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1.
Contents and δ34S values of several S compounds, enumerations of S-reducing bacteria (SRB) and Fe-reducing bacteria (IRB), and Fe, Pb and In concentrations were determined for 210Pb-dated sediment cores from two lakes in Quebec, Canada. Both lakes are located approximately 70 km downwind of the Horne smelter and refinery in Rouyn-Noranda. Increases in Fe, Pb and In concentrations and a decrease in the δ34S values of total S in both lake sediment cores coincide with the start-up of the smelter in 1927. The shift towards more negative δ34S values was primarily caused by an increase in the extent of S isotope fractionation during bacterial (dissimilatory) SO4 reduction due to SO4 loading of the lakes after smelting began. Consequently, an enhanced accumulation of 32S-enriched reduced inorganic S compounds is evident in the sediments. δ34S values of organic S in the sediments decreased only slightly due to the smelter emissions between 1930 and 1980. Hence, due to the sulfide depositing mechanisms, S isotope ratios constitute a useful tracer recording the onset of S pollution in sediments of the two previously SO4-limited lakes investigated. In contrast, total S concentrations alone are not reliable indicators for anthropogenic S loading in lake sediment records.  相似文献   

2.
《Applied Geochemistry》1997,12(1):75-81
The extent of vertical migration of anthropogenic Pb beneath a medieval smelting site in Derbyshire, U.K. has been estimated using the determination of total Pb concentrations and 206Pb/207Pb isotope ratio from samples taken down 6 m of drill core. Preliminary studies of total Pb concentrations established that the surface slag derived from the smelting contained up to 16% Pb and that the normal background levels in uncontaminated sandstone were 10±2 ppm. Sample analyses beneath the site revealed elevated Pb concentrations in fracture infill clays (270 ppm Pb) and sandstone (76–83 ppm Pb). Both are well above the background Pb concentration.Lead isotope analysis of the slag wastes, the underlying contaminated sandstone and fracture infill has shown that all 3 contain very similar isotope ratios for 206Pb/207Pb (1.1802–1.1820). However, matched control sandstone samples show that the background 206Pb/207Pb isotope ratio (1.1670 ± 0.003) is distinctly different. This would indicate that both the sandstone and fracture infill underlying the historical smelting site contain a substantial proportion of Pb that has been derived from the overlying contamination.The application of total Pb concentrations along the core and isotope analysis suggest that anthropogenically derived Pb from the smelting site (that was operated between 665 and 445 a BP) has migrated to a depth of 4.50 m. Assuming a uniform migration rate and a mean time of migration of 555 a, then the mean migration rate is estimated to be 8 ± 2 mm/a.The proportion of natural versus anthropogenic Pb in the samples has been estimated from small variations in the 206Pb/207Pb isotope ratio. If the slag is considered to contain 100% anthropogenic Pb and the uncontaminated sandstone considered to contain 100% natural Pb, the linear interpolation can be applied between the 2 end members of the isotope ratio. The use of this approach to the 206Pb/207Pb ratio measurements has shown that 88% of the Pb in the contaminated sandstone (i.e. 69 ppm from a mean total Pb concentration of 78.5 ppm) has been derived from the anthropogenic Pb at the surface. For the fracture infill sample taken at a depth of 4.50 m, and with a total Pb concentration of 270 ppm, the % of Pb that has been derived from the slag wastes is approximately 98% (equivalent to 265 ppm Pb). The remaining Pb in both these samples (9.4 and 5 ppm, respectively) is deduced to have originated from the natural background concentration of Pb in the sandstone.The closeness of these estimates to the measured background concentration, suggests that a simple two-source model of Pb contamination is valid for this site.  相似文献   

