Updating the conceptual model for fine particle mass emissions from combustion systems

Atmospheric transformations determine the contribution of emissions from combustion systems to fine particulate matter (PM) mass. For example, combustion systems emit vapors that condense onto existing particles or form new particles as the emissions are cooled and diluted. Upon entering the atmosphere, emissions are exposed to atmospheric oxidants and sunlight, which causes them to evolve chemically and physically, generating secondary PM. This review discusses these transformations, focusing on organic PM. Organic PM emissions are semi-volatile at atmospheric conditions and thus their partitioning varies continuously with changing temperature and concentration. Because organics contribute a large portion of the PM mass emitted by most combustion sources, these emissions cannot be represented using a traditional, static emission factor. Instead, knowledge of the volatility distribution of emissions is required to explicitly account for changes in gas-particle partitioning. This requires updating how PM emissions from combustion systems are measured and simulated from combustion systems. Secondary PM production often greatly exceeds the direct or primary PM emissions; therefore, secondary PM must be included in any assessment of the contribution of combustion systems to ambient PM concentrations. Low-volatility organic vapors emitted by combustion systems appear to be very important secondary PM precursors that are poorly accounted for in inventories and models. The review concludes by discussing the implications that the dynamic nature of these PM emissions have on source testing for emission inventory development and regulatory purposes. This discussion highlights important linkages between primary and secondary PM, which could lead to simplified certification test procedures while capturing the emission components that contribute most to atmospheric PM mass.     

Aerosol laser ablation mass spectrometry of suspended powders from PM sources and its implications to receptor modeling

Primary sources of particulate matter (PM) were analyzed by suspending powdered samples into an aerosol laser ablation mass spectrometer (LAMS). PM sources studied included vehicle exhaust particulates, dust from a non-ferrous smelter, cement powder, incinerator fly ash, two coal fly ash samples, and two soils. Marker peaks signified certain PM source sectors: construction particles could be distinguished by abundant Ca and Ca compounds, fuel combustion was marked by elemental carbon clusters, and nonferrous industrial particles showed inorganic As, Cu, Pb, Zn, and SOx. In addition to the distinction between particles from these different source sectors, mass spectral results also showed that for a single source, different particle types existed, and among different sources within a sector, similar spectra were present. The aerosol LAMS results show the difficulty in differentiating among separate fly ash sources as well as among different soil samples. A particle class balance receptor model that measures the amount of specific particle types rather than the amount of a chemical component is suggested as a means of source apportionment when particle spectra with overlapping source possibilities occur. The assumptions and limitations of receptor modeling aerosol LAMS data are also described. In particular, methods need to be developed to account for the contribution of secondary sources.     

Inorganic and carbonaceous components in indoor/outdoor particulate matter in two residential houses in Oslo, Norway

A detailed analysis of indoor/outdoor physicochemical aerosol properties has been performed. Aerosol measurements were taken at two dwellings, one in the city center and the other in the suburbs of the Oslo metropolitan area, during summer/fall and winter/spring periods of 2002-2003. In this paper, emphasis is placed on the chemical characteristics (water-soluble ions and carbonaceous components) of fine (PM2.5) and coarse (PM2.5-10) particles and their indoor/outdoor relationship. Results demonstrate that the carbonaceous species were dominant in all fractions of the PM10 particles (cut off size: 0.09-11.31 microm) during all measurement periods, except winter 2003, when increased concentrations of water-soluble inorganic ions were predominant because of sea salt transport. The concentration of organic carbon was higher in the fine and coarse PM10 fractions indoors, whereas elemental carbon was higher indoors only in the coarse fraction. In regards to the carbonaceous species, local traffic and secondary organic aerosol formation were, probably, the main sources outdoors, whereas indoors combustion activities such as preparation of food, burning of candles, and cigarette smoking were the main sources. In contrast, the concentrations of water-soluble inorganic ions were higher outdoors than indoors. The variability of water-soluble inorganic ion concentrations outdoors was related to changes in emissions from local anthropogenic sources, long-range transport of particles, sea salt emissions, and resuspension of roadside and soil dusts. In the indoor environment the infiltration of the outdoor air indoors was the major source of inorganic ions.     

