从气溶胶微物理属性分析冬季重庆地区霾的垂直分布特征

采用2007~2011年冬季(12月~次年2月)CALIPSO星载激光雷达L1监测数据,通过分析532 nm总后向散射系数、体积退偏比和色比,对重庆地区冬季霾期间气溶胶光学和微物理特性的垂直分布进行了研究。结果表明:重庆地区冬季霾期间,大气散射能力随高度减弱,在0~1 km高度最强;各高度层气溶胶粒子规则性与粒径大小的分布情况与全年总体分布情况基本相同,但变化趋势单调性更强,0~1 km高度层规则的、大颗粒气溶胶所占比例最大,3~4 km高度不规则的、小颗粒气溶胶所占比例最大;年际变化上,气溶胶散射强度逐年增强,其中2008~2010年变化较小,2011年明显增强;各年均以规则的、小颗粒气溶胶为主,2011年不规则气溶胶所占比例最大,而大颗粒气溶胶所占比例逐年增大。     

Aerosol filtration by a cocurrent moving granular bed: Penetration mechanisms

An experimental apparatus has been constructed to investigate aerosol filtration by a cocurrent moving granular bed filter (CMGBF). In a CMGBF, aerosol passes downward through a descending bed of dirty granules while clean granules are added continously at the bed top. The effect of an intergranular dust deposit on penetration in a CMGBF was investigated in a 2⁴ factorial experiment in which the control variables were superficial gas velocity (100 and 250 mm/s), bed depth (130 and 230 mm), granule size (2.1 and 2.7 mm), and the intergranular dust deposit expressed as percent by weight of collected dust in the bed (1% and 5%). All tests were conducted at ambient temperature and pressure using resuspended utility boiler fly ash as the test aerosol.Mass penetration data identified two major penetration mechanisms: (1) straight through penetration and (2) reentrainment due to granular motion. A static, intergranular dust deposit produced high filtration efficiency (>99%) at the low superficial velocity. When the bed was moving, reentrainment of collected dust was significant and accounted for about three-quarters of the penetrating dust. Particle size analyses reveal that the two penetration mechanisms are size dependent. Most particles larger than about one micrometer in diameter that penetrate the CMGBF do so by reentrainment after being collected initially. Virtually no particles smaller than about 0.3 μm in diameter penetrate by reentrainment; when these small particles penetrate, they pass straight through without being collected.     

Seasonal variation of 210Pb activity concentration in outdoor air of Milan (Italy)

Weekly measurements of 210Pb activity concentration on aerosol particles were performed at ground level in outdoor air in Milan (Italy) during the years 2000-2001. The experimental method was based on the delayed alpha spectrometry of in-grown 210Po activity detected on airborne particles collected on a filter support. On the same filter the 214Pb activity concentration was also measured during the sampling. 210Pb weekly concentration values showed a great variability and the average monthly values exhibited a seasonal pattern characterised by maxima in winter and minima in spring-summer. The same seasonal trend was also observed in 214Pb concentration values. 210Pb average yearly values were 0.70 and 0.82 mBq/m3 in 2000 and 2001, respectively, in good agreement with literature data registered at continental sites of similar latitude and longitude. The activity ratio 210Pb/214Pb was used to evaluate the residence time of fine aerosols in the urban air of Milan, which was 1-2 days.     

Preparation of size-selected fibers and fibrous aerosols for biological experiments

A size-selective procedure was developed for the preparation of fiber fractions of uniform size of chrysotile, crocidolite, amosite, and glass. The raw material was first ground to a suitable fineness, then suspended in liquids by ultrasonic agitation and separated by fiber diameter by means of slow sedimentation. The fractionation by fiber length was done by a vibrating sieve method. Fibrous aerosols of different size distributions could be prepared by using a vibrating bed aerosol generator.     

