A 40+ year record of Cd,Hg, Pb,and U deposition in sediments of Patroon Reservoir,Albany County,NY, USA

Sediments of the Patroon Creek watershed (33 km(2)) are known to contain significant concentrations of heavy metals derived from two industrial sites within the watershed. Mercury Refining, Inc (Mereco) has stored and recycled Hg from 1955 to the present day, and National Lead Industries (NLI) manufactured aircraft components containing Cd, Pb, and U from 1958 to 1984. Here we present the first record of heavy metal deposition as preserved in a 3-m long sediment core collected in 1999 from Patroon Reservoir, a small water body (1.3 ha) downstream of the industrial sites. Bulk sediment samples were collected from the core at 0.05-m intervals and analyzed for total Cd, Pb, and U by ICP-MS and total Hg by CVAAS. Total Hg increases from less than 1 mg kg(-1) (dw) below 1.68 m, to a maximum of 6.2 mg kg(-1) at 0.80 m, and then declines to the sediment-water interface. Total Cd, Pb, and U concentrations increase abruptly above 1.68 m to maximum values of 25, 320, and 3600 mg kg(-1) (dw), respectively, and then decline gradually upwards. By correlating metal profiles with industrial history, we conclude that the 1.68 m horizon was deposited no earlier than 1958, the beginning of aircraft component manufacturing at NLI. The average, apparent sedimentation rate within the reservoir has a minimum value of approximately 0.04 m year(-1) for the 41-year period from 1958 to 1999. In the interval 0--1.68 m, average concentrations of Cd, Hg, Pb, and U are 1.69, 1.50, 461, and 13 mg kg(-1), respectively. These levels are comparable with other lake, reservoir and stream sediments that have been moderately to severely impacted by industrial pollution and are above levels expected to be detrimental to aquatic organisms.     

Regional variation in the chemical composition of winter snow pack and terricolous lichens in relation to sources of acid emissions in the Usa river basin,northeast European Russia

The chemical composition of snow and terricolous lichens was determined along transects through the Subarctic towns of Vorkuta (130 km west-east), Inta (240 km south-north) and Usinsk (140 km, southwest-northeast) in the Usa river basin, northeast European Russia. Evidence of pollution gradients was found on two spatial scales. First, on the Inta transect, northward decreases in concentrations of N in the lichen Cladonia stellaris (from 0.57 mmol N g(-1) at 90 km south to 0.43 mmol N g(-1) at 130 km north of Inta) and winter deposition of non-sea salt sulphate (from 29.3 to 12.8 mol ha(-1) at 90 km south and 110 km north of Inta, respectively) were attributed to long range transport of N and S from lower latitudes. Second, increased ionic content (SO42-, Ca2+, K+) and pH of snow, and modified N concentration and the concentration ratios K+:Mg2+ and K+: (Mg2++Ca2+) in lichens (Cladonia arbuscula and Flavocetraria cucullata) within ca. 25-40 km of Vorkuta and Inta were largely attributed to local deposition of alkaline coal ash. Total sulphate concentrations in snow varied from ca. 5 micromol l(-1) at remote sites to ca. 19 micromol l(-1) near Vorkuta. Nitrate concentration in snow (typically ca. 9 micromol l(-1)) did not vary with proximity to perceived pollution sources.     

Storm flow export of metolachlor from a coastal plain watershed

During an 18-month (1994-1995) survey of the surface water in an Atlantic Coastal Plain watershed, metolachlor was most frequently detected during storm flow events. Therefore, a sampling procedure, focused on storm flow, was implemented in June of 1996. During 1996, three tropical cyclones made landfall within 150 km of the watershed. These storms, as well as several summer thunderstorms, produced six distinct storm flow events within the watershed. Metolachlor was detected leaving the watershed during each event. In early September, Hurricane Fran produced the largest storm flow event and accounted for the majority of the metolachlor exports. During the storm event triggered by Hurricane Fran, the highest daily average flow (7.5 m2 s-1) and highest concentration (5.1 micrograms L-1) ever measured at the watershed outlet were recorded. Storm flow exports leaving the watershed represented 0.1 g ha-1 or about 0.04% of active ingredient applied.     

