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.     

Estimation of source locations of total gaseous mercury measured in New York State using trajectory-based models

Ambient gaseous phase mercury concentrations (TGM) were measured at three locations in NY State including Potsdam, Stockton, and Sterling from May 2000 to March 2005. Using these data, three hybrid receptor models incorporating backward trajectories were used to identify source areas for TGM. The models used were potential source contribution function (PSCF), residence time weighted concentration (RTWC), and simplified quantitative transport bias analysis (SQTBA). Each model was applied using multi-site measurements to resolve the locations of important mercury sources for New York State.PSCF results showed that southeastern New York, Ohio, Indiana, Tennessee, Louisiana, and Virginia were important TGM source areas for these sites. RTWC identified Canadian sources including the metal production facilities in Ontario and Quebec, but US regional sources including the Ohio River Valley were also resolved. Sources in southeastern NY, Massachusetts, western Pennsylvania, Indiana, and northern Illinois were identified to be significant by SQTBA. The three modeling results were combined to locate the most important probable source locations, and those are Ohio, Indiana, Illinois, and Wisconsin. The Atlantic Ocean was suggested to be a possible source as well.     

A study on the potential sources of air pollutants observed at Tjörn,Sweden

The Potential Source Contribution Function (PSCF) receptor model combines both chemical and meteorological information. In this study, PSCF was employed to identify the potential source emission regions for aerosol compositions measured at Tjörn, Sweden (58.01 °N, 11.36 °E). PSCF was for the first time applied on a European scale. One hundred and fifty-two four-day air parcel backward trajectories were combined with concentrations of sixteen elements determined in 33 coarse and fine aerosol samples. The observations were made between February 17 and March 26, 1985. The modeling results of the heavy metals V, Pb, Zn, and As are presented and compared with available emission inventory data. A number of known industrialized regions in the former USSR and Europe are found of high potential to be the emission source areas. These areas are in good agreement with the known emission information. The PSCF maps of total sulfur, Non-Seasalt-Sulfur (N.S.S.) and chlorine are also presented. High potential regions in the Arctic area exist in the PSCF map for total sulfur wheres they do not occur in that for N.S.S.     

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.     

Seasonal variation and spatial distribution of atmospheric mercury and its gas-particulate partition in the vicinity of a semiconductor manufacturing complex

This study investigated the tempospatial variation of atmospheric mercury and its gas-particulate partition in the vicinity of a semiconductor manufacturing complex, where a plenty of flat-monitor manufacturing plants using elemental mercury as a light-initiating medium to produce backlight fluorescence tubes and may fugitively emit mercury-containing air pollutants to the atmosphere. Atmospheric mercury speciation, concentration, and the partition of total gaseous mercury (TGM) and particulate mercury (Hg_p) were measured at four sites surrounding the semiconductor manufacturing intensive district/complex. One-year field measurement showed that the seasonal averaged concentrations of TGM and Hg_p were in the range of 3.30–6.89 and 0.06–0.14 ng/m³, respectively, whereas the highest 24-h TGM and Hg_p concentrations were 10.33 and 0.26 ng/m³, respectively. Atmospheric mercury apportioned as 92.59–99.01 % TGM and 0.99–7.41 % Hg_p. As a whole, the highest and lowest concentrations of TGM were observed in the winter and summer sampling periods, respectively, whereas the concentration of Hg_p did not vary much seasonally. The highest TGM concentrations were always observed at the downwind sites, indicating that the semiconductor manufacturing complex was a hot spot of mercury emission source, which caused severe atmospheric mercury contamination over the investigation region.     

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.     

