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PubMed2001

Modeling aerosol formation from alpha-pinene + NOx in the presence of natural sunlight using gas-phase kinetics and gas-particle partitioning theory.

A kinetic mechanism was used to link and model the gas-phase reactions and aerosol accumulation resulting from alpha-pinene reactions in the presence of sunlight, ozone (O3), and oxides of nitrogen (NOx). Reaction products and aerosol formation from the kinetic model were compared to outdoor smog chamber experiments conducted under natural sunlight in the presence of NOx and in the dark in the presence of O3. The gas-particle partitioning of semivolatile organics generated in the gas phase was treated as an equilibrium process between particle absorption and desorption. Models vs experimental aerosol yields illustrate that reasonable predictions of secondary aerosol formation are possible from both dark ozone and light NOx/alpha-pinene systems over a variety of different outdoor conditions. On average, measured gas- and particle-phase products accounted for approximately 54-72% of the reacted alpha-pinene carbon. Model predictions suggest that organic nitrates account for another approximately 25% of the reacted carbon, and most of this is in the gas phase. Measured particle-phase products accounted for 60-100% of the particle filter mass, with pinic acid and pinonic acid being the primary aerosol-phase products. In the gas phase, pinonaldehyde and pinonic acid are major products. Model simulations of these and other products show generally reasonable fits to the experimental data from the perspective of timing and concentrations. These results are very encouraging for a compound such as pinonaldehyde, since it is being formed from OH attack on alpha-pinene and is also simultaneously photolyzed and reacted with OH.

Aerosols↗
PubMed2001

Enhanced effect of in-situ generated ammonium salts aerosols on the removal of NOx from simulated flue gas.

The combined removal of sulfur dioxide (SO2, up to 3,000 ppm) and nitrogen oxides (NO and NO2, up to 1,200 ppm) has been investigated in a bench-scale pulsed-corona enhanced wet electrostatic precipitator (wESP) with the optional injection of ammonia and/or ozone. The reaction of ammonia with SO2 produces submicron aerosols under certain conditions. Experiments have shown the feasibility of combined SO2 and NOx removal from simulated flue gases by the action of these in-situ generated aerosols. The mechanisms for NOx removal include oxidation of NO to NO2 and subsequent absorption of NO2 into the water wall of the wESP. The results have shown that injecting NH3 (NH3/NOx molar ratio 1) resulted in NOx removal of approximately 13% in a simulated combustion flue gas. Injecting 200 ppm ozone (no ammonia) increased NO conversion to 35% by oxidation, but total NOx removal increased to only 17%. Without the formation of ammonium salts aerosols (e.g., without SO2 in the gas), co-injection of ammonia and ozone increased NO conversion to 60% and NOx removal to 40%. However, high NOx removals were measured in simulated flue gas that contained NH3, SO2, and ozone. The total NOx removal efficiency was 79% when the ammonium salts aerosols were formed in the presence of 2400 ppm SO2, 312 ppm O3, and 2,900 ppm NH3. The energy efficiency of collection improved by approximately 250% for SO2 removal and more than 4700% for NOx removal under these conditions. It was determined that the ammonium salts aerosols produced from the reaction of ammonia and sulfur dioxide substantially enhanced total NOx removal.

Absorption↗
PubMed2002

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

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.

Aerosols↗
PubMed2005

Identification and quantification of aerosol polar oxygenated compounds bearing carboxylic or hydroxyl groups. 2. Organic tracer compounds from monoterpenes.