3.
若尔盖高原牧场处于中国偏远洁净高海拔地区,大气沉降是污染物主要来源途径之一。由于季风的影响,污染源的辨析较为困难。本文通过多点大气气溶胶不同季节同时采样方式,利用热电离固体同位素质谱仪可有效校正质谱分析中同位素分馏效应的优点,对若尔盖地区土壤和大气气溶胶的铅同位素比值进行精确分析,并结合季风特征对该地区污染物的来源进行解析。结果表明:土壤的208Pb/204Pb比值变化范围为38.79059±0.00194~38.94461±0.00135,206Pb/207Pb为1.18551±0.00002~1.19362±0.00002;大气气溶胶的208Pb/204Pb比值变化范围为37.49571±0.00117~38.48980±0.00105,206Pb/207Pb为1.12894±0.00001~1.16734±0.00001。该地区土壤铅同位素的特征是放射成因铅高,来自于自身天然存在的岩石矿物,与大气污染关系不大;大气气溶胶的铅同位素组成与土壤差异较大,显示为多元混合模式,受到了天然物质和人类活动来源的混合影响,机动车尾气及来自北部(兰州)和西北部(青海、新疆、哈萨克斯坦、俄罗斯)的大气远程运移是若尔盖大气气溶胶及污染物质的主要来源。  相似文献   

4.
On 25 April 1998 the tailings dam of the Aznalcóllar mine burst, a great quantity of pyrite waste sludge and acid water was spilled reaching the vicinity of the Doñana National Park. In surface and ground water samples taken a week after dam breaking, metals, trace elements and Pb isotopic ratios (206Pb/207Pb and 208Pb/206Pb) were analysed. In September 1998 a second sampling survey was carried out. The surface waters have a similar isotopic composition as the lead contained in the pyrite from the Aznalcóllar mine. The polluted groundwater of the Guadiamar aquifer also shows the influence of the mining origin of the lead. Lead isotope ratios (206Pb/207Pb and 208Pb/206Pb) in the groundwater of the Almonte-Marismas are very low and they differ clearly from the rest of groundwater samples. A further group of wells has a lead isotope composition intermediate between the Aznalcóllar mine and the atmospheric aerosols of the Iberian Peninsula.  相似文献   

5.
The organic horizon (the mor layer) of podzolized boreal forest soils has accumulated atmospheric fallout of mercury and lead over centuries, resulting in current concentrations close to levels where negative effects on soil biota are thought to occur. To what extent the pollution history is preserved in the stratigraphy of this horizon is not well known. In this study we asses whether the chronology of a large historic pulse of atmospheric pollution emitted from the Rönnskär smelter in northern Sweden, particularly between 1950 and 1980, is preserved within the stratigraphy of the mor layer, which is typically 5-cm thick. Vertical sub-sampling (?5 mm) of five mor profiles sampled along a 100-km pollution gradient away from the smelter are analyzed for mercury and lead concentrations, spheroidal carbonaceous particles from fossil fuel combustion (SCPs) and stable lead isotopes (206Pb/207Pb and 208Pb/207Pb). Their vertical distribution is compared with the temporal variations in atmospheric inputs reconstructed for the last ∼100 years from analyses of an ombrotrophic peat core and a varved lake sediment core sampled within a distance of 50 km of the smelter. The mor profiles situated ?12 km from the smelter record the pollution history of the smelter. There is a 20 to 40-times enrichment of Hg, Pb and SCP at the transition in the O-horizon from the F- to H-layer compared to the basal part and a distinct peak in the 206Pb/207Pb ratio (∼1.22) in the F-layer. The mor profiles situated outside the historical contamination range of the smelter (80 and 100 km away) record no obvious influence from the Rönnskär smelter, instead their vertical 206Pb/207Pb profiles follow the general regional pollution history in northern Sweden. We conclude that the mor layer preserves a record of atmospheric Hg, Pb and SCP inputs and due to low leaching rates this organic horizon serves as a semi-archive of atmospheric Hg and Pb pollution. We stress the need of including this property in the existing ‘black-box’ models predicting the fate of Hg and Pb within contaminated boreal forest soils.  相似文献   

