Overview of surface measurements and spatial characterization of submicrometer particulate matter during the DISCOVER-AQ 2013 campaign in Houston,TX

The sources of submicrometer particulate matter (PM₁) remain poorly characterized in the industrialized city of Houston, TX. A mobile sampling approach was used to characterize PM₁ composition and concentration across Houston based on high-time-resolution measurements of nonrefractory PM₁ and trace gases during the DISCOVER-AQ Texas 2013 campaign. Two pollution zones with marked differences in PM₁ levels, character, and dynamics were established based on cluster analysis of organic aerosol mass loadings sampled at 16 sites. The highest PM₁ mass concentrations (average 11.6 ± 5.7 µg/m³) were observed to the northwest of Houston (zone 1), dominated by secondary organic aerosol (SOA) mass likely driven by nighttime biogenic organonitrate formation. Zone 2, an industrial/urban area south/east of Houston, exhibited lower concentrations of PM₁ (average 4.4 ± 3.3 µg/m³), significant organic aerosol (OA) aging, and evidence of primary sulfate emissions. Diurnal patterns and backward-trajectory analyses enable the classification of airmass clusters characterized by distinct PM sources: biogenic SOA, photochemical aged SOA, and primary sulfate emissions from the Houston Ship Channel. Principal component analysis (PCA) indicates that secondary biogenic organonitrates primarily related with monoterpenes are predominant in zone 1 (accounting for 34% of the variability in the data set). The relevance of photochemical processes and industrial and traffic emission sources in zone 2 also is highlighted by PCA, which identifies three factors related with these processes/sources (~50% of the aerosol/trace gas concentration variability). PCA reveals a relatively minor contribution of isoprene to SOA formation in zone 1 and the absence of isoprene-derived aerosol in zone 2. The relevance of industrial amine emissions and the likely contribution of chloride-displaced sea salt aerosol to the observed variability in pollution levels in zone 2 also are captured by PCA.

Implications: This article describes an urban-scale mobile study to characterize spatial variations in submicrometer particulate matter (PM₁) in greater Houston. The data set indicates substantial spatial variations in PM₁ sources/chemistry and elucidates the importance of photochemistry and nighttime oxidant chemistry in producing secondary PM₁. These results emphasize the potential benefits of effective control strategies throughout the region, not only to reduce primary emissions of PM₁ from automobiles and industry but also to reduce the emissions of important secondary PM₁ precursors, including sulfur oxides, nitrogen oxides, ammonia, and volatile organic compounds. Such efforts also could aid in efforts to reduce mixing ratios of ozone.     

Development of a PM2 5 Emissions Inventory for the South Coast Air Basin

ABSTRACT

With the promulgation of a national PM_2.5 ambient air quality standard, it is important that PM_2.5 emissions inventories be developed as a tool for understanding the magnitude of potential PM2.5 violations. Current PM₁₀ inventories include only emissions of primary particulate matter (1 ^ï PM), whereas, based on ambient measurements, both PM₁₀ and PM2.5 emissions inventories will need to include sources of both 1^ï PM and secondary particulate matter (2^ï PM). Furthermore, the U. S. Environmental Protection Agency’s (EPA) current edition of AP-42 includes size distribution data for 1o PM that overestimate the PM_2.5 fraction of fugitive dust sources by at least a factor of 2 based on recent studies.

This paper presents a PM_2.5 emissions inventory developed for the South Coast Air Basin (SCAB) that for the first time includes both 1^ï PM and 2^ï PM. The former is calculated by multiplying PM₁₀ emissions estimates by the PM_2.5/PM₁₀ ratios for different sources. The latter is calculated from estimated emission rates of gas-phase aerosol precursor and gas to aerosol conversion rates consistent with the measured chemical composition of ambient PM_2.5 concentrations observed in the SCAB. The major finding of this PM_2.5 emissions inventory is that the ^2ï aerosol component is more than twice the ^1ï aerosol component, which may result in widely different control strategies being required for fine PM and coarse PM.     