Regional transport and urban contributions to fine particle concentrations in southeastern Canada

The impact of various atmospheric transport directions on ambient fine particle (PM2.5) concentrations at several sites in southeastern Canada was estimated (for May-September) using back-trajectory analysis. Three-day back trajectories (four per day) were paired with 6-hr average PM2.5 mass concentrations measured using tapered element oscillating microbalances (TEOM). PM2.5 concentrations at rural locations in the region were affected by nonlocal sources originating in both Canada and the United States. Comparison of sites revealed that, on average, the local contribution to total PM2.5 in the greater Toronto area (GTA) is approximately 30-35%. At each location, average PM2.5 concentrations under south/southwesterly flow conditions were 2-4 times higher than under the corresponding northerly flow conditions. The chemical composition of both urban and rural PM2.5 was determined during two separate 2-week spring/summer measurement campaigns. Components identified included SO4(2-) NO3-, NH4+, black carbon and organic carbon (OC), and trace elements. Higher particle mass at the urban Toronto site was composed of a higher proportion of all components. However, black carbon, NO3-, NaCl, and trace elements were found to be the most enriched over the rural/regional background levels.     

Historical trends in the mass and chemical species concentrations of coarse particulate matter in the Los Angeles Basin and relation to sources and air quality regulations

To assess the impact of past, current and proposed air quality regulations on coarse particulate matter (CPM), the concentrations of CPM mass and its chemical constituents were examined in the Los Angeles Basin from 1986 to 2009 using PM data acquired from peer-reviewed journals and regulatory agency database. PM10 mass levels decreased by approximately half from 1988 to 2009 at the three sampling sites examined- located in downtown Los Angeles, Long Beach and Riverside. Annual CPM mass concentrations were calculated from the difference between daily PM10 and PM2.5 from 1999 to 2009. High CPM episodes driven by high wind speed/stagnant condition caused year-to-year fluctuations in the 99th/98th percentile CPM levels. The reductions of average CPM levels were lower than those of PM10 in the same period, therefore the decrease of PM10 level was mainly driven by reductions in the emission levels of PM2.5 (or fine) particles, as demonstrated by the higher annual reduction of average PM2.5 (0.92 microg/m3) compared with CPM (0.39 microg/m3) from 1999 to 2009 in downtown Los Angeles despite their comparable concentrations. This is further confirmed by the significant decrease of Ni, Cr, V and EC in the coarse fraction after 1995. On the other hand, the levels of several inorganic ions (sulfate, chloride and to a lesser extent nitrate) remained comparable. From 1995 to 2008, levels of Cu, a tracer of brake wear, either remained similar or decreased at a smaller rate compared with elements of combustion origins. This differential reduction of CPM components suggests that past and current regulations may have been more effective in reducing fugitive dust (Al, Fe and Si) and combustion emissions (Ni, Cr, V, and EC) rather than CPM from vehicular abrasion (Cu) and inorganic ions (NO3(-), SO4(2-) and Cl(-)) in urban areas. Implications: Limited information is currently available to provide the scientific basis for understanding the sources and physical and chemical variations of CPM, and their relations to air quality regulations and adverse health effects. This study investigates the historical trends of CPM mass and its chemical components in the Los Angeles Basin to advance our understanding on the impact of past and current air quality regulations on the coarse fraction of PM. The results of this study will aid policy makers to design more targeted regulations to control CPM sources to ensure substantial protection of public health from CPM exposure. Supplemental Materials: Supplemental materials are available for this article. Go to the publisher's online edition of the Journal of the Air & Waste Management Association for (1) details of the sampling sites and (2) the daily concentrations of high CPM/PM10 episodes.     

The major components of particles emitted during recycling of waste printed circuit boards in a typical e-waste workshop of South China

