Temporal patterns in daily measurements of inorganic and organic speciated PM2.5 in Denver

Airborne particulate matter less than 2.5 μm in aerodynamic diameter (PM_2.5) has been linked to a wide range of adverse health effects and as a result is currently regulated by the U.S. Environmental Protection Agency. PM_2.5 originates from a multitude of sources and has heterogeneous physical and chemical characteristics. These features complicate the link between PM_2.5 emission sources, ambient concentrations and health effects. The goal of the Denver Aerosol Sources and Health (DASH) study is to investigate associations between sources and health using daily measurements of speciated PM_2.5 in Denver.The datxa set being collected for the DASH study will be the longest daily speciated PM_2.5 data set of its kind covering 5.5 years of daily inorganic and organic speciated measurements. As of 2008, 4.5 years of bulk measurements (mass, inorganic ions and total carbon) and 1.5 years of organic molecular marker measurements have been completed. Several techniques were used to reveal long-term and short-term temporal patterns in the bulk species and the organic molecular marker species. All species showed a strong annual periodicity, but their monthly and seasonal behavior varied substantially. Weekly periodicities appear in many compound classes with the most significant weekday/weekend effect observed for elemental carbon, cholestanes, hopanes, select polycyclic aromatic hydrocarbons (PAHs), heavy n-alkanoic acids and methoxyphenols. Many of the observed patterns can be explained by meteorology or anthropogenic activity patterns while others do not appear to have such obvious explanations. Similarities and differences in these findings compared to those reported from other cities are highlighted.     

PM2.5 characterization for time series studies: Pointwise uncertainty estimation and bulk speciation methods applied in Denver

Many studies have identified associations between adverse health effects and short-term exposure to particulate matter less than 2.5 μm in diameter (PM_2.5). These effects, however, are not consistent across geographical regions. This may be due in part to variations in the chemical make-up of PM_2.5 resulting from unique combinations of sources, both primary and secondary, in different regions. The Denver Aerosol Sources and Health (DASH) study is a multi-year time series study designed to characterize the daily chemical composition of PM_2.5 in Denver, identify the major contributing sources, and investigate associations between sources and a broad array of adverse health outcomes.Measurement methodology, field blank correction, pointwise uncertainty estimation and detection limit consideration are discussed in the context of bulk speciation for the DASH study. Results are presented for the first 4.5 years of mass, inorganic ion and bulk carbon speciation. The derived measurement uncertainties were propagated using the root sum of squares method and show good agreement with precision estimates derived from bi-weekly duplicate samples collected on collocated samplers. Gravimetric mass has the most uncertainty of any measurement and reconstructed mass generated from the sum of the individual species shows less uncertainty than measured mass on average. The methods discussed provide a good framework for PM_2.5 speciation measurements and are generalizable to analysis of other environmental measures.     

A functional group characterization of organic PM2.5 exposure: Results from the RIOPA study

The functional group (FG) composition of urban residential outdoor, indoor, and personal fine particle (PM_2.5) samples is presented and used to provide insights relevant to organic PM_2.5 exposure. PM_2.5 samples (48 h) were collected during the Relationship of Indoor, Outdoor, and Personal Air (RIOPA) study at 219 non-smoking homes (once or twice) in Los Angeles County, CA, Elizabeth, NJ, and Houston, TX. Fourier transform infrared (FTIR) spectra of PM_2.5 samples were collected, and FG absorbances were quantified by partial least squares (PLS) regression, a multivariate calibration method.There is growing evidence in the literature that a large majority of indoor-generated PM_2.5 is organic. The current research suggests that indoor-generated PM_2.5 is enriched in aliphatic carbon–hydrogen (CH) FGs relative to ambient outdoor PM_2.5. Indoor-generated CH exceeded outdoor-generated CH in 144 of the 167 homes for which indoor or outdoor CH was measurable; estimated indoor emission rates are provided. The strong presence of aliphatic CH FGs in indoor PM_2.5 makes particulate organic matter substantially less polar indoors and in personal exposures than outdoors. This is a substantial new finding. Based on the quantified FGs, the average organic molecular weight (OM) per carbon weight (OC), a measure of the degree of oxygenation of organic PM, is in the range of 1.7–2.6 for outdoor samples and 1.3–1.7 for indoor and personal samples. Polarity or degree of oxygenation effects particle deposition in exposure environments and in the respiratory system.     