Characterization of organic aerosol in Big Bend National Park,Texas

The Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study was conducted in Big Bend National Park, Texas, July through October 1999. Daily PM_2.5 organic aerosol samples were collected on pre-fired quartz fiber filters. Daily concentrations were too low for detailed organic analysis by gas chromatography-mass spectrometry (GC-MS) and were grouped based on their air mass trajectories. A total of 12 composites, each containing 3–10 daily samples, were analyzed. Alkane carbon preference indices suggest primary biogenic emissions were small contributors to primary PM_2.5 organic matter (OM) during the first 3 months, while in October air masses advecting from the north and south were more strongly influenced by biogenic sources. A series of trace organic compounds previously shown to serve as particle phase tracers for various carbonaceous aerosol source types were examined. Molecular tracer species were generally at or below detection limits, except for the wood smoke tracer levoglucosan in one composite, so maximum possible source influences were calculated using the detection limit as an upper bound to the tracer concentration. Wood smoke was found not to contribute significantly to PM_2.5 OM, with contributions for most samples at <1% of the total organic particulate matter. Vehicular exhaust also appeared to make only minor contributions, with maximum possible influences calculated to be 1–4% of PM_2.5 OM. Several factors indicate that secondary organic aerosol formation was important throughout the study, and may have significantly altered the molecular composition of the aerosol during transport.     

Contribution of Primary and Secondary Sources to Organic Aerosol and PM2.5 at SEARCH Network Sites

Abstract

Chemical tracer methods for determining contributions to primary organic aerosol (POA) are fairly well established, whereas similar techniques for secondary organic aerosol (SOA), inherently complicated by time-dependent atmospheric processes, are only beginning to be studied. Laboratory chamber experiments provide insights into the precursors of SOA, but field data must be used to test the approaches. This study investigates primary and secondary sources of organic carbon (OC) and determines their mass contribution to particulate matter 2.5 µm or less in aerodynamic diameter (PM_2.5) in Southeastern Aerosol Research and Characterization (SEARCH) network samples. Filter samples were taken during 20 24-hr periods between May and August 2005 at SEARCH sites in Atlanta, GA (JST); Birmingham, AL (BHM); Centerville, AL (CTR); and Pensacola, FL (PNS) and analyzed for organic tracers by gas chromatography-mass spectrometry. Contribution to primary OC was made using a chemical mass balance method and to secondary OC using a mass fraction method. Aerosol masses were reconstructed from the contributions of POA, SOA, elemental carbon, inorganic ions (sulfate [SO₄ ^2?], nitrate [NO₃ ^?], ammonium [NH₄ ⁺]), metals, and metal oxides and compared with the measured PM_2.5. From the analysis, OC contributions from seven primary sources and four secondary sources were determined. The major primary sources of carbon were from wood combustion, diesel and gasoline exhaust, and meat cooking; major secondary sources were from isoprene and monoterpenes with minor contributions from toluene and β-caryophyllene SOA. Mass concentrations at the four sites were determined using source-specific organic mass (OM)-to-OC ratios and gave values in the range of 12–42 µg m^?3. Reconstructed masses at three of the sites (JST, CTR, PNS) ranged from 87 to 91% of the measured PM_2.5 mass. The reconstructed mass at the BHM site exceeded the measured mass by approximately 25%. The difference between the reconstructed and measured PM_2.5 mass for nonindustrial areas is consistent with not including aerosol liquid water or other sources of organic aerosol.     

Evaluation of the community multiscale air quality (CMAQ) model version 4.5: Sensitivities impacting model performance; Part II—particulate matter

This paper is Part II in a pair of papers that examines the results of the Community Multiscale Air Quality (CMAQ) model version 4.5 (v4.5) and discusses the potential explanations for the model performance characteristics seen. The focus of this paper is on fine particulate matter (PM_2.5) and its chemical composition. Improvements made to the dry deposition velocity and cloud treatment in CMAQ v4.5 addressing compensating errors in 36-km simulations improved particulate sulfate (SO₄²⁻) predictions. Large overpredictions of particulate nitrate (NO₃⁻) and ammonium (NH₄⁺) in the fall are likely due to a gross overestimation of seasonal ammonia (NH₃) emissions. Carbonaceous aerosol concentrations are substantially underpredicted during the late spring and summer months, most likely due, in part, to a lack of some secondary organic aerosol (SOA) formation pathways in the model. Comparisons of CMAQ PM_2.5 predictions with observed PM_2.5 mass show mixed seasonal performance. Spring and summer show the best overall performance, while performance in the winter and fall is relatively poor, with significant overpredictions of total PM_2.5 mass in those seasons. The model biases in PM_2.5 mass cannot be explained by summing the model biases for the major inorganic ions plus carbon. Errors in the prediction of other unspeciated PM_2.5 (PM_Other) are largely to blame for the errors in total PM_2.5 mass predictions, and efforts are underway to identify the cause of these errors.     

