Optical remote sensing to quantify fugitive particulate mass emissions from stationary short-term and mobile continuous sources: part II. Field applications

Quantification of emissions of fugitive particulate matter (PM) into the atmosphere from military training operations is of interest by the United States Department of Defense. A new range-resolved optical remote sensing (ORS) method was developed to quantify fugitive PM emissions from puff sources (i.e., artillery back blasts), ground-level mobile sources (i.e., movement of tracked vehicles), and elevated mobile sources (i.e., airborne helicopters) in desert areas that are prone to generating fugitive dust plumes. Real-time, in situ mass concentration profiles for PM mass with particle diameters <10 μm (PM(10)) and <2.5 μm (PM(2.5)) were obtained across the dust plumes that were generated by these activities with this new method. Back blasts caused during artillery firing were characterized as a stationary short-term puff source whose plumes typically dispersed to <10 m above the ground with durations of 10-30 s. Fugitive PM emissions caused by artillery back blasts were related to the zone charge and ranged from 51 to 463 g PM/firing for PM(10) and 9 to 176 g PM/firing for PM(2.5). Movement of tracked vehicles and flying helicopters was characterized as mobile continuous sources whose plumes typically dispersed 30-50 m above the ground with durations of 100-200 s. Fugitive PM emissions caused by moving tracked vehicles ranged from 8.3 to 72.5 kg PM/km for PM(10) and 1.1 to 17.2 kg PM/km for PM(2.5), and there was no obvious correlation between PM emission and vehicle speed. The emission factor for the helicopter flying at 3 m above the ground ranged from 14.5 to 114.1 kg PM/km for PM(10) and 5.0 to 39.5 kg PM/km for PM(2.5), depending on the velocity of the helicopter and type of soil it flies over. Fugitive PM emissions by an airborne helicopter were correlated with helicopter speed for a particular soil type. The results from this range-resolved ORS method were also compared with the data obtained with another path-integrated ORS method and a Flux Tower method.     

Current and future linked responses of ozone and PM2.5 to emission controls

Responses of ozone and PM2.5 to emission changes are coupled because of interactions between their precursors. Here we show the interdependencies of ozone and PM2.5 responses to emission changes in 2001 and 2050, with the future case accounting for both currently planned emission controls and climate change. Current responses of ozone and PM2.5 to emissions are quantified and linked on a daily basis for five cities in the continental United States: Atlanta, Chicago, Houston, Los Angeles, and NewYork. Reductions in anthropogenic NO(x) emissions decrease 24-h average PM2.5 levels but may either increase or decrease daily maximum 8-h average ozone levels. Regional ozone maxima for all the cities are more sensitive to NO(x) reductions than at the city center, particularly in New York and Chicago. Planned controls of anthropogenic NO(x) emissions lead to more positive responses to NO(x) reductions in the future. Sensitivities of ozone and PM2.5 to anthropogenic VOC emissions are predicted to decrease between 2001 and 2050. Ammonium nitrate formation is predicted to be less ammonia-sensitive in 2050 than 2001 while the opposite is true for ammonium sulfate. Sensitivity of PM2.5 to SO2 and NO(x) emissions changes little between 2001 and 2050. Both ammonium sulfate and ammonium nitrate are predicted to decrease in sensitivity to SO2 and NO(x) emissions between 2001 and 2050. The complexities, linkages, and daily changes in the pollutant responses to emission changes suggest that strategies developed to meet specific air quality standards should consider other air quality impacts as well.     

How does infiltration behavior modify the composition of ambient PM2.5 in indoor spaces? An analysis of RIOPA data

