Mercury in fish in Swedish lakes — Linkages to domestic and European sources of emission

The work deals primarily with data from 894 Swedish lakes. The following parameters are discussed: Hg- and Se-concentrations and Hg-quantity in the mor layer reflecting the atmospheric deposition of Hg and Se-, Hg- and S-emissions deposition from Swedish and continental sources, precipitation, Hg in pike, lake area, lake mean depth, pH, color, alkalinity, hardness, S and chloride in lake water. The results are focused on geographical variations and statistical correlations for the Hg-content in 1-kg pike (=FHg), and on computer simulations to get insights and data on the linkages between various historical Hg-emissions and FHg. Selected results: Increased FHg-values may be attributed to atmospheric emissions of Hg and to acid rain. Southern Sweden is significantly influenced by continental Hg-emissions. East Germany, Great Britain, West Germany and Poland seem to have contributed with the largest foreign Hg-amounts in the Swedish mor layer and, at the end, to increased Hg-concentrations in Swedish fish. We have calculated that there are about 10 300 Swedish lakes with FHg > 1 mg Hg kg^?1 (= the Swedish blacklisting limit). What would happen with FHg if atmospheric depositions of Hg and S were significantly reduced? Reductions of S would be beneficial primarily for lakes in S. Sweden. About 50% of the elevated levels of Hg in Swedish pike in the 1980s may be linked to Swedish Hg-emissions during the last 100 yr, about 10 to 15% could be attributed to foreign Hg-emissions and 35 to 40% to acid rain. There is a long lag phase between emission reduction and reduction of FHg. The known, major Swedish emissions of Hg have already been significantly reduced, but new point sources of Hg have appeared. There has been a significant change in the character of the Hg-emissions during the last decades. High FHg-values in fish in Swedish lakes will be a major environmental problem for decades to come.     

Mercury in the Swedish mor layer — linkages to mercury deposition and sources of emission

The report deals with data from 363 Swedish mor samples. The following parameters are discussed: Hg-, organic and Se-concentrations and Hg-quantity in mor, Hg- and S-deposition from Swedish and continental emissions (point sources and diffuse emissions) and precipitation. The results are focused on mean, geographical variations, statistical correlations and calculations to get first insights and order of magnitude data on the linkages between the Hg-contamination of the Swedish mor layer and the various sources of Hg-emissions. Southern Sweden is significantly influenced by continental Hg-emissions. Several previously unknown domestic discharge sources of Hg have been identified. The total amount of Hg in the Swedish mor layer has been estimated to be about 615 t. East. Germany, United Kingdom, West Germany and Poland seem to have contributed with the largest continental emissions of Hg entering the Swedish mor layers. The countries which early started to build up their industry probably are responsible for greater Hg-contamination than indicated by our figures, and vice versa. If no measures are taken to reduce the emissions, the present contamination will continue. Then, the ‘burden of guilt’ ought to be redistributed so that a higher proportion of the Swedish Hg-contamination would be linked to continental discharges since considerable reductions have already occurred as regards Hg-discharges from large Swedish sources. The problems with elevated Hg-levels in the mor layer and, at the end point, the high concentrations of Hg in lake fish in Sweden, will remain far into the next century.     

The origin and deposition history of polycyclic aromatic hydrocarbons in the finger lakes region of New York

Studies aimed at determining the deposition history of energy related, potentially carcinogenic, polycyclic aromatic hydrocarbons (PAHs) deposited in the sediments of Cayuga Lake, in the Finger Lakes Region of central New York State, are described. PAH fluxes in the 1850's were at least an order of magnitude less than the maximum rates in the period of 1940 to 1955. PAH fluxes began to decline before the Milliken coal fired power plant, located on Cayuga Lake, started service in 1955. Correlation between the PAH flux into the sediments and fossil fuel usage and emissions for the states of New York, Ohio and Pennsylvania and the United States as a whole, suggests that modern, high efficiency fossil fuel fired power plants are minor sources of PAHs compared to coal related residential heating and industrial combustion. Similar comparisons with historic emissions data do not support the hypothesis that PAH flux is a useful indicator of the combustion sources which produce the `acidifying' compounds SO₂ and NO_x for the Finger Lakes region.     

Climate confounds detection of chemical trends related to acid deposition in upper Midwest lakes in the USA

Between 1983–94, as acid deposition rates declined, SO₄ ^2? concentrations decreased in 18 of 28 lakes monitored by the upper Midwest LTM program. The expected recovery of ANC and pH was less common, however. Differences in climate may account for divergent trend patterns across the region. Only in Minnesota, where climatic shifts were less pronounced, did we observe a general pattern of increasing lake ANC and pH accompanying declines in SO₄ ^2?. In contrast, the widespread negative trends in lake SO₄ ^2? in the upper Michigan lakes were generally not associated with recovery of ANC and pH, but with decreases in Ca+Mg. These cation decreases may be linked to decreased groundwater inputs during the drier climatic conditions characterizing the study period and decreases in Ca+Mg in atmospheric deposition. In many of the Wisconsin lakes, an overall decline in SO₄ ^2? was precluded by SO₄ ^2? increases during a 4-year drought midway through the study period. During the drought, declining lake water level and volume caused evaporative concentration of solutes, and may have decreased the areal extent of sulfate reduction. Despite controls on sulfur emissions across the region, recovery of pH and ANC has been hindered by climatic shifts and concurrent decreases in atmospheric deposition of cations.     