In this study, a comparison is made of polar organic compounds found in the field with those produced in secondary organic aerosol from laboratory irradiations of natural hydrocarbons and oxides of nitrogen (NOx). The field samples comprised atmospheric particulate matter (PM2.5) collected at Research Triangle Park (RTP), NC, during the summer of 2003, and the laboratory samples originated from the photooxidation of the following monoterpenes: alpha-pinene, beta-pinene, and d-limonene. To determine the structural characteristics of the polar compounds, the filter samples were solvent extracted and derivatized using a technique based on single and multistep derivatizations. The resulting compound derivatives were analyzed by GC-MS in the methane-Cl and El modes. In addition to previously reported biogenic oxidation products (pinic acid, pinonic acid, norpinic acid, nopinone, and pinonaldehyde), seven multifunctional organic compounds were found in both field and laboratory samples. These compounds, which are proposed as possible atmospheric tracers for secondary organic aerosol from monoterpenes, were consistent with the following identifications: 3-isopropyl pentanedioic acid; 3-acetyl pentanedioic acid; 3-carboxy heptanedioic acid; 3-acetyl hexanedioic acid; 2-isopropyl-1,2-dihydroxybutanol; 4-isopropyl-2,4-dihydroxyhexanol; and 3-(2-hydroxy-ethyl)-2,2-dimethyl-cyclobutane carboxylic acid. Initial attempts have been made to quantify the concentrations of these tracer compounds on the basis of surrogate compound calibrations. The occurrence of these compounds in both laboratory and field measurements suggests that secondary organic aerosol originating from biogenic hydrocarbons are contributing to the regional aerosol burden in the southeastern United States. Several of these compounds also appear to contribute to the global aerosol burden in that they have also been identified in Europe and Brazil.

Aerosols↗
PubMed2005

Aerosol transport in the California Central Valley observed by airborne lidar.

An aerosol lidar system was deployed on the NASA DC-8 and used to measure aerosol vertical profiles in the California Central Valley. The nadir-pointing Nd:YAG lidar operated at 532 and 1064 nm at 20 Hz. The resulting aerosol profiles were plotted in a unique three-dimensional format that allowed the visual observation of the aerosol scattering ratio profiles, the valley topography, and corresponding backward trajectory air masses. The accumulation of aerosols from the Bakersfield area can be seen in the southern end of the valley due to topography and prevailing winds.

Aerosols↗
PubMed2004

Surfactants in atmospheric aerosols.

The concentration and characteristics of anionic and cationic aerosol surfactants at a range of locations were determined as methylene blue active substances (MBAS) and ethyl violet active substances (EVAS) for anionic surfactants and as disulfine blue active substances (DBAS) for the cationic surfactants. Results showed that the anionic surfactants (in the pmol m(-3) range) dominated the concentration of surfactant in atmospheric aerosols. The concentration of both MBAS and EVAS is typically higher on the finer aerosol fractions. Further study on the aerosols found both MBAS and EVAS had the ability to reduce the surface tension of aqueous extracts of the aerosol. MBAS were more readily destroyed on exposure to a high intensity of UV light than were EVAS. The source of these seemingly ubiquitous compounds is not clear, but we note that anionic surfactants are easily derived from degraded or oxidized soots, especially that from diesel engines.

Aerosols↗
PubMed2005

Sorption of a diverse set of organic vapors to urban aerosols.

Sorption to urban aerosols is a key process in determining the transport and fate of organic pollutants in the atmosphere. The sorption properties of two urban aerosol samples have been determined using aerosol/air partition coefficients measured for a large set of diverse organic vapors. The dominant sorption process could be identified for both samples with two complementary methods: (a) by applying poly-parameter linear free energy relationships (LFERs) to the data sets, and (b) by evaluating the specific surface area, the elemental carbon (EC) content, and the organic matter (OM) content of the aerosols in combination with various sorbent-air partition coefficients from the literature. This revealed that sorption to the two urban aerosols was dominated by absorption into OM and that the diverse data set could be evaluated with an absorption model. The data further revealed that neither EC nor OM was fully available for sorption. The latter leads to the hypothesis that aerosol OM in urban samples has characteristics comparable to those of glassy polymers.

Adsorption↗
PubMed2005

Simultaneous determination of mono- and dicarboxylic acids, omega-Oxo-carboxylic acids, midchain ketocarboxylic acids, and aldehydes in atmospheric aerosol samples.