Changes in water-extractability of soil inorganic phosphate induced by chloride and sulfate salts

GOAL, SCOPE AND BACKGROUND: One of the principal experimental variables which effect the results of phosphorus (P) sorption studies is the ionic composition, in addition to both species and concentrations of the contacting solution. In spite of the realization that ionic species, concentrations and their compositions effect P sorption and/or desorption, most of the salt-related studies are confined to Cl- (anion) in association with different cations. While the knowledge about the comparative response of P to Cl- and SO4(2-) ions was lacking, the current study was conducted to evaluate the comparative effects of anions (in association with cations) on inorganic P release and P fractions in the soil. METHODS: The test soil was amended with livestock compost manure (OP); KH2PO4 (IPk) or Ca(H2PO4)2 (IPc) at a rate of 1ppm. Soil was subjected to one salt and nine subsequent water extractions and different P fractions were measured. Four salt types, NaCl, Na2SO4, KCl and K2SO4, were used at levels of 0.5 M. RESULTS: Irrespective of P sources, P release was substantially increased in the salt-pretreated soil as compared to the non-saline soil. Sulfate salts released more P in subsequent water extractions than Cl-. Phosphorus release decreased for salt types with Na2SO4 > NaCl > K2SO4 > KCl and for P sources with OP approximately IPk > Control (without P application) > IPc, respectively. DISCUSSION: No previous study was found to compare the results of more P release by SO4(2-) than Cl- salt. Most of the previous studies focused on anion sorption capacities, but the mechanism for their adsorption is not fully known. Most of the authors suggested that the mechanisms of SO4(2-) and PO4(3-) adsorption are similar, and that both ions compete for the same sorption sites (Kamprath et al. 1956, Couto et al. 1979, Pasricha and Fox 1993). Although adsorbed SO4(2-) does not compete strongly with PO4(3-), there is likely to be some competition for sorption between these anions which may cause comparatively more P release by SO4(2-) than Cl- salts. Higher P release by Na-saturation could be due to the release of P associated with oxide surfaces or due to dissolution of Ca-P phases (Curtin et al. 1987). CONCLUSIONS: Study clearly showed that not only cations species differ for P desorption capacity, but associated anions also play a vital role in the fate of P under saline environments. Synergetic effects exist between Na and SO4(2-) ions which enhanced the P release. This study has also confirmed the fact that P from organic sources is available as well as from inorganic P sources. However, P release depends more on the type of P source applied than on total P. RECOMMENDATIONS AND PERSPECTIVES: It is highly recommended that more than one anion species must be used in the research plans for evaluating the P response in a saline environment. The results have important implications from the point of view of research, as most of the researchers focus on different cations only for evaluating P response to salts from an environmental point of view. However, our study has made it clear that anions in association with cations differed for their effects on P release.     

Distribution, origin and fate of chromium in soils in Guanajuato, Mexico

Total, hexavalent and trivalent chromium were determined in surface and 30-cm depth soil samples from a highly chromium-polluted area in Guanajuato state, central México. Four samples were also analyzed by a sequential extraction procedure. Nearly 0.9 km(2) out of the 8 km(2) area sampled was polluted with chromium, at concentrations up to 12960 mg kg(-1), mostly as Cr(III). Concentrations of Cr(VI) were lower than 0.5 mg kg(-1) in most sampled points, with the exception of one, where the concentration was found to be 65.14 mg kg(-1). Chromiumcontaining dust from a chromate factory accounted for most of the contamination. The highest concentrations of hexavalent chromium in soil, were in the bottom sediments of an abandoned water reservoir used to store polluted water from a well, before use of the water in the factory process. Tannery wastes, dust from a sanitary landfill of chromate compounds and the transport of chromium products are the sources of chromium at other sites. Chromium is fixed preferentially in the hydrous Fe and Mn oxides in the more polluted soils. Less polluted soils have a high proportion of chromium associated with the sulfide and organic fraction. Cr(III) is retained preferentially in the superficial soil layer. Variations in the physical characteristics of the soil, relative abundance of the various soil components and characteristics of the contaminant source, give rise to differences in chromium soil concentrations with depth.     