Reconstruction of radioactive plume characteristics along Chernobyl's Western Trace

Using data obtained from 435 radiation sampling stations in the Red Forest, 1.5 km W if the Chernobyl Nuclear Complex, we reconstructed the deposition pathway of the first plume released by the accident, Chernobyl's Western Trace. The dimensions and deposition rates of the plume remain sharply defined 15 years after the accident. Assuming a uniform particle distribution within the original cloud, we derived estimates of plume dimensions by applying geometric transformations to the coordinates at each sample point. Our derived estimates for the radioactive cloud accounted for 87% of the variation of radioactivity in this region. Results show a highly integrated bell-shaped cross-section of the cloud of radiation, approximately 660 m wide and 290 m high, traveling at a bearing of 264 degrees from reactor IV. Particle sizes within Chernobyl's Western Trace were within the most dangerous range for inhaled aerosols (2-5 microm). Therefore, reconstruction of the dispersion of such particles is critical for understanding the aftermath of nuclear and biological aerosol releases.     

Use of a culture-independent approach to characterize aerosolized bacteria near an open-freestall dairy operation

Animal manures are known to harbor a variety of zoonotic pathogens, which are suspected of being transported off-site as aerosols from confined feeding operations. In this study, aerosols were collected using a high-volume sampler downwind from a 10,000 cow open-freestall dairy and nearby fields being sprinkler irrigated with wastewater. DNA extracts were prepared from the aerosol samples, then a region of the16S ribosomal RNA gene was sequenced for bacterial identification and phylogenetic classification. At the dairy and irrigation sites, Proteobacteria (α-, β-, and γ-subdivisions) was the most abundant phylum, representing 78% and 69% of all sequences, respectively, while Actinobacteria, Bacteroidetes and Firmicutes represented only 10% or less of the sequences. Of the 191 clones sequenced from the dairy aerosol samples, 6 sequences were found to be homologous with uncultured bacteria from cow milk, rumen, and fecal samples. However, none of the sequence matches was affiliated with bacteria known to be pathogenic to otherwise healthy humans. Although our results do suggest a high diversity among the aerosolized bacteria, the sampling strategy employed in this study may not account for the variable nature of bioaerosol emissions.     

Experimental measurements of aerosol concentrations in offices

A new automated version of the piezoelectric microbalance measures the mass concentration of airborne particles smaller than a preselected aerodynamic cutoff diameter. It is designed for near-real-time, unattended, round-the-clock measurements of nearly any aerosol environment inhabited by humans. The instrument uses an electrostatic precipitator to deposit particles with greater than 95% efficiency onto a piezoelectric quartz crystal sensor which is able to detect a deposit of 0.005 μg. The precipitator and sensor are nearly identical to those in the portable instrument reported previously. Measurements comparing within ± 15% with gravimetrically measured filter samples are documented for a wide variety of aerosols in the 50 μg/m³ to 5.5 mg/m³ range. The instrument measures particles from 10 μm down to 0.01 μm in diameter, including submicron combustion smokes and metallic fumes. The piezoelectric microbalance technique senses the mass concentration of the aerosol, rather than light scattering properties as is done by photometers and nephelometers. The piezobalance, with 1 L/min sample flow, is more sensitive than any other mass-sensing instrument, making it especially suited for low concentration indoor measurements, even below 50 μg/m³. An automatic piezobalance recently measured respirable aerosol mass concentrations in several offices. Each measurement was the average concentration during a 30-min period. The 24-h/day measurements continued for several days. Especially interesting is the diurnal pattern, both for offices with and without smokers. The effect of a single nearby smoker was clearly illustrated when the smoker was absent one day in the middle of a week. Normal daytime peak concentrations in that office reached 80–110 μg/m³ with a smoker present, but only 50–60 μg/m³ when the smoker was absent. Curious smokers who briefly stopped byt o see the instrument caused single half-hour averages to triple, to values as high as 294 μg/m³ in one office.     

