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Particulate matter (PM) is a major primary pollutant emitted during wildland fires that has the potential to pose significant health risks to individuals/communities who live and work in areas impacted by smoke events. Limiting exposure is the principle measure available to mitigate health impacts of smoke and therefore the accurate determination of ambient PM concentrations during wildland fire events is critical to protecting public health. However, monitoring air pollutants in smoke impacted environments has proven challenging in that measurement interferences or sampling conditions can result in both positive and negative artifacts. The EPA has performed research on methods for the measurement of PM2.5 in a series of laboratory-based studies including evaluation in smoke. This manuscript will summarize the results of the laboratory-based evaluation of federal equivalent method (FEM) monitors for PM2.5 with particular attention being given to the Teledyne-API Model T640 PM Mass monitor, as compared to the filter-based federal reference method (FRM). The T640 is an optical-based PM monitor and has been gaining wide use by state and local agencies in monitoring for PM2.5 U.S. National Ambient Air Quality Standards (NAAQS) attainment. At present, the T640 (includes both T640 and T640×) comprises ~44% of the PM2.5 FEM monitors in U.S. regulatory monitoring networks. In addition, the T640 has increasingly been employed for the higher time resolution comparison/evaluation of low-cost PM sensors including during smoke impacted events. Results from controlled non-smoke laboratory studies using generated ammonium sulfate aerosols demonstrated a generally negative T640 measurement artifact that was significantly related to the PM2.5 concentration and particle size distribution. Results from biomass burning chamber studies demonstrated positive and negative artifacts significantly associated with PM2.5 concentration and optical wavelength-dependent absorption properties of the smoke aerosol. Implications: The results detailed in this paper will provide state and local air monitoring agencies with the tools and knowledge to address PM2.5 measurement challenges in areas frequently impacted by wildland fire smoke. The observed large positive and negative artifacts in the T640 PM mass determination have the potential to result in false exceedances of the PM2.5 NAAQS or in the disqualification of monitoring data through an exceptional event designation. In addition, the observed artifacts in smoke impacted air will have a detrimental effect on providing reliable public information when wildfires occur and also in identifying reference measurements for small sensor evaluation studies. Other PM2.5 FEMs such as the BAM-1022 perform better in smoke and are comparable to the filter-based FRM. Care must be taken in choosing high time resolution FEM monitors that will be operated at smoke impacted sites. Accurate methods, such as the FRM and BAM-1022 will reduce the burden of developing and reviewing exceptional event request packages, data loss/disqualification, and provide states with tools to adequately evaluate public exposure risks and provide accurate public health messaging during wildfire/smoke events.

Air quality models are used to assess the impact of smoke from wildland fires, both prescribed and natural, on ambient air quality and human health. However, the accuracy of these models is limited by uncertainties in the parametrisation of smoke plume injection height (PIH) and its vertical distribution. We compared PIH estimates from the plume rise method (Briggs) in the Community Multiscale Air Quality (CMAQ) modelling system with observations from the 2013 California Rim Fire and 2017 prescribed burns in Kansas. We also examined PIHs estimated using alternative plume rise algorithms, model grid resolutions and temporal burn profiles. For the Rim Fire, the Briggs method performed as well or better than the alternatives evaluated (mean bias of less than ±5–20% and root mean square error lower than 1000 m compared with the alternatives). PIH estimates for the Kansas prescribed burns improved when the burn window was reduced from the standard default of 12 h to 3 h. This analysis suggests that meteorological inputs, temporal allocation and heat release are the primary drivers for accurately modelling PIH.

Wildland fire activity and associated emission of particulate matter air pollution is increasing in the United States over the last two decades due primarily to a combination of increased temperature, drought, and historically high forest fuel loading. The regulatory monitoring networks in the Unites States are mostly concentrated in larger population centers where anthropogenic air pollution sources are concentrated. Smaller population centers in areas more likely to be impacted by wildland fire smoke in many instances lack adequate observational air quality data. Several commercially available small form factor filter-based PM

Air pollution has been associated with poor health outcomes and continues to be a risk factor for respiratory health in children. While higher particulate matter (PM) levels are associated with increased frequency of symptoms, lower lung function, and increase airway inflammation from asthma, the precise composition of the particles that are more highly associated with poor health outcomes or healthcare utilization are not fully elucidated. PM is measured quantifiably by current air pollution monitoring systems. To better determine sources of PM and speciation of such sources, a particulate matter (PM) source apportionment study, the Cleveland Multiple Air Pollutant Study (CMAPS), was conducted in Cleveland, Ohio, in 2009–2010, which allowed more refined assessment of associations with health outcomes. This article presents an evaluation of short-term (daily) and long-term associations between motor vehicle and industrial air pollution components and pediatric asthma emergency department (ED) visits by evaluating two sets of air quality data with healthcare utilization for pediatric asthma. Exposure estimates were developed using land use regression models for long-term exposures for nitrogen dioxide (NO2) and coarse (i.e., with aerodynamic diameters between 2.5 and 10 μm) particulate matter (PM) and the US EPA Positive Matrix Factorization receptor model for short-term exposures to fine (

The extraction and upgrading of bitumen have been identified as sources of enhanced atmospheric deposition of pollutant elements to ecosystems in the Athabasca Oil Sands Region (AOSR) in northern Alberta, Canada. Bitumen extraction became increasingly efficient, and oil prices surged in the 1990s, resulting in rapid expansion and increased production over the last two decades. Here, we examine temporal and spatial trends in wintertime atmospheric deposition of pollutant elements in 1978, 1981, 2008, and 2011–2016 at broad spatial scales using snowpack measurements. A hybrid source analysis was conducted, including (i) simple and multiple linear regression (MLR) of identified source locations and elemental deposition, (ii) spatially resolved aluminum enrichment factors (Al EFs), and (iii) positive matrix factorization (PMF) to determine source profiles. Temporal trends revealed a general decrease in atmospheric loadings; however, near-field V, Ti, and Al loadings in 2016 were an order of magnitude greater ...

A comprehensive filter-based particulate matter polycyclic aromatic hydrocarbon (PAH) source apportionment study was conducted at the Wood Buffalo Environmental Association Bertha Ganter-Fort McKay (BGFM) community monitoring station from 2014 to 2015 to quantify ambient concentrations and identify major sources. The BGFM station is located in close proximity to several surface oil sands production facilities and was previously found to be impacted by their air emissions. 24-hour integrated PM2.5 and PM10–2.5 samples were collected on a 1-in-3-day schedule yielding 108 complete organic/inorganic filter sets for source apportionment modeling. During the study period PM2.5 averaged 8.6 ± 11.8 μg m−3 (mean ± standard deviation), and PM10–2.5 averaged 8.5 ± 9.5 μg m−3. Wind regression analysis indicated that the oil sands production facilities were significant sources of PM2.5 mass and black carbon (BC), and that wildland fires were a significant source of the highest PM2.5 (>10 μg m−3) and BC events. A six-factor positive matrix factorization (PMF) model solution explained 95% of the measured PM2.5 and 78% of the measured ΣPAH. Five sources significantly contributed to PM2.5 including: Biomass Combustion (3.57 μg m−3; 40%); Fugitive Dust (1.86 μg m−3; 28%); Upgrader Stack Emissions (1.44 μg m−3; 21%); Petrogenic PAH (1.20 μg m−3; 18%); and Transported Aerosol (0.43 μg m−3 and 6%). However, the analysis indicated that only the pyrogenic PAH source factor significantly contributed (78%) to the measured ΣPAH. A five-factor PMF model dominated by fugitive dust sources explained 98% of PM10–2.5 mass and 86% of the ΣPAH. The predominant sources of PM10–2.5 mass were (i) Haul Road Dust (4.82 μg m−3; 53%), (ii) Mixed Fugitive Dust (2.89 μg m−3; 32%), (iii) Fugitive Oil Sand (0.88 μg m−3; 10%), Mobile Sources (0.23 μg m−3; 2%), and Organic Aerosol (0.06 μg m−3; 1%). Only the Organic Aerosol source significantly contributed (86%) to the measured ΣPAH.

