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.     

Mercury fluxes and pools in three subtropical forested catchments, southwest China

Forested catchments are an important part of the mercury (Hg) cycle and a link between the atmospheric and the aquatic environments. In this study, Hg input and output fluxes and its retention were investigated at subtropical forested catchments in southwest China. Significantly enhanced atmospheric Hg inputs were observed, and the contribution of litterfall Hg plays a more important role at these subtropical forested catchments. The ratios of Hg output fluxes from stream water to total input were 2.5% and 1.2% for LGS and TSP, which were markedly lower than those reported from Europe and North America. The current annual input Hg only accounted for 0.8 and 1.8 per mille to the Hg stored in the upper 90 cm of soil in LGS and TSP. These suggest that subtropical forested catchments are important for retention of atmospheric mercury deposition in southwest China.     

Comparison of land nitrogen budgets for European agriculture by various modeling approaches

A comparison of nitrogen (N) budgets for the year 2000 of agro-ecosystems is made for the EU 27 countries by four models with different complexity and data requirements, i.e. INTEGRATOR, IDEAg, MITERRA and IMAGE. The models estimate a comparable total N input in European agriculture, i.e. 23.3–25.7 Mton N yr⁻¹, but N uptake varies more, i.e. from 11.3 to 15.4 Mton N yr⁻¹ leading to total N surpluses varying from 10.4 to 13.2 Mton N yr⁻¹. The estimated overall variation at EU 27 is small for the emissions of ammonia (2.8–3.1 Mton N yr⁻¹) and nitrous oxide (0.33–0.43 Mton N yr⁻¹), but large for the sum of N leaching and runoff (2.7–6.3 Mton N yr⁻¹). Unlike the overall EU estimates, the difference in N output fluxes between models is large at regional scale. This is mainly determined by N inputs, differences being highest in areas with high livestock density.     

Atmospheric concentrations, occurrence and deposition of persistent organic pollutants (POPs) in a Mediterranean coastal site (Etang de Thau, France)

Atmospheric concentrations and deposition fluxes of PCDD/F and PCB have been evaluated over a 1-year period in a Mediterranean coastal lagoon (Etang de Thau, France). Indicative PBDE air concentrations in the hot season are also reported in this work. ∑2,3,7,8-PCDD/Fs and ∑18PCBs (gas + particulate) air concentrations ranged from 67 to 1700 fg m⁻³ and from 13 to 95 pg m⁻³, respectively whereas ∑8PBDEs (gas + particulate) summer time levels varied from 158 to 230 pg m⁻³. The PCDD/F and PCB atmospheric occurrence over Thau lagoon and subsequent inputs to the surface waters are determined by an assemble of factors, being the seasonality of atmospheric concentration, the air mass origin and meteorological conditions important drivers. Total (wet + dry) ∑2,3,7,8-PCDD/Fs and ∑18PCBs deposition fluxes to Thau Lagoon waters are 117 and 715 pg m⁻² d⁻¹, respectively.     

Organophosphorus flame retardants and plasticizers in the atmosphere of the North Sea

Air samples collected in the German part of the North Sea from March to July 2010 were investigated for organophosphorus compounds (OPs) being applied as flame retardants and plasticizers. The ∑₈OPs concentration ranged from 110 to 1400 pg m⁻³ while tris(2-chloroisopropyl) phosphate (TCPP) dominated all samples with individual concentrations up to 1200 pg m⁻³. The highest concentrations were observed in continental air masses showing the high influence of industrialized regions including production sites on atmospheric emissions and concentrations. The occurrence of OPs even in oceanic/Arctic air masses shows that OPs can undergo long-range atmospheric transport. Dry particle-bound deposition fluxes from 9 to 240 ng m⁻² d⁻¹ for ∑₈OPs were estimated leading to a minimum annual flux of 710 ± 580 kg y⁻¹ OPs into the German North Sea. This study presents the first occurrence of OPs in the marine atmosphere together with important information on their long-range transport potential.     