Instantaneous dust exposure monitors

This is a review of investigations conducted to evaluate portable, direct reading instruments employing the principles of light scattering and the attenuation of beta-rays to measure the respirable mass concentration of airborne particulates. Data are presented on comparative measurements obtained with several different models of beta-ray attenuation instruments manufactured by the GCA Corporation and light scattering instruments manufactured by GCA Corporation, USA, Ernst Leitz, GmbH, Germany, Rotheroe and Mitchell, England, and Sibata Chemical Apparatus Manufacturing Company, Ltd., Japan, using aerosols of coal, limestone, Arizona road dust, and silica. The effect of aerosol parameters (concentration, size distribution, index of refraction) on instrument calibration and precision are discussed.     

Mineralogical,chemical and toxicological characterization of urban air particles

Systematic characterization of morphological, mineralogical, chemical and toxicological properties of various size fractions of the atmospheric particulate matter was a main focus of this study together with an assessment of the human health risks they pose. Even though near-ground atmospheric aerosols have been a subject of intensive research in recent years, data integrating chemical composition of particles and health risks are still scarce and the particle size aspect has not been properly addressed yet. Filling this gap, however, is necessary for reliable risk assessment. A high volume ambient air sampler equipped with a multi-stage cascade impactor was used for size specific particle collection, and all 6 fractions were a subject of detailed characterization of chemical (PAHs) and mineralogical composition of the particles, their mass size distribution and genotoxic potential of organic extracts. Finally, the risk level for inhalation exposure associated to the carcinogenic character of the studied PAHs has been assessed. The finest fraction (< 0.45 μm) exhibited the highest mass, highest active surface, highest amount of associated PAHs and also highest direct and indirect genotoxic potentials in our model air sample. Risk assessment of inhalation scenario indicates the significant cancer risk values in PM 1.5 size fraction. This presented new approach proved to be a useful tool for human health risk assessment in the areas with significant levels of air dust concentration.     

Resuspension of coarse fuel hot particles in the Chernobyl area

Measurements of resuspended aerosol in the Chernobyl 30-km exclusion zone have shown coarse fuel hot particles in the activity range 1-12 Bq 137Cs per particle. The particles were sampled with newly designed rotating arm impactors which simultaneously collect during the same experiment three samples with fuel particles in the size ranges larger than 3 microns, larger than 6 microns and larger than 9 microns in geometric diameter. The radionuclide ratios, determined after gamma-spectrometry, were in good agreement with the theoretical calculations for the radionuclide-composition of the Chernobyl Nuclear Power Plant at the moment of the accident and the measured hot particles in soil in the early years after the accident. The number concentrations of airborne hot particles were derived from digital autoradiography. For wind resuspension, maximal concentrations of 2.6 coarse hot particles per 1000 m3 and during agricultural activities 36 coarse hot particles per 1000 m3 were measured. The geometric diameter of single hot particles was estimated to be between 6 and 12 microns.     

Detection of 210Po on filter papers 16 years after use for the collection of short-lived radon progeny in a room

Radon gas was allowed to accumulate in its radium source and then injected into a 36 m(3) test room, resulting in an initial radon concentration of 15 kBq m(-3). Filter papers were used to collect the short-lived radon progeny and thus to measure the Potential Alpha Energy Concentration (PAEC) in-situ in the year 1984 at different times and conditions according to the experimental design. The radon progeny collected on the filter papers were studied as a function of aerosol particle concentration ranging from 10(2)-10(5) particles cm(-3) in three different experiments. The highest aerosol particle concentration was generated by indoor cigarette smoking. Those filters were stored after the experiment, and were used after 16 years to study the activity of the radon long-lived alpha emitter progeny, (210)Po (T(1/2)=138 days). This isotope is separated from the short-lived progeny by (210)Pb beta emitter with 22.3 years half-life. After 16 years' storage of these filters, each filter paper was sandwiched and wrapped between two CR-39 nuclear track detectors, to put the detectors in contact with the surfaces of different filters, for 337 days. Correlation between the PAEC measured using filter papers in the year 1984 and the activity of long-lived alpha emitter (210)Po on the same filter papers measured in the year 2000 were studied. The results of the (210)Po activity showed a very good correlation of 0.92 with the PAEC 16 years ago. The results also depict that the PAEC and (210)Po activity in indoor air increased with the increase of aerosol particle concentration, which shows the attachment of short-lived radon progeny with the aerosol particles. The experiment proves that indoor cigarette smoking is a major source of aerosol particles carrying radon progeny and, thus, indoor cigarette smoking is an additional source of internal radiation hazard to the occupants whether smoker or non-smoker.     

