Transport patterns and potential sources of total gaseous mercury measured in Canadian high Arctic in 1995

Trajectory cluster analysis and the potential source contribution function (PSCF) model have been used to investigate the source–receptor relationship for the total gaseous mercury (TGM) measured in the Canadian High Arctic (Alert, 82.5°N, 62.3°W) during 1995. Cluster analysis of 10-day back-trajectories in 1995 shows that the synoptic flows arriving at Alert are dominated by the air masses from the north. Long-range transport only occurs in the cold seasons while summertime flows tend to circulate in the Arctic Ocean. The potential source regions identified by the PSCF modeling include Eurasia and populated areas in the North America and Europe. Based on the modeling results, it is suggested that the elevated TGM concentrations found in the Arctic summer should be of geological origins, mainly from the evasion of volatile Hg⁰ from earth's surfaces. In the autumn and winter, mercury is transported to the receptor site from remote anthropogenic sources. The preferred sources of TGM in the spring cannot be clearly determined due to the Arctic springtime mercury depletion, which significantly reduces the number of trajectories contributing to PSCF values. Using TGM data of higher temporal resolution improves the sensitivity of the PSCF modeling results.     

Source apportionment of fine particles utilizing partially speciated carbonaceous aerosol data at two rural locations in New York State

A source apportionment study was conducted at two rural locations, Potsdam and Stockton, to assess the in-state/out-of-state sources of PM_2.5 and Hg in New York State. At both locations, samples were collected between November 2002 and August 2005 and analyzed for fine PM mass and its chemical constituents. The measured chemical constituents included elements, cations, anions, organic and elemental carbon (OC and EC), black carbon (BC), and water-soluble short-chain (WSSC) organic acids. Positive matrix factorization (PMF) was applied to the measured concentrations and eight and seven factors were resolved at Potsdam and Stockton, respectively. Four factors were resolved in common between the two locations including secondary sulfate, secondary nitrate, secondary OC, and a crustal factor. The factor profiles of mixed industrial and motor vehicle factors resolved at Potsdam were different compared with the corresponding profiles for these factors at Stockton. A resuspended road salt factor was identified at Potsdam, while an aged sea salt factor was identified at Stockton. At Potsdam, a wood smoke factor was also resolved. Among the resolved factors, secondary sulfate was the highest contributor to the measured mass at both sites. Potential source contribution function (PSCF) analysis indicated the Ohio River Valley region as a common potential source region for this factor at both locations. For the secondary nitrate factor, at Potsdam PSCF analysis indicated the Midwestern US (NO_x emissions), and the US farm belt (ammonia emissions) as potential source regions, while at Stockton, the Midwestern US (power plant NO_x emissions) was indicated as a major potential source region.     

Potential sources of atmospheric total gaseous mercury in the St. Lawrence River valley

The potential source contribution function (PSCF) has been used to study the source–receptor relationships for total gaseous mercury (TGM) found in air collected at two sites along the St. Lawrence River valley, namely at St. Anicet and Mingan. TGM concentrations have been measured with high time-resolution analysers (Tekran instrument). The source–receptor analyses have been applied with regards to the seasonality of TGM. Median TGM concentrations are significantly less (χ²: α=0.01) during the summertime than other periods at both sites. A total of 12 225 trajectory end-points for St. Anicet and 4480 trajectory end points for Mingan have been used to create potential source area maps. This study identifies preferred potential sources of TGM at St. Anicet during wintertime with strongest probability stretching from the Gulf of Mexico to the southern tip of Greenland. This pattern mimics, the North American anthropogenic Hg emission inventory. Furthermore, some Eurasian mercury air mass intrusions are suggested at Mingan during wintertime. The summertime period at Mingan points out some potential sources stretching from the american mid-west to the St. Lawrence River valley as well as areas around the southern tip of the Hudson Bay.     

