蜂窝煤燃烧烟气中多环芳烃的定量研究及粒径分布特征

通过对蜂窝煤燃烧排放的烟气中多环芳烃的定量分析,研究了17种多环芳烃在烟气颗粒相和气相中的分配以及在不同粒径颗粒物上的分布特征。结果表明：在室温下燃煤排放的多环芳烃总量以在气相中存在为主,但总体毒性则主要存在于颗粒相中;多环芳烃主要分布在亚微米级颗粒上,分子量越大的多环芳烃越趋于富集在细颗粒上,因而对健康的危害就越大。     

Health Effects and Energy Choices

ABSTRACT

Day- and nighttime total suspended particulate matter was collected inside and outside Emperor Qin's Terra-Cotta Museum in winter and summer 2008. The purpose was to characterize the winter and summer differences of indoor airborne particles in two display halls with different architectural and ventilation conditions, namely the Exhibition Hall and Pit No. 1. The morphology and elemental composition of two season samples were investigated using scanning electron microscopy and energy dispersive X-ray spectrometry. It is found that the particle size, particle mass concentration, and particle type were associated with the visitor numbers in the Exhibition Hall and with the natural ventilation in Pit No. 1 in both winter and summer. Evident winter and summer changes in the composition and physicochemical properties of the indoor suspended particulate matters were related to the source emission and the meteorological conditions. Particle mass concentrations in both halls were higher in winter than in summer. In winter, the size of the most abundant particles at the three sites were all between 0.5 and 1.0 μm, whereas in summer the peaks were all located at less than 0.5 μm. The fraction of sulfur-containing particles was 2–7 times higher in winter than in summer. In addition to the potential soiling hazard, the formation and deposition of sulfur-containing particles in winter may lead to the chemical and physical weathering of the surfaces of the terra-cotta statues.

IMPLICATIONS Relatively few microanalyses of indoor airborne particles inside museums in China have been performed. The mass concentrations of winter and summer indoor total suspended particulate (TSP) are presented for the Emperor Qin's Terra-Cotta Museum along with the characterization of individual particles via computerized scanning electron microscopy and an energy dispersive X-ray spectrometry. The results indicate that both the high level of particle mass concentrations in winter and the predominant fine particles in summer were responsible for the soiling of the statues over a long period of time. The irreplaceable statues were also facing with weathering hazards posed by abundant sulfur-containing particles, especially in winter. Data provided in this study suggested that mechanical ventilation, air filtration, and air conditioning systems should be installed in Pit No. 1 display hall and proper display strategy should be adopted in Exhibition Hall.     

The Mass Distribution of Large Atmospheric Particles

This paper describes the results of a study to determine the total mass and the mass distribution of atmospheric aerosols, especially that mass associated with particles greater than 10 μm diameter. This study also determined what fraction of the total aerosol mass a standard high-volume air sampler collects and what fraction and size interval settle out on a dust fall plate. A special aerosol sampling system was designed for this study to obtain representative samples of large airborne particles. A suburban sampling site was selected because no local point sources of aerosols existed nearby. Samples were collected under various conditions of wind velocity and direction to obtain measurements on different types of aerosols.

Study measurements show that atmospheric particulate matter has a bimodal mass distribution. Mass associated with large particles mainly ranged from 5 to 100 μm in size, while mass associated with small particles ranged from an estimated 0.03 to 5 μm in size. Combined, these two distributions produced a bimodal mass distribution with a minimum around 5 μm diameter. The high-volume air sampler was found to collect most of the total aerosol mass, not just that fraction normally considered suspended particulate. Dust fall plates did not provide a good or very useful measure of total aerosol mass. The two fundamental processes of aerosol formation, condensation and dispersion appear to account for the formation of a bimodal mass distribution in both natural and anthropogenic aerosols. Particle size distribution measurements frequently are in error because representative samples of large airborne particles are not obtained. Considering this descrepancy, air pollution regulations should specify or be based upon an upper particle size limit.     

