACDEX) provides the first detailed sampling of dust-soot mixtures from the western Pacific to the eastern Pacific Ocean. The data includes down and up spectral irradiance, mixing state of dust and soot, and other aerosol properties. This study attempts to simulate the radiative forcing by dust-soot mixtures during the experimental period. The MODTRAN band model was employed to investigate the spectral signatures of solar irradiance change induced by aerosols at moderate spectral resolutions. For the short wave band (300-1100nm) used in this study, the reduction of downward irradiance at surface by aerosols greatly enhances with increasing wavelength in the UV band (300-400nm), reaches a maximum in the blue band, then gradually decreases toward the red band. In the near-IR band (700-1100nm), irradiance reduction by aerosols shows great fluctuations in the band with center wavelength at around 940nm, 820nm, 720nm, 760nm, 690nm, where the aerosol effect is overwhelmed by the water vapor and O2 absorptions. The spectral pattern of irradiance reduction varies for different aerosol species. The maximum reduction lies at around 450nm for soot, and shifting to about 490nm for East Asian mineral dust. It's worth noting that although soot aerosols reduce more irradiance than East Asian dust in the UV and blue band, the impact of dust to the irradiance exceeds that by soot at the longer wavelength band (i.e. around 550nm). The reduction of irradiance by East Asian dust (soot) in the UV band, visible band, and near-IR accounts for about 6% (10%), 56% (64%), and 38% (26%) of total irradiance reduction. As large amount of soot aerosols are involved during the long range transport of East Asian dust, the optical properties of dust aerosols are modified with different mixing state with soot, the spectral pattern of the irradiance reduction will be changed. The study of aerosol forcing at moderate spectral resolutions has the potential application for

Aerosol effects on UV radiation

International Nuclear Information System (INIS)

Koepke, P.; Reuder, J.; Schwander, H.

2000-01-01

The reduction of erythemally weighted UV-irradiance (given as UV index, UVI) due to aerosols is analyzed by variation of the tropospheric particles in a wide, but realistic range. Varied are amount and composition of the particles and relative humidity and thickness of the mixing layer. The reduction of UVI increases with aerosol optical depth and the UV change is around 10% for a change aerosol optical depth from 0.25 to 0.1 and 0.4 respectively. Since both aerosol absorption and scattering are of relevance, the aerosol effect depends besides total aerosol amount on relative amount of soot and on relative humidity

Biomass burning plumes and the aging of black carbon aerosols in the tropopause region observed with the CARIBIC single particle soot photometer

Science.gov (United States)

Ditas, J.; Ma, N.; Zhang, Y.; Assmann, D. N.; Neumaier, M.; Wang, S.; Wang, J.; Zahn, A.; Hermann, M.; Brenninkmeijer, C. A. M.; Poeschl, U.; Su, H.; Cheng, Y.

2017-12-01

Biomass burning (BB) events can release large amounts of refractory black carbon (rBC) into the upper troposphere and lowermost stratosphere (UT/LMS) (Dahlkötter et al., 2014). To explore this effect, a Single Particle Soot Photometer (SP2) was added to the scientific payload of the instrumented CARIBIC container that is installed monthly in the cargo bay of a passenger aircraft (the IAGOS-CARIBIC atmospheric observatory, www.iagos.org). Regular measurement flights with different destinations are performed, covering an area of about 120°W to 120°E and 75°N to 30°S. A wide range of in situ measurements (CO, O3, greenhouse gases, aerosol particles and volatile organic compounds) is combined with a collection of air and aerosol samples for laboratory analyses. Since August 2014, the SP2 measures BC number and mass concentration at altitudes between 8 and 12 km. More than 600 BC measurement hours show a strong impact of BB emissions on the lowermost stratosphere. The BB plumes are identified with the help of concurrent carbon monoxide and acetonitrile measurements showing substantially increased concentrations compared to their background level. Transported into the lowermost stratosphere, BB smoke can be transported over long distances and the BC particles can stay in the atmosphere up to one year. The monthly missions of four consecutive CARIBIC flights sometimes enable to revisit a certain air mass, as was the case during a measurement flight to San Francisco in August 2014, with a stopover time of 2h. The revisited biomass burning plume located over the Altlantic ocean near Greenland was traced back by backward and forward trajectories to open fires in Canada (upper Fig.). The transit time of the smoke plume was estimated to 16 - 19h which perfectly matches our flight time difference ( 18h). Based on the LEO-fit method (Leading Edge Only fit) from Gao et al. (2007), the mixing state of the BC particles within the BB plume was calculated. Our unique data set

Development of high fidelity soot aerosol dynamics models using method of moments with interpolative closure

KAUST Repository

Roy, Subrata P.

2014-01-28

The method of moments with interpolative closure (MOMIC) for soot formation and growth provides a detailed modeling framework maintaining a good balance in generality, accuracy, robustness, and computational efficiency. This study presents several computational issues in the development and implementation of the MOMIC-based soot modeling for direct numerical simulations (DNS). The issues of concern include a wide dynamic range of numbers, choice of normalization, high effective Schmidt number of soot particles, and realizability of the soot particle size distribution function (PSDF). These problems are not unique to DNS, but they are often exacerbated by the high-order numerical schemes used in DNS. Four specific issues are discussed in this article: the treatment of soot diffusion, choice of interpolation scheme for MOMIC, an approach to deal with strongly oxidizing environments, and realizability of the PSDF. General, robust, and stable approaches are sought to address these issues, minimizing the use of ad hoc treatments such as clipping. The solutions proposed and demonstrated here are being applied to generate new physical insight into complex turbulence-chemistry-soot-radiation interactions in turbulent reacting flows using DNS. © 2014 Copyright Taylor and Francis Group, LLC.

Modelling heterogeneous ice nucleation on mineral dust and soot with parameterizations based on laboratory experiments

Science.gov (United States)

Hoose, C.; Hande, L. B.; Mohler, O.; Niemand, M.; Paukert, M.; Reichardt, I.; Ullrich, R.

2016-12-01

Between 0 and -37°C, ice formation in clouds is triggered by aerosol particles acting as heterogeneous ice nuclei. At lower temperatures, heterogeneous ice nucleation on aerosols can occur at lower supersaturations than homogeneous freezing of solutes. In laboratory experiments, the ability of different aerosol species (e.g. desert dusts, soot, biological particles) has been studied in detail and quantified via various theoretical or empirical parameterization approaches. For experiments in the AIDA cloud chamber, we have quantified the ice nucleation efficiency via a temperature- and supersaturation dependent ice nucleation active site density. Here we present a new empirical parameterization scheme for immersion and deposition ice nucleation on desert dust and soot based on these experimental data. The application of this parameterization to the simulation of cirrus clouds, deep convective clouds and orographic clouds will be shown, including the extension of the scheme to the treatment of freezing of rain drops. The results are compared to other heterogeneous ice nucleation schemes. Furthermore, an aerosol-dependent parameterization of contact ice nucleation is presented.

Light scattering and extinction measurements combined with laser-induced incandescence for the real-time determination of soot mass absorption cross section.

Science.gov (United States)

Wei, Yiyi; Ma, Lulu; Cao, Tingting; Zhang, Qing; Wu, Jun; Buseck, Peter R; Thompson, J E

2013-10-01

An aerosol albedometer was combined with laser-induced incandescence (LII) to achieve simultaneous measurements of aerosol scattering, extinction coefficient, and soot mass concentration. Frequency doubling of a Nd:YAG laser line resulted in a colinear beam of both λ = 532 and 1064 nm. The green beam was used to perform cavity ring-down spectroscopy (CRDS), with simultaneous measurements of scattering coefficient made through use of a reciprocal sphere nephelometer. The 1064 nm beam was selected and directed into a second integrating sphere and used for LII of light-absorbing kerosene lamp soot. Thermal denuder experiments showed the LII signals were not affected by the particle mixing state when laser peak power was 1.5-2.5 MW. The combined measurements of optical properties and soot mass concentration allowed determination of mass absorption cross section (M.A.C., m(2)/g) with 1 min time resolution when soot concentrations were in the low microgram per cubic meter range. Fresh kerosene nanosphere soot (ns-soot) exhibited a mean M.A.C and standard deviation of 9.3 ± 2.7 m(2)/g while limited measurements on dry ambient aerosol yielded an average of 8.2 ± 5.9 m(2)/g when soot was >0.25 μg/m(3). The method also detected increases in M.A.C. values associated with enhanced light absorption when polydisperse, laboratory-generated ns-soot particles were embedded within or coated with ammonium nitrate, ammonium sulfate, and glycerol. Glycerol coatings produced the largest fractional increase in M.A.C. (1.41-fold increase), while solid coatings of ammonium sulfate and ammonium nitrate produced increases of 1.10 and 1.06, respectively. Fresh, ns-soot did not exhibit increased M.A.C. at high relative humidity (RH); however, lab-generated soot coated with ammonium nitrate and held at 85% RH exhibited M.A.C. values nearly double the low-humidity case. The hybrid instrument for simultaneously tracking soot mass concentration and aerosol optical properties in real time is a

Laboratory and modeling studies on the effects of water and soot emissions and ambient conditions on the properties of contrail ice particles in the jet regime

Directory of Open Access Journals (Sweden)

H.-W. Wong

2013-10-01

Full Text Available Contrails and contrail-induced cirrus clouds are identified as the most uncertain components in determining aviation impacts on global climate change. Parameters affecting contrail ice particle formation immediately after the engine exit plane (< 5 s in plume age may be critical to ice particle properties used in large-scale models predicting contrail radiative forcing. Despite this, detailed understanding of these parametric effects is still limited. In this paper, we present results from recent laboratory and modeling studies conducted to investigate the effects of water and soot emissions and ambient conditions on near-field formation of contrail ice particles and ice particle properties. The Particle Aerosol Laboratory (PAL at the NASA Glenn Research Center and the Aerodyne microphysical parcel model for contrail ice particle formation were employed. Our studies show that exhaust water concentration has a significant impact on contrail ice particle formation and properties. When soot particles were introduced, ice particle formation was observed only when exhaust water concentration was above a critical level. When no soot or sulfuric acid was introduced, no ice particle formation was observed, suggesting that ice particle formation from homogeneous nucleation followed by homogeneous freezing of liquid water was unfavorable. Soot particles were found to compete for water vapor condensation, and higher soot concentrations emitted into the chamber resulted in smaller ice particles being formed. Chamber conditions corresponding to higher cruising altitudes were found to favor ice particle formation. The microphysical model captures trends of particle extinction measurements well, but discrepancies between the model and the optical particle counter measurements exist as the model predicts narrower ice particle size distributions and ice particle sizes nearly a factor of two larger than measured. These discrepancies are likely due to particle

Aerosol composition and properties variation at the ground and over the column under different air masses advection in South Italy.

Science.gov (United States)

Pavese, G; Lettino, A; Calvello, M; Esposito, F; Fiore, S

2016-04-01

Aerosol composition and properties variation under the advection of different air masses were investigated, as case studies, by contemporary measurements over the atmospheric column and at the ground in a semi-rural site in South Italy. The absence of local strong sources in this area allowed to characterize background aerosol and to compare particle mixing effects under various atmospheric circulation conditions. Aerosol optical depth (AOD) and Ǻngström parameters from radiometric measurements allowed the detection and identification of polluted, dust, and volcanic atmospheric conditions. AODs were the input for a suitable model to evaluate the columnar aerosol composition, according to six main atmospheric components (water-soluble, soot, sea salt accumulation, sea salt coarse, mineral dus,t and biological). Scanning electron microscope (SEM) analysis of particulate sampled with a 13-stage impactor at the ground showed not only fingerprints typical of the different air masses but also the effects of transport and aging on atmospheric particles, suggesting processes that changed their chemical and optical properties. Background columnar aerosol was characterized by 72% of water-soluble and soot, in agreement with ground-based findings that highlighted 60% of contribution from anthropogenic carbonate particles and soot. In general, a good agreement between ground-based and columnar results was observed. Under the advection of trans-boundary air masses, water-soluble and soot were always present in columnar aerosol, whereas, in variable percentages, sea salt and mineral particles characterized both dust and volcanic conditions. At the ground, sulfates characterized the amorphous matrix produced in finer stages by the evaporation of solutions of organic and inorganic aerosols. Sulfates were also one of the key players involved in heterogeneous chemical reactions, producing complex secondary aerosol, as such clay-sulfate internally mixed particle externally mixed

Quantitative effects of rapid heating on soot-particle sizing through analysis of two-pulse LII

KAUST Repository

Cenker, Emre; Roberts, William L.

2017-01-01

particle size, respectively. Overall, effects of these two processes on soot and LII model-based particle sizing are investigated by measuring the two-color time-resolved (2C-TiRe) LII signal decay from in-flame soot after two consecutive laser pulses

Smog chamber study on aging of combustion soot in isoprene/SO2/NOx system: Changes of mass, size, effective density, morphology and mixing state

Science.gov (United States)

Li, Kangwei; Chen, Linghong; Han, Ke; Lv, Biao; Bao, Kaiji; Wu, Xuecheng; Gao, Xiang; Cen, Kefa

2017-02-01

Atmospheric soot aging process is always accompanied by secondary particle formation, which is a comprehensive environmental issue that deserves great attention. On one hand, aging of primary soot could change its own physicochemical properties; on the other hand, complex air pollution caused by pollutant emission from various sources (e.g., vehicle exhausts, coal-fired flue gases and biogenic VOCs emission) may contribute to secondary particle formation onto primary particle surface. In this study, aging of combustion soot in isoprene/SO2/NOx system was investigated under controlled laboratory conditions in several smog chamber experiments. During the evolution of soot, several physical properties such as mass, size, effective density, morphology and mixing state were determined simultaneously by an integrated aerosol analytical system of Scanning Mobility Particle Sizer (SMPS), Differential Mobility Analyzer-Aerosol Particle Mass Analyzer-Condensation Particle Counter (DMA-APM-CPC) and Transmission Electron Microscopy coupled with Energy-dispersive X-ray Spectrometry (TEM/EDX) techniques. Here, based on the experimental results of soot aging under different gas-phase composition and relative humidity (RH), we firstly proposed possible aging pathways of soot in isoprene/SO2/NOx system. A synergetic effect was speculated to exist between SO2 and isoprene on soot aging process, which led to more secondary particle formation. At the same time, TEM/EDX analysis showed that a competitive mechanism between H2SO4(g) and isoprene oxidation vapor may exist: H2SO4(g) firstly condensed onto fresh soot, then an acceleration of isoprene oxidation products formed onto H2SO4 pre-coated soot. In isoprene/SO2/NOx system, high RH conditions could contribute to soot aging and new particle formation. The changes of effective density and dynamic shape factor of soot also indicated that high RH conditions could accelerate soot aging process, and led chain-like soot into more spherical

Elemental composition of aerosol particles from two atmospheric monitoring stations in the Amazon Basin

International Nuclear Information System (INIS)

Artaxo, P.; Gerab, F.; Rabello, M.L.C.

1993-01-01

One key region for the study of processes that are changing the composition of the global atmosphere is the Amazon Basin tropical rain forest. The high rate of deforestation and biomass burning is emitting large amounts of gases and fine-mode aerosol particles to the global atmosphere. Two background monitoring stations are operating continuously measuring aerosol composition, at Cuiaba, and Serra do Navio. Fine- and coarse-mode aerosol particles are being collected using stacked filter units. Particle induced X-ray emission (PIXE) was used to measure concentrations of up to 21 elements: Al, Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Se, Br, Rb, Sr, Zr, and Pb. The elemental composition was measured at the new PIXE facility from the University of Sao Paulo, using a dedicated 5SDH tandem Pelletron nuclear accelerator. Absolute principal factor analysis (APFA) has derived absolute elemental source profiles. At the Serra do Navio sampling site a very clean background aerosol is being observed. Biogenic aerosol dominates the fine-mode mass concentration, with the presence of K, P, S, Cl, Zn, Br, and FPM. Three components dominate the aerosol composition: Soil dust particles, the natural biogenic release by the forest, and a marine aerosol component. At the Cuiaba site, during the dry season, a strong component of biomass burning is observed. An aerosol mass concentration up to 120 μg/m 3 was measured. APFA showed three components: Soil dust (Al, Ca, Ti, Mn, Fe), biomass burning (soot, FPM, K, Cl) and natural biogenic particles (K, S, Ca, Mn, Zn). The fine-mode biogenic component of both sites shows remarkable similarities, although the two sampling sites are 3000 km apart. Several essential plant nutrients like P, K, S, Ca, Ni and others are transported in the atmosphere as a result of biomass burning processes. (orig.)

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the UK

Science.gov (United States)

McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

2011-05-01

Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the UK. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA observed in

Formation of secondary organic aerosol coating on black carbon particles near vehicular emissions

Science.gov (United States)

Lee, Alex K. Y.; Chen, Chia-Li; Liu, Jun; Price, Derek J.; Betha, Raghu; Russell, Lynn M.; Zhang, Xiaolu; Cappa, Christopher D.

2017-12-01

Black carbon (BC) emitted from incomplete combustion can result in significant impacts on air quality and climate. Understanding the mixing state of ambient BC and the chemical characteristics of its associated coatings is particularly important to evaluate BC fate and environmental impacts. In this study, we investigate the formation of organic coatings on BC particles in an urban environment (Fontana, California) under hot and dry conditions using a soot-particle aerosol mass spectrometer (SP-AMS). The SP-AMS was operated in a configuration that can exclusively detect refractory BC (rBC) particles and their coatings. Using the -log(NOx / NOy) ratio as a proxy for photochemical age of air masses, substantial formation of secondary organic aerosol (SOA) coatings on rBC particles was observed due to active photochemistry in the afternoon, whereas primary organic aerosol (POA) components were strongly associated with rBC from fresh vehicular emissions in the morning rush hours. There is also evidence that cooking-related organic aerosols were externally mixed from rBC. Positive matrix factorization and elemental analysis illustrate that most of the observed SOA coatings were freshly formed, providing an opportunity to examine SOA coating formation on rBCs near vehicular emissions. Approximately 7-20 wt % of secondary organic and inorganic species were estimated to be internally mixed with rBC on average, implying that rBC is unlikely the major condensation sink of SOA in this study. Comparison of our results to a co-located standard high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) measurement suggests that at least a portion of SOA materials condensed on rBC surfaces were chemically different from oxygenated organic aerosol (OOA) particles that were externally mixed with rBC, although they could both be generated from local photochemistry.

Numerical simulations on the effect of aerosols on tropospheric chemistry and range of sight; Numerische Simulationen zur Wirkung des Aerosols auf die troposphaerische Chemie und die Sichtweite

Energy Technology Data Exchange (ETDEWEB)

Riemer, N.

2002-05-01

In this study the mesoscale KAMM/DRAS model system was extended by an MADE aerosol module with a view to studying tropospheric aerosols in terms of composition and size distribution in the greatest possible detail. In particular, the MADE aerosol module was supplemented by a routine for soot. This routine involves the parameterisation of the ageing process of soot through coagulation of soot particles with soluble particles and condensation of sulphuric acid on the soot particles. This transforms the soot from an external into an internal mixture and changes its hygroscopic properties. Thus extended the model system was used to study two aspects of the effects of aerosols on the physical and chemical environment of the troposphere. The first of these two tasks was to quantify the influence of heterogeneous hydrolysis of dinitrogen pentoxide (N{sub 2}O{sub 5}) on tropospheric chemistry under summer smog conditions. The second was to study the optical properties of aerosols. The paper shows a way of deriving extinction coefficients from the calculated aerosol distributions. This is then used as a starting point for developing a method for determining range of sight. [German] Das mesoskalige Modellsystem KAMM/DRAIS wird im Rahmen dieser Arbeit um das Aerosolmodul MADE erweitert, um das troposphaerische Aerosol sowohl bezueglich seiner Zusammensetzung als auch bezueglich seiner Groessenverteilung moeglichst detailliert zu behandeln. Insbesondere wird das Aerosolmodul MADE um die Behandlung der Substanz Russ ergaenzt. Hierbei wird der Alterungsprozess von Russ durch Koagulation der Russteilchen mit loeslichen Partikeln und durch Kondensation von Schwefelsaeure auf den Russpartikeln, wodurch der Russ von einer externen in eine interne Mischung uebergeht und seine hygroskopischen Eigenschaften aendert, parametrisiert. Mit dem so erweiterten Modellsystem wird fuer zwei Themenschwerpunkte die Wirkung des Aerosols auf die physikalischen und chemischen Bedingungen in der

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the United Kingdom

Science.gov (United States)

McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

2011-09-01

Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the United Kingdom. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the United Kingdom

Directory of Open Access Journals (Sweden)

G. R. McMeeking

2011-09-01

Full Text Available Black carbon (BC aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2 measurements of refractory BC (rBC mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the United Kingdom. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA operated by the Facility for Airborne Atmospheric Measurements (FAAM. We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS and used positive matrix factorization to separate hydrocarbon-like (HOA and oxygenated organic aerosols (OOA. We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NO_x ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NO_x and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA did change for

A computational study of ethylene–air sooting flames: Effects of large polycyclic aromatic hydrocarbons

KAUST Repository

Selvaraj, Prabhu

2015-11-05

An updated reduced gas-phase kinetic mechanism was developed and integrated with aerosol models to predict soot formation characteristics in ethylene nonpremixed and premixed flames. A primary objective is to investigate the sensitivity of the soot formation to various chemical pathways for large polycyclic aromatic hydrocarbons (PAH). The gas-phase chemical mechanism adopted the KAUST-Aramco PAH Mech 1.0, which utilized the AramcoMech 1.3 for gas-phase reactions validated for up to C2 fuels. In addition, PAH species up to coronene (C24H12 or A7) were included to describe the detailed formation pathways of soot precursors. In this study, the detailed chemical mechanism was reduced from 397 to 99 species using directed relation graph with expert knowledge (DRG-X) and sensitivity analysis. The method of moments with interpolative closure (MOMIC) was employed for the soot aerosol model. Counterflow nonpremixed flames at low strain rate sooting conditions were considered, for which the sensitivity of soot formation characteristics to different nucleation pathways were investigated. Premixed flame experiment data at different equivalence ratios were also used for validation. The findings show that higher PAH concentrations result in a higher soot nucleation rate, and that the total soot volume and average size of the particles are predicted in good agreement with experimental results. Subsequently, the effects of different pathways, with respect to pyrene- or coronene-based nucleation models, on the net soot formation rate were analyzed. It was found that the nucleation processes (i.e., soot inception) are sensitive to the choice of PAH precursors, and consideration of higher PAH species beyond pyrene is critical for accurate prediction of the overall soot formation.

Ultra-small-angle X-ray scattering characterization of diesel/gasoline soot: sizes and particle-packing conditions

Science.gov (United States)

Kameya, Yuki; Lee, Kyeong O.

2013-10-01

Regulations on particulate emissions from internal combustion engines tend to become more stringent, accordingly the importance of particulate filters in the after-treatment system has been increasing. In this work, the applicability of ultra-small-angle X-ray scattering (USAXS) to diesel soot cake and gasoline soot was investigated. Gasoline-direct-injection engine soot was collected at different fuel injection timings. The unified fits method was applied to analyze the resultant scattering curves. The validity of analysis was supported by comparing with carbon black and taking the sample images using a transmission electron microscope, which revealed that the primary particle size ranged from 20 to 55 nm. In addition, the effects of particle-packing conditions on the USAXS measurement were demonstrated by using samples suspended in acetone. Then, the investigation was extended to characterization of diesel soot cake deposited on a diesel particulate filter (DPF). Diesel soot was trapped on a small piece of DPF at different deposition conditions which were specified using the Peclet number. The dependence of scattering curve on soot-deposition conditions was demonstrated. To support the interpretation of the USAXS results, soot cake samples were observed using a scanning electron microscope and the influence of particle-packing conditions on scattering curve was discussed.

Ultra-small-angle X-ray scattering characterization of diesel/gasoline soot: sizes and particle-packing conditions

International Nuclear Information System (INIS)

Kameya, Yuki; Lee, Kyeong O.

2013-01-01

Regulations on particulate emissions from internal combustion engines tend to become more stringent, accordingly the importance of particulate filters in the after-treatment system has been increasing. In this work, the applicability of ultra-small-angle X-ray scattering (USAXS) to diesel soot cake and gasoline soot was investigated. Gasoline-direct-injection engine soot was collected at different fuel injection timings. The unified fits method was applied to analyze the resultant scattering curves. The validity of analysis was supported by comparing with carbon black and taking the sample images using a transmission electron microscope, which revealed that the primary particle size ranged from 20 to 55 nm. In addition, the effects of particle-packing conditions on the USAXS measurement were demonstrated by using samples suspended in acetone. Then, the investigation was extended to characterization of diesel soot cake deposited on a diesel particulate filter (DPF). Diesel soot was trapped on a small piece of DPF at different deposition conditions which were specified using the Peclet number. The dependence of scattering curve on soot-deposition conditions was demonstrated. To support the interpretation of the USAXS results, soot cake samples were observed using a scanning electron microscope and the influence of particle-packing conditions on scattering curve was discussed

Ultra-small-angle X-ray scattering characterization of diesel/gasoline soot: sizes and particle-packing conditions

Energy Technology Data Exchange (ETDEWEB)

Kameya, Yuki, E-mail: ykameya@anl.gov; Lee, Kyeong O. [Argonne National Laboratory, Center for Transportation Research (United States)

2013-10-15

Regulations on particulate emissions from internal combustion engines tend to become more stringent, accordingly the importance of particulate filters in the after-treatment system has been increasing. In this work, the applicability of ultra-small-angle X-ray scattering (USAXS) to diesel soot cake and gasoline soot was investigated. Gasoline-direct-injection engine soot was collected at different fuel injection timings. The unified fits method was applied to analyze the resultant scattering curves. The validity of analysis was supported by comparing with carbon black and taking the sample images using a transmission electron microscope, which revealed that the primary particle size ranged from 20 to 55 nm. In addition, the effects of particle-packing conditions on the USAXS measurement were demonstrated by using samples suspended in acetone. Then, the investigation was extended to characterization of diesel soot cake deposited on a diesel particulate filter (DPF). Diesel soot was trapped on a small piece of DPF at different deposition conditions which were specified using the Peclet number. The dependence of scattering curve on soot-deposition conditions was demonstrated. To support the interpretation of the USAXS results, soot cake samples were observed using a scanning electron microscope and the influence of particle-packing conditions on scattering curve was discussed.

Comprehensive Measurement of Atmospheric Aerosols with a Wide Range Aerosol Spectrometer

International Nuclear Information System (INIS)

Keck, L; Pesch, M; Grimm, H

2011-01-01

A wide range aerosol spectrometer (WRAS) was used for comprehensive long term measurements of aerosol size distributions. The system combines the results of an optical aerosol spectrometer with the results of a Scanning Mobility Particle Sizer (SMPS) to record essentially the full size range (5 nm - 32 μm) of atmospheric particles in 72 channels. Measurements were carried out over one year (2009) at the Global Atmospheric Watch (GAW)-Station Hohenpeissenberg, Bavaria. Total particle number concentrations obtained from the aerosol size distributions were compared to the total number concentrations measured by a Condensation Particle Counter (CPC). The comparison showed an excellent agreement of the data. The high time resolution of 5 minutes allows the combination of the measured size distributions with meteorological data and correlations to gaseous pollutants (CO, NOx and SO2). A good correlation of particle number and CO concentrations was found for long distance transported small particles, which were probably mainly soot particles. Correlations to NOx were observed for aerosols from local sources such as traffic emissions. The formation of secondary aerosols from gaseous precursors was also observed. Episodes of relatively high concentration of particles in the range of 2-3 μm were probably caused by pollen.

Molecular Characterization of the Gas-Particle Interface of Soot Sampled from a Diesel Engine Using a Titration Method.

Science.gov (United States)

Tapia, A; Salgado, M S; Martín, María Pilar; Lapuerta, M; Rodríguez-Fernández, J; Rossi, M J; Cabañas, B

2016-03-15

Surface functional groups of two different types of combustion aerosols, a conventional diesel (EN 590) and a hydrotreated vegetable oil (HVO) soot, have been investigated using heterogeneous chemistry (i.e., gas-particle surface reactions). A commercial sample of amorphous carbon (Printex XE2-B) was analyzed as a reference substrate. A Knudsen flow reactor was used to carry out the experiments under molecular flow conditions. The selected gases for the titration experiments were: N(CH3)3 for the identification of acidic sites, NH2OH for the presence of carbonyl groups, CF3COOH and HCl for basic sites of different strength, and O3 and NO2 for reducing groups. Reactivity with N(CH3)3 indicates a lower density of acidic functionalities for Printex XE2-B in relation to diesel and HVO soot. Results for NH2OH experiments indicates that commercial amorphous carbon exhibits a lower abundance of available carbonyl groups at the interface compared to the results from diesel and HVO soot, the latter being the one with the largest abundance of carbonyl functions. Reactions with acids indicate the presence of weak basic oxides on the particle surface that preferentially interact with the strong acid CF3COOH. Finally, reactions with O3 and NO2 reveal that diesel and especially HVO have a significantly higher reactivity with both oxidizers compared to that of Printex XE2-B because they have more reducing sites by roughly a factor of 10 and 30, respectively. The kinetics of titration reactions have also been investigated.

Carbon Nanostructure of Diesel Soot Particles Emitted from 2 and 4 Stroke Marine Engines Burning Different Fuels.

Science.gov (United States)

Lee, Won-Ju; Park, Seul-Hyun; Jang, Se-Hyun; Kim, Hwajin; Choi, Sung Kuk; Cho, Kwon-Hae; Cho, Ik-Soon; Lee, Sang-Min; Choi, Jae-Hyuk

2018-03-01

Diesel soot particles were sampled from 2-stroke and 4-stroke engines that burned two different fuels (Bunker A and C, respectively), and the effects of the engine and fuel types on the structural characteristics of the soot particle were analyzed. The carbon nanostructures of the sampled particles were characterized using various techniques. The results showed that the soot sample collected from the 4-stroke engine, which burned Bunker C, has a higher degree of order of the carbon nanostructure than the sample collected from the 2-stroke engine, which burned Bunker A. Furthermore, the difference in the exhaust gas temperatures originating from the different engine and fuel types can affect the nanostructure of the soot emitted from marine diesel engines.

Dynamics of very small soot particles during soot burnout in diesel engines; Dynamik kleinster Russteilchen waehrend der Russausbrandphase im Dieselmotor

Energy Technology Data Exchange (ETDEWEB)

Bockhorn, H. [Karlsruhe Univ. (T.H.) (Germany). Inst. fuer Chemische Technik; Peters, N. [RWTH Aachen (DE). Institut fuer Technische Mechanik (ITM); Pittermann, R. [WTZ fuer Motoren- und Maschinenforschung Rosslau gGmbH (Germany); Hentschel, J.; Weber, J.

2003-07-01

The investigations used advanced laser-optical methods for measuring soot particle size distributions, temporally and spectrally resolved measurements of engine combustion, measurements of composition and size distribution of particles in exhaust, and further development and validation of reaction-kinetic models. In all, it can be stated that mixing will affect not only soot particle formation but also soot particle emissions. Mixing can be influenced by using a fuel-water emulsion and by CR injection. Experiments and models both showed the advantageous effects of water added to the diesel fuels and of CR injection. The higher OH radical concentrations in the later combustion stages also serve to ensure faster oxidation of soot. (orig.) [German] Ziel des Projektes war es, Informationen ueber die Bildung und Oxidation von Russ sowie die Teilchendynamik der Russteilchen waehrend der Ausbrandphase zu erhalten. Dies wurde erreicht durch die Weiterentwicklung laseroptischer Methoden zur Bestimmung der Groessenverteilung von Russpartikeln, durch zeit- und spektral aufgeloeste Erfassung der motorischen Verbrennung, durch die Bestimmung von Zusammensetzung und Groessenverteilung von Partikeln im Abgas sowie durch die Weiterentwicklung und Validierung von reaktionskinetischen Modellen. Zusammenfassend laesst sich sagen, dass sich die Gemischbildung im Dieselmotor nicht nur auf die Bildung der Russpartikel sondern auch auf die Russpartikelemission auswirkt. Die Verwendung einer Kraftstoff-Wasser-Emulsion und die Common-Rail-Einspritzung stellen zwei Verfahren zur Beeinflussung der Gemischbildung dar. Sowohl die experimentellen Untersuchungen als auch die Modellierung zeigen den die Gemischbildung foerdernden Einfluss des Zusatzes von Wasser zum Dieselbrennstoff. Ein erhoehter Anteil an vorgemischter Verbrennung, wie er auch durch die Verwendung hoher Einspritzdruecke bei der Common-Rail-Einspritzung erreicht werden kann, verringert die waehrend der Verbrennung entstehende

Black carbon aerosol properties measured by a single particle soot photometer in emissions from biomass burning in the laboratory and field

Science.gov (United States)

G. R. McMeeking; J. W. Taylor; A. P. Sullivan; M. J. Flynn; S. K. Akagi; C. M. Carrico; J. L. Collett; E. Fortner; T. B. Onasch; S. M. Kreidenweis; R. J. Yokelson; C. Hennigan; A. L. Robinson; H. Coe

2010-01-01

We present SP2 observations of BC mass, size distributions and mixing state in emissions from laboratory and field biomass fires in California, USA. Biomass burning is the primary global black carbon (BC) source, but understanding of the amount emitted and its physical properties at and following emission are limited. The single particle soot photometer (SP2) uses a...

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

Science.gov (United States)

Xu, Zhongjun; Shan, Wei; Qi, Tao; Gao, Jian

2018-05-01

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 0.5-2.5 μm and mineral particles were dominant in the size range of 2.5-10 μm. 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.

Laboratory evaluation of a gasifier particle sampling system using model compounds of different particle morphology

Energy Technology Data Exchange (ETDEWEB)

Nilsson, Patrik T.; Malik, Azhar; Pagels, Joakim; Lindskog, Magnus; Rissler, Jenny; Gudmundsson, Anders; Bohgard, Mats; Sanati, Mehri [Lund University, Division of Ergonomics and Aerosol Technology, P.O. Box 118, Lund (Sweden)

2011-07-15

The objective of this work was to design and evaluate an experimental setup to be used for field studies of particle formation in biomass gasification processes. The setup includes a high-temperature dilution probe and a denuder to separate solid particles from condensable volatile material. The efficiency of the setup to remove volatile material from the sampled stream and the influence from condensation on particles with different morphologies is presented. In order to study the sampling setup model, aerosols were created with a nebulizer to produce compact and solid KCl particles and a diffusion flame burner to produce agglomerated and irregular soot particles. The nebulizer and soot generator was followed by an evaporation-condensation section where volatile material, dioctylsebacete (DOS), was added to the system as a tar model compound. The model aerosol particles were heated to 200 C to create a system containing both solid particles and volatile organic material in gas phase. The heated aerosol particles were sampled and diluted at the same temperature with the dilution probe. Downstream the probe, the DOS was adsorbed in the denuder. This was achieved by slowly decreasing the temperature of the diluted sample towards ambient level in the denuder. Thereby the supersaturation of organic vapors was reduced which decreased the probability for tar condensation and nucleation of new particles. Both the generation system and the sampling technique gave reproducible results. A DOS collection efficiency of >99% was achieved if the denuder inlet concentration was diluted to less than 1-6 mg/m{sup 3} depending on the denuder flow rate. Concentrations higher than that lead to significant impact on the resulting KCl size distribution. The choice of model compounds was done to study the effect from the particle morphology on the achieved particle characteristics after the sampling setup. When similar amounts of volatile material condensed on soot agglomerates and

Stratospheric Aerosol Measurements

Science.gov (United States)

Pueschel, Rudolf, F.; Gore, Warren J. (Technical Monitor)

1998-01-01

Stratospheric aerosols affect the atmospheric energy balance by scattering and absorbing solar and terrestrial radiation. They also can alter stratospheric chemical cycles by catalyzing heterogeneous reactions which markedly perturb odd nitrogen, chlorine and ozone levels. Aerosol measurements by satellites began in NASA in 1975 with the Stratospheric Aerosol Measurement (SAM) program, to be followed by the Stratospheric Aerosol and Gas Experiment (SAGE) starting in 1979. Both programs employ the solar occultation, or Earth limb extinction, techniques. Major results of these activities include the discovery of polar stratospheric clouds (PSCs) in both hemispheres in winter, illustrations of the impacts of major (El Chichon 1982 and Pinatubo 1991) eruptions, and detection of a negative global trend in lower stratospheric/upper tropospheric aerosol extinction. This latter result can be considered a triumph of successful worldwide sulfur emission controls. The SAGE record will be continued and improved by SAGE III, currently scheduled for multiple launches beginning in 2000 as part of the Earth Observing System (EOS). The satellite program has been supplemented by in situ measurements aboard the ER-2 (20 km ceiling) since 1974, and from the DC-8 (13 km ceiling) aircraft beginning in 1989. Collection by wire impactors and subsequent electron microscopic and X-ray energy-dispersive analyses, and optical particle spectrometry have been the principle techniques. Major findings are: (1) The stratospheric background aerosol consists of dilute sulfuric acid droplets of around 0.1 micrometer modal diameter at concentration of tens to hundreds of monograms per cubic meter; (2) Soot from aircraft amounts to a fraction of one percent of the background total aerosol; (3) Volcanic eruptions perturb the sulfuric acid, but not the soot, aerosol abundance by several orders of magnitude; (4) PSCs contain nitric acid at temperatures below 195K, supporting chemical hypotheses

Laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF): performance, reference spectra and classification of atmospheric samples

Science.gov (United States)

Shen, Xiaoli; Ramisetty, Ramakrishna; Mohr, Claudia; Huang, Wei; Leisner, Thomas; Saathoff, Harald

2018-04-01

The laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF, AeroMegt GmbH) is able to identify the chemical composition and mixing state of individual aerosol particles, and thus is a tool for elucidating their impacts on human health, visibility, ecosystem, and climate. The overall detection efficiency (ODE) of the instrument we use was determined to range from ˜ (0.01 ± 0.01) to ˜ (4.23 ± 2.36) % for polystyrene latex (PSL) in the size range of 200 to 2000 nm, ˜ (0.44 ± 0.19) to ˜ (6.57 ± 2.38) % for ammonium nitrate (NH4NO3), and ˜ (0.14 ± 0.02) to ˜ (1.46 ± 0.08) % for sodium chloride (NaCl) particles in the size range of 300 to 1000 nm. Reference mass spectra of 32 different particle types relevant for atmospheric aerosol (e.g. pure compounds NH4NO3, K2SO4, NaCl, oxalic acid, pinic acid, and pinonic acid; internal mixtures of e.g. salts, secondary organic aerosol, and metallic core-organic shell particles; more complex particles such as soot and dust particles) were determined. Our results show that internally mixed aerosol particles can result in spectra with new clusters of ions, rather than simply a combination of the spectra from the single components. An exemplary 1-day ambient data set was analysed by both classical fuzzy clustering and a reference-spectra-based classification method. Resulting identified particle types were generally well correlated. We show how a combination of both methods can greatly improve the interpretation of single-particle data in field measurements.

Climate impact of anthropogenic aerosols on cirrus clouds

Science.gov (United States)

Penner, J.; Zhou, C.

2017-12-01

Cirrus clouds have a net warming effect on the atmosphere and cover about 30% of the Earth's area. Aerosol particles initiate ice formation in the upper troposphere through modes of action that include homogeneous freezing of solution droplets, heterogeneous nucleation on solid particles immersed in a solution, and deposition nucleation of vapor onto solid particles. However, the efficacy with which particles act to form cirrus particles in a model depends on the representation of updrafts. Here, we use a representation of updrafts based on observations of gravity waves, and follow ice formation/evaporation during both updrafts and downdrafts. We examine the possible change in ice number concentration from anthropogenic soot originating from surface sources of fossil fuel and biomass burning and from aircraft particles that have previously formed ice in contrails. Results show that fossil fuel and biomass burning soot aerosols with this version exert a radiative forcing of -0.15±0.02 Wm-2 while aircraft aerosols that have been pre-activated within contrails exert a forcing of -0.20±0.06 Wm-2, but it is possible to decrease these estimates of forcing if a larger fraction of dust particles act as heterogeneous ice nuclei. In addition aircraft aerosols may warm the climate if a large fraction of these particles act as ice nuclei. The magnitude of the forcing in cirrus clouds can be comparable to the forcing exerted by anthropogenic aerosols on warm clouds. This assessment could therefore support climate models with high sensitivity to greenhouse gas forcing, while still allowing the models to fit the overall historical temperature change.

Simulation and analysis of the soot particle size distribution in a turbulent nonpremixed flame

KAUST Repository

Lucchesi, Marco

2017-02-05

A modeling framework based on Direct Simulation Monte Carlo (DSMC) is employed to simulate the evolution of the soot particle size distribution in turbulent sooting flames. The stochastic reactor describes the evolution of soot in fluid parcels following Lagrangian trajectories in a turbulent flow field. The trajectories are sampled from a Direct Numerical Simulation (DNS) of a n-heptane turbulent nonpremixed flame. The DSMC method is validated against experimentally measured size distributions in laminar premixed flames and found to reproduce quantitatively the experimental results, including the appearance of the second mode at large aggregate sizes and the presence of a trough at mobility diameters in the range 3–8 nm. The model is then applied to the simulation of soot formation and growth in simplified configurations featuring a constant concentration of soot precursors and the evolution of the size distribution in time is found to depend on the intensity of the nucleation rate. Higher nucleation rates lead to a higher peak in number density and to the size distribution attaining its second mode sooner. The ensemble-averaged PSDF in the turbulent flame is computed from individual samples of the PSDF from large sets of Lagrangian trajectories. This statistical measure is equivalent to time-averaged, scanning mobility particle size (SMPS) measurements in turbulent flames. Although individual trajectories display strong bimodality as in laminar flames, the ensemble-average PSDF possesses only one mode and a long, broad tail, which implies significant polydispersity induced by turbulence. Our results agree very well with SMPS measurements available in the literature. Conditioning on key features of the trajectory, such as mixture fraction or radial locations does not reduce the scatter in the size distributions and the ensemble-averaged PSDF remains broad. The results highlight and explain the important role of turbulence in broadening the size distribution of

Investigation of mass and energy coupling between soot particles and gas species in modelling ethylene counterflow diffusion flames

NARCIS (Netherlands)

Zimmer, L.; Pereira, F.M.; van Oijen, J.A.; de Goey, L.P.H.

2017-01-01

A numerical model is developed aiming at investigating soot formation in ethylene counterflow diffusion flames. The mass and energy coupling between soot solid particles and gas-phase species is investigated in detail. A semi-empirical two-equation model is chosen for predicting soot mass fraction

Comparison of the tribology performance of nano-diesel soot and graphite particles as lubricant additives

International Nuclear Information System (INIS)

Zhang, Zu-chuan; Cai, Zhen-bing; Peng, Jin-fang; Zhu, Min-hao

2016-01-01

The tribology behavior of exhaust diesel soot as a lubricant additive was investigated and then compared with that of a selection of commercial nano-graphite particles. Specifically, 0.01 wt% particles were dispersed in PAO4 oil with 1 wt% sorbitan monooleate (Span 80) as a dispersing agent, and wear tests based on the ball against plate mode were conducted at various temperatures. Different analytical techniques (e.g. transmission electron, scanning electron and infrared microscopy; energy dispersive x-ray and Raman spectroscopy; and charge measurement) were employed to characterize the chemistry and morphology of the additives and their tribology performance. The oil containing only 0.01 wt% diesel soot clearly improved wear resistance over 60 °C. In particular, at 100 °C the wear rate decreased by approximately 90% compared to the function of base oil. In the same test conditions, diesel soot exhibited better anti-wear performance than nano-graphite at high temperatures. The potential measure showed that the nano-graphite had positive charge and the diesel soot had negative charge. Electrochemical action may play an important role in the lubricant mechanisms of diesel soot and graphite as oil additives. (paper)

A review of optical measurements at the aerosol and cloud chamber AIDA

International Nuclear Information System (INIS)

Wagner, Robert; Linke, Claudia; Naumann, Karl-Heinz; Schnaiter, Martin; Vragel, Marlen; Gangl, Martin; Horvath, Helmuth

2009-01-01

This paper provides a survey of recent studies on the optical properties of aerosol and cloud particles that have been conducted at the AIDA facility of Forschungszentrum Karlsruhe (Aerosol Interactions and Dynamics in the Atmosphere). Reflecting the broad accessible temperature range of the AIDA chamber which extends from ambient temperature down to 183 K, the investigations feature a broad diversity of research topics, such as the wavelength-dependence of the specific absorption cross sections of soot and mineral dust aerosols at room temperature, depolarization and infrared extinction measurements of ice crystal clouds generated at temperatures below 235 K, and the optical properties of polar stratospheric cloud constituents whose formation was studied in chamber experiments at temperatures well below 200 K. After reviewing the AIDA research activity of the past decade and introducing the optical instrumentation of the AIDA facility, this paper presents illustrative examples of ongoing and already published work on optical measurements of soot aerosols, mineral dust particles, and ice crystal clouds.