One century sedimentary records of polycyclic aromatic hydrocarbons, mercury and trace elements in the Qinghai Lake, Tibetan Plateau

Sediments from a remote lake of northeastern Tibetan Plateau were analyzed for polycyclic aromatic hydrocarbons (PAHs) and trace metals. USEPA priority PAHs, ranged from 11 in 1860 to 279 ng g⁻¹ in 2002, while, the deposition fluxes were in the range of 0.2-11.4 ng cm⁻² yr⁻¹. Similarly, from 1860 to 2002, an increased trend of Hg flux was observed (0.5-3.2 ng cm⁻² yr⁻¹). Remarkable increase of PAHs and Hg concentration began from 1970, nearly the same period of the “Reform and Open” Policy had been embarked (1978) in China. Good correlations were found between concentrations of Pb, Zn, Cd, As, Hg, and PAHs, which suggested the sources of these chemicals in the sediment is analogous, likely from anthroprogenic sources. Based on isomer ratios, PAHs in core were dominantly from the incomplete combustion of coal. Owing to the proximity to dust source area (Qaidam Basin) and the close association between PAHs, Hg, Pb, and particle matters, atmospheric dust-transport and deposition might be the main pathways that pollutants enter into Qinghai Lake.     

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.     

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.     

Arsenic species in ecosystems affected by arsenic-rich spring water near an abandoned mine in Korea

The objectives of this study were to quantitatively estimate the distribution of arsenic with its speciation and to identify potential pathways for transformation of arsenic species from samples of water, sediments, and plants in the ecosystem affected by the Cheongog Spring, where As(V) concentration reached levels up to 0.270 mg L⁻¹. After flowing about 100 m downstream, the arsenic level showed a marked reduction to 0.044 mg L⁻¹ (about 84% removal) without noticeable changes in major water chemistry. The field study and laboratory hydroponic experiments with the dominant emergent plants along the creek (water dropwort and thunbergian smartweed) indicated that arsenic distribution, reduction, and speciation appear to be controlled by, (i) sorption onto stream sediments in exchangeable fractions, (ii) bioaccumulation by and possible release from emergent plants, and (iii) transformation of As(V) to As(III) and organic species through biological activities.     

Atmospheric deposition of phthalate esters in a subtropical city

In Chinese cities, air pollution has become a serious and aggravating environmental problem undermining the sustainability of urban ecosystems and the quality of urban life. Bulk atmospheric deposition samples were collected two-weekly, from February 2007 to January 2008, at three representative areas, one suburban and two urbanized, in the subtropical city, Guangzhou, China, to assess the deposition fluxes and seasonal variations of phthalate esters (PAEs). Sixteen PAE congeners in bulk deposition samples were measured and the depositional fluxes of ∑₁₆PAEs ranged from 3.41 to 190 μg m^?2 day^?1, and were highly affected by local anthropogenic activities. The significant relationship between PAEs and particulate depositional fluxes (correlation coefficient R² = 0.72, P < 0.001) showed PAEs are associated primarily with particles. Temporal flux variations of PAEs were influenced by seasonal changes in meteorological parameters, and the deposition fluxes of PAEs were obviously higher in wet season than in dry season. Diisobutyl phthalate (DiBP), Di-n-butyl phthalate (DnBP), and Di(2-ethylhexyl) phthalate (DEHP) dominated the PAE pattern in bulk depositions, which is consistent with a high consumption of the plasticizer market in China. PAE profiles in bulk deposition showed similarities exhibited in both time and space, and a weak increase of high molecular weight PAE (HMW PAE) contribution in the wet season compared to those in the dry season. Average atmospheric deposition fluxes of PAEs in the present study were significantly higher than those from other studies, reflecting strong anthropogenic inputs as a consequence of rapid industrial and urban development in the region.     