The Southeastern Aerosol Research and Characterization Study: Part II. Filter-Based Measurements of Fine and Coarse Particulate Matter Mass and Composition

Abstract

The Southeastern Aerosol Research and Characterization Study (SEARCH) was implemented in 1998–1999 to provide data and analyses for the investigation of the sources, chemical speciation, and long-term trends of fine particulate matter (PM_2.5) and coarse particulate matter (PM_10–2.5) in the Southeastern United States. This work is an initial analysis of 5 years (1999–2003) of filter-based PM_2.5 and PM_10–2.5 data from SEARCH. We find that annual PM_2.5 design values were consistently above the National Ambient Air Quality Standards (NAAQS) 15 µg/m³ annual standard only at monitoring sites in the two largest urban areas (Atlanta, GA, and North Birmingham, AL). Other sites in the network had annual design values below the standard, and no site had daily design values above the NAAQS 65 µg/m³ daily standard. Using a particle composition monitor designed specifically for SEARCH, we found that volatilization losses of nitrate, ammonium, and organic carbon must be accounted for to accurately characterize atmospheric particulate matter. In particular, the federal reference method for PM_2.5 underestimates mass by 3–7% as a result of these volatilization losses. Organic matter (OM) and sulfate account for ≥60% of PM_2.5 mass at SEARCH sites, whereas major metal oxides (MMO) and unidentified components (“other”) account for ≥80% of PM_10–2.5 mass. Limited data suggest that much of the unidentified mass in PM_10–2.5 may be OM. For paired comparisons of urban-rural sites, differences in PM_2.5 mass are explained, in large part, by higher OM and black carbon at the urban site. For PM₁₀, higher urban concentrations are explained by higher MMO and “other.” Annual means for PM_2.5 and PM_10–2.5 mass and major components demonstrate substantial declines at all of the SEARCH sites over the 1999–2003 period (10–20% in the case of PM_2.5, dominated by 14–20% declines in sulfate and 11–26% declines in OM, and 14–25% in the case of PM_10–2.5, dominated by 17–30% declines in MMO and 14–31% declines in “ other”). Although declining national emissions of sulfur dioxide and anthropogenic carbon may account for a portion of the observed declines, additional investigation will be necessary to establish a quantitative assessment, especially regarding trends in local and regional emissions, primary carbon emissions, and meteorology.     

Comparison of summer and winter California central valley aerosol distributions from lidar and MODIS measurements

Aerosol distributions from two aircraft lidar campaigns conducted in the California Central Valley are compared in order to identify seasonal variations. Aircraft lidar flights were conducted in June 2003 and February 2007. While the ground PM_2.5 (particulate matter with diameter ≤ 2.5 μm) concentration was highest in the winter, the aerosol optical depth (AOD) measured from the MODIS and lidar instruments was highest in the summer. A multiyear seasonal comparison shows that PM_2.5 in the winter can exceed summer PM_2.5 by 68%, while summer AOD from MODIS exceeds winter AOD by 29%. Warmer temperatures and wildfires in the summer produce elevated aerosol layers that are detected by satellite measurements, but not necessarily by surface particulate matter monitors. Temperature inversions, especially during the winter, contribute to higher PM_2.5 measurements at the surface. Measurements of the mixing layer height from lidar instruments provide valuable information needed to understand the correlation between satellite measurements of AOD and in situ measurements of PM_2.5. Lidar measurements also reflect the ammonium nitrate chemistry observed in the San Joaquin Valley, which may explain the discrepancy between the MODIS AOD and PM_2.5 measurements.     