Ambient air particulate matter (PM) was collected at the Wood Buffalo Environmental Association Bertha Ganter Fort McKay monitoring station in the Athabasca Oil Sand Region (AOSR) in Alberta, Canada from February 2010 to July 2011 as part of an air quality source assessment study. Daily 24-hour duration fine (PM2.5) and coarse (PM10–2.5) PM was collected using a sequential dichotomous sampler. 100 pairs of PM2.5 and PM10–2.5 were selected for lead (Pb) concentration and isotope analysis. Pb isotope and concentration results from 250 epiphytic lichen samples collected as far as 160 km from surface mining operations in 2008, 2011, and 2014 were analyzed to examine longer term spatial variations in Pb source contributions. A key finding was recognition of thorogenic 208Pb from eastern Asia in the springtime in the PM2.5 in 2010 and 2011. 206Pb/207Pb and 208Pb/207Pb isotope ratios were used in a three-component mixing model to quantify local, regional, and global Pb sources in the PM and lichen data sets. 47 ± 3% of the Pb in the PM2.5 at AMS-1 was attributed to sources from eastern Asia. Combined results from PM10–2.5 and PM2.5 indicate PM2.5 Pb contributions from eastern Asia (34%) exceed local AOSR sources of PM2.5 Pb (20%), western Canada sources of PM2.5 Pb (19%), and PM10–2.5 Pb from fugitive dust including oil sands (14%), tailings (10%), and haul roads (3%). The lichen analysis indicates regional sources contribute 46% of the Pb, local sources 32%, and global sources 22% over the 2008–2014 timeframe. Local sources dominate atmospheric Pb deposition to lichens at near field sites (0–30 km from mining operations) whereas regional Pb sources are prevalent at distal sites (30–160 km). The Pb isotope methodology successfully quantified trans-Pacific transport of Pb to the AOSR superimposed over the aerosol footprint of the world's largest concentration of bitumen mining and upgrading facilities.

The sources and spatial distribution of polycyclic aromatic hydrocarbons (PAHs) atmospheric deposition in the boreal forests surrounding bitumen production operations in the Athabasca Oil Sands Region (AOSR), Alberta, Canada were investigated as part of a 2014 passive in-situ bioindicator source apportionment study. Epiphytic lichen species Hypogymnia physodes samples (n = 127) were collected within a 150 km radius of the main surface oil sand production operations and analyzed for total sulfur, total nitrogen, forty-three elements, twenty-two PAHs, ten groups of C1-C2-alkyl PAHs and dibenzothiophenes (polycyclic aromatic compounds; PACs), five C1- and C2-alkyldibenzothiophenes, and retene. The ΣPAH + PAC in H. physodes ranged from 54 to 2778 ng g−1 with a median concentration of 317 ng g−1. Source apportionment modeling found an eight-factor solution that explained 99% of the measured ΣPAH + PAC lichen concentrations from four anthropogenic oil sands production sources (Petroleum Coke, Haul Road Dust, Stack Emissions, Raw Oil Sand), two local/regional sources (Biomass Combustion, Mobile Source), and two lichen biogeochemical factors. Petroleum Coke and Raw Oil Sand dust were identified as the major contributing sources of ΣPAH + PAC in the AOSR. These two sources accounted for 63% (43.2 μg g−1) of ΣPAH + PAC deposition to the entire study domain. Of this overall 43.2 μg g−1 contribution, approximately 90% (39.9 μg g−1) ΣPAH + PAC was deposited within 25 km of the closest oil sand production facility. Regional sources (Biomass Combustion and Mobile Sources) accounted for 19% of ΣPAH + PAC deposition to the entire study domain, of which 46% was deposited near-field to oil sand production operations. Source identification was improved over a prior lichen-based study in the AOSR through incorporation of PAH and PAC analytes in addition to inorganic analytes.

In recent years wildland fires in the United States have had significant impacts on local and regional air quality and negative human health outcomes. Although the primary health concerns from wildland fires come from fine particulate matter (PM2.5), large increases in ozone (O3) have been observed downwind of wildland fire plumes (DeBell et al., 2004; Bytnerowicz et al., 2010; Preisler et al., 2010; Jaffe et al., 2012; Bytnerowicz et al., 2013; Jaffe et al., 2013; Lu et al., 2016; Lindaas et al., 2017; McClure and Jaffe, 2018; Liu et al., 2018; Baylon et al., 2018; Buysse et al., 2019). Conditions generated in and around wildland fire plumes, including the presence of interfering chemical species, can make the accurate measurement of O3 concentrations using the ultraviolet (UV) photometric method challenging if not impossible. UV photometric method instruments are prone to interferences by volatile organic compounds (VOCs) that are present at high concentrations in wildland fire smoke. Four different O3 measurement methodologies were deployed in a mobile sampling platform downwind of active prescribed grassland fire lines in Kansas and Oregon and during controlled chamber burns at the United States Forest Service, Rocky Mountain Research Station Fire Sciences Laboratory in Missoula, Montana. We demonstrate that the Federal Reference Method (FRM) nitric oxide (NO) chemiluminescence monitors and Federal Equivalent Method (FEM) gas-phase (NO) chemical scrubber UV photometric O3 monitors are relatively interference-free, even in near-field combustion plumes. In contrast, FEM UV photometric O3 monitors using solid-phase catalytic scrubbers show positive artifacts that are positively correlated with carbon monoxide (CO) and total gas-phase hydrocarbon (THC), two indicator species of biomass burning. Of the two catalytic scrubber UV photometric methods evaluated, the instruments that included a Nafion® tube dryer in the sample introduction system had artifacts an order of magnitude smaller than the instrument with no humidity correction. We hypothesize that Nafion®-permeating VOCs (such as aromatic hydrocarbons) could be a significant source of interference for catalytic scrubber UV photometric O3 monitors and that the inclusion of a Nafion® tube dryer assists with the mitigation of these interferences. The chemiluminescence FRM method is highly recommended for accurate measurements of O3 in wildland fire plume studies and at regulatory ambient monitoring sites frequently impacted by wildland fire smoke.

This air synthesis review presents the current state of knowledge on the sources, fates, and effects for polycyclic aromatic compounds (PACs) and related chemicals released to air in the oil sands region (OSR) in Alberta, Canada. Through the implementation of the Joint Canada–Alberta Oil Sands Monitoring Program in 2012 a vast amount of new information on PACs has been acquired through directed monitoring and research projects and reported to the scientific community and public. This new knowledge addresses questions related to cumulative effects and informs the sustainable management of the oil sands resource while helping to identify gaps in understanding and priorities for future work. As a result of this air synthesis review on PACs, the following topics have been identified as new science priorities: (i) improving emissions reporting to better account for fugitive mining emissions of PACs that includes a broader range of PACs beyond the conventional polycyclic aromatic hydrocarbons (PAHs) including, inter alia, alkylated-PAHs (alk-PAHs), dibenzothiophene (DBT), alk-DBTs, nitro-PAHs, oxy-PAHs including quinones and thia- and aza-arenes; (ii) improving information on the ambient concentrations, long-range transport, and atmospheric deposition of these broader classes of PACs and their release (with co-contaminants) from different types of mining activities; (iii) further optimizing electricity-free and cost-effective approaches for assessing PAC deposition (e.g., snow sampling, lichens, passive ambient sampling) spatially across the OSR and downwind regions; (iv) designing projects that integrate monitoring efforts with source attribution models and ecosystem health studies to improve understanding of sources, receptors, and effects; (v) further optimizing natural deposition archives (e.g., sediment, peat, tree rings) and advanced forensic techniques (e.g., isotope analysis, marker compounds) to provide better understanding of sources of PACs in the OSR over space and time; (vi) conducting process research to improve model capabilities for simulating atmospheric chemistry of PACs and assessing exposure to wildlife and humans; and (vii) developing tools and integrated strategies for assessing cumulative risk to wildlife and humans by accounting for the toxicity of the mixture of chemicals in air rather than on a single compound basis.