Electronic waste from across the world is dismantled and disposed of in China. The low-tech recycling methods have caused severe air pollution. Air particle samples from a typical workshop of South China engaged in recycling waste printed circuit boards have been analyzed with respect to chemical constituents. This is the first report on the chemical composition of particulate matter (PM) emitted in an e-waste recycling workshop of South China. The results show that the composition of PM from this recycling process was totally different from other emission sources. Organic matter comprised 46.7–51.6% of the PM. The major organic constituents were organophosphates consisting mainly of triphenyl phosphate (TPP) and its methyl substituted compounds, methyl esters of hexadecanoic and octadecanoic acids, levoglucosan and bisphenol A. TPP and bisphenol A were present at 1–5 orders of magnitude higher than in other indoor and outdoor environments throughout the world, which implies that they might be used as potential markers for e-waste recycling. The elemental carbon, inorganic elements and ions had a minor contribution to the PM (<5% each). The inorganic elements were dominated by phosphorus and followed by crustal elements and metal elements Pb, Zn, Sn, and lesser Cu, Sb, Mn, Ni, Ba and Cd. The recycling of printed circuit boards was demonstrated as an important contributor of heavy metal contamination, particularly Cd, Pb and Ni, to the local environment. These findings suggest that this recycling method represents a strong source of PM associated with pollutants to the ambient atmosphere of an e-waste recycling locale.     

Influences of natural emission sources (wildfires and Saharan dust) on the urban organic aerosol in Barcelona (Western Mediterranean Basis) during a PM event

The urban air quality in Barcelona in the Western Mediterranean Basin is characterized by overall high particulate matter (PM) concentrations, due to intensive local anthropogenic emissions and specific meteorological conditions. Moreover, on several days, especially in summer, natural PM sources, such as long-range transported Saharan dust from Northern Africa or wildfires on the Iberian Peninsula and around the Mediterranean Basin, may influence the levels and composition of the organic aerosol. In the second half of July 2009, daily collected PM₁₀ filter samples in an urban background site in Barcelona were analyzed on organic tracer compounds representing several emission sources. During this period, an important PM peak event was observed. Individual organic compound concentrations increased two to five times during this event. Although highest increase was observed for the organic tracer of biomass burning, the contribution to the organic aerosol was estimated to be around 6?%. Organic tracers that could be related to Saharan dust showed no correlation with the PM and OC levels, while this was the case for those related to fossil fuel combustion from traffic emissions. Moreover, a change in the meteorological conditions gave way to an overall increase of the urban background contamination. Long-range atmospheric transport of organic compounds from primary emissions sources (i.e., wildfires and Saharan dust) has a relatively moderate impact on the organic aerosol in an urban area where the local emissions are dominating.     

Seasonal variations in the chemical composition of particulate matter: a case study in the Po Valley. Part I: macro-components and mass closure

The seasonal variability in the mass concentration and chemical composition of atmospheric particulate matter (PM₁₀ and PM_2.5) was studied during a 2-year field study carried out between 2010 and 2012. The site of the study was the area of Ferrara (Po Valley, Northern Italy), which is characterized by frequent episodes of very stable atmospheric conditions in winter. Chemical analyses carried out during the study allowed the determination of the main components of atmospheric PM (macro-elements, ions, elemental carbon, organic matter) and a satisfactory mass closure was obtained. Accordingly, chemical components could be grouped into the main macro-sources of PM: soil, sea spray, inorganic compounds from secondary reactions, vehicular emission, organics from domestic heating, organics from secondary formation, and other sources. The more significant seasonal variations were observed for secondary inorganic species in the fine fraction of PM; these species were very sensitive to air mass age and thus to the frequency of stable atmospheric conditions. During the winter ammonium nitrate, the single species with the highest concentration, reached concentrations as high as 30 μg/m³. The intensity of natural sources was fairly constant during the year; increases in natural aerosols were linked to medium and long-range transport episodes. The ratio of winter to summer concentrations was roughly 2 for combustion product, close to 3 for secondary inorganic species, and between 2 and 3 for organics. The winter increase of organics was due to poorer atmospheric dispersion and to the addition of the emission from domestic heating. A similar winter to summer ratio (around 3) was observed for the fine fraction of PM.     