Health effects of PM2.5 constituents and source contributions in major metropolitan cities,South Korea

Ambient PM_2.5 is one of the major risk factors for human health, and is not fully explained solely by mass concentration. We examined the short-term associations of cause-specific mortality (i.e., all-cause, cardiovascular, and respiratory mortality) with the 15 chemical constituents and sources of PM_2.5 in four metropolitan cities of South Korea during 2014–2018. We found transition metals consistently showed significant associations with all-cause mortality, while the effects of other constituents varied across the cities and for cause of death. Carbonaceous components strongly affected the all-cause, cardiovascular, and respiratory mortality in Daejeon. Secondary inorganic aerosols, SO₄^2? and NH₄⁺, showed significant associations with respiratory mortality in Gwangju. We also found the sources from which species closely linked to mortality generally increased the relative mortality risks. Heavy metal markers from soil or industrial sources were significantly associated with mortality in all cities. However, several sources influenced mortality despite their marker species not being significantly associated with it. Secondary nitrate and secondary sulfate sources were linked to mortality in DJ. This could be attributed to the deep inland location, which might have facilitated formation of secondary inorganic aerosols. In addition, primary sources including mobile and coal combustion seemed to have acute impacts on respiratory mortality in Gwangju. Our findings suggest the necessity of positive matrix factorization (PMF)-based approaches for evaluating health effects of PM_2.5 while considering the spatial heterogeneity in the compositions and source contributions of PM_2.5.

     

PM2.5 source apportionment with organic markers in the Southeastern Aerosol Research and Characterization (SEARCH) study

Positive matrix factorization (PMF) and effective variance (EV) solutions to the chemical mass balance (CMB) were applied to PM_2.5 (particulate matter with an aerodynamic diameter <2.5 μm) mass and chemically speciated measurements for samples taken from 2008 to 2010 at the Atlanta, Georgia, and Birmingham, Alabama, sites. Commonly measured PM_2.5 mass, elemental, ionic, and thermal carbon fraction concentrations were supplemented with detailed nonpolar organic speciation by thermal desorption-gas chromatography/mass spectrometry (TD-GC/MS). Source contribution estimates were calculated for motor vehicle exhaust, biomass burning, cooking, coal-fired power plants, road dust, vegetative detritus, and secondary sulfates and nitrates for Atlanta. Similar sources were found for Birmingham, with the addition of an industrial source and the separation of biomass burning into open burning and residential wood combustion. EV-CMB results based on conventional species were qualitatively similar to those estimated by PMF-CMB. Secondary ammonium sulfate was the largest contributor, accounting for 27–38% of PM_2.5, followed by biomass burning (21–24%) and motor vehicle exhaust (9–24%) at both sites, with 4–6% of PM_2.5 attributed to coal-fired power plants by EV-CMB. Including organic compounds in the EV-CMB reduced the motor vehicle exhaust and biomass burning contributions at both sites, with a 13–23% deficit for PM_2.5 mass. The PMF-CMB solution showed mixing of sources within the derived factors, both with and without the addition of speciated organics, as is often the case with complex source mixtures such as those at these urban-scale sites. The nonpolar TD-GC/MS compounds can be obtained from existing filter samples and are a useful complement to the elements, ions, and carbon fractions. However, they should be supplemented with other methods, such as TD-GC/MS on derivitized samples, to obtain a wider range of polar compounds such as sterols, sugars, and organic acids. The PMF and EV solutions to the CMB equations are complementary to, rather than replacements for, each other, as comparisons of their results reveal uncertainties that are not otherwise evident.

