Mercury transport between sediments and the overlying water of the St. Lawrence River area of concern near Cornwall, Ontario

Contaminated sediments in the St. Lawrence River remain a difficult problem despite decreases in emissions. Here, sediment and pore water phases were analyzed for total mercury (THg) and methyl mercury (MeHg) and diffusion from the sediment to the overlying water was 17.5 ± 10.6 SE ng cm⁻² yr⁻¹ for THg and 3.8 ± 1.7 SE ng cm⁻² yr⁻¹ for MeHg. These fluxes were very small when compared to the particle-bound mercury flux accumulating in the sediment (183 ± 30 SE ng cm⁻² yr⁻¹). Studies have reported that fish from the westernmost site have higher Hg concentrations than fish collected from the other two sites of the Cornwall Area of Concern, which could not be explained by differences in the Hg flux or THg concentrations in sediments, but the highest concentrations of sediment MeHg, and the greatest proportions of MeHg to THg in both sediment and pore water were observed where fish had highest MeHg concentrations.     

Elevated atmospheric deposition and dynamics of mercury in a remote upland forest of southwestern China

Mt. Gongga area in southwest China was impacted by Hg emissions from industrial activities and coal combustion, and annual means of atmospheric TGM and PHg concentrations at a regional background station were 3.98 ng m⁻³ and 30.7 pg m⁻³, respectively. This work presents a mass balance study of Hg in an upland forest in this area. Atmospheric deposition was highly elevated in the study area, with the annual mean THg deposition flux of 92.5 μg m⁻² yr⁻¹. Total deposition was dominated by dry deposition (71.8%), and wet deposition accounted for the remaining 28.2%. Forest was a large pool of atmospheric Hg, and nearly 76% of the atmospheric input was stored in forest soil. Volatilization and stream outflow were identified as the two major pathways for THg losses from the forest, which yielded mean output fluxes of 14.0 and 8.6 μg m⁻² yr⁻¹, respectively.     

Reduced mercury deposition in New Hampshire from 1996 to 2002 due to changes in local sources

Changes in deposition of gaseous divalent mercury (Hg(II)) and particulate mercury (Hg(p)) in New Hampshire due to changes in local sources from 1996 to 2002 were assessed using the Industrial Source Complex Short Term (ISCST3) model (regional and global sources and Hg atmospheric reactions were not considered). Mercury (Hg) emissions in New Hampshire and adjacent areas decreased significantly (from 1540 to 880 kg yr⁻¹) during this period, and the average annual modeled deposition of total Hg also declined from 17 to 7.0 μg m⁻² yr⁻¹ for the same period. In 2002, the maximum amount of Hg deposition was modeled to be in southern New Hampshire, while for 1996 the maximum deposition occurred farther north and east. The ISCST3 was also used to evaluate two future scenarios. The average percent difference in deposition across all cells was 5% for the 50% reduction scenario and 9% for the 90% reduction scenario.     

Sedimentary record of PAHs in the Liangtan River and its relation to socioeconomic development of Chongqing, Southwest China

Concentrations of polycyclic aromatic hydrocarbons (PAHs) were detected in sediment cores and surface sediment samples from the Liangtan River of Chongqing, Southwest China. The total concentration of 16 PAHs ranged from 69 to 6251 ng g⁻¹. The spatial distribution of the PAHs reflects the intensity and scope of human activity in the catchment. A historical record of PAH contamination was reconstructed using a sediment core from a background segment of the river. The characteristic changes of concentrations, fluxes and patterns of 16 PAHs over the past ∼90 years were captured in detail. An obvious peak of PAH concentration and flux was found in the 1940s, i.e., during war time, and then a sharp increase was observed from the early 1980s to the present. The maximum concentration and flux reached 1260 ng g⁻¹ and 470 ng cm⁻² year⁻¹, respectively. The sharp increase was attributed to the contribution of pyrogenic sources of PAHs. The population, length of highways and energy consumption of Chongqing, as indexes of socioeconomic development, were positively correlated with PAH input in the sediment core from the 1950s to the present. The results clearly show that the local socioeconomic development in the last decades remarkably aggravated the environmental load of sedimentary PAHs.     