Subsonic aircraft soot. A tracer documenting barriers to inter-hemispheric mixing

Energy Technology Data Exchange (ETDEWEB)

Pueschel, R F [NASA Ames Research Center, Moffett Field, CA (United States)

1998-12-31

Meridional observations of soot aerosols and radioactive {sup 14}C, and models of the geographic distribution of nuclear bomb-released {sup 14}C and aircraft-emitted NO{sub x}, all show strong gradients between the hemispheres. Reason for it are decade-long inter-hemispheric mixing times which are much in excess of yearlong stratospheric residence times of tracers. Vertical mixing of soot aerosol is not corroborated by {sup 14}C observations. The reason could be radiometric forces that act on strongly absorbing soot. (author) 10 refs.

Subsonic aircraft soot. A tracer documenting barriers to inter-hemispheric mixing

Energy Technology Data Exchange (ETDEWEB)

Pueschel, R.F. [NASA Ames Research Center, Moffett Field, CA (United States)

1997-12-31

Meridional observations of soot aerosols and radioactive {sup 14}C, and models of the geographic distribution of nuclear bomb-released {sup 14}C and aircraft-emitted NO{sub x}, all show strong gradients between the hemispheres. Reason for it are decade-long inter-hemispheric mixing times which are much in excess of yearlong stratospheric residence times of tracers. Vertical mixing of soot aerosol is not corroborated by {sup 14}C observations. The reason could be radiometric forces that act on strongly absorbing soot. (author) 10 refs.

Laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF: performance, reference spectra and classification of atmospheric samples

Directory of Open Access Journals (Sweden)

X. Shen

2018-04-01

Full Text Available The laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF, AeroMegt GmbH is able to identify the chemical composition and mixing state of individual aerosol particles, and thus is a tool for elucidating their impacts on human health, visibility, ecosystem, and climate. The overall detection efficiency (ODE of the instrument we use was determined to range from  ∼  (0.01 ± 0.01 to  ∼  (4.23 ± 2.36 % for polystyrene latex (PSL in the size range of 200 to 2000 nm,  ∼  (0.44 ± 0.19 to  ∼  (6.57 ± 2.38 % for ammonium nitrate (NH4NO3, and  ∼  (0.14 ± 0.02 to  ∼  (1.46 ± 0.08 % for sodium chloride (NaCl particles in the size range of 300 to 1000 nm. Reference mass spectra of 32 different particle types relevant for atmospheric aerosol (e.g. pure compounds NH4NO3, K2SO4, NaCl, oxalic acid, pinic acid, and pinonic acid; internal mixtures of e.g. salts, secondary organic aerosol, and metallic core–organic shell particles; more complex particles such as soot and dust particles were determined. Our results show that internally mixed aerosol particles can result in spectra with new clusters of ions, rather than simply a combination of the spectra from the single components. An exemplary 1-day ambient data set was analysed by both classical fuzzy clustering and a reference-spectra-based classification method. Resulting identified particle types were generally well correlated. We show how a combination of both methods can greatly improve the interpretation of single-particle data in field measurements.

TEM and HRTEM of Soot-in-oil particles and agglomerates from internal combustion engines

International Nuclear Information System (INIS)

Fay, M W; Rocca, A La; Shayler, P J

2014-01-01

Over time, the performance of lubricating oil in a diesel engine is affected by the build-up of carbon soot produced by the combustion process. TEM and HRTEM are commonly used to investigate the characteristics of individual and agglomerated particles from diesel exhaust, to understand the structure and distribution of the carbon sheets in the primary particles and the nanostructure morphology. However, high resolution imaging of soot-in-oil is more challenging, as mineral oil is a contaminant for the electron microscope and leads to instability under the electron beam. In this work we compare solvent extraction and centrifugation techniques for removing the mineral oil contaminant, and the effect on particle size distribution

Comprehensive Laser-induced Incandescence (LII) modeling for soot particle sizing

KAUST Repository

Lisanti, Joel

2015-03-30

To evaluate the current state of the art in LII particle sizing, a comprehensive model for predicting the temporal incandescent response of combustion-generated soot to absorption of a pulsed laser is presented. The model incorporates particle heating through laser absorption, thermal annealing, and oxidation at the surface as well as cooling through sublimation and photodesorption, radiation, conduction and thermionic emission. Thermodynamic properties and the thermal accommodation coefficient utilized in the model are temperature dependent. In addition, where appropriate properties are also phase dependent, thereby accounting for annealing effects during laser heating and particle cooling.

Simulation of soot size distribution in an ethylene counterflow flame

KAUST Repository

Zhou, Kun

2014-01-06

Soot, an aggregate of carbonaceous particles produced during the rich combustion of fossil fuels, is an undesirable pollutant and health hazard. Soot evolution involves various dynamic processes: nucleation soot formation from polycyclic aromatic hydrocarbons (PAHs) condensation PAHs condensing on soot particle surface surface processes hydrogen-abstraction-C2H2-addition, oxidation coagulation two soot particles coagulating to form a bigger particle This simulation work investigates soot size distribution and morphology in an ethylene counterflow flame, using i). Chemkin with a method of moments to deal with the coupling between vapor consumption and soot formation; ii). Monte Carlo simulation of soot dynamics.

Reservoir patterns of soot, organic particles, total carbon, soluble substances and aerosols (numbers and mass) in the droplet and interstitial phase of clouds; Reservoiraufteilung von Russ, organischen Bestandteilen, Gesamtkohlenstoff, loeslichen Substanzen und Aerosolpartikeln (Anzahl und Masse) in der Tropfen- und Zwischenraumphase von Wolken. Abschlussbericht

Energy Technology Data Exchange (ETDEWEB)

Wieprecht, W.; Acker, K.; Moeller, D.; Auel, R.; Hofmeister, J.; Kalass, D.

2002-07-01

The reservoir patterns of the constitutents of representative clouds over Germany were investigated for a better characterisation of their optical, microphysical and chemical properties. One of the key points of interest was the distribution of carbonaceous aerosol particles in the droplet and interstitial phase, which was to provide information on the role of absorbing (soot or BC) and organic carbon (OC) in cloud formation. Data about the effects of potential CCN on cloud characteristics and about the changes in aerosol particles induced by cloud processes are required as input for models of the chemical and climate effects of atmospheric aerosol. [German] Ziel des Projektes war eine moeglichst umfassende experimentelle Ermittlung der Reservoiraufteilung der Inhaltsstoffe repraesentativer Wolken ueber der Bundesrepublik Deutschland, um ihre optischen, mikrophysikalischen und chemischen Eigenschaften besser zu charakterisieren. Ein besonderer Schwerpunkt des Gesamtprojekts lag auf der Bestimmung der Verteilung kohlenstoffhaltiger Aerosolpartikel auf die Tropfen- und interstitielle Phase, um Aufschluesse ueber die Rolle von absorbierendem (Russ oder BC) und organischem Kohlenstoff (OC) bei der Wolkenbildung zu erhalten. Erkenntnisse sowohl ueber die Beeinflussung potentieller CCN auf Wolkeneigenschaften als auch ueber die Veraenderung der Aerosolpartikel durch Wolkenprozesse sind erforderlich als Eingangsdaten in entsprechende Modelle, um die chemischen und klimatischen Effekte des atmosphaerischen Aerosols zu bestimmen. (orig.)

Mass spectrometric analysis and aerodynamic properties of various types of combustion-related aerosol particles

Science.gov (United States)

Schneider, J.; Weimer, S.; Drewnick, F.; Borrmann, S.; Helas, G.; Gwaze, P.; Schmid, O.; Andreae, M. O.; Kirchner, U.

2006-12-01

Various types of combustion-related particles in the size range between 100 and 850 nm were analyzed with an aerosol mass spectrometer and a differential mobility analyzer. The measurements were performed with particles originating from biomass burning, diesel engine exhaust, laboratory combustion of diesel fuel and gasoline, as well as from spark soot generation. Physical and morphological parameters like fractal dimension, effective density, bulk density and dynamic shape factor were derived or at least approximated from the measurements of electrical mobility diameter and vacuum aerodynamic diameter. The relative intensities of the mass peaks in the mass spectra obtained from particles generated by a commercial diesel passenger car, by diesel combustion in a laboratory burner, and by evaporating and re-condensing lubrication oil were found to be very similar. The mass spectra from biomass burning particles show signatures identified as organic compounds like levoglucosan but also others which are yet unidentified. The aerodynamic behavior yielded a fractal dimension (Df) of 2.09 +/- 0.06 for biomass burning particles from the combustion of dry beech sticks, but showed values around three, and hence more compact particle morphologies, for particles from combustion of more natural oak. Scanning electron microscope images confirmed the finding that the beech combustion particles were fractal-like aggregates, while the oak combustion particles displayed a much more compact shape. For particles from laboratory combusted diesel fuel, a Df value of 2.35 was found, for spark soot particles, Df [approximate] 2.10. The aerodynamic properties of fractal-like particles from dry beech wood combustion indicate an aerodynamic shape factor [chi] that increases with electrical mobility diameter, and a bulk density of 1.92 g cm-3. An upper limit of [chi] [approximate] 1.2 was inferred for the shape factor of the more compact particles from oak combustion.

Facile synthesis of nano cauliflower and nano broccoli like hierarchical superhydrophobic composite coating using PVDF/carbon soot particles via gelation technique.

Science.gov (United States)

Sahoo, Bichitra Nanda; Balasubramanian, Kandasubramanian

2014-12-15

We have elucidated a cost effective fabrication technique to produce superhydrophobic polyvinylidene fluoride (PVDF/DMF/candle soot particle and PVDF/DMF/camphor soot particle composite) porous materials. The water repellent dry composite was formed by the interaction of non-solvent (methanol) into PVDF/carbon soot particles suspension in N,N-dimethylformamide (DMF). It is seen that longer quenching time effectively changes the surface morphology of dry composites. The nano broccoli like hierarchical microstructure with micro or nano scaled roughen surface was obtained for PVDF/DMF/camphor soot particle, which reveals water contact angle of 172° with roll off angle of 2°. However, composite coating of PVDF/DMF/candle soot particle shows nano cauliflower like hierarchical, which illustrates water contact angle of 169° with roll off angle of 3°. To elucidate the enhancement of water repellent property of PVDF composites, we further divulge the evolution mechanism of nano cauliflower and nano broccoli structure. In order to evaluate the water contact angle of PVDF composites, surface diffusion of water inside the pores is investigated. Furthermore, the addition of small amount of carbon soot particles in composite not only provides the crystallization of PVDF, but also leads to dramatical amendment of surface morphology which increases the surface texture and roughness for superhydrophobicity. Copyright © 2014 Elsevier Inc. All rights reserved.

Numerical investigation on soot particles emission in compression ignition diesel engine by using particulate mimic soot model

Directory of Open Access Journals (Sweden)

Ibrahim Fadzli

2017-01-01

Full Text Available Research via computational method, specifically by detailed-kinetic soot model offers much more advantages than the simple model as more detailed formation/oxidation process is taken into consideration, thus providing better soot mass concentration, soot size, soot number density as well as information regarding other related species. In the present computational study, investigation of in-cylinder soot concentration as well as other emissions in a single cylinder diesel engine has been conducted, using a commercial multidimensional CFD software, CONVERGE CFD. The simulation was carried out for a close-cycle combustion environment from inlet valve closing (IVC to exhaust valve opening (EVO. In this case, detailed-kinetic Particulate Mimic (PM soot model was implemented as to take benefit of the method of moment, instead of commonly implemented simple soot model. Analyses of the results are successfully plotted to demonstrate that the soot size and soot mass concentration are strongly dependent on the detailed soot formation and oxidation process rates. The calculated of soot mass concentration and average soot size at EVO provide the end value of 29.2 mg/m3 and 2.04 × 10−8 m, respectively. Besides, post-processing using EnSight shows the qualitative results of soot concentration along simulation period in the combustion chamber.

Size-resolved measurement of the mixing state of soot in the megacity Beijing, China: diurnal cycle, aging and parameterization

Directory of Open Access Journals (Sweden)

Y. F. Cheng

2012-05-01

Full Text Available Soot particles are the most efficient light absorbing aerosol species in the atmosphere, playing an important role as a driver of global warming. Their climate effects strongly depend on their mixing state, which significantly changes their light absorbing capability and cloud condensation nuclei (CCN activity. Therefore, knowledge about the mixing state of soot and its aging mechanism becomes an important topic in the atmospheric sciences.

The size-resolved (30–320 nm diameter mixing state of soot particles in polluted megacity air was measured at a suburban site (Yufa during the CAREBeijing 2006 campaign in Beijing, using a volatility tandem differential mobility analyzer (VTDMA. Particles in this size range with non-volatile residuals at 300 °C were considered to be soot particles. On average, the number fraction of internally mixed soot in total soot particles (F_in, decreased from 0.80 to 0.57 when initial D_p increased from 30 to 320 nm. Further analysis reveals that: (1 F_in was well correlated with the aerosol hygroscopic mixing state measured by a CCN counter. More externally mixed soot particles were observed when particles showed more heterogeneous features with regard to hygroscopicity. (2 F_in had pronounced diurnal cycles. For particles in the accumulation mode (D_p at 100–320 nm, largest F_in were observed at noon time, with "apparent" turnover rates (k_{ex → in} up to 7.8% h⁻¹. (3 F_in was subject to competing effects of both aging and emissions. While aging increases F_in by converting externally mixed soot particles into internally mixed ones, emissions tend to reduce F_in by emitting more fresh and externally mixed soot particles. Similar competing effects were also found with air mass age indicators. (4 Under the estimated emission

International Workshop on Stratospheric Aerosols: Measurements, Properties, and Effects

Science.gov (United States)

Pueschel, Rudolf F. (Editor)

1991-01-01

Following a mandate by the International Aerosol Climatology Program under the auspices of International Association of Meteorology and Atmospheric Physics International Radiation Commission, 45 scientists from five nations convened to discuss relevant issues associated with the measurement, properties, and effects of stratospheric aerosols. A summary is presented of the discussions on formation and evolution, transport and fate, effects on climate, role in heterogeneous chemistry, and validation of lidar and satellite remote sensing of stratospheric aerosols. Measurements are recommended of the natural (background) and the volcanically enhanced aerosol (sulfuric acid and silica particles), the exhaust of shuttle, civil aviation and supersonic aircraft operations (alumina, soot, and ice particles), and polar stratospheric clouds (ice, condensed nitric and hydrochloric acids).

Development and Characterization of a Thermodenuder for Aerosol Volatility Measurements

Energy Technology Data Exchange (ETDEWEB)

Dr. Timothy Onasch

2009-09-09

due to coatings on soot particles). The successfully completed Phase I project included construction of a prototype design for the TD with detailed physical modeling, testing with laboratory and ambient aerosol particles, and the initiation of a detailed microphysical model of the aerosol particles passing through the TD to extract vapor pressure distributions. The objective of the microphysical model is to derive vapor pressure distributions (i.e. vapor pressure ranges, including single chemical compounds, mixtures of known compounds, and complex ‘real-world’ aerosols, such as SOA, and soot particles with absorbing and nonabsorbing coatings) from TD measurements of changes in particle size, mass, and chemical composition for known TD temperatures and flow rates (i.e. residence times). The proposed Phase II project was designed to optimize several TD systems for different instrument applications and to combine the hardware and modeling into a robust package for commercial sales.

Morphological transformation of soot: investigation of microphysical processes during the condensation of sulphuric acid and limonene ozonolysis products vapours

Science.gov (United States)

Pathak, R. K. P.; Pei, X.; Hallquist, M.; Pagels, J. H.

2017-12-01

Morphological transformation of soot particle by condensation of low volatility materials on it is a dominant atmospheric process with serious implications for its optical and hygroscopic properties, and atmospheric lifetime. In this study, the morphological transformation of soot agglomerate under the influence of condensation of vapours of sulphuric acid, and/or limonene ozonolysis products were investigated systematically using a Differential Mobility Analyser-Aerosol Particle Mass Analyser (DMA-APM) and the Tandem DMA techniques integrated with a laminar flow-tube system. We discovered that the morphology transformation of soot in general was a sequence of two-step process, i.e. (i) filling of void space within soot agglomerate; (ii) growth of particle diameter. These two steps followed and complimented each other. In the very beginning the filling was the dominant process followed by growth until it led to the accumulation of enough material that in turn exerted surface forces that eventually facilitated the further filling. The filling of void space was constrained by the initial morphology of fresh soot and the nature and amount of the material condensed. This process continued in several sequential steps until all void space within the soot agglomerate was filled completely and then growth of a spherical particle continued as long as mass was condensed on it. In this study, we developed a framework to quantify the microphysical transformation of soot upon the condensation of various materials. The framework utilized experimental data and hypothesis of ideal sphere growth and filling of voids to quantify the distribution of condensed materials in these two processes complimenting each other. Using this framework, we have quantified the percentage of material that went into processes of particle growth and void filling at each step. Using the same framework, we further estimated the fraction of internal voids and open voids and used this information to derive

Sooting turbulent jet flame: characterization and quantitative soot measurements

Science.gov (United States)

Köhler, M.; Geigle, K. P.; Meier, W.; Crosland, B. M.; Thomson, K. A.; Smallwood, G. J.

2011-08-01

Computational fluid dynamics (CFD) modelers require high-quality experimental data sets for validation of their numerical tools. Preferred features for numerical simulations of a sooting, turbulent test case flame are simplicity (no pilot flame), well-defined boundary conditions, and sufficient soot production. This paper proposes a non-premixed C2H4/air turbulent jet flame to fill this role and presents an extensive database for soot model validation. The sooting turbulent jet flame has a total visible flame length of approximately 400 mm and a fuel-jet Reynolds number of 10,000. The flame has a measured lift-off height of 26 mm which acts as a sensitive marker for CFD model validation, while this novel compiled experimental database of soot properties, temperature and velocity maps are useful for the validation of kinetic soot models and numerical flame simulations. Due to the relatively simple burner design which produces a flame with sufficient soot concentration while meeting modelers' needs with respect to boundary conditions and flame specifications as well as the present lack of a sooting "standard flame", this flame is suggested as a new reference turbulent sooting flame. The flame characterization presented here involved a variety of optical diagnostics including quantitative 2D laser-induced incandescence (2D-LII), shifted-vibrational coherent anti-Stokes Raman spectroscopy (SV-CARS), and particle image velocimetry (PIV). Producing an accurate and comprehensive characterization of a transient sooting flame was challenging and required optimization of these diagnostics. In this respect, we present the first simultaneous, instantaneous PIV, and LII measurements in a heavily sooting flame environment. Simultaneous soot and flow field measurements can provide new insights into the interaction between a turbulent vortex and flame chemistry, especially since soot structures in turbulent flames are known to be small and often treated in a statistical manner.

Structural effects on the oxidation of soot particles by O2: Experimental and theoretical study

KAUST Repository

Raj, Abhijeet

2013-09-01

Soot particles are composed of polycyclic aromatic hydrocarbons (PAHs), which have either planar or curved structures. The oxidation behaviors of soot particles differ depending on their structures, arrangement of PAHs, and the type of surface functional groups. The oxidation rate of curved PAHs in soot is thought to be higher than that of planar ones. To understand the role that PAH structure plays in soot reactivity towards O2, experimental studies are conducted on two types of commercially produced soot, Printex-U and Fullerene soot, using high resolution transmission electron microscopy, electron energy loss spectroscopy, thermo-gravimetric analysis and elemental analysis. The relative concentrations of active sites, oxygenated functional groups, aliphatics and aromatics present in soots are evaluated. The activation energies for soot oxidation at different conversion levels are determined. The average activation energies of the two soots are found to differ by 26kJ/mol. To understand the reason for this difference, quantum calculations using density functional (B3LYP) and Hartree-Fock theories are conducted to study the reaction pathways of the oxidation by O2 of planar and curved PAHs using 4-pyrenyl and 1-corannulenyl as their model molecules, respectively. The energetically preferred channels for curved PAH oxidation differ from the planar one. The addition of O2 on a radical site of a six-membered ring to form a peroxyl radical is found to be barrierless for both the model PAHs. For peroxyl decomposition, three pathways are suggested, each of which involve the activation energies of 108, 170 and 121kJ/mol to form stable molecules in the case of planar PAH, and 94, 155 and 125kJ/mol in the case of curved PAH. During the oxidation of a five-membered ring, to form stable molecules, the activation energies of 90kJ/mol for the curved PAH and 169kJ/mol for the planar PAH relative to the energy of the peroxyl radical are required. The low activation barriers of

Biomass Burning Research Using DOE ARM Single-Particle Soot Photometer (SP2) Field Campaign Report

Energy Technology Data Exchange (ETDEWEB)

Onasch, Timothy B [Aerodyne Research, Inc., Billerica, MA (United States); Sedlacek, Arthur J [Brookhaven National Lab. (BNL), Upton, NY (United States); Lewis, Ernie [Brookhaven National Lab. (BNL), Upton, NY (United States)

2017-03-01

The focus of this laboratory study was to investigate the chemical and optical properties, and the detection efficiencies, of tar balls generated in the laboratory using the same instruments deployed on the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility Gulfstream-1 (G-1) aircraft during the 2013 Biomass Burning Observation Project (BBOP) field study, during which tar balls were observed in wildland biomass burning particulate emissions. Key goals of this laboratory study were: (a) measuring the chemical composition of tar balls to provide insights into the atmospheric processes that form (evaporation/oxidation) and modify them in biomass burning plumes, (b) identifying whether tar balls contain refractory black carbon, (c) determining the collection efficiencies of tar balls impacting on the 600oC heated tungsten vaporizer in the Aerodyne Soot Particle Aerosol Mass Spectrometer (SP-AMS) (i.e., given the observed low volatilities, AMS measurements might underestimate organic biomass burning plume loadings), and (d) measuring the wavelength-dependent, mass-specific absorption cross-sections of brown carbon components of tar balls. This project was funded primarily by the DOE Atmospheric System Research (ASR) program, and the ARM Facility made their single-particle soot photometer (SP2) available for September 1-September 31, 2016 in the Aerodyne laboratories. The ARM mentor (Dr. Sedlacek) requested no funds for mentorship or data reduction. All ARM SP2 data collected as part of this project are archived in the ARM Data Archive in accordance with established protocols. The main objectives of the ARM Biomass Burning Observation Period (BBOP, July-October, 2013) field campaign were to (1) assess the impact of wildland fires in the Pacific Northwest on climate, through near-field and regional intensive measurement campaigns, and (2) investigate agricultural burns to determine how those biomass burn plumes differ from

Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic

Science.gov (United States)

Kirpes, Rachel M.; Bondy, Amy L.; Bonanno, Daniel; Moffet, Ryan C.; Wang, Bingbing; Laskin, Alexander; Ault, Andrew P.; Pratt, Kerri A.

2018-03-01

Few measurements of aerosol chemical composition have been made during the winter-spring transition (following polar sunrise) to constrain Arctic aerosol-cloud-climate feedbacks. Herein, we report the first measurements of individual particle chemical composition near Utqiaġvik (Barrow), Alaska, in winter (seven sample days in January and February 2014). Individual particles were analyzed by computer-controlled scanning electron microscopy with energy dispersive X-ray spectroscopy (CCSEM-EDX, 24 847 particles), Raman microspectroscopy (300 particles), and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS, 290 particles). Sea spray aerosol (SSA) was observed in all samples, with fresh and aged SSA comprising 99 %, by number, of 2.5-7.5 µm diameter particles, 65-95 % from 0.5-2.5 µm, and 50-60 % from 0.1-0.5 µm, indicating SSA is the dominant contributor to accumulation and coarse-mode aerosol during the winter. The aged SSA particles were characterized by reduced chlorine content with 94 %, by number, internally mixed with secondary sulfate (39 %, by number, internally mixed with both nitrate and sulfate), indicative of multiphase aging reactions during transport. There was a large number fraction (40 % of 1.0-4.0 µm diameter particles) of aged SSA during periods when particles were transported from near Prudhoe Bay, consistent with pollutant emissions from the oil fields participating in atmospheric processing of aerosol particles. Organic carbon and sulfate particles were observed in all samples and comprised 40-50 %, by number, of 0.1-0.4 µm diameter particles, indicative of Arctic haze influence. Soot was internally mixed with organic and sulfate components. All sulfate was mixed with organic carbon or SSA particles. Therefore, aerosol sources in the Alaskan Arctic and resulting aerosol chemical mixing states need to be considered when predicting aerosol climate effects, particularly cloud

The Impact of Aerosol Particle Mixing State on the Hygroscopicity of Sea Spray Aerosol.

Science.gov (United States)

Schill, Steven R; Collins, Douglas B; Lee, Christopher; Morris, Holly S; Novak, Gordon A; Prather, Kimberly A; Quinn, Patricia K; Sultana, Camille M; Tivanski, Alexei V; Zimmermann, Kathryn; Cappa, Christopher D; Bertram, Timothy H

2015-06-24

Aerosol particles influence global climate by determining cloud droplet number concentrations, brightness, and lifetime. Primary aerosol particles, such as those produced from breaking waves in the ocean, display large particle-particle variability in chemical composition, morphology, and physical phase state, all of which affect the ability of individual particles to accommodate water and grow into cloud droplets. Despite such diversity in molecular composition, there is a paucity of methods available to assess how particle-particle variability in chemistry translates to corresponding differences in aerosol hygroscopicity. Here, an approach has been developed that allows for characterization of the distribution of aerosol hygroscopicity within a chemically complex population of atmospheric particles. This methodology, when applied to the interpretation of nascent sea spray aerosol, provides a quantitative framework for connecting results obtained using molecular mimics generated in the laboratory with chemically complex ambient aerosol. We show that nascent sea spray aerosol, generated in situ in the Atlantic Ocean, displays a broad distribution of particle hygroscopicities, indicative of a correspondingly broad distribution of particle chemical compositions. Molecular mimics of sea spray aerosol organic material were used in the laboratory to assess the volume fractions and molecular functionality required to suppress sea spray aerosol hygroscopicity to the extent indicated by field observations. We show that proper accounting for the distribution and diversity in particle hygroscopicity and composition are important to the assessment of particle impacts on clouds and global climate.

Morphology and Chemical Composition of soot particles emitted by Wood-burning Cook-Stoves: a HRTEM, XPS and Elastic backscattering Studies.

Science.gov (United States)

Carabali-Sandoval, G. A., Sr.; Castro, T.; Peralta, O.; De la Cruz, W.; Días, J.; Amelines, O.; Rivera-Hernández, M.; Varela, A.; Muñoz-Muñoz, F.; Policroniades, R.; Murillo, G.; Moreno, E.

2014-12-01

The morphology, microstructure and the chemical composition on surface of soot particles were studied by using high resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS) and elastic backscattering spectrometry. In order to obtain freshly soot particles emitted by home-made wood-burning cook stoves, copper grids for Transmission Electron Microscope (TEM) were placed on the last two of an 8-stages MOUDI cascade impactor. The analysis of HRTEM micrographs revealed the nanostructure and the particle size of soot particles. The XPS survey spectra show a large carbon peak around 285 eV and the oxygen signal at 533 eV. Some differences observed in the carbon/oxygen (C/O) ratio of the particles probably depend on the combustion process efficiency of each cook-stove analyzed. The C-1s XPS spectra show an asymmetric broad peak and other with low intensity that corresponds to sp2 and sp3hybridization, which were fitted with a convolution using Gaussian functions. Elastic backscattering technique allows a chemical elemental analysis of samples and confirms the presence of C, O and Si observed by XPS. Additionally, the morphological properties of soot aggregates were analyzed calculating the border-based fractal dimension (Df). Particles exhibit complex shapes with high values of Df. Also, real-time absorption (σabs) and scattering (σsct) coefficients of fine (with aerodynamic diameter < 2.5 µm) soot particles were measured. The trend in σabs and σsct indicate that the cooking process has two important combustion stages which varied in its flaming strength, being vigorous in the first stage and soft in the second one.

Investigation of soot morphology and particle size distrib ution in a turbulent nonpremixed flame via Monte Carlo simulations

KAUST Repository

Abdelgadir, Ahmed

2015-03-30

Recently, our group performed a set of direct numerical simulations (DNS) of soot formation and growth in a n-heptane three dimensional non-premixed jet flame [Attili et al., Proc. Comb. Inst, 35, 2015], [Attili et al., Comb. Flame, 161, 2014], [Bisetti et al.,Trans of the Royal Soc, 372, 2014]. The evolution of species relevant to soot formation and growth have been sampled along a large number of Lagrangian trajectories in the DNS. In this work, the DNS results are post-processed to compute the soot evolution along selected Lagrangian trajectories using a Monte Carlo method. An operator splitting approach is adopted to split the deterministic processes (nucleation, surface growth and oxidation) from coagulation, which is treated stochastically. The morphological properties of soot and the particlesize distribution are investigated. For trajectories that experience an early strong nucleation event, the particle size distribution is found to be bimodal, as the soot particles have enough time to coagulate and grow while it is unimodal for trajectories characterized by only late nucleation events. As a results, the average size distribution at two different crosswise positions in the flame is unimodal.

The Ice Nucleation Activity of Surface Modified Soot

Science.gov (United States)

Häusler, Thomas; Witek, Lorenz; Felgitsch, Laura; Hitzenberger, Regina; Grothe, Hinrich

2017-04-01

The ice nucleation efficiency of many important atmospheric particles remains poorly understood. Since soot is ubiquitous in the Earth's troposphere, they might have the potential to significantly impact the Earth's climate (Finlayson-Pitts and Pitts, 2000; Seinfeld and Pandis, 1998). Here we present the ice nucleation activity (INA) in immersion freezing mode of different types of soot. Therefor a CAST (combustion aerosol standard) generator was used to produce different kinds of soot samples. The CAST generator combusts a propane-air-mixture and deposits thereby produced soot on a polyvinyl fluoride filter. By varying the propane to air ratio, the amount of organic portion of the soot can be varied from black carbon (BC) with no organic content to brown carbon (BrC) with high organic content. To investigate the impact of functional sites of ice nuclei (IN), the soot samples were exposed to NO2 gas for a certain amount of time (30 to 360 minutes) to chemically modify the surface. Immersion freezing experiments were carried out in a unique reaction gadget. In this device a water-in-oil suspension (with the soot suspended in the aqueous phase) was cooled till the freezing point and was observed through a microscope (Pummer et al., 2012; Zolles et al., 2015) It was found that neither modified nor unmodified BC shows INA. On the contrary, unmodified BrC shows an INA at -32˚ C, which can be increased up to -20˚ C. The INA of BrC depends on the duration of NO2- exposure. To clarify the characteristics of the surface modifications, surface sensitive analysis like infrared spectroscopy and X-ray photoelectron spectroscopy were carried out. Finlayson-Pitts, B. J. and Pitts, J. N. J.: Chemistry of the Upper and Lower Atmosphere, Elsevier, New York, 2000. Pummer, B. G., Bauer, H., Bernardi, J., Bleicher, S., and Grothe, H.: Suspendable macromolecules are responsible for ice nucleation activity of birch and conifer pollen, Atmos Chem Phys, 12, 2541-2550, 2012. Seinfeld, J

Possible influence of anthropogenic aerosols on cirrus clouds and anthropogenic forcing

Directory of Open Access Journals (Sweden)

J. E. Penner

2009-02-01

Full Text Available Cirrus clouds have a net warming effect on the atmosphere and cover about 30% of the Earth's area. Aerosol particles initiate ice formation in the upper troposphere through modes of action that include homogeneous freezing of solution droplets, heterogeneous nucleation on solid particles immersed in a solution, and deposition nucleation of vapor onto solid particles. Here, we examine the possible change in ice number concentration from anthropogenic soot originating from surface sources of fossil fuel and biomass burning, from anthropogenic sulfate aerosols, and from aircraft that deposit their aerosols directly in the upper troposphere. We use a version of the aerosol model that predicts sulfate number and mass concentrations in 3-modes and includes the formation of sulfate aerosol through homogeneous binary nucleation as well as a version that only predicts sulfate mass. The 3-mode version best represents the Aitken aerosol nuclei number concentrations in the upper troposphere which dominated ice crystal residues in the upper troposphere. Fossil fuel and biomass burning soot aerosols with this version exert a radiative forcing of −0.3 to −0.4 Wm⁻² while anthropogenic sulfate aerosols and aircraft aerosols exert a forcing of −0.01 to 0.04 Wm⁻² and −0.16 to −0.12 Wm⁻², respectively, where the range represents the forcing from two parameterizations for ice nucleation. The sign of the forcing in the mass-only version of the model depends on which ice nucleation parameterization is used and can be either positive or negative. The magnitude of the forcing in cirrus clouds can be comparable to the forcing exerted by anthropogenic aerosols on warm clouds, but this forcing has not been included in past assessments of the total anthropogenic radiative forcing of climate.

Lab-scale development of a high temperature aerosol particle sampling probe system for field measurements in thermochemical conversion of biomass

Energy Technology Data Exchange (ETDEWEB)

Lindskog, M.; Malik, A.; Pagels, J.; Sanati, M. [Lund Univ., Lund (Sweden). Div. of Ergonomics and Aerosol Technology

2010-07-01

Thermochemical conversion of biomass requires both combustion in an oxygen rich environment and gasification in an oxygen deficient environment. Therefore, the mass concentration of fly ash from combustion processes is dominated by inorganic compounds, and the particulate matter obtained from gasification is dominated by carbonaceous compounds. The fine fly ash particles can initiate corrosion and fouling and also increases emissions of fine particulates to the atmosphere. This study involved the design of a laboratory scale setup consisting of a high temperature sampling probe and an aerosol generation system to study the formation of fine particle from biomass gasification processes. An aerosol model system using potassium chloride (KCl) as the ash compound and Di Octyl Sebacate oil (DOS) as the volatile organic part was used to test the high temperature sampling probe. Tests conducted at 200 degrees C showed good reproducibility of the aerosol generator. The tests also demonstrated suitable dilution ratios which enabled the denuder to absorb all of the gaseous organic compounds in the set up, thus enabling measurement of only the particle phase. Condensable organic concentrations of 1-68 mg/m{sup 3} were easily handled by the high temperature sampling probe system, indicating that the denuder worked well. Additional tests will be performed using an Aerosol Mass Spectrometer (AMST) to verify that the denuder can capture all of the gaseous organic compounds also when condensed onto agglomerated soot particles. 6 refs., 1 tab., 9 figs.

PIXE analysis of atmospheric aerosol and hydrometeor particles

International Nuclear Information System (INIS)

Groeneveld, K.O.; Hofmann, D.; Georgii, H.W.

1993-01-01

Atmospheric aerosol and hydrometeor particles act decisively on our weather, climate and thereby on all living conditions on Earth. Particle induced X-ray emission (PIXE) analysis has been demonstrated to be an extremely valuable tool for quantitative and qualitative elemental analysis of aerosol particles and hydrometeors. Reliability and detection limits of PIXE are determined, including comparison with other techniques. Aerosol particles are collected on a global scale in ground stations, or by ships and by planes. Correlation between wind direction and elemental composition of atmospheric aerosols, elemental particle size distributions of the tropospheric aerosol, aerosol elemental composition in particle size fractions in the case of long range transport, transport pathways of pollution aerosol, and trace element content precipitation are discussed. Hydrometeors were studied in the form of rain, snow, fog, dew and frost. The time dependence of the melting process of snow was studied in detail, in particular the washout phenomena of impurity ions. (orig.)

Particle pollution changes the atmospheric circulation

International Nuclear Information System (INIS)

Kristjansson, Jon Egill; Iversen, Trond; Kirkevaag, Alf; Seland, Oeyvind; Debernard, Jens; Roeed, Lars Petter

2002-01-01

Industrial emissions and combustion of fossil fuels create large amounts of sulfate- and carbon containing soot particles. These mix with natural particles to change the natural aerosols. Such anthropogenic changes in the aerosols may have a great impact on the climate of the earth. Altered properties of the aerosols may change the atmosphere's absorption and reflection of solar radiation and contribute to heating or cooling. This is the direct effect. Changes in the properties of aerosols may also affect the number and size of recently formed cloud droplets. This may change the ability of the clouds to reflect solar radiation and to produce precipitation. This is the indirect effect. Recent research at the University of Oslo shows that anthropogenic particles significantly change the atmospheric circulation, in particular in the tropics, but also at European latitudes

Monte carlo simulation for soot dynamics

KAUST Repository

Zhou, Kun

2012-01-01

A new Monte Carlo method termed Comb-like frame Monte Carlo is developed to simulate the soot dynamics. Detailed stochastic error analysis is provided. Comb-like frame Monte Carlo is coupled with the gas phase solver Chemkin II to simulate soot formation in a 1-D premixed burner stabilized flame. The simulated soot number density, volume fraction, and particle size distribution all agree well with the measurement available in literature. The origin of the bimodal distribution of particle size distribution is revealed with quantitative proof.

Physical and chemical characterization of urban winter-time aerosols by mobile measurements in Helsinki, Finland

Science.gov (United States)

Pirjola, Liisa; Niemi, Jarkko V.; Saarikoski, Sanna; Aurela, Minna; Enroth, Joonas; Carbone, Samara; Saarnio, Karri; Kuuluvainen, Heino; Kousa, Anu; Rönkkö, Topi; Hillamo, Risto

2017-06-01

A two-week measurement campaign by a mobile laboratory van was performed in urban environments in the Helsinki metropolitan area, Finland, in winter 2012, to obtain a comprehensive view on aerosol properties and sources. The abundances and physico-chemical properties of particles varied strongly in time and space, depending on the main sources of aerosols. Four major types of winter aerosol were recognized: 1) clean background aerosol with low particle number (Ntot) and lung deposited surface area (LDSA) concentrations due to marine air flows from the Atlantic Ocean; 2) long-range transported (LRT) pollution aerosol due to air flows from eastern Europe where the particles were characterized by the high contribution of oxygenated organic aerosol (OOA) and inorganic species, particularly sulphate, but low BC contribution, and their size distribution possessed an additional accumulation mode; 3) fresh smoke plumes from residential wood combustion in suburban small houses, these particles were characterized by high biomass burning organic aerosol (BBOA) and black carbon (BC) concentrations; and 4) fresh emissions from traffic while driving on busy streets in the city centre and on the highways during morning rush hours. This aerosol was characterized by high concentration of Ntot, LDSA, small particles in the nucleation mode, as well as high hydrocarbon-like organic aerosol (HOA) and BC concentrations. In general, secondary components (OOA, NO3, NH4, and SO4) dominated the PM1 chemical composition during the LRT episode accounting for 70-80% of the PM1 mass, whereas fresh primary emissions (BC, HOA and BBOA) dominated the local traffic and wood burning emissions. The major individual particle types observed with electron microscopy analysis (TEM/EDX) were mainly related to residential wood combustion (K/S/C-rich, soot, other C-rich particles), traffic (soot, Si/Al-rich, Fe-rich), heavy fuel oil combustion in heat plants or ships (S with V-Ni-Fe), LRT pollutants (S

Stochastic Simulation of Soot Formation Evolution in Counterflow Diffusion Flames

Directory of Open Access Journals (Sweden)

Xiao Jiang

2018-01-01

Full Text Available Soot generally refers to carbonaceous particles formed during incomplete combustion of hydrocarbon fuels. A typical simulation of soot formation and evolution contains two parts: gas chemical kinetics, which models the chemical reaction from hydrocarbon fuels to soot precursors, that is, polycyclic aromatic hydrocarbons or PAHs, and soot dynamics, which models the soot formation from PAHs and evolution due to gas-soot and soot-soot interactions. In this study, two detailed gas kinetic mechanisms (ABF and KM2 have been compared during the simulation (using the solver Chemkin II of ethylene combustion in counterflow diffusion flames. Subsequently, the operator splitting Monte Carlo method is used to simulate the soot dynamics. Both the simulated data from the two mechanisms for gas and soot particles are compared with experimental data available in the literature. It is found that both mechanisms predict similar profiles for the gas temperature and velocity, agreeing well with measurements. However, KM2 mechanism provides much closer prediction compared to measurements for soot gas precursors. Furthermore, KM2 also shows much better predictions for soot number density and volume fraction than ABF. The effect of nozzle exit velocity on soot dynamics has also been investigated. Higher nozzle exit velocity renders shorter residence time for soot particles, which reduces the soot number density and volume fraction accordingly.

Workplace aerosol mass concentration measurement using optical particle counters.

Science.gov (United States)

Görner, Peter; Simon, Xavier; Bémer, Denis; Lidén, Göran

2012-02-01

Direct-reading aerosol measurement usually uses the optical properties of airborne particles to detect and measure particle concentration. In the case of occupational hygiene, mass concentration measurement is often required. Two aerosol monitoring methods are based on the principle of light scattering: optical particle counting (OPC) and photometry. The former analyses the light scattered by a single particle, the latter by a cloud of particles. Both methods need calibration to transform the quantity of scattered light detected into particle concentration. Photometers are simpler to use and can be directly calibrated to measure mass concentration. However, their response varies not only with aerosol concentration but also with particle size distribution, which frequently contributes to biased measurement. Optical particle counters directly measure the particle number concentration and particle size that allows assessment of the particle mass provided the particles are spherical and of known density. An integrating algorithm is used to calculate the mass concentration of any conventional health-related aerosol fraction. The concentrations calculated thus have been compared with simultaneous measurements by conventional gravimetric sampling to check the possibility of field OPC calibration with real workplace aerosols with a view to further monitoring particle mass concentration. Aerosol concentrations were measured in the food industry using the OPC GRIMM® 1.108 and the CIP 10-Inhalable and CIP 10-Respirable (ARELCO®) aerosol samplers while meat sausages were being brushed and coated with calcium carbonate. Previously, the original OPC inlet had been adapted to sample inhalable aerosol. A mixed aerosol of calcium carbonate and fungi spores was present in the workplace. The OPC particle-size distribution and an estimated average particle density of both aerosol components were used to calculate the mass concentration. The inhalable and respirable aerosol fractions

Changes in background aerosol composition in Finland during polluted and clean periods studied by TEM/EDX individual particle analysis

Directory of Open Access Journals (Sweden)

J. V. Niemi

2006-01-01

Full Text Available Aerosol samples were collected at a rural background site in southern Finland in May 2004 during pollution episode (PM1~16 µg m−3, backward air mass trajectories from south-east, intermediate period (PM1~5 µg m−3, backtrajectories from north-east and clean period (PM1~2 µg m−3, backtrajectories from north-west/north. The elemental composition, morphology and mixing state of individual aerosol particles in three size fractions were studied using transmission electron microscopy (TEM coupled with energy dispersive X-ray (EDX microanalyses. The TEM/EDX results were complemented with the size-segregated bulk chemical measurements of selected ions and organic and elemental carbon. Many of the particles in PM0.2–1 and PM1–3.3 size fractions were strongly internally mixed with S, C and/or N. The major particle types in PM0.2–1 samples were 1 soot and 2 (ammoniumsulphates and their mixtures with variable amounts of C, K, soot and/or other inclusions. Number proportions of those two particle groups in PM0.2–1 samples were 0–12% and 83–97%, respectively. During the pollution episode, the proportion of Ca-rich particles was very high (26–48% in the PM1–3.3 and PM3.3–11 samples, while the PM0.2–1 and PM1–3.3 samples contained elevated proportions of silicates (22–33%, metal oxides/hydroxides (1–9% and tar balls (1–4%. These aerosols originated mainly from polluted areas of Eastern Europe, and some open biomass burning smoke was also brought by long-range transport. During the clean period, when air masses arrived from the Arctic Ocean, PM1–3.3 samples contained mainly sea salt particles (67–89% with a variable rate of Cl substitution (mainly by NO3−. During the intermediate period, the PM1–3.3 sample contained porous (sponge-like Na-rich particles (35% with abundant S, K and O. They might originate from the burning of wood pulp wastes of paper industry. The proportion of biological particles and C-rich fragments

Dynamics of neutral and charged aerosol particles

Energy Technology Data Exchange (ETDEWEB)

Leppae, J.