Wildland fire activity and associated emission of particulate matter air pollution is increasing in the United States over the last two decades due primarily to a combination of increased temperature, drought, and historically high forest fuel loading. The regulatory monitoring networks in the Unites States are mostly concentrated in larger population centers where anthropogenic air pollution sources are concentrated. Smaller population centers in areas more likely to be impacted by wildland fire smoke in many instances lack adequate observational air quality data. Several commercially available small form factor filter-based PM2.5 samplers (SFFFS) were evaluated under typical ambient and simulated near-to mid-field wildland fire smoke conditions to evaluate their accuracy for use in temporary deployments during prescribed and wildfire events. The performance of all the SFFFS tested versus the designated federal reference methods (FRM) was acceptable in determining PM2.5 concentration in both ambient (2.7–14.0 μg m−3) and chamber smoke environments (24.6–3044.6 μg m−3) with accuracies ranging from ∼92 to 98%. However, only the ARA Instruments model N-FRM Sampler was found to provide PM2.5 mass measurement accuracies that meet FRM guideline performance specifications under both typical ambient (97.3 ± 1.9%) and simulated wildland fire conditions (98.2 ± 1.4%).

The increasing emission of primary and gaseous precursors of secondarily formed atmospheric particulate matter due to continuing industrial development and urbanization are leading to an increased public awareness of environmental issues and human health risks in China. As part of a pilot study, 12-h integrated fine fraction particulate matter (PM2.5) filter samples were collected to chemically characterize and investigate the sources of ambient particulate matter in Guiyang City, Guizhou Province, southwestern China. Results showed that the 12-h integrated PM2.5 concentrations exhibited a daytime average of 51 ± 22 µg m−3 (mean ± standard deviation) with a range of 17–128 µg m−3 and a nighttime average of 55 ± 32 µg m−3 with a range of 4–186 µg m−3. The 24-h integrated PM2.5 concentrations varied from 15 to 157 µg m−3, with a mean value of 53 ± 25 µg m−3, which exceeded the 24-h PM2.5 standard of 35 µg m−3 set by USEPA, but was below the standard of 75 µg m−3, set by China Ministry of Environmental Protection. Energy-dispersive X-ray fluorescence spectrometry (XRF) was applied to determine PM2.5 chemical element concentrations. The order of concentrations of heavy metals in PM2.5 were iron (Fe) > zinc (Zn) > manganese (Mn) > lead (Pb) > arsenic (As) > chromium (Cr). The total concentration of 18 chemical elements was 13 ± 2 µg m−3, accounting for 25% in PM2.5, which is comparable to other major cities in China, but much higher than cities outside of China.

An unprecedented wildfire impacted the northern Alberta city of Fort McMurray in May 2016 causing a mandatory city wide evacuation and the loss of 2,400 homes and commercial structures. A two-hectare wildfire was discovered on May 1, grew to ~157,000 ha by May 5, and continued to burn an estimated ~590,000 ha by June 13. A comprehensive air monitoring network operated by the Wood Buffalo Environmental Association (WBEA) in and around Fort McMurray provided essential health-related real-time air quality data to firefighters during the emergency, and provided a rare opportunity to elucidate the impact of gaseous and particulate matter emissions on near-field communities and regional air pollution concentrations. The WBEA network recorded 188 fire-related exceedances of 1-hr and 24-hr Alberta Ambient Air Quality Objectives. Two air monitoring sites within Fort McMurray recorded mean/maximum 1-hr PM2.5 concentrations of 291/5229 μg m−3 (AMS-6) and 293/3259 μg m−3 (AMS-7) during fire impact periods. High correlations (r2 = 0.83–0.97) between biomass combustion related gases (carbon monoxide (CO), non-methane hydrocarbons (NMHC), total hydrocarbons (THC), total reduced sulfur (TRS), ammonia) and PM2.5 were observed at the sites. Filter-based 24-hr integrated PM2.5 samples collected every 6 days showed maximum concentrations of 267 μg m−3 (AMS-6) and 394 μg m−3 (AMS-7). Normalized excess emission ratios relative to CO were 149.87 ± 3.37 μg m−3 ppm−1 (PM2.5), 0.274 ± 0.002 ppm ppm−1 (THC), 0.169 ± 0.001 ppm ppm−1 (NMHC), 0.104 ± 0.001 ppm ppm−1 (CH4), 0.694 ± 0.007 ppb ppm−1 (TRS), 0.519 ± 0.040 ppb ppm−1 (SO2), 0.412 ± 0.045 ppb ppm−1 (NO), 1.968 ± 0.053 ppb ppm−1 (NO2), and 2.337 ± 0.077 ppb ppm−1 (NOX). A subset of PM2.5 filter samples was analyzed for trace elements, major ions, organic carbon, elemental carbon, and carbohydrates. Sample mass reconstruction and fire specific emission profiles are presented and discussed. Potential fire-related photometric ozone instrument positive interferences were observed and were positively correlated with NO and NMHC., GRAPHICAL ABSTRACT

A 2014 case study investigated the relative accumulation efficiency of polycyclic aromatic hydrocarbons (PAHs), total sulfur (S), total nitrogen (N), major and minor elements and Pb isotopes in five common lichen species at three boreal forest sites in the Athabasca Oil Sands Region (AOSR) in northeastern Alberta, Canada to identify the optimum lichen species for future biomonitoring. Differences in concentrations of PAHs, multiple elements, and Pb isotopes in fruticose (Bryoria furcellata, Cladina mitis, Evernia mesomorpha) and foliose (Hypogymnia physodes and Tuckermannopsis americana) lichens were found along a 100 km distance gradient from the primary oil sands operations. Integration of insights from emission source samples and oil sands mineralogy in consort with aerosol collection indicates incorporation of more fine particulate matter (PM) into foliose than fruticose lichen biomass. Contrasting PAH with element concentrations allowed lichen species specific accumulation patterns to be identified. The ability of lichen species to incorporate different amounts of gas phase (S and N), petrogenic (V, Ni, Mo), clay (low Si/Al and more rare earth elements), and sand (higher Si/Al and Ti) components from the oil sand operations reflects aerosol particle size and lichen physiology differences that translate into differences in PM transport distances and lichen accumulation efficiencies. Based on these findings Hypogymnia physodes is recommended for future PAH biomonitoring and source attribution studies.

International audience; Mercury (Hg) emissions from biomass burning (BB) are an important source of atmospheric Hg and a major factor driving the interannual variation of Hg concentrations in the troposphere. The greatest fraction of Hg from BB is released in the form of elemental Hg (Hg0(g)). However, little is known about the fraction of Hg bound to particulate matter (HgP) released from BB, and the factors controlling this fraction are also uncertain. In light of the aims of the Minamata Convention to reduce intentional Hg use and emissions from anthropogenic activities, the relative importance of Hg emissions from BB will have an increasing impact on Hg deposition fluxes. Hg speciation is one of the most important factors determining the redistribution of Hg in the atmosphere and the geographical distribution of Hg deposition. Using the latest version of the Global Fire Emissions Database (GFEDv4.1s) and the global Hg chemistry transport model, ECHMERIT, the impact of Hg speciation in BB emissions, and the factors which influence speciation, on Hg deposition have been investigated for the year 2013. The role of other uncertainties related to physical and chemical atmospheric processes involving Hg and the influence of model parametrisations were also investigated, since their interactions with Hg speciation are complex. The comparison with atmospheric HgP concentrations observed at two remote sites, Amsterdam Island (AMD) and Manaus (MAN), in the Amazon showed a significant improvement when considering a fraction of HgP from BB. The set of sensitivity runs also showed how the quantity and geographical distribution of HgP emitted from BB has a limited impact on a global scale, although the inclusion of increasing fractions HgP does limit Hg0(g) availability to the global atmospheric pool. This reduces the fraction of Hg from BB which deposits to the world's oceans from 71 to 62 %. The impact locally is, however, significant on northern boreal and tropical forests, where fires are frequent, uncontrolled and lead to notable Hg inputs to local ecosystems. In the light of ongoing climatic changes this effect could be potentially be exacerbated in the future.

