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Huang J.,University of North Carolina at Chapel Hill | Miller M.B.,University of Nevada, Reno | Edgerton E.,Atmospheric Research and Analysis Inc. | Gustin M.S.,University of Nevada, Reno
Atmospheric Chemistry and Physics | Year: 2017

The highest mercury (Hg) wet deposition in the United States of America (USA) occurs along the Gulf of Mexico, and in the southern and central Mississippi River Valley. Gaseous oxidized Hg (GOM) is thought to be a major contributor due to high water solubility and reactivity. Therefore, it is critical to understand concentrations, potential for wet and dry deposition, and GOM compounds present in the air. Concentrations and dry-deposition fluxes of GOM were measured and calculated for Naval Air Station Pensacola Outlying Landing Field (OLF) in Florida using data collected by a Tekran® 2537/1130/1135, the University of Nevada Reno Reactive Mercury Active System (UNRRMAS) with cation exchange and nylon membranes, and the Aerohead samplers that use cation-exchange membranes to determine dry deposition. Relationships with Tekran®-derived data must be interpreted with caution, since the GOM concentrations measured are biased low depending on the chemical compounds in air and interferences with water vapor and ozone. Criteria air pollutants were concurrently measured. This allowed for comparison and better understanding of GOM. In addition to other methods previously applied at OLF, use of the UNRRMAS provided a platform for determination of the chemical compounds of GOM in the air. Results from nylon membranes with thermal desorption analyses indicated seven GOM compounds in this area, including HgBr2, HgCl2, HgO, Hg-nitrogen and sulfur compounds, and two unknown compounds. This indicates that the site is influenced by different gaseous phase reactions and sources. Using back-trajectory analysis during a high-GOM event related to high CO, but average SO2, indicated air parcels moved from the free troposphere and across Arkansas, Mississippi, and Alabama at low elevation (< 300m). This event was initially characterized by HgBr2, followed by a mixture of GOM compounds. Overall, GOM chemistry indicates oxidation reactions with local mobile source pollutants and long-range transport. In order to develop methods to measure GOM concentrations and chemistry, and model dry-deposition processes, the actual GOM compounds need to be known, as well as their corresponding physicochemical properties, such as Henry's Law constants.

Zhang X.,Georgia Institute of Technology | Liu Z.,Georgia Institute of Technology | Liu Z.,Sandia National Laboratories | Hecobian A.,Georgia Institute of Technology | And 5 more authors.
Atmospheric Chemistry and Physics | Year: 2012

Secondary organic aerosol (SOA) in the southeastern US is investigated by analyzing the spatial-temporal distribution of water-soluble organic carbon (WSOC) and other PM 2.5 components from 900 archived 24-h Teflon filters collected at 15 urban or rural EPA Federal Reference Method (FRM) network sites throughout 2007. Online measurements of WSOC at an urban/rural-paired site in Georgia in the summer of 2008 are contrasted to the filter data. Based on FRM filters, excluding biomass-burning events (levoglucosan < 50 ng m -3), WSOC and sulfate were highly correlated with PM 2.5 mass (r 2̃0.7). Both components comprised a large mass fraction of PM 2.5 (13% and 31%, respectively, or ̃25% and 50% for WSOM and ammonium sulfate). Sulfate and WSOC both tracked ambient temperature throughout the year, suggesting the temperature effects were mainly linked to faster photochemistry and/or synoptic meteorology and less due to enhanced biogenic hydrocarbon emissions. FRM WSOC, and to a lesser extent sulfate, were spatially homogeneous throughout the region, yet WSOC was moderately enhanced (27%) in locations of greater predicted isoprene emissions in summer. A Positive Matrix Factorization (PMF) analysis identified two major source types for the summer WSOC; 22% of the WSOC were associated with ammonium sulfate, and 56% of the WSOC were associated with brown carbon and oxalate. A small urban excess of FRM WSOC (10%) was observed in the summer of 2007, however, comparisons of online WSOC measurements at one urban/rural pair (Atlanta/Yorkville) in August 2008 showed substantially greater difference in WSOC (31%) relative to the FRM data, suggesting a low bias for urban filters. The measured Atlanta urban excess, combined with the estimated boundary layer heights, gave an estimated Atlanta daily WSOC production rate in August of 0.55 mgC m 2 h -1 between mid-morning and mid-afternoon. This study characterizes the regional nature of fine particles in the southeastern US, confirming the importance of SOA and the roles of both biogenic and anthropogenic emissions. © Author(s) 2012.