Long-term assessment of particulate matter using CHIMERE model

Particulate matter (PM) and aerosols have became a critical pollutant and object of several research applications, due to their increasing levels, especially in urban areas, causing air pollution problems and thus effects on human health. The main purpose of this study is to perform a first long-term air quality assessment for Portugal, regarding aerosols and PM pollution. The CHIMERE chemistry-transport model, forced by the MM5 meteorological fields, was applied over Portugal for 2001 year, with 10 km horizontal resolution, using an emission inventory obtained from a spatial top-down disaggregation of the 2001 national inventory database. The evaluation model exercise shows a model trend to overestimate particulate pollution episodes (peaks) at urban sites, especially in winter season. This could be due to an underprediction of the winter model vertical mixing and also to an overestimation of PM emissions. Simulated inorganic components (ammonium and sulfate) and secondary organic aerosols (SOA) were compared to measurements taken at Aveiro (northwest coast of Portugal). An underestimation of the three components was verified. However, the model is able to predict their seasonal variation. Nevertheless, as a first approach, and despite the complex topography and coastal location of Portugal affected by sea salt natural aerosols emissions, the results obtained show that the model reproduces the PM levels, temporal evolution, and spatial patterns. The concentration maps reveal that the areas with high PM values are covered by the air quality monitoring network.     

Mass-size distributions of particulate sulfate, nitrate, and ammonium in a particulate matter nonattainment region in southern Taiwan

Concentrations and distributions of three major water-soluble ion species (sulfate, nitrate, and ammonium) contained in ambient particles were measured at three sampling sites in the Kao-ping ambient air quality basin, Taiwan. Ambient particulate matter (PM) samples were collected in a Micro-orifice Uniform Deposit Impactor from February to July 2003 and were analyzed for water-soluble ion species with an ion chromatograph. The PM1/ PM2.5 and PM1/PM10 concentration ratios at the emission source site were 0.73 and 0.53 and were higher than those (0.68 and 0.48) at the background site because there are more combustion sources (i.e., industrial boilers and traffic) around the emission source site. Mass-size distributions of PM NO3- were found in both the fine and coarse modes. SO4(2-)and NH4+ were found in the fine particle mode (PM2.5), with significant fractions of submicron particles (PM1). The source site had higher PM1/PM10(79, 42, and 90%) and PM1/PM2.5 concentration ratios (90, 58, and 93%) for the three major inorganic secondary aerosol components (SO4(2-), NO3-, and NH4+) than the receptor site (65, 27, and 65% for PM1/PM10, 69, 51, and 70% for PM1/PM2.5. Results obtained in this study indicate that the PM1 (submicron aerosol particles) fraction plays an important role in the ambient atmosphere at both emission source and receptor sites. Further studies regarding the origin and formation of ambient secondary aerosols are planned.     

Size distribution and diurnal characteristics of particle-bound metals in source and receptor sites of the Los Angeles Basin

Measurement of daily size-fractionated ambient PM₁₀ mass, metals, inorganic ions (nitrate and sulfate) and elemental and organic carbon were conducted at source (Downey) and receptor (Riverside) sites within the Los Angeles Basin. In addition to 24-h concentration measurements, the diurnal patterns of the trace element and metal content of fine (0–2.5 μm) and coarse (2.5–10 μm) PM were studied by determining coarse and fine PM metal concentrations during four time intervals of the day.The main source of crustal metals (e.g., Al, Si, K, Ca, Fe and Ti) can be attributed to the re-suspension of dust at both source and receptor sites. All the crustals are predominantly present in supermicron particles. At Downey, potentially toxic metals (e.g., Pb, Sn, Ni, Cr, V, and Ba) are predominantly partitioned (70–85%, by mass) in the submicron particles. Pb, Sn and Ba have been traced to vehicular emissions from nearby freeways, whereas Ni and Cr have been attributed to emissions from powerplants and oil refineries upwind in Long Beach. Riverside, adjacent to Southern California deserts, exhibits coarser distributions for almost all particle-bound metals as compared to Downey. Fine PM metal concentrations in Riverside seem to be a combination of few local emissions and those transported from urban Los Angeles. The majority of metals associated with fine particles are in much lower concentrations at Riverside compared to Downey. Diurnal patterns of metals are different in coarse and fine PM modes in each location. Coarse PM metal concentration trends are governed by variations in the wind speeds in each location, whereas the diurnal trends in the fine PM metal concentrations are found to be a function both of the prevailing meteorological conditions and their upwind sources.     

Routine, automated determination of inorganic and total mercury in multimedia using cold vapour atomic absorption spectrometry

A routine, automated analytical method for simultaneous determination of total and inorganic mercury by cold vapour atomic absorption spectrometry in multimedia is described. Excellent accuracy and precision results were obtained with human hair certified reference materials namely, BCR-397 and IAEA-086. The reproducibility relative standard deviation for total mercury was 4% and 22%, respectively. The limit of detection for total and inorganic mercury was 0.2 μg/g hair. The described method has been successfully applied in determination of total and inorganic mercury as well as organic mercury in human hair, urine and fish tissue samples.     