Polycyclic aromatic hydrocarbons in urban soils of Beijing: status, sources, distribution and potential risk

We studied the source, concentration, spatial distribution and health risk of 16 polycyclic aromatic hydrocarbons (PAHs) in urban soils of Beijing. The total mass concentration of 16 PAHs ranged from 93 to 13 141 μg kg⁻¹ with a mean of 1228 μg kg⁻¹. The contour map of soil PAH concentrations showed that the industrial zone, the historical Hutong district and the university district of Beijing have significantly higher concentrations than those in remainder of the city. The results of sources identification suggested that the primary sources of PAHs were vehicle exhaust and coal combustion and the secondary source was the atmospheric deposition of long-range transported PAHs. The incremental lifetime cancer risks (ILCRs) of exposing to PAHs in the urban soils of Beijing for adult were 1.77 × 10⁻⁶ and 2.48 × 10⁻⁵, respectively under normal and extreme conditions. For child, they were 8.87 × 10⁻⁷ and 6.72 × 10⁻⁶, respectively under normal and extreme conditions.     

Mercury deposition/accumulation rates in the vicinity of a lead smelter as recorded by a peat deposit

Mercury (Hg) concentration profiles and historical accumulation rates were determined in three ²¹⁰Pb-dated cores from a peat deposit in the vicinity of a lead (Pb) smelter at Příbram, Czech Republic. The Hg concentrations in peat samples ranged from 66 to 701 μg kg⁻¹. Cumulative Hg inventories from each core (for the past 150 yr) varied by a factor of 1.4 (13.6–18.5 mg Hg m⁻²), indicating variations of net Hg accumulation rate within the peat deposit. Historical changes in vegetation cover (leading to variable interception by trees) are probably responsible for this variation in space and time. The uncorrected Hg accumulation rates peaked between the 1960s and 1980s (up to 226 μg m⁻² yr⁻¹). Recent findings show that Hg records from peat tend to overestimate historical levels of Hg deposition. Therefore we used the mass loss compensation factor (MLCF) to normalize Hg accumulation rates. These corrected Hg accumulation rates were significantly lower (maximum 129 μg m⁻² yr⁻¹) and better corresponded to changes in historical smelter emissions, which were highest in the 1960s. The agreement between the corrected Hg accumulation rates in the uppermost peat sections (2–38 μg m⁻² yr⁻¹) and biomonitoring of atmospheric deposition by mosses in several recent years (4.7–34.4 μg m⁻² yr⁻¹) shows the usefulness of MLCF application on Hg accumulation in peat archives. However, the MLCF correction was unsuitable for Pb. The recent Pb deposition rates obtained by an independent biomonitoring study using mosses (0.5–127 mg m⁻² yr⁻¹) were better correlated with net Pb accumulation rates recorded in peat (7–145 mg m⁻² yr⁻¹) than with corrected rates obtained by the MLCF approach (1–28 mg m⁻² yr⁻¹).     

Atmospheric distribution of polycyclic aromatic hydrocarbons and deposition to Galveston Bay,Texas, USA

Estimates of the atmospheric deposition to Galveston Bay of polycyclic aromatic hydrocarbons (PAHs) are made using precipitation and meteorological data that were collected continuously from 2 February 1995 to 6 August 1996 at Seabrook, TX, USA. Particulate and vapor phase PAHs in ambient air and particulate and dissolved phases in rain samples were collected and analyzed. More than 95% of atmospheric PAHs were in the vapor phase and about 73% of PAHs in the rain were in the dissolved phase. Phenanthrene and napthalene were the dominant compounds in air vapor and rain dissolved phases, respectively, while 5 and 6 ring PAH were predominant in the particulate phase of both air and rain samples. Total PAH concentrations ranged from 4 to 161 ng m⁻³ in air samples and from 50 to 312 ng l⁻¹ in rain samples. Temporal variability in total PAH air concentrations were observed, with lower concentrations in the spring and fall (4–34 ng m ⁻³) compared to the summer and winter (37–161 ng m⁻³). PAHs in the air near Galveston Bay are derived from both combustion and petroleum vaporization. Gas exchange from the atmosphere to the surface water is estimated to be the major deposition process for PAHs (1211 μg m^{− 2} yr^{− 1}), relative to wet deposition (130 μg m⁻² yr^{− 1}) and dry deposition (99 μg m⁻² yr^{− 1}). Annual deposition of PAHs directly to Galveston Bay from the atmosphere is estimated as 2  t yr⁻¹.     