The increasing emission of primary and gaseous precursors of secondarily formed atmospheric particulate matter due to continuing industrial development and urbanization are leading to an increased public awareness of environmental issues and human health risks in China. As part of a pilot study, 12-hr integrated fine fraction particulate matter (PM(2.5)) filter samples were collected to chemically characterize and investigate the sources of ambient particulate matter in Guiyang City, Guizhou Province, southwestern China. Results showed that the 12-hr integrated PM(2.5) concentrations exhibited a daytime average of 51 ± 22μg·m(−3) (mean ± standard deviation) with a range of 17–128μg·m(−3) and a nighttime average of 55 ± 32μg·m(−33) with a range of 4–186 μg·m(−3). The 24-hr integrated PM(2.5) concentrations varied from 15 to 157 μg·m-3, with a mean value of 53 ± 25 μg·m(−3), which exceeded the 24-hr PM(2.5) standard of 35μg·m(−3) set by USEPA, but was below the standard of 75μg·m(−3), set by China Ministry of Environmental Protection. Energy-dispersive X-ray fluorescence spectrometry (XRF) was applied to determine PM(2.5) chemical element concentrations. The order of concentrations of heavy metals in PM(2.5) were iron (Fe) > zinc (Zn) > manganese (Mn) > lead (Pb) > arsenic (As) > chromium (Cr). The total concentration of 18 chemical elements was 13 ± 2 μg·m(−3), accounting for 25% in PM(2.5), which is comparable to other major cities in China, but much higher than cities outside of China.

The characteristics of wildland fire smoke exposures which initiate or exacerbate cardiopulmonary conditions are unclear. We previously reported that, on a mass basis, lung toxicity associated with particulate matter (PM) from flaming smoke aspirated into mouse lungs is greater than smoldering PM. In this study, we developed a computer-controlled inhalation system which can precisely control complex biomass smoke emissions from different combustion conditions. This system was used to examine the toxicity of inhaled biomass smoke from peat, eucalyptus, and oak fuels generated under smoldering and flaming phases with emissions set to the same approximate concentration of carbon monoxide (CO) for each exposure (60–110 ppm), resulting in PM levels of ~ 4 mg/m3 for flaming and ~ 40 mg/m3 for smoldering conditions. Mice were exposed by inhalation 1 h/day for 2 days, and assessed for lung toxicity at 4 and 24 h after the final exposure. Peat (flaming and smoldering) and eucalyptus (smoldering) smoke elicited significant inflammation (neutrophil influx) in mouse lungs at 4 h with the peat (flaming) smoke causing even greater lung inflammation at 24-h post-exposure. A significant alteration in ventilatory timing was also observed in mice exposed to the peat (flaming) and eucalyptus (flaming and smoldering) smoke immediately after each day of exposure. No responses were seen for exposures to similar concentrations of flaming or smoldering oak smoke. The lung toxicity potencies (neutrophil influx per PM mass) agreed well between the inhalation and previously reported aspiration studies, demonstrating that although flaming smoke contains much less PM mass than smoldering smoke, it is more toxic on a mass basis than smoldering smoke exposure, and that fuel type is also a controlling factor.

Temporal and spatial atmospheric deposition trends of elements to the boreal forest surrounding bitumen production operations in the Athabasca Oil Sands Region (AOSR), Alberta, Canada were investigated as part of a long-term lichen bioindicator study. The study focused on eight elements (sulfur, nitrogen, aluminum, calcium, iron, nickel, strontium, vanadium) that were previously identified as tracers for the major oil sand production sources. Samples of the in situ epiphytic lichen Hypogymnia physodes were collected in 2002, 2004, 2008, 2011, 2014, and 2017 within a ~150 km radius from the center of surface oil sand production operations in the AOSR. Site-specific time series analysis conducted at eight jack pine upland sites that were repeatedly sampled generally showed significant trends of increasing lichen concentrations for fugitive dust linked elements, particularly at near-field (25 km from a major oil sands production operation) sample locations. Multiple regional scale geostatistical models were developed and evaluated to characterize broad-scale changes in atmospheric deposition based on changes in H. physodes elemental concentrations between 2008 and 2014. Empirical Bayesian kriging and cokriging lichen element concentrations with oil sands mining, bitumen upgrading, coke materials handling, and limestone quarry/crushing influence variables produced spatial interpolation estimates with the lowest validation errors. Gridded zonal mean lichen element concentrations were calculated for the two comprehensive sampling years (2008, 2014) and evaluated for spatial and temporal change. Lichen sulfur concentrations significantly increased in every grid cell within the domain with the largest increases (44-88%) in the central valley in close proximity to the major surface oil sand production operations, while a minor nitrogen concentration decrease (-20%) in a single grid cell was observed. The areal extent of fugitive dust element deposition generally increased with significantly higher deposition to lichens restricted to the outer grids of the enhanced deposition field, reflecting new and expanding surface mining activity.

Wildland fires can emit substantial amounts of air pollution that may pose a risk to those in proximity (e.g., first responders, nearby residents) as well as downwind populations. Quickly deploying air pollution measurement capabilities in response to incidents has been limited to date by the cost, complexity of implementation, and measurement accuracy. Emerging technologies including miniaturized direct-reading sensors, compact microprocessors, and wireless data communications provide new opportunities to detect air pollution in real time. The U.S. Environmental Protection Agency (EPA) partnered with other U.S. federal agencies (CDC, NASA, NPS, NOAA, USFS) to sponsor the Wildland Fire Sensor Challenge. EPA and partnering organizations share the desire to advance wildland fire air measurement technology to be easier to deploy, suitable to use for high concentration events, and durable to withstand difficult field conditions, with the ability to report high time resolution data continuously and wirelessly. The Wildland Fire Sensor Challenge encouraged innovation worldwide to develop sensor prototypes capable of measuring fine particulate matter (PM2.5), carbon monoxide (CO), carbon dioxide (CO2), and ozone (O3) during wildfire episodes. The importance of using federal reference method (FRM) versus federal equivalent method (FEM) instruments to evaluate performance in biomass smoke is discussed. Ten solvers from three countries submitted sensor systems for evaluation as part of the challenge. The sensor evaluation results including sensor accuracy, precision, linearity, and operability are presented and discussed, and three challenge winners are announced. Raw solver submitted PM2.5 sensor accuracies of the winners ranged from ~22 to 32%, while smoke specific EPA regression calibrations improved the accuracies to ~75–83% demonstrating the potential of these systems in providing reasonable accuracies over conditions that are typical during wildland fire events., GRAPHICAL ABSTRACT

Communities near major roadways are disproportionately affected by traffic-related air pollution which can contribute to adverse health outcomes. The specific role of particulate matter (PM) from traffic sources is not fully understood due to complex emissions processes and physical/chemical properties of PM in the near-road environment. To investigate the spatial profile and water solubility of elemental PM species near a major roadway, filter-based measurements of fine (PM 2.5 ) and coarse (PM 10-2.5 ) PM were simultaneously collected at multiple distances (10 m, 100 m, and 300 m) from Interstate I-96 in Detroit, Michigan during September–November 2010. Filters were extracted in water, followed by a hot acid extraction, and analyzed by magnetic sector field high resolution inductively coupled plasma mass spectrometry (HR-ICPMS) to quantify water-soluble and acid-soluble trace elements for each PM size fraction. PM 2.5 and PM 10-2.5 species measured in the near-road samples included elements associated with traffic activity, local industrial sources, and regional pollution. Metals indicative of brake wear (Ba, Cu) were dramatically enriched near the roadway during downwind conditions (factor of 5 concentration increase), with the largest increase within 100 m of the roadway. Moderate near-roadway increases were observed for crustal elements and other traffic-related PM (Fe, Ca), and the lowest increases observed for regional PM species (S). Water solubility varied by PM species and size, and for PM 2.5 included highly (S, K, Ca, Mg, Zn, Ba), moderately (Cu, Mn, Sb, Pb), and minimally (Fe, Ti) water-soluble species, with lower water solubility for most species in PM 10-2.5 . Results from this study indicate that water-soluble PM 2.5 and PM 10-2.5 metals, particularly from brake/tire wear, were enhanced in the near-roadway environment which may have human health implications.