This paper describes a method for the simultaneous determination of monocarboxylic acids (C6-C34), dicarboxylic acids (C2-C24), omega-oxo-carboxylic acids (C2-C9), ketocarboxylic acids (pyruvic and pinonic acid), and select aldehydes (glyoxal, methylglyoxal, and nonanal) in atmospheric particles. Quantification of these compounds gives information on important chemical characteristics of aerosols for source apportioning of aerosol organics and for studying atmospheric processes leading to secondary organic aerosol formation. These target analytes were determined as their butyl ester or butyl acetal derivatives using gas-chromatography mass spectrometry. The method is modified from a method described by Kawamura. Kawamura's original method involved a water extraction step, which practically restricted the method to the determination of only those compounds that are water-soluble. Our method eliminates the water extraction step and combines extraction and derivatization of the target compounds in one step. A mixture of hexane/butanol/BF3 simultaneously derivatizes the polar function groups (i.e., -COOH, -C=O) and extracts the target analytes from the aerosol filter substrates. A prominent advantage of our method is improved recoveries for the more volatile analytes in the target compound classes as a result of eliminating the water evaporation step. Recoveries better than 66% were obtained for the target analytes, including the relatively volatile ones. This improvement for the light species has allowed detection of a new midchain ketocarboxylic acid, 4-oxopentanoic acid, which would have escaped detection by the Kawamura method because of its high susceptibility to evaporative loss. Examples are presented to demonstrate the use of this method in analysis of ambient aerosol samples.

Aerosols↗
PubMed2005

Molecular characteristics of urban organic aerosols from Nanjing: a case study of A mega-city in China.

Over 90 organic species have been determined in fine aerosols (PM2.5) collected during the summer and winter in Nanjing, a typical mega-city in China, using gas chromatography-mass spectrometry. The organic compounds detected were apportioned to four emission sources (i.e., plant emission, fossil fuel combustion, biomass burning, and soil resuspension) and secondary oxidation products. The most abundant classes of compounds are fatty acids, followed by sugars, dicarboxylic acids excluding oxalic and malonic acids, and n-alkanes, while alcohols, polyols/polyacids and lignin/sterols are less abundant. Total amounts of the seven classes of compounds were on average 938 ng m(-3) in the summer and 1301 ng m(-3) in the winter, respectively, contributing 0.26-1.96% of particle mass (PM2.5). In the summer, n-alkanes were heavily enhanced by vegetation emissions with a maximum carbon number (Cmax) at C29, whereas they were dominated by emissions from fossil fuels combustion with a Cmax at C22/ C23 in the winter. Concentrations of unsaturated fatty acids were lower in the summer than in the winter, being consistent with enhanced photooxidation of unsaturated fatty acids in the summer. Concentrations of dicarboxylic acids for the summer aerosols were much higher in the daytime than in the nighttime, indicating increased photochemical production in the daytime. In the summer, plant emissions were the most significant source of organic aerosols, contributing more than 33% of total compound mass (TCM), followed by fossil fuel combustion or secondary oxidation. In contrast, fossil fuel combustion was the dominant source of winter organic aerosols, contributing more than 51% of TCM, followed by plant emissions and secondary oxidation products. The quantitative results on sugars and lignin pyrolysis products further suggested that biomass burning and soil resuspension are also significant sources of urban organic aerosols.

Aerosols↗
PubMed2006

Characterization of water-soluble organic carbon in urban atmospheric aerosols using solid-state 13C NMR spectroscopy.