Mercury mass balance study in Wujiangdu and Dongfeng Reservoirs, Guizhou, China

From October 2003 to September 2004, we conducted a detailed study on the mass balance of total mercury (THg) and methylmercury (MeHg) of Dongfeng (DF) and Wujiangdu (WJD) reservoirs, which were constructed in 1992 and 1979, respectively. Both reservoirs were net sinks for THg on an annual scale, absorbing 3319.5 g km⁻² for DF Reservoir, and 489.2 g km⁻² for WJD Reservoirs, respectively. However, both reservoirs were net sources of MeHg to the downstream ecosystems. DF Reservoir provided a source of 32.9 g MeHg km⁻² yr⁻¹, yielding 10.3% of the amount of MeHg that entered the reservoir, and WJD Reservoir provided 140.9 g MeHg km⁻² yr⁻¹, yielding 82.5% of MeHg inputs. Our results implied that water residence time is an important variable affecting Hg methylation rate in the reservoirs. Our study shows that building a series of reservoirs in line along a river changes the riverine system into a natural Hg methylation factory which markedly increases the %MeHg in the downstream reservoirs; in effect magnifying the MeHg buildup problem in reservoirs.     

Levels,sources, and health risk assessment of polycyclic aromatic hydrocarbons in Brno,Czech Republic: a 5-year study

This work aimed to determine the seasonal variations of polycyclic aromatic hydrocarbons (PAHs) in airborne PM₁₀ at two background sites (Masná—MS, Líšeň—LN) in Brno over a 5-year period (2009–2013). Samples were collected on quartz filters using a low-volume sampler by continual filtration. Concentrations of PAHs in collected PM₁₀ samples were determined using a gas chromatography with a mass spectrometer as a detector. A different number of PAHs were determined to be at each site, i.e., 11 PAHs at the MS site and six PAHs at the LN site, and similarities between them were identified using non-parametric analysis of variance. Potential sources were identified using principal component analysis (PCA) and PAHs diagnostic ratios. The work also focused on health risk assessment. This was estimated using toxic equivalent factors to calculate individual lifetime cancer risk, which quantifies risk of exposure to PAHs for specific age groups. The average 11-PAH concentrations in M|S site annually ranged from 19.28 ± 19.02 ng m⁻³ (2011) to 40.37 ± 21.35 ng m⁻³ (2013). With regard to the LN site, the average six-PAH concentrations annually ranged from 3.64 ± 3.87 ng m⁻³ (2009) and 5.27 ± 6.19 ng m⁻³ (2012). PCA and diagnostic ratios indicate the main sources to be traffic emissions and coal combustion. Health risk assessment showed carcinogenic risk under limit value in all cases.

     

Distribution of PAHs in tissues of wetland plants and the surrounding sediments in the Chongming wetland, Shanghai, China

Polycyclic aromatic hydrocarbons (PAHs) concentrations were determined in sediments and three types of wetland plants collected from the intertidal flats in the Chongming wetland. The concentration of total PAHs in sediments ranged from 38.7 to 136.2 ng g⁻¹. Surface sediment concentrations were higher in regions with plant cover than in bare regions. Rhizome-layer sediments (56.8-102.4 ng g⁻¹) contained less PAHs than surface sediments (0-5 cm). Concentrations of PAHs in plant tissues ranged from 51.9 to 181.2 ng g⁻¹, with highest concentrations in the leaves of Scirpus. Most of the PAHs in the leaves and other plant tissues were low molecular weight compounds (LMW, 2-4 rings), and a similar distribution pattern of PAHs in different types of plants was also observed. Source analysis indicated that plants and sediments both came from pyrogenic sources, but plants had additional petroleum contamination. The low ratio of benzo[a]anthracene over chrysene suggests that the wetland PAHs came mainly from long-distance atmospheric transportation. Significant bioaccumulation of PAHs from the sediments into plants was not observed for high molecular weight PAHs (HMW, 5-6 rings) in Chongming wetland. The small RCFs (root concentration factor from sediments) for HMW PAHs and large RCFs for LMW PAHs suggested that roots accumulated LMW PAHs selectively from sediments in Chongming wetland.     