Mercury in fish muscle in acidified and limed lakes

The concentration of Hg in muscle was monitored during 10 to 12 years in different size and age groups of pike (Esox lucius) and perch (Perca fluviatilis). The study was performed in one reference and five lime treated lakes. Before liming, the highest levels of Hg in fish were measured in a lake with an annual mean pH just above 5.0. Lower levels were obtained both in lakes which were more acidified and in those which were less acidified. After the start of liming, the fastest and largest changes were obtained in the lakes which were moderately acid before liming (mean pH 5.4–5.8). In small perch, the Hg-concentration was markedly reduced in two years and showed an 80 % decrease in ten years. A slower response was registered in the lakes originally having about 0.5 units lower pH. In the most acidified lake (pH 4.9) the concentrations even increased the first years after liming, but decreased again later on. The possible mechanisms involved are discussed.     

Mercury in the surface water of Swedish forest lakes —concentrations,speciation and controlling factors

Concentrations of total Hg and five operationally defined Hg species were determined in the surface water of 25 Swedish forest lakes of different type. Regional and seasonal variations were studied during the ice-free season of 1986. The concentration of total Hg was usually in the range of 2 to 10 μg m-3. Hg concentrations were highly correlated to the concentration of humic matter measured as water color. Hg concentrations were about twice as high in acidic lakes (pH 5) than in circumneutral lakes, which is attributed basically to the acidity of humic compounds acting as Hg carriers in boreal waters. Significant seasonal variations were caused by hydrological processes. During periods of high water flow, Hg concentrations increased dramatically, especially in humic lakes. Between spring and autumn, chemically reactive Hg compounds were gradually replaced by more inert species. Hg/C ratios were higher than in surface runoff from forest watersheds, indicating a significant impact of direct deposition of Hg on lake surfaces during summer. Regional differences were small despite differences in Hg contamination.     

Mercury in humus horizons of soils in the Transbaikal region

The total mercury content has been determined in gray forest soils, chernozems, chestnut soils, and in different parent materials in the Transbaikal region. The mercury content is below the clarke value in the intrusive, effusive, and alluvial soil-forming rocks (0.004–0.024 mg/kg). In the humus horizons of the soils, it reaches 0.011–0.026 mg/kg, which is higher than the clarke value for the pedosphere. The mean background content of mercury in the soils of the Transbaikal region is 0.018 mg/kg. No significant positive correlation between the mercury content and the humus content of the soils has been revealed.     

Mercury in forest canopy throughfall water and its relation to atmospheric deposition

A seasonal variation of both particle and gaseous Hg concentrations in the atmosphere is present in south-western Sweden. An average gaseous Hg level of 3.7 ng m⁻³ is found in winter, compared to 2.8 ng m⁻³ in summer. A weak decreasing south-north gradient for gaseous Hg in air over the Nordic countries is also present, with yearly average values from 3.2 to 2.8 ng m⁻³. A gradient for particulate Hg is less clear. An air parcel trajectory sector classification of gaseous Hg levels in air, and to some extent the particulate associated Hg, clearly demonstrates the increased concentrations in the southern sectors, especially in south-western Sweden where the gaseous Hg increase is about I ng m⁻³. These observations are consistent with an influence from the European continent. The average concentrations of Hg in precipitation at the various stations show a pronounced decreasing south-north gradient. A major portion of the total Hg present in precipitation is associated with particles. For the southern stations, a strong correlation between Hg and sulfate, or pH, is present suggesting a connection between Hg in precipitation and anthropogenic activities.     