Seasonal air-water exchange fluxes of polychlorinated biphenyls in the Hudson River Estuary

Polychlorinated biphenyls (PCBs) were measured in the air and water over the Hudson River Estuary during six intensive field campaigns from December 1999 to April 2001. Over-water gas-phase SigmaPCB concentrations averaged 1100 pg/m3 and varied with temperature. Dissolved-phase SigmaPCB concentrations averaged 1100 pg/L and displayed no seasonal trend. Uncertainty analysis of the results suggests that PCBs with 5 or fewer chlorines exhibited net volatilization. The direction of net air/water exchange could not be determined for PCBs with 6 or more chlorines. Instantaneous net fluxes of SigmaPCBs ranged from +0.2 to +630 ng m(-2) d(-1). Annual fluxes of SigmaPCBs were predicted from modeled gas-phase concentrations, measured dissolved-phase concentrations, daily surface water temperatures and wind speeds. The net volatilization flux was +62 microg m(-2) yr(-1), corresponding to an annual loss of +28 kg/yr of SigmaPCBs from the Hudson River Estuary for the year of 2000.     

Degradation of microcystins in aqueous solution with in situ electrogenerated active chlorine

A new and efficient method for the degradation of microcystins (one family of blue algal toxins) was developed and studied. Microcystins (MCs) in water were directly and effectively removed by active chlorine transformed in situ from the naturally existing Cl- in water resource using electrochemical method. Titanium coated with RuO2 and TiO2 was used as the anode. Microcystin-RR (MCRR) and Microcystin-LR (MCLR) were chosen as the model compounds of MCs. The results suggested that 20.87 mgl(-1) MCs (12.58 mgl(-1) MCRR and 8.29 mgl(-1) MCLR) in aqueous solution with 1.85 mM Cl- could be synchronously decomposed within 15 min electrolysis under the condition of the current density 8.89 mAcm(-2), 20 degrees C and pH 7.00. The qualitative analysis showed that the heptapetide ring and the Adda group of both treated MCs were changed. The results also indicated that the removal rates of both MCs increased with the increasing of chloride concentration and applied current density, but decreased with the increasing of initial concentration of MCs and initial pH of electrolyte. In the absence of Cl-, only a small fraction of both MCs were decomposed by direct anodic oxidation, while their almost complete removals could be obtained in the case of indirect electrooxidation with in situ electrogenerated active chlorine from Cl- in water.     

Chemical composition and hygroscopic properties of size-segregated aerosol particles collected at the Adriatic coast of Slovenia

The chemical composition as well as the water uptake characteristics of aerosols was determined in size-segregated samples collected during November 2002 on the Slovenian coast. Major ions, water-soluble organic compounds (WSOC), short-chain carboxylic acids and trace elements were determined in the water-soluble fraction of the aerosol. Total aerosol black carbon (BC) was measured from filter samples. Our results showed that the origin of air masses is an important factor that controls the variation in the size distribution of the main components. Very high concentrations of WSOC as well as higher concentrations of BC were found under mostly continental influence. Besides the main ionic species (SO4(2-), NH4(+), K+) in the finest size fraction (0.17-0.53 microm), the concentration of NO3(-) was also high. The difference between the two different air mass origins is particularly expressed for Cl-, Na+, Mg2+ and Ca2+ determined in particles larger than 1.6 microm. As expected, a very good correlation was found between Na+ and Cl-. A good correlation was found between sea salt elements and elements of crustal origin (Na+, Cl-, Mg2+, Ca2+, Sr). A good relationship between typical anthropogenic tracers (K, V and Pb) was also observed. The mass growth factors, for all size fractions of aerosols collected under continental influence were very low (maximum 2.23 at 94%, 1.6-5.1 microm), while under marine influence the mass growth factors increased significantly with the particle size. At 97% humidity, the mass growth factors were 6.95 for the size fraction 0.53-1.6 microm and 9.78 for larger particles (1.6-5.1 microm).     