6.
To discriminate possible anthropogenic and lithogenic sources of Pb in Lower Silesia (SW Poland), the Pb isotope composition was investigated in a spectrum of rocks and anthropogenic materials as well as within 10 soil profiles. Silicate rocks in Lower Silesia have 206Pb/207Pb ratios that vary from 1.17 for serpentinites to 1.38 for gneisses, and this variability is reflected in the isotope composition of the mineral soil horizons. The Pb isotope composition of coals, ores and anthropogenic materials (slags and fly ashes) is rather uniform, with 206Pb/207Pb ratios ranging from 1.17 to 1.18. Similar ratios were observed in ore and coal samples from Upper Silesia. The O soil horizons also have uniform 206Pb/207Pb ratios of 1.17–1.18 and the heterogeneity of the 206Pb/207Pb ratios increases with depth in the soil profiles. Five soils, with varying Pb concentrations, analysed far from contamination centres, show consistent, approximately 2-fold enrichment in Pb concentration from the C to A horizons, which is consistent with natural re-distribution of Pb within the profiles. The increase in the Pb concentration is accompanied by a decrease in 206Pb/207Pb ratios, also attributed to natural Pb isotope fractionation. Four soil profiles from industrial areas show variable enrichments in Pb concentrations and these are attributed to anthropogenic input from air-borne pollutants or even slag particles at smelting sites. The implication is that a lithogenic Pb source can deviate from the basement rock composition, and detailed isotope characteristics of the geological background and natural enrichments in soils are often needed to determine the lithogenic/anthropogenic proportions of Pb in soils.  相似文献   

7.
Moss, O and C horizons of podzols, mainly forming complementary sample triplets, as well as filter residues of molten snow from northern Norway, northern Finland and NW Russia have been analyzed by TIMS for their Pb isotopic composition in order to study the impacts of local geogenic/anthropogenic sources and long range atmospheric transport on the Pb balance in the European Arctic. Samples were taken along two N-S transects covering an area of ∼188.000 km2, including both pristine environments in the W and certain regions towards the E severely contaminated by heavy metal emissions originating from large nickel smelters and processing plants in NW Russia.The lead in moss and O horizon samples clearly reflects atmospheric deposition, as it displays overall uniform isotope ratios and is decoupled from the geogenic background, i.e. the underlying mineral soils in the C horizon. Moss and O horizon samples from the eastern N-S transect are isotopically indistinguishable from those taken along the western transect but their Pb concentrations tend to be ∼2 times higher. This points to considerable contamination originating from the nearby Russian industrial and urban centers. However, isotopic signals of emissions from individual industrial point sources cannot be unambiguously identified because they lack characteristic isotope signatures. Pb derived from gasoline additives is swamped by Pb from other sources and can also be excluded as a major contributor to the environmental Pb in the European Arctic.Overall, the Pb isotopic signatures of moss and O horizon overlap values recorded in atmospheric lead all over central and southern Europe, more than 2000 km south of the study area. This may be taken as indicating continent-wide mixing of Pb derived from similar sources in the atmosphere or as reflecting economic globalization, or both. O horizon samples, which accumulate lead over 20-30 yr, conform to a distinct Pb isotope reference line in 207Pb/206Pb vs. 208Pb/206Pb space (“European Standard Pollution,” ESP) defined by atmospheric Pb considered to be representative for the technical civilization in Europe. Conversely, the Arctic moss samples with a lifetime of <3 yr display a deviating linear trend reflecting a recent change of atmospheric input towards significantly more radiogenic Pb derived from Mississippi Valley-type ores in the U.S., fully compatible with signatures found in epiphytic lichens from Canada, but also in Pb from urban waste incinerators in central Europe. Considering the elevated Pb concentrations in moss collected along the eastern N-S transect, this congruence indicates that the Pb in moss of the European Arctic most probably originates from the nearby Russian centers of urbanization and not from transatlantic transport. We therefore suspect imported industrial goods and their subsequent attrition to be a more plausible explanation for the appearance of MVT lead in Europe.  相似文献   