Characteristics of particulate matter emissions from toy cars with electric motors

Aerosol emissions from toy cars with electric motors were characterized. Particle emission rates from the toy cars, as high as 7.47 × 10⁷ particles/s, were measured. This emission rate is lower than other indoor sources such as smoking and cooking. The particles emitted from toy cars are generated from spark discharges inside the electric motors that power the toy cars. Size distribution measurements indicated that most particles were below 100 nm in diameter. Copper was the dominant inorganic species in these particles. By deploying aerosol mass spectrometers, high concentrations of particulate organic matter were also detected and characterized in detail. Several organic compounds were identified using a thermal desorption aerosol gas chromatography. The mass size distribution of particulate organic matter was bimodal. The formation mechanism of particulate organic matter from toy cars was elucidated.

Implications:?A possible new source of indoor air pollution, particles from electric motors in toy cars, was identified. This study characterized aerosol emissions from toy cars in detail. Most of these particles have a diameter less than 100 nm. Copper and some organics are the major components of these particles. Conditions that minimize these emissions were determined.     

Particulate Air Pollution In the United States

A study was conducted to identify, characterize, and quantify the national particulate air pollution problem from stationary sources. Particulate emissions from stationary sources were determined from data on emission factors, grain loadings, and material balances. The principal method used for establishing the tonnage emitted by an industry utilized uncontrolled emission factors. Total tonnage emitted by a given industry was calculated from four quantities: (1) an emission factor for the uncontrolled source; (2) the total tonnage processed per year by the industry; (3) the efficiency of control equipment used; and (4) the percentage of production capacity equipped with control devices.

Particulate emissions from stationary sources in the United States currently total approximately 18 X 10⁶ ton/yr. The major stationary sources of particulates include electric power generation plants, the crushed stone industry, the forest products industry, agriculture and related operations, the cement industry, and the iron and steel industry.

Three methods were developed to project the total quantity of particulate pollutants emitted up to the year 2000. In making these forecasts, these factors were considered (1) changes in production capacity; (2) improvements in control devices; and (3) regulatory action to enforce installation of control equipment.

These forecasts indicate that particulate emissions can be reduced from the current level of 18 X 10⁶ ton/yr to 3 X 10⁶ ton/yr by 2000 based on the most optimistic forecast. The projections also suggest that major reductions of particulate matter will most likely occur by installation of control equipment on uncontrolled sources and by shifts to more efficient types of collection equipment on existing controlled sources.     

Gas and Particle Emissions from Automobile Tires in Laboratory and Field Studies

This paper is directed to air pollution scientists interested in special mobile emission sources. The purpose was to determine the contribution which automobile tires make to air pollution. The gaseous hydrocarbon and sulfur compounds emitted in laboratory tests were identified. Although these hydrocarbons can participate in smog reactions, their mass emission rate is less than 0.1 % of the current exhaust hydrocarbon emission rate. Hydrocarbons from tires are not measurable near a freeway. The particulate emitted from tires ranges in size from 0.01 μm to more than 30 μm, with the larger particles dominating the total mass. Measurements along a California freeway showed that most of the tire debris had settled within 5 m of the pavement edge. Airborne rubber concentrations were less than 0.5 μg/m³, or less than 5% of the total tire wear. These field measurements confirm the indoor emission pattern and verify that tire wear products are not a significant air pollution problem.     

Characterization of atmospheric particulates, particle-bound transition metals and polycyclic aromatic hydrocarbons of urban air in the centre of Athens (Greece)

The concentrations of trace metals and polycyclic aromatic hydrocarbons (PAHs) adsorbed to total suspended particulate (TSP) and finer fractions of airborne particulate matter (PM) were determined from a site in the centre of Athens (Greece), which is characterized by heavy local traffic and is densely populated, during the winter and summer periods in 2003-2004. Also, we collected and analyzed samples of diesel and gasoline exhaust particles from local vehicles (buses, taxis and private cars) and from chimney exhaust of residential central heating appliances. A seasonal effect was observed for the size distribution of aerosol mass, with a shift to larger fine fractions in winter. The most commonly detected trace metals in the TSP and PM fractions were Fe, Pb, Zn, Cu, Cr, V, Ni and Cd and their concentrations were similar to levels observed in heavily polluted urban areas from local traffic and other anthropogenic emissions. Analysis of 16 PAHs bound to PM showed that they are mostly traffic related. In general, the fine particulate PAHs concentrations were higher than coarse particles. The most common PAHs in PM(10.2) and PM(2.1) were pyrene, phenanthrene, acenapthylene and fluoranthene, which are associated with diesel and gasoline exhaust particles. The results of this study underlined the importance of local emission sources, especially vehicular traffic, central heating and other local anthropogenic emissions. Compared with other big cities, Athens has much higher levels of airborne particles, especially of the finer fractions PM(10) and PM(2.5), correlated with traffic-related air pollution.     