2012-07-01

Atmospheric aerosol particles have various climate effects and adverse health effects, which both depend on the size and number concentration of the particles. Freshly-formed particles are not large enough to impact neither health nor climate and they are most susceptible to removal by collisions with larger pre-existing particles. Consequently, the knowledge of both the formation and the growth rate of particles are crucially important when assessing the health and climate effects of atmospheric new particle formation. The purpose of this thesis is to increase our knowledge of the dynamics of neutral and charged aerosol particles with a specific interest towards the particle growth rate and processes affecting the aerosol charging state. A new model, Ion-UHMA, which simulates the dynamics of neutral and charged particles, was developed for this purpose. Simple analytical formulae that can be used to estimate the growth rate due to various processes were derived and used to study the effects of charged particles on the growth rate. It was found that the growth rate of a freshly-formed particle population due to condensation and coagulation could be significantly increased when a considerable fraction of the particles are charged. Finally, recent data-analysis methods that have been applied to the aerosol charging states obtained from the measurements were modified for a charge asymmetric framework. The methods were then tested on data obtained from aerosol dynamics simulations. The methods were found to be able to provide reasonable estimates on the growth rate and proportion of particles formed via ion-induced nucleation, provided that the growth rate is high enough and that the charged particles do not grow much more rapidly than the neutral ones. A simple procedure for estimating whether the methods are suitable for analysing data obtained in specific conditions was provided. In this thesis, the dynamics of neutral and charged aerosol particles were studied in

Climatic impacts of anthropogenic aerosols

Energy Technology Data Exchange (ETDEWEB)

Iversen, T. [Oslo Univ. (Norway)

1996-03-01

This paper was read at the workshop ``The Norwegian Climate and Ozone Research Programme`` held on 11-12 March 1996. Anthropogenic production of aerosols is mainly connected with combustion of fossil fuel. Measured by particulate mass, the anthropogenic sulphate production is the dominating source of aerosols in the Northern Hemisphere. Particles emitted in mechanical processes, fly ash etc. are less important because of their shorter atmospheric residence time. Possible climatological effects of anthropogenic aerosols are usually classified in two groups: direct and indirect. Direct effects are alterations of the radiative heating budget due to the aerosol particles in clear air. Indirect effects involve the interaction between particles and cloud processes. A simplified one-layer radiation model gave cooling in the most polluted mid-latitude areas and heating due to soot absorption in the Arctic. This differential trend in heating rates may have significant effects on atmospheric meridional circulations, which is important for the atmosphere as a thermodynamic system. Recently the description of sulphur chemistry in the hemispheric scale dispersion model has been improved and will be used in a model for Mie scattering and absorption

Arctic Black Carbon Loading and Profile Using the Single-Particle Soot Photometer (SP2) Field Campaign Report

Energy Technology Data Exchange (ETDEWEB)

Sedlacek, Arthur J [Brookhaven National Lab. (BNL), Upton, NY (United States)

2016-05-01

One of the major issues confronting aerosol climate simulations of the Arctic and Antarctic cryospheres is the lack of detailed data on the vertical and spatial distribution of aerosols with which to test these models. This is due, in part, to the inherent difficulty of conducting such measurements in extreme environments. However given the pronounced sensitivity of the polar regions to radiative balance perturbations, it is incumbent upon our community to better understand and quantify these perturbations, and their unique feedbacks, so that robust model predictions of this region can be realized. One class of under-measured radiative forcing agents in the polar region is the absorbing aerosol—black carbon and brown carbon. Black carbon (BC; also referred to as light-absorbing carbon [LAC], refractory black carbon [rBC], and soot) is second only to CO2 as a positive forcing agent. Roughly 60% of BC emissions can be attributed to anthropogenic sources (fossil fuel combustion and open-pit cooking), with the remaining fraction being due to biomass burning. Brown carbon (BrC), a major component of biomass burning, collectively refers to non-BC carbonaceous aerosols that typically possess minimal light absorption at visible wavelengths but exhibit pronounced light absorption in the near-ultraviolet (UV) spectrum. Both species can be sourced locally or be remotely transported to the Arctic region and are expected to perturb the radiative balance. The work conducted in this field campaign addresses one of the more glaring deficiencies currently limiting improved quantification of the impact of BC radiative forcing in the cryosphere: the paucity of data on the vertical and spatial distributions of BC. By expanding the Gulfstream aircraft (G-1) payload for the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility-sponsored ACME-V campaign to include the Single-Particle Soot Photometer (SP2)) and leveraging the ACME-V campaign�

Mass size distribution of particles emitted by diesel engines and determination of the contribution of diesel particles to the atmospheric aerosol in Vienna by using a tracer suitable for activation analysis

International Nuclear Information System (INIS)

Norek, C.

1985-01-01

In Vienna a large fraction of light absorbing aerosols has been found. The traffic could be a source for the high absorption coefficients, since the time dependent absorption coefficients varise similar to the traffic densities. Diesel vehicles have high soot emissions, so they may contribute considerably to light absorption during the summer. The emission factors of the vehicles were estimated by measurements at different motor and driving conditions by the Constant-Volume-Sampling-Method. To determine the size distributions a 10-stage-low pressure impactor with a lower cut size of 0.015 μm aerodynamic particle diameter was used. In order to estimate the contribution of diesel vehicles to the total mass concentrations all diesel fuel sold in Vienna and its vincinity was marked with an organic Dysprosium compound. This rare earth tracer was emitted by vehicles together with the soot particles and collected at eleven stations in Vienna. The filter samples were extracted with diluted HNO 3 and the extraction was analysed for Dy by neutron activation analysis. The mass size distributions of the particles and the soot emitted from diesel engines are only slightly influenced by motor and driving parameters. The total mass emissions showed considerable variations, but the mean emission factor obtained from the tests was 2.43 g per litre fuel; knowing also the concentration of the tracer in the fuel, the contribution of diesel particles to the mass of the suspended particulates could be estimated. During the measuring period the contribution was c. 25% to the total mass and c. 40% to the absorbing matter in the atmosphere. (Author)

The hygroscopicity of indoor aerosol particles

International Nuclear Information System (INIS)

Wei, L.

1993-07-01

A system to study the hygroscopic growth of particle was developed by combining a Tandem Differential Mobility Analyzer (TDMA) with a wetted wall reactor. This system is capable of mimicking the conditions in human respiratory tract, and measuring the particle size change due to the hygroscopic growth. The performance of the system was tested with three kinds of particles of known composition, NaCl, (NH 4 ) 2 SO 4 , and (NH 4 )HS0 4 particles. The hygroscopicity of a variety of common indoor aerosol particles was studied including combustion aerosols (cigarette smoking, cooking, incenses and candles) and consumer spray products such as glass cleaner, general purpose cleaner, hair spray, furniture polish spray, disinfectant, and insect killer. Experiments indicate that most of the indoor aerosols show some hygroscopic growth and only a few materials do not. The magnitude of hygroscopic growth ranges from 20% to 300% depending on the particle size and fraction of water soluble components

Time-averaged probability density functions of soot nanoparticles along the centerline of a piloted turbulent diffusion flame using a scanning mobility particle sizer

KAUST Repository

Chowdhury, Snehaunshu

2017-01-23

In this study, we demonstrate the use of a scanning mobility particle sizer (SMPS) as an effective tool to measure the probability density functions (PDFs) of soot nanoparticles in turbulent flames. Time-averaged soot PDFs necessary for validating existing soot models are reported at intervals of ∆x/D∆x/D = 5 along the centerline of turbulent, non-premixed, C2H4/N2 flames. The jet exit Reynolds numbers of the flames investigated were 10,000 and 20,000. A simplified burner geometry based on a published design was chosen to aid modelers. Soot was sampled directly from the flame using a sampling probe with a 0.5-mm diameter orifice and diluted with N2 by a two-stage dilution process. The overall dilution ratio was not evaluated. An SMPS system was used to analyze soot particle concentrations in the diluted samples. Sampling conditions were optimized over a wide range of dilution ratios to eliminate the effect of agglomeration in the sampling probe. Two differential mobility analyzers (DMAs) with different size ranges were used separately in the SMPS measurements to characterize the entire size range of particles. In both flames, the PDFs were found to be mono-modal in nature near the jet exit. Further downstream, the profiles were flatter with a fall-off at larger particle diameters. The geometric mean of the soot size distributions was less than 10 nm for all cases and increased monotonically with axial distance in both flames.

Investigations of Sooting Laminar Coflow Diffusion Flames at Elevated Pressures

KAUST Repository

Steinmetz, Scott A.

2016-12-01

Soot is a common byproduct of hydrocarbon based combustion systems. It poses a risk to human and environmental health, and can negatively or positively affect combustor performance. As a result, there is significant interest in understanding soot formation in order to better control it. More recently, the need to study soot formation in engine relevant conditions has become apparent. One engine relevant parameter that has had little focus is the ambient pressure. This body of work focuses on the formation of soot in elevated pressure environments, and a number of investigations are carried out with this purpose. Laminar coflow diffusion flames are used as steady, simple soot producers. First, a commonly studied flame configuration is further characterized. Coflow flames are frequently used for fundamental flame studies, particularly at elevated pressures. However, they are more susceptible to buoyancy induced instabilities at elevated pressures. The velocity of the coflow is known to have an effect on flame stability and soot formation, though these have not been characterized at elevated pressures. A series of flames are investigated covering a range of flowrates, pressures, and nozzle diameters. The stability limits of coflow flames in this range is investigated. Additionally, an alternative strategy for scaling these flames to elevated pressures is proposed. Finally, the effect of coflow rate on soot formation is evaluated. Identification of fundamental flames for coordinated research can facilitate our understanding of soot formation. The next study of this work focuses on adding soot concentration and particle size information to an existing fundamental flame dataset for the purpose of numerical model validation. Soot volume fraction and average particle diameters are successfully measured in nitrogen-diluted ethylene-air laminar coflow flames at pressures of 4, 8, 12, and 16 atm. An increase in particle size with pressure is found up to 12 atm, where particle

Variation of diesel soot characteristics by different types and blends of biodiesel in a laboratory combustion chamber

Energy Technology Data Exchange (ETDEWEB)

Omidvarborna, Hamid; Kumar, Ashok [Department of Civil Engineering, The University of Toledo, Toledo, OH (United States); Kim, Dong-Shik, E-mail: dong.kim@utoledo.edu [Department of Chemical and Environmental Engineering, The University of Toledo, Toledo, OH (United States)

2016-02-15

Very little information is available on the physical and chemical properties of soot particles produced in the combustion of different types and blends of biodiesel fuels. A variety of feedstock can be used to produce biodiesel, and it is necessary to better understand the effects of feedstock-specific characteristics on soot particle emissions. Characteristics of soot particles, collected from a laboratory combustion chamber, are investigated from the blends of ultra-low sulfur diesel (ULSD) and biodiesel with various proportions. Biodiesel samples were derived from three different feedstocks, soybean methyl ester (SME), tallow oil (TO), and waste cooking oil (WCO). Experimental results showed a significant reduction in soot particle emissions when using biodiesel compared with ULSD. For the pure biodiesel, no soot particles were observed from the combustion regardless of their feedstock origins. The overall morphology of soot particles showed that the average diameter of ULSD soot particles is greater than the average soot particles from the biodiesel blends. Transmission electron microscopy (TEM) images of oxidized soot particles are presented to investigate how the addition of biodiesel fuels may affect structures of soot particles. In addition, inductively coupled plasma mass spectrometry (ICP-MS), Fourier transform infrared spectroscopy (FTIR), and thermogravimetric analysis (TGA) were conducted for characterization of soot particles. Unsaturated methyl esters and high oxygen content of biodiesel are thought to be the major factors that help reduce the formation of soot particles in a laboratory combustion chamber. - Highlights: • The unsaturation of biodiesel fuel was correlated with soot characteristics. • Average diameters of biodiesel soot were smaller than that of ULSD. • Eight elements were detected as the marker metals in biodiesel soot particles. • As the degree of unsaturation increased, the oxygen content in FAMEs increased. • Biodiesel

Soot, unburned carbon and ultrafine particle emissions from air- and oxy-coal flames

International Nuclear Information System (INIS)

Morris, W.J.; Yu, Dunxi; Wendt, J.O.L.

2010-01-01

Oxy-coal combustion is one possible solution for the mitigation of greenhouse gases. In this process coal is burned in oxygen, rather than air, and the temperatures in the boiler are mitigated by recycling flue gases, so that the inlet mixture may contain either 27 % O 2 to match adiabatic flame temperatures, or 32 % O 2 to match gaseous radiation heat fluxes in the combustion chamber. However, a major issue for heat transfer from coal combustion is the radiative heat transmission from soot. For this research, air and oxy coal firing were compared regarding the emission of soot. A 100 kW down-fired laboratory combustor was used to determine effects of switching from air to oxy-firing on soot, unburned carbon and ultrafine particle emissions from practical pulverized coal flames. Of interest here were potential chemical effects of substitution of the N 2 in air by CO 2 in practical pulverized coal flames. The oxy-coal configuration investigated used once-through CO 2 , simulating cleaned flue gas recycle with all contaminants and water removed. Three coals were each burned in: a) air, b) 27 % O 2 / 73 % CO 2 , c) 32 % O 2 / 68 % CO 2 . Tests were conducted at (nominally) 3 %, 2 %, 1 % and 0 % O 2 in the exhaust (dry basis). For each condition, particulate samples were iso kinetically withdrawn far from the radiant zone, and analyzed using a photoacoustic analyzer (PA) for black carbon, a scanning mobility particle sizer (SMPS) for ultrafine particles, and a total sample loss on ignition (LOI) method for unburned carbon in ash. Data suggest that at low stoichiometric ratios, ultrafine particles consist primarily of black carbon, which, for the bituminous coal, is produced in lesser amounts under oxy-fired conditions than under the air-fired condition, even when adiabatic flame temperatures are matched. However, significant changes in mineral matter vaporization were not observed unless the flames were hotter. These and other results are interpreted in the light of

Formation and dynamic change of aerosol particles

International Nuclear Information System (INIS)

Kasahara, Mikio

1986-01-01

Processes of aerosol particle nucleation are roughly grouped into two types. In one, aerosol is produced as a result of dispersion of solid or liquid by mechanical force while in the other it is formed through phase transition from gas to solid or liquid due to cohesion caused by cooling, expansion or chemical reaction. This article reviews various aspects of aerosol particle nucleation through the latter type of processes and behaviors of the particles formed. Gas-to-particle conversion processes are divided into those of homogeneous and heterogeneous nucleation, and the former include homogeneous homomolecular and homogeneous heteromolecular nucleation processes. Here, homoneneous homomolecular nucleation is described centering on the theories proposed by Backer and Doring-Zeldovich-Volmer-Frenkel while homogeneous heteromolecular systems are outlined citing the theory developed by Kiang and Stauffer. Heterogeneous nucleation (or heterogeneous condensation) is discussed on the basis of the relationship between the mean free path of air molecules and the particle size. Various theories for particle formation and growth are listed and briefly outlined. Some of them are compared with experimental results. Models are cited to explain behaviors of aerosol particles after being formed. Also described is simulation of particle nucleation and growth in relation to atmospheric pollution and possible accidents of liquid-metal fast breeder reactors. (Nogami, K.)

Experimental determination of soot refractive index in the infrared

International Nuclear Information System (INIS)

Ouf, F.X.; Vendel, J.; Ouf, F.X.; Coppalle, A.; Weil, M.E.; Yon, J.

2007-01-01

The study of physical properties of soot particles produced during combustion is a complex subject but of a great interest within the framework of the study of the safety of an installation, with respect to the fire hazard. These characteristics are, in this case, particularly useful in order to predict the behaviour of containment barriers in situation of fire, but also in order to estimate the contribution of these particles to radiative transfers. The aim of this study is to determine the radiative properties of soot particles produced during combustion. A specific device, which establishes extinction and vertical-vertical scattering coefficients, has been developed and has allowed to determine the refractive index of soot particles in the infrared. This determination also needed the establishment of size distribution and morphological properties of soot aggregates. We present in this document the experimental device developed, and the validation of this device on latex spheres which optical properties are well known. First results of extinction coefficients will be presented and will underline the similar optical behaviour of different soot aggregates. Values of refractive index will be detailed and discussed, and a direct application of these values will be carried out in order to determine the soot volume fraction. A comparison with reference method will underline the efficiency of our method. We will conclude on the validity of the information brought by this device and on the prospects of this study. A discussion is included, on the utility of mean values of refractive index and on the determination of total emissivity of soot particles. (authors)

In-situ studies on volatile jet exhaust particle emissions - impacts of fuel sulfur content and environmental conditions on nuclei-mode aerosols

Energy Technology Data Exchange (ETDEWEB)

Schroeder, F.; Baumann, R.; Petzold, A.; Busen, R.; Schulte, P.; Fiebig, M. [DLR Deutsches Zentrum fuer Luft- und Raumfahrt e.V., Wessling (Germany). Inst. fuer Physik der Atmosphaere; Brock, C.A. [Denver Univ., CO (United States). Dept. of Engineering

2000-02-01

In-situ measurements of ultrafine aerosol particle emissions were performed at cruise altitudes behind the DLR ATTAS research jet (RR M45H M501 engines) and a B737-300 aircraft (CFM56-3B1 engines). Measurements were made 0.15-20 seconds after emission as the source aircraft burned fuel with sulfur contents (FSC) of 2.6, 56 or 118 mg kg{sup -1}. Particle size distributions of from 3 to 60 nm diameter were determined using CN-counters with varying lower size detection limits. Volatile particle concentrations in the aircraft plumes strongly increased as diameter decreased toward the sizes of large molecular clusters, illustrating that apparent particle emissions are extremely sensitive to the smallest particle size detectable by the instrument used. Environmental conditions and plume age alone could influence the number of detected ultrafine (volatile) aerosols within an order of magnitude, as well. The observed volatile particle emissions decreased nonlinearly as FSC decreased to 60 mg kg{sup -1}, reaching minimum values of about 2 x 10{sup 17} kg{sup -1} and 2 x 10{sup 16} kg{sup -1} for particles >3 nm and >5 nm, respectively. Volatile particle emissions did not change significantly as FSCs were further reduced below 60 mg kg{sup -1}. Volatile particle emissions did not differ significantly between the two studied engine types. In contrast, soot particle emissions from the modern CFM56-3B1 engines were 4-5 times less (4 x 10{sup 14} kg{sup -1}) than from the older RR M45H M501 engines (1.8 x 10{sup 15} kg{sup -1}). Contrail processing has been identified as an efficient sink/quenching parameter for ultrafine particles and reduces the remaining interstitial aerosol by factors 2-10 depending on particle size.

Estimating soot emissions from an elevated flare

Science.gov (United States)

Almanza, Victor; Sosa, Gustavo

2009-11-01

Combustion aerosols are one of the major concerns in flaring operations, due to both health and environmental hazards. Preliminary results are presented for a 2D transient simulation of soot formation in a reacting jet with exit velocity of 130 m/s under a 5 m/s crossflow released from a 50 m high elevated flare and a 50 cm nozzle. Combustion dynamics was simulated with OpenFOAM. Gas-phase non-premixed combustion was modeled with the Chalmers PaSR approach and a κ-ɛ turbulence model. For soot formation, Moss model was used and the ISAT algorithm for solving the chemistry. Sulfur chemistry was considered to account for the sourness of the fuel. Gas composition is 10 % H2S and 90 % C2H4. A simplified Glassman reaction mechanism was used for this purpose. Results show that soot levels are sensitive to the sulfur present in the fuel, since it was observed a slight decrease in the soot volume fraction. NSC is the current oxidation model for soot formation. Predicted temperature is high (about 2390 K), perhaps due to soot-radiation interaction is not considered yet, but a radiation model implementation is on progress, as well as an oxidation mechanism that accounts for OH radical. Flame length is about 50 m.

On the Response of Nascent Soot Nanostructure and Oxidative Reactivity to Photoflash Exposure

Directory of Open Access Journals (Sweden)

Wei Wang

2017-07-01

Full Text Available Soot particles are a kind of major pollutant from fuel combustion. To enrich the understanding of soot, this work focuses on investigating detailed influences of instantaneous external irradiation (conventional photoflash exposure on nanostructure as well as oxidation reactivity of nascent soot particles. By detailed soot characterizations flash can reduce the mass of soot and soot nanostructure can be reconstructed substantially without burning. After flash, the degree of soot crystallization increases while the soot reactive rate decreases and the activation energy increases. In addition, nanostructure and oxidative reactivity of soot in air and Ar after flash are different due to their different thermal conductivities.

Mutagenicity of diesel exhaust soot dispersed in phospholipid surfactants

Energy Technology Data Exchange (ETDEWEB)

Wallace, W.; Keane, M.; Xing, S.; Harrison, J.; Gautam, M.; Ong, T.

1994-06-01

Organics extractable from respirable diesel exhaust soot particles by organic solvents have been known for some time to be direct acting frameshift mutagens in the Ames Salmonella typhimurium histidine reversion assay. Upon deposition in a pulmonary alveolus or respiratory bronchiole, respirable diesel soot particles will contact first the hypophase which is coated by and laden with surfactants. To model interactions of soot and pulmonary surfactant, the authors dispersed soots in vitro in the primary phospholipid pulmonary surfactant dipalmitoyl glycerophosphorylcholine (lecithin) (DPL) in physiological saline. They have shown that diesel soots dispersed in lecithin surfactant can express mutagenic activity, in the Ames assay system using S. typhimurium TA98, comparable to that expressed by equal amounts of soot extracted by dichloromethane/dimethylsulfoxide (DCM/DMSO). Here the authors report additional data on the same system using additional exhaust soots and also using two other phospholipids, dipalmitoyl glycerophosphoryl ethanolamine (DPPE), and dipalmitoyl phosphatidic acid (DPPA), with different ionic character hydrophilic moieties. A preliminary study of the surfactant dispersed soot in an eucaryotic cell test system also is reported.

Minor and Trace Element Chemistry of Urban NS-Soot from the Central Valley of CA, USA

Science.gov (United States)

Kleich, S. J.; Hooper, R.

2017-12-01

During a recent study of metal transport in the Central Valley of California, it was noted that ns-soot (soot) occurred as complex clusters of graphene-like spheres admixed with other aerosols and were usually the dominant component of PM2.5 air particulates. These soot clusters contained a wide variety of metals of environmental concern such as As,Pb,Cr, and Ni. This study reports semi-quantitative results for 20 minor and trace elements (calibrated with Smithsonian microbeam standards) using a 200kV Transmission Electron Microscope, EDS, and SAED. This study also examined the mineralogy and crystallinity of admixed aerosols within composite soot clusters. Samples selected represent three contrasting urban settings in the Central Valley: Woodland, on the western side of the valley (Interstate highway to the east); Stockton, an inland sea-port and land transportation corridor in the center of the valley; and Roseville, a major rail-transport hub to the east. The wet/dry Mediterranean climate of California resulted in pronounced seasonal variations in total metal content. Soot cluster chemistry is highly variable however certain patterns emerged. Soot collected during the wet season is generally more aciniform, less structurally complex, and had lower sulfur (sulfate) concentrations but still had significant levels of transition metals (V,Cr,Mn,Fe,Ni,Zn and Pb) . Dry season soot was predominantly admixed with sulfate aerosols, and enriched in alkalis and alkaline earth metals. Stockton (wet-season) soot had up to 6000ppm of Pb. There is appreciable Pb (210ppm-2600ppm) in 38% of samples from Roseville but no Pb greater than 200ppm in Woodland. The highest overall total metals were found in Roseville soot with appreciable As(670ppm), V(100ppm), Pb(2600ppm), Zn(4000 ppm), Cr(90ppm), and Ni(300ppm). Heavy transport (road/rail/port) correlates with higher metal contents regardless of climate.

Effect of Dimethyl Ether Mixing on Soot Size Distribution in Premixed Ethylene Flame

KAUST Repository

Li, Zepeng

2016-04-21

As a byproduct of incomplete combustion, soot attracts increasing attentions as extensive researches exploring serious health and environmental effects from soot particles. Soot emission reduction requires a comprehensive understanding of the mechanism for polycyclic aromatic hydrocarbons and of soot formation and aging processes. Therefore, advanced experimental techniques and numerical simulations have been conducted to investigate this procedure. In order to investigate the effects of dimethyl ether (DME) mixing on soot particle size distribution functions (PSDFs), DME was mixed in premixed ethylene/oxygen/argon at flames at the equivalence ratio of 2.0 with a range of mixing ratio from 0% to 30% of the total carbon fed. Two series of atmospheric pressure flames were tested in which cold gas velocity was varied to obtain different flame temperatures. The evolution of PSDFs along the centerline of the flame was determined by burner stabilized stagnation probe and scanning mobility particle sizer (SMPS) techniques, yielding the PSDFs for various separation distances above the burner surface. Meanwhile, the flame temperature profiles were carefully measured by a thermocouple and the comparison to that of simulated laminar premixed burner-stabilized stagnation flame was satisfactory. Additionally, to understand the chemical role of DME mixing in soot properties, characterization measurements were conducted on soot samples using thermo-gravimetric analysis (TGA) and elemental analysis (EA). Results of the evolution of PSDFs and soot volume fraction showed that adding DME into ethylene flame could reduce soot yield significantly. The addition of DME led to the decrease of both the soot nucleation rate and the particle mass growth rate. To explain the possible mechanism for the observation, numerical simulations were performed. Although DME addition resulted in the slight increase of methyl radicals from pyrolysis, the decrease in acetylene and propargyl radicals

Labeling suspended aerosol particles with short-lived radionuclides for determination of particle deposition

International Nuclear Information System (INIS)

Smith, M.F.; Bryant, S.; Welch, S.; Digenis, G.A.

1984-01-01

Radiotracer techniques were developed to examine parameters that characterize pressurized aerosols designed to deliver insoluble particles suspended in the aerosol formulation. Microaggregated bovine serum albumin microspheres that were to be suspended were labeled with iodine-131 (t1/2 . 8 d). This iodination procedure (greater than 80% effective) is also applicable to iodine-123, which possesses superior characteristics for external imaging and further in vivo studies. This report shows that for pressurized aerosols containing suspended particles, each metered dose is approximately equal (not including the priming doses and the emptying doses). Increase in the delivery of the albumin particles out of the canister was best achieved by pretreating the valve assembly with a solution of 2% (w/v) bovine serum albumin in phosphate buffer. Use of a cascade impactor delineated the particle size distribution of the micropheres, with the majority of particles ranging in size from 2 to 8 microns. The data disclosed here indicate that the techniques developed with short-lived radionuclides can be used to quantitate each metered dose, characterize the particle size distribution profile of the aerosol contents, and determine the extent of deposition of the particles in the aerosol canister and all of its components

Development of a photoacoustic sensor system for the measurement of atmospheric soot aerosols. Final report; Weiterentwicklung und Charakterisierung des photoakustischen Russsensors. Schlussbericht

Energy Technology Data Exchange (ETDEWEB)

Kraemer, L.; Bozoki, Z.; Niessner, R.

2001-03-01

The photoacoustic soot sensor (PASS) has been optimised and characterised in this work to enable online atmospheric black carbon (BC) monitoring. The mobility of the sensor suited for outdoor measurements was already achieved by a former setup. The major technical modifications include the use of a new diode laser with an emission wavelength of 680 nm and an output power of 250 mW and the redesign of the photoacoustic resonance cell and all optical components. Additionally, most of the electronic compounds have been exchanged, e.g. function generator, microphone preamplifier, lock-in amplifier. Due to these modifications, the increase in the sensitivity of the system led to a detection limit in the order of 100 ng per m{sup 3}. The selectivity has been enhanced by the use of a magnetic valve, which enables the independent determination of particular and gaseous compounds of the sample. Cross-sensitivities to water vapor or nitrogen dioxide can be excluded by differential measurement. Any influence by other airborne atmospheric particles like scattering salt aerosols, desert dust or humic acid is negligable under atmospheric conditions as has been shown in laboratory experiments. For the determination of low atmospheric BC concentrations, the time resolution of the entire setup by employing a software controlled, automated measurement cycle equals {proportional_to}5 minutes. The PASS was tested in various field campaigns at different measurement sites to determine atmospheric BC (Munich-Grosshadern, Kleiner Feldberg) and diesel soot (AIDA, FZ Karlsruhe; diesel engine, DaimlerChrysler). (orig.)

Single particle aerosol mass spectrometry of coal combustion particles associated with high lung cancer rates in Xuanwei and Fuyuan, China.

Science.gov (United States)

Lu, Senlin; Tan, Zhengying; Liu, Pinwei; Zhao, Hui; Liu, Dingyu; Yu, Shang; Cheng, Ping; Win, Myat Sandar; Hu, Jiwen; Tian, Linwei; Wu, Minghong; Yonemochi, Shinich; Wang, Qingyue

2017-11-01

Coal combustion particles (CCPs) are linked to the high incidence of lung cancer in Xuanwei and in Fuyuan, China, but studies on the chemical composition of the CCPs are still limited. Single particle aerosol mass spectrometry (SPAMS) was recently developed to measure the chemical composition and size of single particles in real-time. In this study, SPAMS was used to measure individual combustion particles emitted from Xuanwei and Fuyuan coal samples and the results were compared with those by ICP-MS and transmission electron microscopy (TEM). The total of 38,372 particles mass-analyzed by SPAMS can be divided into 9 groups based on their chemical composition and their number percentages: carbonaceous, Na-rich, K-rich, Al-rich, Fe-rich, Si-rich, Ca-rich, heavy metal-bearing, and PAH-bearing particles. The carbonaceous and PAH-bearing particles are enriched in the size range below 0.56 μm, Fe-bearing particles range from 0.56 to 1.0 μm in size, and heavy metals such as Ti, V, Cr, Cu, Zn, and Pb have diameters below 1 μm. The TEM results show that the particles from Xuanwei and Fuyuan coal combustion can be classified into soot aggregates, Fe-rich particles, heavy metal containing particles, and mineral particles. Non-volatile particles detected by SPAMS could also be observed with TEM. The number percentages by SPAMS also correlate with the mass concentrations measured by ICP-MS. Our results could provide valuable insight for understanding high lung cancer incidence in the area. Copyright © 2017 Elsevier Ltd. All rights reserved.

Simulation of soot size distribution in an ethylene counterflow flame

KAUST Repository

Zhou, Kun; Abdelgadir, Ahmed Gamaleldin; Bisetti, Fabrizio

2014-01-01

Soot, an aggregate of carbonaceous particles produced during the rich combustion of fossil fuels, is an undesirable pollutant and health hazard. Soot evolution involves various dynamic processes: nucleation soot formation from polycyclic aromatic

Time-averaged probability density functions of soot nanoparticles along the centerline of a piloted turbulent diffusion flame using a scanning mobility particle sizer

KAUST Repository

Chowdhury, Snehaunshu; Boyette, Wesley; Roberts, William L.

2017-01-01

In this study, we demonstrate the use of a scanning mobility particle sizer (SMPS) as an effective tool to measure the probability density functions (PDFs) of soot nanoparticles in turbulent flames. Time-averaged soot PDFs necessary for validating

Study on soot particle formation and oxidation in DI diesel engine; Chokufunshiki diesel kikan ni okeru susu ryushi no seicho sanka ni kansuru kenkyu

Energy Technology Data Exchange (ETDEWEB)

Kurata, K; Senda, J; Fujimoto, H [Doshisha University, Kyoto (Japan); Asai, G [Yanmar Diesel Engine Co. Ltd., Osaka (Japan)

1997-10-01

To clarify soot formation and oxidation process in diesel combustion, the natural emission of OH radical and the flame temperature were obtained in the combustion chamber of D.I. diesel engine. Further, soot were detected by LII (Laser Induced Incandescence) and LIS (Laser Induced Scattering) technique to assess the relative soot diameter and its number density. OH emission and flame temperature were compared with data of soot diameter and number- density. The results show that : (1) OH emission has relation to flame temperature. (2) OH emission arises latter than soot emission, because early soot at early combustion consume OH to oxidate. (3) As soon as it is ignited, soot particles are formed in the region of low temperature. 6 refs., 7 figs., 2 tabs.

Aromatics Oxidation and Soot Formation in Flames

Energy Technology Data Exchange (ETDEWEB)

Howard, J. B.; Richter, H.

2005-03-29

This project is concerned with the kinetics and mechanisms of aromatics oxidation and the growth process to polycyclic aromatic hydrocarbons (PAH) of increasing size, soot and fullerenes formation in flames. The overall objective of the experimental aromatics oxidation work is to extend the set of available data by measuring concentration profiles for decomposition intermediates such as phenyl, cyclopentadienyl, phenoxy or indenyl radicals which could not be measured with molecular-beam mass spectrometry to permit further refinement and testing of benzene oxidation mechanisms. The focus includes PAH radicals which are thought to play a major role in the soot formation process while their concentrations are in many cases too low to permit measurement with conventional mass spectrometry. The radical species measurements are used in critical testing and improvement of a kinetic model describing benzene oxidation and PAH growth. Thermodynamic property data of selected species are determined computationally, for instance using density functional theory (DFT). Potential energy surfaces are explored in order to identify additional reaction pathways. The ultimate goal is to understand the conversion of high molecular weight compounds to nascent soot particles, to assess the roles of planar and curved PAH and relationships between soot and fullerenes formation. The specific aims are to characterize both the high molecular weight compounds involved in the nucleation of soot particles and the structure of soot including internal nanoscale features indicative of contributions of planar and/or curved PAH to particle inception.

Effects of DME mixing on number density and size properties of soot particles in counterflow non-premixed ethylene flames

KAUST Repository

Choi, J. H.

2015-05-01

In order to investigate the effect of DME mixing on the number density and size of soot particles, DME was mixed in a counter flow non-premixed ethylene flame with mixture ratios of 5%, 14% and 30%. A laser extinction/scattering technique has been adopted to measure the volume fraction, number density, and mean size of soot particles. The experimental results showed that the highest soot concentrations were observed for flames with mixture ratios of 5% and 14%; however, for a mixture ratio of 30% the soot concentration decreased. Numerical results showed that the concentrations of propargyl radicals (C3H3) at the 5% and 14% ratios were higher than those measured in the ethylene-based flame, and the production of benzene (C6H6) in the 5% and 14% DME mixture flames was also increased. This indicates the crucial role of propargyl in benzene ring formation. These reactions generally become stronger with increased DME mixing, except for A1- + H2 → A1 + H (-R554) and n-C4H5 + C2H2 → A1 + H (R542). Therefore, it is indicated that adding DME to ethylene flames promotes benzene ring formation. Note that although the maximum C6H6 concentration is largest in the 30% DME mixing flame, the soot volume fraction is smaller than those for the 5% and 14% mixture ratios. This is because the local C6H6 concentration decreases in the relatively low temperature region in the fuel side where soot growth occurs. © 2015, The Korean Society of Mechanical Engineers and Springer-Verlag Berlin Heidelberg.

Effects of DME mixing on number density and size properties of soot particles in counterflow non-premixed ethylene flames

KAUST Repository

Choi, J. H.; Choi, B. C.; Lee, S. M.; Chung, Suk-Ho; Jung, K. S.; Jeong, W. L.; Choi, S. K.; Park, S. K.

2015-01-01

In order to investigate the effect of DME mixing on the number density and size of soot particles, DME was mixed in a counter flow non-premixed ethylene flame with mixture ratios of 5%, 14% and 30%. A laser extinction/scattering technique has been adopted to measure the volume fraction, number density, and mean size of soot particles. The experimental results showed that the highest soot concentrations were observed for flames with mixture ratios of 5% and 14%; however, for a mixture ratio of 30% the soot concentration decreased. Numerical results showed that the concentrations of propargyl radicals (C3H3) at the 5% and 14% ratios were higher than those measured in the ethylene-based flame, and the production of benzene (C6H6) in the 5% and 14% DME mixture flames was also increased. This indicates the crucial role of propargyl in benzene ring formation. These reactions generally become stronger with increased DME mixing, except for A1- + H2 → A1 + H (-R554) and n-C4H5 + C2H2 → A1 + H (R542). Therefore, it is indicated that adding DME to ethylene flames promotes benzene ring formation. Note that although the maximum C6H6 concentration is largest in the 30% DME mixing flame, the soot volume fraction is smaller than those for the 5% and 14% mixture ratios. This is because the local C6H6 concentration decreases in the relatively low temperature region in the fuel side where soot growth occurs. © 2015, The Korean Society of Mechanical Engineers and Springer-Verlag Berlin Heidelberg.

Continuous air monitor for alpha-emitting aerosol particles

International Nuclear Information System (INIS)

McFarland, A.R.; Ortiz, C.A.; Rodgers, J.C.; Nelson, D.C.

1991-01-01

A new alpha continuous air monitor (CAM) sampler is being developed for use in detecting the presence of alpha-emitting aerosol particles. The effort involves design, fabrication and evaluation of systems for the collection of aerosol and for the processing of data to speciate and quantify the alpha emitters of the interest. At the present time the authors have a prototype of the aerosol sampling system and they have performed wind tunnel tests to characterize the performance of the device for different particle sizes, wind speeds, flow rates and internal design parameters. The results presented herein deal with the aerosol sampling aspects of the new CAM sampler. Wind tunnel tests show that ≥ 50% of 10 μm aerodynamic equivalent diameter (AED) particles penetrate the flow system from the ambient air to the collection filter when the flow rate is 57 L/min (2 cfm) and the wind speed is 1 m/s. The coefficient of variation of deposits of 10 μm AED aerosol particles on the collection filter is 7%. An inlet fractionator for removing high mobility background aerosol particles has been designed and successfully tested. The results show that it is possible to strip 95% of freshly formed radon daughters and 33% of partially aged radon daughters from the aerosol sample. This approach offers the opportunity to improve the signal-to-noise ratio in the alpha energy spectrum region of interest thereby enhancing the performance of background compensation algorithms

Physical characterization of diesel exhaust nucleation mode particles

Energy Technology Data Exchange (ETDEWEB)

Lahde, T.

2013-11-01

An increasing concern of the adverse health effects of aerosol particles is forcing the combustion engine industry to develop engines with lower particle emissions. The industry has put most of their efforts into soot control and has achieved a significant reduction in diesel exhaust particle mass. Nevertheless, it is not clear that the large particles, dominating the mass, cause the harmfulness of the exhaust particles in the biological interaction. Nowadays, the harmful potential of diesel exhaust particles often connects with the particle surface area, and the view has turned to particle number below 100 nm size range. Unfortunately, the achieved low exhaust particle mass does not necessarily imply a low particle number. This text focuses on the physical characteristics of diesel exhaust nucleation model particles. The volatility characteristics and the electrical charge state of the particles are studied first. Second, the relation between the nonvolatile nucleation mode emissions and the soot, the nitrogen oxide (NO{sub x}) emissions and the engine parameters are covered. The nucleation mode particles had distinctively different physical characteristics with different after-treatment systems. The nucleation mode was volatile and electrically neutral with a diesel particle filter after-treatment system. Without an after-treatment system or with an after-treatment system with low particle removal efficiency, the nucleation mode was partly nonvolatile and included an electrical charge. The difference suggests different formation routes for the nucleation particles with different after-treatment systems. The existence of the nonvolatile nucleation mode particles also affected the soot mode charge state. The soot charge state was positively biased when the nonvolatile nucleation mode was detected but slightly negatively biased when the nonvolatile nucleation mode was absent. The nonvolatile nucleation mode was always negatively biased. This electrical charge

Individual particle analysis of aerosols collected under haze and non-haze conditions at a high-elevation mountain site in the North China plain

Directory of Open Access Journals (Sweden)

W. J. Li

2011-11-01

Full Text Available The North China plain is a region with megacities and huge populations. Aerosols over the highly polluted area have a significant impact on the regional and global climate. In order to investigate the physical and chemical characteristics of aerosol particles in elevated layers there, observations were carried out at the summit of Mt. Tai (1534 m a.s.l. from 19 to 28 April, 2010, when the air masses were advected from the east (phase-I: 19–21 April, from the south (phase-II: 22–25 April, and from the northwest (phase-III: 26–28 April. Individual aerosol particles were identified with transmission electron microscopy (TEM, new particle formation (NPF and growth events were monitored by a wide-range particle spectrometer, and ion concentrations in PM_2.5 were analyzed. During phase-I and phase-II, haze layers caused by anthropogenic pollution were observed, and a high percentage of particles were sulfur-rich (47–49%. In phase-III, the haze disappeared due to the intrusion of cold air from the northwest, and mineral dust particles from deserts were dominant (43%. NPF followed by particle growth during daytime was more pronounced on hazy than on clear days. Particle growth during daytime resulted in an increase of particle geometric mean diameter from 10–22 nm in the morning to 56–96 nm in the evening. TEM analysis suggests that sulfuric acid and secondary organic compounds should be important factors for particle nucleation and growth. However, the presence of fine anthropogenic particles (e.g., soot, metal, and fly ash embedded within S-rich particles indicates that they could weaken NPF and enhance particle growth through condensation and coagulation. Abundant mineral particles in phase-III likely suppressed the NPF processes because they supplied sufficient area on which acidic gases or acids condensed.

Investigating Soot Morphology in Counterflow Flames at Elevated Pressures

KAUST Repository

Amin, Hafiz Muhammad Fahid

2018-01-01

Practical combustion devices such as gas turbines and diesel engines operate at high pressures to increase their efficiency. Pressure significantly increases the overall soot yield. Morphology of these ultra-fine particles determines their airborne lifetime and their interaction with the human respiratory system. Therefore, investigating soot morphology at high pressure is of practical relevance. In this work, a novel experimental setup has been designed and built to study the soot morphology at elevated pressures. The experimental setup consists of a pressure vessel, which can provide optical access from 10° to 165° for multi-angle light scattering, and a counterflow burner which produces laminar flames at elevated pressures. In the first part of the study, N2-diluted ethylene/air and ethane air counterflow flames are stabilized from 2 to 5 atm. Two-angle light scattering and extinction technique have been used to study the effects of pressure on soot parameters. Path averaged soot volume fraction is found to be very sensitive to pressure and increased significantly from 2 to 5 atm. Primary particle size and aggregate size also increased with pressure. Multi-angle light scattering is also performed and flames are investigated from 3 to 5 atm. Scattering to absorption ratio is calculated from multi-angle light scattering and extinction data. Scattering to absorption ratio increased with pressure whereas the number of primary particles in an aggregate decreased with increasing pressure. In the next part of the study, Thermophoretic Sampling of soot is performed, in counterflow flames from 3 to 10 atm, followed by transmission electron microscopy. Mean primary particle size increased with pressure and these trends are consistent withour light scattering measurements. Fractal properties of soot aggregates are found to be insensitive to pressure. 2D diffused light line of sight attenuation (LOSA) and Laser Induced Incandescence (LII) are used to measure local soot

Studies of dry deposition of trace elements and diesel soot onto Lake Michigan and the Chesapeake Bay

International Nuclear Information System (INIS)

Ondov, J.M.; Caffrey, P.F.; Suarez, A.E.; Han, M.; Borgoul, P.V.