Heavy metal contamination in the vicinity of an industrial area near Bucharest

BACKGROUND, AIMS AND SCOPE: Chromium enters into the aquatic environment as a result of effluent discharge from steel works, electroplating, leather tanning industries and chemical industries. As the Cr(VI) is very harmful to living organisms, it should be quickly removed from the environment when it happens to be contaminated. Therefore, the aim of this laboratory research was to develop a rapid, simple and adaptable solvent extraction system to quantitatively remove Cr(VI) from polluted waters. METHODS: Aqueous salt-solutions containing Cr(VI) as CrO4(2-) at ppm level (4-6 ppm) were prepared. Equal volumes (5 ml) of aqueous and organic (2-PrOH) phases were mixed in a 10 ml centrifuge tube for 15 min, centrifuged and separated. Concentrations of Cr(VI), in both the aqueous and organic phases, were determined by atomic absorption spectrometry. The effects of salt and acid concentrations, and phase-contact time on the extraction of Cr(VI) were investigated. In addition, the extraction of Cr(VI) was assessed in the presence of tetramethylammonium chloride (TMAC) in 2-PrOH phase. Effects of some other metals, (Cd(II), Co(II), Cu(II), Ni(II) and Zn(II)), on the extraction of Cr(VI) were also investigated. RESULTS AND DISCUSSION: The Cr(VI) at ppm level was extracted quantitatively by salting-out the homogeneous system of water and 2-propanol(2-PrOH) using chloride salts, namely CaCl2 or NaCl, under acidic chloride media. The extracted chemical species of Cr(VI) was confirmed to be the CrO3Cl-. The ion-pair complex extracted into the organic phase was rationalized as the solvated ion-pair complex of [2-PrOH2+, CrO3Cl-]. The complex was no longer stable. It implied the reaction between extracted species. Studies revealed that salts and acid directly participated in the formation of the above complex. Use of extracting agents (TMAC) didn't show any significant effect on the extraction of Cr(VI) under high salting-out conditions. There is no significant interference effect on the extraction of Cr(VI) by the presence of other metals. The Cr(VI) in the organic phase was back-extracted using an aqueous ammonia solution (1.6 mol dm(-3)) containing 3 mol dm(-3) NaCl. The extraction mechanism of Cr(VI) is also discussed. CONCLUSIONS: Salting-out of homogeneous mixed solvent of 2-propanol can be employed to extract Cr(VI) quantitatively, as an ion-pair of [2-PrOH2+ * CrO3Cl-] solvated by 2-PrOH molecules. Then, the complex becomes 'solvent-like' and is readily separated into the organic phase. The increase of Cl- ion concentration in the aqueous phase favors the extraction. The 2-PrOH, salts and acid play important roles in the extraction process. There is no need to use an extracting agent at a high salting-out condition. RECOMMENDATIONS AND PERSPECTIVES: Chromium(VI) must be quickly removed before it enters into the natural cycle. As the 2-PrOH is water-miscible in any proportion, ion-pairing between 2-PrOH2+ and CrO3Cl- becomes very fast. As a result, Cr(VI) can easily be extracted. Therefore, the method is recommended as a simple, rapid and adaptable method to quickly separate Cr(VI) from aqueous samples.     