Winter and summer characteristics of airborne particles inside emperor Qin's Terra-Cotta Museum, China: a study by scanning electron microscopy-energy dispersive X-ray spectrometry

Day- and nighttime total suspended particulate matter was collected inside and outside Emperor Qin's Terra-Cotta Museum in winter and summer 2008. The purpose was to characterize the winter and summer differences of indoor airborne particles in two display halls with different architectural and ventilation conditions, namely the Exhibition Hall and Pit No. 1. The morphology and elemental composition of two season samples were investigated using scanning electron microscopy and energy dispersive X-ray spectrometry. It is found that the particle size, particle mass concentration, and particle type were associated with the visitor numbers in the Exhibition Hall and with the natural ventilation in Pit No. 1 in both winter and summer. Evident winter and summer changes in the composition and physicochemical properties of the indoor suspended particulate matters were related to the source emission and the meteorological conditions. Particle mass concentrations in both halls were higher in winter than in summer. In winter, the size of the most abundant particles at the three sites were all between 0.5 and 1.0 microm, whereas in summer the peaks were all located at less than 0.5 microm. The fraction of sulfur-containing particles was 2-7 times higher in winter than in summer. In addition to the potential soiling hazard, the formation and deposition of sulfur-containing particles in winter may lead to the chemical and physical weathering of the surfaces of the terra-cotta statues.     

Characteristics of inhalable particulate matter concentration and size distribution from power plants in China

In this investigation, the collection efficiency of particulate emission control devices (PECDs), particulate matter (PM) emissions, and PM size distribution were determined experimentally at the inlet and outlet of PECDs at five coal-fired power plants. Different boilers, coals, and PECDs are used in these power plants. Measurement in situ was performed by an electrical low-pressure impactor with a sampling system, which consisted of an isokinetic sampler probe, precut cyclone, and two-stage dilution system with a sample line to the instruments. The size distribution was measured over a range from 0.03 to 10 microm. Before and after all of the PECDs, the particle number size distributions display a bimodal distribution. The PM2.5 fraction emitted to atmosphere includes a significant amount of the mass from the coarse particle mode. The controlled and uncontrolled emission factors of total PM, inhalable PM (PM10), and fine PM P(M2.5) were obtained. Electrostatic precipitator (ESP) and baghouse total collection efficiencies are 96.38-99.89% and 99.94%, respectively. The minimum collection efficiency of the ESP and the baghouse both appear in the particle size range of 0.1-1 microm. In this size range, ESP and baghouse collection efficiencies are 85.79-98.6% and 99.54%. Real-time measurement shows that the mass and number concentration of PM10 will be greatly affected by the operating conditions of the PECDs. The number of emitted particles increases with increasing boiler load level because of higher combustion temperature. During test run periods, the data reproducibility is satisfactory.     

Formation of fine particles enriched by V and Ni from heavy oil combustion: Anthropogenic sources and drop-tube furnace experiments

The present study attempts to investigate the emission characteristics of fine particles with special emphasis on nickel and vanadium metal elements emitted from the heavy oil combustion in industrial boilers and power plant, which are typical anthropogenic sources in Korea. A series of combustion experiments were performed to investigate the emission characteristics of particles in the size range of submicron by means of drop-tube furnace with three major domestic heavy oils. Cascade impactors were utilized to determine the size distribution of particulates as well as to analyze the partitioning enrichment of vanadium and nickel in various size ranges. Experimental results were compared with field data of particle size distribution and metal partitioning at commercial utility boilers with heavy oil combustion. Such data were interpreted by chemical equilibrium and particle growth mechanism by means of computational models. In general, fine particles were the major portion of PM₁₀ emitted from the heavy oil combustion, with significant fraction of ultra-fine particles. The formation of ultra-fine particles through nucleation/condensation/coagulation from heavy oil combustion was confirmed by field and experimental data. Vanadium and nickel were more enriched in fine particles, particularly in ultra-fine particles. The conventional air pollution devices showed inefficient capability to remove ultra-fine particles enriched with hazardous transition metal elements such as vanadium and nickel.     