Assessing the effects of transboundary ozone pollution between Ontario,Canada and New York,USA

We investigated the effects of transboundary pollution between Ontario and New York using both observations and modeling results. Analysis of the spatial scales associated with ozone pollution revealed the regional and international character of this pollutant. A back-trajectory-clustering methodology was used to evaluate the potential for transboundary pollution trading and to identify potential pollution source regions for two sites: CN tower in Toronto and the World Trade Center in New York City. Transboundary pollution transport was evident at both locations. The major pollution source areas for the period examined were the Ohio River Valley and Midwest. Finally, we examined the transboundary impact of emission reductions through photochemical models. We found that emissions from both New York and Ontario were transported across the border and that reductions in predicted O3 levels can be substantial when emissions on both sides of the border are reduced.     

Contributions of global and regional sources to mercury deposition in New York State

A modeling system that includes a global chemical transport model (CTM) and a nested continental CTM (TEAM) was used to simulate the atmospheric transport, transformations and deposition of mercury (Hg). Three scenarios were used: (1) a nominal scenario, (2) a scenario conducive to local deposition and (3) a scenario conducive to long-range transport. Deposition fluxes of Hg were analyzed at three receptor locations in New York State. For the nominal scenario, the anthropogenic emission sources (including re-emission of deposited Hg) in New York State, the rest of the contiguous United States, Asia, Europe, and Canada contributed 11-1, 25-9, 13-19, 5-7, and 2-5%, respectively to total Hg deposition at these three receptors. Natural sources contributed 16-4%. The results from the local deposition and long-range transport scenarios varied only slightly from these results. However, there are still uncertainties in our understanding of the atmospheric chemistry of Hg that are likely to affect these estimates of local, regional and global contributions. Comparison of model simulation results with data from the Mercury Deposition Network suggests that local and regional contributions may currently be overestimated.     

Spatial distribution of source locations for particulate nitrate and sulfate in the upper-midwestern United States

Two back-trajectory analysis methods designed to be used with multiple site data, simplified quantitative transport bias analysis (SQTBA) and residence time weighted concentration (RTWC), were applied to nitrate and sulfate concentration data from two rural sites (the Mammoth Cave National Park and the Great Smoky Mountain National Park) and five urban sites (Chicago, Cleveland, Detroit, Indianapolis, and St. Louis) for an intensive investigation on the spatial patterns of origins for these two species in the upper-midwestern area. The study was made by dividing the data into five categories: all sites and all seasons, rural sites in summer, rural sites in winter, urban sites in summer, and urban sites in winter. A general conclusion was that the origins of the nitrate in these seven sites were mainly in the upper-midwestern areas, while the sulfate in these seven sites were mainly from the Ohio and Tennessee River Valley areas. The upper-midwestern areas are regions of high ammonia emissions rather than high NO_x emissions. In the winter, metropolitan areas showed the highest nitrate emission potential suggesting the importance of local NO_x emissions. In the summer, ammonia emissions from fertilizer application in the lower midwestern area made a significant contribution to nitrate in the rural sites of this study. The impact of the wind direction prevalence on the source spatial patterns was observed by comparing the urban and rural patterns of the summer. The differences between the results of two methods are discussed and suggestions for applying these methods are also provided.     

Source identification of atmospheric PCBs in Philadelphia/Camden using positive matrix factorization followed by the potential source contribution function

The concentrations of gas-phase polychlorinated biphenyls (PCBs) in the atmosphere of the Camden, NJ, USA are elevated by as much as 20 times over regional background. These high PCB levels are a concern because they lead to atmospheric deposition loadings of PCBs to the tidal Delaware River that exceed the entire total maximum daily load (TMDL). Two models were applied to the atmospheric PCB concentration data from Camden in an attempt to identify the PCB source types and regions. Positive matrix factorization (PMF) was used to identify the source types. Four factors were identified which are thought to represent sources such as volatilized Aroclors and particle-phase PCBs. The potential source contribution function (PSCF) model was then used to identify the geographic source regions by examining the origination points for air parcels that result in high PCB concentrations at the Camden receptor site. The PSCF model for ΣPCBs indicates PCB source regions throughout the Philadelphia–Camden metro area, including portions of both Pennsylvania and New Jersey. The PSCF plots for the resolved PMF factors suggest that factors 1–4 show fewer distinct source regions, indicating that their sources are diffuse and/or lie very close to the receptor site. The PSCF plots for factors 2 and 3 reveal very different source regions. Factor 2 primarily arises from the city of Philadelphia, whereas factor 3 originates in southern New Jersey and south of Philadelphia. This study demonstrates the utility of the combined PMF/PSCF approach in identifying atmospheric PCB source types and regions.     