Implications:?Organic markers can be measured on currently acquired PM_2.5 filter samples by thermal methods. These markers can complement element, ion, and carbon fraction measurements from long-term speciation networks. Applying the positive matrix factorization and effective variance solutions for the chemical mass balance equations provides useful information on the accuracy of the source contribution estimates. Nonpolar compounds need to be complemented with polar compounds to better apportion cooking and secondary organic aerosol contributors.     

Concentrations,properties, and health risk of PM2.5 in the Tianjin City subway system

A campaign was conducted to assess and compare the personal exposure in L3 of Tianjin subway, focusing on PM_2.5 levels, chemical compositions, morphology analysis, as well as the health risk of heavy metal in PM_2.5. The results indicated that the average concentration of the PM_2.5 was 151.43 μg/m³ inside the train of the subway during rush hours. PM_2.5 concentrations inside car under the ground are higher than those on the ground, and PM_2.5 concentrations on the platform are higher than those inside car. Regarding metal concentrations, the highest element in PM_2.5 samples was Fe; the level of which is 17.55 μg/m³. OC is a major component of PM_2.5 in Tianjin subway. Secondary organic carbon is the formation of gaseous organic pollutants in subway. SEM–EDX and TEM–EDX exhibit the presence of individual particle with a large metal content in the subway samples. For small Fe metal particles, iron oxide can be formed easily. With regard to their sources, Fe-containing particles are generated mainly from mechanical wear and friction processes at the rail–wheel–brake interfaces. The non-carcinogenic risk to metals Cr, Ni, Cu, Zn and Pb, and carcinogenic hazard of Cr and Ni were all below the acceptable level in L3 of Tianjin subway.

     

Seasonal and spatial trends in the sources of fine particle organic carbon in Israel,Jordan, and Palestine

A study of carbonaceous particulate matter (PM) was conducted in the Middle East at sites in Israel, Jordan, and Palestine. The sources and seasonal variation of organic carbon, as well as the contribution to fine aerosol (PM_2.5) mass, were determined. Of the 11 sites studied, Nablus had the highest contribution of organic carbon (OC), 29%, and elemental carbon (EC), 19%, to total PM_2.5 mass. The lowest concentrations of PM_2.5 mass, OC, and EC were measured at southern desert sites, located in Aqaba, Eilat, and Rachma. The OC contribution to PM_2.5 mass at these sites ranged between 9.4% and 16%, with mean annual PM_2.5 mass concentrations ranging from 21 to 25 ug m^?3. These sites were also observed to have the highest OC to EC ratios (4.1–5.0), indicative of smaller contributions from primary combustion sources and/or a higher contribution of secondary organic aerosol. Biomass burning and vehicular emissions were found to be important sources of carbonaceous PM in this region at the non-southern desert sites, which together accounted for 30%–55% of the fine particle organic carbon at these sites. The fraction of measured OC unapportioned to primary sources (1.4 μgC m^?3 to 4.9 μgC m^?3; 30%–74%), which has been shown to be largely from secondary organic aerosol, is relatively constant at the sites examined in this study. This suggests that secondary organic aerosol is important in the Middle East during all seasons of the year.     

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.     

Source apportionment of PM2.5 for supporting control strategies in the Monterrey Metropolitan Area,Mexico