Blanchard C.L.,Envair | Hidy G.M.,Envair Aerochem | Tanenbaum S.,Envair | Edgerton E.S.,Atmospheric Research and Analysis Inc.
Atmospheric Environment | Year: 2011

Carbonaceous compounds constitute a major fraction of the fine particle mass at locations throughout North America; much of the condensed-phase organic carbon (OC) is produced in the atmosphere from NMOC reactions as " secondary" OC (SOC). Ten years of particulate carbon and speciated non-methane organic compound (NMOC) data combined with other measurements from Southeastern Aerosol Research and Characterization (SEARCH) and other sites provide insight into the association between elemental carbon (EC), OC and NMOCs. Data are analyzed to characterize the OC and SOC contrasts between urban Atlanta, Georgia, and nearby non-urban conditions in the Southeast. Analysis of the monitoring record indicates that the mean Atlanta urban excess of total carbon (TC) is 2.1-2.8μgm -3. The OC/EC ratio of the Atlanta urban excess is in the range 1.3 to 1.8, consistent with OC/EC ratios observed in motor vehicle emissions and a fossil carbon source of urban excess TC. Carbon isotope analysis of a subset of particle samples demonstrates that the urban excess is mainly fossil in origin, even though the majority of the TC is modern at both urban and non-urban sites. Temperature-dependent partitioning of OC between gas and condensed phases cannot explain the observed diurnal and seasonal variations of OC/CO, EC/CO, and OC/EC ratios. Alternatively, a hypothesis involving vertical mixing of OC-enriched air from aloft is supported by the seasonal and diurnal OC, isopentane, aromatic and isoprene observations at the ground. A statistical model is applied to indicate the relative significance of aerometric factors affecting OC and EC concentrations, including meteorological and pollutant associations. The model results demonstrate strong linkages between fine particle carbon and pollutant indicators of source emissions compared with meteorological factors; the model results show weaker dependence of OC on meteorological factors than is the case for ozone (O 3) concentrations. © 2010 Elsevier Ltd.

Blanchard C.L.,Envair | Hidy G.M.,AeroChem Research Laboratories | Shaw S.,EPRI | Baumann K.,Atmospheric Research and Analysis Inc. | Edgerton E.S.,Atmospheric Research and Analysis Inc.
Atmospheric Chemistry and Physics | Year: 2016

Long-term (1999 to 2013) data from the Southeastern Aerosol Research and Characterization (SEARCH) network are used to show that anthropogenic emission reductions led to important decreases in fine-particle organic aerosol (OA) concentrations in the southeastern US On average, 45 % (range 25 to 63 %) of the 1999 to 2013 mean organic carbon (OC) concentrations are attributed to combustion processes, including fossil fuel use and biomass burning, through associations of measured OC with combustion products such as elemental carbon (EC), carbon monoxide (CO), and nitrogen oxides (NOx). The 2013 mean combustion-derived OC concentrations were 0.5 to 1.4 μg-3 at the five sites operating in that year. Mean annual combustion-derived OC concentrations declined from 3.8 ± 0.2 μg-3 (68 % of total OC) to 1.4 ± 0.1 μg-3 (60 % of total OC) between 1999 and 2013 at the urban Atlanta, Georgia, site (JST) and from 2.9 ± 0.4 μg-3 (39 % of total OC) to 0.7 ± 0.1 μg-3 (30 % of total OC) between 2001 and 2013 at the urban Birmingham, Alabama (BHM), site. The urban OC declines coincide with reductions of motor vehicle emissions between 2006 and 2010, which may have decreased mean OC concentrations at the urban SEARCH sites by > 2 μg-3. BHM additionally exhibits a decline in OC associated with SO2 from 0.4 ± 0.04 μg-3 in 2001 to 0.2 ± 0.03 μg-3 in 2013, interpreted as the result of reduced emissions from industrial sources within the city. Analyses using non-soil potassium as a biomass burning tracer indicate that biomass burning OC occurs throughout the year at all sites. All eight SEARCH sites show an association of OC with sulfate (SO4) ranging from 0.3 to 1.0 μg-3 on average, representing ∼25 % of the 1999 to 2013 mean OC concentrations. Because the mass of OC identified with SO4 averages 20 to 30 % of the SO4 concentrations, the mean SO4-associated OC declined by ∼0.5 to 1 μg-3 as SO4 concentrations decreased throughout the SEARCH region. The 2013 mean SO4 concentrations of 1.7 to 2.0 μg-3 imply that future decreases in mean SO4-associated OC concentrations would not exceed ∼0.3 to 0.5 μg-3. Seasonal OC concentrations, largely identified with ozone (O3), vary from 0.3 to 1.4 μg-3 (∼20 % of the total OC concentrations). © Author(s) 2016.