Deposition of contaminant aerosol on human skin

Over recent years, it has been established that deposition of various types of pollutant aerosols (e.g., radioactive) on human skin can have serious deleterious effects on health. However, only few investigations in the past have been devoted to measurement of deposition velocities on skin of particles of the potentially problematic sizes. An experimental programme has shown the deposition velocities on skin of particles in the ca. 0.5-5 microm AMAD range to be high and generally associated with great variations. A series of investigations have been made to identify some of the factors that lead to this variation. Part of the variation was found to be caused by differences between individuals, whereas another part was found to be related to environmental factors. The identification of major influences on skin contaminant deposition is important in estimating health effects as well as in identifying means for their reduction.     

Measurements of major ion concentration in settled coarse particles and aerosols at a semiarid rural site in India

Deposition rates and deposition velocities of water-soluble ions (F, Cl, NO3, SO4, NH4, Ca, Mg, Na and K) were measured at a rural site (Gopalpura, Agra). Dry deposition samples were collected throughout the year from December 1995 to August 1997, while the aerosol samples were collected only during the winter season of 1996. Surrogate technique was used to collect the dry deposition samples, while aerosol samples were collected on PTFE membrane filter. Deposition velocities (Vd) of SO4 and NO3 are < or = 0.01 m s(-1) while Ca, Mg, Na, K, NH4, F and Cl exhibit greater than 0.01 m s(-1) Equivalent concentration ratios of K/Na, Ca/Na and Mg/Na conform with the corresponding ratios of local soil, indicating the dominant contribution of local sources. Deposition rates are maximum in winter, followed by summer and monsoon. No significant differences are found in dry deposition rates of all ions or in atmospheric concentrations of soil-derived elements with respect to wind direction. However, in aerosols, concentrations of F, Cl, NO3 and SO4 are higher with winds from southwesterly and westerly directions corresponding to pollution sources located in these directions. Deposition data have been used to calculate the critical load of S and N for soil with respect to Triticum vulgaris. The critical load of actual acidity was found to be 622.4 eq ha(-1) year(-1) within the range of 500-1,000 eq ha(-1) year(-1) as assessed by the RAINS-Asia model for this region. The present load of S and N (77.4 and 86.4 eq ha(-1) year(-1)) was much lower than the critical load of S and N (622.4 and 2,000 eq ha(-1) year(-1)), indicating that at present there is no harmful effect on ecosystem structure and function.     

Modeling and source apportionment of diesel particulate matter

The fine and ultra fine sizes of diesel particulate matter (DPM) are of greatest health concern. The composition of these primary and secondary fine and ultra fine particles is principally elemental carbon (EC) with adsorbed organic compounds, sulfate, nitrate, ammonia, metals, and other trace elements. The purpose of this study was to use an advanced air quality modeling technique to predict and analyze the emissions and the primary and secondary aerosols concentrations that come from diesel-fueled sources (DFS). The National Emissions Inventory for 1999 and a severe southeast ozone episode that occurred between August and September 1999 were used as reference. Five urban areas and one rural area in the Southeastern US were selected to compare the main results. For urban emissions, results showed that DFS contributed (77.9%+/-8.0) of EC, (16.8%+/-8.2) of organic aerosols, (14.3%+/-6.2) of nitrate, and (8.3%+/-6.6) of sulfate during the selected episodes. For the rural site, these contributions were lower. The highest DFS contribution on EC emissions was allocated in Memphis, due mainly to diesel non-road sources (60.9%). For ambient concentrations, DFS contributed (69.5%+/-6.5) of EC and (10.8%+/-2.4) of primary anthropogenic organic aerosols, where the highest DFS contributions on EC were allocated in Nashville and Memphis on that episode. The DFS contributed (8.3%+/-1.2) of the total ambient PM(2.5) at the analyzed sites. The maximum primary DPM concentration occurred in Atlanta (1.44 microg/m(3)), which was 3.8 times higher than that from the rural site. Non-linearity issues were encountered and recommendations were made for further research. The results indicated significant geographic variability in the EC contribution from DFS, and the main DPM sources in the Southeastern U.S. were the non-road DFS. The results of this work will be helpful in addressing policy issues targeted at designing control strategies on DFS in the Southeastern U.S.     