The Monterrey Metropolitan Area (MMA) in Northeast Mexico has shown high PM_2.5 concentrations since 2003. The data shows that the annual average concentration exceeds from 2 to 3 times the Mexican PM_2.5 annual air quality standard of 12 µg/m³. In a previous work we studied the chemical characterization of PM_2.5 in two sites of the MMA during the winter season. Among the most important components we found ammonium sulfate and nitrate, elemental and organic carbon, and crustal matter. In this work we present the results of a second chemical characterization study performed during the summer time and the application of the chemical mass balance (CMB) model to determine the source apportionment of air pollutants in the region. The chemical analysis results show that the chemical composition of PM_2.5 is similar in both sites and periods of the year. The results of the chemical analysis and the CMB model show that industrial, traffic, and combustion activities in the area are the major sources of primary PM_2.5 and precursor gases of secondary inorganic and organic aerosol (SO₂, NOx, NH₃, and volatile organic compounds [VOCs]). We also found that black carbon and organic carbon are important components of PM_2.5 in the MMA. These results are consistent with the MMA emission inventory that reports as major sources of particles and SO₂ a refinery and fuel combustion, as well as nitrogen oxides and ammonium from transportation and industrial activities in the MMA and ammonium form agricultural activities in the state. The results of this work are important to identify and support effective actions to reduce direct emissions of PM_2.5 and its precursor gases to improve air quality in the MMA. Implications: The Monterrey Metropolitan Area (MMA) has been classified as the most air-polluted area in Mexico by the World Health Organization (WHO). Effective actions need to be taken to control primary sources of PM_2.5 and its precursors, reducing health risks on the population exposed and their associated costs. The results of this study identify the main sources and their estimated contribution to PM_2.5 mass concentration, providing valuable information to the local environmental authorities to take decisions on PM_2.5 control strategies in the MMA.     

Source apportionment of ambient PM2.5 at five spanish centres of the european community respiratory health survey (ECRHS II)

Fine particulate matter (PM_2.5) was sampled at 5 Spanish locations during the European Community Respiratory Health Survey II (ECRHS II). In an attempt to identify and quantify PM_2.5 sources, source contribution analysis by principal component analysis (PCA) was performed on five datasets containing elemental composition of PM_2.5 analysed by ED-XRF. A total of 4–5 factors were identified at each site, three of them being common to all sites (interpreted as traffic, mineral and secondary aerosols) whereas industrial sources were site-specific. Sea-salt was identified as independent source at all coastal locations except for Barcelona (where it was clustered with secondary aerosols). Despite their typically dominant coarse grain-size distribution, mineral and marine aerosols were clearly observed in PM_2.5. Multi-linear regression analysis (MLRA) was applied to the data, showing that traffic was the main source of PM_2.5 at the five sites (39–53% of PM_2.5, 5.1–12.0 μg m⁻³), while regional-scale secondary aerosols accounted for 14–34% of PM_2.5 (2.6–4.5 μg m⁻³), mineral matter for 13–31% (2.4–4.6 μg m⁻³) and sea-salt made up 3–7% of the PM_2.5 mass (0.4–1.3 μg m⁻³). Consequently, despite regional and climatic variability throughout Spain, the same four main PM_2.5 emission sources were identified at all the study sites and the differences between the relative contributions of each of these sources varied at most 20%. This would corroborate PM_2.5 as a useful parameter for health studies and environmental policy-making, owing to the fact that it is not as subject to the influence of micro-sitting as other parameters such as PM₁₀. African dust inputs were observed in the mineral source, adding on average 4–11 μg m⁻³ to the PM_2.5 daily mean during dust outbreaks. On average, levels of Al, Si, Ti and Fe during African episodes were higher by a factor of 2–8 with respect to non-African days, whereas levels of local pollutants (absorption coefficient, S, Pb, Cl) showed smaller variations (factor of 0.5–2).     

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.     

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.     

Influence of tobacco smoke on carcinogenic PAH composition in indoor PM10 and PM2.5