8.
《Applied Geochemistry》2006,21(4):563-579
Element concentrations, element ratios and Pb and Zn isotope data are reported for different geologic samples (barren and ore-bearing granites and host rocks), technogenic products (ore concentrates and tailings) and biologic samples (lichens and birch leaves) from the Orlovka–Spokoinoe mining district, Eastern Transbaikalia, Russia, with the aim to trace the sources of Pb and Zn at a local level within the mining site. Lichens and birch leaves were used as receptors of contamination within the mining site. Pb/Zr and Zn/Zr values indicated Pb and Zn enrichment relative to host rocks. Zn isotope data of 15 geologic and 11 lichen samples showed different Zn isotopic signatures with the total range for the geologic suite of −0.4‰ to +1.2‰ and for lichens of +0.4‰ to +1.4‰ in δ66Zn relative to Lyon JMC Zn standard. The source of isotopically heavy Zn within the Orlovka–Spokoinoe mining site could be potentially associated with long-range atmospheric aerosols that also contributed Pb to the studied mining site. Our results demonstrated that Zn isotopes might be used as new tools for Zn source assessment.  相似文献   

9.
Soil O and C horizon samples (N = 752) were collected at a sample density of 1 site/36 km2 in Nord-Trøndelag and parts of Sør-Trøndelag (c. 25,000 km2), and analysed for Pb and three of the four naturally occurring Pb isotopes (206Pb, 207Pb and 208Pb) in a HNO3/HCl extraction. Soil O and C horizons are decoupled in terms of both Pb concentrations and Pb isotope ratios. In the soil C horizon the Grong-Olden Culmination, a continuous exposure of the Precambrian crystalline basement across the general grain of the Caledonian orogen, is marked by a distinct 206Pb/207Pb isotope ratio anomaly. No clear regional or even local patterns are detected when mapping the Pb isotope ratios in the soil O horizon samples. Variation in the isotope ratios declines significantly from the soil C to the O horizon. On average, Pb concentrations in the O horizon are four times higher and the 206Pb/207Pb isotope ratio is shifted towards a median of 1.15 in comparison to 1.27 in the C horizon. It is demonstrated that natural processes like weathering in combination with plant uptake need to be taken into account in order to distinguish anthropogenic input from natural influences on Pb concentration and the 206Pb/207Pb isotope ratio in the soil O horizon.  相似文献   

10.
Systematic variations in the Cd and Pb isotope ratios in polluted topsoils surrounding the Jinding Pb–Zn mine in China were measured so that the sources of the metals could be traced. The average δ114/110Cd value and 206Pb/207Pb isotope ratio in background soils from the region were +0.41‰ and 1.1902, respectively, whereas the contaminated soil samples had different values, with the δ114/110Cd values varying between −0.59‰ and +0.33‰ and the 206Pb/207Pb isotope ratios varying between 1.1764 and 1.1896. We also measured the Cd and Pb isotopic compositions in oxide ores, sulfide ores, and slags, and found that binary mixing between ores and background soils could explain almost all of the variations in the Cd and Pb isotope ratios in the contaminated soils. This suggests that Cd and Pb pollution in the soils was mainly caused by the deposition of dust emitted during anthropogenic activities (mining and refining). The Pb and Cd isotope ratios clearly showed that contamination in soils in the northeastern part of the area was caused by surface mines and zinc smelters and their slagheaps, while contamination in soils in the southwestern part of the area also came from tailing ponds and underground mines. The main area of soil polluted by dust from Pb–Zn mining processes roughly extended for up to 5 km from the mine itself.  相似文献   