Total gaseous concentrations in mercury in Seoul, Korea: Local sources compared to long-range transport from China and Japan

Total gaseous mercury (TGM) and carbon monoxide (CO) were measured every 5 min and hourly, respectively, in Seoul, Korea, from February 2005 through December 2006. The mean concentrations of TGM and CO were 3.44 ± 2.13 ng m⁻³ and 613 ± 323 ppbv, respectively. TGM and CO concentrations were highest during the winter and lowest during the summer. In total, 154 high TGM concentration events were identified: 86 were classified as long-range transport events and 68 were classified as local events. The TGM and CO concentrations were well correlated during all long-range transport events and were weakly correlated during local events. Five-day backward trajectory analysis for long-range transport events showed four potential source regions: China (79%), Japan (13%), the Yellow Sea (6%), and Russia (2%). Our results suggest that measured ΔTGM/ΔCO can be used to identify long-range transported mercury and to estimate mercury emissions from long-range transport.     

Atmospheric mercury in the marine boundary layer along a cruise path from Shanghai,China to Prydz Bay,Antarctica

The total gaseous mercury (TGM) measurements were performed using an automatic Mercury Vapor Analyze (model 2537B) aboard the Chinese research vessel (R/V) XueLong during the 24th China Antarctic Research Expedition from Shanghai, China to Prydz Bay, Antarctica in 2007. TGM ranged between 0.302 and 4.496 ng m^?3 with an average of 1.536 ± 0.785 ng m^?3 over the entire period. Geographically, TGM in the Northern Hemisphere and the Southern Hemisphere along the cruise path were 1.746 ± 0.513 and 1.471 ± 0.842 ng m^?3 in average, respectively. Higher TGM concentrations were observed in the coastal regions outside the polar region due primarily to air masses transported from the adjacent mainland reflecting the contribution from anthropogenic sources. The pronounced episode was recorded when ship passed through Sunda straits, which should be ascribed to the volcano plume and/or biomass burning contamination. In the maritime Antarctic TGM level was in agreement with the values by land-based observation, presenting a diurnal cycle with the maximum around midday and minimum at night. Atmospheric mercury destruction events dominated by the oxidation of atmospheric Hg⁰ were apparently observed in this region.     

Locations and preferred pathways of possible sources of Arctic aerosol

The chemical composition of particles collected at Alert, Northwest Territories, Canada, show strong, persistent seasonal variations. In a previous study, a 2-way/3-way mixed factor model was performed on the weekly average concentrations of 24 aerosol components measured over the period from 1980 to 1991. The Multilinear Engine (ME), a new mathematical technique, was used to obtain the solution. The two modes of the 2-way model consist of the source composition profiles and mass contributions over the 11 yr, while for the three modes of the 3-way model, source profiles, mass contributions variations over the weeks within a year, and the year-to-year variation over the 11 yr within the measurement period. Five 2-way and two 3-way factors were found to provide a good fit to the data and were easily interpreted. In this investigation, potential source contribution function (PSCF) analysis was applied to the source contributions derived from the ME analysis by incorporating meteorological information in the form of 5-d air parcel back trajectories. The potential locations and/or the preferred pathways of these possible sources were then determined by the PSCF analysis.     

Seasonal and diel variation of atmospheric mercury concentrations in the Reno (Nevada,USA) airshed

This paper describes total gaseous mercury (TGM) concentrations measured in Reno, Nevada from 2002 to 2005. The 3-year mean and median air Hg concentrations were 2.3 and 2.1 ng m⁻³, respectively. Mercury concentrations exhibited seasonality, with the highest concentrations in winter, and the lowest in summer and fall. A well-defined diel pattern in TGM concentration was observed, with maximum daily concentrations observed in the morning and minimum in the afternoon. A gradual increase of TGM concentration was observed in the evening and over night. The early morning increase in TGM was likely due to activation of local surface emission sources by rising solar irradiance and air temperature. The subsequent decline and afternoon minimum in TGM were likely related to increased vertical mixing and the buildup of atmospheric oxidants during the day resulting in increased conversion to oxidized species that are quickly deposited, coupled with weakening of the surface emissions processes. The described diel pattern was seasonally modulated with the greatest amplitude in variation of TGM concentrations occurring in the summer. It is suggested based on the comparison of diel TGM pattern with other gaseous pollutants that natural source surface emissions are a dominant source of TGM in the study area.     