Because of the mutagenic and/or carcinogenic properties, Polycyclic Aromatic Hydrocarbons (PAH), have a direct impact on human population. Consequently, there is a widespread interest in analysing and evaluating the exposure to PAH in different indoor environments, influenced by different emission sources. The information on indoor PAH is still limited, mainly in terms of PAH distribution in indoor particles of different sizes; thus, this study evaluated the influence of tobacco smoke on PM₁₀ and PM_2.5 characteristics, namely on their PAH compositions, with further aim to understand the negative impact of tobacco smoke on human health. Samples were collected at one site influenced by tobacco smoke and at one reference (non-smoking) site using low-volume samplers; the analyses of 17 PAH were performed by Microwave Assisted Extraction combined with Liquid Chromatography (MAE–LC). At the site influenced by tobacco smoke PM concentrations were higher 650% for PM₁₀, and 720% for PM_2.5. When influenced by smoking, 4 ring PAH (fluoranthene, pyrene, and chrysene) were the most abundant PAH, with concentrations 4600–21 000% and 5100–20 800% higher than at the reference site for PM₁₀ and PM_2.5, respectively, accounting for 49% of total PAH (Σ_PAH). Higher molecular weight PAH (5–6 rings) reached concentrations 300–1300% and 140–1700% higher for PM₁₀ and PM_2.5, respectively, at the site influenced by tobacco smoke. Considering 9 carcinogenic PAH this increase was 780% and 760% in PM₁₀ and PM_2.5, respectively, indicating the strong potential risk for human health. As different composition profiles of PAH in indoor PM were obtained for reference and smoking sites, those 9 carcinogens represented at the reference site 84% and 86% of Σ_PAH in PM₁₀ and PM_2.5, respectively, and at the smoking site 56% and 55% of Σ_PAH in PM₁₀ and PM_2.5, respectively. All PAH (including the carcinogenic ones) were mainly present in fine particles, which corresponds to a strong risk for cardiopulmonary disease and lung cancer; thus, these conclusions are relevant for the development of strategies to protect public health.     

Uncertainty in health risks due to anthropogenic primary fine particulate matter from different source types in Finland

The emission-exposure and exposure-response (toxicity) relationships are different for different emission source categories of anthropogenic primary fine particulate matter (PM_2.5). These variations have a potentially crucial importance in the integrated assessment, when determining cost-effective abatement strategies. We studied the importance of these variations by conducting a sensitivity analysis for an integrated assessment model. The model was developed to estimate the adverse health effects to the Finnish population attributable to primary PM_2.5 emissions from the whole of Europe. The primary PM_2.5 emissions in the whole of Europe and in more detail in Finland were evaluated using the inventory of the European Monitoring and Evaluation Programme (EMEP) and the Finnish Regional Emission Scenario model (FRES), respectively. The emission-exposure relationships for different primary PM_2.5 emission source categories in Finland have been previously evaluated and these values incorporated as intake fractions into the integrated assessment model. The primary PM_2.5 exposure-response functions and toxicity differences for the pollution originating from different source categories were estimated in an expert elicitation study performed by six European experts on air pollution health effects. The primary PM_2.5 emissions from Finnish and other European sources were estimated for the population of Finland in 2000 to be responsible for 209 (mean, 95% confidence interval 6–739) and 357 (mean, 95% CI 8–1482) premature deaths, respectively. The inclusion of emission-exposure and toxicity variation into the model increased the predicted relative importance of traffic related primary PM_2.5 emissions and correspondingly, decreased the predicted relative importance of other emission source categories. We conclude that the variations of emission-exposure relationship and toxicity between various source categories had significant impacts for the assessment on premature deaths caused by primary PM_2.5.     

Rapid Nitrate Loss from PM10 Filters

The Monterrey Metropolitan Area (MMA) has shown a high concentration of PM_2.5 in its atmosphere since 2003. The contribution of possible sources of primary PM_2.5 and its precursors is not known. In this paper we present the results of analyzing the chemical composition of sixty 24-hr samples of PM_2.5 to determine possible sources of PM_2.5 in the MMA. The samples were collected at the northeast and southeast of the MMA between November 22 and December 12, 2007, using low-volume devices. Teflon and quartz filters were used to collect the samples. The concentrations of 16 airborne trace elements were determined using x-ray fluorescence (XRF). Anions and cations were determined using ion chromatography. Organic carbon (OC) and elemental carbon (EC) were determined by thermal optical analysis. The results show that Ca had the maximum mean concentration of all elements studied, followed by S. Enrichment factors above 50 were calculated for S, Cl, Cu, Zn, Br, and Pb. This indicates that these elements may come from anthropogenic sources. Overall, the major average components of PM_2.5 were OC (41.7%), SO₄ ^2? (22.9%), EC (7.4%), crustal material (11.4%), and NO₃ ^? (12.6%), which altogether accounted for 96% of the mass. Statistically, we did not find any difference in SO₄ ^2? concentrations between the two sites. The fraction of secondary organic carbon was between 24% and 34%. The results of the factor analysis performed over 10 metals and OC and EC show that there are three main sources of PM_2.5: crustal material and vehicle exhaust; industrial activity; and fuel oil burning. The results show that SO₄ ^2?, OC, and crustal material are important components of PM_2.5 in MMA. Further work is necessary to evaluate the proportion of secondary inorganic and organic aerosol in order to have a better understanding of the sources and precursors of aerosols in the MMA.