Evaluating the dynamical characteristics of particle matter emissions in an open ore yard with industrial operation activities

A study to investigate the dynamical characteristics of particle matter emissions in a working open yard is conducted in Caofeidian Port of Hebei Province, China. The average diurnal concentrations of the total suspended particulate (TSP) matter and respirable particulate matter (PM₁₀ and PM₅) are monitored during the field measurement campaign. Sampling is performed at a regular interval at 8 monitoring stations in the yard with normal industrial activities. The average TSP, PM₁₀ and PM₅ concentrations range from 285 to 568, 198 to 423 and 189 to 330 μg.m-3 in the yard, respectively. The linear regression correlation coefficient of TSP/PM₁₀ and TSP/PM₅ is 0.95±0.01 and 0.88±0.02, respectively.By using the Spearman correlation method, the wind speed and relative humidity are both weakly correlated with the PM₁₀ and PM₅ concentrations according to the measurements. In addition, industrial operation activities, such as vehicular traffic in the yard and the loading time of stackers, are significantly positively correlated with the PM concentration. Using the multivariate regression method, the main parameters influencing the TSP concentration variations are integratedly analysed. The traffic volume is found to be a significant predictor of TSP concentration variation, with the smallest P value (P<0.05).To understand the dynamical characteristics of particle emissions in the yard, the emissions from the truck transports, that is, from unpaved haul roads and from the loading process, are established. Then, the dynamical emission factor (EF_D) based on the industrial activities in the yard is proposed. The dynamical emissions average 5.25x10⁵ kg.year^-1 and EF_D is evaluated to be 0.29 kg.(ton.day)^-1 during the measurement period. These outcomes have meaningful implications not only for understanding the dynamical characteristics of particle emissions in the working stockyard but also for implementing effective control measures at appropriate sites in the harbour area.     

Estimations of primary and secondary organic carbon formation in PM2.5 aerosols of Santiago City,Chile

High concentration of fine airborne particulates is considered one of the major environmental pollutants in Santiago, the Chilean Capital city, which in 1997 was declared a PM₁₀ saturated zone. To date there is no control of the amounts of fine and coarse aerosols concentrations and the source and chemical characterizations of the PM_2.5 particulates in the carbonaceous fractions are not well known even though this fraction could be represented almost the 50% in mass of the PM_2.5.In this work, we present for the first time determinations of primary organic aerosol (POA) and secondary organic aerosol composition (SOA) fractions of the total mass of PM_2.5 particulates collected in the urban atmosphere of Santiago City. Our purpose is to know the anthropogenic contributions to the formation of SOA. To accomplish this we used the elemental carbon (EC) and organic carbon (OC) determinations developed by automatic monitoring stations installed in the city during the period 2002–2005, with a particular analysis of the summer time occurred in February 2004. Based on the EC tracer method, we have estimated the POA and SOA fraction and our data permit us to estimate the SOA reaching up to 20% of total organic aerosol matter, in good agreement to other measurements observed in large cities of Europe and U.S.A.     

Temporal Variations of PM2.5, PM10, and Gaseous Precursors during the 1995 Integrated Monitoring Study in Central California

ABSTRACT

The spatial and temporal distributions of particle mass and its chemical constituents are essential for understanding the source-receptor relationships as well as the chemical, physical, and meteorological processes that result in elevated particulate concentrations in California’s San Joaquin Valley (SJV). Fine particulate matter ₍PM_2.5), coarse particulate matter (PM₁₀), and aerosol precursor gases were sampled on a 3-hr time base at two urban (Bakersfield and Fresno) and two non-urban (Kern Wildlife Refuge and Chowchilla) core sites in the SJV during the winter of 1995–1996.

Day-to-day variations of PM_2.5 and PM₁₀ and their chemical constituents were influenced by the synoptic-scale meteorology and were coherent among the four core sites. Under non-rainy conditions, similar diurnal variations of PM_2.5 and coarse aerosol were found at the two urban sites, with concentrations peaking during the nighttime hours. Conversely, PM_2.5 and coarse aerosol peaked during the morning and afternoon hours at the two non-urban sites. Under rainy and foggy conditions, these diurnal patterns were absent or greatly suppressed.