Predicting particulate (PM10) personal exposure distributions using a random component superposition statistical model

This paper presents a new statistical model designed to extend our understanding from prior personal exposure field measurements of urban populations to other cities where ambient monitoring data, but no personal exposure measurements, exist. The model partitions personal exposure into two distinct components: ambient concentration and nonambient concentration. It is assumed the ambient and nonambient concentration components are uncorrelated and add together; therefore, the model is called a random component superposition (RCS) model. The 24-hr ambient outdoor concentration is multiplied by a dimensionless "attenuation factor" between 0 and 1 to account for deposition of particles as the ambient air infiltrates indoors. The RCS model is applied to field PM10 measurement data from three large-scale personal exposure field studies: THEES (Total Human Environmental Exposure Study) in Phillipsburg, NJ; PTEAM (Particle Total Exposure Assessment Methodology) in Riverside, CA; and the Ethyl Corporation study in Toronto, Canada. Because indoor sources and activities (smoking, cooking, cleaning, the personal cloud, etc.) may be similar in similar populations, it was hypothesized that the statistical distribution of nonambient personal exposure is invariant across cities. Using a fixed 24-hr attenuation factor as a first approximation derived from regression analysis for the respondents, the distributions of nonambient PM10 personal exposures were obtained for each city. Although the mean ambient PM10 concentrations in the three cities varied from 27.9 micrograms/m3 in Toronto to 60.9 micrograms/m3 in Phillipsburg to 94.1 micrograms/m3 in Riverside, the mean nonambient components of personal exposures were found to be closer: 52.6 micrograms/m3 in Toronto; 52.4 micrograms/m3 in Phillipsburg; and 59.2 micrograms/m3 in Riverside. The three frequency distributions of the nonambient components of exposure also were similar in shape, giving support to the hypothesis that nonambient concentrations are similar across different cities and populations. These results indicate that, if the ambient concentrations were completely controlled and set to zero in all three cities, the median of the remaining personal exposures to PM10 would range from 32.0 micrograms/m3 (Toronto) to 34.4 micrograms/m3 (Phillipsburg) to 48.8 micrograms/m3 (Riverside). The highest-exposed 30% of the population in the three cities would still be exposed to 24-hr average PM10 concentrations of 47-74 micrograms/m3; the highest 20% would be exposed to concentrations of 56-92 micrograms/m3; the highest 10% to concentrations of 88-131 micrograms/m3; and the highest 5% to 133-175 micrograms/m3, due only to indoor sources and activities. The distribution for the difference between personal exposures and indoor concentrations, or the "personal cloud," also was similar in the three cities, with a mean of 30-35 micrograms/m3, suggesting that the personal cloud accounts for more than half of the nonambient component of PM10 personal exposure in the three cities. Using only the ambient measurements in Toronto, the nonambient data from THEES in Phillipsburg was used to predict the entire personal exposure distribution in Toronto. The PM10 exposure distribution predicted by the model showed reasonable agreement with the PM10 personal exposure distribution measured in Toronto. These initial results suggest that the RCS model may be a powerful tool for predicting personal exposure distributions and statistics in other cities where only ambient particle data are available.     

Cytotoxic response in human lung epithelial cells and ion characteristics of urban-air particles from Torino,a northern Italian city

Recently, much attention has been devoted to urban air pollution because epidemiological studies have reported health impacts related to particulate matter (PM). PM10 and PM2.5 were collected during different seasons in Torino, a northern Italian city, and were characterised by inorganic chemical species (secondary particulates and bio-available iron). The biological effects of aqueous and organic solvent PM extracts on human epithelial lung A549 were evaluated, and the effects on cell proliferation and lactate dehydrogenase (LDH) release were assayed. The average PM10 concentration during the sampling period was 47.9?±?18.0 μg/m³; the secondary particles accounted for 49 %?±?9 % of the PM10 total mass, and the bio-available iron concentration was 0.067?±?0.045 μg/m³. The PM2.5/PM10 ratio in Torino ranged from 0.47 to 0.90 and was higher in cold months than in warm months. The PM10 and PM2.5 extracts inhibited cell proliferation and induced LDH release in a dose-dependent manner with a seasonal trend. The PM10 extract had a stronger effect on LDH release, whereas the PM2.5 extract more strongly inhibited cell proliferation. No significant differences were observed in the effects induced by the two extracts, and no significant correlations were found between the biological effects and the PM components evaluated in this study, thus emphasising the importance of the entire mixture in inducing a cytotoxic response.     