1995-01-01

As part of the Atmospheric Exchange Over Lakes and Oceans Study (AEOLOS) study, the University of Maryland participated in four intensive field campaigns, three on Lake Michigan (LM) and one on the Chesapeake Bay (CB), to determine the size distributions of potentially toxic elemental aerosol constituents, determine their sources, and their dry deposition loadings to surface waters. The work further seeks to elucidate the relative importance of constituents of fine- and coarse particles, as differentiation of these modes is essential to the eventual formation of control strategies. Unique components of the UMCP studies include (1) resolution of toxic elemental components of aerosol particles depositing to LM and CB by particle size and by source and (2) a Lake-wide evaluation of the importance of fine and coarse particle deposition to inorganic contamination of LM surface waters. In addition, a unique component of the Baltimore Study was the application of a sensitive iridium tracer to intentionally tag emissions form the City of Baltimore's sanitation truck fleet to tag the Baltimore urban plume and to determine the atmospheric behavior of diesel soot particles, a major source of urban carbon aerosol and the principle carrier of toxic polynuclear aromatic hydrocarbons. The work encompasses results for >40 elements by X-ray fluorescence and instrumental neutron activation analyses of more than 700 individual size-segregated aerosol, deposition, urban dust, and surface-water-suspended particulate samples. An overview of the results of these studies will be presented

Nitro-PAH formation studied by interacting artificially PAH-coated soot aerosol with NO 2 in the temperature range of 295-523 K

Science.gov (United States)

Carrara, Matteo; Wolf, Jan-Christoph; Niessner, Reinhard

2010-10-01

Diesel particulate matter poses a threat to human health, and in particular nitrated polycyclic aromatic hydrocarbons (NPAHs) found within and on the surface of these particles. Although diesel particulate filters (DPFs) have been designed and implemented to reduce these and other harmful diesel emissions, the particle loaded filters may act as a reaction chamber for the enhanced production of NPAHs from the nitration of PAHs with NO 2. Focus is on the investigation of the heterogeneous reactions that occur on soot particles by exposing laboratory produced pyrene- or benzo(a)pyrene-coated spark discharge soot particles to varying concentrations of NO 2 and temperatures while following the formation of products over time. The sole nitration product that was observed throughout the experiments with pyrene-coated soot was 1-nitropyrene (1-NPYR), which increased linearly with reaction time for all NO 2 concentrations chosen (0.11, 1.0, 2.0, 4.0 ppm, m m -1). Resulting 1-NPYR formation rate increased exponentially with [NO 2]. Throughout the 3-h experiments less than 10% of pyrene has been converted to 1-NPYR and the partial reaction order with regard to [NO 2] was estimated to 1.52. Benzo(a)pyrene (BaP) was more reactive than pyrene. After 3 h reaction time almost 80% of the BaP has been converted to 6-NBaP. Highest 1-NPYR concentrations on particles were detected at 373 K, and at higher temperatures a considerable decrease in particulate 1-NPYR was observed. A similar trend was observed in a DPF simulation system (PM-Kat ®-like) with BaP-coated soot. In this case, highest 6-NBaP concentration on particles was detected at 423 K. Backed by corroborating results from separate gas/solid-phase partition experiments with 1-NPYR and 6-NBaP, it is likely that the newly formed 1-NPYR and 6-NBaP became transferred from particle to gas phase at higher temperatures. Results from this study confirm the presence of 1-NPYR and 6-NBaP in particulate and gas phase under conditions

Role of Fluid-Dynamics in Soot Formation and Microstructure in Acetylene-Air Laminar Diffusion Flames

Directory of Open Access Journals (Sweden)

Praveen Pandey

2015-03-01

Full Text Available Residence time and thermo-chemical environment are important factors in the soot-formation process in flames. Studies have revealed that flow-dynamics plays a dominant role in soot formation process. For understanding the effect of flow dynamics on soot formation and physical structure of the soot formed in different combustion environments two types of laminar diffusion flames of Acetylene and air, a normal diffusion flame (NDF and an inverse diffusion flame (IDF have been investigated. The fuel and air supply in the reaction zone in two flame types were kept constant but the interchange of relative position of fuel and air altered the burner exit Reynolds and Froude numbers of gases, fuel/air velocity ratio and flame shape. Soot samples were collected using thermophoretic sampling on transmission electron microscope (TEM grids at different flame heights and were analyzed off-line in a Transmission Electron Microscope. Soot primary particle size, soot aggregate size and soot volume fraction were measured using an image analysis software. In NDF the maximum flame temperature was about 1525 K and 1230 K for IDF. The soot primary particles are distinctly smaller in size in IDF (between 19 – 26 nm compared to NDF (between 29–34 nm. Both NDF and IDF show chainlike branched structure of soot agglomerate with soot particles of a nearly spherical shape. The average number of soot primary particles per aggregate in NDF was in the range of 24 to 40 and in IDF it varied between 16 to 24. Soot volume fraction was between 0.6 to 1.5 ppm in NDF where as it was less than 0.2 ppm in IDF. The change in sooting characteristics of the two flame types is attributed to changed fuel/air velocity ratio, entrainment of gas molecules and thermophoresis on soot particles.

Microphysical processing of aerosol particles in orographic clouds

Science.gov (United States)

Pousse-Nottelmann, S.; Zubler, E. M.; Lohmann, U.

2015-08-01

An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented into COSMO-Model, the regional weather forecast and climate model of the Consortium for Small-scale Modeling (COSMO). The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed us to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen (WBF) process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snowflakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snowflakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. Thereby, the processes impact the total aerosol number and mass and additionally alter the shape of the aerosol size distributions by enhancing the internally mixed/soluble Aitken and accumulation mode and generating coarse-mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases

Filter-based Aerosol Measurement Experiments using Spherical Aerosol Particles under High Temperature and High Pressure

Energy Technology Data Exchange (ETDEWEB)

Lee, Jong Chan; Jung, Woo Young; Lee, Hyun Chul; Lee, Doo Young [FNC TECH., Yongin (Korea, Republic of)

2016-05-15

Optical Particle Counter (OPC) is used to provide real-time measurement of aerosol concentration and size distribution. Glass fiber membrane filter also be used to measure average mass concentration. Three tests (MTA-1, 2 and 3) have been conducted to study thermal-hydraulic effect, a filtering tendency at given SiO{sub 2} particles. Based on the experimental results, the experiment will be carried out further with a main carrier gas of steam and different aerosol size. The test results will provide representative behavior of the aerosols under various conditions. The aim of the tests, MTA 1, 2 and 3, are to be able to 1) establish the test manuals for aerosol generation, mixing, sampling and measurement system, which defines aerosol preparation, calibration, operating and evaluation method under high pressure and high temperature 2) develop commercial aerosol test modules applicable to the thermal power plant, environmental industry, automobile exhaust gas, chemical plant, HVAC system including nuclear power plant. Based on the test results, sampled aerosol particles in the filter indicate that important parameters affecting aerosol behavior aerosols are 1) system temperature to keep above a evaporation temperature of ethanol and 2) aerosol losses due to the settling by ethanol liquid droplet.

Single particle composition measurements of artificial Calcium Carbonate aerosols

Science.gov (United States)

Zorn, S. R.; Mentel, T. F.; Schwinger, T.; Croteau, P. L.; Jayne, J.; Worsnop, D. R.; Trimborn, A.

2012-12-01

Mineral dust, with an estimated total source from natural and anthropogenic emissions of up to 2800 Tg/yr, is one of the two largest contributors to total aerosol mass, with only Sea salt having a similar source strength (up to 2600 Tg/yr). The composition of dust particles varies strongly depending on the production process and, most importantly, the source location. Therefore, the composition of single dust particles can be used both to trace source regions of air masses as well as to identify chemical aging processes. Here we present results of laboratory studies on generating artificial calcium carbonate (CaCO3) particles, a model compound for carbonaceous mineral dust particles. Particles were generated by atomizing an aqueous hydrogen carbonate solution. Water was removed using a silica diffusion dryer., then the particles were processed in an oven at temperatures up to 900°C, converting the hydrogen carbonate to its anhydrous form. The resulting aerosol was analyzed using an on-line single particle laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF). The results confirm the conversion to calcium carbonate, and validate that the produced particles indeed can be used as a model compound for carbonaceous dust aerosols.

Dielectric properties of PMMA/Soot nanocomposites.

Science.gov (United States)

Clayton, Lanetra M; Cinke, Martin; Meyyappan, M; Harmon, Julie P

2007-07-01

Dielectric analysis (DEA) of relaxation behavior in poly(methyl methacrylate) (PMMA) soot nanocomposites is described herein. The soot, an inexpensive material, consists of carbon nanotubes, amorphous and graphitic carbon and metal particles. Results are compared to earlier studies on PMMA/multi-walled nanotube (MWNT) composites and PMMA/single-walled nanotube (SWNT) composites. The beta relaxation process appeared to be unaffected by the presence of the soot, as was noted earlier in nanotube composites. The gamma relaxation region in PMMA, normally dielectrically inactive, was "awakened" in the PMMA/soot composite. This occurrence is consistent with previously published data on nanotube composites. The dielectric permittivity, s', increased with soot content. The sample with 1% soot exhibited a permittivity (at 100 Hz and 25 degrees C) of 7.3 as compared to 5.1 for neat PMMA. Soot increased the dielectric strength, deltaE, of the composites. The 1% soot sample exhibited a dielectric strength of 6.38, while the neat PMMA had a value of 2.95 at 40 degrees C. The symmetric broadening term (alpha) was slightly higher for the 1% composite at temperatures near the secondary relaxation and near the primary relaxation, but all samples deviated from symmetrical semi-circular behavior (alpha = 1). The impact of the soot filler is seen more clearly in dielectric properties than in mechanical properties studies conducted earlier.

Aging induced changes on NEXAFS fingerprints in individual combustion particles

Directory of Open Access Journals (Sweden)

V. Zelenay

2011-11-01

Full Text Available Soot particles can significantly influence the Earth's climate by absorbing and scattering solar radiation as well as by acting as cloud condensation nuclei. However, despite their environmental (as well as economic and political importance, the way these properties are affected by atmospheric processing of the combustion exhaust gases is still a subject of discussion. In this work, individual soot particles emitted from two different vehicles, a EURO 2 transporter, a EURO 3 passenger car, and a wood stove were investigated on a single-particle basis. The emitted exhaust, including the particulate and the gas phase, was processed in a smog chamber with artificial solar radiation. Single particle specimens of both unprocessed and aged soot were characterized using near edge X-ray absorption fine structure spectroscopy (NEXAFS and scanning electron microscopy. Comparison of NEXAFS spectra from the unprocessed particles and those resulting from exhaust photooxidation in the chamber revealed changes in the carbon functional group content. For the wood stove emissions, these changes were minor, related to the relatively mild oxidation conditions. For the EURO 2 transporter emissions, the most apparent change was that of carboxylic carbon from oxidized organic compounds condensing on the primary soot particles. For the EURO 3 car emissions oxidation of primary soot particles upon photochemical aging has likely contributed as well. Overall, the changes in the NEXAFS fingerprints were in qualitative agreement with data from an aerosol mass spectrometer. Furthermore, by taking full advantage of our in situ microreactor concept, we show that the soot particles from all three combustion sources changed their ability to take up water under humid conditions upon photochemical aging of the exhaust. Due to the selectivity and sensitivity of the NEXAFS technique for the water mass, also small amounts of water taken up into the internal voids of agglomerated

Nuclear track radiography of 'hot' aerosol particles

International Nuclear Information System (INIS)

Boulyga, S.F.; Kievitskaja, A.I.; Kievets, M.K.; Lomonosova, E.M.; Zhuk, I.V.; Yaroshevich, O.I.; Perelygin, V.P.; Petrova, R.; Brandt, R.; Vater, P.

1999-01-01

Nuclear track radiography was applied to identify aerosol 'hot' particles which contain elements of nuclear fuel and fallout after Chernobyl NPP accident. For the determination of the content of transuranium elements in radioactive aerosols the measurement of the α-activity of 'hot' particles by SSNTD was used in this work, as well as radiography of fission fragments formed as a result of the reactions (n,f) and (γ,f) in the irradiation of aerosol filters by thermal neutrons and high energy gamma quanta. The technique allowed the sizes and alpha-activity of 'hot' particles to be determined without extracting them from the filter, as well as the determination of the uranium content and its enrichment by 235 U, 239 Pu and 241 Pu isotopes. Sensitivity of determination of alpha activity by fission method is 5x10 -6 Bq per particle. The software for the system of image analysis was created. It ensured the identification of track clusters on an optical image of the SSNTD surface obtained through a video camera and the determination of size and activity of 'hot' particles

The effect of mineral dust and soot aerosols on ice microphysics near the foothills of the Himalayas: A numerical investigation

Science.gov (United States)

Hazra, Anupam; Padmakumari, B.; Maheskumar, R. S.; Chen, Jen-Ping

2016-05-01

This study investigates the influence of different ice nuclei (IN) species and their number concentrations on cloud ice production. The numerical simulation with different species of ice nuclei is investigated using an explicit bulk-water microphysical scheme in a Mesoscale Meteorological Model version 5 (MM5). The species dependent ice nucleation parameterization that is based on the classical nucleation theory has been implemented into the model. The IN species considered include dust and soot with two different concentrations (Low and High). The simulated cloud microphysical properties like droplet number concentration and droplet effective radii as well as macro-properties (equivalent potential temperature and relative humidity) are comparable with aircraft observations. When higher dust IN concentrations are considered, the simulation results showed good agreement with the cloud ice and cloud water mixing ratio from aircraft measurements during Cloud Aerosol Interactions and Precipitation Enhancement Experiment (CAIPEEX) and Modern Era Retrospective Analysis for Research and Applications (MERRA) reanalysis. Relative importance of IN species is shown as compared to the homogeneous freezing nucleation process. The tendency of cloud ice production rates is also analyzed and found that dust IN is more efficient in producing cloud ice when compared to soot IN. The dust IN with high concentration can produce more surface precipitation than soot IN at the same concentration. This study highlights the need to improve the ice nucleation parameterization in numerical models.

Electrospray ionizer for mass spectrometry of aerosol particles

Science.gov (United States)

He, Siqin; Hogan, Chris; Li, Lin; Liu, Benjamin Y. H.; Naqwi, Amir; Romay, Francisco

2017-09-19

A device and method are disclosed to apply ESI-based mass spectroscopy to submicrometer and nanometer scale aerosol particles. Unipolar ionization is utilized to charge the particles in order to collect them electrostatically on the tip of a tungsten rod. Subsequently, the species composing the collected particles are dissolved by making a liquid flow over the tungsten rod. This liquid with dissolved aerosol contents is formed into highly charged droplets, which release unfragmented ions for mass spectroscopy, such as time-of-flight mass spectroscopy. The device is configured to operate in a switching mode, wherein aerosol deposition occurs while solvent delivery is turned off and vice versa.

A characterization of Arctic aerosols on the basis of aerosol optical depth and black carbon measurements

Directory of Open Access Journals (Sweden)

R. S. Stone

2014-06-01

Full Text Available Abstract Aerosols, transported from distant source regions, influence the Arctic surface radiation budget. When deposited on snow and ice, carbonaceous particles can reduce the surface albedo, which accelerates melting, leading to a temperature-albedo feedback that amplifies Arctic warming. Black carbon (BC, in particular, has been implicated as a major warming agent at high latitudes. BC and co-emitted aerosols in the atmosphere, however, attenuate sunlight and radiatively cool the surface. Warming by soot deposition and cooling by atmospheric aerosols are referred to as “darkening” and “dimming” effects, respectively. In this study, climatologies of spectral aerosol optical depth AOD (2001–2011 and Equivalent BC (EBC (1989–2011 from three Arctic observatories and from a number of aircraft campaigns are used to characterize Arctic aerosols. Since the 1980s, concentrations of BC in the Arctic have decreased by more than 50% at ground stations where in situ observations are made. AOD has increased slightly during the past decade, with variations attributed to changing emission inventories and source strengths of natural aerosols, including biomass smoke and volcanic aerosol, further influenced by deposition rates and airflow patterns.

Simulation of temporal and spatial soot evolution in an automotive diesel engine using the Moss–Brookes soot model

International Nuclear Information System (INIS)

Pang, Kar Mun; Ng, Hoon Kiat; Gan, Suyin

2012-01-01

Highlights: ► Numerical models were validated against experimental data of two diesel engines. ► Soot model constant values were calibrated to predict in-cylinder soot processes. ► Effects of split-main injection parameters on soot distributions were determined. ► Soot cloud was distributed towards cylinder wall when using large dwell period. ► Greater soot deposition expected with large dwell period and retarded injection. - Abstract: In this reported work, computational study on the formation processes of soot particles from diesel combustion is conducted using an approach where Computational Fluid Dynamics (CFD) is coupled with a chemical kinetic model. A multi-step soot model which accounts for inception, surface growth, coagulation and oxidation was applied. Model constant values in the Moss–Brookes soot formation and Fenimore–Jones soot oxidation models were calibrated, and were validated against in-cylinder soot evolution and exhaust soot density of both heavy- and light-duty diesel engines, respectively. Effects of various injection parameters such as start of injection (SOI) timing, split-main ratio and dwell period of the split-main injection strategy on in-cylinder temporal/spatial soot evolution in a light-duty diesel engine were subsequently investigated. The spatial soot distributions at each crank angle degree after start of injection were found to be insensitive to the change of values in SOI and split-main ratio when close-coupled injection was implemented. Soot cloud was also observed to be distributed towards the cylinder wall when a large separation of 20° was used, even with an advanced SOI timing of −6° after top dead centre (ATDC). The use of large separation is hence not desired for this combustion system as it potentially leads to soot deposition on surface oil film and greater tailpipe soot emissions.

Towards predictive simulations of soot formation: from surrogate to turbulence

Energy Technology Data Exchange (ETDEWEB)

Blanquart, Guillaume [California Inst. of Technology (CalTech), Pasadena, CA (United States)

2017-03-28

The combustion of transportation fuels leads to the formation of several kinds of pollutants, among which are soot particles. These particles, also formed during coal combustion and in fires, are the source of several health problems and environmental issues. Unfortunately, our current understanding of the chemical and physical phenomena leading to the formation of soot particles remains incomplete, and as a result, the predictive capability of our numerical tools is lacking. The objective of the work was to reduce the gap in the present understanding and modeling of soot formation both in laminar and turbulent flames. The effort spanned several length scales from the molecular level to large scale turbulent transport.

Dynamics of flow–soot interaction in wrinkled non-premixed ethylene–air flames

KAUST Repository

Arias, Paul G.

2015-08-17

A two-dimensional simulation of a non-premixed ethylene–air flame was conducted by employing a detailed gas-phase reaction mechanism considering polycyclic aromatic hydrocarbons, an aerosol-dynamics-based soot model using a method of moments with interpolative closure, and a grey gas and soot radiation model using the discrete transfer method. Interaction of the sooting flame with a prescribed decaying random velocity field was investigated, with a primary interest in the effects of velocity fluctuations on the flame structure and the associated soot formation process for a fuel-strip configuration and a composition with mature soot growth. The temporally evolving simulation revealed a multi-layered soot formation process within the flame, at a level of detail not properly described by previous studies based on simplified soot models utilizing acetylene or naphthalene precursors for initial soot inception. The overall effect of the flame topology on the soot formation was found to be consistent with previous experimental studies, while a unique behaviour of localised strong oxidation was also noted. The imposed velocity fluctuations led to an increase of the scalar dissipation rate in the sooting zone, causing a net suppression in the soot production rate. Considering the complex structure of the soot formation layer, the effects of the imposed fluctuations vary depending on the individual soot reactions. For the conditions under study, the soot oxidation reaction was identified as the most sensitive to the fluctuations and was mainly responsible for the local suppression of the net soot production. © 2015 Taylor & Francis

Can Condensing Organic Aerosols Lead to Less Cloud Particles?

Science.gov (United States)

Gao, C. Y.; Tsigaridis, K.; Bauer, S.

2017-12-01

We examined the impact of condensing organic aerosols on activated cloud number concentration in a new aerosol microphysics box model, MATRIX-VBS. The model includes the volatility-basis set (VBS) framework in an aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) that resolves aerosol mass and number concentrations and aerosol mixing state. Preliminary results show that by including the condensation of organic aerosols, the new model (MATRIX-VBS) has less activated particles compared to the original model (MATRIX), which treats organic aerosols as non-volatile. Parameters such as aerosol chemical composition, mass and number concentrations, and particle sizes which affect activated cloud number concentration are thoroughly evaluated via a suite of Monte-Carlo simulations. The Monte-Carlo simulations also provide information on which climate-relevant parameters play a critical role in the aerosol evolution in the atmosphere. This study also helps simplifying the newly developed box model which will soon be implemented in the global model GISS ModelE as a module.

The attachment of radon daughters to submicron aerosol particles

International Nuclear Information System (INIS)

Grenier, M.G.; Bigu, J.

1984-04-01

A study of the effects of aerosol concentration, aerosol size distribution and relative humidity on the Working Level and the radon daughter concentration was conducted in a 3000 L radon environmental chamber. Typical values of the aerosol concentration varied in the 1 x 10 3 particles/cm 3 to 4.5 x 10 5 particles/cm 3 range. Various size distributions of aerosols that have mean diffusional aerodynamic diameters of .025 μm, .045 μm and .090 μm were tested. A good correlation was found between the Working Level and the aerosol concentration as well as the relative humidity. Most of the activity seems to be associated with particles of diameter between .05 μm and .2 μm. The results presented here are in agreement with work done by other investigators in the health physics field

Single-particle characterization of the high-Arctic summertime aerosol

Science.gov (United States)

Sierau, B.; Chang, R. Y.-W.; Leck, C.; Paatero, J.; Lohmann, U.

2014-07-01

Single-particle mass-spectrometric measurements were carried out in the high Arctic north of 80° during summer 2008. The campaign took place onboard the icebreaker Oden and was part of the Arctic Summer Cloud Ocean Study (ASCOS). The instrument deployed was an aerosol time-of-flight mass spectrometer (ATOFMS) that provides information on the chemical composition of individual particles and their mixing state in real time. Aerosols were sampled in the marine boundary layer at stations in the open ocean, in the marginal ice zone, and in the pack ice region. The largest fraction of particles detected for subsequent analysis in the size range of the ATOFMS between approximately 200 and 3000 nm in diameter showed mass-spectrometric patterns, indicating an internal mixing state and a biomass burning and/or biofuel source. The majority of these particles were connected to an air mass layer of elevated particle concentration mixed into the surface mixed layer from the upper part of the marine boundary layer. The second largest fraction was represented by sea salt particles. The chemical analysis of the over-ice sea salt aerosol revealed tracer compounds that reflect chemical aging of the particles during their long-range advection from the marginal ice zone, or open waters south thereof prior to detection at the ship. From our findings we conclude that long-range transport of particles is one source of aerosols in the high Arctic. To assess the importance of long-range particle sources for aerosol-cloud interactions over the inner Arctic in comparison to local and regional biogenic primary aerosol sources, the chemical composition of the detected particles was analyzed for indicators of marine biological origin. Only a minor fraction showed chemical signatures of potentially ocean-derived primary particles of that kind. However, a chemical bias in the ATOFMS's detection capabilities observed during ASCOS might suggest the presence of a particle type of unknown composition

Single-particle characterization of the High Arctic summertime aerosol

Science.gov (United States)

Sierau, B.; Chang, R. Y.-W.; Leck, C.; Paatero, J.; Lohmann, U.

2014-01-01

Single-particle mass spectrometric measurements were carried out in the High Arctic north of 80° during summer 2008. The campaign took place onboard the icebreaker Oden and was part of the Arctic Summer Cloud Ocean Study (ASCOS). The instrument deployed was an Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) that provides information on the chemical composition of individual particles and their mixing state in real-time. Aerosols were sampled in the marine boundary layer at stations in the open ocean, in the marginal ice zone, and in the pack ice region. The largest fraction of particles detected for subsequent analysis in the size range of the ATOFMS between approximately 200 nm to 3000 nm in diameter showed mass spectrometric patterns indicating an internal mixing state and a biomass burning and/or biofuel source. The majority of these particles were connected to an air mass layer of elevated particle concentration mixed into the surface mixed layer from the upper part of the marine boundary layer. The second largest fraction was represented by sea salt particles. The chemical analysis of the over-ice sea salt aerosol revealed tracer compounds that reflect chemical aging of the particles during their long-range advection from the marginal ice zone, or open waters south thereof prior to detection at the ship. From our findings we conclude that long-range transport of particles is one source of aerosols in the High Arctic. To assess the importance of long-range particle sources for aerosol-cloud interactions over the inner Arctic in comparison to local and regional biogenic primary aerosol sources, the chemical composition of the detected particles was analyzed for indicators of marine biological origin. Only a~minor fraction showed chemical signatures of potentially ocean-derived primary particles of that kind. However, a chemical bias in the ATOFMS's detection capabilities observed during ASCOS might suggest a presence of a particle type of unknown composition

Effect of Dimethyl Ether Mixing on Soot Size Distribution in Premixed Ethylene Flame

KAUST Repository

Li, Zepeng

2016-01-01

As a byproduct of incomplete combustion, soot attracts increasing attentions as extensive researches exploring serious health and environmental effects from soot particles. Soot emission reduction requires a comprehensive understanding

On the formation and early evolution of soot in turbulent nonpremixed flames

KAUST Repository

Bisetti, Fabrizio

2012-01-01

A Direct Numerical Simulation (DNS) of soot formation in an n-heptane/air turbulent nonpremixed flame has been performed to investigate unsteady strain effects on soot growth and transport. For the first time in a DNS of turbulent combustion, Polycyclic Aromatic Hydrocarbons (PAH) are included via a validated, reduced chemical mechanism. A novel statistical representation of soot aggregates based on the Hybrid Method of Moments is used [M.E. Mueller, G. Blanquart, H. Pitsch, Combust. Flame 156 (2009) 1143-1155], which allows for an accurate state-of-the-art description of soot number density, volume fraction, and morphology of the aggregates. In agreement with previous experimental studies in laminar flames, Damköhler number effects are found to be significant for PAH. Soot nucleation and growth from PAH are locally inhibited by high scalar dissipation rate, thus providing a possible explanation for the experimentally observed reduction of soot yields at increasing levels of mixing in turbulent sooting flames. Furthermore, our data indicate that soot growth models that rely on smaller hydrocarbon species such as acetylene as a proxy for large PAH molecules ignore or misrepresent the effects of turbulent mixing and hydrodynamic strain on soot formation due to differences in the species Damköhler number. Upon formation on the rich side of the flame, soot is displaced relative to curved mixture fraction iso-surfaces due to differential diffusion effects between soot and the gas-phase. Soot traveling towards the flame is oxidized, and aggregates displaced away from the flame grow primarily by condensation of PAH on the particle surface. In contrast to previous DNS studies based on simplified soot and chemistry models, surface reactions are found to contribute barely to the growth of soot, for nucleation and condensation processes occurring in the fuel stream are responsible for the most of soot mass generation. Furthermore, the morphology of the soot aggregates is

Nuclear track radiography of 'hot' aerosol particles

CERN Document Server

Boulyga, S F; Kievets, M K; Lomonosova, E M; Zhuk, I V; Yaroshevich, O I; Perelygin, V P; Petrova, R I; Brandt, R; Vater, P

1999-01-01

Nuclear track radiography was applied to identify aerosol 'hot' particles which contain elements of nuclear fuel and fallout after Chernobyl NPP accident. For the determination of the content of transuranium elements in radioactive aerosols the measurement of the alpha-activity of 'hot' particles by SSNTD was used in this work, as well as radiography of fission fragments formed as a result of the reactions (n,f) and (gamma,f) in the irradiation of aerosol filters by thermal neutrons and high energy gamma quanta. The technique allowed the sizes and alpha-activity of 'hot' particles to be determined without extracting them from the filter, as well as the determination of the uranium content and its enrichment by sup 2 sup 3 sup 5 U, sup 2 sup 3 sup 9 Pu and sup 2 sup 4 sup 1 Pu isotopes. Sensitivity of determination of alpha activity by fission method is 5x10 sup - sup 6 Bq per particle. The software for the system of image analysis was created. It ensured the identification of track clusters on an optical imag...

Aerosol-Cloud Interactions During Puijo Cloud Experiments - The effects of weather and local sources

Science.gov (United States)

Komppula, Mika; Portin, Harri; Leskinen, Ari; Romakkaniemi, Sami; Brus, David; Neitola, Kimmo; Hyvärinen, Antti-Pekka; Kortelainen, Aki; Hao, Liqing; Miettinen, Pasi; Jaatinen, Antti; Ahmad, Irshad; Lihavainen, Heikki; Laaksonen, Ari; Lehtinen, Kari E. J.

2013-04-01

The Puijo measurement station has provided continuous data on aerosol-cloud interactions since 2006. The station is located on top of the Puijo observation tower (306 m a.s.l, 224 m above the surrounding lake level) in Kuopio, Finland. The top of the tower is covered by cloud about 15 % of the time, offering perfect conditions for studying aerosol-cloud interactions. With a twin-inlet setup (total and interstitial inlets) we are able to separate the activated particles from the interstitial (non-activated) particles. The continuous twin-inlet measurements include aerosol size distribution, scattering and absorption. In addition cloud droplet number and size distribution are measured continuously with weather parameters. During the campaigns the twin-inlet system was additionally equipped with aerosol mass spectrometer (AMS) and Single Particle Soot Photometer (SP-2). This way we were able to define the differences in chemical composition of the activated and non-activated particles. Potential cloud condensation nuclei (CCN) in different supersaturations were measured with two CCN counters (CCNC). The other CCNC was operated with a Differential Mobility Analyzer (DMA) to obtain size selected CCN spectra. Other additional measurements included Hygroscopic Tandem Differential Mobility Analyzer (HTDMA) for particle hygroscopicity. Additionally the valuable vertical wind profiles (updraft velocities) are available from Halo Doppler lidar during the 2011 campaign. Cloud properties (droplet number and effective radius) from MODIS instrument onboard Terra and Aqua satellites were retrieved and compared with the measured values. This work summarizes the two latest intensive campaigns, Puijo Cloud Experiments (PuCE) 2010 & 2011. We study especially the effect of the local sources on the cloud activation behaviour of the aerosol particles. The main local sources include a paper mill, a heating plant, traffic and residential areas. The sources can be categorized and identified

Interdigitated Pt-GaN Schottky interfaces for high-temperature soot-particulate sensing

Science.gov (United States)

So, Hongyun; Hou, Minmin; Jain, Sambhav R.; Lim, Jongwoo; Senesky, Debbie G.

2016-04-01

A microscale soot-particulate sensor using interdigitated platinum-gallium nitride (Pt-GaN) Schottky interfaces was developed to monitor fine soot particles within high-temperature environments (e.g., combustion exhausts and flues). Upon exposure to soot particles (30 to 50 nm in diameter) from an experimental chimney, an increased current (∼43.6%) is observed through the back-to-back Schottky contact to n-type GaN. This is attributed to a reduction in the effective Schottky barrier height (SBH) of ∼10 meV due to the electric field from the charged soot particles in the depletion region and exposed GaN surface. Furthermore, the microfabricated sensor was shown to recover sensitivity and regenerate the sensing response (∼11 meV SBH reduction) after exposure to temperature as high as 550 °C. This study supports the feasibility of a simple and reliable soot sensor to meet the increasing market demand for particulate matter sensing in harsh environments.

Aerosol particle transport modeling for preclosure safety studies of nuclear waste repositories

International Nuclear Information System (INIS)

Gelbard, F.

1989-01-01

An important concern for preclosure safety analysis of a nuclear waste repository is the potential release to the environment of respirable aerosol particles. Such particles, less than 10 μm in aerodynamic diameter, may have significant adverse health effects if inhaled. To assess the potential health effects of these particles, it is not sufficient to determine the mass fraction of respirable aerosol. The chemical composition of the particles is also of importance since different radionuclides may pose vastly different health hazards. Thus, models are needed to determine under normal and accident conditions the particle size and the chemical composition distributions of aerosol particles as a function of time and of position in the repository. In this work a multicomponent sectional aerosol model is used to determine the aerosol particle size and composition distributions in the repository. A range of aerosol mass releases with varying mean particle sizes and chemical compositions is used to demonstrate the sensitivities and uncertainties of the model. Decontamination factors for some locations in the repository are presented. 8 refs., 1 tab

Light-Absorbing Aerosol during NASA GRIP: Overview of Observations in the Free Troposphere and Associated with Tropical Storm Systems

Science.gov (United States)

Ziemba, L. D.; Beyersdorf, A. J.; Chen, G.; Corr, C. A.; Craig, L.; Dhaniyala, S.; Dibb, J. E.; Hudgins, C. H.; Ismail, S.; Latham, T.; Nenes, A.; Thornhill, K. L.; Winstead, E.; Anderson, B. E.

2010-12-01

Aerosols play a significant role in regulating Earth’s climate. Absorbing aerosols typically constitute a small fraction of ambient particle mass but can contribute significantly to direct and indirect climate forcing depending on size, mixing state, concentration, chemical composition, and vertical and spatial distribution. Aerosols may also significantly affect tropical storm/hurricane dynamics through direct light absorption and activation as cloud nuclei. An extensive suite of instrumentation measuring aerosol chemical, physical, and optical properties was deployed aboard the NASA DC-8 to characterize aerosol during the NASA GRIP (Genesis and Rapid Intensification Processes; August-September 2010) mission. The majority of flight time was spent at high altitude (greater than 9 km) and thus much of the sampling was done in the free troposphere, including extensive sampling in the vicinity of tropical storm systems and more diffuse cirrus clouds. With operations based in Fort Lauderdale, FL and St. Croix, U.S. Virgin Islands, a large geographic region was sampled including much of the Gulf of Mexico and tropical Atlantic Ocean. Observations are reported for light-absorbing carbon aerosol (mainly black carbon, BC) primarily using a single particle soot photometer (SP2). The SP2 employs single-particle laser-induced incandescence to provide a mass-specific measurement not subject to scattering interference that is optimal for the low concentration environments like those encountered during GRIP. BC mass concentrations, 100-500 nm size distributions, and mixing state (i.e. coating thickness of scattering material) are presented. Total and sub-micron aerosol absorption coefficients (principally from BC and dust aerosol) are reported using a particle soot absorption photometer (PSAP) along with comparisons with calculated absorption coefficients derived from SP2 observations in various conditions. In addition, dust aerosol is specifically identified using optical and

Soot modeling of counterflow diffusion flames of ethylene-based binary mixture fuels

KAUST Repository

Wang, Yu

2015-03-01

A soot model was developed based on the recently proposed PAH growth mechanism for C1-C4 gaseous fuels (KAUST PAH Mechanism 2, KM2) that included molecular growth up to coronene (A7) to simulate soot formation in counterflow diffusion flames of ethylene and its binary mixtures with methane, ethane and propane based on the method of moments. The soot model has 36 soot nucleation reactions from 8 PAH molecules including pyrene and larger PAHs. Soot surface growth reactions were based on a modified hydrogen-abstraction-acetylene-addition (HACA) mechanism in which CH3, C3H3 and C2H radicals were included in the hydrogen abstraction reactions in addition to H atoms. PAH condensation on soot particles was also considered. The experimentally measured profiles of soot volume fraction, number density, and particle size were well captured by the model for the baseline case of ethylene along with the cases involving mixtures of fuels. The simulation results, which were in qualitative agreement with the experimental data in the effects of binary fuel mixing on the sooting structures of the measured flames, showed in particular that 5% addition of propane (ethane) led to an increase in the soot volume fraction of the ethylene flame by 32% (6%), despite the fact that propane and ethane are less sooting fuels than is ethylene, which is in reasonable agreement with experiments of 37% (14%). The model revealed that with 5% addition of methane, there was an increase of 6% in the soot volume fraction. The average soot particle sizes were only minimally influenced while the soot number densities were increased by the fuel mixing. Further analysis of the numerical data indicated that the chemical cross-linking effect between ethylene and the dopant fuels resulted in an increase in PAH formation, which led to higher soot nucleation rates and therefore higher soot number densities. On the other hand, the rates of soot surface growth per unit surface area through the HACA mechanism were

Nuclear microprobe analysis and source apportionment of individual atmospheric aerosol particles

International Nuclear Information System (INIS)

Artaxo, P.; Rabello, M.L.C.; Watt, F.; Grime, G.; Swietlicki, E.

1993-01-01

In atmospheric aerosol reserach, one key issue is to determine the sources of the airborne particles. Bulk PIXE analysis coupled with receptor modeling provides a useful, but limited view of the aerosol sources influencing one particular site or sample. The scanning nuclear microprobe (SNM) technique is a microanalytical technique that gives unique information on individual aerosol particles. In the SNM analyses a 1.0 μm size 2.4 MeV proton beam from the Oxford SNM was used. The trace elements with Z>11 were measured by the particle induced X-ray emission (PIXE) method with detection limits in the 1-10 ppm range. Carbon, nitrogen and oxygen are measured simultaneously using Rutherford backscattering spectrometry (RBS). Atmospheric aerosol particles were collected at the Brazilian Antarctic Station and at biomass burning sites in the Amazon basin tropical rain forest in Brazil. In the Antarctic samples, the sea-salt aerosol particles were clearly predominating, with NaCl and CaSO 4 as major compounds with several trace elements as Al, Si, P, K, Mn, Fe, Ni, Cu, Zn, Br, Sr, and Pb. Factor analysis of the elemental data showed the presence of four components: 1) Soil dust particles; 2) NaCl particles; 3) CaSO 4 with Sr; and 4) Br and Mg. Strontium, observed at 20-100 ppm levels, was always present in the CaSO 4 particles. The hierarchical cluster procedure gave results similar to the ones obtained through factor analysis. For the tropical rain forest biomass burning aerosol emissions, biogenic particles with a high organic content dominate the particle population, while K, P, Ca, Mg, Zn, and Si are the dominant elements. Zinc at 10-200 ppm is present in biogenic particles rich in P and K. The quantitative aspects and excellent detection limits make SNM analysis of individual aerosol particles a very powerful analytical tool. (orig.)

A recirculation aerosol wind tunnel for evaluating aerosol samplers and measuring particle penetration through protective clothing materials.

Science.gov (United States)

Jaques, Peter A; Hsiao, Ta-Chih; Gao, Pengfei

2011-08-01

A recirculation aerosol wind tunnel was designed to maintain a uniform airflow and stable aerosol size distribution for evaluating aerosol sampler performance and determining particle penetration through protective clothing materials. The oval-shaped wind tunnel was designed to be small enough to fit onto a lab bench, have optimized dimensions for uniformity in wind speed and particle size distributions, sufficient mixing for even distribution of particles, and minimum particle losses. Performance evaluation demonstrates a relatively high level of spatial uniformity, with a coefficient of variation of 1.5-6.2% for wind velocities between 0.4 and 2.8 m s(-1) and, in this range, 0.8-8.5% for particles between 50 and 450 nm. Aerosol concentration stabilized within the first 5-20 min with, approximately, a count median diameter of 135 nm and geometric standard deviation of 2.20. Negligible agglomerate growth and particle loss are suggested. The recirculation design appears to result in unique features as needed for our research.

The circular thermo-phoretic spectrometer (CTSM), a new device for the study of the thermophoresis, Application on the fractals soot particles

International Nuclear Information System (INIS)

Brugiere, E.

2012-01-01

This work aims to improve the understanding of soot particle deposition by thermophoresis. In order to show the influence of the morphology of a fractal aggregate on its thermo-phoretic behavior, a new experimental device has been developed; the SpectroMetre Thermophoretique Circulaire (SMTC). This instrument is used to measure the mean thermo-phoretic velocity of particles selected between a hot plate and a cold plate thanks to a transfer function based on the geometry of the radial flow differential mobility analyser RF-DMA or SMEC (Spectrometre de Mobilite Electrique Circulaire). For the experimental validation, effective thermo-phoretic velocities of monodispersed spherical latex particles for diameters ranging from 64 nm to 500 nm and a temperature gradient equal to 50 750 K/m are measured and compared with theoretical values. The good agreement between the experimental results and theoretical values of Beresnev and Chernyak (1995) helps us to validate the operation of the instrument. Then we compare experimental thermo-phoretic velocity obtained with the SMTC for spherical particles and aggregates produced by a combustion aerosol generator. Contrary to the results obtained with the PSL particles, we observe that the thermo-phoretic velocity of aggregates increases with the electrical mobility diameter. Thanks to a morphological study of the aggregates, we showed that the thermo-phoretic velocity depends on the number of primary particles of the aggregate. These experimental results confirm, for the first time, the theoretical data of Mackowski (2006) obtained by a Monte Carlo simulation. Moreover, a comparison with the experimental results of Messerer et al. (2003) shows that the thermo-phoretic velocity of aggregates seems independent of the primary particle size. (author)

Effect of Drive Cycle and Gasoline Particulate Filter on the Size and Morphology of Soot Particles Emitted from a Gasoline-Direct-Injection Vehicle.

Science.gov (United States)

Saffaripour, Meghdad; Chan, Tak W; Liu, Fengshan; Thomson, Kevin A; Smallwood, Gregory J; Kubsh, Joseph; Brezny, Rasto

2015-10-06

The size and morphology of particulate matter emitted from a light-duty gasoline-direct-injection (GDI) vehicle, over the FTP-75 and US06 transient drive cycles, have been characterized by transmission-electron-microscope (TEM) image analysis. To investigate the impact of gasoline particulate filters on particulate-matter emission, the results for the stock-GDI vehicle, that is, the vehicle in its original configuration, have been compared to the results for the same vehicle equipped with a catalyzed gasoline particulate filter (GPF). The stock-GDI vehicle emits graphitized fractal-like aggregates over all driving conditions. The mean projected area-equivalent diameter of these aggregates is in the 78.4-88.4 nm range and the mean diameter of primary particles varies between 24.6 and 26.6 nm. Post-GPF particles emitted over the US06 cycle appear to have an amorphous structure, and a large number of nucleation-mode particles, depicted as low-contrast ultrafine droplets, are observed in TEM images. This indicates the emission of a substantial amount of semivolatile material during the US06 cycle, most likely generated by the incomplete combustion of accumulated soot in the GPF during regeneration. The size of primary particles and soot aggregates does not vary significantly by implementing the GPF over the FTP-75 cycle; however, particles emitted by the GPF-equipped vehicle over the US06 cycle are about 20% larger than those emitted by the stock-GDI vehicle. This may be attributed to condensation of large amounts of organic material on soot aggregates. High-contrast spots, most likely solid nonvolatile cores, are observed within many of the nucleation-mode particles emitted over the US06 cycle by the GPF-equipped vehicle. These cores are either generated inside the engine or depict incipient soot particles which are partially carbonized in the exhaust line. The effect of drive cycle and the GPF on the fractal parameters of particles, such as fractal dimension and

Single-particle characterization of the high-Arctic summertime aerosol

Directory of Open Access Journals (Sweden)

B. Sierau

2014-07-01

Full Text Available Single-particle mass-spectrometric measurements were carried out in the high Arctic north of 80° during summer 2008. The campaign took place onboard the icebreaker Oden and was part of the Arctic Summer Cloud Ocean Study (ASCOS. The instrument deployed was an aerosol time-of-flight mass spectrometer (ATOFMS that provides information on the chemical composition of individual particles and their mixing state in real time. Aerosols were sampled in the marine boundary layer at stations in the open ocean, in the marginal ice zone, and in the pack ice region. The largest fraction of particles detected for subsequent analysis in the size range of the ATOFMS between approximately 200 and 3000 nm in diameter showed mass-spectrometric patterns, indicating an internal mixing state and a biomass burning and/or biofuel source. The majority of these particles were connected to an air mass layer of elevated particle concentration mixed into the surface mixed layer from the upper part of the marine boundary layer. The second largest fraction was represented by sea salt particles. The chemical analysis of the over-ice sea salt aerosol revealed tracer compounds that reflect chemical aging of the particles during their long-range advection from the marginal ice zone, or open waters south thereof prior to detection at the ship. From our findings we conclude that long-range transport of particles is one source of aerosols in the high Arctic. To assess the importance of long-range particle sources for aerosol–cloud interactions over the inner Arctic in comparison to local and regional biogenic primary aerosol sources, the chemical composition of the detected particles was analyzed for indicators of marine biological origin. Only a minor fraction showed chemical signatures of potentially ocean-derived primary particles of that kind. However, a chemical bias in the ATOFMS's detection capabilities observed during ASCOS might suggest the presence of a particle type of

Contributions of Organic Sources to Atmospheric Aerosol Particle Concentrations and Growth

Science.gov (United States)

Russell, L. M.

