Springtime depletion of mercury in the European Arctic as observed at Svalbard

This study was carried out to see whether the geographical extent of the mercury depletion events (MDEs), first seen at Alert in the Canadian High Arctic, is also covering Svalbard. Another goal was to determine the main reaction products from the MDE and their fate. Gaseous elemental mercury (GEM), total particulate mercury (TPM), reactive gaseous mercury (RGM) and total mercury in surface snow have been measured at the Zeppelin mountain during 2000. GEM has been measured with a high time resolution automatic monitor (Tekran 2537A) based on CV-AFS, TPM was sampled/measured using high volume samplers/CV-AFS and RGM was sampled with annular denuders and measured by CV-AFS (Gardis Hg-monitor). During spring of 2000, in the three-month period following polar sunrise, there were several episodic depletions in GEM concentration correlating well with the depletion of surface ozone. Measurements of RGM and TPM showed higher concentrations of these mercury species during the depletion period than during the rest of the year. Total mercury in surface snow showed a distinct increase from the polar night to the Arctic spring. MDEs are caused by the specific chemical and physical conditions observed in the Arctic during spring. GEM is oxidised and converted to more reactive forms (RGM and/or TPM), which have considerably higher deposition velocities than elemental mercury, leading to an overall enhanced deposition flux of mercury.     

Scavenging of gaseous mercury by acidic snow at Kuujjuarapik, Northern Québec

One fate of gaseous elemental mercury (GEM) in the Arctic has been identified as gas phase oxidation by halogen-containing radicals, leading to abrupt atmospheric mercury depletion concurrent with ozone depletion. Rapid deposition of oxidized mercury leads to snow enrichment in mercury. In this report, we describe experiments that demonstrate the ability of snow to directly scavenge atmospheric mercury. The study was conducted at Kuujjuarapik, Québec, Canada (latitude 55 degrees 17'N). A mercury depletion event (MDE) caused the mercury concentration in the surface snow of the coastal snowpack to double, from (9.4+/-2.0) to (19.2+/-1.7) ng/L. Independent of the MDE, mercury concentrations increased five-fold, from (10.0+/-0.1) to (51.4+/-6.0) ng/L, upon spiking the snow with 500 microM hydrogen peroxide under solar irradiation. Total organic carbon in the spiked irradiated snow samples also decreased, consistent with the formation of strongly oxidizing species. The role of the snowpack in releasing GEM to the atmosphere has been reported; these findings suggest that snow may also play a role in enhancing deposition of mercury.     

Temporal and spatial variabilities of atmospheric polychlorinated biphenyls (PCBs), organochlorine (OC) pesticides and polycyclic aromatic hydrocarbons (PAHs) in the Canadian Arctic: results from a decade of monitoring