The indoor environment is an important venue for exposure to fine particulate matter (PM2.5) of ambient (outdoor) origin. In this work, paired indoor and outdoor PM2.5 species concentrations from three geographically distinct cities (Houston, TX, Los Angeles County, CA, and Elizabeth, NJ) were analyzed using positive matrix factorization (PMF) and demonstrate that the composition and source contributions of ambient PM2.5 are substantially modified by outdoor-to-indoor transport. Our results suggest that predictions of "indoor PM2.5 of ambient origin" are improved when ambient PM2.5 is treated as a combination of four distinct particle types with differing infiltration behavior (primary combustion, secondary sulfate and organics, secondary nitrate, and mechanically generated PM) rather than as a "single internally mixed entity". Study-wide average infiltration factors (i.e., fraction of ambient PM2.5 found indoors) for Relationship of Indoor, Outdoor, and Personal Air (RIOPA) study homes were 0.51, 0.78, and 0.04 (consistent with P = 0.6, 0.9, and 0.09; k = 0.2, 0.1, and 0.6 h(-1)) for PM2.5 associated with primary combustion, secondary formation (excluding nitrate), and mechanical generation, respectively. Modification of the composition, properties, and source contributions of ambient PM2.5 in indoor environments has important implications for exposure mitigation strategies, development of health hypotheses, and evaluation of exposure error in epidemiological studies that use ambient central-site PM2.5 as a surrogate for PM2.5 exposure.     

Lanthanoid geochemistry of urban atmospheric particulate matter

Relatively little is known about the lanthanoid element (La to Lu) chemistry of inhalable urban atmospheric particulate matter (PM). PM samples collected during an air sampling campaign in the Mexico City area contain lanthanoid concentrations of mostly 1-10 ng m(-3), increasing with mass where resuspension of crustal PM is important (low PM2.5/PM10), but not where fine emissions from traffic and industry dominate (high PM2.5/ PM10). Samples show anthropogenic enrichment of lighter over heavier lanthanoids, and Ce enrichment relative to La and Sm occurs in the city center (especially PM10) possibly due to PM from road vehicle catalytic converters. La is especially enriched, although many samples show low La/V values (< 0.11), suggesting the dominating influence of fuel oil combustion sources rather than refinery emissions. We use La/Sm v La/ Ce, LaCeSm, and LaCeV plots to compare Mexico City aerosols with PM from other cities. Lanthanoid aerosol geochemistry can be used not only to identify refinery pollution events, but also as a marker for different hydrocarbon combustion emissions (e.g., oil or coal power stations) on urban background atmospheric PM.     

n-alkane profiles of engine lubricating oil and particulate matter by molecular sieve extraction

As part of the Canadian Atmospheric Fine Particle Research Program to obtain reliable primary source emission profiles, a molecular sieve method was developed to reliably determine n-alkanes in lubricating oils, vehicle emissions, and mobile source dominated ambient particulate matter (PM). This work was also initiated to better calculate carbon preference index values (CPI: the ratio of the sums of odd over even n-alkanes), a parameter for estimating anthropogenic versus biogenic contributions in PM. n-Alkanes in lubricating oil and mobile source dominated PM are difficult to identify and quantify by gas chromatography due to the presence of similar components that cannot be fully resolved. This results in a hump, the unresolved complex mixture (UCM) that leads to incorrect n-alkane concentrations and CPI values. The sieve method yielded better chromatography, unambiguous identification of n-alkanes and allowed examination of differences between n-alkane profiles in light (LDV) and heavy duty vehicle (HDV) lubricating oils that would have been otherwise difficult. These profile differences made it possible to relate the LDV profile to that of the PM samples collected during a tunnel study in August 2001 near Vancouver (British Columbia, Canada). The n-alkane PM data revealed that longer sampling times result in a negative artifact, i.e., the desorption of the more volatile n-alkanes from the filters. Furthermore, the sieve procedure yielded n-alkane data that allowed calculation of accurate CPI values for lubricating oils and PM samples. Finally, this method may prove helpful in estimating the respective diesel and gasoline contributions to ambient PM.     

Optimization-based source apportionment of PM2.5 incorporating gas-to-particle ratios

A modified approach to PM2.5 source apportionment is developed, using source indicative SO2/PM2.5, CO/PM2.5, and NOx/PM2.5 ratios as constraints, in addition to the commonly used particulate-phase source profiles. Additional information from using gas-to-particle ratios assists in reducing collinearity between source profiles, a problem that often limits the source-identification capabilities and accuracy of traditional receptor models. This is especially true in the absence of speciated organic carbon measurements. In the approach presented here, the solution is based on a global optimization mechanism, minimizing the weighted error between apportioned and ambient levels of PM2.5 components, while introducing constraints on calculated source contributions that ensure that the ambient gas-phase pollutants (SO2, CO, and NOy) are reasonable. This technique was applied to a 25-month dataset of daily PM2.5 measurements (total mass and composition) at the Atlanta Jefferson Street SEARCH site. Results indicate that this technique was able to split the contributions of mobile sources (gasoline and diesel vehicles) more accurately than particulate-phase source apportionment methods. Furthermore, this technique was able to better quantify the direct contribution (primary PM2.5) of coal-fired power plants to ambient PM2.5 levels.     