2017-12-01

Organic molecules are important contributors to aerosol particle mass and number concentrations through primary emissions as well as secondary growth in the atmosphere. New techniques for measuring organic aerosol components in atmospheric particles have improved measurements of this contribution in the last 20 years, including Scanning Transmission X-ray Microscopy Near Edge X-ray Absorption Fine Structure (STXM-NEXAFS), Fourier Transform Infrared spectroscopy (FTIR), and High-Resolution Aerosol Mass Spectrometry (AMS). STXM-NEXAFS individual aerosol particle composition illustrated the variety of morphology of organic components in marine aerosols, the inherent relationships between organic composition and shape, and the links between atmospheric aerosol composition and particles produced in smog chambers. This type of single particle microscopy has also added to size distribution measurements by providing evidence of how surface-controlled and bulk-controlled processes contribute to the growth of particles in the atmosphere. FTIR analysis of organic functional groups are sufficient to distinguish combustion, marine, and terrestrial organic particle sources and to show that each of those types of sources has a surprisingly similar organic functional group composition over four different oceans and four different continents. Augmenting the limited sampling of these off-line techniques with side-by-side inter-comparisons to online AMS provides complementary composition information and consistent quantitative attribution to sources (despite some clear method differences). Single-particle AMS techniques using light scattering and event trigger modes have now also characterized the types of particles found in urban, marine, and ship emission aerosols. Most recently, by combining with off-line techniques, single particle composition measurements have separated and quantified the contributions of organic, sulfate and salt components from ocean biogenic and sea spray

Gravitational agglomeration of post-HCDA LMFBR aerosols: nonspherical particles

International Nuclear Information System (INIS)

Tuttle, R.F.; Loyalka, S.K.

1982-12-01

Aerosol behavior analysis computer programs have shown that temporal aerosol size distributions in nuclear reactor containments are sensitive to shape factors. This research investigates shape factors by a detailed theoretical analysis of hydrodynamic interactions between a nonspherical particle and a spherical particle undergoing gravitational collisions in an LMFBR environment. First, basic definitions and expressions for settling speeds and collisional efficiencies of nonspherical particles are developed. These are then related to corresponding quantities for spherical particles through shape factors. Using volume equivalent diameter as the defining length in the gravitational collision kernel, the aerodynamic shape factor, the density correction factor, and the gravitational collision shape factor, are introduced to describe the collision kernel for collisions between aerosol agglomerates. The Navier-Stokes equation in oblate spheroidal coordinates is solved to model a nonspherical particle and then the dynamic equations for two particle motions are developed. A computer program (NGCEFF) is constructed, and the dynamical equations are solved by Gear's method

Source identification of individual soot agglomerates in Arctic air by transmission electron microscopy

Science.gov (United States)

Weinbruch, S.; Benker, N.; Kandler, K.; Schütze, K.; Kling, K.; Berlinger, B.; Thomassen, Y.; Drotikova, T.; Kallenborn, R.

2018-01-01

Individual soot agglomerates collected at four different locations on the Arctic archipelago Svalbard (Norway) were characterised by transmission electron microscopy and energy-dispersive X-ray microanalysis. For source identification of the ambient soot agglomerates, samples from different local sources (coal burning power plants in Longyearbyen and Barentsburg, diesel and oil burning for power generation in Sveagruva and Ny Ålesund, cruise ship) as well as from other sources which may contribute to Arctic soot concentrations (biomass burning, aircraft emissions, diesel engines) were investigated. Diameter and graphene sheet separation distance of soot primary particles were found to be highly variable within each source and are not suited for source identification. In contrast, concentrations of the minor elements Si, P, K, Ca and Fe showed significant differences which can be used for source attribution. The presence/absence of externally mixed particle groups (fly ashes, tar balls, mercury particles) gives additional hints about the soot sources. Biomass/wood burning, ship emissions and coal burning in Barentsburg can be excluded as major source for ambient soot at Svalbard. The coal power plant in Longyearbyen is most likely a major source of soot in the settlement of Longyearbyen but does not contribute significantly to soot collected at the Global Atmosphere Watch station Zeppelin Mountain near Ny Ålesund. The most probable soot sources at Svalbard are aircraft emissions and diesel exhaust as well as long range transport of coal burning emissions.

Non-ammonium reduced nitrogen species in atmospheric aerosol particles

Energy Technology Data Exchange (ETDEWEB)

Dod, R.L.; Gundel, L.A.; Benner, W.H.; Novakov, T.

1983-08-01

The traditional belief that ambient aerosol particles contain nitrogen predominantly in the form of inorganic ionic species such as NH/sub 4//sup +/ and NO/sub 3//sup -/ was challenged about 10 years ago by results from x-ray photoelectron spectroscopic analysis (ESCA) of California aerosol particles. A significant fraction (approx. 50%) of the reduced nitrogen was observed to have an oxidation state more reduced than ammonium, characteristic of organic nitrogen species. We have used a recently developed thermal evolved gas analysis method (NO/sub x/) in conjunction with ESCA to confirm the existence of these species in aerosol particles collected in both the United States and Europe. The agreement of EGA and ESCA analyses indicates that these species are found not only on the surface but also throughout the particles. 9 references, 6 figures.

Determination of the spectral behaviour of atmospheric soot using different particle models

Science.gov (United States)

Skorupski, Krzysztof

2017-08-01

In the atmosphere, black carbon aggregates interact with both organic and inorganic matter. In many studies they are modeled using different, less complex, geometries. However, some common simplification might lead to many inaccuracies in the following light scattering simulations. The goal of this study was to compare the spectral behavior of different, commonly used soot particle models. For light scattering simulations, in the visible spectrum, the ADDA algorithm was used. The results prove that the relative extinction error δCext, in some cases, can be unexpectedly large. Therefore, before starting excessive simulations, it is important to know what error might occur.

Two-dimensional quantification of soot and flame-soot interaction in spray combustion at elevated pressures - Final report

Energy Technology Data Exchange (ETDEWEB)

Gerber, T.

2008-07-15

Single-pulse time-resolved laser-induced incandescence (TiRe-LII) signal transients from soot particulates were acquired during unsteady high pressure Diesel combustion in a constant volume cell near top dead centre conditions typically found in a Diesel engine. Measurements were performed for initial gas pressures between 1 MPa and 3 MPa, injection pressures between 50 MPa and 130 MPa and laser probe timings between 5 ms and 16 ms after start of fuel injection. In separate experiments and for the same cell operating conditions, gas temperatures were deduced from spectrally resolved soot pyrometry measurements. Implementing the LII model of Kock et al. ensemble mean soot particle diameters were evaluated from least-squares fitting of theoretical cooling curves to experimental TiRe-LII signal transients. Since in the experiments the environmental gas temperature and the width of an assumed particle size distribution were not known, the effects of the initial choice of these parameters on retrieved particle diameters were investigated. It is shown that evaluated mean particle diameters are only slightly biased by the choice of typical size distribution widths and gas temperatures. For a fixed combustion phase mean particle diameters are not much affected by gas pressure, however they become smaller at high fuel injection pressure. At a mean chamber pressure of 1.4 MPa evaluated mean particle diameters increased by a factor of two for probe delays between 5 ms and 16 ms after start of injection, irrespective of the choices of first-guess fitting variables, indicating a certain robustness of data analysis procedure. (author)

Developing a predictive model for the chemical composition of soot nanoparticles

Energy Technology Data Exchange (ETDEWEB)

Violi, Angela [Univ. of Michigan, Ann Arbor, MI (United States); Michelsen, Hope [Sandia National Lab. (SNL-CA), Livermore, CA (United States); Hansen, Nils [Sandia National Lab. (SNL-CA), Livermore, CA (United States); Wilson, Kevin [Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

2017-04-07

In order to provide the scientific foundation to enable technology breakthroughs in transportation fuel, it is important to develop a combustion modeling capability to optimize the operation and design of evolving fuels in advanced engines for transportation applications. The goal of this proposal is to develop a validated predictive model to describe the chemical composition of soot nanoparticles in premixed and diffusion flames. Atomistic studies in conjunction with state-of-the-art experiments are the distinguishing characteristics of this unique interdisciplinary effort. The modeling effort has been conducted at the University of Michigan by Prof. A. Violi. The experimental work has entailed a series of studies using different techniques to analyze gas-phase soot precursor chemistry and soot particle production in premixed and diffusion flames. Measurements have provided spatial distributions of polycyclic aromatic hydrocarbons and other gas-phase species and size and composition of incipient soot nanoparticles for comparison with model results. The experimental team includes Dr. N. Hansen and H. Michelsen at Sandia National Labs' Combustion Research Facility, and Dr. K. Wilson as collaborator at Lawrence Berkeley National Lab's Advanced Light Source. Our results show that the chemical and physical properties of nanoparticles affect the coagulation behavior in soot formation, and our results on an experimentally validated, predictive model for the chemical composition of soot nanoparticles will not only enhance our understanding of soot formation since but will also allow the prediction of particle size distributions under combustion conditions. These results provide a novel description of soot formation based on physical and chemical properties of the particles for use in the next generation of soot models and an enhanced capability for facilitating the design of alternative fuels and the engines they will power.

Measurement of particle size distribution and mass concentration of nuclear fuel aerosols

International Nuclear Information System (INIS)

Pickering, S.

1982-01-01

The particle size distribution and particle mass concentration of a nuclear fuel aerosol is measured by admitting the aerosol into a vertically-extending container, positioning an alpha particle detector within the container so that its window is horizontal and directed vertically, stopping the admission of aerosol into the container, detecting the alpha-activity of the particles of the aerosol sedimenting onto the detector window (for example in a series of equal time intervals until a constant level is reached), and converting the alpha-activity measurements into particle size distribution and/or particle mass concentration measurements. The detector is attached to a pivotted arm and by raising a counterweight can be lowered from the container for cleaning. (author)

Effects of morphology and wavelength on the measurement accuracy of soot volume fraction by laser extinction

Science.gov (United States)

Wang, Ya-fei; Huang, Qun-xing; Wang, Fei; Chi, Yong; Yan, Jian-hua

2018-01-01

A novel method to evaluate the quantitative effects of soot morphology and incident wavelength on the measurement accuracy of soot volume fraction, by the laser extinction (LE) technique is proposed in this paper. The results indicate that the traditional LE technique would overestimate soot volume fraction if the effects of morphology and wavelength are not considered. Before the agglomeration of isolated soot primary particles, the overestimation of the LE technique is in the range of 2-20%, and rises with increasing primary particle diameter and with decreasing incident wavelength. When isolated primary particles are agglomerated into fractal soot aggregates, the overestimation would exceed 30%, and rise with increasing primary particle number per soot aggregate, fractal dimension and fractal prefactor and with decreasing incident wavelength to a maximum value of 55%. Finally, based on these results above, the existing formula of the LE technique gets modified, and the modification factor is 0.65-0.77.

Fluorescent biological aerosol particles measured with the Waveband Integrated Bioaerosol Sensor WIBS-4: laboratory tests combined with a one year field study

Directory of Open Access Journals (Sweden)

E. Toprak

2013-01-01

Full Text Available In this paper bioaerosol measurements conducted with the Waveband Integrated Bioaerosol Sensor mark 4 (WIBS-4 are presented. The measurements comprise aerosol chamber characterization experiments and a one-year ambient measurement period at a semi-rural site in South Western Germany. This study aims to investigate the sensitivity of WIBS-4 to biological and non-biological aerosols and detection of biological particles in the ambient aerosol. Several types of biological and non-biological aerosol samples, including fungal spores, bacteria, mineral dust, ammonium sulphate, combustion soot, and fluorescent polystyrene spheres, were analyzed by WIBS-4 in the laboratory. The results confirm the sensitivity of the ultraviolet light-induced fluorescence (UV-LIF method to biological fluorophores and show the good discrimination capabilities of the two excitation wavelengths/detection wavebands method applied in WIBS-4. However, a weak cross-sensitivity to non-biological fluorescent interferers remains and is discussed in this paper.

All the laboratory studies have been undertaken in order to prepare WIBS-4 for ambient aerosol measurements. According to the one-year ambient aerosol study, number concentration of fluorescent biological aerosol particles (FBAP show strong seasonal and diurnal variability. The highest number concentration of FBAP was measured during the summer term and decreased towards the winter period when colder and drier conditions prevail. Diurnal FBAP concentrations start to increase after sunset and reach maximum values during the late night and early morning hours. On the other hand, the total aerosol number concentration was almost always higher during daytime than during nighttime and a sharp decrease after sunset was observed. There was no correlation observed between the FBAP concentration and the meteorological parameters temperature, precipitation, wind direction and wind speed. However, a clear correlation was

Dynamics of flow–soot interaction in wrinkled non-premixed ethylene–air flames

KAUST Repository

Arias, Paul G.; Lecoustre, Vivien R.; Roy, Somesh; Luo, Zhaoyu; Haworth, Daniel C.; Lu, Tianfeng; Trouvé , Arnaud; Im, Hong G.

2015-01-01

A two-dimensional simulation of a non-premixed ethylene–air flame was conducted by employing a detailed gas-phase reaction mechanism considering polycyclic aromatic hydrocarbons, an aerosol-dynamics-based soot model using a method of moments

Aerosol Properties of the Atmospheres of Extrasolar Giant Planets

Energy Technology Data Exchange (ETDEWEB)

Lavvas, P. [Groupe de Spectrométrie Moléculaire et Atmosphérique, UMR CNRS 7331, Université de Reims Champagne Ardenne, Reims (France); Koskinen, T., E-mail: panayotis.lavvas@univ-reims.fr [Lunar and Planetary Laboratory, University of Arizona, Tucson, AZ (United States)

2017-09-20

We use a model of aerosol microphysics to investigate the impact of high-altitude photochemical aerosols on the transmission spectra and atmospheric properties of close-in exoplanets, such as HD 209458 b and HD 189733 b. The results depend strongly on the temperature profiles in the middle and upper atmospheres, which are poorly understood. Nevertheless, our model of HD 189733 b, based on the most recently inferred temperature profiles, produces an aerosol distribution that matches the observed transmission spectrum. We argue that the hotter temperature of HD 209458 b inhibits the production of high-altitude aerosols and leads to the appearance of a clearer atmosphere than on HD 189733 b. The aerosol distribution also depends on the particle composition, photochemical production, and atmospheric mixing. Due to degeneracies among these inputs, current data cannot constrain the aerosol properties in detail. Instead, our work highlights the role of different factors in controlling the aerosol distribution that will prove useful in understanding different observations, including those from future missions. For the atmospheric mixing efficiency suggested by general circulation models, we find that the aerosol particles are small (∼nm) and probably spherical. We further conclude that a composition based on complex hydrocarbons (soots) is the most likely candidate to survive the high temperatures in hot-Jupiter atmospheres. Such particles would have a significant impact on the energy balance of HD 189733 b’s atmosphere and should be incorporated in future studies of atmospheric structure. We also evaluate the contribution of external sources to photochemical aerosol formation and find that their spectral signature is not consistent with observations.

Single-particle characterization of ice-nucleating particles and ice particles residuals sampled by three different techniques

Science.gov (United States)

Kandler, Konrad; Worringen, Annette; Benker, Nathalie; Dirsch, Thomas; Mertes, Stephan; Schenk, Ludwig; Kästner, Udo; Frank, Fabian; Nillius, Björn; Bundke, Ulrich; Rose, Diana; Curtius, Joachim; Kupiszewski, Piotr; Weingartner, Ernest; Vochezer, Paul; Schneider, Johannes; Schmidt, Susan; Weinbruch, Stephan; Ebert, Martin

2015-04-01

During January/February 2013, at the High Alpine Research Station Jungfraujoch a measurement campaign was carried out, which was centered on atmospheric ice-nucleating particles (INP) and ice particle residuals (IPR). Three different techniques for separation of INP and IPR from the non-ice-active particles are compared. The Ice Selective Inlet (ISI) and the Ice Counterflow Virtual Impactor (Ice-CVI) sample ice particles from mixed phase clouds and allow for the analysis of the residuals. The combination of the Fast Ice Nucleus Chamber (FINCH) and the Ice Nuclei Pumped Counterflow Virtual Impactor (IN-PCVI) provides ice-activating conditions to aerosol particles and extracts the activated INP for analysis. Collected particles were analyzed by scanning electron microscopy and energy-dispersive X-ray microanalysis to determine size, chemical composition and mixing state. All INP/IPR-separating techniques had considerable abundances (median 20 - 70 %) of instrumental contamination artifacts (ISI: Si-O spheres, probably calibration aerosol; Ice-CVI: Al-O particles; FINCH+IN-PCVI: steel particles). Also, potential sampling artifacts (e.g., pure soluble material) occurred with a median abundance of separated by all three techniques. Soot was a minor contributor. Lead was detected in less than 10 % of the particles, of which the majority were internal mixtures with other particle types. Sea-salt and sulfates were identified by all three methods as INP/IPR. Most samples showed a maximum of the INP/IPR size distribution at 400 nm geometric diameter. In a few cases, a second super-micron maximum was identified. Soot/carbonaceous material and metal oxides were present mainly in the submicron range. ISI and FINCH yielded silicates and Ca-rich particles mainly with diameters above 1 µm, while the Ice-CVI also separated many submicron IPR. As strictly parallel sampling could not be performed, a part of the discrepancies between the different techniques may result from

Incipient Soot Formation in Rich Partially Premixed Flames under High Pressure Conditions of Relevance to Compression-Ignition Engines

Science.gov (United States)

2017-09-09

a Laminar Premixed Flame, Aerosol Reaction Engineering , Center for Aerosol science and Engineering (CASE) Workshop 2016, Saint Louis, Missouri, May...Publication Type: Conference Paper or Presentation Conference Name: Aerosol Reaction Engineering , Center for Aerosol science and Engineering (CASE...measurements of critical soot precursors up to 3-ring aromatics is available online to modelers to improve the chemical reaction mechanism [24]. To give a

Microphysical processing of aerosol particles in orographic clouds

Directory of Open Access Journals (Sweden)

S. Pousse-Nottelmann

2015-08-01

aerosol cycling in clouds has been implemented into COSMO-Model, the regional weather forecast and climate model of the Consortium for Small-scale Modeling (COSMO. The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed us to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener–Bergeron–Findeisen (WBF process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snowflakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snowflakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. Thereby, the processes impact the total aerosol number and mass and additionally alter the shape of the aerosol size distributions by enhancing the internally mixed/soluble Aitken and accumulation mode and generating coarse-mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases the cloud droplet number concentration with possible implications for the ice crystal number

Hygroscopic growth of atmospheric aerosol particles and its relation to nucleation scavenging in clouds

Energy Technology Data Exchange (ETDEWEB)

Svenningsson, B.

1997-11-01

Aerosol particles in the atmosphere are important in several aspects. Some major aerosol constituents that are deposited in ecosystems are acidic or fertilizers and some minor or trace constituents are toxic. Aerosol particles are also involved in the earth`s radiation balance, both directly by scattering the sunlight and indirectly by influencing the clouds. All these effects are influenced by the interaction between the aerosol particles and water vapour. A tandem differential mobility analyser (TDMA) has been designed to measure hygroscopic growth, i.e. the particle diameter change due to uptake of water at well defined relative humidities below 100%. Tests of the instrument performance have been made using aerosol particles of pure inorganic salts. Three field experiments have been performed as parts of large fog and cloud experiments. Bimodal hygroscopic growth spectra were found: less-hygroscopic particles containing a few percent and more-hygroscopic particles around 50% by volume of hygroscopically active material. In general the fraction of less-hygroscopic particles decreases with particle size and it is larger in polluted continental aerosols than in remote background aerosols. This external mixing cannot be fully understood using present views on the formation of aerosols. Evidence or the importance of the external mixing on the cloud nucleating properties of the particles are found in comparisons between hygroscopic growth spectra for the total aerosol, the interstitial aerosol in clouds, and cloud drop residuals. Cloud condensation nuclei spectra, calculated using aerosol particle size distributions and hygroscopic growth spectra, in combination with information on the major inorganic ions are presented. These CCN spectra reveal for instance that the influence of less-hygroscopic particles on the cloud droplets increases with increasing peak supersaturation. The fraction of the particles that were scavenged to cloud drops, as a function of particle

Effect of Coatings on the Uptake Rate and HONO Yield in Heterogeneous Reaction of Soot with NO2

Science.gov (United States)

Cruz-Quiñones, M.; Khalizov, A. F.; Zhang, R.

2009-12-01

Heterogeneous reaction of nitrogen dioxide on carbon soot aerosols has been suggested as a possible source of nighttime nitrous acid (HONO) in atmosphere boundary layer. Available laboratory data show significant variability in the measured reaction probabilities and HONO yields, making it difficult to asses the atmospheric significance of this process. Moreover, little is known of how aging of soot aerosol through internal mixing with other atmospheric trace constituents will affect the heterogeneous reactivity and HONO production. In this work, the heterogeneous reaction of NO2 on fresh and aged soot films leading to HONO formation was studied through a series of kinetic uptake experiments and HONO yield measurements. Soot samples were prepared by incomplete combustion of propane and kerosene fuels under lean and rich flame conditions. Experiments were performed in a low-pressure, fast-flow reactor coupled to a chemical ionization mass spectrometer (CIMS), using atmospheric-level NO2 concentrations. Heterogeneous uptake coefficients, γ(geom) and γ(BET), were calculated using geometric and internal BET soot surface areas, respectively. The uptake coefficient and the HONO yield depend on the type of fuel and combustion regime and are the highest for soot samples prepared using rich kerosene flame. Although, the internal surface area of soot measured by BET method is a factor of 50 to 500 larger than the geometric surface area, only the top soot layers are involved in heterogeneous reaction with NO2 as follows from the observed weak dependence of γ(geom) and decrease in γ(BET) with increasing sample mass. Heating the soot samples before exposure to NO2 increases the BET surface area, the HONO yield, and the NO2 uptake coefficient due to the removal of the organic fraction from the soot backbone that unblocks active sites and makes them accessible for physical adsorption and chemical reactions. Our results support the oxidation-reduction mechanism involving

Characterization and reactivity of soot from fast pyrolysis of lignocellulosic compounds and monolignols

DEFF Research Database (Denmark)

Trubetskaya, Anna; Brown, Avery; Tompsett, Geoffrey

2018-01-01

spectroscopy. The CO2 reactivity of soot was investigated by thermogravimetric analysis. Soot from cellulose was more reactive than soot produced from extractives, lignin and monolignols. Soot reactivity was correlated with the separation distances between adjacent graphene layers, as measured using...... transmission electron microscopy. Particle size, free radical concentration, differences in a degree of curvature and multi-core structures influenced the soot reactivity less than the interlayer separation distances. Soot yield was correlated with the lignin content of the feedstock. The selection...... of the extraction solvent had a strong influence on the soot reactivity. The Soxhlet extraction of softwood and wheat straw lignin soot using methanol decreased the soot reactivity, whereas acetone extraction had only a modest effect....

Conductometric Sensor for Soot Mass Flow Detection in Exhausts of Internal Combustion Engines.

Science.gov (United States)

Feulner, Markus; Hagen, Gunter; Müller, Andreas; Schott, Andreas; Zöllner, Christian; Brüggemann, Dieter; Moos, Ralf

2015-11-13

Soot sensors are required for on-board diagnostics (OBD) of automotive diesel particulate filters (DPF) to detect filter failures. Widely used for this purpose are conductometric sensors, measuring an electrical current or resistance between two electrodes. Soot particles deposit on the electrodes, which leads to an increase in current or decrease in resistance. If installed upstream of a DPF, the "engine-out" soot emissions can also be determined directly by soot sensors. Sensors were characterized in diesel engine real exhausts under varying operation conditions and with two different kinds of diesel fuel. The sensor signal was correlated to the actual soot mass and particle number, measured with an SMPS. Sensor data and soot analytics (SMPS) agreed very well, an impressing linear correlation in a double logarithmic representation was found. This behavior was even independent of the used engine settings or of the biodiesel content.

Conductometric Sensor for Soot Mass Flow Detection in Exhausts of Internal Combustion Engines

Science.gov (United States)

Feulner, Markus; Hagen, Gunter; Müller, Andreas; Schott, Andreas; Zöllner, Christian; Brüggemann, Dieter; Moos, Ralf

2015-01-01

Soot sensors are required for on-board diagnostics (OBD) of automotive diesel particulate filters (DPF) to detect filter failures. Widely used for this purpose are conductometric sensors, measuring an electrical current or resistance between two electrodes. Soot particles deposit on the electrodes, which leads to an increase in current or decrease in resistance. If installed upstream of a DPF, the “engine-out” soot emissions can also be determined directly by soot sensors. Sensors were characterized in diesel engine real exhausts under varying operation conditions and with two different kinds of diesel fuel. The sensor signal was correlated to the actual soot mass and particle number, measured with an SMPS. Sensor data and soot analytics (SMPS) agreed very well, an impressing linear correlation in a double logarithmic representation was found. This behavior was even independent of the used engine settings or of the biodiesel content. PMID:26580621

Conductometric Sensor for Soot Mass Flow Detection in Exhausts of Internal Combustion Engines

Directory of Open Access Journals (Sweden)

Markus Feulner

2015-11-01

Full Text Available Soot sensors are required for on-board diagnostics (OBD of automotive diesel particulate filters (DPF to detect filter failures. Widely used for this purpose are conductometric sensors, measuring an electrical current or resistance between two electrodes. Soot particles deposit on the electrodes, which leads to an increase in current or decrease in resistance. If installed upstream of a DPF, the “engine-out” soot emissions can also be determined directly by soot sensors. Sensors were characterized in diesel engine real exhausts under varying operation conditions and with two different kinds of diesel fuel. The sensor signal was correlated to the actual soot mass and particle number, measured with an SMPS. Sensor data and soot analytics (SMPS agreed very well, an impressing linear correlation in a double logarithmic representation was found. This behavior was even independent of the used engine settings or of the biodiesel content.

Investigations of the long-term effects of LII on soot and bath gas

KAUST Repository

Cenker, Emre

2017-08-24

A combination of high-repetition rate imaging, laser extinction measurements, two-colour 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 neighbouring 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-colour pyrometry imaging show that the increased temperature of soot both in the heated and neighbouring 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.

Synthesis of nanosized metal particles from an aerosol

Directory of Open Access Journals (Sweden)

Srećko R. Stopić

2013-10-01

Full Text Available The synthesis of metallic nanoparticles from the precursor solution of salts using the ultrasonic spray pyrolysis method was considered in this work. During the control of process parameters (surface tension and density, the concentration of solution, residence time of aerosol in the reactor, presence of additives, gas flow rate, decomposition temperature of aerosol, type of precursor and working atmosphere it is possible to guide the process in order to obtain powders with such a morphology which satisfies more complex requirements for the desired properties of advanced engineering materials.  Significant advance in the improvement of powder characteristics (lower particles sizes, better spheroidity, higher surface area was obtained by the application of the ultrasonic generator for the preparation of aerosols. Ultrasonic spray pyrolysis is performed by the action of a powerful source of ultrasound on the corresponding precursor solution forming the aerosol with a constant droplet size, which depends on the characteristics of liquid and the frequency of ultrasound. The produced aerosols were transported into the hot reactor, which enables the reaction to occur in a very small volume of a particle and formation of  nanosized powder. Spherical, nanosized particles of metals (Cu, Ag, Au, Co were produced with new and improved physical and chemical characteristics at the IME, RWTH Aachen University. The high costs associated with small quantities of produced nanosized particles represent a limitation of the USP-method. Therefore, scale up of the ultrasonic spray pyrolysis was performed as a final target in the synthesis of nanosized powder.

Measurements of Primary Biogenic Aerosol Particles with an Ultraviolet Aerodynamic Particle Sizer (UVAPS) During AMAZE-08

Science.gov (United States)

Wollny, A. G.; Garland, R.; Pöschl, U.

2008-12-01

Biogenic aerosols are ubiquitous in the Earth's atmosphere and they influence atmospheric chemistry and physics, the biosphere, climate, and public health. They play an important role in the spread of biological organisms and reproductive materials, and they can cause or enhance human, animal, and plant diseases. Moreover, they influence the Earth's energy budget by scattering and absorbing radiation, and they can initiate the formation of clouds and precipitation as cloud condensation and ice nuclei. The composition, abundance, and origin of biogenic aerosol particles and components are, however, still not well understood and poorly quantified. Prominent examples of primary biogenic aerosol particles, which are directly emitted from the biosphere to the atmosphere, are pollen, bacteria, fungal spores, viruses, and fragments of animals and plants. During the AMazonian Aerosol CharacteriZation Experiment (AMAZE-08) a large number of aerosol and gas-phase measurements were taken on a remote site close to Manaus, Brazil, during a period of five weeks in February and March 2008. The presented study is focused on data from an ultraviolet aerodynamic particle sizer (UVAPS, TSI inc.) that has been deployed for the first time in Amazonia. In this instrument, particle counting and aerodynamic sizing over the range of 0.5-20 μm are complemented by the measurement of UV fluorescence at 355 nm (excitation) and 420-575 nm (emission), respectively. Fluorescence at these wavelengths is characteristic for reduced pyridine nucleotides (e.g., NAD(P)H) and for riboflavin, which are specific for living cells. Thus particles exhibiting fluorescence signals can be regarded as 'viable aerosols' or 'fluorescent bioparticles' (FBAP), and their concentration can be considered as lower limit for the actual abundance of primary biogenic aerosol particles. First data analyses show a pronounced peak of FBAP at diameters around 2-3 μm. In this size range the biogenic particle fraction was

Sooting Characteristics and Modeling in Counterflow Diffusion Flames

KAUST Repository

Wang, Yu

2013-11-01

Soot formation is one of the most complex phenomena in combustion science and an understanding of the underlying physico-chemical mechanisms is important. This work adopted both experimental and numerical approaches to study soot formation in laminar counterfl ow diffusion flames. As polycyclic aromatic hydrocarbons (PAHs) are the precursors of soot particles, a detailed gas-phase chemical mechanism describing PAH growth upto coronene for fuels with 1 to 4 carbon atoms was validated against laminar premixed and counter- flow diffusion fl ames. Built upon this gas-phase mechanism, a soot model was then developed to describe soot inception and surface growth. This soot model was sub- sequently used to study fuel mixing effect on soot formation in counterfl ow diffusion flames. Simulation results showed that compared to the baseline case of the ethylene flame, the doping of 5% (by volume) propane or ethane in ethylene tends to increase the soot volume fraction and number density while keeping the average soot size almost unchanged. These results are in agreement with experimental observations. Laser light extinction/scattering as well as laser induced fluorescence techniques were used to study the effect of strain rate on soot and PAH formation in counterfl ow diffusion ames. The results showed that as strain rate increased both soot volume fraction and PAH concentrations decreased. The concentrations of larger PAH were more sensitive to strain rate compared to smaller ones. The effect of CO2 addition on soot formation was also studied using similar experimental techniques. Soot loading was reduced with CO2 dilution. Subsequent numerical modeling studies were able to reproduce the experimental trend. In addition, the chemical effect of CO2 addition was analyzed using numerical data. Critical conditions for the onset of soot were systematically studied in counterfl ow diffusion ames for various gaseous hydrocarbon fuels and at different strain rates. A sooting

Infrared remote sensing of atmospheric aerosols; Apports du sondage infrarouge a l'etude des aerosols atmospheriques

Energy Technology Data Exchange (ETDEWEB)

Pierangelo, C

2005-09-15

The 2001 report from the Intergovernmental Panel on Climate Change emphasized the very low level of understanding of atmospheric aerosol effects on climate. These particles originate either from natural sources (dust, volcanic aerosols...) or from anthropogenic sources (sulfates, soot...). They are one of the main sources of uncertainty on climate change, partly because they show a very high spatio-temporal variability. Observation from space, being global and quasi-continuous, is therefore a first importance tool for aerosol studies. Remote sensing in the visible domain has been widely used to obtain a better characterization of these particles and their effect on solar radiation. On the opposite, remote sensing of aerosols in the infrared domain still remains marginal. Yet, not only the knowledge of the effect of aerosols on terrestrial radiation is needed for the evaluation of their total radiative forcing, but also infrared remote sensing provides a way to retrieve other aerosol characteristics (observations are possible at night and day, over land and sea). In this PhD dissertation, we show that aerosol optical depth, altitude and size can be retrieved from infrared sounder observations. We first study the sensitivity of aerosol optical properties to their micro-physical properties, we then develop a radiative transfer code for scattering medium adapted to the very high spectral resolution of the new generation sounder NASA-Aqua/AIRS, and we finally focus on the inverse problem. The applications shown here deal with Pinatubo stratospheric volcanic aerosol, observed with NOAA/HIRS, and with the building of an 8 year climatology of dust over sea and land from this sounder. Finally, from AIRS observations, we retrieve the optical depth at 10 {mu}m, the average altitude and the coarse mode effective radius of mineral dust over sea. (author)

Soot Particle Size Distribution Functions in a Turbulent Non-Premixed Ethylene-Nitrogen Flame

KAUST Repository

Boyette, Wesley

2017-02-21

A scanning mobility particle sizer with a nano differential mobility analyzer was used to measure nanoparticle size distribution functions in a turbulent non-premixed flame. The burner utilizes a premixed pilot flame which anchors a C2H4/N2 (35/65) central jet with ReD = 20,000. Nanoparticles in the flame were sampled through a N2-filled tube with a 500- μm orifice. Previous studies have shown that insufficient dilution of the nanoparticles can lead to coagulation in the sampling line and skewed particle size distribution functions. A system of mass flow controllers and valves were used to vary the dilution ratio. Single-stage and two-stage dilution systems were investigated. A parametric study on the effect of the dilution ratio on the observed particle size distribution function indicates that particle coagulation in the sampling line can be eliminated using a two-stage dilution process. Carbonaceous nanoparticle (soot) concentration particle size distribution functions along the flame centerline at multiple heights in the flame are presented. The resulting distributions reveal a pattern of increasing mean particle diameters as the distance from the nozzle along the centerline increases.

Soot Particle Size Distribution Functions in a Turbulent Non-Premixed Ethylene-Nitrogen Flame

KAUST Repository

Boyette, Wesley; Chowdhury, Snehaunshu; Roberts, William L.

2017-01-01

A scanning mobility particle sizer with a nano differential mobility analyzer was used to measure nanoparticle size distribution functions in a turbulent non-premixed flame. The burner utilizes a premixed pilot flame which anchors a C2H4/N2 (35/65) central jet with ReD = 20,000. Nanoparticles in the flame were sampled through a N2-filled tube with a 500- μm orifice. Previous studies have shown that insufficient dilution of the nanoparticles can lead to coagulation in the sampling line and skewed particle size distribution functions. A system of mass flow controllers and valves were used to vary the dilution ratio. Single-stage and two-stage dilution systems were investigated. A parametric study on the effect of the dilution ratio on the observed particle size distribution function indicates that particle coagulation in the sampling line can be eliminated using a two-stage dilution process. Carbonaceous nanoparticle (soot) concentration particle size distribution functions along the flame centerline at multiple heights in the flame are presented. The resulting distributions reveal a pattern of increasing mean particle diameters as the distance from the nozzle along the centerline increases.

Hygroscopicity and chemical composition of Antarctic sub-micrometre aerosol particles and observations of new particle formation

Directory of Open Access Journals (Sweden)

E. Asmi

2010-05-01

Full Text Available The Antarctic near-coastal sub-micrometre aerosol particle features in summer were characterised based on measured data on aerosol hygroscopicity, size distributions, volatility and chemical ion and organic carbon mass concentrations. Hysplit model was used to calculate the history of the air masses to predict the particle origin. Additional measurements of meteorological parameters were utilised. The hygroscopic properties of particles mostly resembled those of marine aerosols. The measurements took place at 130 km from the Southern Ocean, which was the most significant factor affecting the particle properties. This is explained by the lack of additional sources on the continent of Antarctica. The Southern Ocean was thus a likely source of the particles and nucleating and condensing vapours. The particles were very hygroscopic (HGF 1.75 at 90 nm and very volatile. Most of the sub-100 nm particle volume volatilised below 100 °C. Based on chemical data, particle hygroscopic and volatile properties were explained by a large fraction of non-neutralised sulphuric acid together with organic material. The hygroscopic growth factors assessed from chemical data were similar to measured. Hygroscopicity was higher in dry continental air masses compared with the moist marine air masses. This was explained by the aging of the marine organic species and lower methanesulphonic acid volume fraction together with the changes in the inorganic aerosol chemistry as the aerosol had travelled long time over the continental Antarctica. Special focus was directed in detailed examination of the observed new particle formation events. Indications of the preference of negative over positive ions in nucleation could be detected. However, in a detailed case study, the neutral particles dominated the particle formation process. Freshly nucleated particles had the smallest hygroscopic growth factors, which increased subsequent to particle aging.

New Nanotech from an Ancient Material: Chemistry Demonstrations Involving Carbon-Based Soot

Science.gov (United States)

Campbell, Dean J.; Andrews, Mark J.; Stevenson, Keith J.

2012-01-01

Carbon soot has been known since antiquity, but has recently been finding new uses as a robust, inexpensive nanomaterial. This paper describes the superhydrophobic properties of carbon soot films prepared by combustion of candle wax or propane gas and introduces some of the optical absorption and fluorescence properties of carbon soot particles.…

Measurement of Soot Deposition in Automotive Components Using Neutron Radiography

Energy Technology Data Exchange (ETDEWEB)

Zekveld, David; Liu, Liaohui [AMEC NSS, 700 University Ave, Toronto, Ontario, M5G 1X6 (Canada); UOIT, 2000 Simcoe Street North, Oshawa, Ontario, L1H 7K4 (Canada); Harrison, Andrew; Gill, Spencer; Harvel, Glenn [UOIT, 2000 Simcoe Street North, Oshawa, Ontario, L1H 7K4 (Canada); Chang, Jen-Shih [McMaster University, 1280 Main Street West, Hamilton, Ontario, L8S 4L8 (Canada)

2008-07-01

About 40% of air pollution is generated by vehicles and transportation. The particulate matter (PM) emission significantly impacts human health. Fine particles below 2.5 {mu}m (PM2.5) can enter the lungs and lead to respiratory problems. These particles not only influence human health, but also reduce the capability of many automobile exhaust heat exchanging devices. Neutron radiography is a non-destructive method of analyzing carbonaceous PM. While neutron radiography has been demonstrated for soot measurement in the past, the application has not considered the presence of unburned hydrocarbons, significant amounts of moisture nor examined complex geometrical configurations. The purpose of this work is to study a reliable non-destructive testing methodology using neutron radiography for measurement of soot distribution in automotive components. A soot standard (aluminium target) was designed and manufactured as a calibration tool. The standard is radiographed and used to measure the differences between various soot thickness and compositions. The radiograph images are analyzed to determine a calibration curve based upon the composition of the materials which can then be used for analysis of the automotive components. Experiments are performed using a diesel engine to produce soot deposits on exhaust piping. Soot distribution on exhaust piping is measured using neutron radiography. (authors)

Measurement of Soot Deposition in Automotive Components Using Neutron Radiography

International Nuclear Information System (INIS)

Zekveld, David; Liu, Liaohui; Harrison, Andrew; Gill, Spencer; Harvel, Glenn; Chang, Jen-Shih

2008-01-01

About 40% of air pollution is generated by vehicles and transportation. The particulate matter (PM) emission significantly impacts human health. Fine particles below 2.5 μm (PM2.5) can enter the lungs and lead to respiratory problems. These particles not only influence human health, but also reduce the capability of many automobile exhaust heat exchanging devices. Neutron radiography is a non-destructive method of analyzing carbonaceous PM. While neutron radiography has been demonstrated for soot measurement in the past, the application has not considered the presence of unburned hydrocarbons, significant amounts of moisture nor examined complex geometrical configurations. The purpose of this work is to study a reliable non-destructive testing methodology using neutron radiography for measurement of soot distribution in automotive components. A soot standard (aluminium target) was designed and manufactured as a calibration tool. The standard is radiographed and used to measure the differences between various soot thickness and compositions. The radiograph images are analyzed to determine a calibration curve based upon the composition of the materials which can then be used for analysis of the automotive components. Experiments are performed using a diesel engine to produce soot deposits on exhaust piping. Soot distribution on exhaust piping is measured using neutron radiography. (authors)

Aerosolization, Chemical Characterization, Hygroscopicity and Ice Formation of Marine Biogenic Particles

Science.gov (United States)

Alpert, P. A.; Radway, J.; Kilthau, W.; Bothe, D.; Knopf, D. A.; Aller, J. Y.

2013-12-01

The oceans cover the majority of the earth's surface, host nearly half the total global primary productivity and are a major source of atmospheric aerosol particles. However, effects of biological activity on sea spray generation and composition, and subsequent cloud formation are not well understood. Our goal is to elucidate these effects which will be particularly important over nutrient rich seas, where microorganisms can reach concentrations of 10^9 per mL and along with transparent exopolymer particles (TEP) can become aerosolized. Here we report the results of mesocosm experiments in which bubbles were generated by two methods, either recirculating impinging water jets or glass frits, in natural or artificial seawater containing bacteria and unialgal cultures of three representative phytoplankton species, Thalassiosira pseudonana, Emiliania huxleyi, and Nannochloris atomus. Over time we followed the size distribution of aerosolized particles as well as their hygroscopicity, heterogeneous ice nucleation potential, and individual physical-chemical characteristics. Numbers of cells and the mass of dissolved and particulate organic carbon (DOC, POC), TEP (which includes polysaccharide-containing microgels and nanogels >0.4 μm in diameter) were determined in the bulk water, the surface microlayer, and aerosolized material. Aerosolized particles were also impacted onto substrates for ice nucleation and water uptake experiments, elemental analysis using computer controlled scanning electron microscopy and energy dispersive analysis of X-rays (CCSEM/EDX), and determination of carbon bonding with scanning transmission X-ray microscopy and near-edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). Regardless of bubble generation method, the overall concentration of aerosol particles, TEP, POC and DOC increased as concentrations of bacterial and phytoplankton cells increased, stabilized, and subsequently declined. Particles cloud formation and potential

Time Resolved Measurements of Primary Biogenic Aerosol Particles in Amazonia

Science.gov (United States)

Wollny, A. G.; Garland, R.; Pöschl, U.