A Federal Tax on Energy

Abstract

In this investigation, the collection efficiency of particulate emission control devices (PECDs), particulate matter (PM) emissions, and PM size distribution were determined experimentally at the inlet and outlet of PECDs at five coal-fired power plants. Different boilers, coals, and PECDs are used in these power plants. Measurement in situ was performed by an electrical low-pressure impactor with a sampling system, which consisted of an isokinetic sampler probe, precut cyclone, and two-stage dilution system with a sample line to the instruments. The size distribution was measured over a range from 0.03 to 10 µm. Before and after all of the PECDs, the particle number size distributions display a bimodal distribution. The PM_2.5 fraction emitted to atmosphere includes a significant amount of the mass from the coarse particle mode. The controlled and uncontrolled emission factors of total PM, inhalable PM (PM₁₀), and fine PM P(M_2.5) were obtained. Electrostatic precipitator (ESP) and baghouse total collection efficiencies are 96.38–99.89% and 99.94%, respectively. The minimum collection efficiency of the ESP and the baghouse both appear in the particle size range of 0.1–1 µm. In this size range, ESP and baghouse collection efficiencies are 85.79–98.6% and 99.54%. Real-time measurement shows that the mass and number concentration of PM₁₀ will be greatly affected by the operating conditions of the PECDs. The number of emitted particles increases with increasing boiler load level because of higher combustion temperature. During test run periods, the data reproducibility is satisfactory.     

Dilution-based emissions sampling from stationary sources: Part 2--Gas-fired combustors compared with other fuel-fired systems

With the recent focus on fine particle matter (PM2.5), new, self-consistent data are needed to characterize emissions from combustion sources. Such data are necessary for health assessment and air quality modeling. To address this need, emissions data for gas-fired combustors are presented here, using dilution sampling as the reference. The dilution method allows for collection of emitted particles under conditions simulating cooling and dilution during entry from the stack into the air. The sampling and analysis of the collected particles in the presence of precursor gases, SO2 nitrogen oxide, volatile organic compound, and NH3 is discussed; the results include data from eight gas fired units, including a dual-fuel institutional boiler and a diesel engine powered electricity generator. These data are compared with results in the literature for heavy-duty diesel vehicles and stationary sources using coal or wood as fuels. The results show that the gas-fired combustors have very low PM2.5 mass emission rates in the range of approximately 10(-4) lb/million Btu (MMBTU) compared with the diesel backup generator with particle filter, with approximately 5 x 10(-3) lb/MMBTU. Even higher mass emission rates are found in coal-fired systems, with rates of approximately 0.07 lb/MMBTU for a bag-filter-controlled pilot unit burning eastern bituminous coal. The characterization of PM2.5 chemical composition from the gas-fired units indicates that much of the measured primary particle mass in PM2.5 samples is organic or elemental carbon and, to a much less extent, sulfate. Metal emissions are quite low compared with the diesel engines and the coal- or wood-fueled combustors. The metals found in the gas-fired combustor particles are low in concentration, similar in concentration to ambient particles. The interpretation of the particulate carbon emissions is complicated by the fact that an approximately equal amount of particulate carbon (mainly organic carbon) is found on the particle collector and a backup filter. It is likely that measurement artifacts, mostly adsorption of volatile organic compounds on quartz filters, are positively biasing "true" particulate carbon emission results.     

Trace Metal Pollution in the Environment

Trace metals introduced to the environment from fuel combustion, incineration, and industrial emission sources are causing increasing concern to air pollution researchers. Several metals in urban air, including lead and vanadium, are associated with particles in the predominantly submicrometer diameter range thereby presenting an inhalation threat. There is also growing evidence that some metals emitted from stationary sources are concentrated in submicrometer sized particles which may pass through emission control devices. This report summarizes the concentration and size of trace metals in urban air, the concentration ranges found in selected fuels and emission sources, and describes the areas where further studies are needed.     