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.     

Atmospheric concentrations of chlordane at Mould Bay,N.W.T., Canada

Chlordane and nonachlors isomers in the range 0.1 – 1.8 pg/m³ were measured in the Canadian Arctic in June-July 1984. Implications regarding input to Arctic biota are discussed.Long range transport of air pollution to the remotest parts of the globe is no longer surprising to most atmospheric scientists. Pollution from mid-latitudes has been detected in the Arctic for a number of years¹. The detection of chlorinated pesticides and hydrocarbons in Arctic fauna² and Antarctic fauna³ naturally prompted suspicions of long-range transport of airborne pollutants as a possible source. In this paper, we will report the detection of gas phase chlordane isomers at Mould Bay, Northwest Territories, Canada during the summer of 1984.Mould Bay is a isolated 12 person meteorological outpost on Melville Island (76.5°N, 118°W). Arctic haze has been monitored at this site since 1979^{4 5}. It is believed that Mould Bay is quite representative of the Canadian Arctic archepelago in general, as little difference in air concentrations of sulphate aerosol is seen between Mould Bay, Alert and Igloolik, N.W.T.⁵ This wide spatial homogeneity of the Arctic air mass prompted the Atmospheric Environment Service (AES) to decommission two air monitoring stations, Mould Bay and Igloolik, in 1984. At the decommissioning of the Mould Bay sampler, we converted the high-volume sampler for a short study of organics using glass fibre filters and polyurethane foam plugs⁶.     

Characteristics of mercury exchange flux between soil and air in the heavily air-polluted area,eastern Guizhou,China

To investigate the characteristics of mercury exchange between soil and air in the heavily air-polluted area, total gaseous mercury (TGM) concentration in air and Hg exchange flux were measured in Wanshan Hg mining area (WMMA) in November, 2002 and July–August, 2004. The results showed that the average TGM concentrations in the ambient air (17.8–1101.8 ng m⁻³), average Hg emission flux (162–27827 ng m⁻² h⁻¹) and average Hg dry deposition flux (0–9434 ng m⁻² h⁻¹) in WMMA were 1–4 orders of magnitude higher than those in the background area. It is said that mercury-enriched soil is a significant Hg source of the atmosphere in WMMA. It was also found that widely distributed roasted cinnabar banks are net Hg sources of the atmosphere in WMMA. Relationships between mercury exchange flux and environmental parameters were investigated. The results indicated that the rate of mercury emission from soil could be accelerated by high total soil mercury concentration and solar irradiation. Whereas, highly elevated TGM concentrations in the ambient air can restrain Hg emission from soil and even lead to strongly atmospheric Hg deposition to soil surface. A great amount of gaseous mercury in the heavily polluted atmosphere may cycle between soil and air quickly and locally. Vegetation can inhibit mercury emission from soil and are important sinks of atmospheric mercury in heavily air-polluted area.     

Dynamics of mercury fluxes and their controlling factors in large Hg-polluted floodplain areas

Environmental pollution by mercury (Hg) is a considerable environmental problem world-wide. Due to the occurrence of Hg volatilization from their soils, floodplains can function as an important source of volatile Hg. Soil temperature and soil water content related to flood dynamics are considered as important factors affecting seasonal dynamics of total gaseous mercury (TGM) fluxes. We quantified seasonal variations of TGM fluxes and conducted a laboratory microcosm experiment to assess the effect of temperature and moisture on TGM fluxes in heavily polluted floodplain soils. Observed TGM emissions ranged from 10 to 850 ng m⁻² h⁻¹ and extremely exceeded the emissions of non-polluted sites. TGM emissions increased exponentially with raised air and soil temperatures in both field (R²: 0.49-0.70) and laboratory (R²: 0.99) experiments. Wet soil material showed higher TGM fluxes, whereas the role of soil water content was affected by sampling time during the microcosm experiments.     