Source contributions to atmospheric gases and particulate matter in the southeastern United States

A new approach for determining the contributions of emission sources to concentrations of particulate matter and gases is developed using the chemical mass balance (CMB) method and the U.S. EPA's National Emission Inventory (NEI). The approach apportions combined gas-phase and condensed-phase concentrations of individual compounds as well as PM(2.5) mass. Because the NEI is used to provide source emission profiles for CMB analysis, the method generates information on the consistency of the NEI with ambient monitoring data. The method also tracks secondary species to primary source emissions, permitting a more complete accounting of the impact of aggregated source types on PM(2.5) mass concentrations. An example application is presented using four years of monitoring data collected at eight sites in the Southeastern Aerosol Research and Characterization (SEARCH) network. Including both primary and secondary species, area sources contributed 2.0-3.7 μg m(-3) (13-26%), point sources contributed 3.0-4.6 μg m(-3) (22-33%), and mobile sources contributed 1.0-6.0 μg m(-3) (9-42%) to mean PM(2.5) mass concentrations. Whereas the NEI generally accounts for the ambient concentrations of gases and particles, certain anomalies are identified, especially related to carbonaceous compounds and dust.     

Size-resolved emissions of organic tracers from light- and heavy-duty vehicles measured in a California roadway tunnel

Individual organic compounds found in particulate emissions from vehicles have proven useful in source apportionment of ambient particulate matter. Species of interest include the hopanes, originating in lube oil, and selected PAHs generated via combustion. Most efforts to date have focused on emissions and apportionment PM10 or PM2.5 However, examining how these compounds are segregated by particle size in both emissions and ambient samples will help efforts to apportion size-resolved PM, especially ultrafine particles which have been shown to be more potent toxicologically. To this end, high volume size-resolved (coarse, accumulation, and ultrafine) PM samples were collected inside the Caldecott tunnel in Orinda, California to determine the relative emission factors for these compounds in different size ranges. Sampling occurred in two bores, one off-limits to heavy-duty diesel vehicles, which allows determination of the different emissions profiles for diesel and gasoline vehicles. Although tunnel measurements do not measure emissions over a full engine duty cycle, they do provide an average emissions profile over thousands of vehicles that can be considered characteristic of "freeway" emissions. Results include size-fractionated emission rates for hopanes, PAHs, elemental carbon, and other potential organic markers apportioned to diesel and gasoline vehicles. The results are compared to previously conducted PM2.5 emissions testing using dynamometer facilities and othertunnel environments.     

Climate and health relevant emissions from in-use Indian three-wheelers fueled by natural gas and gasoline

Auto-rickshaws in India use different fuels and engine technologies, with varying emissions and implications for air quality and climate change. Chassis dynamometer emission testing was conducted on 30 in-use auto-rickshaws to quantify the impact of switching from gasoline to compressed natural gas (CNG) in spark-ignition engines. Thirteen test vehicles had two-stroke CNG engines (CNG-2S) and 17 had four-stroke CNG engines (CNG-4S), of which 11 were dual-fuel and operable on a back-up gasoline (petrol) system (PET-4S). Fuel-based emission factors were determined for gaseous pollutants (CO(2), CH(4), NO(X), THC, and CO) and fine particulate matter (PM(2.5)). Intervehicle variability was high, and for most pollutants there was no significant difference (95% confidence level) between "old" (1998-2001) and "new" (2007-2009) age-groups within a given fuel-technology class. Mean fuel-based PM(2.5) emission factor (mean (95% confidence interval)) for CNG-2S (14.2 g kg(-1) (6.2-26.7)) was almost 30 times higher than for CNG-4S (0.5 g kg(-1) (0.3-0.9)) and 12 times higher than for PET-4S (1.2 g kg(-1) (0.8-1.7)). Global warming commitment associated with emissions from CNG-2S was more than twice that from CNG-4S or PET-4S, due mostly to CH(4) emissions. Comprehensive measurements and data should drive policy interventions rather than assumptions about the impacts of clean fuels.     