11.
Lead (Pb) isotopic compositions and concentrations, and barium (Ba) and indium (In) concentrations have been determined at monthly resolution in five Law Dome (coastal Eastern Antarctica) ice core sections dated from ∼1757 AD to ∼1898 AD. ‘Natural’ background Pb concentrations in ∼1757 AD average ∼0.2 pg g−1 and can be attributed to mineral dust and volcanic emissions, with 206Pb/207Pb ratios reaching up to 1.266 ± 0.002. From ∼1887 AD to ∼1898 AD, Pb concentrations reached ∼5 pg g−1 and 206Pb/207Pb ratios decreased to 1.058 ± 0.001 as a result of additional inputs of Pb from anthropogenic sources. Seasonal variability in the late 1880s has been investigated by decoupling volcanic Pb from the total measured Pb concentrations, revealing spring and autumn maxima, and consistent winter minima, in anthropogenic Pb and mineral dust (Ba) concentrations. We link this variability to the annual cycle in the position and strength of the Antarctic Circumpolar Trough and, the Southern Ocean westerly winds to the north of the trough region. During the autumn and spring seasons, these systems increase in strength, transporting more impurity laden air from the Southern Hemisphere continental regions to Eastern Antarctica and Law Dome. As this Pb is isotopically identical to that emitted from south-eastern Australia (Broken Hill, Port Pirie) this implies a relatively direct air trajectory pathway from southern Australia to Law Dome (Eastern Antarctica).  相似文献   

12.
A peat core from an ombrotrophic bog documents the isotopic evolution of atmospheric Pb in central Ontario since AD 1804 ± 53 (210Pb dating). Despite the introduction of unleaded gasoline in the mid-1970’s, the ratio 206Pb/207Pb in atmospheric deposition has not increased as expected, but rather continues to decline. In fact, snowpack sampling (2005 and 2009) and rainwater samples (2008) show that the isotopic composition of atmospheric Pb today is often far less radiogenic than the gasoline lead that had been used in Canada in the past. The peat, snow, and rainwater data presented here are consistent with the Pb isotope data for aerosols collected in Dorset in 1984 and 1986 which were traced by Sturges and Barrie (1989) to emissions from the Noranda smelter in northern Quèbec, Canada’s largest single source of atmospheric Pb. Understanding atmospheric Pb deposition in central Ontario, therefore, requires not only consideration of natural sources and past contributions from leaded gasoline, but also emissions from metal smelting and refining.Lead in the streams which enter Kawagama Lake today (206Pb/207Pb = 1.16 − 1.19) represents a mixture between the natural values (1.191 − 1.201 estimated using pre-industrial lake sediments) and the values found in the humus layer of the surrounding forest soils (206Pb/207Pb = 1.15 − 1.19). In the lake itself, however, Pb is much less radiogenic (206Pb/207Pb as low as 1.09) than in the streams, with the dissolved fraction less radiogenic than particulate material. The evolution of Pb isotope ratios within the watershed apparently reflects preferential removal by sedimentation of comparatively dense, radiogenic, terrestrial particles (derived from the mineral fraction of soils) from the humus particles with lower ratios of 206Pb/207Pb (because of atmospheric Pb contamination). Despite the contemporary enrichments of Pb in rain and snow, concentrations of dissolved Pb in the lake are extremely low (sometimes below 10 ng/l), with Pb concentrations and Pb/Sc ratios approaching “natural” values because of efficient binding to particles, and their subsequent removal in the watershed.  相似文献   