Implications: The MMA has become one of the most air polluted areas in Mexico. High levels of PM_2.5 have been measured and effective actions need to be taken to reduce air pollution and the associated health risks. Several sources of primary PM_2.5 and precursors of secondary particles exist in the MMA. This study provides valuable information for the local environmental authorities to identify possible sources of primary PM_2.5 and its precursors. The effectiveness of the actions taken to improve air quality will lead to health benefits for the population, reducing their associated costs.     

Air Quality Measurements from the Fresno Supersite

ABSTRACT

The Fresno Supersite intends to 1) evaluate non-routine monitoring methods, establishing their comparability with existing methods and their applicability to air quality planning, exposure assessment, and health effects studies; 2) provide a better understanding of aerosol characteristics, behavior, and sources to assist regulatory agencies in developing standards and strategies that protect public health; and 3) support studies that evaluate relationships between aerosol properties, co-factors, and observed health end-points. Supersite observables include in-situ, continuous, short-duration measurements of 1) PM_2.5, PM₁₀, and coarse (PM₁₀ minus PM_2.5) mass; 2) PM_2.5 SO₄ ^-2, NO₃ ^-, carbon, light absorption, and light extinction; 3) numbers of particles in discrete size bins ranging from 0.01 to ~10μm; 4) criteria pollutant gases (O₃, CO, NO_x); 5) reactive gases (NO₂, NO_y, HNO₃, peroxyacetyl nitrate [PAN], NH₃); and 6) single particle characterization by time-of-flight mass spectrometry. Field sampling and laboratory analysis are applied for gaseous and particulate organic compounds (light hydrocarbons, heavy hydrocarbons, carbonyls, polycyclic aromatic hydrocarbons [PAH], and other semi-volatiles), and PM_2.5 mass, elements, ions, and carbon. Observables common to other Supersites are 1) daily PM_2.5 24-hr average mass with Federal Reference Method (FRM) samplers; 2) continuous hourly and 5-min average PM_2.5 and PM₁₀ mass with beta attenuation monitors (BAM) and tapered element oscillating microbalances (TEOM); 3) PM_2.5 chemical specia-tion with a U.S. Environmental Protection Agency (EPA) speciation monitor and protocol; 4) coarse particle mass by dichotomous sampler and difference between PM₁₀ and PM_2.5 BAM and TEOM measurements; 5) coarse particle chemical composition; and 6) high sensitivity and time resolution scalar and vector wind speed, wind direction, temperature, relative humidity, barometric pressure, and solar radiation. The Fresno Supersite is coordinated with health and toxicological studies that will use these data in establishing relationships with asthma, other respiratory disease, and cardiovascular changes in human and animal subjects.     

Spatial differences in ambient coarse and fine particles in the Monterrey metropolitan area,Mexico: Implications for source contribution