The Cleveland airshed comprises a complex mixture of industrial source emissions that contribute to periods of non-attainment for fine particulate matter (PM2.5) and are associated with increased adverse health outcomes in the exposed population. Specific PM sources responsible for health effects however are not fully understood. Size-fractionated PM (coarse, fine, and ultrafine) samples were collected using a ChemVol sampler at an urban site (G.T. Craig (GTC)) and rural site (Chippewa Lake (CLM)) from July 2009 to June 2010, and then chemically analyzed. The resulting speciated PM data were apportioned by EPA positive matrix factorization to identify emission sources for each size fraction and location. For comparisons with the ChemVol results, PM samples were also collected with sequential dichotomous and passive samplers, and evaluated for source contributions to each sampling site. The ChemVol results showed that annual average concentrations of PM, elemental carbon, and inorganic elements in the coarse fraction at GTC were ∼2, ∼7, and ∼3 times higher than those at CLM, respectively, while the smaller size fractions at both sites showed similar annual average concentrations. Seasonal variations of secondary aerosols (e.g., high NO3− level in winter and high SO42− level in summer) were observed at both sites. Source apportionment results demonstrated that the PM samples at GTC and CLM were enriched with local industrial sources (e.g., steel plant and coal-fired power plant) but their contributions were influenced by meteorological conditions and the emission source's operation conditions. Taken together the year-long PM collection and data analysis provides valuable insights into the characteristics and sources of PM impacting the Cleveland airshed in both the urban center and the rural upwind background locations. These data will be used to classify the PM samples for toxicology studies to determine which PM sources, species, and size fractions are of greatest health concern.

The Hg0 time series recorded at the Mauna Loa Observatory (MLO) in Hawaii between 2002 and 2009 has been analyzed using Empirical Mode Decomposition. This technique has been used in numerous contexts in order to identify periodical variations in time series data. The periodicities observed in the tropical Pacific sea surface temperature (SST), through the data collected from five buoys, are also observed in Hg0 concentrations and the relative humidity measured at the MLO. The lag times in the observed periodicities are related to the position of the buoys with respect to the measurement site. This demonstrates a direct link between climatological phenomena, in this case SST, and measured Hg0 and reflects the influence of ocean SST on Hg0 evasion. This is the first long-term experimental evidence of such a direct effect on Hg0 evasion from the oceanic surface driven by temperature.

Continuous measurements of speciated atmospheric mercury (Hg), including gaseous elemental mercury (GEM), particulate mercury (PHg), and reactive gaseous mercury (RGM) were conducted in Guizhou Province, southwestern China. Guiyang Power Plant (GPP), Guiyang Wujiang Cement Plant, Guizhou Aluminum Plant (GAP), and Guiyang Forest Park (GFP) in Guiyang were selected as study sites. Automatic Atmospheric Mercury Speciation Analyzers (Tekran 2537A) were used for GEM analysis. PHg and RGM were simultaneously collected by a manual sampling system, including elutriator, coupler/impactor, KCl-coated annular denuder, and a filter holder. Results show that different emission sources dominate different species of Hg. The highest average GEM value was 22.2 ± 28.3 ng·m−3 and the lowest 6.1 ± 3.9 ng·m−3, from samples collected at GPP and GAP, respectively. The maximum average PHg was 1984.9 pg·m−3 and the minimum average 55.9 pg·m−3, also from GPP and GAP, respectively. Similarly, the highest average RGM of 68.8 pg·m−3 was measured at GPP, and the lowest level of 20.5 pg·m−3 was found at GAP. We conclude that coal combustion sources are still playing a key role in GEM; traffic contributes significantly to PHg; and domestic pollution dominates RGM.

Event-based precipitation samples were collected at a downtown industrial and a predominantly upwind rural location in the Cleveland, Ohio metropolitan area from July 2009 through December 2010 to investigate the potential local total mercury (Hg) wet deposition enhancement in a region with a high concentration of coal combustion sources. Total Hg wet deposition for the 18-month period was 6.8 μg m −2 (n = 81) at the rural site and 10.7 μg m −2 (n = 98) at the urban site demonstrating a significant ( p = 0.046) 37% enhancement in deposition between the two sites. Large deposition events (>0.2 μg m −2 ) occurred predominantly from May through October (n = 16 (urban), n = 10 (rural)) and represented from 2 to 8% of total 18-month deposition per event. At the downtown urban site, the average Hg precipitation concentration was 53% higher for these large deposition events. Concurrently measured precipitation events delivered in aggregate 2.4 times more total Hg wet deposition to the urban site compared to the rural site. Hg rainfall concentrations for concurrent events with similar precipitation depth were 2–4 times higher at the urban site and suggest scavenging of local Hg emissions. Further evaluation of these events revealed 83% more total Hg deposition at the urban site from January to December 2010 compared to July to December 2009, while there was 26% more at the rural site during these same time periods. The larger increase in deposition at the urban site in 2010 may be evidence of increased local emissions from sources that were known to be offline during this study period because of an economic recession.

Trace gas, particulate matter and deposition data collected in the Athabasca Oil Sands Region (AOSR) from 2000 to 2017 were evaluated as part of a broad scientific programmatic review. Results showed significant spatial patterns and temporal trends across the region. Concentrations of reactive gases were highest near the center of surface oil sands production operations and decreased towards the edges of the monitoring domain by factors of 8, 20, 4 and 3 for SO2, NO2, HNO3 and NH3, respectively. 18 of 30 sites showed statistically significant (p 80% of SO42− was in the PM2.5 fraction, while > 60% of Ca2+, Mg2+, Na+ and Cl− were in the PM10-2.5 fraction. Ion balances of both PM10 and PM2.5 contained cation excesses at near-field oil sand sites, but PM2.5 samples at forest health sites >20 km from surface production locations contained anion excesses. Monthly average concentrations of PM10 ions showed peak Ca2+ during March-April to November, but peak SO42−, NH4+ and NO3− from November-March. Deposition estimates showed rapid declines as a function of distance to oil sand operations. Estimated total N and total S deposition to forest health monitoring sites ranged from 2.0 to 5.7 kg ha−1 a−1 and 2.1–14.0 kg ha−1 a−1, respectively. Potential acid input (PAI) ranged from −0.46 to 0.79 keq ha−1 a−1 and was mostly 0.1–0.2 keq ha−1 a−1 throughout the domain, except for two clusters of sites near oil sand operations.

Accurate characterization of the chemical composition of particulate matter (PM) is essential for improved understanding of source attribution and resultant health impacts. To explore this we conducted ambient monitoring of a suite of 15 combustion-related organic species in temporally resolved PM 2.5 samples during an ongoing animal exposure study in a near source environment in Detroit, MI. All of the 15 species detected were above the method detection limit in 8 hour samples. This study focused on two molecular classes: Polycyclic Aromatic Hydrocarbons (PAHs) and Hopanes measured in samples. Of the 12 PAHs studied, benzo[b]fluoranthene (169 pg m−3), benzo[g,h,i]perylene (124 pg m−3), and benzo[e]pyrene (118, pg m−3) exhibited the three highest mean concentrations while 17α(H),21β(H)-Hopane (189 pg m−3) and 17α(H),21β(H)-30-Norhopane (145 pg m−3) had the highest mean concentrations of the 3 Hopanes analyzed in samples. Ratios of individual compound concentrations to total compound concentrations (∑ 15 compounds) showed the greatest daily variation for 17α(H),21β(H)-Hopane (11–28%) and 17α(H),21β(H)-30-Norhopane (8–20%). Diagnostic PAH concentration ratios ([IP]/[IP + BP] (range 0.30 – 0.45), [BaP]/[BaP+BeP] (range 0.26 – 0.44), [BaP]/[BP] (range 0.41 – 0.82), [Bb]/[Bk] (range 2.07 – 2.66), in samples reflected impacts froma mixture of combustion sources consistent with greater prevalence of petroleum combustion source emissions (gasoline, diesel, kerosene, and crude oil) compared to coal or wood combustion emissions impacts at this urban site. Results from this study demonstrate that short duration sampling for organic speciation provides temporally relevant exposure information.