Utilization of selected area electron diffraction patterns for characterization of air submicron particulate matter collected by a thermophoretic precipitator

A thermophoretic precipitator (TP) that uses a novelty of direct sampling of ambient air particulate matter (PM) onto transmission electron microscopy (TEM) grids was designed and utilized to determine its potential applicability for the collection and consequent qualitative analyses of representative PM in the air, especially those with aerodynamic diameter less than 1 microm (PM1.0). After a calibration process, preliminary field tests were performed under different weather conditions, locations, and time frames. TEM, selected area electron diffraction (SAED), and electron energy-dispersive X-ray spectrometry (EDS) analyses were performed on individual samples, and chemical species were analyzed. During this investigation, individual air PM with different sizes ranging from 10 microm to 10 nm for TEM analysis was collected. Two observations were made: (1) a large fraction of collected particulates were aggregates of very small particles of both organic and inorganic origin, and (2) a large fraction of the collected particulates were crystalline or polycrystalline. This study has demonstrated, by utilization of SAED patterns from TEM on air particles collected by a TP, the potential to analyze and identify individual air PM in a nanometer regime qualitatively by combining SAED and EDS data.     

Semi-volatile species in PM2.5: comparison of integrated and continuous samplers for PM2.5 research or monitoring

Fine particles in urban atmospheres contain substantial quantities of semi-volatile material [e.g., NH4NO3 and semi-volatile organic compounds (SVOCs)] that are lost from particles during collection on a filter. Several diffusion denuder samplers have been developed for the determination of both NO3- and organic semi-volatile fine particulate components. The combination of technology used in the BOSS diffusion denuder sampler and the Harvard particle concentrator has resulted in the Particle Concentrator-Brigham Young University Organic Sampling System (PC-BOSS) for the 24-hr (or less) integrated collection of PM2.5, including NH4NO3 and semi-volatile organic material. Modification of the BOSS sampler allows for the weekly determination of these same species. Combination of BOSS denuder and tapered element oscillating microbalance (TEOM) monitor technology has resulted in the real-time ambient mass sampler (RAMS) for the continuous measurement of PM2.5, including the semi-volatile components. Comparison of the results obtained with the BOSS and with each of the newly developed modifications of the BOSS indicates that the modified versions can be used for the continuous, daily, or weekly monitoring of PM2.5, including semi-volatile species, as appropriate to the design of each sampler.     

The impact of infield biomass burning on PM levels and its chemical composition

In the South of Italy, it is common for farmers to burn pruning waste from olive trees in spring. In order to evaluate the impact of the biomass burning source on the physical and chemical characteristics of the particulate matter (PM) emitted by these fires, a PM monitoring campaign was carried out in an olive grove. Daily PM10 samples were collected for 1 week, when there were no open fires, and when biomass was being burned, and at two different distances from the fires. Moreover, an optical particle counter and a polycyclic aromatic hydrocarbon (PAH) analyzer were used to measure the high time-resolved dimensional distribution of particles emitted and total PAHs concentrations, respectively. Chemical analysis of PM10 samples identified organic and inorganic components such as PAHs, ions, elements, and carbonaceous fractions (OC, EC). Analysis of the collected data showed the usefulness of organic and inorganic tracer species and of PAH diagnostic ratios for interpreting the impact of biomass fires on PM levels and on its chemical composition. Finally, high time-resolved monitoring of particle numbers and PAH concentrations was performed before, during, and after biomass burning, and these concentrations were seen to be very dependent on factors such as weather conditions, combustion efficiency, and temperature (smoldering versus flaming conditions), and moisture content of the wood burned.     