The use of calibrated lakes and watersheds for estimating atmospheric deposition near a large point source

We have measured the input and output rates of substances to and from both lakes and watersheds in the Sudbury and Muskoka-Haliburton areas of Ontario. At the former location, we have conducted mass balance studies on 5 lakes and their watersheds for 2½ yrs. At the latter site, we have measured mass balances for 6 lakes and about 30 individual watersheds for the past 5 yrs. Substances studied included SO₄ ^2?, NO₃ ^?, NH₄ ⁺, H⁺, major cations (Ca²⁺, Mg²⁺, Na⁺, K⁺) and HCO₃ ^?. During the course of the investigation at Sudbury we have made several observations that indicate that the inputs of some substances, specifically SO₄ ^2? or SO₄ ^2?-precursors and strong acids, to lakes and watersheds are underestimated when measured as bulk deposition (i.e. by collection in a continuously open container): (a) The output of SO₄ ^2? from the calibrated watersheds was substantially greater than the input measured as bulk deposition. (b) The SO₄ ^2? concentrations of the lakes could not be explained on the basis of the measured inputs. An additional input directly to the lake surface was needed to obtain a mass balance. (c) The net input of acids measured as bulk deposition to the watersheds was much less than the acid consumed, which was estimated by the net output of Ca²⁺, Mg²⁺, Na⁺, K⁺, Al³⁺, and the net retention of NO₃ ^?. (d) The major cation content of the study lakes could be explained on the basis of weathering reactions in the lakes' watersheds only if the input of strong acid had been underestimated. When these observations were quantified, they indicated a major portion of the total input of SO₄ ^2?-precursors and of strong acid was not included in our bulk deposition measurements. Deposition of SO₂ is the most likely explanation for these observations.     

Modelling of sulfur deposition in the Southern Asian region

Acidification problems in developing countries are expected to become more prevalent in the coming decades. Assessments of means of abatement strategies are likely to become of vital interest. This paper presents some preliminary results of modelling of acidic deposition due to anthropogenic emissions of sulfur in the Southern Asian region. It is concluded that the study has some shortcomings, that has to be addressed in future work, such as lack of treatment of deep convection and that deposition and transformation rates used are not adapted to the tropics. Only very limited validation has been possible due to the lack of relevant measurements. Wet deposition data from rural Thailand are in fair agreement with calculated values. The study is one part of a larger project encompassing mapping ecosystem sensitivity to acid deposition, wet chemistry measurements and atmospheric transfer modelling.     

Historical sediment mercury deposition for select South Dakota,USA, lakes: implications for watershed transport and flooding

Purpose

Select South Dakota, USA water bodies, including both natural lakes and man-made impoundments, were sampled and analyzed to assess mercury (Hg) dynamics and historical patterns of total Hg deposition.

Materials and methods

Sediment cores were collected from seven South Dakota lakes. Mercury concentrations and flux profiles were determined using lead (²¹⁰Pb) dating and sedimentation rates.

Results and discussion

Most upper lake sediments contained variable heavy metal concentrations, but became more consistent with depth and age. Five of the seven lakes exhibited Hg accumulation fluxes that peaked between 1920 and 1960, while the remaining two lakes exhibited recent (1995–2009) Hg flux spikes. Historical sediment accumulation rates and Hg flux profiles demonstrate similar peak and stabilized values. Mercury in the sampled South Dakota lakes appears to emanate from watershed transport due to erosion from agricultural land use common to the Northern Great Plains.

Conclusions

For sampled South Dakota lakes, watershed inputs are more significant sources of Hg than atmospheric deposition.

     

Residual soil nitrogen credits for corn production along the upper Texas Gulf Coast region

Studies were conducted to evaluate response of dryland corn (Zea mays L.) along the upper Texas Gulf Coast to residual soil nitrate-nitrogen (NO₃-N) measured to depths of 15, 30, and 61 cm. Residual soil NO₃-N levels ranged from 3.4 to 31.6, 7.8 to 49.3, and 9.0 to 71.7 kg ha^?1, respectively, in 0 to 15, 15 to 30, and 30 to 61 cm depth increments, with cumulative NO₃-N ranging from 23.5 to 114.5 kg ha^?1 across sites-years. Where N fertilizer was reduced due to N crediting, yields and bushel weights at all 13 site-years showed no difference from those receiving full recommended N rates. A yield response to any level of added fertilizer N above the control was observed for only 6 of 13 site-years. These results indicate a high potential for success in crediting carryover soil NO₃-N to 61 cm as a means of reducing applied nitrogen fertilizer rates.     

Chemistry of soft-water seepage lakes in the upper midwest: Lacustrine alkalinity production in summer