The Northern Contaminants Program (NCP) baseline monitoring project was established in 1992 to monitor for persistent organic pollutants (POPs) in Arctic air. Under this project, weekly samples of air were collected at four Canadian and two Russian arctic sites, namely Alert, Nunavut; Tagish, Yukon; Little Fox Lake, Yukon; Kinngait, Nunavut; Dunai Island, Russia and Amderma, Russia. Selected POPs, including polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs) and organochlorine (OC) pesticides, were analyzed in both the gas and particulate phases. This paper summarizes results obtained from this project in the past 5 years. Temporal trends were developed for atmospheric PCBs and OCs observed at Alert using a digital filtration (DF) technique. It was found that trends developed with 5 years of data (1993-1997) did not differ significantly from those determined with 7 years of data (1993-1999). This implies that with the DF technique, long-term trends can still be developed with less than 10 years of data. An acceleration in decline of OC and PCB air concentrations was noted in 1999 for some compounds, although the reason is unknown. Monitoring efforts must continue to assess the effect of this decline on the long-term trends of POPs in the Canadian Arctic. Occasional high trans-/cis-chlordane ratios and heptachlor air concentrations measured at Alert between 1995 and 1997 suggests sporadic fresh usage of chlordane-based pesticides. However, significant decreasing trends of chlordanes along with their chemical signatures has provided evidence that emission of old soil residues is replacing new usage as an important source to the atmosphere. Measurements of OC air concentrations conducted at Kinngait in 1994-1995 and 2000-2001 indicated faster OC removal at this location than at Alert. This may be attributed to the proximity of Kinngait to temperate regions where both biotic and abiotic degradation rates are faster. The PAH concentrations observed at Alert mimic those at mid-latitudes and are consistent with long-range transport to the Arctic, particularly for the lighter PAHs. A decline in particulate PAH was observed, similar to atmospheric sulphate aerosol and can be attributed to the collapse of industrial activity in the former Soviet Union between 1991 and 1995. Spatial comparisons of OC seasonality at Alert, Tagish, Dunai and Kinngait show elevated air concentrations of some compounds in spring. However, elevated spring concentrations were observed for different compounds at different sites. Potential causes are discussed. Further investigation in the atmospheric flow pattern in spring which is responsible for the transport of POPs into the Arctic is required. OC and PCB air concentrations at Alert were found to be influenced by two climate variation patterns, the North Atlantic Oscillation (NAO) and the Pacific North American (PNA) pattern. Planetary atmospheric patterns must be taken into account in the global prediction and modelling of POPs in the future.     

Total gaseous mercury in Quebec (Canada) in 1998

The main objectives of this paper were to report total gaseous mercury (TGM) concentrations at four stations along the St. Lawrence River in 1998 and to give some insights regarding their fate. The TGM network stretches from latitudes 45 degrees N to 50 degrees N. TGM and ozone concentrations (used as complementary pollutant) were presented. The median TGM concentrations throughout the network varied from 1.62 to 1.79 ng/m3. Sites close to Montreal had larger TGM concentrations. Montreal surroundings appeared to be a source of TGM. The TGM concentrations were maximum in wintertime and minimum in summertime throughout the sites. However, the diurnal variations were site specific. St. Anicet and L'Assomption were more variable in terms of large concentrations, whereas Mingan and Villeroy were more variable in terms of low concentrations. Ozone and TGM concentrations were positively correlated at some sites (Villeroy, Mingan and St. Anicet) whereas they were not at L'Assomption (closest site to Montreal). Local TGM and ozone precursor sources would affect the correlation.     

Geographical differences of zinc, cadmium, mercury and selenium in polar bears (Ursus maritimus) from Greenland