Regional air quality: local and interstate impacts of NO(x) and SO2 emissions on ozone and fine particulate matter in the eastern United States

While the U.S. air quality management system is largely designed and managed on a state level, many critical air quality problems are now recognized as regional. In particular, concentrations of two secondary pollutants, ozone and particulate matter, are often above regulated levels and can be dependent on emissions from upwind states. Here, impacts of statewide emissions on concentrations of local and downwind states' ozone and fine particulate matter are simulated for three seasonal periods in the eastern United States using a regional Eulerian photochemical model. Impacts of ground level NO(x) (e.g., mobile and area sources), elevated NO(x) (e.g., power plants and large industrial sources), and SO2 emissions are examined. An average of 77% of each state's ozone and PM(2.5) concentrations that are sensitive to the emissions evaluated here are found to be caused by emissions from other states. Delaware, Maryland, New Jersey, Virginia, Kentucky, and West Virginia are shown to have high concentrations of ozone and PM(2.5) caused by interstate emissions. When weighted by population, New York receives increased interstate contributions to these pollutants and contributions to ozone from local emissions are generally higher. When accounting for emission rates, combined states from the western side of the modeling domain and individual states such as Illinois, Tennessee, Indiana, Kentucky, and Georgia are major contributors to interstate ozone. Ohio, Indiana, Tennessee, Kentucky, and Illinois are the major contributors to interstate PM(2.5). When accounting for an equivalent mass of emissions, Tennessee, Kentucky, West Virginia, Virginia, and Alabama contribute large fractions of these pollutants to other states.     

Intake fraction for particulate matter: recommendations for life cycle impact assessment

Particulate matter (PM) is a significant contributor to death and disease globally. This paper summarizes the work of an international expert group on the integration of human exposure to PM into life cycle impact assessment (LCIA), within the UNEP/SETAC Life Cycle Initiative. We review literature-derived intake fraction values (the fraction of emissions that are inhaled), based on emission release height and "archetypal" environment (indoor versus outdoor; urban, rural, or remote locations). Recommended intake fraction values are provided for primary PM(10-2.5) (coarse particles), primary PM(2.5) (fine particles), and secondary PM(2.5) from SO(2), NO(x), and NH(3). Intake fraction values vary by orders of magnitude among conditions considered. For outdoor primary PM(2.5), representative intake fraction values (units: milligrams inhaled per kilogram emitted) for urban, rural, and remote areas, respectively, are 44, 3.8, and 0.1 for ground-level emissions, versus 26, 2.6, and 0.1 for an emission-weighted stack height. For outdoor secondary PM, source location and source characteristics typically have only a minor influence on the magnitude of the intake fraction (exception: intake fraction values can be an order of magnitude lower for remote-location emission than for other locations). Outdoor secondary PM(2.5) intake fractions averaged over respective locations and stack heights are 0.89 (from SO(2)), 0.18 (NO(x)), and 1.7 (NH(3)). Estimated average intake fractions are greater for primary PM(10-2.5) than for primary PM(2.5) (21 versus 15), owing in part to differences in average emission height (lower, and therefore closer to people, for PM(10-2.5) than PM(2.5)). For indoor emissions, typical intake fraction values are ～1000-7000. This paper aims to provide as complete and consistent an archetype framework as possible, given current understanding of each pollutant. Values presented here facilitate incorporating regional impacts into LCIA for human health damage from PM.     