2009-04-01

Biogenic aerosols are ubiquitous in the Earth's atmosphere and they influence atmospheric chemistry and physics, the biosphere, climate, and public health. They play an important role in the spread of biological organisms and reproductive materials, and they can cause or enhance human, animal, and plant diseases. Moreover, they influence the Earth's energy budget by scattering and absorbing radiation, and they can initiate the formation of clouds and precipitation as cloud condensation and ice nuclei. The composition, abundance, and origin of biogenic aerosol particles and components are, however, still not well understood and poorly quantified. Prominent examples of primary biogenic aerosol particles, which are directly emitted from the biosphere to the atmosphere, are pollen, bacteria, fungal spores, viruses, and fragments of animals and plants. During the Amazonian Aerosol Characterization Experiment (AMAZE-08) a large number of aerosol and gas-phase measurements were taken on a remote site close to Manaus, Brazil, during a period of five weeks in February and March 2008. This presented study is focused on data from an ultraviolet aerodynamic particle sizer (UVAPS, TSI inc.) that has been deployed for the first time in Amazonia. In this instrument, particle counting and aerodynamic sizing over the range of 0.5-20 µm are complemented by the measurement of UV fluorescence at 355 nm (excitation) and 420-575 nm (emission), respectively. Fluorescence at these wavelengths is characteristic for reduced pyridine nucleotides (e.g., NAD(P)H) and for riboflavin, which are specific for living cells. Thus particles exhibiting fluorescence signals can be regarded as "viable aerosols" or "fluorescent bioparticles" (FBAP), and their concentration can be considered as lower limit for the actual abundance of primary biogenic aerosol particles. Data from the UVAPS were averaged over 5 minute time intervals. The presence of bioparticles in the observed size range has been

Reactions and mass spectra of complex particles using Aerosol CIMS

Science.gov (United States)

Hearn, John D.; Smith, Geoffrey D.

2006-12-01

Aerosol chemical ionization mass spectrometry (CIMS) is used both on- and off-line for the analysis of complex laboratory-generated and ambient particles. One of the primary advantages of Aerosol CIMS is the low degree of ion fragmentation, making this technique well suited for investigating the reactivity of complex particles. To demonstrate the usefulness of this "soft" ionization, particles generated from meat cooking were reacted with ozone and the composition was monitored as a function of reaction time. Two distinct kinetic regimes were observed with most of the oleic acid in these particles reacting quickly but with 30% appearing to be trapped in the complex mixture. Additionally, detection limits are measured to be sufficiently low (100-200 ng/m3) to detect some of the more abundant constituents in ambient particles, including sulfate, which is measured in real-time at 1.2 [mu]g/m3. To better characterize complex aerosols from a variety of sources, a novel off-line collection method was also developed in which non-volatile and semi-volatile organics are desorbed from particles and concentrated in a cold U-tube. Desorption from the U-tube followed by analysis with Aerosol CIMS revealed significant amounts of nicotine in cigarette smoke and levoglucosan in oak and pine smoke, suggesting that this may be a useful technique for monitoring particle tracer species. Additionally, secondary organic aerosol formed from the reaction of ozone with R-limonene and volatile organics from orange peel were analyzed off-line showing large molecular weight products (m/z > 300 amu) that may indicate the formation of oligomers. Finally, mass spectra of ambient aerosol collected offline reveal a complex mixture of what appears to be highly processed organics, some of which may contain nitrogen.

Characterisation of nano- and micron-sized airborne and collected subway particles, a multi-analytical approach.

Science.gov (United States)

Midander, Klara; Elihn, Karine; Wallén, Anna; Belova, Lyuba; Karlsson, Anna-Karin Borg; Wallinder, Inger Odnevall

2012-06-15

Continuous daily measurements of airborne particles were conducted during specific periods at an underground platform within the subway system of the city center of Stockholm, Sweden. Main emphasis was placed on number concentration, particle size distribution, soot content (analyzed as elemental and black carbon) and surface area concentration. Conventional measurements of mass concentrations were conducted in parallel as well as analysis of particle morphology, bulk- and surface composition. In addition, the presence of volatile and semi volatile organic compounds within freshly collected particle fractions of PM(10) and PM(2.5) were investigated and grouped according to functional groups. Similar periodic measurements were conducted at street level for comparison. The investigation clearly demonstrates a large dominance in number concentration of airborne nano-sized particles compared to coarse particles in the subway. Out of a mean particle number concentration of 12000 particles/cm(3) (7500 to 20000 particles/cm(3)), only 190 particles/cm(3) were larger than 250 nm. Soot particles from diesel exhaust, and metal-containing particles, primarily iron, were observed in the subway aerosol. Unique measurements on freshly collected subway particle size fractions of PM(10) and PM(2.5) identified several volatile and semi-volatile organic compounds, the presence of carcinogenic aromatic compounds and traces of flame retardants. This interdisciplinary and multi-analytical investigation aims to provide an improved understanding of reported adverse health effects induced by subway aerosols. Copyright © 2012 Elsevier B.V. All rights reserved.

New apparatus of single particle trap system for aerosol visualization

Science.gov (United States)

Higashi, Hidenori; Fujioka, Tomomi; Endo, Tetsuo; Kitayama, Chiho; Seto, Takafumi; Otani, Yoshio

2014-08-01

Control of transport and deposition of charged aerosol particles is important in various manufacturing processes. Aerosol visualization is an effective method to directly observe light scattering signal from laser-irradiated single aerosol particle trapped in a visualization cell. New single particle trap system triggered by light scattering pulse signal was developed in this study. The performance of the device was evaluated experimentally. Experimental setup consisted of an aerosol generator, a differential mobility analyzer (DMA), an optical particle counter (OPC) and the single particle trap system. Polystylene latex standard (PSL) particles (0.5, 1.0 and 2.0 μm) were generated and classified according to the charge by the DMA. Singly charged 0.5 and 1.0 μm particles and doubly charged 2.0 μm particles were used as test particles. The single particle trap system was composed of a light scattering signal detector and a visualization cell. When the particle passed through the detector, trigger signal with a given delay time sent to the solenoid valves upstream and downstream of the visualization cell for trapping the particle in the visualization cell. The motion of particle in the visualization cell was monitored by CCD camera and the gravitational settling velocity and the electrostatic migration velocity were measured from the video image. The aerodynamic diameter obtained from the settling velocity was in good agreement with Stokes diameter calculated from the electrostatic migration velocity for individual particles. It was also found that the aerodynamic diameter obtained from the settling velocity was a one-to-one function of the scattered light intensity of individual particles. The applicability of this system will be discussed.

Soot Formation In Turbulent Combusting Flows

National Research Council Canada - National Science Library

Santoro, Robert

1998-01-01

.... Laser-based techniques were used to measure the soot volume fraction, particle size and number density as well as the temperature and relative concentration of hydroxyl radicals and polycyclic aromatic hydrocarbons...

Aerosol numerical modelling at local scale

International Nuclear Information System (INIS)

Albriet, Bastien

2007-01-01

At local scale and in urban areas, an important part of particulate pollution is due to traffic. It contributes largely to the high number concentrations observed. Two aerosol sources are mainly linked to traffic. Primary emission of soot particles and secondary nanoparticle formation by nucleation. The emissions and mechanisms leading to the formation of such bimodal distribution are still badly understood nowadays. In this thesis, we try to provide an answer to this problematic by numerical modelling. The Modal Aerosol Model MAM is used, coupled with two 3D-codes: a CFD (Mercure Saturne) and a CTM (Polair3D). A sensitivity analysis is performed, at the border of a road but also in the first meters of an exhaust plume, to identify the role of each process involved and the sensitivity of different parameters used in the modelling. (author) [fr

Infrared remote sensing of atmospheric aerosols; Apports du sondage infrarouge a l'etude des aerosols atmospheriques

Energy Technology Data Exchange (ETDEWEB)

Pierangelo, C.

2005-09-15

The 2001 report from the Intergovernmental Panel on Climate Change emphasized the very low level of understanding of atmospheric aerosol effects on climate. These particles originate either from natural sources (dust, volcanic aerosols...) or from anthropogenic sources (sulfates, soot...). They are one of the main sources of uncertainty on climate change, partly because they show a very high spatio-temporal variability. Observation from space, being global and quasi-continuous, is therefore a first importance tool for aerosol studies. Remote sensing in the visible domain has been widely used to obtain a better characterization of these particles and their effect on solar radiation. On the opposite, remote sensing of aerosols in the infrared domain still remains marginal. Yet, not only the knowledge of the effect of aerosols on terrestrial radiation is needed for the evaluation of their total radiative forcing, but also infrared remote sensing provides a way to retrieve other aerosol characteristics (observations are possible at night and day, over land and sea). In this PhD dissertation, we show that aerosol optical depth, altitude and size can be retrieved from infrared sounder observations. We first study the sensitivity of aerosol optical properties to their micro-physical properties, we then develop a radiative transfer code for scattering medium adapted to the very high spectral resolution of the new generation sounder NASA-Aqua/AIRS, and we finally focus on the inverse problem. The applications shown here deal with Pinatubo stratospheric volcanic aerosol, observed with NOAA/HIRS, and with the building of an 8 year climatology of dust over sea and land from this sounder. Finally, from AIRS observations, we retrieve the optical depth at 10 {mu}m, the average altitude and the coarse mode effective radius of mineral dust over sea. (author)

Electrometric aviation soot monitor, Phase I

Data.gov (United States)

National Aeronautics and Space Administration — We propose to develop a highly sensitive and portable device to monitor soot particle mass distribution from aircraft engine exhaust. The proposed method is based on...

Aerosol characteristics and particle production in the upper troposphere over the Amazon Basin

Science.gov (United States)

Andreae, Meinrat O.; Afchine, Armin; Albrecht, Rachel; Amorim Holanda, Bruna; Artaxo, Paulo; Barbosa, Henrique M. J.; Borrmann, Stephan; Cecchini, Micael A.; Costa, Anja; Dollner, Maximilian; Fütterer, Daniel; Järvinen, Emma; Jurkat, Tina; Klimach, Thomas; Konemann, Tobias; Knote, Christoph; Krämer, Martina; Krisna, Trismono; Machado, Luiz A. T.; Mertes, Stephan; Minikin, Andreas; Pöhlker, Christopher; Pöhlker, Mira L.; Pöschl, Ulrich; Rosenfeld, Daniel; Sauer, Daniel; Schlager, Hans; Schnaiter, Martin; Schneider, Johannes; Schulz, Christiane; Spanu, Antonio; Sperling, Vinicius B.; Voigt, Christiane; Walser, Adrian; Wang, Jian; Weinzierl, Bernadett; Wendisch, Manfred; Ziereis, Helmut

2018-01-01

Airborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15 km altitude, with number densities (normalized to standard temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German-Brazilian cooperative aircraft campaign ACRIDICON-CHUVA, where ACRIDICON stands for Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems and CHUVA is the acronym for Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (global precipitation measurement), on the German High Altitude and Long Range Research Aircraft (HALO). The campaign took place in September-October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with atmospheric trace gases, aerosol particles, and atmospheric radiation. Aerosol enhancements were observed consistently on all flights during which the UT was probed, using several aerosol metrics, including condensation nuclei (CN) and cloud condensation nuclei (CCN) number concentrations and chemical species mass concentrations. The UT particles differed sharply in their chemical composition and size distribution from those in the PBL, ruling out convective transport of combustion-derived particles from the boundary layer (BL) as a source. The air in the immediate outflow of deep convective clouds was depleted of aerosol particles, whereas strongly enhanced number concentrations of small particles ( 90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest a conceptual model, where production of new aerosol particles takes place in the continental UT from biogenic volatile organic material brought up by deep convection and converted to condensable

Inverse problem for particle size distributions of atmospheric aerosols using stochastic particle swarm optimization

International Nuclear Information System (INIS)

Yuan Yuan; Yi Hongliang; Shuai Yong; Wang Fuqiang; Tan Heping

2010-01-01

As a part of resolving optical properties in atmosphere radiative transfer calculations, this paper focuses on obtaining aerosol optical thicknesses (AOTs) in the visible and near infrared wave band through indirect method by gleaning the values of aerosol particle size distribution parameters. Although various inverse techniques have been applied to obtain values for these parameters, we choose a stochastic particle swarm optimization (SPSO) algorithm to perform an inverse calculation. Computational performances of different inverse methods are investigated and the influence of swarm size on the inverse problem of computation particles is examined. Next, computational efficiencies of various particle size distributions and the influences of the measured errors on computational accuracy are compared. Finally, we recover particle size distributions for atmospheric aerosols over Beijing using the measured AOT data (at wavelengths λ=0.400, 0.690, 0.870, and 1.020 μm) obtained from AERONET at different times and then calculate other AOT values for this band based on the inverse results. With calculations agreeing with measured data, the SPSO algorithm shows good practicability.

Soot and liquid-phase fuel distributions in a newly designed optically accessible DI diesel engine

Science.gov (United States)

Dec, J. E.; Espey, C.

1993-10-01

Two-dimensional (2-D) laser-sheet imaging has been used to examine the soot and liquid-phase fuel distributions in a newly designed, optically accessible, direct-injection diesel engine of the heavy-duty size class. The design of this engine preserves the intake port geometry and basic dimensions of a Cummins N-series production engine. It also includes several unique features to provide considerable optical access. Liquid-phase fuel and soot distribution studies were conducted at a medium speed (1,200 rpm) using a Cummins closed-nozzle fuel injector. The scattering was used to obtain planar images of the liquid-phase fuel distribution. These images show that the leading edge of the liquid-phase portion of the fuel jet reaches a maximum length of 24 mm, which is about half the combustion bowl radius for this engine. Beyond this point virtually all the fuel has vaporized. Soot distribution measurements were made at a high load condition using three imaging diagnostics: natural flame luminosity, 2-D laser-induced incandescence, and 2-D elastic scattering. This investigation showed that the soot distribution in the combusting fuel jet develops through three stages. First, just after the onset of luminous combustion, soot particles are small and nearly uniformly distributed throughout the luminous region of the fuel jet. Second, after about 2 crank angle degrees a pattern develops of a higher soot concentration of larger sized particles in the head vortex region of the jet and a lower soot concentration of smaller sized particles upstream toward the injector. Third, after fuel injection ends, both the soot concentration and soot particle size increase rapidly in the upstream portion of the fuel jet.

Chemical and Physical Properties of Individual Aerosol Particles Characterized in Sacramento, CA during CARES Field Campaign

Science.gov (United States)

Zelenyuk, A.; Beranek, J.; Vaden, T.; Imre, D. G.; Zaveri, R. A.

2011-12-01

We present results of measurements conducted by our Single Particle Mass Spectrometer, SPLAT II, in Sacramento, CA over the month of June 2010. SPLAT II measured the size of 195 million particles, and compositions of 10 million particles. In addition to size and composition, SPLAT II simultaneously measured size, density and composition of 121,000 individual particles. These measurements were conducted 2 - 3 times per day, depending on conditions. The data show that throughout the day particles were relatively small (<200 nm), and the vast majority were composed of oxygenated organics mixed with various amounts of sulfate. In addition, we characterized fresh and processed soot, biomass burning aerosol, organic amines, fresh and processed sea salt, and few dust particles. The data show a reproducible diurnal pattern in aerosol size distributions, number concentrations, and compositions. Early in the day, number concentrations were low, particles were very small, and the size distributions peaked at ~70 nm. At this time of the day, 80 nm particles had a density of 1.3 g cm-3; while the density of 200 nm particles was 1.6 g cm-3, consistent with our mass spectra showing that smaller particles were composed of organics mixed with ~10% sulfates, while larger particles were composed mostly of sulfate mixed with a small amount of organics. Later in the day, secondary organic aerosols (SOA) formation led to a number of nucleation events that significantly increased the number concentrations of very small particles. By mid-afternoon, as more SOA formed and condensed, particles increased in size the number concentrations of particles larger than 70 nm increased and the densities of particles 80 to 200 nm particles was ~1.3 g cm-3. The vast majority of these particles were composed of oxygenated organics mixed with a ~10% sulfate. In other words they were SOA particles mixed with a small amount of sulfate. The mass spectra of these particles shows that there were two types of

Characterization of aerosol particles at the forested site in Lithuania

Science.gov (United States)

Rimselyte, I.; Garbaras, A.; Kvietkus, K.; Remeikis, V.

2009-04-01

Atmospheric particulate matter (PM), especially fine particles (particles with aerodynamic diameter less than 1 m, PM1), has been found to play an important role in global climate change, air quality, and human health. The continuous study of aerosol parameters is therefore imperative for better understanding the environmental effects of the atmospheric particles, as well as their sources, formation and transformation processes. The particle size distribution is particularly important, since this physical parameter determines the mass and number density, lifetime and atmospheric transport, or optical scattering behavior of the particles in the atmosphere (Jaenicke, 1998). Over the years several efforts have been made to improve the knowledge about the chemical composition of atmospheric particles as a function of size (Samara and Voutsa, 2005) and to characterize the relative contribution of different components to the fine particulate matter. It is well established that organic materials constitute a highly variable fraction of the atmospheric aerosol. This fraction is predominantly found in the fine size mode in concentrations ranging from 10 to 70% of the total dry fine particle mass (Middlebrook et al., 1998). Although organic compounds are major components of the fine particles, the composition, formation mechanism of organic aerosols are not well understood. This is because particulate organic matter is part of a complex atmospheric system with hundreds of different compounds, both natural and anthropogenic, covering a wide range of chemical properties. The aim of this study was to characterize the forest PM1, and investigate effects of air mass transport on the aerosol size distribution and chemical composition, estimate and provide insights into the sources and characteristics of carbonaceous aerosols through analysis ^13C/12C isotopic ratio as a function of the aerosol particles size. The measurements were performed at the Rugšteliškis integrated

Crystallization of aqueous ammonium sulfate particles internally mixed with soot and kaolinite: crystallization relative humidities and nucleation rates.

Science.gov (United States)

Pant, Atul; Parsons, Matthew T; Bertram, Allan K

2006-07-20

Using optical microscopy, we investigated the crystallization of aqueous ammonium sulfate droplets containing soot and kaolinite, as well as the crystallization of aqueous ammonium sulfate droplets free of solid material. Our results show that soot did not influence the crystallization RH of aqueous ammonium sulfate particles under our experimental conditions. In contrast, kaolinite increased the crystallization RH of the aqueous ammonium sulfate droplets by approximately 10%. In addition, our results show that the crystallization RH of aqueous ammonium sulfate droplets free of solid material does not depend strongly on particle size. This is consistent with conclusions made previously in the literature, based on comparisons of results from different laboratories. From the crystallization results we determined the homogeneous nucleation rates of crystalline ammonium sulfate in aqueous ammonium sulfate droplets and the heterogeneous nucleation rates of crystalline ammonium sulfate in aqueous ammonium sulfate particles containing kaolinite. Using classical nucleation theory and our experimental data, we determined that the interfacial tension between an ammonium sulfate critical nucleus and an aqueous ammonium sulfate solution is 0.064 +/- 0.003 J m(-2) (in agreement with our previous measurements), and the contact angle between an ammonium sulfate critical nucleus and a kaolinite surface is 59 +/- 2 degrees. On the basis of our results, we argue that soot will not influence the crystallization RH of aqueous ammonium sulfate droplets in the atmosphere, but kaolinite can significantly modify the crystallization RH of atmospheric ammonium sulfate droplets. As an example, the CRH50 (the relative humidity at which 50% of the droplets crystallize) ranges from about 41 to 51% RH when the diameter of the kaolinite inclusion ranges from 0.1 to 5 microm. For comparison, the CRH50 of aqueous ammonium sulfate droplets (0.5 microm diameter) free of solid material is

Particle-Resolved Modeling of Aerosol Mixing State in an Evolving Ship Plume

Science.gov (United States)

Riemer, N. S.; Tian, J.; Pfaffenberger, L.; Schlager, H.; Petzold, A.

2011-12-01

The aerosol mixing state is important since it impacts the particles' optical and CCN properties and thereby their climate impact. It evolves continuously during the particles' residence time in the atmosphere as a result of coagulation with other particles and condensation of secondary aerosol species. This evolution is challenging to represent in traditional aerosol models since they require the representation of a multi-dimensional particle distribution. While modal or sectional aerosol representations cannot practically resolve the aerosol mixing state for more than a few species, particle-resolved models store the composition of many individual aerosol particles directly. They thus sample the high-dimensional composition state space very efficiently and so can deal with tens of species, fully resolving the mixing state. Here we use the capabilities of the particle-resolved model PartMC-MOSAIC to simulate the evolution of particulate matter emitted from marine diesel engines and compare the results to aircraft measurements made in the English Channel in 2007 as part of the European campaign QUANTIFY. The model was initialized with values of gas concentrations and particle size distributions and compositions representing fresh ship emissions. These values were obtained from a test rig study in the European project HERCULES in 2006 using a serial four-stroke marine diesel engine operating on high-sulfur heavy fuel oil. The freshly emitted particles consisted of sulfate, black carbon, organic carbon and ash. We then tracked the particle population for several hours as it evolved undergoing coagulation, dilution with the background air, and chemical transformations in the aerosol and gas phase. This simulation was used to compute the evolution of CCN properties and optical properties of the plume on a per-particle basis. We compared our results to size-resolved data of aged ship plumes from the QUANTIFY Study in 2007 and showed that the model was able to reproduce

Relative importance of nitrate and sulfate aerosol production mechanisms in urban atmospheres

International Nuclear Information System (INIS)

Middleton, P.; Kiang, C.S.

1979-01-01

The relative importance of the various sulfate and nitrate aerosol production mechanisms is calculated for different atmospheric conditions. The calculation scheme used to determine the rates of nitrate and sulfate production, based on the concept that vapor transfer to the aerosols and nitrate and sulfate formation within the aerosols are coupled kinetic processes, considers sulfate formation by ozone and hydrogen peroxide oxidation and catalytic oxidation in the presence of soot, iron and manganese of sulfite solutions and sulfuric acid condensation and nitrate formation by the liquid-phase oxidation of dissolved nitrogen oxides for different initial gas concentrations and particle compositions and sizes. It is found that sulfate production is higher under daytime conditions, primarily proceeding by mechanisms involving sulfuric acid and hydrogen peroxide, while at night oxidation processes on the surface of the aerosol film are more important. Nitrate tends to decrease nighttime sulfate production due to an increase in aerosol acidity and nitrate production is found to be higher under nighttime conditions and in the winter

Ice Nucleation Activity of Various Agricultural Soil Dust Aerosol Particles

Science.gov (United States)

Schiebel, Thea; Höhler, Kristina; Funk, Roger; Hill, Thomas C. J.; Levin, Ezra J. T.; Nadolny, Jens; Steinke, Isabelle; Suski, Kaitlyn J.; Ullrich, Romy; Wagner, Robert; Weber, Ines; DeMott, Paul J.; Möhler, Ottmar

2016-04-01

Recent investigations at the cloud simulation chamber AIDA (Aerosol Interactions and Dynamics in the Atmosphere) suggest that agricultural soil dust has an ice nucleation ability that is enhanced up to a factor of 10 compared to desert dust, especially at temperatures above -26 °C (Steinke et al., in preparation for submission). This enhancement might be caused by the contribution of very ice-active biological particles. In addition, soil dust aerosol particles often contain a considerably higher amount of organic matter compared to desert dust particles. To test agricultural soil dust as a source of ice nucleating particles, especially for ice formation in warm clouds, we conducted a series of laboratory measurements with different soil dust samples to extend the existing AIDA dataset. The AIDA has a volume of 84 m3 and operates under atmospherically relevant conditions over wide ranges of temperature, pressure and humidity. By controlled adiabatic expansions, the ascent of an air parcel in the troposphere can be simulated. As a supplement to the AIDA facility, we use the INKA (Ice Nucleation Instrument of the KArlsruhe Institute of Technology) continuous flow diffusion chamber based on the design by Rogers (1988) to expose the sampled aerosol particles to a continuously increasing saturation ratio by keeping the aerosol temperature constant. For our experiments, soil dust was dry dispersed into the AIDA vessel. First, fast saturation ratio scans at different temperatures were performed with INKA, sampling soil dust aerosol particles directly from the AIDA vessel. Then, we conducted the AIDA expansion experiment starting at a preset temperature. The combination of these two different methods provides a robust data set on the temperature-dependent ice activity of various agriculture soil dust aerosol particles with a special focus on relatively high temperatures. In addition, to extend the data set, we investigated the role of biological and organic matter in more

Molecular dynamics simulations of laser disintegration of amorphous aerosol particles with spatially nonuniform absorption

International Nuclear Information System (INIS)

Schoolcraft, Tracy A.; Constable, Gregory S.; Jackson, Bryan; Zhigilei, Leonid V.; Garrison, Barbara J.

2001-01-01

A series of molecular dynamics (MD) simulations are performed in order to provide qualitative information on the mechanisms of disintegration of aerosol particles as used in aerosol mass spectrometry. Three generic types of aerosol particles are considered: strongly absorbing particles with homogeneous composition, transparent particles with absorbing inclusion, and absorbing particles with transparent inclusion. To study the effect of the mechanical properties of the aerosol material on the disintegration process, the results for crystalline (brittle) and amorphous (ductile) particles are compared. For large laser fluences, nearly complete dissociation of the absorbing material is observed, whereas the nonabsorbing portions remain fairly intact. Because large fluences can cause photofragmentation of constituent molecules, multiple pulses at low laser fluence and/or lasers with different wavelengths are recommended for the best representative sampling of multicomponent aerosol particles in laser desorption/ionization (LDI) mass spectrometry

A comparison of chemical structures of soot precursor nanoparticles from liquid fuel combustion in flames and engine

International Nuclear Information System (INIS)

Paul, Bireswar; Datta, Amitava; Datta, Aparna; Saha, Abhijit

2013-01-01

A comparative study of the chemical structures of soot precursor nanoparticles from the liquid fuel flame and engine exhaust has been performed in this work to establish an association between the particles from both the sources. Different ex-situ measurement techniques have been used to characterize the nanoparticles in samples collected from the laboratory petrol/air and iso-octane/air flames, as well as from a gasoline engine. The TEM images of the sampled material along with the EDS spectra corroborate the existence of carbonaceous nanoparticles. The nature of the UV absorption and fluorescence spectra of the samples from the iso-octane flame environment further confirms the sampled materials to be soot precursor nanoparticles. The DLS size distribution of the particles shows them to be below 10 nm size. FTIR spectrum of the precursor nanoparticles collected form the non-sooting zone of the flame and that of fully grown soot particles show few similarities and dissimilarities among them. The soot particles are found to be much more aromatized as compared to its precursor nanoparticles. The presence of carbonyl functional group (C=O) at around 1,720 cm −1 has been observed in soot precursor nanoparticles, while such oxygenated functional groups are not prominent in soot structure. The absorption (UV and IR) and fluorescence spectra of the carbonaceous material collected from the gasoline engine exhaust show many resemblances with those of soot precursor nanoparticles from flames. These spectroscopic resemblances of the soot precursor nanoparticles from the flame environment and engine exhaust gives the evidence that the in-cylinder combustion is the source of these particles in the engine exhaust.

Physicochemical characterization of Capstone depleted uranium aerosols I: uranium concentration in aerosols as a function of time and particle size.

Science.gov (United States)

Parkhurst, Mary Ann; Cheng, Yung Sung; Kenoyer, Judson L; Traub, Richard J

2009-03-01

During the Capstone Depleted Uranium (DU) Aerosol Study, aerosols containing DU were produced inside unventilated armored vehicles (i.e., Abrams tanks and Bradley Fighting Vehicles) by perforation with large-caliber DU penetrators. These aerosols were collected and characterized, and the data were subsequently used to assess human health risks to personnel exposed to DU aerosols. The DU content of each aerosol sample was first quantified by radioanalytical methods, and selected samples, primarily those from the cyclone separator grit chambers, were analyzed radiochemically. Deposition occurred inside the vehicles as particles settled on interior surfaces. Settling rates of uranium from the aerosols were evaluated using filter cassette samples that collected aerosol as total mass over eight sequential time intervals. A moving filter was used to collect aerosol samples over time, particularly within the first minute after a shot. The results demonstrate that the peak uranium concentration in the aerosol occurred in the first 10 s after perforation, and the concentration decreased in the Abrams tank shots to about 50% within 1 min and to less than 2% after 30 min. The initial and maximum uranium concentrations were lower in the Bradley vehicle than those observed in the Abrams tank, and the concentration levels decreased more slowly. Uranium mass concentrations in the aerosols as a function of particle size were evaluated using samples collected in a cyclone sampler, which collected aerosol continuously for 2 h after perforation. The percentages of uranium mass in the cyclone separator stages ranged from 38 to 72% for the Abrams tank with conventional armor. In most cases, it varied with particle size, typically with less uranium associated with the smaller particle sizes. Neither the Abrams tank with DU armor nor the Bradley vehicle results were specifically correlated with particle size and can best be represented by their average uranium mass concentrations of 65

Characteristics of agglomerates of sodium oxide aerosol particles: Task 7, topical report

International Nuclear Information System (INIS)

Gieseke, J.A.; Reed, L.D.; Jordan, H.; Lee, K.W.

1977-01-01

Accurate macroscopic predictions of aerosol population behavior within enclosed containments are known to depend strongly upon the microscopic characteristics of the individual aerosols. Also, coagulation rates due to mechanisms which produce relative motions between particles within the suspended aerosol are known to depend upon the cross sectional areas of the individual particles. Hence, it has been the primary concern of this study to examine experimentally the microscopic characteristics of sodium oxide aerosols produced in air. The results of these measurements can now be incorporated into the various macroscopic aerosol behavior prediction models

Single-Particle Soot Photometer (SP2) Instrument Handbook

Energy Technology Data Exchange (ETDEWEB)

Sedlacek, Arthur [Brookhaven National Lab. (BNL), Upton, NY (United States)

2017-02-01

The SP2 is an instrument that measures, in situ, the time-dependent scattering and incandescence signals produced by individual BC-containing particles as they travel through a continuous-wave laser beam. Any particle traversing the laser beam will scatter light, and the BC component of a BC-containing particle will absorb some of the laser energy until its temperature is raised to the point at which it incandesces (hereafter we adopt the standard terminology of the SP2 community and denote any substance determined by the SP2 to be BC as refractory black carbon (rBC)). The amplitude of the rBC incandescence signal is related to the amount of refractory material contained in the illuminated particle. By binning the individual incandescence signals per unit sample volume, the mass concentration [ng/m3] of rBC can be derived. By binning the individual signals by volume equivalent diameter the size distribution (dN/dlogDVED) per unit time can be derived. The rBC mass loading per unit time and the rBC size distribution unit time are the core data products produced by the SP2. Additionally, the scattering channel can be used to provide information on the rBC particle population-based mixing states within ambient aerosols. However, this data product is produced on a requested-basis since additional detailed analysis and QC/QA must be conducted.

Aging fingerprints in combustion particles

Science.gov (United States)

Zelenay, V.; Mooser, R.; Tritscher, T.; Křepelová, A.; Heringa, M. F.; Chirico, R.; Prévôt, A. S. H.; Weingartner, E.; Baltensperger, U.; Dommen, J.; Watts, B.; Raabe, J.; Huthwelker, T.; Ammann, M.

2011-05-01

Soot particles can significantly influence the Earth's climate by absorbing and scattering solar radiation as well as by acting as cloud condensation nuclei. However, despite their environmental (as well as economic and political) importance, the way these properties are affected by atmospheric processing is still a subject of discussion. In this work, soot particles emitted from two different cars, a EURO 2 transporter, a EURO 3 passenger vehicle, and a wood stove were investigated on a single-particle basis. The emitted exhaust, including the particulate and the gas phase, was processed in a smog chamber with artificial solar radiation. Single particle specimens of both unprocessed and aged soot were characterized using x-ray absorption spectroscopy and scanning electron microscopy. Comparison of the spectra from the unprocessed and aged soot particles revealed changes in the carbon functional group content, such as that of carboxylic carbon, which can be ascribed to both the condensation of secondary organic compounds on the soot particles and oxidation of primary soot particles upon photochemical aging. Changes in the morphology and size of the single soot particles were also observed upon aging. Furthermore, we show that the soot particles take up water in humid environments and that their water uptake capacity increases with photochemical aging.

Formation of charged particles in condensation aerosol generators used for inhalation studies

International Nuclear Information System (INIS)

Ramu, M.C.R.; Vohra, K.G.

1976-01-01

Formation of charged particles in a condensation aerosol generator has been studied using a charge collector and a mobility analyzer. Measurements carried out using the charge collector show that the number of charged particles increases with an increase in the particle diameter. The number of charged particles measured also depends on the thickness of the sodium chloride coating on the platinum wire used in the aerosol generator for the production of condensation nuclei. It was found that the charged particle concentration increases with decreasing coating thickness. Mobility measurements have shown that the particles are singly and doubly charged. It has been estimated that about 10% of the particles produced in the generator are charged. The mechanism of formation of charged particles in the aerosol generator has been briefly discussed. (author)

Durable superhydrophobic carbon soot coatings for sensor applications

Science.gov (United States)

Esmeryan, K. D.; Radeva, E. I.; Avramov, I. D.

2016-01-01

A novel approach for the fabrication of durable superhydrophobic (SH) carbon soot coatings used in quartz crystal microbalance (QCM) based gas or liquid sensors is reported. The method uses modification of the carbon soot through polymerization of hexamethyldisiloxane (HMDSO) by means of glow discharge RF plasma. The surface characterization shows a fractal-like network of carbon nanoparticles with diameter of ~50 nm. These particles form islands and cavities in the nanometer range, between which the plasma polymerized hexamethyldisiloxane (PPHMDSO) embeds and binds to the carbon chains and QCM surface. Such modified surface structure retains the hydrophobic nature of the soot and enhances its robustness upon water droplet interactions. Moreover, it significantly reduces the insertion loss and dynamic resistance of the QCM compared to the commonly used carbon soot/epoxy resin approach. Furthermore, the PPHMDSO/carbon soot coating demonstrates durability and no aging after more than 40 probing cycles in water based liquid environments. In addition, the surface layer keeps its superhydrophobicity even upon thermal annealing up to 540 °C. These experiments reveal an opportunity for the development of soot based SH QCMs with improved electrical characteristics, as required for high-resolution gas or liquid measurements.

The statistical distribution of aerosol properties in sourthern West Africa

Science.gov (United States)

Haslett, Sophie; Taylor, Jonathan; Flynn, Michael; Bower, Keith; Dorsey, James; Crawford, Ian; Brito, Joel; Denjean, Cyrielle; Bourrianne, Thierry; Burnet, Frederic; Batenburg, Anneke; Schulz, Christiane; Schneider, Johannes; Borrmann, Stephan; Sauer, Daniel; Duplissy, Jonathan; Lee, James; Vaughan, Adam; Coe, Hugh

2017-04-01

The population and economy in southern West Africa have been growing at an exceptional rate in recent years and this trend is expected to continue, with the population projected to more than double to 800 million by 2050. This will result in a dramatic increase in anthropogenic pollutants, already estimated to have tripled between 1950 and 2000 (Lamarque et al., 2010). It is known that aerosols can modify the radiative properties of clouds. As such, the entrainment of anthropogenic aerosol into the large banks of clouds forming during the onset of the West African Monsoon could have a substantial impact on the region's response to climate change. Such projections, however, are greatly limited by the scarcity of observations in this part of the world. As part of the Dynamics-Aerosol-Chemistry-Cloud Interactions in West Africa (DACCIWA) project, three research aircraft were deployed, each carrying equipment capable of measuring aerosol properties in-situ. Instrumentation included Aerosol Mass Spectrometers (AMS), Single Particle Soot Photometers (SP2), Condensation Particle Counters (CPC) and Scanning Mobility Particle Sizers (SMPS). Throughout the intensive aircraft campaign, 155 hours of scientific flights covered an area including large parts of Benin, Togo, Ghana and parts of Côte D'Ivoire. Approximately 70 hours were dedicated to the measurement of cloud-aerosol interactions, with many other flights producing data contributing towards this objective. Using datasets collected during this campaign period, it is possible to build a robust statistical understanding of aerosol properties in this region for the first time, including size distributions and optical and chemical properties. Here, we describe preliminary results from aerosol measurements on board the three aircraft. These have been used to describe aerosol properties throughout the region and time period encompassed by the DACCIWA aircraft campaign. Such statistics will be invaluable for improving future

Nuclear track radiography of 'hot' aerosol particles

Energy Technology Data Exchange (ETDEWEB)

Boulyga, S.F.; Kievitskaja, A.I.; Kievets, M.K.; Lomonosova, E.M.; Zhuk, I.V.; Yaroshevich, O.I.; Perelygin, V.P.; Petrova, R.; Brandt, R.; Vater, P

1999-06-01

Nuclear track radiography was applied to identify aerosol 'hot' particles which contain elements of nuclear fuel and fallout after Chernobyl NPP accident. For the determination of the content of transuranium elements in radioactive aerosols the measurement of the {alpha}-activity of 'hot' particles by SSNTD was used in this work, as well as radiography of fission fragments formed as a result of the reactions (n,f) and ({gamma},f) in the irradiation of aerosol filters by thermal neutrons and high energy gamma quanta. The technique allowed the sizes and alpha-activity of 'hot' particles to be determined without extracting them from the filter, as well as the determination of the uranium content and its enrichment by {sup 235}U, {sup 239}Pu and {sup 241}Pu isotopes. Sensitivity of determination of alpha activity by fission method is 5x10{sup -6} Bq per particle. The software for the system of image analysis was created. It ensured the identification of track clusters on an optical image of the SSNTD surface obtained through a video camera and the determination of size and activity of 'hot' particles00.

Aerosols from biomass combustion. Particle formation, relevance on air quality, and measures for particle reduction

International Nuclear Information System (INIS)

Nussbaumer, Thomas

2005-01-01

Biomass combustion is a relevant source of particle emissions. In Switzerland, wood combustion contributes with 2% to the energy supply but with more than 4% to Particulate Matter smaller 10 microns (PM 10) in the ambient air. In areas with high density of residential wood heating (e.g. in the south of Chile), wood particles are the dominant source of PM 10 resulting in heavy local smog situations. Since combustion particles are regarded as health relevant and since immission limit values on PM 10 are widely exceeded, measures for particle reduction from biomass combustion are of high priority. With respect to aerosols from biomass combustion, two sources of particles are distinguished: 1. an incomplete combustion can lead to soot and organic matter contained in the particles, 2. ash constituents in the fuel lead to the formation of inorganic fly ash particles mainly consisting of salts such as chlorides and oxides. The theory of aerosol formation from fuel constituents is described and two hypotheses to reduce inorganic particles from biomass combustion are proposed: 1. a reduced oxygen content in the solid fuel conversion zone (glow bed in a fixed bed combustion) is assumed to reduce the particle mass concentration due to three mechanisms: a) reduced oxidation of fuel constituents to compounds with higher volatility, b) reduced local temperature for solid fuel conversion, c) a reduced entrainmed of fuel constituents 2. a reduced total excess air can reduce the particle number due to enhanced coagulation. The proposed low-particle concept has been implemented for an automatic furnace for wood pellets in the size range from 100 kW to 500 kW. Furthermore, the furnace design was optimised to enable a part load operation without increased emissions of carbon monoxide (CO) and particles. In a 100 kW prototype furnace the low-particle conditions resulted in particle emissions between 6 mg/m n 3 to 11 mg/m n 3 at 13 vol.-% O2 and CO emissions below 70 mg/m n 3 in the

Scattering of aerosol particles by a Hermite-Gaussian beam in marine atmosphere.

Science.gov (United States)

Huang, Qingqing; Cheng, Mingjian; Guo, Lixin; Li, Jiangting; Yan, Xu; Liu, Songhua

2017-07-01

Based on the complex-source-point method and the generalized Lorenz-Mie theory, the scattering properties and polarization of aerosol particles by a Hermite-Gaussian (HG) beam in marine atmosphere is investigated. The influences of beam mode, beam width, and humidity on the scattered field are analyzed numerically. Results indicate that when the number of HG beam modes u (v) increase, the radar cross section of aerosol particles alternating appears at maximum and minimum values in the forward and backward scattering, respectively, because of the special petal-shaped distribution of the HG beam. The forward and backward scattering of aerosol particles decreases with the increase in beam waist. When beam waist is less than the radius of the aerosol particle, a minimum value is observed in the forward direction. The scattering properties of aerosol particles by the HG beam are more sensitive to the change in relative humidity compared with those by the plane wave and the Gaussian beam (GB). The HG beam shows superiority over the plane wave and the GB in detecting changes in the relative humidity of marine atmosphere aerosol. The effects of relative humidity on the polarization of the HG beam have been numerically analyzed in detail.

Polyhexamethylene guanidine phosphate aerosol particles induce pulmonary inflammatory and fibrotic responses.

Science.gov (United States)

Kim, Ha Ryong; Lee, Kyuhong; Park, Chang We; Song, Jeong Ah; Shin, Da Young; Park, Yong Joo; Chung, Kyu Hyuck

2016-03-01

Polyhexamethylene guanidine (PHMG) phosphate was used as a disinfectant for the prevention of microorganism growth in humidifiers, without recognizing that a change of exposure route might cause significant health effects. Epidemiological studies reported that the use of humidifier disinfectant containing PHMG-phosphate can provoke pulmonary fibrosis. However, the pulmonary toxicity of PHMG-phosphate aerosol particles is unknown yet. This study aimed to elucidate the toxicological relationship between PHMG-phosphate aerosol particles and pulmonary fibrosis. An in vivo nose-only exposure system and an in vitro air-liquid interface (ALI) co-culture model were applied to confirm whether PHMG-phosphate induces inflammatory and fibrotic responses in the respiratory tract. Seven-week-old male Sprague-Dawley rats were exposed to PHMG-phosphate aerosol particles for 3 weeks and recovered for 3 weeks in a nose-only exposure chamber. In addition, three human lung cells (Calu-3, differentiated THP-1 and HMC-1 cells) were cultured at ALI condition for 12 days and were treated with PHMG-phosphate at set concentrations and times. The reactive oxygen species (ROS) generation, airway barrier injuries and inflammatory and fibrotic responses were evaluated in vivo and in vitro. The rats exposed to PHMG-phosphate aerosol particles in nanometer size showed pulmonary inflammation and fibrosis including inflammatory cytokines and fibronectin mRNA increase, as well as histopathological changes. In addition, PHMG-phosphate triggered the ROS generation, airway barrier injuries and inflammatory responses in a bronchial ALI co-culture model. Those results demonstrated that PHMG-phosphate aerosol particles cause pulmonary inflammatory and fibrotic responses. All features of fibrogenesis by PHMG-phosphate aerosol particles closely resembled the pathology of fibrosis that was reported in epidemiological studies. Finally, we expected that PHMG-phosphate infiltrated into the lungs in the form of

Shortwave radiative effects of unactivated aerosol particles in clouds

International Nuclear Information System (INIS)

Ackerman, T.; Baker, M.B.

1977-01-01

Clouds in some polluted areas may contain high concentrations of anthropogenic aerosol particles. The possible role of these particles in perturbing the optical and dynamical properties of the clouds is an important question for climate studies. The direct radiative effects of unactivated aerosol particles in stable stratus clouds have been calculated at lambda=0.5μm. Several simplifying asumptions have been made relating the behavior of such particles in the high humidity enviornment within the cloud to their physicochemical make-up. It is shown that the energy absorbed by particles within the clouds may be, for realistic concentrations, comparable to the latent heat released and thus may play a significant role in cloud dynamics in some areas. These results are shown to be relatively insensitive to the assumptions about the particle properties within the cloud

Characterization of Diesel Soot Aggregates by Scattering and Extinction Methods

Science.gov (United States)

Kamimoto, Takeyuki

2006-07-01

Characteristics of diesel soot particles sampled from diesel exhaust of a common-rail turbo-charged diesel engine are quantified by scattering and extinction diagnostics using newly build two laser-based instruments. The radius of gyration representing the aggregates size is measured by the angular distribution of scattering intensity, while the soot mass concentration is measured by a two-wavelength extinction method. An approach to estimate the refractive index of diesel soot by an analysis of the extinction and scattering data using an aggregates scattering theory is proposed.