Atmospheric nitrogen inputs to the Delaware Inland Bays: the role of ammonia

A previous assessment of nitrogen loading to the Delaware Inland Bays indicates that atmospheric deposition provides 15-25% of the total, annual N input to these estuaries. A large and increasing fraction of the atmospheric wet flux is NH(4)(+), which for most aquatic organisms represents the most readily assimilated form of this nutrient. Particularly noteworthy is a 60% increase in the precipitation NH(4)(+) concentration at Lewes, DE over the past 20 years, which parallels the increase in poultry production on the Delmarva Peninsula over this period (currently standing at nearly 585 million birds annually). To further examine the relationship between local NH(3) emissions and deposition, biweekly-integrated gaseous NH(3) concentrations were determined using Ogawa passive samplers deployed at 13 sampling sites throughout the Inland Bays watershed over a one-year period. Annual mean concentrations at the 13 sites ranged from <0.5 microg NH(3)m(-3) to >6 microg NH(3)m(-3), with a mean of 1.6+/-1.0 microg NH(3)m(-3). At most sites, highest NH(3) concentrations were evident during spring and summer, when fertilizer application and poultry house ventilation rates are greatest, and seasonally elevated temperatures induce increased rates of microbial activity and volatilization from soils and animal wastes. The observed north-to-south concentration gradient across the watershed is consistent with the spatial distribution of poultry houses, as revealed by a GIS analysis of aerial photographs. Based on the average measured NH(3) concentration and published NH(3) deposition rates to water surfaces (5-8 mm s(-1)), the direct atmospheric deposition of gaseous NH(3) to the Inland Bays is 3.0-4.8 kg ha(-1)yr(-1). This input, not accounted for in previous assessments of atmospheric loading to the Inland Bays, would effectively double the estimated direct dry deposition rate, and is on par with the NO(3)(-) and NH(4)(+) wet fluxes. A second component of this study examined spatial differences in NO(3)(-) and NH(4)(+) wet deposition within the Inland Bays watershed. In a pilot study, precipitation composition at the Lewes NADP-AIRMoN site (DE 02) was compared with that at a satellite site established at Riverdale on the Indian River Estuary, approximately 21 km southwest. While the volume-weighted mean precipitation NO(3)(-) concentrations did not differ significantly between sites, the NH(4)(+) concentration observed at Riverdale (26.3 micromoles L(-1)) was 73% greater than at Lewes (15.2 micromoles L(-1)). More recently, a NADP site was established at Trap Pond, DE (DE 99), which was intentionally located within the region of intense poultry production. A comparison of the initial two years (6/2001-5/2003) of precipitation chemistry data from Trap Pond with other nearby NADP-AIRMoN sites (Lewes and Smith Island) reveals fairly homogeneous NO(3)(-) wet deposition, but significant spatial differences ( approximately 60%) in the NH(4)(+) wet flux. Overall, these results suggest that local emissions and below-cloud scavenging provide a significant contribution to regional atmospheric N deposition.     

Arsenic and mercury concentrations in major landscape components of an intensively cultivated watershed

To provide an understanding of arsenic (As) and mercury (Hg) concentrations in soil, sediment, water, and fish tissues, samples were collected from a Mississippi River alluvial floodplain located in northwest Mississippi. As concentrations increased approximately an order of magnitude from water (5.12 micrograms/l) to fish tissues (36.99 micrograms/kg) and an additional two orders of magnitude in soils, lake sediments, and wetland sediments (5728, 5614, and 6746 micrograms/kg), respectively. Average Hg concentrations in water, soils, lake sediments, and fish were 2.16 micrograms/l, 55.1, 14.5 and 125 micrograms/kg, respectively. As and Hg concentrations were within published ranges for uncontaminated soil, water, and sediments. As concentrations represented a low risk. Hg concentrations were also low but showed a greater tendency to concentrate in fish tissue. The dominant mode of entry of these materials into aquatic systems is through storm-generated runoff. Since both metals accompany sediments, agricultural conservation practices such as reduced tillage, buffer riparian strips, and bordering sediment ponds or drainage wetlands will minimize watershed input to aquatic systems.     

A study of polonium-210 distribution aspects in the riverine ecosystem of Kaveri, Tiruchirappalli, India

Distribution of a natural radionuclide (210Po) in water, sediment and biota was quantified along a 95 km reach of the Kaveri River, India. It is observed that the soft tissues of animals concentrated a higher level of 210Po than the hard parts like shell and bone. The ranges of 210Po activity in biological samples were 2.32-10.78 Bq kg(-1) wet (aquatic weeds), 18.94-28.55 Bq kg(-1) wet (plankton), 32.51 to 46.17 Bq kg(-1) wet (snail), 57.42 to 105.78 Bq kg(-1) wet (bivalve), 12.13 to 19.10 Bq kg(-1) wet (prawn) and 1.86 to 4.17 Bq kg(-1) wet (fish). The concentration factors (CFs) for the aquatic organisms ranged from 10(3) to 10(4), indicating a high affinity of 210Po for organic moieties. The bivalve mollusc, Lamellidens marginalis, accumulated higher concentrations of 210Po, suggesting that it could serve as a biomonitor of 210Po radionuclide in riverine systems. Further, the levels of 210Po in water, sediment and biological samples from impoundments were higher than those from stations located in the open river. This may be largely due to aerial inputs of the radionuclide, accumulation of radionucliderich silt and organic matter, and increased biological production in the impounded water body.     