Solid-state 13C nuclear magnetic resonance (NMR) spectroscopy has been used to investigate the distribution of carbon functional groups in urban Atlanta aerosol fine (PM2.5) particles. Carbonaceous aerosol particles comprise a significant fraction of the ambient particle mass and are environmentally significant as they may influence radiative and cloud-nucleating properties and can also produce adverse health effects upon inhalation. The water-soluble organic carbon (WSOC) fraction was extracted from multiple 24 h integrated high-volume quartz filter samples and further separated into recovered hydrophobic and hydrophilic fractions using an approach similar to that used to extract humic and fulvic acids from aqueous samples. Solid-state 13C NMR results indicate that WSOC in urban atmospheric aerosol particles is mostly aliphatic in nature (approximately 95% by C mass) with major contributions from alkyl and oxygenated alkyls (approximately 80%), carboxylic acid (approximately 10%), and aromatic functional groups (approximately 4%). The aromatic C is associated with the recovered hydrophobic fraction of WSOC. These spectra have been compared to the 13C NMR results obtained from Suwannee River humic acid and a fractionated biomass burning sample. WSOC, and more importantly, its recovered hydrophobic fraction, is found to be only qualitatively similar to aqueous humic material. The biomass burning sample is significantly different from urban Atlanta WSOC and is composed of substantial amounts of sugar derivatives and phenolic compounds, as expected. The NMR results demonstrate the potential of this technique to investigate aerosol WSOC composition and to study its variations with changes in parameters such aerosol sources.

Aerosols↗
PubMed2006

Molecular size evolution of oligomers in organic aerosols collected in urban atmospheres and generated in a smog chamber.

Only a minor fraction of the total organic aerosol mass can be resolved on a molecular level. High molecular weight compounds in organic aerosols have recently gained much attention because this class of compound potentially explains a major fraction of the unexplained organic aerosol mass. These compounds have been identified with different mass spectrometric methods, and compounds with molecular masses up to 1000 Da are found in secondary organic aerosols (SOA) generated from aromatic and terpene precursors in smog chamber experiments. Here, we apply matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS) to SOA particles from two biogenic precursors, alpha-pinene and isoprene. Similar oligomer patterns are found in these two SOA systems, but also in SOA from trimethylbenzene, an anthropogenic SOA precursor. However, different maxima molecular sizes were measured for these three SOA systems. While oligomers in alpha-pinene and isoprene have sizes mostly below 600-700 Da, they grow up to about 1000 Da in trimethylbenzene-SOA. The final molecular size of the oligomers is reached early during the particle aging process, whereas other particle properties related to aging, such as the overall acid concentration or the oligomer concentration, increase continuously over a much longer time scale. This kinetic behavior of the oligomer molecular size growth can be explained by a chain growth kinetic regime. Similar oligomer mass patterns were measured in aqueous extracts of ambient aerosol samples (measured with the same technique). Distinct differences between summer and winter were observed. In summer a few single mass peaks were measured with much higher intensity than in winter, pointing to a possible difference in the formation processes of these compounds in winter and summer.

Aerosols↗
PubMed2001

Photodegradation of nitro-PAHs in viscous organic media used as models of organic aerosols.

Many types of organic aerosol material have been found to behave as viscous liquids. In the current work, photodegradation of selected nitrated polycyclic aromatic compounds, 1-nitropyrene and 3-nitrofluoranthene, in viscous organic phases used as model systems for organic aerosols has been investigated. Experiments have been conducted in the presence and absence of anthraquinone, an atmospherically relevant photochemical radical sensitizer. The photodegradation of nitro-PAH is strongly accelerated by the presence of anthraquinone, and a viscous medium does not inhibit the photoinduced decay of nitro-PAH. In fact, the effect of anthraquinone is more pronounced in a viscous solvent containing tertiary hydrogen, DOP, compared to cyclohexane, a nonviscous solvent. This is related to a faster decay of anthraquinone in DOP and hence, presumably, a higher radical yield in DOP. The nitro-PAH degradation in DOP is faster at higher temperature; an observation primarily ascribed to faster diffusion at higher temperature giving rise to more efficient radical formation. In glycerine, a polar viscous solvent, significant formation of amino-PAH occurs due to photoreduction of the nitro-PAH. This is also the case in N2-purged guaiacol, a model substance for wood smoke organic material. Nitro-PAH photoreduction is enabled by the presence of hydrogen-atom donors and low levels of dissolved O2. A simple approach to estimate the O2 concentration in atmospheric organic aerosol material is presented. Low levels of O2 are predicted for wood smoke and secondary organic aerosol making amino-PAH formation in this aerosol material an interesting possibility.