Historical deposition of mercury and selected trace elements to high-elevation National Parks in the Western U.S. inferred from lake-sediment cores

Atmospheric deposition of Hg and selected trace elements was reconstructed over the past 150 years using sediment cores collected from nine remote, high-elevation lakes in Rocky Mountain National Park in Colorado and Glacier National Park in Montana. Cores were age dated by ²¹⁰Pb, and sedimentation rates were determined using the constant rate of supply model. Hg concentrations in most of the cores began to increase around 1900, reaching a peak sometime after 1980. Other trace elements, particularly Pb and Cd, showed similar post-industrial increases in lake sediments, confirming that anthropogenic contaminants are reaching remote areas of the Rocky Mountains via atmospheric transport and deposition. Preindustrial (pre-1875) Hg fluxes in the sediment ranged from 5.7 to 42 μg m^?2 yr^?1 and modern (post-1985) fluxes ranged from 17.7 to 141 μg m^?2 yr^?1. The average ratio of modern to preindustrial fluxes was 3.2, which is similar to remote lakes elsewhere in North America. Estimates of net atmospheric deposition based on the cores were 3.1 μg m^?2 yr^?1 for preindustrial and 11.7 μg m^?2 yr^?1 for modern times. Current-day measurements of wet deposition range from 5.0 to 8.6 μg m^?2 yr^?1, which are lower than the modern sediment-based estimate of 11.7 μg m^?2 yr^?1, perhaps owing to inputs of dry-deposited Hg to the lakes.     

Polybrominated diphenyl ethers occurrence in major inflowing rivers of Lake Chaohu (China): Characteristics,potential sources and inputs to lake

Eight commonly occurring polybrominated diphenyl ethers (PBDEs), including BDE 28, 47, 99, 100, 153, 154, 183, 207, and 209, were investigated in water samples from seven major inflowing rivers of Lake Chaohu to determine the distribution characteristics, potential sources and inputs to the lake. The sum of 8 BDE congeners (Σ₈PBDEs) had a concentration varied from 0.31 to 84 ng L⁻¹, with those of BDE 209, BDE 47, BDE 99, and BDE 153 being 0.31–83, <0.012–0.36, <0.012–1.3, and <0.012–0.77 ng L⁻¹, respectively. These levels were in the high range of the global PBDEs concentrations in the water environments. The highest concentrations of Σ₈PBDEs were detected in the western rivers, of which the main pollution sources were strongly related to human activities in urban centers, such as automobile-derived wastes. A sewage treatment plant was likely an important source of the lower brominated BDEs input to one western river. The correlation analyses (all p < 0.05) between PBDEs and DOC, TN, TP, and EC, suggested that the distributions and sources of PBDEs in rivers might also be related with the soil erosion by heave floods. Σ₈PBDEs input to Lake Chaohu from the rivers outlets was estimated at 344 kg yr⁻¹ during the flood season. BDE 209 was the dominant contributor with an input of 340 kg yr⁻¹, followed by BDE 99 (1.3 kg yr⁻¹), BDE 47 (0.83 kg yr⁻¹) and BDE 153 (0.60 kg yr⁻¹).     

Persistent organic pollutants in plastic marine debris found on beaches in San Diego, California

Plastic debris were collected from eight beaches around San Diego County, California. Debris collected include: pre-production pellets and post-consumer plastics including fragments, polystyrene (PS) foam, and rubber. A total of n = 2453 pieces were collected ranging from <5 mm to 50 mm in size. The plastic pieces were separated by type, location, and appearance and analyzed for polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs), dichlorodiphenyltrichloroethane (DDT) and its breakdown products, and chlordanes. PAH concentrations ranged from 30 ng g⁻¹ to 1900 ng g⁻¹, PCBs from non-detect to 47 ng g⁻¹, chlordanes from 1.8 ng g⁻¹ to 60 ng g⁻¹, and DDTs from non-detect to 76 ng g⁻¹. Consistently higher PAH concentrations found in PS foam samples (300-1900 ng g⁻¹) led us to examine unexposed PS foam packaging materials and PS virgin pellets. Unexposed PS foam contained higher concentrations of PAHs (240-1700 ng g⁻¹) than PS virgin pellets (12-15 ng g⁻¹), suggesting that PAHs may be produced during manufacturing. Temporal trends of debris were investigated at one site, Ocean Beach, where storm events and beach maintenance were found to be important variables influencing debris present at a given time.     