Inorganic PM2.5 at a U.S. agricultural site

In this study, we present approximately two years (January 1999-December 2000) of atmospheric NH3, NH4+, HCl, Cl-, HNO3, NO3-, SO2, and SO4= concentrations measured by the annular denuder/filter pack method at an agricultural site in eastern North Carolina. This site is influenced by high NH3 emissions from animal production and fertilizer use in the surrounding area and neighboring counties. The two-year mean NH3 concentration is 5.6 (+/-5.13) microg m(-3). The mean concentration of total inorganic PM2.5, which includes SO4=, NO3-, NH4+, and Cl-, is 8.0 (+/-5.84) microg m(-3). SO4=, NO3-, NH4+, and Cl- represent, respectively, 53, 24, 22, and 1% of measured inorganic PM2.5. NH3 contributes 72% of total NH3 + NH4+, on an average. Equilibrium modeling of the gas+aerosol NH3/H2SO4/HNO3 system shows that inorganic PM2.5 is more sensitive to reductions in gas + aerosol concentrations of sulfate and nitrate relative to NH3.     

Dynamic factor analysis of groundwater quality trends in an agricultural area adjacent to Everglades National Park

The extensive eastern boundary of Everglades National Park (ENP) in south Florida (USA) is subject to one of the most expensive and ambitious environmental restoration projects in history. Understanding and predicting the water quality interactions between the shallow aquifer and surface water is a key component in meeting current environmental regulations and fine-tuning ENP wetland restoration while still maintaining flood protection for the adjacent developed areas. Dynamic factor analysis (DFA), a recent technique for the study of multivariate non-stationary time-series, was applied to study fluctuations in groundwater quality in the area. More than two years of hydrological and water quality time series (rainfall; water table depth; and soil, ground and surface water concentrations of N-NO3-, N-NH4+, P-PO4(3-), Total P, F-and Cl-) from a small agricultural watershed adjacent to the ENP were selected for the study. The unexplained variability required for determining the concentration of each chemical in the 16 wells was greatly reduced by including in the analysis some of the observed time series as explanatory variables (rainfall, water table depth, and soil and canal water chemical concentration). DFA results showed that groundwater concentration of three of the agrochemical species studied (N-NO3-, P-PO4(3-)and Total P) were affected by the same explanatory variables (water table depth, enriched topsoil, and occurrence of a leaching rainfall event, in order of decreasing relative importance). This indicates that leaching by rainfall is the main mechanism explaining concentration peaks in groundwater. In the case of N-NH4+, in addition to leaching, groundwater concentration is governed by lateral exchange with canals. F-and Cl- are mainly affected by periods of dilution by rainfall recharge, and by exchange with the canals. The unstructured nature of the common trends found suggests that these are related to the complex spatially and temporally varying land use patterns in the watershed. The results indicate that peak concentrations of agrochemicals in groundwater could be reduced by improving fertilization practices (by splitting and modifying timing of applications) and by operating the regional canal system to maintain the water table low, especially during the rainy periods.     

Caesium-137 in Perch in Swedish Lakes after Chernobyl-present situation, relationships and trends