Lin Y.-H.,University of North Carolina at Chapel Hill | Knipping E.M.,EPRI | Edgerton E.S.,Atmospheric Research and Analysis Inc. | Shaw S.L.,EPRI | Surratt J.D.,University of North Carolina at Chapel Hill
Atmospheric Chemistry and Physics | Year: 2013

Filter-based PM2.5 samples were chemically analyzed to investigate secondary organic aerosol (SOA) formation from isoprene in a rural atmosphere of the southeastern US influenced by both anthropogenic sulfur dioxide (SO2) and ammonia (NH3) emissions. Daytime PM2.5 samples were collected during summer 2010 using conditional sampling approaches based on pre-defined high and low SO2 or NH3 thresholds. Known molecular-level tracers for isoprene SOA formation, including 2-methylglyceric acid, 3-methyltetrahydrofuran-3,4-diols, 2-methyltetrols, C5-alkene triols, dimers, and organosulfate derivatives, were identified and quantified by gas chromatography coupled to electron ionization mass spectrometry (GC/EI-MS) and ultra performance liquid chromatography coupled to electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-Q-TOFMS). Mass concentrations of six isoprene low-NOx SOA tracers contributed to 12-19% of total organic matter (OM) in PM2.5 samples collected during the sampling period, indicating the importance of the hydroxyl radical (OH)-initiated oxidation (so-called photooxidation) of isoprene under low-NOx conditions that lead to SOA formation through reactive uptake of gaseous isoprene epoxydiols (IEPOX) in this region. The contribution of the IEPOX-derived SOA tracers to total organic matter was enhanced by 1.4% (p Combining double low line 0.012) under high-SO2 sampling scenarios, although only weak associations between aerosol acidity and mass of IEPOX SOA tracers were observed. This suggests that IEPOX-derived SOA formation might be modulated by other factors simultaneously, rather than only aerosol acidity. No clear associations between isoprene SOA formation and high or low NH3 conditional samples were found. Positive correlations between sulfate aerosol loadings and IEPOX-derived SOA tracers for samples collected under all conditions indicates that sulfate aerosol could be a surrogate for surface accommodation in the uptake of IEPOX onto preexisting aerosols. © 2013 Author(s).

Saylor R.D.,Atmospheric Research and Analysis Inc. | Edgerton E.S.,Atmospheric Research and Analysis Inc. | Hartsell B.E.,Atmospheric Research and Analysis Inc. | Baumann K.,Atmospheric Research and Analysis Inc. | Hansen D.A.,EPRI
Atmospheric Environment | Year: 2010

Continuous ammonia (NH 3) measurements with a temporal resolution of 5min were implemented at selected SEARCH sites in the southeastern U. S. during 2007. The SEARCH continuous NH 3 instrument uses a citric acid denuder difference technique employing a dual-channel nitric oxide-ozone chemiluminescence analyzer. Data from two SEARCH sites are presented, Jefferson Street, Atlanta (JST) (urban), and Yorkville, Georgia (YRK) (rural), for the period July-December, 2007. Highest NH x (total ammonia=gaseous NH 3+PM 2.5 NH 4 +) values were observed in August and September at both JST and YRK. Highest NH 3 values occurred in August and September at JST, but in August through October at YRK. Lowest NH 3 and NH x values occurred in December at both sites. YRK is significantly impacted by nearby poultry sources, routinely experiencing hourly average NH 3 mixing ratios above 20ppbv. Wind sector analysis clearly implicates the nearby poultry operations as the source of the high NH 3 values. Weekday versus weekend differences in composite hourly mean diurnal profiles of NH 3 at JST indicate that mobile sources have a measurable but relatively small impact on NH 3 observed at that site, and little or no impact on NH 3 observed at YRK. A distinctive composite mean hourly diurnal variation was observed at both JST and YRK, exhibiting maxima in the morning and evening with a broad minimum during midday. Analysis of observed NH 3 diurnal variations from the literature suggests a hypothesized mechanism for the observed behavior based on interaction of local emissions and dry deposition with the formation and collapse of the dynamically mixed atmospheric boundary layer during the day and shallow nocturnal layer at night. Simple mixed layer concentration box model simulations confirm the plausibility of the suggested mechanism. © 2010.