Muscle, liver, and kidney tissues from 100 polar bears (Ursus maritimus), caught in the Avanersuaq area, north-west Greenland, and Ittoqqortoormiit area, central-east Greenland, were analysed for zinc, cadmium, mercury and selenium. The zinc concentrations in muscle and liver were higher than in kidney. Mean zinc concentrations ranged from 19.7 to 76.0 micrograms/g (all data are presented as geometric means on a wet wt. basis). The presented cadmium concentrations by area and age groups were all low in muscle and in many cases below the detection limit (range: < 0.015-0.048 microgram/g). Cadmium concentrations were intermediate in liver (range: 0.120-1.98 micrograms/g) and highest in kidney tissue (range: 2.16-28.9 micrograms/g). Mercury was likewise lowest in muscle tissue (range: 0.034-0.191 microgram/g). Mercury concentration ranged quite similarly in liver and kidney tissue (liver range: 2.13-22.0 micrograms/g; kidney range: 2.87-32.0 micrograms/g). The selenium concentration increased from muscle (range: < 0.2-0.452 microgram/g) over liver (range: 1.20-9.80 micrograms/g) to kidney (range: 2.34-13.9 micrograms/g). No age accumulation was found for zinc. A weak increase was found for selenium, whereas cadmium and mercury clearly accumulated with age. An exception was mercury concentrations in muscle tissue, where no clear pattern was observed. Polar bears had significantly lower cadmium concentrations than ringed seals from the same area in all three tissues. Likewise mercury was significantly lower in the muscle tissue of polar bears than in ringed seals, whereas liver and kidney concentrations were higher. Biomagnification factors are provided for different tissues and age groups. Tissue ratios are given for different age groups and metals to enable a rough extrapolation from one tissue to another. Tissue ratios for cadmium, selenium and for mercury vary up to a factor of 6 with age. No significant differences could be detected between the elements analysed in bears from two management zones in north-west Greenland. This finding is in agreement with the genetic pattern in the two areas. In central-east Greenland, however, cadmium, selenium, and some of the mercury concentrations in polar bears from the southern area were higher than from the northern area, indicating that the east Greenland area represents two different ecological regions with different polar bear populations. Geographical differences between polar bears from north-west and east Greenland were only found for mercury and cadmium in liver tissue, where the concentrations were highest in bears from north-west Greenland. The geographical trend of increasing cadmium concentrations in polar bear liver tissue from west to east, which has been found previously in Canada, could be extended to cover north-west Greenland as well. East of this region a decrease was found. Mercury concentrations in polar bear liver tissue showed an increase from Svalbard over east and north-west Greenland, peaking in bears from south-west Melville Island. A marked decrease was found west of Melville Island, and the lowest concentrations were found in the Chukchi Sea.     

The delivery of mercury to the Beaufort Sea of the Arctic Ocean by the Mackenzie River

Very high levels of mercury (Hg) have recently been reported in marine mammals and other higher trophic-level biota in the Mackenzie Delta and Beaufort Sea of the western Arctic Ocean. To quantify the input of Hg (particulate, dissolved and methylated) by the Mackenzie River as a potential source for Hg in the ecosystem, surface water and sediment samples were taken from 79 sites in the lower Mackenzie Basin during three consecutive summers (2003-2005) and analyzed for Hg and methylmercury (MeHg). Intensive studies were also carried out in the Mackenzie Delta during the freshets of 2004 and 2005. Large seasonal and annual variations were found in Hg concentrations in the river, coincident with the variations in water discharge. Increased discharges during spring freshet and during the summers of 2003 and 2005 compared to 2004 were mirrored by higher Hg concentrations. The correlation between Hg concentration and riverflow suggests additional Hg sources during periods of high water, potentially from increased surface inundation and increased bank erosion. The increase in the Hg concentration with increasing water discharge amplifies the annual Hg and MeHg fluxes during high water level years. For the period 2003-2005, the Hg and MeHg fluxes from the Mackenzie River to the Beaufort Sea averaged 2.2 tonnes/yr and 15 kg/yr, respectively, the largest known Hg source to the Beaufort Sea. More than half of the mercury flux occurs during the short spring freshet season which coincides with the period of rapid growth of marine biota. Consequently, the Mackenzie River input potentially provides the major mercury source to marine mammals of the Beaufort Sea. The Hg and MeHg fluxes from the Mackenzie River are expected to further increase with the projected climate warming in the Mackenzie Basin.     

Atmospheric monitoring of organic pollutants in the Arctic under the Arctic Monitoring and Assessment Programme (AMAP): 1993-2006