In the urban areas, elevated concentrations of primary pollutants (e.g., organic and elemental carbons) during the late afternoon and nighttime hours reflected the impact from residential wood combustion and motor vehicle exhaust. During the daytime, these concentrations decreased as the mixed layer deepened. Increases of secondary nitrate and sulfate concentrations were found during the daylight hours as a result of photochemical reactions. At the non-urban sites, the same increases in secondary aerosol concentrations occurred during the daylight hours but with a discernable lag time. Concentrations of the primary pollutants also increased at the non-urban sites during the daytime. These observations are attributed to mixing aloft of primary aerosols and secondary precursor gases in urban areas followed by rapid transport aloft to non-urban areas coupled with photochemical conversion.     

Measurements and modelling of PM2.5 concentrations near a major road in Kuopio,Finland

A particle measurement campaign was conducted in a suburban environment near a major road in Kuopio, Central Finland from 3 August to 9 September 1999. The mass concentrations of fine particles (PM_2.5) were measured simultaneously at distances of 12, 25, 52 and 87 m from the centre of a major road at a height of 1.8 m, using identical samplers. The concentration measurements were conducted during 16 daytime hours (from 6.00 a.m. to 10.00 p.m.) for 27 days. Traffic flows and relevant meteorological parameters were measured on-site; meteorological measurements from a nearby synoptic weather station were also utilised. We also suggest a preliminary model for predicting the concentrations of PM_2.5 and apply this model in order to analyse the measured data. The regionally and long-range transported contribution was evaluated on the basis of a semi-empirical mathematical model utilising as input values the daily sulphate, nitrate and ammonium measurements at the EMEP stations (Co-operative programme for monitoring and evaluation of the long-range transmission of air pollutants in Europe). The influence of primary vehicular emissions from the nearest roads was evaluated using a roadside emission and dispersion model, CAR-FMI, in combination with a meteorological pre-processing model, MPP-FMI. The contribution of non-exhaust particulate matter emissions (including resuspension of particulate matter from road surfaces) was estimated simply to be directly proportional to the concentrations originating from primary vehicular emissions. Comparison of the predicted results and measurements yields information on the relative importance of various source categories of the measured concentrations of PM_2.5. The regionally and long-range transported contribution, the primary and non-exhaust vehicular emissions, and other sources were estimated to contribute on average 41±6%, 33±6% and 26±7% of the observed PM_2.5 concentrations, respectively. The model presented could also be applied in other European cities for analysing the source contributions to measured fine particulate matter concentrations.     

Processes Influencing Secondary Aerosol Formation in the San Joaquin Valley during Winter

Abstract

Air quality data collected in the California Regional PM₁₀/PM_2.5 Air Quality Study (CRPAQS) are analyzed to qualitatively assess the processes affecting secondary aerosol formation in the San Joaquin Valley (SJV). This region experiences some of the highest fine particulate matter (PM_2.5) mass concentrations in California (≤188 μg/m³ 24-hr average), and secondary aerosol components (as a group) frequently constitute over half of the fine aerosol mass in winter. The analyses are based on 15 days of high-frequency filter and canister measurements and several months of wintertime continuous gas and aerosol measurements. The phase-partitioning of nitrogen oxide (NO_x)-related nitrogen species and carbonaceous species shows that concentrations of gaseous precursor species are far more abundant than measured secondary aerosol nitrate or estimated secondary organic aerosols. Comparisons of ammonia and nitric acid concentrations indicate that ammonium nitrate formation is limited by the availability of nitric acid rather than ammonia. Time-resolved aerosol nitrate data collected at the surface and on a 90-m tower suggest that both the daytime and nighttime nitric acid formation pathways are active, and entrainment of aerosol nitrate formed aloft at night may explain the spatial homogeneity of nitrate in the SJV. NO_x and volatile organic compound (VOC) emissions plus background O₃ levels are expected to determine NO_x oxidation and nitric acid production rates, which currently control the ammonium nitrate levels in the SJV. Secondary organic aerosol formation is significant in winter, especially in the Fresno urban area. Formation of secondary organic aerosol is more likely limited by the rate of VOC oxidation than the availability of VOC precursors in winter.     