Trends in air concentration and deposition of mercury in the coastal environment of the North Sea Area

An evaluation of mercury observations from North Sea coastal stations during 1995–2002 has been performed. The mercury data originate from EMEP/OSPAR stations in Ireland, Netherlands, Germany, Norway and Sweden where mercury in precipitation and Total Gaseous Mercury (TGM) have been measured. A decreasing trend in mercury wet deposition is observed. The decrease is sufficiently large to be significant considering measurement precision and appears to occur at all the studied sites. The reduction in deposition is 10–30% when comparing the two periods 1995–1998 and 1999–2002. The trend is likely to be due to emission controls in Europe. In contrast, no decreasing trend in TGM could be observed during the same time periods. A plausible explanation is that the TGM concentration measured in the OSPAR area to a larger extent than before is dominated by the hemispherical background concentration of TGM.     

International field intercomparison measurements of atmospheric mercury species at Mace Head,Ireland

Eleven laboratories from North America and Europe met at Mace Head, Ireland for the period 11–15 September 1995 for the first international field intercomparison of measurement techniques for atmospheric mercury species in ambient air and precipitation at a marine background location. Different manual methods for the sampling and analysis of total gaseous mercury (TGM) on gold and silver traps were compared with each other and with new automated analyzers. Additionally, particulate-phase mercury (Hg_part) in ambient air, total mercury, reactive mercury and methylmercury in precipitation were analyzed by some of the participating laboratories. Whereas measured concentrations of TGM and of total mercury in precipitation show good agreement between the participating laboratories, results for airborne particulate-phase mercury show much higher differences. Two laboratories measured inorganic oxidized gaseous mercury species (IOGM), and obtained levels in the low picogram m^-3 range.     

Atmospheric mercury pollution at an urban site in central Taiwan: mercury emission sources at ground level

Total gaseous mercury (Hg) (TGM), gaseous oxidized Hg (GOM), and particulate-bound Hg (PBM) concentrations and dry depositions were measured at an urban site in central Taiwan. The concentrations were 6.14 ± 3.91 ng m⁻³, 332 ± 153, and 71.1 ± 46.1 pg m⁻³, respectively. These results demonstrate high Hg pollution at the ground level in Taiwan. A back trajectory plot shows the sources of the high TGM concentration were in the low atmosphere (<500 m) and approximately 50% of the air masses coming from upper troposphere (>500 m) were associated with low TGM concentrations. This finding implies that Hg is trapped in the low atmosphere and comes from local Hg emission sources. The conditional probability function (CPF) reveals that the plumes of high TGM concentrations come from the south and northwest of the site. The plume from the south comes from two municipal solid waste incinerators (MSWIs). However, no significant Hg point source is located to the northwest of the site; therefore, the plumes from the northwest are hypothesized to be related to the combustion of agricultural waste. Dry deposition fluxes of Hg measured at this site considerably exceeded those measured in North America. Overall, this area is regarded as a highly Hg contaminated area because of local Hg emission sources.     

Modeling of mercury emission,transport and deposition in North America

Most studies on the atmospheric behaviour of mercury in North America have excluded a detailed treatment of natural mercury emissions. The objective of this work is to report a detailed simulation of the atmospheric mercury in a domain that covers a significant part of North America and includes not only anthropogenic mercury emissions but also those from natural sources including vegetation, soil and water.The simulations were done using a natural mercury emission model coupled with the US EPA's SMOKE/CMAQ modelling system. The domain contained 132×90 grid cells at a resolution of 36 km, covering the continental United States, and major parts of Canada and Mexico. The simulation was carried out for 2002, using boundary conditions from a global mercury model. Estimated total natural mercury emission in the domain was 230 tonnes (1 tonne=1000 kg) and the ratio of natural to anthropogenic emissions varied from 0.7 in January to 3.2 in July. Average total gaseous mercury (TGM) concentration ranged between 1 and 4 ng m⁻³. Good agreement was found between the modelled results and measurements at three Ontario sites for ambient mercury concentrations, and at 72 mercury deposition network sites in the domain for wet deposition. The correlation coefficient between the simulated and the measured values of the daily average TGM at three monitoring sites varied between 0.48 and 0.64. When natural emissions were omitted, the correlation coefficients dropped to between 0.15 and 0.40. About 335 tonnes of mercury were deposited in the domain during the simulation period but overall, it acted as a net source of mercury and contributed about 21 tonnes to the global pool. The net deposition of mercury to the Great Lakes was estimated to be about 2.4 tonnes. The estimated deposition values were similar to those reported by other researchers.     