Continuous and comparable atmospheric monitoring programs to study the transport and occurrence of persistent organic pollutants (POPs) in the atmosphere of remote regions is essential to better understand the global movement of these chemicals and to evaluate the effectiveness of international control measures. Key results from four main Arctic research stations, Alert (Canada), Pallas (Finland), Storhofdi (Iceland) and Zeppelin (Svalbard/Norway), where long-term monitoring have been carried out since the early 1990s, are summarized. We have also included a discussion of main results from various Arctic satellite stations in Canada, Russia, US (Alaska) and Greenland which have been operational for shorter time periods. Using the Digital Filtration temporal trend development technique, it was found that while some POPs showed more or less consistent declines during the 1990s, this reduction is less apparent in recent years at some sites. In contrast, polybrominated diphenyl ethers (PBDEs) were still found to be increasing by 2005 at Alert with doubling times of 3.5 years in the case of deca-BDE. Levels and patterns of most POPs in Arctic air are also showing spatial variability, which is typically explained by differences in proximity to suspected key source regions and long-range atmospheric transport potentials. Furthermore, increase in worldwide usage of certain pesticides, e.g. chlorothalonil and quintozene, which are contaminated with hexachlorobenzene (HCB), may result in an increase in Arctic air concentration of HCB. The results combined also indicate that both temporal and spatial patterns of POPs in Arctic air may be affected by various processes driven by climate change, such as reduced ice cover, increasing seawater temperatures and an increase in biomass burning in boreal regions as exemplified by the data from the Zeppelin and Alert stations. Further research and continued air monitoring are needed to better understand these processes and its future impact on the Arctic environment.     

Mercury speciation and exchanges at the air-water interface of a tropical artificial reservoir, French Guiana

The distribution and speciation of mercury (Hg) in air, rain, and surface waters from the artificial tropical lake of Petit-Saut in French Guiana were investigated during the 2003/04 period. In the air, total gaseous mercury (TGM) at the dam station averaged 12+/-2 pmol m(-3) of which >98% was gaseous elemental mercury (GEM). GEM distribution depicted a day-night cycling with high concentrations (up to 15 pmol m(-3)) at dawn and low concentrations (down to 5 pmol m(-3)) at nightfall. Reactive gaseous mercury (RGM) represented <1% of the GEM with a mean concentration of 4+/-3 fmol m(-3). Diel RGM variations were negatively related to GEM. In the rain, the sum of all Hg species in the unfiltered (HgT(UNF)) averaged 16+/-12 pmol L(-1). Temporal distribution of HgT(UNF) exhibited a pattern of high concentrations during the late dry seasons (up to 57.5 pmol L(-1)) and low concentrations (down to 2.7 pmol L(-1)) in the course of the wet seasons. Unfiltered reactive (HgR(UNF)), dissolved gaseous (DGM) and monomethyl (MMHg(UNF)) Hg constituted 20, 5 and 5% of HgT(UNF), respectively. All measured Hg species were positively related and displayed negative relationships with the pH of the rain. In the reservoir surface waters, dissolved total mercury (HgT(D)) averaged 3.4+/-1.2 pmol L(-1) of which 10% consisted of DGM. DGM showed a trend of high concentrations during the dry seasons (480+/-270 fmol L(-1)) and lower (230+/-130 fmol L(-1)) in the course of the wet seasons. Diel variations included diurnal photo-induced DGM production (of about 60 fmol L(-1) h(-1)) coupled to minute to hour oxidation/reduction cycles (of >100 fmol L(-1) amplitude). Finally, calculated atmospheric Hg inputs to the Petit-Saut reservoir represented 14 mol yr(-1) whereas DGM evasion reached 23 mol yr(-1). Apportionment among forms of Hg deposition indicated that up to 75% of the total Hg invasive flux follows the rainfall pathway.     