Characterization of Particulate Matter in California

ABSTRACT

The size, composition, and concentration of particulate matter (PM) vary with location and time. Several monitoring/sampling programs are operated in California to characterize PM less than 2.5 and 10 µm in aerodynamic diameter (PM_2.5 and PM₁₀). This paper presents a broad summary of the spatial and temporal variations observed in ambient PM_2.5 and PM₁₀ concentrations in California. Many areas that have high PM₁₀ concentrations also have relatively high PM_2.5 concentrations, and data indicate that a significant portion of the PM₁₀ air quality problem is caused by PM_2.5. To develop effective plans for attaining the ambient PM standards, improved understanding of these unique problems is needed. Since 1989, pollution control efforts—whether specifically targeted for particulate matter or indirectly via controls on gaseous emissions—have caused annual average PM_2.5 and PM₁₀ concentrations to decline at most sites in California.     

What are the sources and conditions responsible for exceedences of the 24 h PM10 limit value (50 μg m−3) at a heavily trafficked London site?

The European Union has set limit values for PM₁₀ to be met in 2005. At Marylebone Road, London, where the traffic is heavy, the daily limit value of 50 μg m⁻³ is exceeded more than 35 times a year. A total of 185 days with daily PM₁₀ concentrations exceeding the limit value of 50 μg m⁻³ measured between January 2002 and December 2004 (data capture of 89.5%) are discussed in this paper. These exceedences were more frequent in early spring and in autumn. Concentrations have been disaggregated into regional, urban (background) and local (street) contributions. Most of the episodes of gravimetric PM₁₀ above the limit value were associated with a high regional background and very often the regional contribution dominated the PM₁₀ mass. The secondary aerosol (especially the particulate nitrate) made a major contribution to the PM₁₀ load. These situations were frequently observed when air masses came from the European mainland (showing that both emissions from the UK and other EU countries contributed to the exceedences), and less frequently with maritime air masses that have stagnated over the UK (showing that emissions from the UK alone less frequently contributed to the high regional background). However, the higher frequency of episodes breaching the limit value at the roadside site than at the rural site and the higher frequency of PM₁₀ concentrations above the limit value on weekdays show that the high regional contributions are additional to local and urban emissions. Local emissions mainly due to traffic were the second important contributor to the exceedences, while the contribution of the urban background of London was less important than the local emissions and the regional background. Applying the pragmatic mass closure model of Harrison et al. [2003. A pragmatic mass closure model for airborne particulate matter at urban background and roadside sites. Atmospheric Environment 37, 4927–4933], revealed that the regional aerosol is comprised very largely of ammonium nitrate and sulphate and secondary organic aerosol. Findings suggest that international abatement of secondary aerosol precursors may be the most effective measure to fulfil the requirements of the European Directive 1999/30/CE by lowering the regional background.     

Source apportionment of PM2.5 and PM10 aerosols in Brisbane (Australia) by receptor modelling

Aerosol samples for PM_2.5 and PM₁₀ (particulate matter with aerodynamic diameters less than 2.5 and 10 μm, respectively) were collected from 1993 to 1995 at five sites in Brisbane, a subtropical coastal city in Australia. This paper investigates the contributions of emission sources to PM_2.5 and PM₁₀ aerosol mass in Brisbane. Source apportionment results derived from the chemical mass balance (CMB), target transformation factor analysis (TTFA) and multiple linear regression (MLR) methods agree well with each other. The contributions from emission sources exhibit large variations in particle size with temporal and spatial differences. On average, the major contributors of PM₁₀ aerosol mass in Brisbane include: soil/road side dusts (25% by mass), motor vehicle exhausts (13%, not including the secondary products), sea salt (12%), Ca-rich and Ti-rich compounds (11%, from cement works and mineral processing industries), biomass burning (7%), and elemental carbon and secondary products contribute to around 15% of the aerosol mass on average. The major sources of PM_2.5 aerosols at the Griffith University (GU) site (a suburban site surrounded by forest area) are: elemental carbon (24% by mass), secondary organics (21%), biomass burning (15%) and secondary sulphate (14%). Most of the secondary products are related to motor vehicle exhausts, so, although motor vehicle exhausts contribute directly to only 6% of the PM_2.5 aerosol mass, their total contribution (including their secondary products) could be substantial. This pattern of source contribution is similar to the results for Rozelle (Sydney) among the major Australian studies, and is less in contributions from industrial and motor vehicular exhausts than the other cities. An attempt was made to estimate the contribution of rural dust and road side dust. The results show that road side dusts could contribute more than half of the crustal matter. More than 80% of the contribution of vehicle exhausts arises from diesel-fuelled trucks/buses. Biomass burning, large contributions of crustal matter, and/or local contributing sources under calm weather conditions, are often the cause of the high PM₁₀ episodes at the GU site in Brisbane.     