Surface water conductivity measurements were used to evaluate the combined contribution of anions in western Pennsylvania from brines discharged by sources such as oil and gas wastewater treatment, coal-fired power plants, and coal mining activities. Conductivity sensor data were collected in the Allegheny River during a US Environmental Protection Agency and US Fish and Wildlife study that included seven sites covering 256 river km during the fall of 2012. Intermittent discharges, such as oil and gas wastewater, and continuous sources contributing to the conductivity were quantified using constrained and adaptive decomposition of time-series (CADETS) frequency analysis. CADETS was able to quantify the intermittent or short-term component of conductivity at sites where the intermittent fraction was 1 to 22% of the total conductivity. The demonstrated efficacy of the CADETS method for surface water quality analysis suggests it could be widely used to evaluate other water sensor data in rivers with both continuous and intermittent source impacts.

During May 2016 a very large boreal wildfire burned throughout the Athabasca Oil Sands Region (AOSR) in central Canada, and in close proximity to an extensive air quality monitoring network. This study examines speciated 24-h integrated polycyclic aromatic hydrocarbon (PAH) and volatile organic compound (VOC) measurements collected every sixth day at four and seven sites, respectively, from May to August 2016. The sum of PAHs (ΣPAH) was on average 17 times higher in fire-influenced samples (852 ng m-3, n = 8), relative to non-fire influenced samples (50 ng m-3, n = 64). Diagnostic PAH ratios in fire-influenced samples were indicative of a biomass burning source, whereas ratios in June to August samples showed additional influence from petrogenic and fossil fuel combustion. The average increase in the sum of VOCs (ΣVOC) was minor by comparison: 63 ppbv for fire-influenced samples (n = 16) versus 46 ppbv for non-fire samples (n = 90). The samples collected on August 16th and 22nd had large ΣVOC concentrations at all sites (average of 123 ppbv) that were unrelated to wildfire emissions, and composed primarily of acetaldehyde and methanol suggesting a photochemically aged air mass. Normalized excess enhancement ratios (ERs) were calculated for 20 VOCs and 23 PAHs for three fire influenced samples, and the former were generally consistent with previous observations. To our knowledge, this is the first study to report ER measurements for a number of VOCs and PAHs in fresh North American boreal wildfire plumes. During May the aged wildfire plume intercepted the cities of Edmonton (∼380 km south) or Lethbridge (∼790 km south) on four separate occasions. No enhancement in ground-level ozone (O3) was observed in these aged plumes despite an assumed increase in O3 precursors. In the AOSR, the only daily-averaged VOCs which approached or exceeded the hourly Alberta Ambient Air Quality Objectives (AAAQOs) were benzene (during the fire) and acetaldehyde (on August 16th and 22nd). Implications for local and regional air quality as well as suggestions for supplemental air monitoring during future boreal fires, are also discussed.

Background: The increasing size and frequency of wildland fires are leading to greater potential for cardiopulmonary disease and cancer in exposed populations; however, little is known about how the types of fuel and combustion phases affect these adverse outcomes. Objectives: We evaluated the mutagenicity and lung toxicity of particulate matter (PM) from flaming vs. smoldering phases of five biomass fuels, and compared results by equal mass or emission factors (EFs) derived from amount of fuel consumed. Methods: A quartz-tube furnace coupled to a multistage cryotrap was employed to collect smoke condensate from flaming and smoldering combustion of red oak, peat, pine needles, pine, and eucalyptus. Samples were analyzed chemically and assessed for acute lung toxicity in mice and mutagenicity in Salmonella. Results: The average combustion efficiency was 73 and 98% for the smoldering and flaming phases, respectively. On an equal mass basis, PM from eucalyptus and peat burned under flaming conditions induced significant lung toxicity potencies (neutrophil/mass of PM) compared to smoldering PM, whereas high levels of mutagenicity potencies were observed for flaming pine and peat PM compared to smoldering PM. When effects were adjusted for EF, the smoldering eucalyptus PM had the highest lung toxicity EF (neutrophil/mass of fuel burned), whereas smoldering pine and pine needles had the highest mutagenicity EF. These latter values were approximately 5, 10, and 30 times greater than those reported for open burning of agricultural plastic, woodburning cookstoves, and some municipal waste combustors, respectively. Conclusions: PM from different fuels and combustion phases have appreciable differences in lung toxic and mutagenic potency, and on a mass basis, flaming samples are more active, whereas smoldering samples have greater effect when EFs are taken into account. Knowledge of the differential toxicity of biomass emissions will contribute to more accurate hazard assessment of biomass smoke exposures. https://doi.org/10.1289/EHP2200

International audience; The probability density function (PDF) of the time intervals between subsequent extreme events in atmospheric Hg0 concentration data series from different latitudes has been investigated. The Hg0 dynamic possesses a long-term memory autocorrelation function. Above a fixed threshold Q in the data, the PDFs of the interoccurrence time of the Hg0 data are well described by a Tsallis q-exponential function. This PDF behavior has been explained in the framework of superstatistics, where the competition between multiple mesoscopic processes affects the macroscopic dynamics. An extensive parameter μ, encompassing all possible fluctuations related to mesoscopic phenomena, has been identified. It follows a χ2 distribution, indicative of the superstatistical nature of the overall process. Shuffling the data series destroys the long-term memory, the distributions become independent of Q, and the PDFs collapse on to the same exponential distribution. The possible central role of atmospheric turbulence on extreme events in the Hg0 data is highlighted.

Oil and gas extraction and coal-fired electrical power generating stations produce wastewaters that are treated and discharged to rivers in Western Pennsylvania with public drinking water system (PDWS) intakes. Inductively coupled plasma optical emission spectroscopy (ICP-OES) was used to quantify inorganic species in wastewater and river samples using a method based on EPA Method 200.7 rev4.4. A total of 53 emission lines from 30 elements (Al, As, B, Ba, Ca, Cd, Ce, Co, Cr, Cu, Fe, K, Li, Mg, Mn, Mo, Na, Ni, P, Pb, S, Sb, Se, Si, Sn, Sr, Ti, Tl, V, and Zn) were investigated. Samples were prepared by microwave-assisted acid digestion using a mixture of 2% HNO3 and 0.5% HCl. Lower interferences and better detection characteristics resulted in selection of alternative wavelengths for Al, As, Sb, Mg, Mo, and Na. Radial view measurements offered accurate determinations of Al, Ba, K, Li, Na, and Sr in high-brine samples. Spike recovery studies and analyses of reference materials showed 80-105% recoveries for most analytes. This method was used to quantify species in samples with high to low brine concentrations with method detection limits a factor of 2 below the maximum contaminant limit concentrations of national drinking water standards. Elements B, Ca, K, Li, Mg, Na, and Sr were identified as potential tracers for the sources impacting PDWS intakes. Usability of the ICP-OES derived data for factor analytic model applications was also demonstrated.

The anthropogenic emission and subsequent deposition of heavy metals including mercury (Hg) and lead (Pb) present human health and environmental concerns. Although it is known that local and regional sources of these metals contribute to deposition in the Great Lakes region, it is difficult to trace emissions from point sources to impacted sites. Recent studies suggest that metal isotope ratios may be useful for distinguishing between and tracing source emissions. We measured Pb, strontium (Sr), and Hg isotope ratios in daily precipitation samples that were collected at seven sites across the Great Lakes region between 2003 and 2007. Lead isotope ratios (207Pb/206Pb = 0.8062 to 0.8554) suggest that Pb deposition was influenced by coal combustion and processing of Mississippi Valley-Type Pb ore deposits. Regional differences in Sr isotope ratios (87Sr/86Sr = 0.70859 to 0.71155) are likely related to coal fly ash and soil dust. Mercury isotope ratios (δ202Hg = − 1.13 to 0.13‰) also varied among the sites, likely due to regional differences in coal isotopic composition, and fractionation occurring within industrial facilities and in the atmosphere. These data represent the first combined characterization of Pb, Sr, and Hg isotope ratios in precipitation collected across the Great Lakes region. We demonstrate the utility of multiple metal isotope ratios in parallel with traditional trace element multivariate statistical modeling to enable more complete pollution source attribution.