Methyl mercury production and loss in Arctic soil

Mercury has been found in polar bears and other top predators in the Arctic at concentrations that pose a risk to the indigenous population, however, the means by which this occurs is uncertain. There has been extensive research on the atmospheric cycling of mercury but little is known about mercury cycling in Arctic terrestrial ecosystems. The objective of this study was to determine whether wet sedge meadow soils within the Truelove Lowlands, Devon Island, NT, Canada (75° 33′N, 84° 40′N) were acting as sources or sinks for methylmercury (MeHg). Over the course of an Arctic summer, MeHg concentrations and other biophysical characteristics were measured at four wet sedge meadows over a 19 day study period that commenced approximately 1 month after snowmelt. Soil MeHg concentrations declined during the study period, indicating a net loss of MeHg over the summer. The dominant ligand in solution appeared to be dissolved organic matter, little sulfide was detected, and it would seem that most of the mercury was unavailable for methylation during the summer sampling period. In soil microcosms, spiked with 5.0 nmol g^− 1 (1 µg g^− 1) HgCl₂, the soil did methylate mercury suggesting that there is the potential for mercury methylation. We also noted significant spatial variability in MeHg concentrations between catenas that could not be explained by other biophysical parameters, which are known to affect methylation. Given our data and previous geochemical data collected from suprapermafrost groundwater during snowmelt, it seems likely that methylation may occur during the spring melt period in the arctic. Furthermore the geochemical variability of the melt water may lead to the spatial variability observed in MeHg concentrations in this study.     

Atmospheric concentrations and air-soil gas exchange of polycyclic aromatic hydrocarbons (PAHs) in remote, rural village and urban areas of Beijing-Tianjin region, North China

Forty passive air samplers were deployed to study the occurrence of gas and particulate phase PAHs in remote, rural village and urban areas of Beijing-Tianjin region, North China for four seasons (spring, summer, fall and winter) from 2007 to 2008. The influence of emissions on the spatial distribution pattern of air PAH concentrations was addressed. In addition, the air-soil gas exchange of PAHs was studied using fugacity calculations. The median gaseous and particulate phase PAH concentrations were 222 ng/m³ and 114 ng/m³, respectively, with a median total PAH concentration of 349 ng/m³. Higher PAH concentrations were measured in winter than in other seasons. Air PAH concentrations measured at the rural villages and urban sites in the northern mountain region were significantly lower than those measured at sites in the southern plain during all seasons. However, there was no significant difference in PAH concentrations between the rural villages and urban sites in the northern and southern areas. This urban-rural PAH distribution pattern was related to the location of PAH emission sources and the population distribution. The location of PAH emission sources explained 56%-77% of the spatial variation in ambient air PAH concentrations. The annual median air-soil gas exchange flux of PAHs was 42.2 ng/m²/day from soil to air. Among the 15 PAHs measured, acenaphthylene (ACY) and acenaphthene (ACE) contributed to more than half of the total exchange flux. Furthermore, the air-soil gas exchange fluxes of PAHs at the urban sites were higher than those at the remote and rural sites. In summer, more gaseous PAHs volatilized from soil to air because of higher temperatures and increased rainfall. However, in winter, more gaseous PAHs deposited from air to soil due to higher PAH emissions and lower temperatures. The soil TOC concentration had no significant influence on the air-soil gas exchange of PAHs.     

Mercury in muscle tissue of lesser-spotted dogfish (Scyliorhinus caniculus L.) from the north-east Irish Sea.

This paper reports concentrations of mercury in muscle tissue of lesser-spotted dogfish (Scyliorhinus caniculus L.) from various locations within Liverpool Bay and the north-east Irish Sea. Concentrations of mercury in fish muscle showed distinct spatial variation, with values from the northern sectors of the Irish Sea significantly lower than those for the southern area, particularly sites in Liverpool Bay and around the mouth of the Mersey Estuary. The data support the hypothesis that there are several major populations of lesser-spotted dogfish within the study area, each of which remains quite distinct during seasonal movements. Consequently, exposure to environmental mercury is reflected in muscle concentrations of mercury. Regressions of mercury concentration against fish length showed significant relationships for the majority of sites, with the slope relating to distance from known sources of mercury contamination. Mean mercury concentrations were higher than in corresponding populations of flatfish from the same areas.     