Life cycle impact assessment modeling for particulate matter: A new approach based on physico-chemical particle properties

Particulate matter (PM) causes severe damage to human health globally. Airborne PM is a mixture of solid and liquid droplets suspended in air. It consists of organic and inorganic components, and the particles of concern range in size from a few nanometers to approximately 10 μm. The complexity of PM is considered to be the reason for the poor understanding of PM and may also be the reason why PM in environmental impact assessment is poorly defined. Currently, life cycle impact assessment is unable to differentiate highly toxic soot particles from relatively harmless sea salt. The aim of this article is to present a new impact assessment for PM where the impact of PM is modeled based on particle physico-chemical properties. With the new method, 2781 characterization factors that account for particle mass, particle number concentration, particle size, chemical composition and solubility were calculated. Because particle sizes vary over four orders of magnitudes, a sound assessment of PM requires that the exposure model includes deposition of particles in the lungs and that the fate model includes coagulation as a removal mechanism for ultrafine particles. The effects model combines effects from particle size, solubility and chemical composition. The first results from case studies suggest that PM that stems from emissions generally assumed to be highly toxic (e.g. biomass combustion and fossil fuel combustion) might lead to results that are similar compared with an assessment of PM using established methods. However, if harmless PM emissions are emitted, established methods enormously overestimate the damage. The new impact assessment allows a high resolution of the damage allocatable to different size fractions or chemical components. This feature supports a more efficient optimization of processes and products when combating air pollution.     

Source apportionment of fine carbonaceous particles by positive matrix factorization at Gosan background site in East Asia

Fine particle (aerodynamic diameter <2.5 microm) samples were collected during six intensive measurement periods from November 2001 to August 2003 at Gosan, Jeju Island, Korea, which is one of the representative background sites in East Asia. Chemical composition of these aerosol samples including major ion components, trace elements, organic and elemental carbon (OC and EC), and particulate polycyclic aromatic hydrocarbons (PAHs) were analyzed to study the impact of long-range transport of anthropogenic aerosol. Aerosol chemical composition data were then analyzed using the positive matrix factorization (PMF) technique in order to identify the possible sources and estimate their contribution to particulate matter mass. Fourteen sources were then resolved including soil dust, fresh sea salt, transformed natural source, ammonium sulfate, ammonium nitrate, secondary organic carbon, diesel vehicle, gasoline vehicle, fuel oil combustion, biomass burning, coal combustion, municipal incineration, metallurgical emission source, and volcanic emission. The PMF analysis results of source contributions showed that the natural sources including soil dust, fresh and aged sea salt, and volcanic emission contributed to about 20% of the measured PM(2.5) mass. Other primary anthropogenic sources such as diesel and gasoline vehicle, coal and fuel oil combustion, biomass burning, municipal incineration, metallurgical source contributed about 34% of PM(2.5) mass. Especially, the secondary aerosol mainly involved with sulfate, nitrate, ammonium, and organic carbon contributed to about 39% of the PM(2.5) mass.     