Impact of the 2002 Canadian forest fires on particulate matter air quality in Baltimore city

With increasing evidence of adverse health effects associated with particulate matter (PM), the exposure impact of natural sources, such as forest fires, has substantial public health relevance. In addition to the threat to nearby communities, pollutants released from forest fires can travel thousands of kilometers to heavily populated urban areas. There was a dramatic increase in forest fire activity in the province of Quebec, Canada, during July 2002. The transport of PM released from these forest fires was examined using a combination of a moderate-resolution imaging spectroradiometer satellite image, back-trajectories using a hybrid single-particle Lagrangian integrated trajectory, and local light detection and ranging measurements. Time- and size-resolved PM was evaluated at three ambient and four indoor measurement sites using a combination of direct reading instruments (laser, time-of-flight aerosol spectrometer, nephelometer, and an oscillating microbalance). The transport and monitoring results consistently identified a forest fire related PM episode in Baltimore that occurred the first weekend of July 2002 and resulted in as much as a 30-fold increase in ambientfine PM. On the basis of tapered element oscillating microbalance measurements, the 24 h PM25 concentration reached 86 microg/m3 on July 7, 2002, exceeding the 24 h national ambient air quality standard. The episode was primarily comprised of particles less than 2.5 microm in aerodynamic diameter, highlighting the preferential transport of the fraction of PM that is of greatest health concern. Penetration of the ambient episode indoors was efficient (median indoor-to-outdoor ratio 0.91) such that the high ambient levels were similarly experienced indoors. These results are significant in demonstrating the impact of a natural source thousands of kilometers away on ambient levels of and potential exposures to air pollution within an urban center. This research highlights the significance of transboundary air pollution and the need for studies that assess the public health impacts associated with such sources and transport processes.     

Sensitivities of ozone and fine particulate matter formation to emissions under the impact of potential future climate change

Impact of climate change alone and in combination with currently planned emission control strategies are investigated to quantify effectiveness in decreasing regional ozone and PM2.5 over the continental U.S. using MM5, SMOKE, and CMAQ with DDM-3D. Sensitivities of ozone and PM2.5 formation to precursor emissions are found to change only slightly in response to climate change. In many cases, mass per ton sensitivities to NO(x) and SO2 controls are predicted to be greater in the future due to both the lower emissions as well as climate, suggesting that current control strategies based on reducing such emissions will continue to be effective in decreasing ground-level ozone and PM2.5 concentrations. SO2 emission controls are predicted to be most beneficial for decreasing summertime PM2.5 levels, whereas controls of NO(x) emissions are effective in winter. Spatial distributions of sensitivities are also found to be only slightly affected assuming no changes in land-use. Contributions of biogenic VOC emissions to PM2.5 formation are simulated to be more important in the future because of higher temperatures, higher biogenic emissions, and lower anthropogenic NO(x) and SO2 emissions.     

Air quality impacts from prescribed forest fires under different management practices

Large amounts of air pollutants are emitted during prescribed forest fires. Such emissions and corresponding air quality impacts can be modulated by different forest management practices. The impacts of changing burning seasons and frequencies and of controlling emissions during smoldering on regional air quality in Georgia are quantified using source-oriented air quality modeling, with modified emissions from prescribed fires reflecting effects of each practice. Equivalent fires in the spring and winter are found to have a greater impact on PM2.5 than those in summer, though ozone impacts are larger from spring and summer fires. If prescribed fires are less frequent more biofuel is burnt in each fire, leading to larger emissions and air quality impacts per fire. For example, emissions from a fire with a 5-year fire return interval (FRI) are 72% larger than those from a fire of the same acreage with a 2-year FRI. However, corresponding long-term regional impacts are reduced with the longer FRI since the annual burned area is reduced. Total emissions for fires in Georgia with a 5-year FRI are 32% less than those with a 2-year FRI. Smoldering emissions can lead to approximately 1.0 or 1.9 microg/m3 of PM2.5 in the Atlanta PM2.5 nonattainment area during March 2002.     