A total of 26 soft-water, seepage lakes in the Northern Highlands (NH) of Wisconsin (N =16) and the Upper Peninsula (UP) of Michigan (N=10) were sampled four times between early May and mid October 1984 as part of the ‘PIRLA’ Project (Paleolimnological Investigations of Recent Lake Acidification). Because of low antecedent recharge of the local water-table, this ‘summer’ interval likely featured minimal groundwater inputs (<2 cm over lake surface) to most of these seepage lakes. Based on this hydrogeologic relationship, and on regional deposition data, I evaluated short-term net epilimnetic (June–August) and whole-lake (May–October) sediment-water exchange of ANC, base cations, acid oxy-anions, Al, DOC and silicic acid in these lakes using a simplified mass balance algorithm. Silica, nitrate and ammonium were all efficiently retained in these seepage lakes. The assimilation of NO₃ ^? (19±4 meq m^?2) slightly exceeded assimilation of NH₄ ⁺ (16±4), resulting in a net internal ANC production of only +3 meq m^?2 over 161 d between early May and mid October 1984. Over this same interval ANC production resulting from lacustrine S retention averaged +35±8 meq m^?2 in the NH, but was too variable to be statistically significant (+21±21 meq m^?2) in the UP. Epilimnetic S retentions in mid summer were more comparable (21±4 in NH; 14±5 meq m^?2 in UP). McNearney Lake (UP) illustrates how high sulfate, linked to low alkalinity, high Al, low P, and low productivity, can become a negative correlate of lacustrine S retention. Temporal changes in base cations in the 26 lakes were generally small and erratic compared with uncertainties in deposition inputs and analytical errors, rendering estimates of related ANC production inconclusive. Even small analytical biases can be critical when designing and interpreting lake monitoring studies.     

Sulfate in lakes of eastern Canada: Calculated yields compared with measured wet and dry deposition

Sulfate yields in eastern Canada, calculated as lake concentration times runoff, are presented on an approximately west to east axis, and are compared with wet deposition data from CANSAP (Canadian Network for Sampling Precipitation) and APN (Air Pollution Network) data on dry deposition. The agreement is very good, and shows clearly that dry deposition is greatest near the center of the continental pollution plume and is less important in remote areas. The good agreement also indicates that most of the sulfate in these lakes is from atmospheric deposition and that there is little retention of sulfate in their watersheds.     

Use of chemistry and stable sulfur isotopes to determine sources of trends in sulfate of Colorado lakes

The chemistry of lakes in the Mt. Zirkel Wilderness Area (MZWA) and the Weminuche Wilderness Area (WWA) of Colorado has been monitored since 1985. The initial results indicate that changes have occurred in the chemistry of some lakes in both areas. Increased concentration of sulfate in lakes may be related to increased atmospheric depositon of sulfate or to changes of sulfate released by weathering and to changing dilution of sulfate by snowmelt. Stable S isotopes seem to be capable of separating the fraction of change in sulfate that is related to atmospheric and watershed sources. Because of the short period of record, it is not possible to determine whether the changes are part of a long-term trend or are merely natural fluctuations about some baseline.     

Pattern and cause of acidic deposition in the Chongqing region,Sichuan Province,China

The Chongqing region located in Sichuan Province of China, comprises a large city, many small towns and rural areas. The region relies heavily on high-sulfur coal for energy production. Atmospheric pollution by sulfur oxides and other compounds from coal burning has become a major issue. Acid rain is observed throughout the region; volume weighted average pH is about 4.30. Average total S deposition for the region is estimated to be about 8 g S m^?2 yr^?1. In this paper we report concentrations of major ions in rain, fog, dew and clouds, of SO₂ in air and of airborne particles as well as dustfall. The emissions and interactions between important chemical species in air and water droplets are discussed.     

Wet deposition of non sea-salt sulphate in the United Kingdom: The influence of natural sources

Because of its position to the west of Europe, much of the wet sulphur deposition in the west of the UK is background in the sense that it is not attributable to pollutants emitted within Europe less than four days previously. There are both natural and anthropogenic sources of this sulphur. An important natural source, especially during the summer, is dimethylsulphide (DMS) produced by marine phytoplankton. To identify the contribution of marine biogenic sulphur we have measured stable sulphur isotope ratios in precipitation. We show that biogenic sulphur is significant in summer but contributes little in winter and that around 5–10% of the annual background wet sulphur deposition is due to biogenic sources. During July and December 1993, airflow across the UK was predominantly westerly. The measured biogenic component of precipitation sulphate accounted for around 30 % of background sulphate in July but was negligible in December. Investigation of five day back-trajectories for the period indicated little opportunity for re-circulation of European emissions, suggesting that other (non-DMS) natural sources and non-European anthropogenic emissions were responsible for most of the background sulphur.     

The Health Safety Programme for Workers Exposed to Elemental Mercury at the Mercury Mine in Idrija

In the Idrija Mine ore appears in two forms: the first as cinnabar (70%) and the second as native mercury (30%). In the area where native mercury was mined the concentrations of elemental mercury in the working and unventilated areas of the pit were very high, they periodically reached over and above 3 mg/m³ of air and most of the time exceeded the maximum acceptable levels of mercury vapours in the air (0.1 mg/m³). In such specific working conditions the number of workers suffering from the effects of mercury was very high. Work conditions in the mine urgently required more effective and preventative measures against exposure to mercury. The health and safety program includes monitoring of mercury concentrations, technical measures, personal protection, evaluation of individual external intensity of exposure and medical surveillance. The results were very successful, the number of mercun intoxicated workers dropped and after 1975 there were no more intoxicated workers, in spite of the increase in the number of areas worked where native mercury was present.