Nair U.S.,University of Alabama in Huntsville | Wu Y.,University of Alabama in Huntsville | Walters J.,Southern Company | Jansen J.,Southern Company | Edgerton E.S.,Atmospheric Research and Analysis Inc.
Atmospheric Environment | Year: 2012

Observations for the 2005-2008 time period from three Southeastern Aerosol Research and Characterization (SEARCH) air quality monitoring sites are examined for diurnal and seasonal variation in concentrations of gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM), and particle bound mercury (HgP-<-2.5-μm). The sites are located at 1) a suburban-coastal location near Pensacola, Florida (OLF), 2) an urban location in Birmingham, Alabama (BHM), and 3) a rural location west-northwest of Atlanta, Georgia (YRK). Average concentrations of GEM at both OLF and YRK are 1.35-ng-m -3, whereas at BHM it is 2.12-ng-m -3. All sites show increase in GEM concentration during the morning hours (0.023 and 0.011-ng-m -3hr -1 at OLF and YRK between 6 and 10-AM, 0.038-ng-m -3hr -1 at BHM between 5 and 10-AM) due to downward mixing of higher concentrations from the residual layer, after which OLF and YRK show negligible variation compared to decrease in concentration at BHM (2.3-1.9-ng-m -3 from 10-AM to 6-PM). All sites show seasonal variation of GEM with enhanced concentrations found in winter and spring. Average GOM concentrations are 4.26, 8.55, and 78.2-pg-m -3 at OLF, YRK, and BHM, respectively. Seasonally, GOM values are enhanced during fall and spring. All sites undergo a sinusoidal daytime variation of GOM that peaks in the afternoon, while BHM additionally exhibits an early morning enhancement likely caused by vertical mixing. The average HgP concentrations at OLF, YRK, and BHM are 2.49, 4.43, and 39.5-pg-m -3, respectively. At OLF, vertical mixing causes an early morning increase in HgP concentration followed by an afternoon decline during all seasons. A daytime increase in HgP is found at YRK for all seasons, while at BHM, nocturnal accumulation followed by a daytime decline is also found for most seasons except winter. In winter, concentrations increase due to vertical mixing in the morning and then decline as the boundary layer grows. Boundary layer processes appear to play an important role in the seasonal and diurnal variation of Hg species and further investigation utilizing a boundary layer process model is warranted. © 2011 Elsevier Ltd.

Liu J.,Georgia Institute of Technology | Bergin M.,Georgia Institute of Technology | Guo H.,Georgia Institute of Technology | King L.,Georgia Institute of Technology | And 3 more authors.
Atmospheric Chemistry and Physics | Year: 2013

Light absorbing organic carbon, often called brown carbon, has the potential to significantly contribute to the visible light-absorption budget, particularly at shorter wavelengths. Currently, the relative contributions of particulate brown carbon to light absorption, as well as the sources of brown carbon, are poorly understood. With this in mind size-resolved direct measurements of brown carbon were made at both urban (Atlanta), and rural (Yorkville) sites in Georgia. Measurements in Atlanta were made at both a representative urban site and a road-side site adjacent to a main highway. Fine particle absorption was measured with a multi-angle absorption photometer (MAAP) and seven-wavelength Aethalometer, and brown carbon absorption was estimated based on Mie calculations using direct size-resolved measurements of chromophores in solvents. Size-resolved samples were collected using a cascade impactor and analyzed for water-soluble organic carbon (WSOC), organic and elemental carbon (OC and EC), and solution light-absorption spectra of water and methanol extracts. Methanol extracts were more light-absorbing than water extracts for all size ranges and wavelengths. Absorption refractive indices of the organic extracts were calculated from solution measurements for a range of wavelengths and used with Mie theory to predict the light absorption by fine particles comprised of these components, under the assumption that brown carbon and other aerosol components were externally mixed. For all three sites, chromophores were predominately in the accumulation mode with an aerodynamic mean diameter of 0.5 μm, an optically effective size range resulting in predicted particle light absorption being a factor of 2 higher than bulk solution absorption. Mie-predicted brown carbon absorption at 350 nm contributed a significant fraction (20 to 40%) relative to total light absorption, with the highest contributions at the rural site where organic to elemental carbon ratios were highest. Brown carbon absorption, however, was highest by the roadside site due to vehicle emissions. The direct size-resolved measurement of brown carbon in solution definitively shows that it is present and optically important in the near-UV range in both a rural and urban environment during the summer when biomass burning emissions are low. These results allow estimates of brown carbon aerosol absorption from direct measurements of chromophores in aerosol extracts. © Author(s) 2013.