Aerosol transport model evaluation of an extreme smoke episode in Southeast Asia

Biomass burning is one of many sources of particulate pollution in Southeast Asia, but its irregular spatial and temporal patterns mean that large episodes can cause acute air quality problems in urban areas. Fires in Sumatra and Borneo during September and October 2006 contributed to 24-h mean PM₁₀ concentrations above 150 μg m^?3 at multiple locations in Singapore and Malaysia over several days. We use the FLAMBE model of biomass burning emissions and the NAAPS model of aerosol transport and evolution to simulate these events, and compare our simulation results to 24-h average PM₁₀ measurements from 54 stations in Singapore and Malaysia. The model simulation, including the FLAMBE smoke source as well as dust, sulfate, and sea salt aerosol species, was able to explain 50% or more of the variance in 24-h PM₁₀ observations at 29 of 54 sites. Simulation results indicated that biomass burning smoke contributed to nearly all of the extreme PM₁₀ observations during September–November 2006, but the exact contribution of smoke was unclear because the model severely underestimated total smoke emissions. Using regression analysis at each site, the bias in the smoke aerosol flux was determined to be a factor of between 2.5 and 10, and an overall factor of 3.5 was estimated. After application of this factor, the simulated smoke aerosol concentration averaged 20% of observed PM₁₀, and 40% of PM₁₀ for days with 24-h average concentrations above 150 μg m^?3. These results suggest that aerosol transport models can aid analysis of severe pollution events in Southeast Asia, but that improvements are needed in models of biomass burning smoke emissions.     

A European aerosol phenomenology – 3: Physical and chemical characteristics of particulate matter from 60 rural,urban, and kerbside sites across Europe

This paper synthesizes data on aerosol (particulate matter, PM) physical and chemical characteristics, which were obtained over the past decade in aerosol research and monitoring activities at more than 60 natural background, rural, near-city, urban, and kerbside sites across Europe. The data include simultaneously measured PM₁₀ and/or PM_2.5 mass on the one hand, and aerosol particle number concentrations or PM chemistry on the other hand. The aerosol data presented in our previous works (Van Dingenen et al., 2004, Putaud et al., 2004) were updated and merged to those collected in the framework of the EU supported European Cooperation in the field of Scientific and Technical action COST633 (Particulate matter: Properties related to health effects). A number of conclusions from our previous studies were confirmed. There is no single ratio between PM_2.5 and PM₁₀ mass concentrations valid for all sites, although fairly constant ratios ranging from 0.5 to 0.9 are observed at most individual sites. There is no general correlation between PM mass and particle number concentrations, although particle number concentrations increase with PM_2.5 levels at most sites. The main constituents of both PM₁₀ and PM_2.5 are generally organic matter, sulfate and nitrate. Mineral dust can also be a major constituent of PM₁₀ at kerbside sites and in Southern Europe. There is a clear decreasing gradient in SO₄^2? and NO₃^? contribution to PM₁₀ when moving from rural to urban to kerbside sites. In contrast, the total carbon/PM₁₀ ratio increases from rural to kerbside sites. Some new conclusions were also drawn from this work: the ratio between ultrafine particle and total particle number concentration decreases with PM_2.5 concentration at all sites but one, and significant gradients in PM chemistry are observed when moving from Northwestern, to Southern to Central Europe. Compiling an even larger number of data sets would have further increased the significance of our conclusions, but collecting all the aerosol data sets obtained also through research projects remains a tedious task.     