Development of the Athabasca Oil Sands Region in northeastern Alberta, Canada has contributed polycyclic aromatic hydrocarbons (PAHs) and polycyclic aromatic compounds (PACs), which include alkyl PAHs and dibenzothiophenes, to the regional environment. A new analytical method was developed for quantification of PAHs and PACs in the epiphytic lichen bioindicator species Hypogymnia physodes for use in the development of receptor models for attribution of PAH and PAC concentrations to anthropogenic and natural emission sources. Milled lichens were extracted with cyclohexane, and extracts were cleaned on silica gel using automated solid phase extraction techniques. Quantitative analysis was performed by gas chromatography with selected ion monitoring (GC-SIM-MS) for PAHs, and by GC with time-of-flight mass spectrometry (GC-TOF-MS) for PACs. PACs were quantitated in groups using representative reference compounds as calibration standards. Analytical detection limits were ≤2.5 ng g−1 for all individual compounds. Precision as measured by laboratory duplicates was variable; for individual analytes above 5 ng g−1 the mean absolute difference between duplicates was typically

A new source-type identification method, Reduction and Species Clustering Using Episodes (ReSCUE), was developed to exploit the temporal synchronicity typically observed between ambient species in high time resolution fine particulate matter (PM2.5) data to form clusters that vary together. High time-resolution (30 min) PM2.5 sampling was conducted for a month during the summer of 2006 in Steubenville, OH, an EPA designated nonattainment area for the U.S. National Ambient Air Quality Standards (NAAQS). When the data were evaluated, the species clusters from ReSCUE matched extremely well with the source types identified by EPA Unmix demonstrating that ReSCUE is a valuable tool in identifying source types. Results from EPA Unmix show that contributions to PM2.5 are mostly from iron/steel manufacturing (36% ± 9%), crustal matter (33% ± 11%), and coal combustion (11% ± 19%). More importantly, ReSCUE was useful in (i) providing objective data driven guidance for the number of source factors and key fitting species for EPA Unmix, and (ii) detecting tenuous associations between some species and source types in the results derived by EPA Unmix.

Prescribed pasture burning plays a critical role in ecosystem maintenance in tallgrass prairie ecosystems and may contribute to agricultural productivity but can also have negative impacts on air quality. Volatile organic compound (VOC) concentrations were measured immediately downwind of prescribed tallgrass prairie fires in the Flint Hills region of Kansas, United States. The VOC mixture is dominated by alkenes and oxygenated VOCs, which are highly reactive and can drive photochemical production of ozone downwind of the fires. The computed emission factors are comparable to those previous measured from pasture maintenance fires in Brazil. In addition to the emission of large amounts of particulate matter, hazardous air pollutants such as benzene and acrolein are emitted in significant amounts and could contribute to adverse health effects in exposed populations.

A technique that couples lead (Pb) isotopes and multi-element concentrations with meteorological analysis was used to assess source contributions to precipitation samples at the Bondville, Illinois USA National Trends Network (NTN) site. Precipitation samples collected over a 16month period (July 1994-October 1995) at Bondville were parsed into six unique meteorological flow regimes using a minimum variance clustering technique on back trajectory endpoints. Pb isotope ratios and multi-element concentrations were measured using high resolution inductively coupled plasma-sector field mass spectrometry (ICP-SFMS) on the archived precipitation samples. Bondville is located in central Illinois, ~250km downwind from smelters in southeast Missouri. The Mississippi Valley Type ore deposits in Missouri provided a unique multi-element and Pb isotope fingerprint for smelter emissions which could be contrasted to industrial emissions from the Chicago and Indianapolis urban areas (~125km north and east, of Bondville respectively) and regional emissions from electric utility facilities. Differences in Pb isotopes and element concentrations in precipitation corresponded to flow regime. Industrial sources from urban areas, and thorogenic Pb from coal use, could be differentiated from smelter emissions from Missouri by coupling Pb isotopes with variations in element ratios and relative mass factors. Using a three endmember mixing model based on Pb isotope ratio differences, industrial processes in urban airsheds contributed 56±19%, smelters in southeast Missouri 26±13%, and coal combustion 18±7%, of the Pb in precipitation collected in Bondville in the mid-1990s.

An ambient air particulate matter sampling study was conducted at the Wood Buffalo Environmental Association (WBEA) AMS-1 Fort McKay monitoring station in the Athabasca Oil Sand Region (AOSR) in Alberta, Canada from February 2010 to July 2011. Daily 24h integrated fine (PM2.5) and coarse (PM10-2.5) particulate matter was collected using a sequential dichotomous sampler. Over the duration of the study, 392 valid daily dichotomous PM2.5 and PM10-2.5 sample pairs were collected with concentrations of 6.8±12.9μgm-3 (mean±standard deviation) and 6.9±5.9μgm-3, respectively. A subset of 100 filter pairs was selected for element analysis by energy dispersive X-ray fluorescence and dynamic reaction cell inductively coupled plasma mass spectrometry. Application of the U.S. EPA positive matrix factorization (PMF) receptor model to the study data matrix resolved five PM2.5 sources explaining 96% of the mass including oil sands upgrading (32%), fugitive dust (26%), biomass combustion (25%), long-range Asian transport lead source (9%), and winter road salt (4%). An analysis of historical PM2.5 data at this site shows that the impact of smoke from wildland fires was particularly high during the summer of 2011. PMF resolved six PM10-2.5 sources explaining 99% of the mass including fugitive haul road dust (40%), fugitive oil sand (27%), a mixed source fugitive dust (16%), biomass combustion (12%), mobile source (3%), and a local copper factor (1%). Results support the conclusion of a previous epiphytic lichen biomonitor study that near-field atmospheric deposition in the AOSR is dominated by coarse fraction fugitive dust from bitumen mining and upgrading operations, and suggest that fugitive dust abatement strategies targeting the three major sources of PM10-2.5 (e.g., oil sand mining, haul roads, bulk material stockpiles) would significantly reduce near-field atmospheric deposition gradients in the AOSR and reduce ambient PM concentrations in the Fort McKay community.

This paper describes the development of a new artificial turf surrogate surface (ATSS) sampler for use in the measurement of mercury (Hg) dry deposition. In contrast to many existing surrogate surface designs, the ATSS utilizes a three-dimensional deposition surface that may more closely mimic the physical structure of many natural surfaces than traditional flat surrogate surface designs (water, filter, greased Mylar film). The ATSS has been designed to overcome several complicating factors that can impact the integrity of samples with other direct measurement approaches by providing a passive system which can be deployed for both short and extended periods of time (days to weeks), and is not contaminated by precipitation and/or invalidated by strong winds. Performance characteristics including collocated precision, in-field procedural and laboratory blanks were evaluated. The results of these performance evaluations included a mean collocated precision of 9%, low blanks (0.8 ng), high extraction efficiency (97%–103%), and a quantitative matrix spike recovery (100%).

A field study was conducted to evaluate the performance of a Semi-continuous Elements in Aerosol Sampler-III (SEAS-III), designed to collect ambient PM2.5 aerosol samples at a time resolution of 30 min for elemental concentration measurements. Two identical but modified SEAS-III samplers were operated for four continuous weeks in Dearborn, MI, during July–August 2007. A total of 2308 samples were collected from the two samplers. Sampling completeness from the primary and duplicate samplers was 90% and 84%, respectively. All of the collected samples were analyzed for dilute acid-extractable trace metal concentrations using HR-ICPMS. A total of 878 collection time-matched sample pairs were available to evaluate whole-system uncertainty from collocated concentration measurements. The collocated precision for the 27 studied elements (Al, As, Ba, Ca, Cd, Ce, Cs, Cu, Fe, Ge, K, La, Mg, Mn, Mo, Na, P, Pb, Rb, S, Sb, Se, Sn, Sr, Ti, V, and Zn) varied between 9% and 40%. Twenty elements showed precision better than 25%. Uncertainty estimates from propagation of errors compared well with the whole-system uncertainty values for all minor aerosol elements studied. SEAS-III measurements of As, Cd, Ge, K, La, Mn, Mo, Na, Rb, Se, Sb, Sr, Ti, V, and Zn correlated well (r > 0.8) with a FRM equivalent PM2.5 integrated filter sampling method. Based on these measurements, collection efficiency of SEAS-III was estimated to be 87 ± 16%. Solubility of particles in the collection medium (water) was identified as a possible reason for low recovery of Al, Fe, Pb, Sb, and Sn.