Diagnosis of aged prescribed burning plumes impacting an urban area

An unanticipated wind shift led to the advection of plumes from two prescribed burning sites that impacted Atlanta, GA, producing a heavy smoke event late in the afternoon on February 28, 2007. Observed PM2.5 concentrations increased to over 140 microg/m3 and O3 concentrations up to 30 ppb in a couple of hours, despite the late hour in February when photochemistry is less vigorous. A detailed investigation of PM2.5 chemical composition and source apportionment analysis showed that the increase in PM2.5 mass was driven mainly by organic carbon (OC). However, both results from source apportionment and an observed nonlinear relationship between OC and PM2.5 potassium (K) indicate that the increased OC was not due solely to primary emissions. Most of the OC was water-soluble organic carbon (WSOC) and was dominated by hydrophobic compounds. The data are consistent with large enhancements in isoprenoid (isoprene and monoterpenes) and other volatile organic compounds emitted from prescribed burning that led to both significant O3 and secondary organic aerosol (SOA) production. Formation of oligomers from oxidation products of isoprenoid compounds or condensation of volatile organic compounds (VOCs) with multiple functional groups emitted during prescribed burning appears to be a major component of the secondary organic contributor of the SOA. The results from this study imply that enhanced emissions due to the fire itself and elevated temperature in the burning region should be considered in air quality models (e.g., receptor and emission-based models) to assess impacts of prescribed burning emissions on ambient air quality.     

Characterization and source apportionment of particulate matter < or = 2.5 micrometer in Sumatra, Indonesia, during a recent peat fire episode

An intensive field study was conducted in Sumatra, Indonesia, during a peat fire episode to investigate the physical and chemical characteristics of particulate emissions in peat smoke and to provide necessary data for source-receptor analyses. Ambient air sampling was carried out at three different sites located at varying distances from the peatfires to determine changes in mass and number concentrations of PM2.5 and its chemical composition (carbonaceous and nitrogenous materials, polycyclic aromatic hydrocarbons, water-soluble inorganic and organic ions, and total and water-soluble metals). The three sites represent a rural site directly affected by the local peat combustion, a semirural site, and an urban site situated downwind of the peat fires. The mass concentration of PM2.5 and the number concentration of airborne particles were as high as 1600 microg/m3 and 1.7 x 10(5) cm(-3), respectively, in the vicinity of peat fires. The major components of PM2.5 in peat smoke haze were carbonaceous particles, particularly organic carbon, NO3-, and SO4(2-), while the less abundant constituents included ions such as NH4+, NO2-, Na+, K+, organic acids, and metals such as Al, Fe, and Ti. Source apportionment by chemical mass balance receptor modeling indicates that peat smoke can travel long distances and significantly affect the air quality at locations downwind.     

Electric vehicles in China: emissions and health impacts

E-bikes in China are the single largest adoption of alternative fuel vehicles in history, with more than 100 million e-bikes purchased in the past decade and vehicle ownership about 2× larger for e-bikes as for conventional cars; e-car sales, too, are rapidly growing. We compare emissions (CO(2), PM(2.5), NO(X), HC) and environmental health impacts (primary PM(2.5)) from the use of conventional vehicles (CVs) and electric vehicles (EVs) in 34 major cities in China. CO(2) emissions (g km(-1)) vary and are an order of magnitude greater for e-cars (135-274) and CVs (150-180) than for e-bikes (14-27). PM(2.5) emission factors generally are lower for CVs (gasoline or diesel) than comparable EVs. However, intake fraction is often greater for CVs than for EVs because combustion emissions are generally closer to population centers for CVs (tailpipe emissions) than for EVs (power plant emissions). For most cities, the net result is that primary PM(2.5) environmental health impacts per passenger-km are greater for e-cars than for gasoline cars (3.6× on average), lower than for diesel cars (2.5× on average), and equal to diesel buses. In contrast, e-bikes yield lower environmental health impacts per passenger-km than the three CVs investigated: gasoline cars (2×), diesel cars (10×), and diesel buses (5×). Our findings highlight the importance of considering exposures, and especially the proximity of emissions to people, when evaluating environmental health impacts for EVs.     