Aerosols↗
PubMed1997

Disposition of aerosolized liposomal amphotericin B.

Amphotericin B (AmB) is an important drug for the treatment of fungal infection, but toxicity limits the lung tissue doses which may be achieved through intravenous administration. Although incorporation of AmB in liposomes reduces these effects and increases the therapeutic index for intravenous administration, targeted delivery to lung tissues via inhaled liposomal AmB aerosol may be a more effective approach. Aerosolization of liposomal amphotericin B targets the lungs, the organs first infested by many fungi. Development of optimal aerosolized liposomal AmB therapies requires a better understanding of the effect that liposome surface charge has on lung clearance kinetics. In this work we evaluated the clearance kinetics and organ distribution of inhaled liposomal AmB in male Balb/C mice. Mice were exposed via nose only to AmB-containing liposomal aerosols having positive, negative, or neutral surface charge characteristics. The formulations were aerosolized using a Collison nebulizer. Groups of animals were euthanized at predetermined times and the lungs and other organs were analyzed for AmB. AmB was not detected in serum and other organs such as kidneys, liver, and brain. The disposition of neutral and positive liposomal amphotericin B in lungs followed biexponential kinetics. The alpha and beta phase half-lives for positive liposomes were 1.3 and 15.1 days, respectively, and 2.3 and 22 days for neutral liposomes. AmB delivered via negative liposomes exhibited monoexponential clearance with a half-life of 4.5 days. These results suggest that toxic side effects in nontarget tissues are minimal and may indicate a potential for long term protection against fungal infections.

Aerosols↗
PubMed2001

Distribution of polycyclic aromatic hydrocarbons in aerosols and dustfall in Macao.

Polycyclic aromatic hydrocarbons (PAHs), widespread environmental pollutants, have been measured in aerosols and dustfall in Macao. In this paper, we compare concentration distributions and determine the partitioning of PAHs in aerosols and dustfall for different areas, sampling times and sampling heights. The results demonstrate that the concentrations of sigmaPAHs in aerosols and dustfall vary at the different sites and heights. The concentrations of sigmaPAHs and most of the individual PAHs in aerosols at night were higher than those in the daytime when using the unit of microg/g and lower than those when using the unit of microg m(-3). It is shown that the distribution of individual PAHs in aerosols differs significantly from that in dustfall.

Aerosols↗
PubMed1992

The pharmacokinetics of pulmonary-delivered insulin: a comparison of intratracheal and aerosol administration to the rabbit.

The pulmonary deposition and pharmacokinetics of insulin, administered via an endotracheal tube as an aerosol and instillate, in formulations containing either 113mIn-DTPA or 99mTc-DTPA (for gamma scintigraphic imaging) have been studied in four male New Zealand White rabbits. Using a randomized crossover design, the pharmacokinetics of intravenous insulin were also characterized. Recovery of immunoreactive insulin after nebulization was greater than 90%, indicating that the aerosolisation procedure did not cause appreciable insulin degradation. Gamma scintigraphy demonstrated that the penetration index (peripheral:central deposition) for the aerosolized formulation (1.52) was much greater than that for the instillate (0.32). Gamma scintigraphy also allowed exact quantification of the dose deposited after aerosol administration and thus permitted accurate determination of bioavailabilities. The bioavailable fraction for aerosolized insulin was 10-fold greater than for instilled insulin (57.2 vs 5.6%). Mucociliary clearance was likely to be greater for the instillate since it showed a preferential central deposition; this may account for the lower bioavailability. Insulin pharmacokinetics from both pulmonary formulations were absorption rate limited, resulting in postpeak half-lives which were approximately 20-fold greater than the intravenous elimination half-life (3 min). The apparent absorption rate constants resulting from instillation and aerosolisation were statistically equivalent (0.015 and 0.011 min-1, respectively). Mucociliary clearance of insulin would result in an overestimation of the true absorption rate constant; hence if mucociliary transport were greater for the instillate, then the true airways to blood transfer rate constant will be higher for the aerosolized formulation.