Phosphine migration at the water-air interface in Lake Taihu, China

The diurnal atmospheric phosphine (PH₃) concentrations and fluxes at the water-air interface in Lake Taihu were reported. The results showed that the PH₃ flux at the water-air interface ranged from −69.9 ± 29.7 to 121 ± 42 ng m⁻² h⁻¹, with a mean flux of 14.4 ± 22.5 ng m⁻² h⁻¹. The fluxes were both negative and positive during the diurnal period, indicating that the lake can act as a sink and a source of PH₃. In addition, the PH₃ fluxes were positively correlated with water temperature, total soluble phosphorus and soluble reactive phosphorus, while they were negatively correlated with water redox potential. A similar diurnal variation curve of atmospheric PH₃ concentrations was observed during all four seasons, with the maximum level occurring in early morning and the minimum appearing around midday. These findings suggest that light plays an important role in the elimination of atmospheric PH₃. A significant positive correlation was also found between air temperature and atmospheric PH₃ concentration. The mean flux of PH₃ in Lake Taihu was higher than in other reported wetlands, with an estimated annual emission of PH₃ to the atmosphere of 2.94 × 10⁵ g y⁻¹.     

Wet deposition mercury fluxes in the Canadian sub-Arctic and southern Alberta,measured using an automated precipitation collector adapted to cold regions

This paper reports mercury (Hg) concentrations and fluxes in precipitation that was collected from 2006 to 2008 at three sites in Canada: sub-Arctic boreal forest, sub-Arctic coast, and southern Alberta, using cold-adapted precipitation collectors which operated reliably at temperatures below ?30 °C during the study. The southern Alberta site (Crossfield) may be influenced by Calgary urban air, whereas the sub-Arctic coastal (Churchill, Manitoba) and boreal forest (Fort Vermilion, Alberta) sites are in more remote northern areas. Annual mean Hg concentrations in precipitation (5.0–9.2 ng L^?1) at the study sites were in the lower half of the range reported for southern Canada and the USA by the Mercury Deposition Network (MDN). But owing to typically low precipitation rates, gross wet Hg fluxes (0.54–2.0 μg m^?2 yr^?1) were among the lowest reported by MDN, with Crossfield having about twice the flux in 2007 of the other two sites. Flux was significantly correlated with precipitation, and thus was highest in summer (June–August) and lowest during winter, a pattern typical of other temperate continental locations. There was no evidence of higher wet Hg fluxes or concentrations in springtime at Churchill where atmospheric mercury depletion events (AMDEs) occur. Measured gross deposition fluxes at the study locations were ～2–8 times lower than estimated by GEOS-Chem and GRAHM atmospheric models. The largest discrepancy occurred for Churchill, which raises the question of how well Hg deposition from AMDEs is described by current models. Better agreement between measurements and models was obtained from MDN stations in Alberta and Alaska, where wet Hg fluxes were 2–10 times higher than the study sites either because of power plant emissions (Alberta), or because of high precipitation rates (Alaska).     

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.     

Thallium in the hydrosphere of south west England

Thallium is a highly toxic metal whose environmental concentrations, distributions and behaviour are not well understood. In the present study we measure the concentrations of Tl in filtered and unfiltered samples of rain, tap, river, estuarine and waste waters collected from south west England. Dissolved Tl was lowest (<20 ng L⁻¹) in tap water, rain water, treated sewage and landfill effluents, estuarine waters, and rivers draining catchments of sandstones and shales. Concentrations up to about 450 ng L⁻¹ were observed in rivers whose catchments are partly mineralized and where metal mining was historically important, and the highest concentration (∼1400 ng L⁻¹) was measured in water abstracted directly from an abandoned mine. Compared with other trace metals measured (e.g. As, Cd, Co, Cr, Cu, Ni, Pb, Zn), Tl has a low affinity for suspended particles and undergoes little removal by conventional (hydroxide precipitation) treatment of mine water.     