The ambient air of the Monterrey Metropolitan Area (MMA) in Mexico frequently exhibits high levels of PM₁₀ and PM_2.5. However, no information exists on the chemical composition of coarse particles (PM_c = PM₁₀ – PM_2.5). A monitoring campaign was conducted during the summer of 2015, during which 24-hr average PM₁₀ and PM_2.5 samples were collected using high-volume filter-based instruments to chemically characterize the fine and coarse fractions of the PM. The collected samples were analyzed for anions (Cl^–, NO₃^–, SO₄^2–), cations (Na⁺, NH₄⁺, K⁺), organic carbon (OC), elemental carbon (EC), and 35 trace elements (Al to Pb). During the campaign, the average PM_2.5 concentrations did not showed significance differences among sampling sites, whereas the average PM_c concentrations did. In addition, the PM_c accounted for 75% to 90% of the PM₁₀ across the MMA. The average contribution of the main chemical species to the total mass indicated that geological material including Ca, Fe, Si, and Al (45%) and sulfates (11%) were the principal components of PM_c, whereas sulfates (54%) and organic matter (30%) were the principal components of PM_2.5. The OC-to-EC ratio for PM_c ranged from 4.4 to 13, whereas that for PM_2.5 ranged from 3.97 to 6.08. The estimated contribution of Secondary Organic Aerosol (SOA) to the total mass of organic aerosol in PM_2.5 was estimated to be around 70–80%; for PM_c, the contribution was lower (20–50%). The enrichment factors (EF) for most of the trace elements exhibited high values for PM_2.5 (EF: 10–1000) and low values for PM_c (EF: 1–10). Given the high contribution of crustal elements and the high values of EFs, PM_c is heavily influenced by soil resuspension and PM_2.5 by anthropogenic sources. Finally, the airborne particles found in the eastern region of the MMA were chemically distinguishable from those in its western region.

Implications: Concentration and chemical composition patterns of fine and coarse particles can vary significantly across the MMA. Public policy solutions have to be built based on these observations. There is clear evidence that the spatial variations in the MMA’s coarse fractions are influenced by clearly recognizable primary emission sources, while fine particles exhibit a homogeneous concentration field and a clear spatial pattern of increasing secondary contributions. Important reductions in the coarse fraction can come from primary particles’ emission controls; for fine particles, control of gaseous precursors—particularly sulfur-containing species and organic compounds—should be considered.     

Is remaining indoors an effective way of reducing exposure to fine particulate matter during biomass burning events?

Bushfires, prescribed burns, and residential wood burning are significant sources of fine particles (aerodynamic diameter <2.5 μm; PM_2.5) affecting the health and well-being of many communities. Despite the lack of evidence, a common public health recommendation is to remain indoors, assuming that the home provides a protective barrier against ambient PM_2.5. The study aimed to assess to what extent houses provide protection against peak concentrations of outdoor PM_2.5 and whether remaining indoors is an effective way of reducing exposure to PM_2.5. The effectiveness of this strategy was evaluated by conducting simultaneous week-long indoor and outdoor measurements of PM_2.5 at 21 residences in regional areas of Victoria, Australia. During smoke plume events, remaining indoors protected residents from peak outdoor PM_2.5 concentrations, but the level of protection was highly variable, ranging from 12% to 76%. Housing stock (e.g., age of the house) and ventilation (e.g., having windows/doors open or closed) played a significant role in the infiltration of outdoor PM_2.5 indoors. The results also showed that leaving windows and doors closed once the smoke plume abates trapped PM_2.5 indoors and increased indoor exposure to PM_2.5. Furthermore, for approximately 50% of households, indoor sources such as cooking activities, smoking, and burning candles or incense contributed significantly to indoor PM_2.5.

Implications: Smoke from biomass burning sources can significantly impact on communities. Remaining indoors with windows and doors closed is a common recommendation by health authorities to minimize exposures to peak concentrations of fine particles during smoke plume events. Findings from this study have shown that the protection from fine particles in biomass burning smoke is highly variable among houses, with information on housing age and ventilation status providing an approximate assessment on the protection of a house. Leaving windows closed once a smoke plume abates traps particles indoors and increases exposures.     

Temporal variations of fine and coarse particulate matter sources in Jeddah,Saudi Arabia