13.
Abundances of 35 elements and ions were determined by inductively coupled plasma mass spectrometry, inductively coupled plasma atomic emission spectroscopy, and ion chromatography, in samples of snowpack obtained using ultraclean procedures, along three 50-km radial transects emanating from the Horne base metal smelter in Rouyn-Noranda, Quebec. This was done to constrain: what is emitted; regional background concentrations of elements in snow; the rate of anthropogenic deposition on the surrounding landscape; how far emissions are transported; and what processes control their deposition. The approach used is at least as effective as methods based on isotopic ratios but has the added advantage of providing direct constraint on a large suite of elements, and of being independent of changes in the isotopic composition of emissions. Reproducibility of the method was determined using field duplicates and blanks. This accounts for snow heterogeneity, analytical precision, reagent quality, and sample handling and was determined to be ±20%.Concentrations of Cu, Pb, and Zn near the smelter are 525, 353, and 149 μg/Lmeltwater, respectively, and drop to 2.1, 3.5, and 3.1 μg/L by 45 km distance. The level of enrichment of these elements, relative to upper crustal abundances, similarly drops from about 10,000 to 100 from proximal through to distal sites, forming an “enrichment gradient.” This is the result of a binary mix of smelter emissions and regional background concentrations. Elements that display a significant gradient must therefore be emitted by the smelter. This method shows that Cu, Ag, In, Sb, Pb, As, Tl, Mo, Zn, Cd, Co, Be, Ni, Na, Ba, Fe, Cr, V, Ti, Y, Al, U, Ce, Li, S, La, and Sr are deposited on the landscape by the smelter. For many elements, the slope of this binary mixing line is still non-zero at a distance of 50 km, indicating that the impact of the smelter is still detectable, and that regional background levels have not yet been reached. Data from more distant sites are used to estimate regional background concentrations to be 1.1, 1.7, and 1.6 μg/Lmeltwater for Cu, Pb, and Zn, respectively.We quantify the partitioning of elements between the dissolved phase (meltwater) and the solid phase (particulates) in melted snow. It varies with distance from the smelter but is element specific. Representative end-members are: Tl, Cu, Pb, Zn, and Sb with 78, 68, 67, 55, and 20% in the dissolved phase near the smelter, respectively, vs. 4, 60, 73, 80, 58% at distances greater than 35 km. This is due to changes in mineralogy and particle size. The significance of this is, that for those elements with high variation such as Tl and Sb, only the total load (meltwater + particulate) can reliably reflect atmospheric deposition. For those elements that vary little such as Cu and Pb, measurement of just the dissolved load (meltwater) can be used as an adequate proxy for the total deposition.Observed patterns of deposition suggest that inside 15 km radius, it occurs by wet+dry mechanisms whereas beyond 15 km wet deposition dominates. Emissions transported beyond 15 km are therefore available for long-range transport during dry weather and likely have an atmospheric residence time similar to that of water vapour. A well fitting mathematical model supports this interpretation. Using modelled background concentrations, the model can account for only 49, 15, 23, and 9% of reported emissions of Cu, Pb, Zn, and Cd within 50 km of the smelter, respectively. Using lower (minimal) background concentrations based on observations at more distant sites, these numbers increase to 78, 19, and 43%, respectively (Cd excluded), and can be considered maximums. The rest of the emissions are therefore transported further distances during dry weather.  相似文献   

14.
Three soil profiles taken from the Hartwood Research Station in Central Scotland have been analyzed using chemical digestion and extraction techniques to investigate the chemical association of heavy metals deposited from the atmosphere. Total digestion, EDTA extraction and the BCR (Bureau Communitaire de Reference) sequential extraction procedure were used. In addition, lead isotope ratios in the whole soils and in the fractions from the sequential extraction procedure were measured using thermal ionisation mass spectrometry. All the digestion and extraction procedures gave clear indication of enhanced concentrations of heavy metals in surface soils, in particular for lead and zinc. Whereas total digestion gave a good indication of the heavy metal status of the soils, the extraction procedures were necessary to provide information on chemical association of the metals with soil components, information needed to understand the soil processes involved in mobilization of metals. Lead isotope analysis of the whole soils revealed a consistent picture of lower 206Pb/207Pb ratios in surface soils (1.140-1.147) than in soils at 20-30 cm depth (1.182-1.190). The steady progression from the lower to higher ratios down the profile was clear indication that anthropogenic lead had penetrated to some degree into the deeper soils. The combination of sequential extraction and lead isotope analysis proved to be a powerful approach to studying this effect in more detail and showed that the fractions extractable from 20 to 30 cm soils contained lead with much lower 206Pb/207Pb ratios (1.174-1.178) than the residual fraction (1.196-1.200). As the extractable fractions contained ≥85% of the lead in the soil, a substantial portion of lead at 20-30 cm depth was of anthropogenic origin. The 206Pb/207Pb ratios of 1.174-1.178 found in the extractable fractions suggested that the mobile component of the anthropogenic lead was that deposited before the introduction of leaded petrol.  相似文献   