Atmospheric mercury (Hg) species were measured in Guiyang City, the capital of Guizhou province, southwestern China at the Guiyang Monitoring Station Agency (GMSA) from September to November 2008 and at the Institute of Geochemistry, Chinese Academy of Sciences (IGCAS) during February, May, and July, 2009. Monitoring results found elevated concentrations of all three Hg species in ambient air in Guiyang. Large temporal and spatial variation patterns in the resulting data were also obtained. The overall average TGM concentrations at the GMSA and IGCAS sampling sites were 7.4 ± 4.8 ng m− 3 and 6.2 ± 5.1 ng m− 3, respectively. The average Hg(p) and RGM concentrations at GMSA were 1330 pg m− 3 and 24 pg m− 3, and at IGCAS were 250 pg m− 3 and 19 pg m− 3, respectively. It is hypothesized that local anthropogenic sources and the seasonal variability result in the high degree of spatial and temporal variability.

Intensive ambient air sampling was conducted in Tampa, FL, during October and November of 2002. Fine particulate matter (PM(2.5)) was collected at 30 min resolution using the Semicontinuous Elements in Aerosol Sampler II (SEAS-II) and analyzed off-line for up to 45 trace elements by high-resolution ICPMS (HR-ICPMS). Divalent reactive gaseous mercury and particulate bound mercury were also measured semicontinuously (2 h). Application of the United States Environmental Protection Agency's (EPA) Unmix receptor model on the 30 min resolution trace metals data set identified eight possible sources: residual oil combustion, lead recycling, coal combustion, a Cd-rich source, biomass burning, marine aerosol, general industrial, and coarse dust contamination. The source contribution estimates from EPA Unmix were then run in a nonparametric wind regression (NWR) model, which convincingly identified plausible source origins. When the 30 min ambient concentrations of trace elements were time integrated (2 h) and combined with speciated mercury concentrations, the model identified only four sources, some of which appeared to be merged source profiles that were identified as separate sources by using the 30 min resolution data. This work demonstrates that source signatures that can be captured at 30 min resolution may be lost when sampling for longer durations.

Although the toxicity of oil combustion emissions is a significant public health concern, few studies characterize the emissions from plant-scale utility boilers firing residual oil. This study remedies that deficiency by diluting, sampling, and monitoring stack emissions from a 432 gigajoules (GJ) front-fired fossil fuel steam generator burning residual oil. Over a 3-day test period, continuous CO2, SO2, and NOx emissions monitoring confirms a steady fuel feed rate, high combustion efficiency (3.4 kg of CO2/kg of fuel oil burned), and evidence of a nocturnal soot-blowing event. The utility boiler emits fine aerosol (PM2.5) at a rate of 53 ± 2 μg/kJ (2 g/kg of oil burned). Vesicular coarse particles composed of C and S and spherical Al silicates with V and Ni inclusions are identified in a cyclone rinse using scanning electron microscopy and backscatter analysis. Ion chromatography results establish that the fine aerosol is predominantly sulfate (44% ± 0.2%, w/w) which is likely coordinated to transition ...

Extensive exploration of event precipitation data in the Ohio River Valley indicates that coal combustion emissions play an important role in mercury (Hg) wet deposition. During July-September 2006, an intensive study was undertaken to discern the degree of local source influence. Source-receptor relationships were explored by establishing a set of wet deposition sites in and around Steubenville, Ohio. For the three month period of study, volume-weighted mean Hg concentrations observed at the eight sites ranged from 10.2 to 223 ng L(-1), but this range increased drastically on an event basis with a maximum concentration of 89.4 ng L(-1) and a minimum concentration of 4.1 ng L(-1). A subset of events was explored in depth, andthe degree of variability in Hg concentrations between sites was linked to the degree of local source enhancement. Samples collected at sites less than 1 km from coal-fired utility stacks (near-field) exhibited up to 72% enhancement in Hg concentrations over regionally representative samples on an event basis. Air mass transport and precipitating cell histories were traced in order to evaluate relationships between local point sources and receptor sites. It was found that the interaction of several dynamic atmospheric parameters combined to favor local Hg concentration enhancement over the more regional contribution. When significant meteorological factors (wind speed at time of maximum rain rate, wind speed 24 h prior to precipitation, mixing height, and observed ceiling) were explored, it was estimated that during summertime precipitation, 42% of Hg concentration in near-field samples could be attributed to the adjacent coal-fired utility source.

Mechanisms of particulate matter (PM)-induced cardiotoxicity are not fully understood. Direct translocation of PM-associated metals, including zinc, may mediate this effect. We hypothesized that following a single intratracheal instillation (IT), zinc directly translocates outside of the lungs, reaching the heart. To test this, we used high resolution magnetic sector field inductively coupled plasma mass spectrometry to measure levels of five stable isotopes of zinc ((64)Zn, (66)Zn, (67)Zn, (68)Zn, (70)Zn), and copper in lungs, plasma, heart, liver, spleen, and kidney of male Wistar Kyoto rats (13 weeks old, 250-300 g), 1, 4, 24, and 48 h following a single IT or oral gavage of saline or 0.7 micromol/rat (70)Zn, using a solution enriched with 76.6% (70)Zn. Natural abundance of (70)Zn is 0.62%, making it an easily detectable tracer following exposure. In IT rats, lung (70)Zn was highest 1 h post IT and declined by 48 h. Liver endogenous zinc was increased 24 and 48 h post IT. (70)Zn was detected in all extrapulmonary organs, with levels higher following IT than following gavage. Heart (70)Zn was highest 48 h post IT. Liver, spleen and kidney (70)Zn peaked 4 h following gavage, and 24 h following IT. (70)Zn IT exposure elicited changes in copper homeostasis in all tissues. IT instilled (70)Zn translocates from lungs into systemic circulation. Route of exposure affects (70)Zn translocation kinetics. Our data suggests that following pulmonary exposure, zinc accumulation and subsequent changes in normal metal homeostasis in the heart and other organs could induce cardiovascular injury.

During the fall of 1998, the US Environmental Protection Agency and the Florida Department of Environmental Protection sponsored a 7-day study at the Ft. McHenry tunnel in Baltimore, MD with the objective of obtaining PM 2.5 vehicle source profiles for use in atmospheric mercury source apportionment studies. PM 2.5 emission profiles from gasoline and diesel powered vehicles were developed from analysis of trace elements, polycyclic aromatic hydrocarbons (PAH), and condensed aliphatic hydrocarbons. PM 2.5 samples were collected using commercially available sampling systems and were extracted and analyzed using conventional well-established methods. Both inorganic and organic profiles were sufficiently unique to mathematically discriminate the contributions from each source type using a chemical mass balance source apportionment approach. However, only the organic source profiles provided unique PAH tracers (e.g., fluoranthene, pyrene, and chrysene) for diesel combustion that could be used to identify source contributions generated using multivariate statistical receptor modeling approaches. In addition, the study found significant emission of gaseous elemental mercury (Hg 0 ), divalent reactive gaseous mercury (RGM), and particulate mercury (Hg(p)) from gasoline but not from diesel powered motor vehicles. Fuel analysis supported the tunnel measurement results showing that total mercury content in all grades of gasoline (284±108 ng L −1 ) was substantially higher than total mercury content in diesel fuel (62±37 ng L −1 ) collected contemporaneously at local Baltimore retailers.