Total and methyl mercury concentrations and fluxes from small boreal forest catchments in Finland

Total mercury (TotHg) and methyl mercury (MeHg) concentrations were studied in runoff from eight small (0.02-1.3 km2) boreal forest catchments (mineral soil and peatland) during 1990-1995. Runoff waters were extremely humic (TOC 7-70 mg l-1). TotHg concentrations varied between 0.84 and 24 ng l-1 and MeHg between 0.03 and 3.8 ng l-1. TotHg fluxes from catchments ranged from 0.92 to 1.8 g km-2 a-1, and MeHg fluxes from 0.03 to 0.33 g km-2 a-1. TotHg concentrations and output fluxes measured in runoff water from small forest catchments in Finland were comparable with those measured in other boreal regions. By contrast, MeHg concentrations were generally higher. Estimates for MeHg output fluxes in this study were comparable at sites with forests and wetlands in Sweden and North America, but clearly higher than those measured at upland or agricultural sites in other studies. Peatland catchments released more MeHg than pure mineral soil or mineral soil catchments with minor area of peatland.     

Ozone flux over a Norway spruce forest and correlation with net ecosystem production

Daily ozone deposition flux to a Norway spruce forest in Czech Republic was measured using the gradient method in July and August 2008. Results were in good agreement with a deposition flux model. The mean daily stomatal uptake of ozone was around 47% of total deposition. Average deposition velocity was 0.39 cm s⁻¹ and 0.36 cm s⁻¹ by the gradient method and the deposition model, respectively. Measured and modelled non-stomatal uptake was around 0.2 cm s⁻¹. In addition, net ecosystem production (NEP) was measured by using Eddy Covariance and correlations with O₃ concentrations at 15 m a.g.l., total deposition and stomatal uptake were tested. Total deposition and stomatal uptake of ozone significantly decreased NEP, especially by high intensities of solar radiation.     

Arsenic contamination and potential health risk implications at an abandoned tungsten mine, southern China

In an extensive environmental study, field samples, including soil, water, rice, vegetable, fish, human hair and urine, were collected at an abandoned tungsten mine in Shantou City, southern China. Results showed that arsenic (As) concentration in agricultural soils ranged from 3.5 to 935 mg kg⁻¹ with the mean value of 129 mg kg⁻¹. In addition, As concentration reached up to 325 μg L⁻¹ in the groundwater, and the maximum As concentration in local food were 1.09, 2.38 and 0.60 mg kg⁻¹ for brown rice, vegetable and fish samples, respectively, suggesting the local water resource and food have been severely contaminated with As. Health impact monitoring data revealed that As concentrations in hair and urine samples were up to 2.92 mg kg⁻¹ and 164 μg L⁻¹, respectively, indicating a potential health risk among the local residents. Effective measurements should be implemented to protect the local community from the As contamination in the environment.     

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.     

Polycyclic aromatic hydrocarbon (PAH) deposition to and exchange at the air-water interface of Luhu, an urban lake in Guangzhou, China

Urban lakes are vulnerable to the accumulation of semivolatile organic compounds, such as PAHs from wet and dry atmospheric deposition. Little was reported on the seasonal patterns of atmospheric deposition of PAHs under Asian monsoon climate. Bulk (dry + wet) particle deposition, air-water diffusion exchange, and vapour wet deposition of PAHs in a small urban lake in Guangzhou were estimated based on a year-round monitoring. The total PAH particle deposition fluxes observed were 0.44-3.46 μg m⁻² day⁻¹. The mean air-water diffusive exchange flux was 20.7 μg m⁻² day⁻¹. The vapour deposition fluxes of PAHs ranged 0.15-8.26 μg m⁻² day⁻¹. Remarkable seasonal variations of particulate PAH deposition, air-water exchange fluxes and vapour wet deposition were influenced by seasonal changes in meteorological parameters. The deposition fluxes were predominantly controlled by the precipitation intensity in wet season whereas by atmospheric concentration in dry season.     

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.