Characterization of Diesel Soot Aggregates by Scattering and Extinction Methods

International Nuclear Information System (INIS)

Kamimoto, Takeyuki

2006-01-01

Characteristics of diesel soot particles sampled from diesel exhaust of a common-rail turbo-charged diesel engine are quantified by scattering and extinction diagnostics using newly build two laser-based instruments. The radius of gyration representing the aggregates size is measured by the angular distribution of scattering intensity, while the soot mass concentration is measured by a two-wavelength extinction method. An approach to estimate the refractive index of diesel soot by an analysis of the extinction and scattering data using an aggregates scattering theory is proposed

Numerical Investigation of Soot Formation in Non-premixed Flames

KAUST Repository

Abdelgadir, Ahmed Gamaleldin

2017-05-01

Soot is a carbon particulate formed as a result of the combustion of fossil fuels. Due to the health hazard posed by the carbon particulate, government agencies have applied strict regulations to control soot emissions from road vehicles, airplanes, and industrial plants. Thus, understanding soot formation and evolution is critical. Practical combustion devices operate at high pressure and in the turbulent regime. Elevated pressures and turbulence on soot formation significantly and fundamental understanding of these complex interactions is still poor. In this study, the effects of pressure and turbulence on soot formation and growth are investigated numerically. As the first step, the evolution of the particle size distribution function (PSDF) and soot particles morphology are investigated in turbulent non-premixed flames. A Direct Simulation Monte Carlo (DSMC) code is developed and used. The stochastic reactor describes the evolution of soot in fluid parcels following Lagrangian trajectories in a turbulent flow field. The trajectories are sampled from a Direct Numerical Simulation (DNS) of an n-heptane turbulent non-premixed flame. Although individual trajectories display strong bimodality as in laminar flames, the ensemble-average PSDF possesses only one mode and a broad tail, which implies significant polydispersity induced by turbulence. Secondly, the effect of the flow and mixing fields on soot formation at atmospheric and elevated pressures is investigated in coflow laminar diffusion flames. The experimental observation and the numerical prediction of the spatial distribution are in good agreement. Based on the common scaling methodology of the flames (keeping the Reynolds number constant), the scalar dissipation rate decreases as pressure increases, promoting the formation of PAH species and soot. The decrease of the scalar dissipation rate significantly contributes to soot formation occurring closer to the nozzle and outward on the flames wings as pressure

Determination of Aerosol Particle Diameter Using Cascade Impactor Procedure

International Nuclear Information System (INIS)

Bunawas; Ruslanto, P. O

1998-01-01

Determination of aerosol particle size distribution has been done using a low pressure Andersen's cascade impactor with 13 stages. The aerosol has been sampled with flow rate of aerosol sampling of 28.3 Ipm. Preliminary study result shows that aerosol in the simulation chamber was spread in monomodal distribution with Mass Median Aerodynamic Diameter of 4.9 μm. The aerosol measurement in Japan Power Demonstration Reactor has been spread in trimodal distribution with Activity Median Aerodynamic Diameter equal to 13.3 μm. The use of mylar as impaction plate instead of aluminum foil gives good result

NAA of an iridium tracer to determine soot exposure of students commuting on Baltimore`s buses

Energy Technology Data Exchange (ETDEWEB)

Ondov, J.M.; Wu, C.C.; Lin, Zhibo; Kidwell, C.B. [Univ. of Maryland, College Park, MD (United States)

1997-12-01

Epidemiologic studies suggest that short-term increases in indices of particulate air pollution are associated with increased mortality and morbidity from respiratory and cardiovascular diseases. An important component of urban aerosol, diesel soot, is a known respiratory irritant and contains mutagenic and carcinogenic organic compounds. In the United States, motor vehicles are thought to be the largest single source of atmospheric soot and account for {approximately}36% of the annual anthropogenic emission of toxic polynuclear aromatic hydrocarbons (PAH). Much of the motor-vehicle-derived PAH originates from diesel-powered vehicles because their PAH emissions are up to 50-fold greater than those from gasoline engines. In Baltimore, city high school students take public buses to school and, often, must stand at bus stops while many diesel buses pass or stop before their own buses arrive. To estimate student exposures to soot emitted from public diesel buses (MTA) during commutes to city high schools, the Baltimore municipal fuel supply was tagged with an iridium tracer, and exposure was monitored during commutes with personal aerosol monitors as a part of the Baltimore Environmental Justice Project.

Impact of morphology on the radiative properties of fractal soot aggregates

International Nuclear Information System (INIS)

Doner, Nimeti; Liu, Fengshan

2017-01-01

The impact of morphology on the radiative properties of fractal soot aggregates was investigated using the discrete dipole approximation (DDA). The optical properties of four different types of aggregates of freshly emitted soot with a fractal dimension D f =1.65 and a fractal pre-factor k f =1.76 were calculated. The four types of aggregates investigated are formed by uniform primary particles in point-touch, by uniform but overlapping primary particles, by uniform but enlarged primary particles in point-touch, and formed by point-touch and polydisperse primary particles. The radiative properties of aggregates consisting of N=20, 56 and 103 primary particles were numerically evaluated for a given refractive index at 0.532 and 1.064 μm. The radiative properties of soot aggregates vary strongly with the volume equivalent radius a eff and wavelength. The accuracy of DDA was evaluated in the first and fourth cases against the generalized multi-sphere Mie (GMM) solution in terms of the vertical–vertical differential scattering cross section (C vv ). The model predicted the average relative deviations from the base case to be within 15–25% for C vv , depending on the number of particles for the aggregate. The scattering cross sections are only slightly affected by the overlapping but more significantly influenced by primary particle polydispersity. It was also found that the enlargement of primary particles by 20% has a strong effect on soot aggregate radiative properties. - Highlights: • The radiative properties of aggregates of N=20, 56 and 103 primary particles were investigated. • Four different cases, formed by point-touch, overlapping, aggregate expansion and polydispersion, were studied. • The effects of overlapping and aggregate expansion on morphology are found to be the same.

Single-particle characterization of urban aerosol particles collected in three Korean cites using low-Z electron probe X-ray microanalysis.

Science.gov (United States)

Ro, Chul-Un; Kim, HyeKyeong; Oh, Keun-Young; Yea, Sun Kyung; Lee, Chong Bum; Jang, Meongdo; Van Grieken, René

2002-11-15

A recently developed single-particle analytical technique, called low-Z electron probe X-ray microanalysis (low-Z EPMA), was applied to characterize urban aerosol particles collected in three cities of Korea (Seoul, CheongJu, and ChunCheon) on single days in the winter of 1999. In this study, it is clearly demonstrated that the low-Z EPMA technique can provide detailed and quantitative information on the chemical composition of particles in the urban atmosphere. The collected aerosol particles were analyzed and classified on the basis of their chemical species. Various types of particles were identified, such as soil-derived, carbonaceous, marine-originated, and anthropogenic particles. In the sample collected in Seoul, carbonaceous, aluminosilicates, silicon dioxide, and calcium carbonate aerosol particles were abundantly encountered. In the CheongJu and ChunCheon samples, carbonaceous, aluminosilicates, reacted sea salts, and ammonium sulfate aerosol particles were often seen. However, in the CheongJu sample, ammonium sulfate particles were the most abundant in the fine fraction. Also, calcium sulfate and nitrate particles were significantly observed. In the ChunCheon sample, organic particles were the most abundant in the fine fraction. Also, sodium nitrate particles were seen at high levels. The ChunCheon sample seemed to be strongly influenced by sea-salt aerosols originating from the Yellow Sea, which is located about 115 km away from the city.

Wintertime water-soluble aerosol composition and particle water content in Fresno, California

Science.gov (United States)

Parworth, Caroline L.; Young, Dominique E.; Kim, Hwajin; Zhang, Xiaolu; Cappa, Christopher D.; Collier, Sonya; Zhang, Qi

2017-03-01

The composition and concentrations of water-soluble gases and ionic aerosol components were measured from January to February 2013 in Fresno, CA, with a particle-into-liquid sampler with ion chromatography and annular denuders. The average (±1σ) ionic aerosol mass concentration was 15.0 (±9.4) µg m-3, and dominated by nitrate (61%), followed by ammonium, sulfate, chloride, potassium, nitrite, and sodium. Aerosol-phase organic acids, including formate and glycolate, and amines including methylaminium, triethanolaminium, ethanolaminium, dimethylaminium, and ethylaminium were also detected. Although the dominant species all came from secondary aerosol formation, there were primary sources of ionic aerosols as well, including biomass burning for potassium and glycolate, sea spray for sodium, chloride, and dimethylamine, and vehicles for formate. Particulate methanesulfonic acid was also detected and mainly associated with terrestrial sources. On average, the molar concentration of ammonia was 49 times greater than nitric acid, indicating that ammonium nitrate formation was limited by nitric acid availability. Particle water was calculated based on the Extended Aerosol Inorganics Model (E-AIM) thermodynamic prediction of inorganic particle water and κ-Köhler theory approximation of organic particle water. The average (±1σ) particle water concentration was 19.2 (±18.6) µg m-3, of which 90% was attributed to inorganic species. The fractional contribution of particle water to total fine particle mass averaged at 36% during this study and was greatest during early morning and night and least during the day. Based on aqueous-phase concentrations of ions calculated by using E-AIM, the average (±1σ) pH of particles in Fresno during the winter was estimated to be 4.2 (±0.2).

Effects of methyl group on aromatic hydrocarbons on the nanostructures and oxidative reactivity of combustion-generated soot

KAUST Repository

Guerrero Peñ a, Gerardo D.J.; Alrefaai, Mhd Maher; Yang, Seung Yeon; Raj, Abhijeet; Brito, Joaquin L.; Stephen, Samuel; Anjana, Tharalekshmy; Pillai, Vinu; Al Shoaibi, Ahmed; Chung, Suk-Ho

2016-01-01

The substituted and unsubstituted aromatic hydrocarbons, present in transportation fuels such as gasoline and diesel, are thought to be responsible for most of the soot particles produced during their combustion. However, the effects of the substituted alkyl groups on the aromatic hydrocarbons on their sooting tendencies, and on the physical and chemical properties of soot produced from them are not well understood. In this work, the effect of the presence of methyl groups on aromatic hydrocarbons on their sooting propensity, and on the oxidative reactivity, morphology, and chemical composition of soot generated from them in diffusion flames is studied using benzene, toluene, and m-xylene as fuels. Several experimental techniques including high resolution transmission electron microscopy and X-ray diffraction are used to identify the morphological changes in soot, whereas the elemental and thermo-gravimetric analyses, electron energy loss spectroscopy, and Fourier transform infrared spectroscopy are used to study the changes in its chemical properties and reactivity. The activation energies for soot oxidation are calculated at different conversion levels, and a trend in the reactivity of soots from benzene, toluene and m-xylene is reported. It is observed that the sizes of primary particles and graphene-like sheets, and the concentrations of aliphatics and oxygenated groups in soot particles decreased with the addition of methyl group(s) on the aromatic ring. The physicochemical changes in soot are found to support the oxidative reactivity trends. © 2016 The Combustion Institute

Effects of methyl group on aromatic hydrocarbons on the nanostructures and oxidative reactivity of combustion-generated soot

KAUST Repository

Guerrero Peña, Gerardo D.J.

2016-07-23

The substituted and unsubstituted aromatic hydrocarbons, present in transportation fuels such as gasoline and diesel, are thought to be responsible for most of the soot particles produced during their combustion. However, the effects of the substituted alkyl groups on the aromatic hydrocarbons on their sooting tendencies, and on the physical and chemical properties of soot produced from them are not well understood. In this work, the effect of the presence of methyl groups on aromatic hydrocarbons on their sooting propensity, and on the oxidative reactivity, morphology, and chemical composition of soot generated from them in diffusion flames is studied using benzene, toluene, and m-xylene as fuels. Several experimental techniques including high resolution transmission electron microscopy and X-ray diffraction are used to identify the morphological changes in soot, whereas the elemental and thermo-gravimetric analyses, electron energy loss spectroscopy, and Fourier transform infrared spectroscopy are used to study the changes in its chemical properties and reactivity. The activation energies for soot oxidation are calculated at different conversion levels, and a trend in the reactivity of soots from benzene, toluene and m-xylene is reported. It is observed that the sizes of primary particles and graphene-like sheets, and the concentrations of aliphatics and oxygenated groups in soot particles decreased with the addition of methyl group(s) on the aromatic ring. The physicochemical changes in soot are found to support the oxidative reactivity trends. © 2016 The Combustion Institute

Ultrasonic-resonator-combined apparatus for purifying nuclear aerosol particles

Energy Technology Data Exchange (ETDEWEB)

Hou, Suxia; Zhang, Quanhu; Li, Sufen; Chen, Chen; Su, Xianghua [Xi' an Hi-Tech Institute, Xi' an (China)

2017-12-15

The radiation hazards of radionuclides in the air arising from the storage room of nuclear devices to the operators cannot be ignored. A new ultrasonic-resonator-combined method for purifying nuclear aerosol particles is introduced. To remove particles with diameters smaller than 0.3 μm, an ultrasonic chamber is induced to agglomerate these submicron particles. An apparatus which is used to purify the nuclear aerosol particles is described in the article. The apparatus consists of four main parts: two filtering systems, an ultrasonic chamber and a high-pressure electrostatic precipitator system. Finally, experimental results demonstrated the effectiveness of the implementation of the ultrasonic resonators. The feasibility of the method is proven by its application to the data analysis of the experiments.

Bounce behavior of freshly nucleated biogenic secondary organic aerosol particles

Directory of Open Access Journals (Sweden)

A. Virtanen

2011-08-01

Full Text Available The assessment of the climatic impacts and adverse health effects of atmospheric aerosol particles requires detailed information on particle properties. However, very limited information is available on the morphology and phase state of secondary organic aerosol (SOA particles. The physical state of particles greatly affects particulate-phase chemical reactions, and thus the growth rates of newly formed atmospheric aerosol. Thus verifying the physical phase state of SOA particles gives new and important insight into their formation, subsequent growth, and consequently potential atmospheric impacts. According to our recent study, biogenic SOA particles produced in laboratory chambers from the oxidation of real plant emissions as well as in ambient boreal forest atmospheres can exist in a solid phase in size range >30 nm. In this paper, we extend previously published results to diameters in the range of 17–30 nm. The physical phase of the particles is studied by investigating particle bounce properties utilizing electrical low pressure impactor (ELPI. We also investigate the effect of estimates of particle density on the interpretation of our bounce observations. According to the results presented in this paper, particle bounce clearly decreases with decreasing particle size in sub 30 nm size range. The comparison measurements by ammonium sulphate and investigation of the particle impaction velocities strongly suggest that the decreasing bounce is caused by the differences in composition and phase of large (diameters greater than 30 nm and smaller (diameters between 17 and 30 nm particles.

Source apportionment of aerosol particles using polycapillary slightly focusing X-ray lens

Energy Technology Data Exchange (ETDEWEB)

Sun Tianxi [Key Laboratory of Beam Technology and Materials Modification of Ministry of Education, Beijing Normal University, Beijing 100875 (China) and Institute of Low Energy Nuclear Physics, Beijing Normal University, Beijing 100875 (China) and Beijing Radiation Center, Beijing 100875 (China)], E-mail: stxbeijing@163.com; Liu Zhiguo [Key Laboratory of Beam Technology and Materials Modification of Ministry of Education, Beijing Normal University, Beijing 100875 (China) and Institute of Low Energy Nuclear Physics, Beijing Normal University, Beijing 100875 (China) and Beijing Radiation Center, Beijing 100875 (China)], E-mail: liuzgbeijing@163.com; Zhu Guanghua; Liu Hui [Key Laboratory of Beam Technology and Materials Modification of Ministry of Education, Beijing Normal University, Beijing 100875 (China); Institute of Low Energy Nuclear Physics, Beijing Normal University, Beijing 100875 (China); Beijing Radiation Center, Beijing 100875 (China); Ma Yongzhong [Center for Disease Control and Prevention of Beijing, Beijing 100013 (China); Xu Qing [Institute of High Energy Physics, Chinese Academy of Science, Beijing 100039 (China); Li Yude; Wang Guangpu; Luo Ping; Pan Qiuli; Ding Xunliang [Key Laboratory of Beam Technology and Materials Modification of Ministry of Education, Beijing Normal University, Beijing 100875 (China); Institute of Low Energy Nuclear Physics, Beijing Normal University, Beijing 100875 (China); Beijing Radiation Center, Beijing 100875 (China)

2009-06-11

A micro-X-ray fluorescence (Micro-XRF) spectrometer based on a polycapillary slightly focusing X-ray lens (PSFXRL) and laboratory X-ray source was designed to carry out the source apportionment of aerosol particles. In the distribution curve of the X-ray intensity in the focal spot of PSFXRL, there was a plateau with a diameter of about 65 {mu}m. The uniformity of this plateau was about 3%. This was helpful in measuring the XRF spectrum of a single aerosol particle in which the element distributions are not uniform. The minimum detection limit (MDL) of this Micro-XRF spectrometer was 15 ppm for the Fe-K{sub {alpha}}. The origins of the aerosol particles at the exit of a subway station and a construction site were apportioned. This Micro-XRF spectrometer has potential applications in analysis of single aerosol particles.

Deposition of aerosol particles in bent pipe

International Nuclear Information System (INIS)

Matsui, Hiroshi; Ohhata, Tsutomu

1989-01-01

An equation to estimate deposition fraction of aerosol particles in a bent pipe is derived and the validity is verified experimentally. The equation is obtained by assuming that the resultant acceleration of the gravity and the centrifugal force induced in the bend acts on the aerosol particles, and is found to give a relatively accurate estimation of the deposition fraction if a certain correction factor is introduced to the equation. The deposition fraction has a minimum against Reynold number, and the deposition due to centrifugal force dominates at greater Reynolds number than that at the minimum deposition fraction. On the other hand, the smaller the radius of curvature of the bend is, the larger the deposition fraction due to the centrifugal force is. (author)

An analysis of direct-injection spark-ignition (DISI) soot morphology

Science.gov (United States)

Barone, Teresa L.; Storey, John M. E.; Youngquist, Adam D.; Szybist, James P.

2012-03-01

We have characterized particle emissions produced by a 4-cylinder, 2.0 L DISI engine using transmission electron microscopy (TEM) and image analysis. Analyses of soot morphology provide insight to particle formation mechanisms and strategies for prevention. Particle emissions generated by two fueling strategies were investigated, early injection and injection modified for low particle number concentration emissions. A blend of 20% ethanol and 80% emissions certification gasoline was used for the study given the likelihood of increased ethanol content in widely available fuel. In total, about 200 particles and 3000 primary soot spherules were individually measured. For the fuel injection strategy which produced low particle number concentration emissions, we found a prevalence of single solid sub-25 nm particles and fractal-like aggregates. The modal diameter of single solid particles and aggregate primary particles was between 10 and 15 nm. Solid particles as small as 6 nm were present. Although nanoparticle aggregates had fractal-like morphology similar to diesel soot, the average primary particle diameter per aggregate had a much wider range that spanned from 7 to 60 nm. For the early fuel injection strategy, liquid droplets were prevalent, and the modal average primary particle diameter was between 20 and 25 nm. The presence of liquid droplets may have been the result of unburned fuel and/or lubricating oil originating from fuel impingement on the piston or cylinder wall; the larger modal aggregate primary particle diameter suggests greater fuel-rich zones in-cylinder than for the low particle number concentration point. However, both conditions produced aggregates with a wide range of primary particle diameters, which indicates heterogeneous fuel and air mixing.

Novel Measurements of Aerosol Particle Interfaces Using Biphasic Microfluidics

Science.gov (United States)

Metcalf, A. R.; Dutcher, C. S.

2014-12-01

Secondary organic aerosol (SOA) particles are nearly ubiquitous in the atmosphere and yet there remains large uncertainties in their formation processes and ambient properties. These particles are complex microenvironments, which can contain multiple interfaces due to internal aqueous-organic phase partitioning and to the external liquid-vapor surface. These aerosol interfaces can profoundly affect the fate of condensable organic compounds emitted into the atmosphere by altering the way in which organic vapors interact with the ambient aerosol. Aerosol interfaces affect particle internal structure, species uptake, equilibrium partitioning, activation to cloud condensation or ice nuclei, and optical properties. For example, organic thin films can shield the core of the aerosol from the ambient environment, which may disrupt equilibrium partitioning and mass transfer. To improve our ability to accurately predict the fate of SOA in the atmosphere, we must improve our knowledge of aerosol interfaces and their interactions with the ambient environment. Few technologies exist to accurately probe aerosol interfaces at atmospherically-relevant conditions. In this talk, a novel method using biphasic microscale flows will be introduced for generating, trapping, and perturbing complex interfaces at atmospherically relevant conditions. These microfluidic experiments utilize high-speed imaging to monitor interfacial phenomena at the microscale and are performed with phase contrast and fluorescence microscopy on a temperature-controlled inverted microscope stage. From these experiments, interfacial thermodynamic properties such as surface tension, rheological properties such as interfacial moduli, and kinetic properties such as mass transfer coefficients can be measured or inferred. Chemical compositions of the liquid phases studied here span a range of viscosities and include electrolyte and water soluble organic acid species often observed in the atmosphere, such as mixtures

Aerosol particle size distribution in the stratosphere retrieved from SCIAMACHY limb measurements

Science.gov (United States)

Malinina, Elizaveta; Rozanov, Alexei; Rozanov, Vladimir; Liebing, Patricia; Bovensmann, Heinrich; Burrows, John P.

2018-04-01

health, stratospheric aerosol plays an important role in atmospheric chemistry and climate change. In particular, information about the amount and distribution of stratospheric aerosols is required to initialize climate models, as well as validate aerosol microphysics models and investigate geoengineering. In addition, good knowledge of stratospheric aerosol loading is needed to increase the retrieval accuracy of key trace gases (e.g. ozone or water vapour) when interpreting remote sensing measurements of the scattered solar light. The most commonly used characteristics to describe stratospheric aerosols are the aerosol extinction coefficient and Ångström coefficient. However, the use of particle size distribution parameters along with the aerosol number density is a more optimal approach. In this paper we present a new retrieval algorithm to obtain the particle size distribution of stratospheric aerosol from space-borne observations of the scattered solar light in the limb-viewing geometry. While the mode radius and width of the aerosol particle size distribution are retrieved, the aerosol particle number density profile remains unchanged. The latter is justified by a lower sensitivity of the limb-scattering measurements to changes in this parameter. To our knowledge this is the first data set providing two parameters of the particle size distribution of stratospheric aerosol from space-borne measurements of scattered solar light. Typically, the mode radius and w can be retrieved with an uncertainty of less than 20 %. The algorithm was successfully applied to the tropical region (20° N-20° S) for 10 years (2002-2012) of SCIAMACHY observations in limb-viewing geometry, establishing a unique data set. Analysis of this new climatology for the particle size distribution parameters showed clear increases in the mode radius after the tropical volcanic eruptions, whereas no distinct behaviour of the absolute distribution width could be identified. A tape recorder

Real-time measurement of aerosol particle concentration at high temperatures; Hiukkaspitoisuuden reaaliaikainen mittaaminen korkeassa laempoetilassa

Energy Technology Data Exchange (ETDEWEB)

Keskinen, J; Hautanen, J; Laitinen, A [Tampere Univ. of Technology (Finland). Physics

1997-10-01

The aim of this project is to develop a new method for continuous aerosol particle concentration measurement at elevated temperatures (up to 800-1000 deg C). The measured property of the aerosol particles is the so called Fuchs surface area. This quantity is relevant for diffusion limited mass transfer to particles. The principle of the method is as follows. First, aerosol particles are charged electrically by diffusion charging process. The charging takes place at high temperature. After the charging, aerosol is diluted and cooled. Finally, aerosol particles are collected and the total charge carried by the aerosol particles is measured. Particle collection and charge measurement take place at low temperature. Benefits of this measurement method are: particles are charged in-situ, charge of the particles is not affected by the temperature and pressure changes after sampling, particle collection and charge measurement are carried out outside the process conditions, and the measured quantity is well defined. The results of this study can be used when the formation of the fly ash particles is studied. Another field of applications is the study and the development of gasification processes. Possibly, the method can also be used for the monitoring the operation of the high temperature particle collection devices. (orig.)

Size measurement of radioactive aerosol particles in intense radiation fields using wire screens and imaging plates

Energy Technology Data Exchange (ETDEWEB)

Oki, Yuichi; Tanaka, Toru; Takamiya, Koichi; Ishi, Yoshihiro; UesugI, Tomonori; Kuriyama, Yasutoshi; Sakamoto, Masaaki; Ohtsuki, Tsutomu [Kyoto University Research Reactor Institute, Osaka (Japan); Nitta, Shinnosuke [Graduate School of Engineering, Kyoto University, Kyoto (Japan); Osada, Naoyuki [Advanced Science Research Center, Okayama University, Okayama (Japan)

2016-09-15

Very fine radiation-induced aerosol particles are produced in intense radiation fields, such as high-intensity accelerator rooms and containment vessels such as those in the Fukushima Daiichi nuclear power plant (FDNPP). Size measurement of the aerosol particles is very important for understanding the behavior of radioactive aerosols released in the FDNPP accident and radiation safety in high-energy accelerators. A combined technique using wire screens and imaging plates was developed for size measurement of fine radioactive aerosol particles smaller than 100 nm in diameter. This technique was applied to the radiation field of a proton accelerator room, in which radioactive atoms produced in air during machine operation are incorporated into radiation-induced aerosol particles. The size of 11C-bearing aerosol particles was analyzed using the wire screen technique in distinction from other positron emitters in combination with a radioactive decay analysis. The size distribution for 11C-bearing aerosol particles was found to be ca. 70 μm in geometric mean diameter. The size was similar to that for 7Be-bearing particles obtained by a Ge detector measurement, and was slightly larger than the number-based size distribution measured with a scanning mobility particle sizer. The particle size measuring method using wire screens and imaging plates was successfully applied to the fine aerosol particles produced in an intense radiation field of a proton accelerator. This technique is applicable to size measurement of radioactive aerosol particles produced in the intense radiation fields of radiation facilities.

Quantifying uncertainty in soot volume fraction estimates using Bayesian inference of auto-correlated laser-induced incandescence measurements

Science.gov (United States)

Hadwin, Paul J.; Sipkens, T. A.; Thomson, K. A.; Liu, F.; Daun, K. J.

2016-01-01

Auto-correlated laser-induced incandescence (AC-LII) infers the soot volume fraction (SVF) of soot particles by comparing the spectral incandescence from laser-energized particles to the pyrometrically inferred peak soot temperature. This calculation requires detailed knowledge of model parameters such as the absorption function of soot, which may vary with combustion chemistry, soot age, and the internal structure of the soot. This work presents a Bayesian methodology to quantify such uncertainties. This technique treats the additional "nuisance" model parameters, including the soot absorption function, as stochastic variables and incorporates the current state of knowledge of these parameters into the inference process through maximum entropy priors. While standard AC-LII analysis provides a point estimate of the SVF, Bayesian techniques infer the posterior probability density, which will allow scientists and engineers to better assess the reliability of AC-LII inferred SVFs in the context of environmental regulations and competing diagnostics.

Elucidating determinants of aerosol composition through particle-type-based receptor modeling

Science.gov (United States)

McGuire, M. L.; Jeong, C.-H.; Slowik, J. G.; Chang, R. Y.-W.; Corbin, J. C.; Lu, G.; Mihele, C.; Rehbein, P. J. G.; Sills, D. M. L.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2011-08-01

An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources was reflected through three factors: two Biomass Burning factors and a highly chemically processed Long Range Transport factor. The Biomass Burning factors were separated by PMF due to differences in chemical processing which were in part elucidated by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique

Simultaneous measurement of the concentrations of soot particles and gas species in light hydrocarbon flames using mass spectrometry

International Nuclear Information System (INIS)

Li, Qingxun; Liu, Fang; Wang, Dezheng; Wang, Tiefeng

2014-01-01

Besides gas species concentrations, soot volume fractions are also important data in the study of flames. This work describes the simultaneous measurement of the concentrations of soot and gas species in light hydrocarbon flames by in situ sampling and mass spectrometry (MS).The reaction medium was frozen by sampling into a very low-pressure tube, and the soot selectivity (proportion of carbon atoms in the reactant converted to soot) was determined from the C and H mass balances using the measured concentrations of the gas species and the mass of soot present per unit gas volume. The H/C ratio of the soot was measured by a thermogravimetry–mass spectrometry combination. The soot volume fraction was calculated from the soot selectivity and density of the soot. The soot selectivity measured by this reduced pressure sampling mass spectrometry (RPSMS) method was verified by measurements using the gravimetric sampling technique where the mass of soot collected in a volume of gas was weighed by a high precision balance. For most of the measurements, the uncertainty in the soot volume fraction was ±5%, but this would be larger when the soot volume fractions are less than 1 ppm. For demonstration, the RPSMS method was used to study a methane fuel-rich flame where the soot volume fractions were 1–5 ppm. The simultaneous measurement of concentrations of soot and gas species is useful for the quantitative study of flames. (paper)

Carbonaceous aerosol particles from common vegetation in the Grand Canyon

International Nuclear Information System (INIS)

Hallock, K.A.; Mazurek, M.A.; Cass, G.R.

1992-05-01

The problem of visibility reduction in the Grand Canyon due to fine organic aerosol particles in the atmosphere has become an area of increased environmental concern. Aerosol particles can be derived from many emission sources. In this report, we focus on identifying organic aerosols derived from common vegetation in the Grand Canyon. These aerosols are expected to be significant contributors to the total atmospheric organic aerosol content. Aerosol samples from living vegetation were collected by resuspension of surface wax and resin components liberated from the leaves of vegetation common to areas of the Grand Canyon. The samples were analyzed using high-resolution gas chromatography/mass spectrometry (GC/MS). Probable identification of compounds was made by comparison of sample spectra with National Institute of Standards and Technology (NIST) mass spectral references and positive identification of compounds was made when possible by comparison with authentic standards as well as NIST references. Using these references, we have been able to positively identify the presence of n-alkane and n-alkanoic acid homolog series in the surface waxes of the vegetation sampled. Several monoterpenes, sesquiterpenes, and diterpenes were identified also as possible biogenic aerosols which may contribute to the total organic aerosol abundance leading to visibility reduction in the Grand Canyon

Influence of particle size and chemistry on the cloud nucleating properties of aerosols

Directory of Open Access Journals (Sweden)

P. K. Quinn

2008-02-01

Full Text Available The ability of an aerosol particle to act as a cloud condensation nuclei (CCN is a function of the size of the particle, its composition and mixing state, and the supersaturation of the cloud. In-situ data from field studies provide a means to assess the relative importance of these parameters. During the 2006 Texas Air Quality – Gulf of Mexico Atmospheric Composition and Climate Study (TexAQS-GoMACCS, the NOAA RV Ronald H. Brown encountered a wide variety of aerosol types ranging from marine near the Florida panhandle to urban and industrial in the Houston-Galveston area. These varied sources provided an opportunity to investigate the role of aerosol sources and chemistry in the potential activation of particles to form cloud droplets. Measurements were made of CCN concentrations, aerosol chemical composition in the size range relevant for particle activation in warm clouds, and aerosol size distributions. Variability in aerosol composition was parameterized by the mass fraction of Hydrocarbon-like Organic Aerosol (HOA for particle diameters less than 200 nm (vacuum aerodynamic. The HOA mass fraction in this size range was lowest for marine aerosol and highest for aerosol sampled close to anthropogenic sources. Combining all data from the experiment reveals that composition (defined by HOA mass fraction explains 40% of the variance in the critical diameter for particle activation at the instrumental supersaturation (S of 0.44%. Correlations between HOA mass fraction and aerosol mean diameter show that these two parameters are essentially independent of one another for this data set. We conclude that, based on the variability of the HOA mass fraction observed during TexAQS-GoMACCS, variability in particle composition played a significant role in determining the fraction of particles that could activate to form cloud droplets. Using a simple model based on Köhler theory and the assumption that HOA is insoluble, we estimate the

Effect of strain rate on sooting limits in counterflow diffusion flames of gaseous hydrocarbon fuels: Sooting temperature index and sooting sensitivity index

KAUST Repository

Wang, Yu

2014-05-01

The effect of the strain rate on the sooting limits in counterflow diffusion flames was investigated in various gaseous hydrocarbon fuels by varying the nitrogen dilution in the fuel and oxidizer streams. The sooting limit was defined as the critical fuel and oxygen mole fraction at which soot started to appear in the elastic light scattering signal. The sooting region for normal alkane fuels at a specified strain rate, in terms of the fuel and oxygen mole fraction, expanded as the number of carbon atoms increased. The alkene fuels (ethylene, propene) tested had a higher propensity for sooting as compared with alkane fuels with the same carbon numbers (ethane, propane). Branched iso-butane had a higher propensity for sooting than did n-butane. An increase in the strain rate reduced the tendency for sooting in all the fuels tested. The sensitivity of the sooting limit to the strain rate was more pronounced for less sooting fuels. When plotted in terms of calculated flame temperature, the critical oxygen mole fraction exhibited an Arrhenius form under sooting limit conditions, which can be utilized to significantly reduce the effort required to determine sooting limits at different strain rates. We found that the limiting temperatures of soot formation flames are viable sooting metrics for quantitatively rating the sooting tendency of various fuels, based on comparisons with threshold soot index and normalized smoke point data. We also introduce a sooting temperature index and a sooting sensitivity index, two quantitative measures to describe sooting propensity and its dependence on strain rate. © 2013 The Combustion Institute.

Number concentrations of solid particles from the spinning top aerosol generator

International Nuclear Information System (INIS)

Mitchell, J.P.

1983-02-01

A spinning top aerosol generator has been used to generate monodisperse methylene blue particles in the size range from 0.6 to 6 μm. The number concentrations of these aerosols have been determined by means of an optical particle counter and compared with the equivalent measurements obtained by filter collection and microscopy. (author)

Aerosol composition and microstructure in the smoky atmosphere of Moscow during the August 2010 extreme wildfires

Science.gov (United States)

Popovicheva, O. B.; Kistler, M.; Kireeva, E. D.; Persiantseva, N. M.; Timofeev, M. A.; Shoniya, N. K.; Kopeikin, V. M.

2017-01-01

This is a comprehensive study of the physicochemical characterization of multicomponent aerosols in the smoky atmosphere of Moscow during the extreme wildfires of August 2010 and against the background atmosphere of August 2011. Thermal-optical analysis, liquid and ion chromatography, IR spectroscopy, and electron microscopy were used to determine the organic content (OC) and elemental content (EC) of carbon, organic/inorganic and ionic compounds, and biomass burning markers (anhydrosaccharides and the potassium ion) and study the morphology and elemental composition of individual particles. It has been shown that the fires are characterized by an increased OC/EC ratio and high concentrations of ammonium, potassium, and sulfate ions in correlation with an increased content of levoglucosan as a marker of biomass burning. The organic compounds containing carbonyl groups point to the process of photochemical aging and the formation of secondary organic aerosols in the urban atmosphere when aerosols are emitted from forest fires. A cluster analysis of individual particles has indicated that when the smokiest atmosphere is characterized by prevailing soot/tar ball particles, which are smoke-emission micromarkers.

Effect of Pore Structure on Soot Deposition in Diesel Particulate Filter

Directory of Open Access Journals (Sweden)

Kazuhiro Yamamoto

2016-12-01

Full Text Available Nowadays, in the after-treatment of diesel exhaust gas, a diesel particulate filter (DPF has been used to trap nano-particles of the diesel soot. However, as there are more particles inside the filter, the pressure which corresponds to the filter backpressure increases, which worsens the fuel consumption rate, together with the abatement of the available torque. Thus, a filter with lower backpressure would be needed. To achieve this, it is necessary to utilize the information on the phenomena including both the soot transport and its removal inside the DPF, and optimize the filter substrate structure. In this paper, to obtain useful information for optimization of the filter structure, we tested seven filters with different porosities and pore sizes. The porosity and pore size were changed systematically. To consider the soot filtration, the particle-laden flow was simulated by a lattice Boltzmann method (LBM. Then, the flow field and the pressure change were discussed during the filtration process.

The formation of aerosol particles during combustion of biomass and waste. Final report

Energy Technology Data Exchange (ETDEWEB)

Hjerrild Zeuthen, J

2007-05-15

This thesis describes the formation of aerosol particles during combustion of biomass and waste. The formation of aerosol particles is investigated by studying condensation of alkali salts from synthetic flue gasses in a laboratory tubular furnace. In this so-called laminar flow aerosol condenser-furnace gaseous alkali chlorides are mixed with sulphur dioxide, water vapour and oxygen. At high temperatures the alkali chloride reacts with sulphur dioxide to form alkali sulphate. During subsequent cooling of the synthetic flue gas the chlorides and sulphates condense either as deposits on walls or on other particles or directly from the gas phase by homogenous nucleation. A previously developed computer code for simulation of one-component nucleation of particles in a cylindrical laminar flow is extended to include a homogeneous gas phase reaction to produce gaseous alkali sulphate. The formation of aerosol particles during full-scale combustion of wheat straw is investigated in a 100 MW grate-fired boiler. Finally, aerosols from incineration of waste are investigated during full-scale combustion of municipal waste in a 22 MW grate-fired unit. (BA)

Prospects of real-time single-particle biological aerosol analysis: A comparison between laser-induced breakdown spectroscopy and aerosol time-of-flight mass spectrometry

International Nuclear Information System (INIS)

Beddows, D.C.S.; Telle, H.H.

2005-01-01

In this paper we discuss the prospects of real-time, in situ laser-induced breakdown spectroscopy applied for the identification and classification of bio-aerosols (including species of potential bio-hazard) within common urban aerosol mixtures. In particular, we address the issues associated with the picking out of bio-aerosols against common background aerosol particles, comparing laser-induced breakdown spectroscopy measurements with data from a mobile single-particle aerosol mass spectrometer (ATOFMS). The data from the latter provide statistical data over an extended period of time, highlighting the variation of the background composition. While single-particle bio-aerosols are detectable in principle, potential problems with small (∼ 1 μm size) bio-aerosols have been identified; constituents of the air mass other than background aerosols, e.g. gaseous CO 2 in conjunction with common background aerosols, may prevent unique recognition of the bio-particles. We discuss whether it is likely that laser-induced breakdown spectroscopy on its own can provide reliable, real-time identification of bio-aerosol in an urban environment, and it is suggested that more than one technique should be or would have to be used. A case for using a combination of laser-induced breakdown spectroscopy and Raman (and/or) laser-induced fluorescence spectroscopy is made

Diurnal Cycles of Aerosol Optical Properties at Pico Tres Padres, Mexico City: Evidences for Changes in Particle Morphology and Secondary Aerosol Formation

Science.gov (United States)

Mazzoleni, C.; Dubey, M.; Chakrabarty, R.; Moosmuller, H.; Onasch, T.; Zavala, M.; Herndon, S.; Kolb, C.

2007-12-01

Aerosol optical properties affect planetary radiative balance and depend on chemical composition, size distribution, and morphology. During the MILAGRO field campaign, we measured aerosol absorption and scattering in Mexico City using the Los Alamos aerosol photoacoustic (LAPA) instrument operating at 781 nm. The LAPA was mounted on-board the Aerodyne Research Inc. mobile laboratory, which hosted a variety of gaseous and aerosol instruments. During the campaign, the laboratory was moved to different sites, capturing spatial and temporal variability. Additionally, we collected ambient aerosols on Nuclepore filters for scanning electron microscopy (SEM) analysis. SEM images of selected filters were taken to study particle morphology. Between March 7th and 19th air was sampled at the top of Pico Tres Padres, a mountain on the north side of Mexico City. Aerosol absorption and scattering followed diurnal patterns related to boundary layer height and solar insulation. We report an analysis of aerosol absorption, scattering, and morphology for three days (9th, 11th and 12th of March 2006). The single scattering albedo (SSA, ratio of scattering to total extinction) showed a drop in the tens-of-minutes-to-hour time frame after the boundary layer grew above the sampling site. Later in the day the SSA rose steadily reaching a maximum in the afternoon. The SEM images showed a variety of aerosol shapes including fractal-like aggregates, spherical particles, and other shapes. The absorption correlated with the CO2 signal and qualitatively with the fraction of fractal-like particles to the total particle count. In the afternoon the SSA qualitatively correlated with a relative increase in spherical particles and total particle count. These observed changes in optical properties and morphology can be explained by the dominant contribution of freshly emitted particles in the morning and by secondary particle formation in the afternoon. SSA hourly averaged values ranged from ~0.63 in

CCN activation experiments with adipic acid: effect of particle phase and adipic acid coatings on soluble and insoluble particles

Directory of Open Access Journals (Sweden)

S. S. Hings

2008-07-01

Full Text Available Slightly soluble atmospherically relevant organic compounds may influence particle CCN activity and therefore cloud formation. Adipic acid is a frequently employed surrogate for such slightly soluble organic materials. The 11 published experimental studies on the CCN activity of adipic acid particles are not consistent with each other nor do they, in most cases, agree with the Köhler theory. The CCN activity of adipic acid aerosol particles was studied over a significantly wider range of conditions than in any previous single study. The work spans the conditions of the previous studies and also provides alternate methods for producing "wet" (deliquesced solution droplets and dry adipic acid particles without the need to produce them by atomization of aqueous solutions. The experiments suggest that the scatter in the previously published CCN measurements is most likely due to the difficulty of producing uncontaminated adipic acid particles by atomization of solutions and possibly also due to uncertainties in the calibration of the instruments. The CCN activation of the small (d_m<150 nm initially dry particles is subject to a deliquescence barrier, while for the larger particles the activation follows the Köhler curve. Wet adipic acid particles follow the Köhler curve over the full range of particle diameters studied. In addition, the effect of adipic acid coatings on the CCN activity of both soluble and insoluble particles has also been studied. When a water-soluble core is coated by adipic acid, the CCN-hindering effect of particle phase is eliminated. An adipic acid coating on hydrophobic soot yields a CCN active particle. If the soot particle is relatively small (d_core≤102 nm, the CCN activity of the coated particles approaches the deliquescence line of adipic acid, suggesting that the total size of the particle determines CCN activation and the soot core acts as a scaffold.

AKTIS Nr. 12: To better understand radioactive aerosol deposit in order to better measure it; Radio-induced lesions: a new step towards healing; Modelling the collapse of an immersed grain column; To better model soot deposit; Towards the prediction of the leakage rate of containment enclosures

International Nuclear Information System (INIS)

Benderitter, Marc; Perales, Frederic; Monerie, Yann; Maro, Denis; Boyer, Patrick; Lemaitre, Pascal; Porcheron, Emmanuel; Depuydt, Guillaume; Masson, Olivier; Gensdarmes, Francois

2013-04-01

This publication presents the main results of researches undertaken by the IRSN in the field of radiation protection, nuclear safety and security. The topics herein addressed are: radio-induced lesions as a new step towards healing (case of injection mesenchymal stem cells for the treatment of induced severe colorectal lesions), the modelling of the collapse of an immersed grain column (to study the nuclear fuel behaviour in an accidental situation through a modelling of fluid-grain interactions), a better understanding of radioactive aerosol deposit (to study particle or aerosol deposits after radioactive releases in the atmosphere in case of accident), a better modelling of soot deposits (in case of fire), the prediction of leakage rates of containment enclosures (ageing phenomena of installations, systems and equipment, with the case of cracks due to material ageing and resulting in confinement losses which could thus be quantified)

On the sources of submicron aerosol particles in savannah: implications for climate and air quality

Energy Technology Data Exchange (ETDEWEB)

Vakkari, V.