Characteristics of atmospheric speciated mercury concentrations (TGM,Hg(II) and Hg(p)) in Seoul,Korea

Ambient speciated mercury concentrations including total gaseous mercury (TGM), gaseous divalent mercury (Hg(II)), and particulate mercury (Hg(p)) were measured on the roof of the Graduate School of Public Health building in Seoul, Korea from February 2005 to February 2006. The average concentrations were 3.22 ± 2.10 ng m^?3, 27.2 ± 19.3 pg m^?3, and 23.9 ± 19.6 pg m^?3 for TGM, Hg(II), and Hg(p), respectively. Hg(II) and Hg(p) concentrations were higher during the daytime than during the nighttime, probably because of high photochemical activity. Hg⁰ concentrations were not significantly correlated with ozone however a positive correlation between ozone and Hg(II) was found during periods of high humidity. Eighteen days were characterized as pollution events with 24 h average PM_2.5 concentrations >65 μg m^?3. The average concentrations of TGM and Hg(p) during these events were 1.4–2 times higher than those during non-pollution events. In order to identify the contribution of long-range transported mercury to the enhanced mercury concentrations in Korea, an episode was defined as a period with hourly average TGM and CO concentrations higher than the monthly average TGM and CO concentrations and with significant enhancement of both TGM and CO concentrations for at least 10 h. A total of 70 episodes were identified during the sampling period: 36 local episodes and 34 long-range transport episodes. The mean ΔTGM/ΔCO slope for all episodes was 0.0063 ng m^?3 ppbv^?1 which agreed well with the slope (0.0036–0.0074 ng m^?3 ppbv^?1) found in previous studies that identified long-range transport of TGM from China. The mean slope during non-events was 0.0011 ng m^?3 ppbv^?1. Back-trajectory analysis showed that during episodes, air parcels arrived mostly from the major industrial areas in China (n = 25, 73%), followed by Japan (n = 4, 12%), Yellow Sea (n = 3, 9%), and Russia (n = 2, 6%).     

Simultaneous measurements of total gaseous mercury at four sites on a 800 km transect: spatial distribution and short-time variability of total gaseous mercury over central Europe

Over a distance of approximately 800 km simultaneous measurements of total gaseous mercury (TGM) were performed at four sampling sites between Stockholm and Berlin. The time resolution of mercury concentration measurements was 5 min. During the sampling period from 26 June to 7 July 1995, event sampling for precipitation was carried out using bulk samplers. In addition to the mercury data, the most common meteorological and air-quality parameters were determined. Comparing the TGM background concentrations at the four sites, a weak but statistically significant south-to-north declining TGM gradient was found. From the most southern sampling site to the northern most site median values of 1.93, 1.78, 1.53 and 1.54 ng m^-3 TGM were detected. Compared with the median TGM concentration observed at the two Swedish sites, the regional background concentration near Berlin was elevated by about 25%. Whereas the 0.5 h average TGM concentration varies at the Swedish sampling sites in a very narrow range of only 0.69 ng m^-3, a much broader range of 3.28 ng m^-3 was observed at the southern sites. The increased TGM variability near Berlin was characterised by a diurnal cycle with a distinct maximum in the early morning hours (about 4:00 a.m.) before sun rise. The short time variability of the TGM concentration measured at the four sites on the south-to-north transect shows regional differences. A decreasing variability from the most southern to the most northern site became evident.