Characteristics of total gaseous mercury concentrations at a coastal area of the Yangtze Delta,China

In this study, we report on total gaseous mercury (TGM) field observations made in the rural area of Shanghai, Chongming Island, China, from September 2009 to April 2012. The average TGM was 2.65 ± 1.73 ng m^?3 in Chongming Island, which is higher than the TGM background value of the Northern Hemisphere (1.5–1.7 ng m^?3); this indicates that to some extent, the Chongming area has been affected by anthropogenic mercury emissions. The observed TGM follows a seasonal pattern; concentrations are highest in winter, followed by autumn, summer, and spring. There is also a clear diurnal variation in TGM. All peak values appear between 7:00 and 9:00 in all four seasons; this appears to be the result of the height change in the atmospheric boundary layer that occurs between day and night. TGM concentrations in Chongming remain high in the westerly wind direction, especially in the southwest direction because of its low frequency, so the greatest source contribution to TGM in Chongming lies to the northwest. Wind speed is also a significant factor affecting TGM, and was negatively correlated with TGM concentrations. TGM is also closely related to carbon monoxide (CO) concentrations, indicating that TGM is impacted by human activities. The slope of the linear fitting of TGM and CO demonstrates that the contribution of noncoal source emissions to TGM in summer is greater than in autumn, mainly because the high temperature and intensive sunlight in summer increase mercury emissions from natural sources.

Implications: Except for some studies in the coastal areas (e.g., Kang Hwa Island by Kim et al., 2006, An–Myun Island by Kim et al., 2002, and Okinawa by Chan et al., 2008), data specifically for coastal areas are lacking. Monitoring of total gaseous mercury (TGM) in the rural area of Shanghai, Chongming Island, can help us understand mercury distribution.     

Characterization of atmospheric trace elements on PM2.5 particulate matter over the New York–New Jersey harbor estuary

The purpose of this work is to characterize trace elements associated with atmospheric particulate matter of 2.5 μm and smaller in size (PM_2.5) over the New York–New Jersey (NY–NJ) Harbor Bight. Using low-volume PM_2.5 samplers, aerosol particulate samples were simultaneously collected for the first time at three locations in the region, Sandy Hook in the coast, New Brunswick and Liberty Science Center (Jersey City) in nearby urban areas, during January 1998–January 1999. Sample analysis for trace elements was accomplished by inductively coupled plasma mass spectrometry. Many elements in ambient air exhibit strong spatial gradients from urban centers to the coast, and the concentrations of most elements at Liberty Science Center are significantly higher than at the other two locations. Seasonal patterns are not apparent for most elements at all locations, suggesting continuous contributions from their sources. The elements Pb, Cd, Zn, Cu, Ni, V, Sb, are enriched by factors of 200 to 20,000 relative to their natural abundance in crustal soil. Major sources that contribute to the atmospheric loading of these elements include fossil fuel combustion, oil combustion, metal processing industry, and waste incineration. Atmospheric dry deposition of these trace elements associated with PM_2.5 to the coastal waters of the NY–NJ estuary may account for a significant portion of the total dry deposition fluxes for these elements.     

Source apportionment of polychlorinated biphenyls in the New York/New Jersey Harbor

The New York/New Jersey Harbor (also known as the Hudson River Estuary) is heavily contaminated with polychlorinated biphenyls (PCBs) arising in part from inputs from the Upper Hudson River, which is a Superfund site containing historical PCB contamination, and also due to inputs from the New York City metropolitan area. The Contamination Assessment and Reduction Project (CARP) measured PCBs and other contaminants in ambient water samples collected throughout the Harbor region during 1998-2001. In order to investigate the sources of PCBs to the NY/NJ Harbor, this data base of PCB concentrations was analyzed using Positive Matrix Factorization (PMF). This analysis resolved seven factors that are thought to be associated with sources such as the Upper Hudson River, storm water runoff, combined sewer overflows (CSOs), and wastewater effluents. The PMF model also produced a factor that appears to be related to sites contaminated with Aroclor 1260. To the extent that the NY/NJ Harbor is typical of urbanized estuaries throughout the United States, these results suggest that storm water runoff is probably a significant source of PCBs to surface waters in urban areas.     