Comparison of real-time instruments used to monitor airborne particulate matter

Measurements collected using five real-time continuous airborne particle monitors were compared to measurements made using reference filter-based samplers at Bakersfield, CA, between December 2, 1998, and January 31, 1999. The purpose of this analysis was to evaluate the suitability of each instrument for use in a real-time continuous monitoring network designed to measure the mass of airborne particles with an aerodynamic diam less than 2.5 microns (PM2.5) under wintertime conditions in the southern San Joaquin Valley. Measurements of airborne particulate mass made with a beta attenuation monitor (BAM), an integrating nephelometer, and a continuous aerosol mass monitor (CAMM) were found to correlate well with reference measurements made with a filter-based sampler. A Dusttrak aerosol sampler overestimated airborne particle concentrations by a factor of approximately 3 throughout the study. Measurements of airborne particulate matter made with a tapered element oscillating microbalance (TEOM) were found to be lower than the reference filter-based measurements by an amount approximately equal to the concentration of NH4NO3 observed to be present in the airborne particles. The performance of the Dusttrak sampler and the integrating nephelometer was affected by the size distribution of airborne particulate matter. The performance of the BAM, the integrating nephelometer, the CAMM, the Dusttrak sampler, and the TEOM was not strongly affected by temperature, relative humidity, wind speed, or wind direction within the range of conditions encountered in the current study. Based on instrument performance, the BAM, the integrating nephelometer, and the CAMM appear to be suitable candidates for deployment in a real-time continuous PM2.5 monitoring network in central California for the range of winter conditions and aerosol composition encountered during the study.     

On-road and laboratory investigation of low-level PM emissions of a modern diesel particulate filter equipped diesel passenger car

Modern diesel particulate filter (DPF) systems are very effective in reducing particle emissions from diesel vehicles. In this work low-level particulate matter (PM) emissions from a DPF equipped EURO-4 diesel vehicle were studied in the emission test laboratory as well as during real-world chasing on a high-speed test track. Size and time resolved data obtained from an engine exhaust particle sizer (EEPS) and a condensation particle counter (CPC) are presented for both loaded and unloaded DPF condition. The corresponding time and size resolved emission factors were calculated for acceleration, deceleration, steady state driving and during DPF regeneration, and are compared with each other. In addition, the DPF efficiency of the tested vehicle was evaluated during the New European Driving Cycle (NEDC) by real time pre-/post-DPF measurements and was found to be 99.5% with respect to PM number concentration and 99.3% for PM mass, respectively. PM concentrations, which were measured at a distance of about 10 m behind the test car, ranged from 1 to 1.5 times background level when the vehicle was driven on the test track under normal acceleration conditions or at constant speeds below 100 kmh^?1. Only during higher speeds and full load accelerations concentrations above 3 times background level could be observed. The corresponding tests in the emission laboratory confirmed these results. During DPF regeneration the total PM number emission of nucleation mode particles was 3–4 orders of magnitude higher compared to those emitted at the same speed without regeneration, while the level of the accumulation mode particles remained about the same. The majority of the particles emitted during DPF regeneration was found to be volatile, and is suggested to originate from accumulated sulfur compounds.     

Bioethanol-gasoline fuel blends: exhaust emissions and morphological characterization of particulate from a moped engine

This study was aimed at evaluating the effects of gasoline-ethanol blends on the exhaust emissions in a catalyst-equipped four-stroke moped engine. The ethanol was blended with unleaded gasoline in at percentages (10, 15, and 20% v/v). The regulated pollutants and the particulate matter emissions were evaluated over the European ECE R47 driving cycle on the chassis dynamometer bench. Particulate matter was characterized in terms of total mass collected on filters and total number ofparticles in the range 7 nm-10 microm measured by electrical low-pressure impactor (ELPI). In addition, particle-phase polycyclic aromatic hydrocarbons (PAHs) emissions were evaluated to assess the health impact of the emitted particulate. Finally, an accurate morphological analysis was performed on the particulate by high-resolution transmission electron microscope (TEM) equipped with a digital image-processing/data-acquisition system. In general, CO emission reductions of 60-70% were obtained with 15 and 20% v/v ethanol blends, while the ethanol use did not reduce hydrocarbon (HC) and NOx emissions. No evident effect of ethanol on the particulate mass emissions and associated PAHs emissions was observed. Twenty-one PAHs were quantified in the particulate phase with emissions ranging from 26 to 35 microg/km and benzo[a]pyrene equivalent (BaPeq) emission factors from 2.2 to 4.1 microg/km. Both particulate matter and associated PAHs with higher carcinogenic risk were mainly emitted in the submicrometer size range (<0.1 microm). On the basis of the TEM observations, no relevant effect of the ethanol use on the particulate morphology was evidenced, showing aggregates composed ofprimary particles with mean diameters in the range 17.5-32.5 nm.     