2013-11-01

Aerosol is defined as solid or liquid particles suspended in a gas lighter than the particles, which means that the atmosphere we live in is an aerosol in itself. Although aerosol particles are only a trace component of the atmosphere they affect our lives in several ways. The aerosol particles can cause adverse health effects and deteriorate visibility, but they affect also the Earth s climate directly by scattering and absorbing solar radiation and indirectly by modulating the properties of the clouds. Anthropogenic aerosol particles have a net cooling effect on the climate, but the uncertainty in the amount of cooling is presently as large as the heating effect of carbon dioxide. To reduce the uncertainty in the aerosol climate effects, spatially representative reference data of high quality are needed for the global climate models. To be able to capture the diurnal and seasonal variability the data have to be collected continuously over time periods that cover at least one full seasonal cycle. Until recently such data have been nearly non-existing for continental Africa and hence one aim of this work was to establish a permanent measurement station measuring the key aerosol particle properties in a continental location in southern Africa. In close collaboration with the North-West University in South Africa this aim has now been achieved at the Welgegund measurement station. The other aims of this work were to determine the aerosol particle concentrations including their seasonal and diurnal variation and to study the most important aerosol particle sources in continental southern Africa. In this thesis the aerosol size distribution and its seasonal and diurnal variation is reported for different environments ranging from a clean rural background to an anthropogenically heavily influenced mining region in continental southern Africa. Atmospheric regional scale new particle formation has been observed at a world record high frequency and it dominates the diurnal

Interpretation of aerosol trace metal particle size distributions

International Nuclear Information System (INIS)

Johansson, T.B.; Van Grieken, R.E.; Winchester, J.W.

1974-01-01

Proton-induced X-ray emission (PIXE) analysis is capable of rapid routine determination of 10--15 elements present in amounts greater than or equal to 1 ng simultaneously in aerosol size fractions as collected by single orifice impactors over short periods of time. This enables detailed study of complex relationships between elements detected. Since absolute elemental concentrations may be strongly influenced by meteorological and topographical conditions, it is useful to normalize to a reference element. Comparison between the ratios of concentrations with aerosol and corresponding values for anticipated sources may lead to the identification of important sources for the elements. Further geochemical insights may be found through linear correlation coefficients, regression analysis, and cluster analysis. By calculating correlations for elemental pairs, an indication of the degree of covariance between the elements is obtained. Preliminary results indicate that correlations may be particle size dependent. A high degree of covariance may be caused either by a common source or may only reflect the conservative nature of the aerosol. In a regression analysis, by plotting elemental pairs and estimating the regression coefficients, we may be able to conclude if there is more than one source operating for a given element in a certain size range. Analysis of clustering of several elements, previously investigated for aerosol filter samples, can be applied to the analysis of aerosol size fractions. Careful statistical treatment of elemental concentrations as a function of aerosol particle size may thus yield significant information on the generation, transport and deposition of trace metals in the atmosphere

Real-time aerosol photometer and optical particle counter comparison

International Nuclear Information System (INIS)

Santi, E.; Belosi, F.; Santachiara, G.; Prodi, F.; Berico, M.

2010-01-01

The paper presents the results of a comparison exercise among real-time aerosol samplers, based on different light scattering techniques. The comparison was carried out near to the ISAC institute in a box positioned inside the CNR research area in Bologna. Two nephelometers (Dust Trak from TSI, and Air Genius from Unitec) and an optical particle counter (ENVIRO-check from Grimm) were used for P M1 and P M10 fraction assessment. In the case of the optical particle counter, the particle number concentration in each size bin was also used. In parallel, two manual sampling lines were employed for reference (gravimetric) measurements. The results highlight different factor scales for the dust monitors, in comparison with gravimetric assessment, underlining the importance of a user calibration of such monitors as a function of the specific aerosol sampled. Moreover, the relative fluctuations of the hourly P M 10 and P M1 concentrations, against daily average concentrations, were studied in order to compare the ability of each sampler to follow changes in the aerosol size distribution. It was found that the photometers and optical particle counter revealed different behaviours. In the latter, a small increase in the particle concentration number in the coarse fraction gave a relatively high increase in the mass concentration that was not measured by the photometers. The explanation could be the relatively slight influence of a small particle number variation on the total scattered light for the photometers, unlike the case of the optical particle counter, where each particle contributes to the mass concentration. This aspect merits future research in order to better understand optical particle counter output used in P Mx monitoring activities.

Electron mean free path from angle-dependent photoelectron spectroscopy of aerosol particles

Energy Technology Data Exchange (ETDEWEB)

Goldmann, Maximilian; Miguel-Sánchez, Javier; West, Adam H. C.; Yoder, Bruce L.; Signorell, Ruth, E-mail: rsignorell@ethz.ch [Laboratory of Physical Chemistry, ETH Zürich, Vladimir-Prelog-Weg 2, 8093 Zürich (Switzerland)

2015-06-14

We propose angle-resolved photoelectron spectroscopy of aerosol particles as an alternative way to determine the electron mean free path of low energy electrons in solid and liquid materials. The mean free path is obtained from fits of simulated photoemission images to experimental ones over a broad range of different aerosol particle sizes. The principal advantage of the aerosol approach is twofold. First, aerosol photoemission studies can be performed for many different materials, including liquids. Second, the size-dependent anisotropy of the photoelectrons can be exploited in addition to size-dependent changes in their kinetic energy. These finite size effects depend in different ways on the mean free path and thus provide more information on the mean free path than corresponding liquid jet, thin film, or bulk data. The present contribution is a proof of principle employing a simple model for the photoemission of electrons and preliminary experimental data for potassium chloride aerosol particles.

Oxalate metal complexes in aerosol particles: implications for the hygroscopicity of oxalate-containing particles

Directory of Open Access Journals (Sweden)

T. Furukawa

2011-05-01

Full Text Available Atmospheric aerosols have both a direct and an indirect cooling effect that influences the radiative balance at the Earth's surface. It has been estimated that the degree of cooling is large enough to weaken the warming effect of carbon dioxide. Among the cooling factors, secondary organic aerosols (SOA play an important role in the solar radiation balance in the troposphere as SOA can act as cloud condensation nuclei (CCN and extend the lifespan of clouds because of their high hygroscopic and water soluble nature. Oxalic acid is an important component of SOA, and is produced via several formation pathways in the atmosphere. However, it is not certain whether oxalic acid exists as free oxalic acid or as metal oxalate complexes in aerosols, although there is a marked difference in their solubility in water and their hygroscopicity. We employed X-ray absorption fine structure spectroscopy to characterize the calcium (Ca and zinc (Zn in aerosols collected at Tsukuba in Japan. Size-fractionated aerosol samples were collected for this purpose using an impactor aerosol sampler. It was shown that 10–60% and 20–100% of the total Ca and Zn in the finer particles (<2.1 μm were present as Ca and Zn oxalate complexes, respectively. Oxalic acid is hygroscopic and can thus increase the CCN activity of aerosol particles, while complexes with various polyvalent metal ions such as Ca and Zn are not hygroscopic, which cannot contribute to the increase of the CCN activity of aerosols. Based on the concentrations of noncomplexed and metal-complexed oxalate species, we found that most of the oxalic acid is present as metal oxalate complexes in the aerosols, suggesting that oxalic acid does not always increase the hygroscopicity of aerosols in the atmosphere. Similar results are expected for other dicarboxylic acids, such as malonic and succinic acids. Thus, it is advisable that the cooling effect of organic aerosols should be estimated by including the

Particle size of radioactive aerosols generated during machine operation in high-energy proton accelerators

International Nuclear Information System (INIS)

Oki, Yuichi; Kanda, Yukio; Kondo, Kenjiro; Endo, Akira

2000-01-01

In high-energy accelerators, non-radioactive aerosols are abundantly generated due to high radiation doses during machine operation. Under such a condition, radioactive atoms, which are produced through various nuclear reactions in the air of accelerator tunnels, form radioactive aerosols. These aerosols might be inhaled by workers who enter the tunnel just after the beam stop. Their particle size is very important information for estimation of internal exposure doses. In this work, focusing on typical radionuclides such as 7 Be and 24 Na, their particle size distributions are studied. An aluminum chamber was placed in the EP2 beam line of the 12-GeV proton synchrotron at High Energy Accelerator Research Organization (KEK). Aerosol-free air was introduced to the chamber, and aerosols formed in the chamber were sampled during machine operation. A screen-type diffusion battery was employed in the aerosol-size analysis. Assuming that the aerosols have log-normal size distributions, their size distributions were obtained from the radioactivity concentrations at the entrance and exit of the diffusion battery. Radioactivity of the aerosols was measured with Ge detector system, and concentrations of non-radioactive aerosols were obtained using condensation particle counter (CPC). The aerosol size (radius) for 7 Be and 24 Na was found to be 0.01-0.04 μm, and was always larger than that for non-radioactive aerosols. The concentration of non-radioactive aerosols was found to be 10 6 - 10 7 particles/cm 3 . The size for radioactive aerosols was much smaller than ordinary atmospheric aerosols. Internal doses due to inhalation of the radioactive aerosols were estimated, based on the respiratory tract model of ICRP Pub. 66. (author)

Numerical simulation of combustion and soot under partially premixed combustion of low-octane gasoline

KAUST Repository

An, Yanzhao

2017-09-23

In-cylinder combustion visualization and engine-out soot particle emissions were investigated in an optical diesel engine fueled with low octane gasoline. Single injection strategy with an early injection timing (−30 CAD aTDC) was employed to achieve partially premixed combustion (PPC) condition. A high-speed color camera was used to record the combustion images for 150 cycles. The regulated emission of carbon dioxide, carbon monoxide, nitrogen oxides and soot mass concentration were measured experimentally. Full cycle engine simulations were performed using CONVERGE™ and the simulation results matched with the experimental results. The in-cylinder soot particle evolution was performed by coupling a reduced toluene reference fuel mechanism including the PAHs formation/oxidation reactions with particulate size mimic model. The results showed that PPC presents typical stratified combustion characteristics, which is significantly different from the conventional diesel spray-driven combustion. The in-cylinder temperature and equivalence ratio overlaid with soot-NO formation regime revealed that PPC operating condition under study mostly avoided the main sooting conditions throughout the entire combustion. The evaluation of temperature distribution showed formaldehyde could be regarded as an indicator for low temperature reactions, while hydroxyl group represents the high temperature reactions. Soot evolution happened during the combustion process, hydroxyl radicals promoted the soot oxidation.

Numerical simulation of combustion and soot under partially premixed combustion of low-octane gasoline

KAUST Repository

An, Yanzhao; Jaasim, Mohammed; Vallinayagam, R.; Vedharaj, S.; Im, Hong G.; Johansson, Bengt.

2017-01-01

In-cylinder combustion visualization and engine-out soot particle emissions were investigated in an optical diesel engine fueled with low octane gasoline. Single injection strategy with an early injection timing (−30 CAD aTDC) was employed to achieve partially premixed combustion (PPC) condition. A high-speed color camera was used to record the combustion images for 150 cycles. The regulated emission of carbon dioxide, carbon monoxide, nitrogen oxides and soot mass concentration were measured experimentally. Full cycle engine simulations were performed using CONVERGE™ and the simulation results matched with the experimental results. The in-cylinder soot particle evolution was performed by coupling a reduced toluene reference fuel mechanism including the PAHs formation/oxidation reactions with particulate size mimic model. The results showed that PPC presents typical stratified combustion characteristics, which is significantly different from the conventional diesel spray-driven combustion. The in-cylinder temperature and equivalence ratio overlaid with soot-NO formation regime revealed that PPC operating condition under study mostly avoided the main sooting conditions throughout the entire combustion. The evaluation of temperature distribution showed formaldehyde could be regarded as an indicator for low temperature reactions, while hydroxyl group represents the high temperature reactions. Soot evolution happened during the combustion process, hydroxyl radicals promoted the soot oxidation.

Improved identification of primary biological aerosol particles using single-particle mass spectrometry

Directory of Open Access Journals (Sweden)

M. A. Zawadowicz

2017-06-01

Full Text Available Measurements of primary biological aerosol particles (PBAP, especially at altitudes relevant to cloud formation, are scarce. Single-particle mass spectrometry (SPMS has been used to probe aerosol chemical composition from ground and aircraft for over 20 years. Here we develop a method for identifying bioaerosols (PBAP and particles containing fragments of PBAP as part of an internal mixture using SPMS. We show that identification of bioaerosol using SPMS is complicated because phosphorus-bearing mineral dust and phosphorus-rich combustion by-products such as fly ash produce mass spectra with peaks similar to those typically used as markers for bioaerosol. We have developed a methodology to differentiate and identify bioaerosol using machine learning statistical techniques applied to mass spectra of known particle types. This improved method provides far fewer false positives compared to approaches reported in the literature. The new method was then applied to two sets of ambient data collected at Storm Peak Laboratory and a forested site in Central Valley, California to show that 0.04–2 % of particles in the 200–3000 nm aerodynamic diameter range were identified as bioaerosol. In addition, 36–56 % of particles identified as biological also contained spectral features consistent with mineral dust, suggesting internal dust–biological mixtures.

Spatial Variability of CCN Sized Aerosol Particles

Science.gov (United States)

Asmi, A.; Väänänen, R.

2014-12-01

The computational limitations restrict the grid size used in GCM models, and for many cloud types they are too large when compared to the scale of the cloud formation processes. Several parameterizations for e.g. convective cloud formation exist, but information on spatial subgrid variation of the cloud condensation nuclei (CCNs) sized aerosol concentration is not known. We quantify this variation as a function of the spatial scale by using datasets from airborne aerosol measurement campaigns around the world including EUCAARI LONGREX, ATAR, INCA, INDOEX, CLAIRE, PEGASOS and several regional airborne campaigns in Finland. The typical shapes of the distributions are analyzed. When possible, we use information obtained by CCN counters. In some other cases, we use particle size distribution measured by for example SMPS to get approximated CCN concentration. Other instruments used include optical particle counters or condensational particle counters. When using the GCM models, the CCN concentration used for each the grid-box is often considered to be either flat, or as an arithmetic mean of the concentration inside the grid-box. However, the aircraft data shows that the concentration values are often lognormal distributed. This, combined with the subgrid variations in the land use and atmospheric properties, might cause that the aerosol-cloud interactions calculated by using mean values to vary significantly from the true effects both temporary and spatially. This, in turn, can cause non-linear bias into the GCMs. We calculate the CCN aerosol concentration distribution as a function of different spatial scales. The measurements allow us to study the variation of these distributions within from hundreds of meters up to hundreds of kilometers. This is used to quantify the potential error when mean values are used in GCMs.

Characterization of aerosol particles from grass mowing by joint deployment of ToF-AMS and ATOFMS instruments

Science.gov (United States)

Drewnick, Frank; Dall'Osto, Manuel; Harrison, Roy

During a measurement campaign at a semi-urban/industrial site a grass-cutting event was observed, when the lawn in the immediate surrounding of the measurement site was mowed. Using a wide variety of state-of-the-art aerosol measurement technology allowed a broad characterization of the aerosol generated by the lawn mowing. The instrumentation included two on-line aerosol mass spectrometers: an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (ToF-AMS) and a TSI Aerosol Time-of-Flight Mass Spectrometer (ATOFMS); in addition, a selection of on-line aerosol concentration and size distribution instruments (OPC, APS, SMPS, CPC, FDMS-TEOM, MAAP) was deployed. From comparison of background aerosol measurements during most of the day with the aerosol measured during the lawn mowing, the grass cutting was found to generate mainly two different types of aerosol particles: an intense ultrafine particle mode (1 h average: 4 μg m -3) of almost pure hydrocarbon-like organics and a distinct particle mode in the upper sub-micrometer size range containing particles with potassium and nitrogen-organic compounds. The ultrafine particles are probably lubricating oil particles from the lawn mower exhaust; the larger particles are swirled-up plant debris particles from the mowing process. While these particle types were identified in the data from the two mass spectrometers, the on-line aerosol concentration and size distribution data support these findings. The results presented here show that the combination of quantitative aerosol particle ensemble mass spectrometry (ToF-AMS) and single particle mass spectrometry (ATOFMS) provides much deeper insights into the nature of the aerosol properties than each of the instruments could do alone. Therefore a combined deployment of both types of instruments is strongly recommended.

Role of engine age and lubricant chemistry on the characteristics of EGR soot

Science.gov (United States)

Adeniran, Olusanmi Adeniji

Exhaust products of Diesel Engines serves as an environmental hazard, and to curtail this problem a Tier 3 emission standard was introduced which involves change in engine designs and introduction of EGR systems in Diesel engines. EGR systems, however has the challenge of generating soot which are abrasive and are major causes of wear in Diesel engines. This work has studied the characteristics of EGR soot formed in different range of engine age and in different lubricant chemistries of Mineral and Synthetic based diesel Oils. It is found that lubricant degradation is encouraged by less efficient combustion as engine age increases, and these are precursors to formation of crystalline and amorphous particles that are causes of wear in Diesel Engines. It is found that soot from new engine is dominated by calcium based crystals which are from calcium sulfonate detergent, which reduces formation of second phase particles that can be abrasive. Diversity and peak intensity is seen to increase in soot samples as engine age increases. This understanding of second phase particles formed in engines across age ranges can help in the durability development of engine, improvement of Oil formulation for EGR engines, and in development of chemistries for after-treatment Oil solutions that can combat formation of abrasive particles in Oils.

Algorithm of Data Reduce in Determination of Aerosol Particle Size Distribution at Damps/C

International Nuclear Information System (INIS)

Muhammad-Priyatna; Otto-Pribadi-Ruslanto

2001-01-01

The analysis had to do for algorithm of data reduction on Damps/C (Differential Mobility Particle Sizer with Condensation Particle Counter) system, this is for determine aerosol particle size distribution with range 0,01 μm to 1 μm in diameter. Damps/C (Differential Mobility Particle Sizer with Condensation Particle Counter) system contents are software and hardware. The hardware used determine of mobilities of aerosol particle and so the software used determine aerosol particle size distribution in diameter. The mobilities and diameter particle had connection in the electricity field. That is basic program for reduction of data and particle size conversion from particle mobility become particle diameter. The analysis to get transfer function value, Ω, is 0.5. The data reduction program to do conversation mobility basis become diameter basis with number efficiency correction, transfer function value, and poly charge particle. (author)

AEROSOL PARTICLE COLLECTOR DESIGN STUDY

Energy Technology Data Exchange (ETDEWEB)

Lee, S; Richard Dimenna, R

2007-09-27

A computational evaluation of a particle collector design was performed to evaluate the behavior of aerosol particles in a fast flowing gas stream. The objective of the work was to improve the collection efficiency of the device while maintaining a minimum specified air throughput, nominal collector size, and minimal power requirements. The impact of a range of parameters was considered subject to constraints on gas flow rate, overall collector dimensions, and power limitations. Potential improvements were identified, some of which have already been implemented. Other more complex changes were identified and are described here for further consideration. In addition, fruitful areas for further study are proposed.

Inside versus Outside: Ion Redistribution in Nitric Acid Reacted Sea Spray Aerosol Particles as Determined by Single Particle Analysis (Invited)

Science.gov (United States)

Ault, A. P.; Guasco, T.; Ryder, O. S.; Baltrusaitis, J.; Cuadra-Rodriguez, L. A.; Collins, D. B.; Ruppel, M. J.; Bertram, T. H.; Prather, K. A.; Grassian, V. H.

2013-12-01

Sea spray aerosol (SSA) particles were generated under real-world conditions using natural seawater and a unique ocean-atmosphere facility equipped with actual breaking waves or a marine aerosol reference tank (MART) that replicates those conditions. The SSA particles were exposed to nitric acid in situ in a flow tube and the well-known chloride displacement and nitrate formation reaction was observed. However, as discussed here, little is known about how this anion displacement reaction affects the distribution of cations and other chemical constituents within and phase state of individual SSA particles. Single particle analysis of individual SSA particles shows that cations (Na+, K+, Mg2+ and Ca2+) within individual particles undergo a spatial redistribution after heterogeneous reaction with nitric acid, along with a more concentrated layer of organic matter at the surface of the particle. These data suggest that specific ion and aerosol pH effects play an important role in aerosol particle structure in ways that have not been previously recognized. The ordering of organic coatings can impact trace gas uptake, and subsequently impact trace gas budgets of O3 and NOx.

Measurements of phoretic velocities of aerosol particles in microgravity conditions

Science.gov (United States)

Prodi, F.; Santachiara, G.; Travaini, S.; Vedernikov, A.; Dubois, F.; Minetti, C.; Legros, J. C.

2006-11-01

Measurements of thermo- and diffusio-phoretic velocities of aerosol particles (carnauba wax, paraffin and sodium chloride) were performed in microgravity conditions (Drop Tower facility, in Bremen, and Parabolic Flights, in Bordeaux). In the case of thermophoresis, a temperature gradient was obtained by heating the upper plate of the cell, while the lower one was maintained at environmental temperature. For diffusiophoresis, the water vapour gradient was obtained with sintered plates imbued with a water solution of MgCl 2 and distilled water, at the top and at the bottom of the cell, respectively. Aerosol particles were observed through a digital holographic velocimeter, a device allowing the determination of 3-D coordinates of particles from the observed volume. Particle trajectories and consequently particle velocities were reconstructed through the analysis of the sequence of particle positions. The experimental values of reduced thermophoretic velocities are between the theoretical values of Yamamoto and Ishihara [Yamamoto, K., Ishihara, Y., 1988. Thermophoresis of a spherical particle in a rarefied gas of a transition regime. Phys. Fluids. 31, 3618-3624] and Talbot et al. [Talbot, L., Cheng, R.K., Schefer, R.W., Willis, D.R., 1980. Thermophoresis of particles in a heated boundary layer. J. Fluid Mech. 101, 737-758], and do not show a clear dependence on the thermal conductivity of the aerosol. The existence of negative thermophoresis is not confirmed in our experiments. Concerning diffusiophoretic experiments, the results obtained show a small increase of reduced diffusiophoretic velocity with the Knudsen number.

Simulation and analysis of the soot particle size distribution in a turbulent nonpremixed flame

KAUST Repository

Lucchesi, Marco; Abdelgadir, Ahmed Gamaleldin; Attili, Antonio; Bisetti, Fabrizio

2017-01-01

to the simulation of soot formation and growth in simplified configurations featuring a constant concentration of soot precursors and the evolution of the size distribution in time is found to depend on the intensity of the nucleation rate. Higher nucleation rates

Cavity Ring-Down Measurement of Aerosol Optical Properties During the Asian Dust Above Monterey Experiment and DOE Aerosol Intensive Operating Period

Science.gov (United States)

Ricci, K.; Strawa, A. W.; Provencal, R.; Castaneda, R.; Bucholtz, A.; Schmid, B.

2004-01-01

Large uncertainties in the effects of aerosols on climate require improved in-situ measurements of extinction coefficient and single-scattering albedo. This paper describes preliminary results from Cadenza, a new continuous wave cavity ring-down (CW-CRD) instrument designed to address these uncertainties. Cadenza measures the aerosol extinction coefficient for 675 nm and 1550 nm light, and simultaneously measures the scattering coefficient at 675 nm. In the past year Cadenza was deployed in the Asian Dust Above Monterey (ADAM) and DOE Aerosol Intensive Operating Period (IOP) field projects. During these flights Cadenza produced measurements of aerosol extinction in the range from 0.2 to 300/Mm with an estimated precision of 0.1/Mm for 1550 nm light and 0.2/Mm for 675 nm light. Cadenza data from the ADAM and Aerosol IOP missions compared favorably with data from the other instruments aboard the CIRPAS Twin Otter aircraft and participating in those projects. We present comparisons between the Cadenza measurements and those from a TSI nephelometer, Particle Soot Absorption Photometer (PSAP), and the AATS 14 sun-photometer. Measurements of the optical properties of smoke and dust plumes sampled during these campaigns are presented and estimates of heating rates due to these plumes are made.

A model study of aggregates composed of spherical soot monomers with an acentric carbon shell

Science.gov (United States)

Luo, Jie; Zhang, Yongming; Zhang, Qixing

2018-01-01

Influences of morphology on the optical properties of soot particles have gained increasing attentions. However, studies on the effect of the way primary particles are coated on the optical properties is few. Aimed to understand how the primary particles are coated affect the optical properties of soot particles, the coated soot particle was simulated using the acentric core-shell monomers model (ACM), which was generated by randomly moving the cores of concentric core-shell monomers (CCM) model. Single scattering properties of the CCM model with identical fractal parameters were calculated 50 times at first to evaluate the optical diversities of different realizations of fractal aggregates with identical parameters. The results show that optical diversities of different realizations for fractal aggregates with identical parameters cannot be eliminated by averaging over ten random realizations. To preserve the fractal characteristics, 10 realizations of each model were generated based on the identical 10 parent fractal aggregates, and then the results were averaged over each 10 realizations, respectively. The single scattering properties of all models were calculated using the numerically exact multiple-sphere T-matrix (MSTM) method. It is found that the single scattering properties of randomly coated soot particles calculated using the ACM model are extremely close to those using CCM model and homogeneous aggregate (HA) model using Maxwell-Garnett effective medium theory. Our results are different from previous studies. The reason may be that the differences in previous studies were caused by fractal characteristics but not models. Our findings indicate that how the individual primary particles are coated has little effect on the single scattering properties of soot particles with acentric core-shell monomers. This work provides a suggestion for scattering model simplification and model selection.

Soot Formation in Laminar Premixed Methane/Oxygen Flames at Atmospheric Pressure

Science.gov (United States)

Xu, F.; Lin, K.-C.; Faeth, G. M.

1998-01-01

Flame structure and soot formation were studied within soot-containing laminar premixed mc1hane/oxygen flames at atmospheric pressure. The following measurements were made: soot volume fractions by laser extinction, soot temperatures by multiline emission, gas temperatures (where soot was absent) by corrected fine-wire thermocouples, soot structure by thermophoretic sampling and transmission electron microscope (TEM), major gas species concentrations by sampling and gas chromatography, and gas velocities by laser velocimetry. Present measurements of gas species concentrations were in reasonably good agreement with earlier measurements due to Ramer et al. as well as predictions based on the detailed mechanisms of Frenklach and co-workers and Leung and Lindstedt: the predictions also suggest that H atom concentrations are in local thermodynamic equilibrium throughout the soot formation region. Using this information, it was found that measured soot surface growth rates could be correlated successfully by predictions based on the hydrogen-abstraction/carbon-addition (HACA) mechanisms of both Frenklach and co-workers and Colket and Hall, extending an earlier assessment of these mechanisms for premixed ethylene/air flames to conditions having larger H/C ratios and acetylene concentrations. Measured primary soot particle nucleation rates were somewhat lower than the earlier observations for laminar premixed ethylene/air flames and were significantly lower than corresponding rates in laminar diffusion flames. for reasons that still must be explained.

Aerosol vertical distribution, new particle formation, and jet aircraft particle emissions in the free troposhere and tropopause region; Vertikalverteilung und Neubildungsprozesse des Aerosols und partikelfoermige Flugzeugemissionen in der freien Troposphaere und Tropopausenregion

Energy Technology Data Exchange (ETDEWEB)

Schroeder, F P

2000-07-01

A contribution to the understanding of natural and anthropogenously induced particle formation as well as aerosol physical transformation processes within the free troposphere (FT) is introduced. Documentation and interpretation of empirical data relevant with respect to possible climatologic impact of anthropogenous aerosol emissions into the atmosphere is presented. The first section describes new technique for high spatial resolution measurements of ultrafine aerosol particles by condensation nucleus counters (CNCs), a necessary prerequisite for the observation of natural particle formation and jet aircraft emissions. The second section illustrates vertical distribution and variability ranges of the aerosol in the FT and the tropopause region (TP). Typical microphysical states of the atmospheric aerosol within the Northern Hemisphere are documented by means of systematic measurements during more than 60 flight missions. Simple mathematical parameterizations of the aerosol vertical distribution and aerosol size distributions are developed. Important aerosol sources within the FT are localized and possible aerosol formation processes are discussed. The third section is focussed on jet-engine particle emissions within the FT and TP. A unique inflight experiment for detection of extremely high concentrations (>10{sup 6} cm{sup -3}) of extremely small (donw to <3 nm) aerosols inside the exhaust plumes of several jet aircraft is described. Particle emission indices and emission-controlling parameters are deduced. Most important topic is the impact of fuel sulfur content of kerosine on number, size and chemical composition of jet particle emissions. Generalized results are parameterized in form of lognormal aerosol particle size distributions. (orig.) [German] Ein Beitrag zum Verstaendnis natuerlicher und anthropogen induzierter Aerosolneubildung sowie physikalischer Aerosolumwandlung in der freien Troposphaere wird vorgestellt. Empirisch gewonnenes Datenmaterial wird

Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation

Science.gov (United States)

Shiraiwa, Manabu; Yee, Lindsay D.; Schilling, Katherine A.; Loza, Christine L.; Craven, Jill S.; Zuend, Andreas; Ziemann, Paul J.; Seinfeld, John H.

2013-01-01

Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process. PMID:23818634

Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation.

Science.gov (United States)

Shiraiwa, Manabu; Yee, Lindsay D; Schilling, Katherine A; Loza, Christine L; Craven, Jill S; Zuend, Andreas; Ziemann, Paul J; Seinfeld, John H

2013-07-16

Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process.

Particle size distribution of aerosols sprayed from household hand-pump sprays containing fluorine-based and silicone-based compounds.

Science.gov (United States)

Kawakami, Tsuyoshi; Isama, Kazuo; Ikarashi, Yoshiaki

2015-01-01

Japan has published safety guideline on waterproof aerosol sprays. Furthermore, the Aerosol Industry Association of Japan has adopted voluntary regulations on waterproof aerosol sprays. Aerosol particles of diameter less than 10 µm are considered as "fine particles". In order to avoid acute lung injury, this size fraction should account for less than 0.6% of the sprayed aerosol particles. In contrast, the particle size distribution of aerosols released by hand-pump sprays containing fluorine-based or silicone-based compounds have not been investigated in Japan. Thus, the present study investigated the aerosol particle size distribution of 16 household hand-pump sprays. In 4 samples, the ratio of fine particles in aerosols exceeded 0.6%. This study confirmed that several hand-pump sprays available in the Japanese market can spray fine particles. Since the hand-pump sprays use water as a solvent and their ingredients may be more hydrophilic than those of aerosol sprays, the concepts related to the safety of aerosol-sprays do not apply to the hand pump sprays. Therefore, it may be required for the hand-pump spray to develop a suitable method for evaluating the toxicity and to establish the safety guideline.

Global Distribution of Solid Ammonium Sulfate Aerosols and their Climate Impact Acting as Ice Nuclei

Science.gov (United States)

Zhou, C.; Penner, J.

2017-12-01

Laboratory experiments show that liquid ammonium sulfate particles effloresce when RHw is below 34% to become solid and dissolve when RHw is above 79%. Solid ammonium sulfate aerosols can act as heterogeneous ice nuclei particles (INPs) to form ice particles in deposition mode when the relative humidity over ice is above 120%. In this study we used the coupled IMPACT/CAM5 model to track the efflorescence and deliquescence processes of ammonium sulfate. Results show that about 20% of the total simulated pure sulfate aerosol mass is in the solid state and is mainly distributed in the northern hemisphere (NH) from 50 hPa to 200 hPa. When these solid ammonium sulfate aerosols are allowed to act as ice nuclei particles, they act to increase the ice water path in the NH and reduce ice water path in the tropics. The addition of these particles leads to a positive net radiative effect at the TOA ranging from 0.5-0.9 W/m2 depending on the amounts of other ice nuclei particles (e.g., dust, soot) used in the ice nucleation process. The short-term climate feedback shows that the ITCZ shifts northwards and precipitation increases in the NH. There is also an average warming of 0.05-0.1 K near the surface (at 2 meter) in the NH which is most obvious in the Arctic region.

Reduced anthropogenic aerosol radiative forcing caused by biogenic new particle formation

Science.gov (United States)

Gordon, Hamish; Sengupta, Kamalika; Rap, Alexandru; Duplissy, Jonathan; Frege, Carla; Williamson, Christina; Heinritzi, Martin; Simon, Mario; Yan, Chao; Almeida, João; Tröstl, Jasmin; Nieminen, Tuomo; Ortega, Ismael K.; Wagner, Robert; Dunne, Eimear M.; Adamov, Alexey; Amorim, Antonio; Bernhammer, Anne-Kathrin; Bianchi, Federico; Breitenlechner, Martin; Brilke, Sophia; Chen, Xuemeng; Craven, Jill S.; Dias, Antonio; Ehrhart, Sebastian; Fischer, Lukas; Flagan, Richard C.; Franchin, Alessandro; Fuchs, Claudia; Guida, Roberto; Hakala, Jani; Hoyle, Christopher R.; Jokinen, Tuija; Junninen, Heikki; Kangasluoma, Juha; Kim, Jaeseok; Kirkby, Jasper; Krapf, Manuel; Kürten, Andreas; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mathot, Serge; Molteni, Ugo; Monks, Sarah A.; Onnela, Antti; Peräkylä, Otso; Piel, Felix; Petäjä, Tuukka; Praplan, Arnaud P.; Pringle, Kirsty J.; Richards, Nigel A. D.; Rissanen, Matti P.; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Scott, Catherine E.; Seinfeld, John H.; Sharma, Sangeeta; Sipilä, Mikko; Steiner, Gerhard; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Virtanen, Annele; Vogel, Alexander Lucas; Wagner, Andrea C.; Wagner, Paul E.; Weingartner, Ernest; Wimmer, Daniela; Winkler, Paul M.; Ye, Penglin; Zhang, Xuan; Hansel, Armin; Dommen, Josef; Donahue, Neil M.; Worsnop, Douglas R.; Baltensperger, Urs; Kulmala, Markku; Curtius, Joachim; Carslaw, Kenneth S.

2016-10-01

The magnitude of aerosol radiative forcing caused by anthropogenic emissions depends on the baseline state of the atmosphere under pristine preindustrial conditions. Measurements show that particle formation in atmospheric conditions can occur solely from biogenic vapors. Here, we evaluate the potential effect of this source of particles on preindustrial cloud condensation nuclei (CCN) concentrations and aerosol-cloud radiative forcing over the industrial period. Model simulations show that the pure biogenic particle formation mechanism has a much larger relative effect on CCN concentrations in the preindustrial atmosphere than in the present atmosphere because of the lower aerosol concentrations. Consequently, preindustrial cloud albedo is increased more than under present day conditions, and therefore the cooling forcing of anthropogenic aerosols is reduced. The mechanism increases CCN concentrations by 20-100% over a large fraction of the preindustrial lower atmosphere, and the magnitude of annual global mean radiative forcing caused by changes of cloud albedo since 1750 is reduced by 0.22 W m-2 (27%) to -0.60 W m-2. Model uncertainties, relatively slow formation rates, and limited available ambient measurements make it difficult to establish the significance of a mechanism that has its dominant effect under preindustrial conditions. Our simulations predict more particle formation in the Amazon than is observed. However, the first observation of pure organic nucleation has now been reported for the free troposphere. Given the potentially significant effect on anthropogenic forcing, effort should be made to better understand such naturally driven aerosol processes.

Reduced anthropogenic aerosol radiative forcing caused by biogenic new particle formation.

Science.gov (United States)

Gordon, Hamish; Sengupta, Kamalika; Rap, Alexandru; Duplissy, Jonathan; Frege, Carla; Williamson, Christina; Heinritzi, Martin; Simon, Mario; Yan, Chao; Almeida, João; Tröstl, Jasmin; Nieminen, Tuomo; Ortega, Ismael K; Wagner, Robert; Dunne, Eimear M; Adamov, Alexey; Amorim, Antonio; Bernhammer, Anne-Kathrin; Bianchi, Federico; Breitenlechner, Martin; Brilke, Sophia; Chen, Xuemeng; Craven, Jill S; Dias, Antonio; Ehrhart, Sebastian; Fischer, Lukas; Flagan, Richard C; Franchin, Alessandro; Fuchs, Claudia; Guida, Roberto; Hakala, Jani; Hoyle, Christopher R; Jokinen, Tuija; Junninen, Heikki; Kangasluoma, Juha; Kim, Jaeseok; Kirkby, Jasper; Krapf, Manuel; Kürten, Andreas; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mathot, Serge; Molteni, Ugo; Monks, Sarah A; Onnela, Antti; Peräkylä, Otso; Piel, Felix; Petäjä, Tuukka; Praplan, Arnaud P; Pringle, Kirsty J; Richards, Nigel A D; Rissanen, Matti P; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Scott, Catherine E; Seinfeld, John H; Sharma, Sangeeta; Sipilä, Mikko; Steiner, Gerhard; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Virtanen, Annele; Vogel, Alexander Lucas; Wagner, Andrea C; Wagner, Paul E; Weingartner, Ernest; Wimmer, Daniela; Winkler, Paul M; Ye, Penglin; Zhang, Xuan; Hansel, Armin; Dommen, Josef; Donahue, Neil M; Worsnop, Douglas R; Baltensperger, Urs; Kulmala, Markku; Curtius, Joachim; Carslaw, Kenneth S

2016-10-25

The magnitude of aerosol radiative forcing caused by anthropogenic emissions depends on the baseline state of the atmosphere under pristine preindustrial conditions. Measurements show that particle formation in atmospheric conditions can occur solely from biogenic vapors. Here, we evaluate the potential effect of this source of particles on preindustrial cloud condensation nuclei (CCN) concentrations and aerosol-cloud radiative forcing over the industrial period. Model simulations show that the pure biogenic particle formation mechanism has a much larger relative effect on CCN concentrations in the preindustrial atmosphere than in the present atmosphere because of the lower aerosol concentrations. Consequently, preindustrial cloud albedo is increased more than under present day conditions, and therefore the cooling forcing of anthropogenic aerosols is reduced. The mechanism increases CCN concentrations by 20-100% over a large fraction of the preindustrial lower atmosphere, and the magnitude of annual global mean radiative forcing caused by changes of cloud albedo since 1750 is reduced by [Formula: see text] (27%) to [Formula: see text] Model uncertainties, relatively slow formation rates, and limited available ambient measurements make it difficult to establish the significance of a mechanism that has its dominant effect under preindustrial conditions. Our simulations predict more particle formation in the Amazon than is observed. However, the first observation of pure organic nucleation has now been reported for the free troposphere. Given the potentially significant effect on anthropogenic forcing, effort should be made to better understand such naturally driven aerosol processes.

The physico-chemical evolution of atmospheric aerosols and the gas-particle partitioning of inorganic aerosol during KORUS-AQ

Science.gov (United States)

Lee, T.; Park, T.; Lee, J. B.; Lim, Y. J.; Ahn, J.; Park, J. S.; Soo, C. J.; Desyaterik, Y.; Collett, J. L., Jr.

2017-12-01

Aerosols influence climate change directly by scattering and absorption and indirectly by acting as cloud condensation nuclei and some of the effects of aerosols are reduction in visibility, deterioration of human health, and deposition of pollutants to ecosystems. Urban area is large source of aerosols and aerosol precursors. Aerosol sources are both local and from long-range transport. Long-range transport processed aerosol are often dominant sources of aerosol pollution in Korea. To improve our knowledge of aerosol chemistry, Korea and U.S-Air Quality (KORUS-AQ) of Aircraft-based aerosol measurement took place in and around Seoul, Korea during May and June 2016. KORUS-AQ campaigns were conducted to study the chemical characterization and processes of pollutants in the Seoul Metropolitan area to regional scales of Korean peninsula. Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed on aircraft platforms on-board DC-8 (NASA) aircraft. We characterized aerosol chemical properties and mass concentrations of sulfate, nitrate, ammonium and organics in polluted air plumes and investigate the spatial and vertical distribution of the species. The results of studies show that organics is predominant in Aerosol and a significant fraction of the organics is oxygenated organic aerosol (OOA) at the high altitude. Both Nitrate and sulfate can partition between the gas and particle phases. The ratios for HNO3/(N(V) (=gaseous HNO3 + particulate Nitrate) and SO2/(SO2+Sulfate) were found to exhibit quite different distributions between the particles and gas phase for the locations during KORUS-AQ campaign, representing potential for formation of additional particulate nitrate and sulfate. The results of those studies can provide highly resolved temporal and spatial air pollutant, which are valuable for air quality model input parameters for aerosol behaviour.

Volatile release and particle formation characteristics of injected pulverized coal in blast furnaces

International Nuclear Information System (INIS)

Chen, Wei-Hsin; Du, Shan-Wen; Yang, Tsung-Han

2007-01-01

Volatiles release and particle formation for two kinds of pulverized coals (a high volatile bituminous coal and a low volatile bituminous coal) in a drop tube furnace are investigated to account for the reactions of pulverized coal injected in blast furnaces. Two different sizes of feed particles are considered; one is 100-200 mesh and the other is 200-325 mesh. By evaluating the R-factor, the devolatilization extent of the larger feed particles is found to be relatively poor. However, the swelling behavior of individual or two agglomerated particles is pronounced, which is conducive to gasification of the chars in blast furnaces. In contrast, for the smaller feed particles, volatiles liberated from the coal particles can be improved in a significant way as a result of the amplified R-factor. This enhancement can facilitate the performance of gas phase combustion. Nevertheless, the residual char particles are characterized by agglomeration, implying that the reaction time of the char particles will be lengthened, thereby increasing the possibility of furnace instability. Double peak distributions in char particle size are observed in some cases. This possibly results from the interaction of the plastic state and the blowing effect at the particle surface. Considering the generation of tiny aerosols composed of soot particles and tar droplets, the results indicate that their production is highly sensitive to the volatile matter and elemental oxygen contained in the coal. Comparing the reactivity of the soot to that of the unburned char, the former is always lower than the latter. Consequently, the lower is the soot formation, the better is the blast furnace stability

Aerosol Particle Interfacial Thermodynamics and Phase Partitioning Measurements Using Biphasic Microfluidics

Science.gov (United States)

Dutcher, Cari; Metcalf, Andrew

2015-03-01

Secondary organic aerosol particles are nearly ubiquitous in the atmosphere and yet there remain large uncertainties in their formation processes and ambient properties. These particles are complex microenvironments, which can contain multiple interfaces due to internal aqueous-organic phase partitioning and to the external liquid-vapor surface. Interfacial properties affect the ambient aerosol morphology, or internal structure of the particle, which in turn can affect the way a particle interacts with an environment of condensable clusters and organic vapors. To improve our ability to accurately predict ambient aerosol morphology, we must improve our knowledge of aerosol interfaces and their interactions with the ambient environment. Unfortunately, many techniques employed to measure interfacial properties do so in bulk solutions or in the presence of a ternary (e.g. solid) phase. In this talk, a novel method using biphasic microscale flows will be introduced for generating, trapping, and perturbing complex interfaces at atmospherically relevant conditions. These microfluidic experiments utilize high-speed imaging to monitor interfacial phenomena at the microscale and are performed with phase contrast and fluorescence microscopy on a temperature-controlled inverted microscope stage. From these experiments, interfacial thermodynamic properties such as surface or interfacial tension, rheological properties such as interfacial moduli, and kinetic properties such as mass transfer coefficients can be measured or inferred.

Soot measurements by two angle scattering and extinction in an N 2 -diluted ethylene/air counterflow diffusion flame from 2 to 5 atm

KAUST Repository

Amin, Hafiz M.F.

2016-06-27

The soot formed in an N-diluted ethylene/air counterflow diffusion flame at elevated pressure was investigated using two angle light scattering/extinction technique. To provide a well-controlled pressurized environment for the flame, a novel pressure vessel was built with the required optical access. The soot parameters were measured along the centerline of the counterflow flame. These properties included soot volume fraction (f ), primary particle diameter (d ), population averaged radius of gyration (R ) and number density of primary particles (n ). The Rayleigh-Debye-Gans theory for Fractal Aggregates (RDG-FA) was used to retrieve these properties from scattering and extinction measurements. Soot volume fraction was measured via light extinction from 2 to 5atm while maintaining the same global strain rate at all pressures. Scattered light from soot particles was measured at 45° and 135° and primary particle diameter was calculated using scattering/extinction ratio and the radius of gyration was determined from the dissymmetry ratio. Soot volume fraction, primary particle diameter and radius of gyration all increased with pressure while the number density of primary particles decreased with increasing pressure.