Atmospheric mercury monitoring survey in Beijing,China

With the aid of one industrial, two urban, two suburban, and two rural sampling locations, diurnal patterns of total gaseous mercury (TGM) were monitored in January, February and September of 1998 in Beijing, China. Monitoring was conducted in six (two urban, two suburban, one rural and the industrial sites) of the seven sampling sites during January and February (winter) and in four (two urban, one rural, and the industrial sites) of the sampling locations during September (summer) of 1998. In the three suburban sampling stations, mean TGM concentrations during the winter sampling period were 8.6, 10.7, and 6.2 ng/m3, respectively. In the two urban sampling locations mean TGM concentrations during winter and summer sampling periods were 24.7, 8.3, 10, and 12.7 ng/m3, respectively. In the suburban-industrial and the two rural sampling locations, mean mercury concentrations ranged from 3.1-5.3 ng/m3 in winter to 4.1-7.7 ng/m3 in summer sampling periods. In the Tiananmen Square (urban), and Shijingshan (suburban) sampling locations the mean TGM concentrations during the summer sampling period were higher than winter concentrations, which may have been caused by evaporation of soil-bound mercury in warm periods. Continuous meteorological data were available at one of the suburban sites, which allowed the observation of mercury concentration variations associated with some weather parameters. It was found that there was a moderate negative correlation between the wind speed and the TGM concentration at this suburban sampling location. It was also found that during the sampling period at the same site, the quantity of TGM transported to or from the sampling site was mainly influenced by the duration and frequency of wind occurrence from certain directions.     

Trend,seasonal and multivariate analysis study of total gaseous mercury data from the Canadian atmospheric mercury measurement network (CAMNet)

Long-term monitoring data of total gaseous mercury (TGM) concentrations from the Canadian Atmospheric Mercury Measurement Network (CAMNet) were analysed for temporal trends, seasonality and comparability within the network and compared to other network and model results. Data collected from 11 Canadian measurement sites between 1995 and 2005 were analysed. Sites within CAMNet were characterized by principle component analysis (PCA) into four main categories. For the first time since automated TGM measurements have been made within CAMNet, this paper reveals statistically significant decreasing TGM concentrations from rural locations in Canada during this time period. The largest declines were observed close to the urban areas of Toronto and Montreal, where levels fell by 17% at Point Petre, and 13% at St. Anicet, respectively. Many of the TGM changes are comparable with the overall trends observed in total mercury concentrations in precipitation, for similar time periods, at co-located or nearby National Atmospheric Deposition programme's Mercury Deposition Network (NADP-MDN) sites. The results show that these changes are mostly driven by local or regional changes in mercury emissions. Other sites within CAMNet reflect reported changes in hemispherical global background concentrations of airborne mercury, where slight decreases or no statistically significant trend in TGM concentrations exist over the same time period.     

Atmospheric mercury distribution in Northern Europe and in the Mediterranean region

Mercury species in air have been measured at five sites in Northwest Europe and at five coastal sites in the Mediterranean region during measurements at four seasons. Observed concentrations of total gaseous mercury (TGM), total particulate mercury (TPM) and reactive gaseous mercury (RGM) were generally slightly higher in the Mediterranean region than in Northwest Europe. Incoming clean Atlantic air seems to be enriched in TGM in comparison to air in Scandinavia. Trajectory analysis of events where high concentrations of TPM simultaneously were observed at sites in North Europe indicate source areas in Central Europe and provide evidence of transport of mercury on particles on a regional scale.     