Contribution of lubricating oil to particulate matter emissions from light-duty gasoline vehicles in Kansas City

The contribution of lubricating oil to particulate matter (PM) emissions representative of the in-use 2004 light-duty gasoline vehicles fleet is estimated from the Kansas City Light-Duty Vehicle Emissions Study (KCVES). PM emissions are apportioned to lubricating oil and gasoline using aerosol-phase chemical markers measured in PM samples obtained from 99 vehicles tested on the California Unified Driving Cycle. The oil contribution to fleet-weighted PM emission rates is estimated to be 25% of PM emission rates. Oil contributes primarily to the organic fraction of PM, with no detectable contribution to elemental carbon emissions. Vehicles are analyzed according to pre-1991 and 1991-2004 groups due to differences in properties of the fitting species between newer and older vehicles, and to account for the sampling design of the study. Pre-1991 vehicles contribute 13.5% of the KC vehicle population, 70% of oil-derived PM for the entire fleet, and 33% of the fuel-derived PM. The uncertainty of the contributions is calculated from a survey analysis resampling method, with 95% confidence intervals for the oil-derived PM fraction ranging from 13% to 37%. The PM is not completely apportioned to the gasoline and oil due to several contributing factors, including varied chemical composition of PM among vehicles, metal emissions, and PM measurement artifacts. Additional uncertainties include potential sorption of polycyclic aromatic hydrocarbons into the oil, contributions of semivolatile organic compounds from the oil to the PM measurements, and representing the in-use fleet with a limited number of vehicles.     

Measurements of size-segregated emission particles by a sampling system based on the cascade impactor

A special sampling system for measurements of size-segregated particles directly at the source of emission was designed and constructed. The central part of this system is a low-pressure cascade impactor with 10 collection stages for the size ranges between 15 nm and 16 microm. Its capability and suitability was proven by sampling particles atthe stack (100 degrees C) of a coal-fired power station in Slovenia. These measurements showed very reasonable results in comparison with a commercial cascade impactor for PM10 and PM2.5 and with a plane device for total suspended particulate matter (TSP). The best agreement with the measurements made by a commercial impactor was found for concentrations of TSP above 10 mg m(-3), i.e., the average PM2.5/PM10 ratios obtained by a commercial impactor and by our impactor were 0.78 and 0.80, respectively. Analysis of selected elements in size-segregated emission particles additionally confirmed the suitability of our system. The measurements showed that the mass size distributions were generally bimodal, with the most pronounced mass peak in the 1-2 microm size range. The first results of elemental mass size distributions showed some distinctive differences in comparison to the most common ambient anthropogenic sources (i.e., traffic emissions). For example, trace elements, like Pb, Cd, As, and V, typically related to traffic emissions, are usually more abundant in particles less than 1 microm in size, whereas in our specific case they were found at about 2 microm. Thus, these mass size distributions can be used as a signature of this source. Simultaneous measurements of size-segregated particles at the source and in the surrounding environment can therefore significantly increase the sensitivity of the contribution of a specific source to the actual ambient concentrations.     

Ammonia emission controls as a cost-effective strategy for reducing atmospheric particulate matter in the Eastern United States

Current regulation aimed at reducing inorganic atmospheric fine particulate matter (PM2.5) is focused on reductions in sulfur dioxide (SO2) and oxides of nitrogen (NO(x) = NO + NO2); however, controls on these pollutants are likely to increase in cost and decrease in effectiveness in the future. A supplementary strategy is reduction in ammonia (NH3) emissions, yet an evaluation of controls on ammonia has been limited by uncertainties in emission levels and in the cost of control technologies. We use state of the science emission inventories, an emission-based regional air quality model, and an explicit treatment of uncertainty to estimate the cost-effectiveness and uncertainty of ammonia emission reductions on inorganic particulate matter in the Eastern United States. Since a paucity of data on agricultural operations precludes a direct calculation of the costs of ammonia control, we calculate the "ammonia savings potential", defined as the minimum cost of applying SO2 and NO(x) emission controls in order to achieve the same reduction in ambient inorganic PM2.5 concentration as obtained from a 1 ton decrease in ammonia emissions. Using 250 scenarios of NH3, SO2, and NO(x) emission reductions, we calculate the least-cost SO2 and NO(x) control scenarios that achieve the same reduction in ambient inorganic PM2.5 concentration as a decrease in ammonia emissions. We find that the lower-bound ammonia savings potential in the winter is $8,000 per ton NH3; therefore, many currently available ammonia control technologies are cost-effective compared to current controls on SO2 and NO(x) sources. Larger reductions in winter inorganic particulate matter are available at lower cost through controls on ammonia emissions.