西安采暖期PM2.5及其水溶性无机离子的时段分布特征

为了探讨西安市采暖期大气颗粒物PM2.5及其水溶性无机成分的污染水平,于2010年1月4日—2月1日按一天8个时段(每个时段3 h)连续采集PM2.5样品四周,每周更换一次滤膜。结果显示,西安市采暖期PM2.5的质量浓度时段差异较大,呈现明显的双峰分布特征:21:00—24:00时段(147.516μg/m3)和09:00—12:00时段(141.678μg/m3)。4种被测水溶性无机组分总浓度为39.801μg/m3,占PM2.5总浓度的30.5%。SO24-和NO3-是最主要组分,占到4种无机组分的86.2%。各离子间相关分析显示,Cl-只与NO3-有较强的相关性,表明机动车尾气对Cl-有较大的贡献。SO24-和NO3-时段分布规律较为相似,与PM2.5浓度的时段分布特征相反:在PM2.5污染最轻的15:00—18:00时段,SO24-和NO3-的相对含量达到一天中的最高浓度时段,而在PM2.5双峰时段,它们的含量有所降低。     

Size and composition distributions of particulate matter emissions: part 2--heavy-duty diesel vehicles

Particulate matter (PM) emissions from heavy-duty diesel vehicles (HDDVs) were collected using a chassis dynamometer/dilution sampling system that employed filter-based samplers, cascade impactors, and scanning mobility particle size (SMPS) measurements. Four diesel vehicles with different engine and emission control technologies were tested using the California Air Resources Board Heavy Heavy-Duty Diesel Truck (HHDDT) 5 mode driving cycle. Vehicles were tested using a simulated inertial weight of either 56,000 or 66,000 lb. Exhaust particles were then analyzed for total carbon, elemental carbon (EC), organic matter (OM), and water-soluble ions. HDDV fine (< or =1.8 microm aerodynamic diameter; PM1.8) and ultrafine (0.056-0.1 microm aerodynamic diameter; PM0.1) PM emission rates ranged from 181-581 mg/km and 25-72 mg/km, respectively, with the highest emission rates in both size fractions associated with the oldest vehicle tested. Older diesel vehicles produced fine and ultrafine exhaust particles with higher EC/OM ratios than newer vehicles. Transient modes produced very high EC/OM ratios whereas idle and creep modes produced very low EC/OM ratios. Calcium was the most abundant water-soluble ion with smaller amounts of magnesium, sodium, ammonium ion, and sulfate also detected. Particle mass distributions emitted during the full 5-mode HDDV tests peaked between 100-180 nm and their shapes were not a function of vehicle age. In contrast, particle mass distributions emitted during the idle and creep driving modes from the newest diesel vehicle had a peak diameter of approximately 70 nm, whereas mass distributions emitted from older vehicles had a peak diameter larger than 100 nm for both the idle and creep modes. Increasing inertial loads reduced the OM emissions, causing the residual EC emissions to shift to smaller sizes. The same HDDV tested at 56,000 and 66,000 lb had higher PM0.1 EC emissions (+22%) and lower PM0.1 OM emissions (-38%) at the higher load condition.     

Emissions from charbroiling and grilling of chicken and beef

Emission rates for fine particle (<2.5 microm) mass (PM2.5), carbon (organic/elemental), inorganic ions (SO4(2-), NO3-, NH4+), elements (primarily metals), and speciated organic compounds are reported for charbroiling hamburger, steak, and chicken. The PM2.5 rates for charbroiling meats ranged from 4.4 to 11.6 g/kg of uncooked meat in this study. No mass-emission rates are available from grilling, but the speciated organic data are available for these samples. Emission rates varied by type of appliance, meat, meat-fat content, and cooking conditions. High-fat hamburger cooked on an underfired charbroiler emitted the highest amount of PM2.5. The emissions were almost exclusively composed of organic carbon, with small amounts of elements and inorganic ions. Water-soluble K+ and Cl-, which are used as indicators of wood smoke in source apportionment studies, were also present in meat-cooking emissions. The speciated organic compounds that were measured include polycyclic aromatic hydrocarbons (PAHs), cholesterol, and the long-chain gamma-lactones. Charbroiling emissions yielded an average of approximately 3-5 times more PAHs, approximately 20 times more cholesterol, and approximately 10 times more lactones than grilling. These data were utilized in the ambient source apportionment analysis for the 1997 Northern Front Range Air Quality Study source apportionment.