Hecobian A.,Georgia Institute of Technology | Zhang X.,Georgia Institute of Technology | Zheng M.,Georgia Institute of Technology | Frank N.,U.S. Environmental Protection Agency | And 2 more authors.
Atmospheric Chemistry and Physics | Year: 2010

Light absorption of fine particle (PM2.5) aqueous extracts between wavelengths of 200 and 800 nm were investigated from two data sets: 24-h Federal Reference Method (FRM) filter extracts from 15 Southeastern US monitoring sites over the year of 2007 (900 filters), and online measurements from a Particle-Into-Liquid Sampler deployed from July to mid-August 2009 in Atlanta, Georgia. Three main sources of soluble chromophores were identified: biomass burning, mobile source emissions, and compounds linked to secondary organic aerosol (SOA) formation. Absorption spectra of aerosol solutions from filter extracts were similar for different sources. Angstrom exponents were ∼7±1 for biomass burning and non-biomass burning-impacted 24-h filter samples (delineated by a levoglucosan concentration of 50 ng mg-3) at both rural and urban sites. The absorption coefficient from measurements averaged between wavelength 360 and 370 nm (Abs365, in units mg -1) was used as a measure of overall brown carbon light absorption. Biomass-burning-impacted samples were highest during winter months and Abs 365 was correlated with levoglucosan at all sites. During periods of little biomass burning in summer, light absorbing compounds were still ubiquitous and correlated with fine particle Water-Soluble Organic Carbon (WSOC), but comprised a much smaller fraction of the WSOC, where Abs 365/WSOC (i.e., mass absorption efficiency) was typically ∼3 times higher in biomass burning-impacted samples. Factor analysis attributed 50% of the yearly average Abs365 to biomass burning sources. Brown carbon from primary urban emissions (mobile sources) was also observed and accounted for ∼10% of the regional yearly average Abs365. Summertime diurnal profiles of Abs365 and WSOC showed that morning to midday increases in WSOC from photochemical production were associated with a decrease in Abs365/WSOC. After noon, this ratio substantially increased, indicating that either some fraction of the non-light absorbing fresh SOA was rapidly (within hours) converted to chromophores heterogeneously, or that SOA from gas-particle partitioning later in the day was more light-absorbing. Factor analysis on the 24-h integrated filter data associated ∼20 to 30% of Abs365 over 2007 with a secondary source that was highest in summer and also the main source for oxalate, suggesting that aqueous phase reactions may account for the light-absorbing fraction of WSOC observed throughout the Southeastern US in summer. © 2010 Author(s).

McClure C.D.,University of Washington | Jaffe D.A.,University of Washington | Edgerton E.S.,Atmospheric Research and Analysis Inc.
Environmental Science and Technology | Year: 2014

During the summer of 2013, we examined the performance of KCl-coated denuders for measuring gaseous oxidized mercury (GOM) by calibrating with a known source of GOM (i.e., HgBr2) at the North Birmingham SouthEastern Aerosol Research and Characterization (SEARCH) site. We found that KCl-coated denuders have near 95% collection efficiency for HgBr2 in zero air (i.e., air scrubbed of mercury and ozone). However, in ambient air, the efficiency of KCl-coated denuders in capturing HgBr2 dropped to 20-54%. We also found that absolute humidity and ozone each demonstrate a significant inverse correlation with HgBr2 recovery in ambient air. Subsequent laboratory tests with HgBr2 and the KCl-coated denuder show that ozone and absolute humidity cause the release of gaseous elemental Hg from the denuder and thus appear to explain the low recovery in ambient air. Based on these findings, we infer that the KCl denuder method underestimates atmospheric GOM concentrations and a calibration system is needed to accurately measure GOM. The system described in this paper for HgBr2 could be implemented with existing mercury speciation instrumentation and this would improve our knowledge of the response to one potentially important GOM compound. © 2014 American Chemical Society.

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