Seasonal variability in gaseous mercury fluxes measured in a high-elevation meadow

Seasonal patterns of atmospheric mercury (Hg) fluxes measured over vegetated terrestrial systems can provide insight into the underlying process controlling emission and deposition of Hg to vegetated surfaces. Gaseous elemental Hg fluxes were measured for week-long periods in each season (spring, summer, fall, and winter) over an uncontaminated high-elevation wetland meadow in Shenandoah National Park, Virginia using micrometeorological methods. Mean net deposition was observed in the spring (?4.8 ng m^?2 h^?1), emission in the summer (2.5 ng m^?2 h^?1), near zero flux in the fall (0.3 ng m^?2 h^?1), and emission in the winter (4.1 ng m^?2 h^?1). Nighttime deposition (when stomata are closed) and the poor correlation between Hg fluxes and canopy conductance during periods of active vegetation growth suggest that stomatal processes are not the dominant mechanism for ecosystem-level GEM exchange at this site. The strong springtime deposition relative to summer implies that young vegetation is better at scavenging Hg, with the highest deposition occurring at night possibly via a cuticular pathway. These results suggest that spring is a period of GEM deposition while other seasons exhibit net emission, emphasizing the importance of capturing GEM flux seasonality when determining total Hg budgets.     

Atmospheric particle characterization, distribution, and deposition in Xi'an, Shaanxi Province, Central China

Physical characterization and chemical analysis of settled dusts collected in Xi’an from November 2007 to December 2008 show that (1) dust deposition rates ranged from 14.6 to 350.4 g m⁻² yr⁻¹. The average deposition rate (76.7 g m⁻² yr⁻¹) ranks the 11th out of 56 dust deposition rates observed throughout the world. The coal-burning power was the major particle source; (2) on average (except site 4), ∼10% of the settled dusts having size <2.6, ∼30% having size <10.5, and >70% having size <30 μm; (3) the concentrations for 20 out of 27 elements analyzed were upto 18 times higher than their soil background values in China. With such high deposition rates of dusts that contain elevated levels of toxic elements, actions should be taken to reduce emission and studies are needed to assess the potential impacts of settled particles on surface ecosystem, water resource, and human health in the area.     

Wet deposition of poly- and perfluorinated compounds in Northern Germany

Twenty precipitation samples were taken concurrently with air samples at a northern German monitoring site over a period of 7 months in 2007 and 2008. Thirty four poly- and perfluorinated compounds (PFC) were determined in rain water samples by solid phase extraction and HPLC-MS/MS analysis. Seventeen compounds were detected in rain water with ΣPFC concentrations ranging from 1.6 ng L⁻¹ to 48.6 ng L⁻¹. Perfluorooctanoate (PFOA) and perfluorobutanate (PFBA) were the compounds that were usually observed in highest concentrations. Calculated ΣPFC deposition rates were between 2 and 91 ng m⁻² d⁻¹. These findings indicate that particle phase PFC are deposited from the atmosphere by precipitation. A relationship between PFC wet deposition and air concentration may be established via precipitation amounts. Trajectory analysis revealed that PFC concentration and deposition estimates in precipitation can only be explained if a detailed air mass history is considered.     

Oxygen-containing polycyclic aromatic hydrocarbons (OPAHs) in urban soils of Bratislava, Slovakia: patterns, relation to PAHs and vertical distribution

We determined concentrations, sources, and vertical distribution of OPAHs and PAHs in soils of Bratislava. The ∑14 OPAHs concentrations in surface soil horizons ranged 88-2692 ng g⁻¹ and those of ∑34 PAHs 842-244,870 ng g⁻¹. The concentrations of the ∑9 carbonyl-OPAHs (r = 0.92, p = 0.0001) and the ∑5 hydroxyl-OPAHs (r = 0.73, p = 0.01) correlated significantly with ∑34 PAHs concentrations indicating the close association of OPAHs with parent-PAHs. OPAHs were quantitatively dominated by 9-fluorenone, 9,10-anthraquinone, 1-indanone and benzo[a]anthracene-7,12-dione. At several sites, individual carbonyl-OPAHs had higher concentrations than parent PAHs. The concentration ratios of several OPAHs to their parent-PAHs and contribution of the more soluble OPAHs (1-indanone and 9-fluorenone) to ∑14 OPAHs concentrations increased with soil depth suggesting that OPAHs were faster vertically transported in the study soils by leaching than PAHs which was supported by the correlation of subsoil:surface soil ratios of OPAH concentrations at several sites with K_OW.     