This study provides the first comprehensive analysis of the seasonal variations and weekday/weekend differences in fine (aerodynamic diameter <2.5 μm; PM_2.5) and coarse (aerodynamic diameter 2.5–10 μm; PM_2.5–10) particulate matter mass concentrations, elemental constituents, and potential source origins in Jeddah, Saudi Arabia. Air quality samples were collected over 1 yr, from June 2011 to May 2012 at a frequency of three times per week, and analyzed. The average mass concentrations of PM_2.5 (21.9 μg/m³) and PM₁₀ (107.8 μg/m³) during the sampling period exceeded the recommended annual average levels by the World Health Organization (WHO) for PM_2.5 (10 μg/m³) and PM₁₀ (20 μg/m³), respectively. Similar to other Middle Eastern locales, PM_2.5–10 is the prevailing mass component of atmospheric particulate matter at Jeddah, accounting for approximately 80% of the PM₁₀ mass. Considerations of enrichment factors, absolute principal component analysis (APCA), concentration roses, and backward trajectories identified the following source categories for both PM_2.5 and PM_2.5–10: (1) soil/road dust, (2) incineration, and (3) traffic; and for PM_2.5 only, (4) residual oil burning. Soil/road dust accounted for a major portion of both the PM_2.5 (27%) and PM_2.5–10 (77%) mass, and the largest source contributor for PM_2.5 was from residual oil burning (63%). Temporal variations of PM_2.5–10 and PM_2.5 were observed, with the elevated concentration levels observed for mass during the spring (due to increased dust storm frequency) and on weekdays (due to increased traffic). The predominant role of windblown soil and road dust in both the PM_2.5 and PM_2.5–10 masses in this city may have implications regarding the toxicity of these particles versus those in the Western world where most PM health assessments have been made in the past. These results support the need for region-specific epidemiological investigations to be conducted and considered in future PM standard setting.

Implications: Temporal variations of fine and coarse PM mass, elemental constituents, and sources were examined in Jeddah, Saudi Arabia, for the first time. The main source of PM_2.5–10 is natural windblown soil and road dust, whereas the predominant source of PM_2.5 is residual oil burning, generated from the port and oil refinery located west of the air sampler, suggesting that targeted emission controls could significantly improve the air quality in the city. The compositional differences point to a need for health effect studies to be conducted in this region, so as to directly assess the applicability of the existing guidelines to the Middle East air pollution.     

Seasonal ambient particulate matter and population health outcomes among communities impacted by road dust in British Columbia,Canada

In recent years, many air quality monitoring programs have favored measurement of particles less than 2.5 µm (PM_2.5) over particles less than 10 µm (PM₁₀) in light of evidence that health impacts are mostly from the fine fraction. However, the coarse fraction (PM_10-2.5) may have independent health impacts that support continued measurement of PM₁₀ in some areas, such as those affected by road dust. The objective of this study was to evaluate the associations between different measures of daily PM exposure and two daily indicators of population health in seven communities in British Columbia, Canada, where road dust is an ongoing concern. The measures of exposure were PM₁₀, PM_2.5, PM_10-2.5, PM_2.5 adjusted for PM_10-2.5, and PM_10-2.5 adjusted for PM_2.5. The indicators of population health were dispensations of the respiratory reliever medication salbutamol sulfate and nonaccidental mortality. This study followed a time-series design using Poisson regression over a 2003–2015 study period, with analyses stratified by three seasons: residential woodsmoke in winter; road dust in spring; and wildfire smoke in summer. A random-effects meta-analysis was conducted to establish a pooled estimate. Overall, an interquartile range increase in daily PM_10-2.5 was associated with a 3.6% [1.6, 5.6] increase in nonaccidental mortality during the road dust season, which was reduced to 3.1% [0.8, 5.4] after adjustment for PM_2.5. The adjusted coarse fraction had no effect on salbutamol dispensations in any season. However, an interquartile range increase in PM_2.5 was associated with a 2.7% [2.0, 3.4] increase in dispensations during the wildfire season. These analyses suggest different impacts of different PM fractions by season, with a robust association between the coarse fraction and nonaccidental mortality in communities and periods affected by road dust. We recommend that PM₁₀ monitoring networks be maintained in these communities to provide feedback for future dust mitigation programs.

Implications: There was a significant association between daily concentrations of the coarse fraction and nonaccidental mortality during the road dust season, even after adjustment for the fine fraction. The acute and chronic health effects associated with exposure to the coarse fraction remain unclear, which supports the maintenance of PM₁₀ monitoring networks to allow for further research in communities affected by sources such as road dust.