Aerosols↗
PubMed2002

Artificial neural network prediction of aerosol deposition in human lungs.

PURPOSE: To develop a rapid and reliable method for predicting the pattern of aerosol particle deposition within the human lungs, using artificial neural networks (ANNs). METHODS: Experimental data from the literature were used to train multi-layer perceptron (MLP) networks to allow for prediction of regional and total aerosol particle deposition patterns in human lungs. These data covered particle sizes in the range 0.05-15 microm and three different breathing patterns (ranging from "quiet" breathing to breathing "under physical work conditions"). Three different MLPs were trained, to provide separate predictions of aerosol particle deposition in the laryngeal, bronchial, and alveolar regions. The total deposition fraction for a given set of breathing conditions was computed simply as the sum of the outputs produced from the corresponding regional deposition MLPs. RESULTS: The ANNs developed are shown to give highly accurate predictions for both regional and total aerosol deposition patterns for all particle sizes and breathing conditions (with errors typically less than 0.04%). CONCLUSIONS: We conclude that the current set of ANNs can be used to give good predictions of particle deposition from polydisperse pharmaceutical aerosols generated from breath-actuated dry powder inhalers, nebulizers, and metered dose inhalers with spacers.

Aerosols↗
PubMed1987

Concepts for collection of aerosols in Titan's atmosphere.

In this paper we consider design of instruments for collection of aerosols during entry in Titan's atmosphere. Major constraints on designs are small sample collection time, low aerosol column density, and the need to collect 1-10 micrograms of aerosol for gas chromatographic analysis. Thus it is important to maximize aerosol collection through collector design, which includes consideration of various types of collectors and maximizing the collection efficiency of a given type of collector. Sampling systems discussed include inertial impactors, filters, electrostatic devices, and multistage instruments. Aerosol sampling is reviewed in the context of high-altitude (200-70 km) and low-altitude (60-30 km) regions of Titan's atmosphere.

Aerosols↗
PubMed2002

Bronchial challenges with aerosolized food in asthmatic, food-allergic children.

BACKGROUND: Allergic asthma is usually considered to be provoked by aeroallergens. However, we have recently recognized a group of children with food allergies who also develop asthma when exposed to the aerosolized form of the food. METHODS: Between 1997 and 1999 we prospectively identified children with an immunoglobulin (Ig)E-mediated food allergy who develop asthma on inhalational exposure to the relevant food allergen while it is being cooked. Subjects were exposed for 20 min to the aerosolized form of the allergen and the symptoms and the lung function were monitored. Aerosolization was achieved by cooking the food in a small room. Where possible challenges were double-blinded. RESULTS: We identified 12 children with an IgE-mediated food allergy who developed asthma on inhalational exposure to food. The implicated foods were fish, chickpea, milk, egg or buckwheat. Nine out of the 12 children consented to undergo a bronchial food challenge. Five challenges were positive with objective clinical features of asthma. Additionally, two children developed late-phase symptoms with a decrease in lung function. Positive reactions were seen with fish, chickpea and buckwheat. There were no reactions to the seven placebo challenges. CONCLUSIONS: We have presented a prospective series of children with food allergy who developed symptoms of asthma with exposure to aerosolized food allergens. Our data demonstrates that, as in the case of other aeroallergens, inhaled food allergens can produce both early- and late-phase asthmatic responses. This highlights the importance of considering foods as aeroallergens in children with coexistent food allergy and allergic asthma. For these children, dietary avoidance alone may not be sufficient and further environmental measures may be required to limit exposure to aerosolized food.

Aerosols↗