Rural and Urban Ozone Relationships In New York State

High ozone concentrations, often in excess of the national ambient air quality standard for photochemical oxidants, have been measured simultaneously in urban and rural areas of New York State. Average daily rural ozone concentrations were found to correlate well with daily maximum urban ozone concentrations suggesting a common source. Estimations of the quantity of ozone advectively transported into New York State are more than an order of magnitude greater than estimations of the potential photochemical generation of ozone from hydrocarbon emissions within New York State. It is suggested thai the high rural ozone levels are not primarily due to the transport of ozone and ozone precursors from olher urban areas, but are rather due to natural phenomena such as photochemical generation from naturally occurring precursors or transport of ozone from the stratosphere to the troposphere. The effectiveness of a hydrocarbon control strategy for New York State to meet the ambient air quality standard for photochemical oxidants when background levels themselves may be above the standard is questioned.     

Polychlorinated biphenyls (PCB) and dichlorodiphenyltrichloroethane (DDE) air concentrations in the Lake Ontario region: Trends and potential sources

Airborne particle and gas samples were collected approx every 12 days from April 2002 to June 2006 at the Sterling Nature Center located near the southeast corner of Lake Ontario. These samples were analyzed for polychlorinated biphenyls (PCBs) and dichlorodiphenyltrichloroethane (DDE). Clausius-Clapeyron (C–C) regression analyses of PCBs and DDE yielded moderate correlations (r² = 0.54, p < 0.001; r² = 0.74, p < 0.001, respectively) indicating that much of the variations in concentrations can be explained by temperature. Back trajectory analysis indicated that the most important factors driving unusually high PCB partial pressures relative to those predicted by the C–C regression were slow wind speeds and winds generally from the southwest. This combination, which occurred frequently in 2004, increased contact of the air with contaminated upwind surfaces with minimum dilution. Hybrid receptor modeling (Potential Source Contribution Function (PSCF)) results for the total PCBs identified the midwestern US region that contains the urban areas of southern Indiana (IN), southwestern Ohio (OH), and northern Kentucky (KY) having the highest PSCF values. In general urban areas like Chicago (IL), Detroit (MI), Cleveland (OH), St. Louis (MO), and Nashville (TN) also had significant possibilities. In contrast, the PSCF modeling for DDE identified northern Alabama as the area with the highest probability where DDT was applied to cotton fields.     

A Receptor Climatology of Trajectories Originating in New York State

Air parcel trajectories originating from three locations in New York State are calculated for a three year period using the ARL-ATAD long-range transport model. Model output consisting of a trajectory segment's end point longitude and latitude position are analyzed to describe the long-range transport climatology by computing the frequency of occurrence of segment end points terminating over 33 receptor areas comprising east-central North America and a portion of the Atlantic Ocean. Results of the frequency of occurrence data show how often air pollutants emitted at or near the origin may be expected to drift over a specific downwind region. For the New York City airshed, it was found that 26.2% of the trajectories remain over New York State for transport times of 3 h and the frequency decreases to 5.2% after 24 h of transport. Approximately 40% of all trajectories are found to be over the Atlantic Ocean after 3 h of transport. When allowances are made for losses of data over the Atlantic Ocean, up to 64% of all trajectories are over the Atlantic Ocean after 24 h of transport. This frequency of trajectories over the Atlantic Ocean was found to be in agreement with wet and dry deposition modeling results conducted for power plants in New York City.     

Estimation of source apportionment and potential source locations of PM2.5 at a west coastal IMPROVE site

Particle composition data for PM_2.5 samples collected at Kalmiopsis Interagency Monitoring of Protected Visual Environments (IMPROVE) site in southwestern Oregon from March 2000 to May 2004 were analyzed to provide source identification and apportionment. A total of 493 samples were collected and 32 species were analyzed by particle induced X-ray emission, proton elastic scattering analysis, photon-induced X-ray fluorescence, ion chromatography, and thermal optical reflectance methods. Positive matrix factorization (PMF) was used to estimate the source profiles and their mass contributions. The PMF modeling identified nine sources. In the Kalmiopsis site, the average mass was apportioned to wood/field burning (38.4%), secondary sulfate (26.9%), airborne soil including Asian dust (8.6 %), secondary nitrate (7.6%), fresh sea salt (5.8%), OP-rich sulfate (4.9%), aged sea salt (4.5 %), gasoline vehicle (1.9%), and diesel emission (1.4%). The potential source contribution function (PSCF) was then used to help identify likely locations of the regional sources of pollution. The PSCF map for wood/field burning indicates there is a major potential source area in the Siskiyou County and eastern Oregon. The potential source locations for secondary sulfate are found in western Washington, northwestern Oregon, and the near shore Pacific Ocean where there are extensive shipping lanes. It was not possible to extract a profile directly attributable to ship emissions, but indications of their influence are seen in the secondary sulfate and aged sea salt compositions.     