Chemical characterization and source apportionment of fine and coarse particulate matter in Lahore,Pakistan

Lahore, Pakistan is an emerging megacity that is heavily polluted with high levels of particle air pollution. In this study, respirable particulate matter (PM_2.5 and PM₁₀) were collected every sixth day in Lahore from 12 January 2007 to 19 January 2008. Ambient aerosol was characterized using well-established chemical methods for mass, organic carbon (OC), elemental carbon (EC), ionic species (sulfate, nitrate, chloride, ammonium, sodium, calcium, and potassium), and organic species. The annual average concentration (±one standard deviation) of PM_2.5 was 194 ± 94 μg m^?3 and PM₁₀ was 336 ± 135 μg m^?3. Coarse aerosol (PM_10?2.5) was dominated by crustal sources like dust (74 ± 16%, annual average ± one standard deviation), whereas fine particles were dominated by carbonaceous aerosol (organic matter and elemental carbon, 61 ± 17%). Organic tracer species were used to identify sources of PM_2.5 OC and chemical mass balance (CMB) modeling was used to estimate relative source contributions. On an annual basis, non-catalyzed motor vehicles accounted for more than half of primary OC (53 ± 19%). Lesser sources included biomass burning (10 ± 5%) and the combined source of diesel engines and residual fuel oil combustion (6 ± 2%). Secondary organic aerosol (SOA) was an important contributor to ambient OC, particularly during the winter when secondary processing of aerosol species during fog episodes was expected. Coal combustion alone contributed a small percentage of organic aerosol (1.9 ± 0.3%), but showed strong linear correlation with unidentified sources of OC that contributed more significantly (27 ± 16%). Brick kilns, where coal and other low quality fuels are burned together, are suggested as the most probable origins of unapportioned OC. The chemical profiling of emissions from brick kilns and other sources unique to Lahore would contribute to a better understanding of OC sources in this megacity.     

Chemical characteristics of long-range transport aerosol at background sites in Korea

In this study, background concentration sites of Deokjeok and Gosan, which were deemed suitable for monitoring the impact of long-range transported air pollutants, were selected. An investigation of the source types of pollutants, their locations, and relative quantitative contributions to the particulate concentrations at both sites using appropriate methodologies to make initial estimations was conducted. Episodic measurements of PM_2.5, PM₁₀, and size distribution, along with its ion and carbon components were performed from 2005 to 2007, and a comprehensive analysis of the results was conducted utilizing back trajectory analysis. As for frequency of wind direction, it was quite apparent that the two sites are heavily influenced by air masses originating from the eastern and northern regions of China. For PM_2.5 and PM₁₀, the mass concentrations from north and east China were higher than other cases, originating from the ocean. In the northerly-wind case, meteorological properties for Deokjeok and Gosan and the influence of carbon emissions from northwest Korea resulted in a changing of air mass properties during transport. As was the case with mass concentration, the highest contribution for ionic and carbon components of PM_2.5 and PM₁₀ for both sites appeared for the westerly wind case. A specially high relative contribution, greater than 1.4 times, was apparent in the secondary aerosol case because of a large influence of long-range transported pollutants from east China. Carbon components exhibited different behaviors for the northerly and westerly wind cases compared with secondary aerosol. The major reason for this discrepancy appears to be the carbon emissions from northwest Korea.     

Natural emissions for regional modeling of background ozone and particulate matter and impacts on emissions control strategies

Natural emissions adopted in current regional air quality modeling are updated to better describe natural background ozone and PM concentrations for North America. The revised natural emissions include organosulfur from the ocean, NO from lightning, sea salt, biogenic secondary organic aerosol (SOA) precursors, and pre-industrial levels of background methane. The model algorithm for SOA formation was also revised. Natural background ozone concentrations increase by up to 4 ppb in annual average over the southeastern US and Gulf of Mexico due to added NO from lightning while the revised biogenic emissions produced less ozone in the central and western US. Natural PM_2.5 concentrations generally increased with the revised natural emissions. Future year (2018) simulations were conducted for several anthropogenic emission reduction scenarios to assess the impact of the revised natural emissions on anthropogenic emission control strategies. Overall, the revised natural emissions did not significantly alter the ozone responses to the emissions reductions in 2018. With revised natural emissions, ozone concentrations were slightly less sensitive to reducing NOx in the southeastern US than with the current natural emissions due to higher NO from lightning. The revised natural emissions have little impact on modeled PM_2.5 responses to anthropogenic emission reductions. However, there are substantial uncertainties in current representations of natural sources in air quality models and we recommend that further study is needed to refine these representations.