Developing consensus: mercury science and policy in the NAFTA countries (Canada, the United States and Mexico)

The international science community has recognized methylmercury in the aquatic food chain, as a potential environmental and human health risk. As a result, countries around the world have implemented a number of mercury management initiatives. The United States, Mexico and Canada in consultation with stakeholders are developing a trilateral North American Regional Action Plan (NARAP) on mercury. Through public involvement in the decision making process, the NARAP has offered opportunities for more transparency in transactions between governments, industry and stakeholders. In spite of the available scientific information, there are still important uncertainties associated with the mercury issue. These knowledge gaps include: the most appropriate methylmercury reference dose for sensitive groups; the percentage of the North American population that is at risk from methylmercury exposure; spatial and temporal mercury deposition patterns in each country; the link between mercury emissions, atmospheric deposition and methylmercury concentrations in fish; and the relative magnitude of contributions from natural and anthropogenic sources.     

Distribution of total and methyl mercury in sediments along Steamboat Creek (Nevada, USA)

In the late 1800s, mills in the Washoe Lake area, Nevada, used elemental mercury to remove gold and silver from the ores of the Comstock deposit. Since that time, mercury contaminated waste has been distributed from Washoe Lake, down Steamboat Creek, and to the Truckee River. The creek has high mercury concentrations in both water and sediments, and continues to be a constant source of mercury to the Truckee River. The objective of this study was to determine concentrations of total and methyl mercury (MeHg) in surface sediments and characterize their spatial distribution in the Steamboat Creek watershed. Total mercury concentrations measured in channel and bank sediments did not decrease downstream, indicating that mercury contamination has been distributed along the creek's length. Total mercury concentrations in sediments (0.01-21.43 microg/g) were one to two orders of magnitude higher than those in pristine systems. At 14 out of 17 sites, MeHg concentrations in streambank sediments were higher than the concentrations in the channel, suggesting that low banks with wet sediments might be important sites of mercury methylation in this system. Both pond/wetland and channel sites exhibited high potential for mercury methylation (6.4-30.0 ng g(-1) day(-1)). Potential methylation rates were positively correlated with sulfate reduction rates, and decreased as a function of reduced sulfur and MeHg concentration in the sediments. Potential demethylation rate appeared not to be influenced by MeHg concentration, sulfur chemistry, DOC, sediment grain size or other parameters, and showed little variation across the sites (3.7-7.4 ng g(-1) day(-1)).     

Total gaseous mercury in the atmosphere of Guiyang,PR China

Four measurement campaigns were carried out to monitor total gaseous mercury (TGM) at one site in the Guiyang City, PR China in the following periods: April 19-30, 2000; February 26-March 14, 2001; June 26-July 20, 2001; and October 9-November 22, 2001, respectively. High temporal resolved data were obtained by using automated mercury analyzers Gardis 1A and Tekran 2537A. TGM data from all measurement periods followed the typical log normal distribution pattern. The geometric mean of TGM from different seasons were 8.56, 7.45, 5.20 and 8.33 ngm(-3) in spring 2000, winter 2001, summer 2001 and autumn 2001, respectively. The overall average TGM covering the sampling periods was 7.39 ngm(-3), which is significantly elevated comparing to global background of approximately 1.5-2.0 ngm(-3). The major anthropogenic atmospheric mercury emission sources differed significantly among seasons, which caused the seasonal variability of TGM level. Distinct daily variability of TGM was observed among seasons. The daytime TGM concentrations were larger than that of nighttime in spring and winter seasons, while in summer and autumn the opposite daily TGM distribution pattern was observed.     

Temporal and spatial trends of mercury in fish collected in the English-Wabigoon river system in Ontario, Canada

The First Nations communities of Grassy Narrows and Wabaseemong (Ontario, Canada) have been impacted by mercury pollution since the 1960s. This study was implemented with the objective of providing these communities with information on current mercury concentrations in their catch, in order to make appropriate fish consumption choices. A total of 851 fish samples, including Walleye, Northern Pike, Large-mouth Bass, and Whitefish, were collected from thirteen lakes and rivers. Total mercury was measured and the relationship between fish length, mercury concentration, and lake of origin were assessed. It was found that fish from most of the lakes exhibit a positive relationship between length and mercury accumulation. Mercury concentrations in fish collected from Clay Lake, closest to the original source of contamination, are higher than those from other lakes. Mercury concentrations have declined over the last 25 years but the gradient of contamination was still observed. Results were communicated to the communities for public health purposes.     