Physical characterization of diesel exhaust particles in exposure chambers

Since the deposition of particulate in the respiratory system is strongly influenced by particle size, a correct assessment of this parameter is important for any inhalation experiment studying the potential health effects of air pollutants. Measuring the distribution of particles according to their aerodynamic diameter and mechanical mobility diameter is crucial in analyzing the deposition of submicron particles in the lower respiratory system. Cascade impactor measurements of diluted diesel exhaust in 12.6 m³ animal exposure chambers in the GMR Biomedical Science Department showed that the mass median aerodynamic diameter of the aerosol was 0.2 μm with 88% of the mass in particles smaller than 1 μm. Diffusion battery measurements showed that the mass median mechanical mobility diameter was about 0.11 μm. Transmission electron micrographs of particles deposited on chamber surfaces revealed both agglomerates and nearly spherical particles. The particles in these chambers are similar in size and shape to diesel particles described elsewhere. The flux of diesel particles to food surfaces was measured. Calculations of the expected daily dose by inhalation and by feeding showed that the “worst case” dose by feeding was only about one-tenth the dose by breathing.     

Deposition and biological availability of diesel particles and their associated mutagenic chemicals

To estimate the human health risk of inhaled diesel particles, it is necessary to know their deposition and retention in the respiratory tract and the rate of dissociation of mutagenic compounds associated with the particles. The deposition of a chain aggregate aerosol of ⁶⁷Ga₂O₃ with size and shape characteristics similar to diesel exhaust particles has been evaluated using Beagle dogs. Approximately one-third of the inhaled activity is deposited in the respiratory tract with most of the particles deposited in the lung. The mutagenic activity present in dichloromethane, dog serum, dog lung lavage fluid, saline, dipalmitoyl lecithin (DPL) and albumin following incubation of these fluids with diesel exhaust particles was determined in the Ames Salmonella system. As observed by other investigators, large quantities of mutagenic activity were removed by dichloromethane. A very small amount of mutagenic activity was removed by the serum and lavage fluid over a 3-day incubation period. No activity was detected following elution with the other solvents. The finding that minimal mutagenic activity could be demonstrated in the biological media following incubation with diesel exhaust particles may be due to a lack of removal of mutagens from the particles or an inactivation of removed mutagens by protein binding or other processes.     

Seasonal variations of aerosol residence time in the lower atmospheric boundary layer

During a one year period, from Jan. 2002 up to Dec. 2002, approximately 130 air samples were analyzed to determine the atmospheric air activity concentrations of short- and long-lived (222Rn) decay products 214Pb and 210Pb. The samples were taken by using a single-filter technique and gamma-spectrometry was applied to determine the activity concentrations. A seasonal fluctuation in the concentration of 214Pb and 210Pb in surface air was observed. The activity concentrations of both radionuclides were observed to be relatively higher during the winter/autumn season than in spring/summer season. The mean activity concentration of 214Pb and 210Pb within the whole year was found to be 1.4+/-0.27 Bq m(-3) and 1.2+/-0.15 mBq m(-3), respectively. Different 210Pb:214Pb activity ratios during the year varied between 1.78 x 10(-4) and 1.6 x 10(-3) with a mean value of 8.9 x 10(-4) +/- 7.6 x 10(-5). From the ratio between the activity concentrations of the radon decay products 214Pb and 210Pb a mean residence time (MRT) of aerosol particles in the atmosphere of about 10.5+/-0.91 d could be estimated. The seasonal variation pattern shows relatively higher values of MRT in spring/summer season than in winter/autumn season. The MRT data together with relative humidity (RH), air temperature (T) and wind speed (WS), were used for a comprehensive regression analysis of its seasonal variation in the atmospheric air.     

The sources and fate of 210Po in the urban air: A review

The origin of ²¹⁰Po activity and its fluctuations in the air are discussed in this paper. In the case of atmospheric aerosol samples, a comparison of the ²¹⁰Po/²¹⁰Pb and ²¹⁰Bi/²¹⁰Pb activity ratios makes it possible not only to determine aerosol residence times but also to appraise the contribution of the unsupported ²¹⁰Po coming from other sources than ²²²Rn decay, such as human industrial activities, especially coal combustion. A simple mathematical method makes it possible to observe the seasonal fluctuations of the anthropogenic excess of ²¹⁰Po in the urban air. The average doses of ²¹⁰Po intake with food (including drinking water) and inhalation of urban aerosols are usually lower than those from ²¹⁰Po intake by cigarette smokers and negligible in comparison to total natural radiation exposure.