Organochlorine pesticides in soils of Mexico and the potential for soil-air exchange

The spatial distribution of organochlorine pesticides (OCs) in soils and their potential for soil-air exchange was examined. The most prominent OCs were the DDTs (Geometric Mean, GM = 1.6 ng g⁻¹), endosulfans (0.16 ng g⁻¹), and toxaphenes (0.64 ng g⁻¹). DDTs in soils of southern Mexico showed fresher signatures with higher F_DDTe = p,p′-DDT/(p,p′-DDT + p,p′-DDE) and more racemic o,p′-DDT, while the signatures in the central and northern part of Mexico were more indicative of aged residues. Soil-air fugacity fractions showed that some soils are net recipients of DDTs from the atmosphere, while other soils are net sources. Toxaphene profiles in soils and air showed depletion of Parlar 39 and 42 which suggests that soil is the source to the atmosphere. Endosulfan was undergoing net deposition at most sites as it is a currently used pesticide. Other OCs showed wide variability in fugacity, suggesting a mix of net deposition and volatilization.     

Local to regional emission sources affecting mercury fluxes to New York lakes

Lake-sediment records across the Northern Hemisphere show increases in atmospheric deposition of anthropogenic mercury (Hg) over the last 150 years. Most of the previous studies have examined remote lakes affected by the global atmospheric Hg reservoir. In this study, we present Hg flux records from lakes in an urban/suburban setting of central New York affected also by local and regional emissions. Sediment cores were collected from the Otisco and Skaneateles lakes from the Finger Lakes region, Cross Lake, a hypereutrophic lake on the Seneca River, and Glacial Lake, a small seepage lake with a watershed that corresponds with the lake area. Sediment accumulation rates and dates were established by ²¹⁰Pb. The pre-anthropogenic regional atmospheric Hg flux was estimated to be 3.0 μg m⁻² yr⁻¹ from Glacial Lake, which receives exclusively direct atmospheric deposition. Mercury fluxes peaked during 1971–2001, and were 3 to more than 30 times greater than pre-industrial deposition. Land use change and urbanization in the Otisco and Cross watersheds during the last century likely enhanced sediment loads and Hg fluxes to the lakes. Skaneateles and Glacial lakes have low sediment accumulation rates, and thus are excellent indicators for atmospheric Hg deposition. In these lakes, we found strong correlations with emission records for the Great Lakes region that markedly increased in the early 1900s, and peaked during WWII and in the early 1970s. Declines in modern Hg fluxes are generally evident in the core records. However, the decrease in sediment Hg flux at Glacial Lake was interrupted and has increased since the early 1990s probably due to the operation of new local emission sources. Assuming the global Hg reservoir tripled since the pre-industrial period, the contribution of local and regional emission sources to central New York lakes was estimated to about 80% of the total atmospheric Hg deposition.     

Spatial distribution and seasonal variation of atmospheric bulk deposition of polycyclic aromatic hydrocarbons in Beijing-Tianjin region, North China

Bulk deposition samples were collected in remote, rural village and urban areas of Beijing-Tianjin region, North China in spring, summer, fall and winter from 2007 to 2008. The annually averaged PAHs concentration and deposition flux were 11.81 ± 4.61 μg/g and 5.2 ± 3.89 μg/m²/day respectively. PHE and FLA had the highest deposition flux, accounting for 35.3% and 20.7% of total deposition flux, respectively. More exposure risk from deposition existed in the fall for the local inhabitants. In addition, the PAHs deposition flux in rural villages (3.91 μg/m²/day) and urban areas (8.28 μg/m²/day) was 3.8 and 9.1 times higher than in background area (0.82 μg/m²/day), respectively. This spatial variation of deposition fluxes of PAHs was related to the PAHs emission sources, local population density and air concentration of PAHs, and the PAHs emission sources alone can explain 36%, 49%, 21% and 30% of the spatial variation in spring, summer, fall and winter, respectively.