Atmospheric mercury depletion event study in Ny-Alesund (Svalbard) in spring 2005. Deposition and transformation of Hg in surface snow during springtime

A field campaign was conducted in Ny-Alesund (78 degrees 54'N, 11 degrees 53'E), Svalbard (Norway) during April and May 2005. An Atmospheric Mercury (Hg) Depletion Event (AMDE) was observed from the morning of April 24 until the evening of April 27. Transport of already Hg and ozone (O3) depleted air masses could explain this observed depletion. Due to a snowfall event during the AMDE, surface snow Hg concentrations increased two fold. Hg deposition took place over a short period of time corresponding to 3-4 days. More than 80% of the deposited Hg was estimated to be reemitted back to the atmosphere in the days following the event. During the campaign, we observed night and day variations in surface snow Hg concentrations, which may be the result of gaseous elemental mercury (GEM) oxidation to divalent Hg at the snow/air interface by daylight surface snow chemistry. Finally, a decrease in the reactive Hg (HgR) fraction of total Hg (HgT) in the surface snow was observed during spring. We postulate that the transformation of HgR to a more stable form may occur in Arctic snow during spring.     

Seasonal, interannual, and long-term variation in sport fish contamination, San Francisco Bay

This study documents changes in contamination over time at seasonal, interannual, and decadal time scales for sport fish collected in San Francisco Bay. Samples from seven fish species were prepared according to common consumption practices (muscle fillets either with or without skin) and analyzed for trace metals (mercury and selenium) and trace organochlorine contaminants (PCBs, DDTs, chlordanes, and dieldrin). In 2000, sport fish samples exceeded human health screening values for mercury, PCBs, DDTs, selenium, and dieldrin but did not exceed screening values for chlordanes. On a seasonal time scale, white croaker (Genyonemus lineatus) exhibited significantly lower PCB and lipid concentrations in spring, and a general increase in concentrations in other seasons. When monitoring data were compared among 1994, 1997, and 2000, analysis of variance indicated that concentrations of mercury, PCBs, DDTs, and chlordanes varied significantly among years for several fish species. Interannual variation in DDTs often correlated to changes in sampled fish size or lipid content among years. Interannual variation in mercury and PCBs was evident in striped bass (Morone saxatilis) but absent in shiner surfperch (Cymatogaster aggregata), leopard shark (Triakis semifasciata), and white croaker. The higher interannual variability of striped bass contaminant concentrations may result from migratory behavior and wide home ranges. Chlordanes significantly declined between 1994 and 2000 in white croaker and striped bass. Of the historical data analyzed (1986-2000), only DDT concentrations in white sturgeon (Acipenser transmontanus) showed evidence of a significant decline. Neither PCBs nor selenium showed evidence of a trend in white sturgeon. Between 1970 and 2000, mercury concentrations in striped bass showed no evidence of a trend. The absence of recent trends in mercury may result from the presence of widespread and historic sources, with use reductions occurring in the early 20th century. In contrast to mercury, apparent recent declines in fish tissue DDT and chlordane concentrations may result from use curtailment in the 1970s and 1980s.     