Characterization of indoor particle sources using continuous mass and size monitors

A comprehensive indoor particle characterization study was conducted in nine Boston-area homes in 1998 in order to characterize sources of PM in indoor environments. State-of-the-art sampling methodologies were used to obtain continuous PM2.5 concentration and size distribution particulate data for both indoor and outdoor air. Study homes, five of which were sampled during two seasons, were monitored over week-long periods. Among other data collected during the extensive monitoring efforts were 24-hr elemental/organic carbon (EC/OC) particulate data as well as semi-continuous air exchange rates and time-activity information. This rich data set shows that indoor particle events tend to be brief, intermittent, and highly variable, thus requiring the use of continuous instrumentation for their characterization. In addition to dramatically increasing indoor PM2.5 concentrations, these data demonstrate that indoor particle events can significantly alter the size distribution and composition of indoor particles. Source event data demonstrate that the impacts of indoor activities are especially pronounced in the ultrafine (da < or = 0.1 micron) and coarse (2.5 < or = da < or = 10 microns) modes. Among the sources of ultrafine particles characterized in this study are indoor ozone/terpene reactions. Furthermore, EC/OC data suggest that organic carbon is a major constituent of particles emitted during indoor source events. Whether exposures to indoor-generated particles, particularly from large short-term peak events, may be associated with adverse health effects will become clearer when biological mechanisms are better known.     

Effect of Roadbed Configuration on Traffic Derived Aerosols

Aerosols present upwind and downwind of freeways in the Los Angeles Basin were collected in five particle size ranges by Lundgren impactors with after filters and analyzed for elemental content by ion-excited x-ray emission. The contribution of freeway traffic to total airborne particulate load was obtained by subtracting the local background, measured by an upwind sampler, from the values obtained by downwind samplers on a size by size, element by element basis. This contribution correlated reasonably well with estimates derived from automotive and roadbed expendable rates. Traffic-derived aerosols, normalized to vehicular flow, were considerably lower in mass downwind of depressed roadbed configurations than either at grade or raised configurations. A line source model, combined with literature values for emitted lead, produced good agreement with results obtained in the at grade configuration.     

Fugitive dust emission source profiles and assessment of selected control strategies for particulate matter at gravel processing sites in Taiwan

Particles emitted from gravel processing sites are one contributor to worsening air quality in Taiwan. Major pollution sources at gravel processing sites include gravel and sand piles, unpaved roads, material crushers, and bare ground. This study analyzed fugitive dust emission characteristics at each pollution source using several types of particle samplers, including total suspended particulates (TSP), suspended particulate (PM10), fine suspended particulate (PM2.5), particulate sizer, and dust-fall collectors. Furthermore, silt content and moisture in the gravel were measured to develop particulate emission factors. The results showed that TSP (< 100 microm) concentrations at the boundary of gravel sites ranged from 280 to 1290 microg/m3, which clearly exceeds the Taiwan hourly air quality standard of 500 microg/m3. Moreover, PM10 concentrations, ranging from 135 to 550 microg/m3, were also above the daily air quality standard of 125 microg/m3 and approximately 1.2 and 1.5 times the PM2.5 concentrations, ranging from 105 to 470 microg/m3. The size distribution analysis reveals that mass mean diameter and geometric standard deviation ranged from 3.2 to 5.7 microm and from 2.82 to 5.51, respectively. In this study, spraying surfactant was the most effective control strategy to abate windblown dust from unpaved roads, having a control efficiency of approximately 93%, which is significantly higher than using paved road strategies with a control efficiency of approximately 45%. For paved roads, wet suppression provided the best dust control efficiencies ranging from 50 to 83%. Re-vegetation of disturbed ground had dust control efficiencies ranging from 48 to 64%.