The Chernobyl accident, and the general acidification of Swedish water systems, form the base for this project. The aims of the work have been to present results on the linkage between the concentration of Cs-137 in fish, lake load of Cs and lake characteristics, to give a preliminary prognosis on the recovery, and to put the results within a wider framework of environmental hazard analysis. A broad set of data on limnology, morphometry and drainage area conditions from 41 lakes were collected during 1986 and 1987. Cs-137 was determined in 1 + perch (Cs-pe, 1-year-old perch), water, material collected by sediment traps and from surficial sediments. The main results are as follows. The average value of Cs-pe for all lakes has dropped from 9800 Bq kg(-1) (wet) to 5040 between the 2 years. Generally, the decrease is between 5 and 90%. We have tested if any factor(s) could be specifically linked to this decrease-no such factors have been found. The concentrations of Cs in sediment traps have, on average, decreased by 80%. Very high correlations exist between Cs-pe and the caesium load as determined from the sediment traps. Between 1 and 10% (mean 3.9%) of the initial fall-out deposition to the drainage area was transported from land to water during June to August 1986. The variation in initial fall-out deposition explains 65-69% of the variability in Cs-pe; the degree of explanation (= coefficient of determination, r2) increases to about 85% if one also takes into account the lake water hardness and totP. A map showing with lakes likely to have 1 + perch with higher mean Cs-concentrations than 1500 Bq kg(-1) wet is presented. Between 4000 and 7000 lakes in Sweden appear to have Cs-pe higher than 1500 Bq kg(-1) wet, figures which emphasize the serious impact of the Chernobyl accident on the environmental conditions in Sweden.     

The effective source area of 90Sr for a stream near Chernobyl, Ukraine

Remediation of streams impacted by non-point source contaminants requires an understanding of both the areas within a watershed that are contributing contamination to streams and the pathways of contaminant migration to streams. From 1998 to 2002, we studied the migration of 90Sr in the Borschi watershed, a small (8.5 km2) catchment three km south of the Chernobyl Nuclear Power Plant, Ukraine. Fuel particles, distributed in a heterogeneous pattern across the watershed, are weathering and releasing 90Sr from the fuel matrix. Depletion of (90)Sr, evaluated in comparison to the immobile fission product europium-154, is occurring in the channel and wetland sediment. Channel sediments are uniformly depleted in 90Sr with depth. In wetland sediments, there is a zone of depletion in the top 10 cm and a zone of accumulation at depths from 10 to 25 cm. Estimates of 90Sr depletion are used to map the effective source area that has contributed (90)Sr loading to the main channel. The effective source area includes channel bottom sediments, a wetland in the central region of the watershed, and periodically flooded soils surrounding the wetland. The total depletion from the effective source area is estimated to be 36 +/- 7 x 10(10) Bq. Based on observations of stream flow rate and water quality in 1999-2001, the annual 90Sr removal rate from the watershed is estimated to be 1.4 +/-0.2 x 10(10) or 1.5% of the inventory per year. When extrapolated over a 15-year period following the Chernobyl accident, the last value is in reasonable agreement with the estimated depletion of the source area based on 90Sr/154Eu ratios. The 90Sr yearly leaching rate considering the whole watershed is 0.2% while the 90Sr leaching rate considering the effective source area is an order of magnitude higher. Most of the 90Sr release in the watershed has originated from an effective source area of 0.62 km2, or 7% of the watershed area.     

Decreased acid deposition and the chemical recovery of Killarney,Ontario, lakes

Lakes in Killarney Park near Sudbury, Ontario, Canada, have shown dramatic water quality changes including general increases in pH and alkalinity, and decreases in SO4(2-), base cations and metals. While some lakes have recovered to pH > 6.0, many are still highly acidic despite decades of improvement. Very high historical S deposition related to emissions from the Sudbury metal smelters dominated the acidification process in this region. However, since the implementation of substantial S emission controls (90%) at the smelters, the Sudbury emissions are no longer the major source of S deposition in the Sudbury area. Wet deposition of SO4(2-) and SO4(2-) concentrations in lakewaters at Killarney now approach values in the Dorset, Ontario, area, about 200 km from Sudbury. This suggests that the S deposition to the Killarney area is now primarily from long-range transport, not from local sources. Studies of Killarney lakes are revealing the complex nature of the chemical recovery process. As lake acidity decreases, other changes including decreased Ca2+ concentrations, increased transparency, and altered thermal regimes may potentially affect some of these ecosystems. It is clear that continuing assessments of the recovery of Killarney lakes, within a multiple-stressor framework, are needed.     