Methylated mercury species in municipal waste landfill gas sampled in Florida,USA

Mercury-bearing material has been placed in municipal landfills from a wide array of sources including fluorescent lights, batteries, electrical switches, thermometers, and general waste. Despite its known volatility, persistence, and toxicity in the environment, the fate of mercury in landfills has not been widely studied. The nature of landfills designed to reduce waste through generation of methane by anaerobic bacteria suggests the possibility that these systems might also serve as bioreactors for the production of methylated mercury compounds. The toxicity of such species mandates the need to determine if they are emitted in municipal landfill gas (LFG). In a previous study, we had measured levels of total gaseous mercury (TGM) in LFG in the μg/m³ range in two Florida landfills, and elevated levels of monomethyl mercury (MMM) were identified in LFG condensate, suggesting the possible existence of gaseous organic Hg compounds in LFG. In the current study, we measured TGM, Hg⁰, and methylated mercury compounds directly in LFG from another Florida landfill. Again, TGM was in the μg/m³ range, MMM was found in condensate, and this time we positively identified dimethyl mercury (DMM) in the LGF in the ng/m³ range. These results identify landfills as a possible anthropogenic source of DMM emissions to air, and may help explain the reports of MMM in continental rainfall.     

Analysis of trace elements and ions in ambient fine particulate matter at three elementary schools in Ohio

The results from a chemical characterization study of fine particulate matter (PM2.5) measured at three elementary schools in Central and Southeast Ohio is presented here. PM2.5 aerosol samples were collected from outdoor monitors and indoor samplers at each monitoring location during the period of February 1, 1999, through August 31, 2000. The locations included a rural elementary school in Athens, OH, and two urban schools within Columbus, OH. The trace metal and ionic concentrations in the collected samples were analyzed using an X-ray fluorescence spectrophotometer and ion chromatography unit, respectively. Sulfate ion was found to be the largest component present in the samples at all three of the sites. Other abundant components included nitrate, chloride, ammonium, and sodium ions, as well as calcium, silicon, and iron. The average PM2.5 concentrations showed similar temporal variations among the three sites within the study region. PM2.5 and its major component, sulfate ion, showed strong seasonal variations with maximum concentrations observed during the summer at all three of the sites. The indoor environment was found to be more contaminated during the spring months (March through May) at New Albany (a suburb of Columbus, OH) and East Athens (rural Ohio area). Potential source contribution function analysis showed that particulate matter levels at the monitoring sites were affected by transport from adjoining urban areas and industrial complexes located along the Ohio River Valley. A preliminary outdoor source apportionment using the principal component analysis (PCA) technique was performed. The results from the PCA suggest that the study region was primarily impacted by industrial, fossil fuel combustion, and geological sources. The 2002 emissions inventory data for PM2.5 compiled by Ohio Environmental Protection Agency also showed impacts of similar source types, and this was used to validate the PCA analysis.     

Lake variability: key factors controlling mercury concentrations in New York State fish

A 4year study surveyed 131 lakes across New York State beginning in 2003 to improve our understanding of mercury and gather information from previously untested waters. Our study focused on largemouth and smallmouth bass, walleye and yellow perch, common piscivorous fish shown to accumulate high mercury concentrations and species important to local fisheries. Fish from Adirondack and Catskill Forest Preserve lakes generally had higher mercury concentrations than those from lakes in other areas of the state. Variability between nearby individual lakes was observed, and could be due to differences in water chemistry, lake productivity or the abundance of wetlands in the watershed. We found the following factors impact mercury bioaccumulation: fish length, lake pH, specific conductivity, chlorophyll a, mercury concentration in the water, presence of an outlet dam and amount of contiguous wetlands.