Fine-scale mercury trends in temperate deciduous tree leaves from Ontario, Canada

This study focused on the value of deciduous leaves as biomonitors of total mercury (THg). Leaf samples were collected from a range of deciduous species from five sampling sites in the province of Ontario, Canada. These included a site in the northwest (the Experimental Lakes Area, ELA), two sites in central Ontario (the town of Dorset and the Centre for Atmospheric Research Experiments, CARE), and two sites in the southeast (Sandbanks Provincial Park, SBPP and the City of Kingston). The sampled species exhibited distinctive species-specific differences with red oaks consistently having lower leaf THg concentrations than all maple species, while black and white ash leaves had the highest concentrations. Spatially, leaves collected across the distance between ELA and SBPP (~ 1500 km apart) had overlapping THg concentrations between 20 and 40 ng/g. Unexpectedly, leaves from urban parks of Kingston had considerably lower THg concentrations (< 25 ng/g) than the other sites, which suggested leaves may not reflect subtle gradients of atmospheric THg found under field conditions. Leaf THg increased with the growing season, with highest THg leaf concentrations found in early autumn just before senescence. Microspatial differences within a single tree, such as position on a branch are important, since higher mercury concentrations were associated with leaves positioned deeper into the canopy relative to outer leaves more exposed to wind turbulence and sunlight. Within any single leaf, THg concentrations were highest in the leaf tissue, and consistently distributed, while the vein and petiole tissue had lower THg concentrations. There was no relationship between THg concentrations and leaf area. Using deciduous tree leaves as regional temporal monitors of bioavailable mercury may be feasible, but careful selection of leaf sampling sites on the tree itself and the timing is of utmost importance for ensuring consistent and high quality biomonitoring data.     

Effects of forest cover and topographic factors on TOC and associated metals at various scales in western Scotland

Studies at the stream catchment scale have yielded inconclusive evidence of the effects of forest land use on the concentrations of organic carbon in drainage waters. The aim of this paper is to examine the effects of forests on carbon in drainage waters at the plot scale by comparing concentrations of total organic carbon (TOC) and associated metals in soil solutions from sites under forest and moorland vegetation. At an upland site in south-west Scotland soil solution TOC, aluminium and iron concentrations varied with land cover. Mean concentrations of all three determinands were at least 1.5 times greater under forest than under moorland, despite considerable spatial and temporal (seasonal) variability. TOC in soil solutions was also found to vary significantly with both relief and altitude. The altitude effect was particularly marked, with an increase of 26 mg x l(-1) x 100 m(-1) increase in altitude found at an upland site in west-central Scotland. There were no differences in chloride, sulphate or base cation concentrations between forest and moorland sites. Differences in aluminium concentrations could not be linked to atmospheric scavenging at the forest sites, but were closely linked to differences in TOC.     

Study of atmospheric mercury budget in East Asia using STEM-Hg modeling system

East Asia is the largest source region of global anthropogenic mercury emissions, and contributes to atmospheric mercury concentration and deposition in other regions. Similarly, mercury from the global pool also plays a role in the chemical transport of mercury in East Asia. Annual simulations of atmospheric mercury in East Asia were performed using the STEM-Hg modeling system to study the mass budgets of mercury in the region. The model results showed strong seasonal variation in mercury concentration and deposition, with signals from large point sources. The annual mean concentrations for gaseous elemental mercury, reactive gaseous mercury and particulate mercury in central China and eastern coastal areas were 1.8 ng m^− 3, 100 pg m^− 3 and 150 pg m^− 3, respectively. Boundary conditions had a strong influence on the simulated mercury concentration and deposition, contributing to 80% of the concentration and 70% of the deposition predicted by the model. The rest was caused by the regional emissions before they were transported out of the model domain. Using different oxidation rates reported for the Hg⁰-O₃ reaction (i.e., by Hall, 1995 vs. by Pal and Ariya, 2004) led to a 9% difference in the predicted mean concentration and a 40% difference in the predicted mean deposition. The estimated annual dry and wet deposition for East Asia in 2001 was in the range of 590-735 Mg and 482-696 Mg, respectively. The mercury mass outflow caused by the emissions in the domain was estimated to be 681-714 Mg yr^− 1. This constituted 70% of the total mercury emission in the domain. The greatest outflow occurred in spring and early summer.