Temporal variation in daily concentrations of ozone and acid-related substances at Saturna Island, British Columbia

A multiple linear regression model was used to investigate seasonal and long-term trends in concentrations of ozone (O3) and acid-related substances at the Saturna Island monitoring station in southwestern British Columbia from 1991 to 2000. Statistically significant primary (dominant) cycles with a period of 1 yr were found for O3, sulfur dioxide (SO2), nitric acid (HNO3), and aerosol concentrations of sulfate (SO4(2-)), calcium (Ca2+) and chloride (Cl-). Of these, peak median concentrations occurred during the spring for O3 and Ca2+, during the warmer, drier months (April-September) for SO4(2-) and HNO3, and during the cooler, wetter months (October-March) for SO2 and Cl-. Statistically significant secondary cycles of 6 months duration were seen for concentrations of O3, SO4(2-), HNO3, Ca2+, and Cl-. Daily maximum O3 concentrations exhibited a statistically significant increase over the period of record of 0.33 +/- 0.26 ppb/yr. Statistically significant declines were found for concentrations of SO2, SO4(2-), HNO3, Ca2+, and potassium, ranging from 20 to 36% from levels at the start of the sampling period. Declines in ambient concentrations of SO2, SO4(2-), and HNO3 reflect local declines in anthropogenic emissions of the primary precursors SO2 and NOx over the past decade. Trends in Ca2+ and potassium ion concentrations are in line with a broader North American declining trend in acid-neutralizing cations.     

Reproductive status, blood chemistry, gill histology and growth of perch (Perca fluviatilis) in three acidic lakes

Perch (Perca fluviatilis L.) were sampled soon after spawning in three small acidic lakes (pH 4.3-6.1, Al(lab) 5-106 microg litre(-1), Ca2+ 0.01-0.08 mmol litre(-1)) and in one circumneutral lake (pH 5.9-6.4, Al(lab) 4-12 microg litre(-1), Ca2+ 0.06-0.07 mmol litre(-1)) in southern Finland. Due to the delayed spawning of perch in the acidic lakes, sampling in those lakes was performed later than in the reference lake. In spite of that, the gonadosomatic index (GSI) of males in all the acidic lakes was significantly greater than in the reference lake. Of the two lakes with similar low water pH, the effects on reproduction were more prominent in the lake with higher water Al content. The plasma Ca2+ concentrations of females in the acidic lakes were significantly smaller than in the females of the reference lake. The low female:male plasma Ca2+ ratio (1.0-1.32) depicted delay of spawning. Stress in perch in acidic water was also seen in elevated blood haematocrit values, especially in females. On the other hand, a low plasma Cl- level, a common response to acidic water in salmonids, was not detected in perch in the most acidic lakes. The amount of Al accumulated in the gill epithelium was highest in the most acidified lake with high Al concentration, but was also pronounced in a lake with low pH and low Al concentration.     

Mercury levels in surface waters of the Carson River-Lahontan Reservoir system, Nevada: Influence of historic mining activities

Total mercury (HgT), methylmercury (MeHg), and other operationally defined Hg species were determined on water samples collected from a river-reservoir system impacted by historic mine wastes. Simultaneously, a comprehensive study was undertaken to determine the influence of some major physico-chemical parameters on the fate of Hg within the system. Total Hg levels showed an increase from background concentrations of 4 ng liter(-1) upstream of mining activity, to peak values of 1500-2100 ng liter(-1) downstream of Hg contaminated mine tailings piles. MeHg concentrations varied from 0.1 to 7 ng liter(-1) in surface waters. In both cases, peak values were associated with the highest concentrations of total suspended solids (TSS). Particulate Hg (HgP) was typically >50% of HgT and increased downstream. The dissolved fraction of MeHg (MeHgD) always constituted a large portion of total methylmercury (MeHgT). The [MeHgT]/[HgT] ratio decreased downstream suggesting either a high percentage of inorganic Hg input from point sources, or low specific rates of MeHg production within the aquatic system. The latter could be due to the combined effects on microbial populations of both high levels of Hg concentrations found in water and sediments, and other factors related to the aqueous geochemistry of the system. Concentrations of HgT in the water column appeared to be enhanced by inputs of contaminated particles from the watershed during spring snow melt. In the reservoir, significant losses of Hg from the water column were observed. In addition to losses of Hg bound to particles by sedimentation, the removal through volatilization of dissolved gaseous Hg could be an important pathway.