15.
《Applied Geochemistry》1997,12(5):607-623
The aim of this study is to characterize the processes and phases which control migration and retention of rare earth elements (REE) in a heavy metal contaminated soil. In addition to concentration data, we used Pb, Sr and Nd isotopic compositions in order to distinguish between natural and anthropogenic trace metals and to characterize the phases leached away during the sequential extraction procedure.The samples were sequentially extracted in 3 steps with 1 N acetic acid (HAc), 1 N HCl and 1 N HNO3. The Pb isotope data showed that anthropogenic Pb had mainly been retained in the uppermost 10 cm by the organic matter of the topsoil. The87Sr/86Sr ratios of the HAc extracts are almost constant and indicate that soil carbonate is derived from regionally outcropping carbonate-rich sediments. Most HCl and HNO3 extracts have more radiogenic Sr isotopic compositions, but it is unclear whether this reflects a growing influence of anthropogenic or silicate-derived Sr.The depth distribution of the REE is mainly controlled by two different parameters: soil pH for the HAc extractable REE and FeMn oxides for the REE in the HCl and HNO3 extracts. A part of the HNO3 extractable REE was also bound to the organic matter of the topsoil. The REE concentrations in the HAc extractable phase increase with depth and increasing soil pH, which indicates that they are derived from the surface and hence are of anthropogenic origin. This is confirmed by143Nd/144Nd isotope ratios which show a mixing between a natural end-member at the top and an anthropogenic end-member at the base of the profile. We assume that the anthropogenic REE were transported in dissolved form as carbonate complexes and then precipitated during downward migration as soil pH increased.  相似文献   

16.
 Heavy metal and metalloid concentrations within stream-estuary sediments (<180-μm size fraction) in north-eastern New South Wales largely represent natural background values. However, element concentrations (Ag, As, Cd, Cr, Cu, Hg, Ni, Pb, Sb, Zn) of Hunter River sediments within the heavily industrialized and urbanized Newcastle region exceed upstream background values by up to one order of magnitude. High element concentrations have been found within sediments of the Newcastle Harbour and Throsby Creek which drains into urbanized and light industry areas. Observed Pb enrichments and low 208Pb/204Pb, 207Pb/204Pb and 206Pb/204Pb ratios are likely caused by atmospheric deposition of Pb additives from petrol and subsequent Pb transport by road run-off waters into the local drainage system. Sediments of the Richmond River and lower Manning, Macleay, Clarence, Brunswick and Tweed River generally display no evidence for anthropogenic heavy metal and metalloid contamination (Ag, As, Cd, Cr, Cu, Hg, Ni, Pb, Sb, Zn). However, the rivers and their tributaries possess localized sedimentary traps with elevated heavy metal concentrations (Cu, Pb, Zn). Lead isotope data indicate that anthropogenic Pb provides a detectable contribution to investigated sediments. Such contributions are evident at sample sites close to sewage outlets and in the vicinity of the Pacific Highway. In addition, As concentrations of Richmond River sediments gradually increase downstream. This geochemical trend may be the result of As mobilization from numerous cattle-dip sites within the region into the drainage system and subsequent accumulation of As in downstream river and estuary sediments. Received: 5 September 1997 · Accepted: 4 November 1997  相似文献   

17.
Concentrations of Fe, Mn, Cu, Zn, U and Pb, and stable Pb isotopes 206Pb, 207Pb and 208Pb were measured via inductively coupled plasma mass spectrometry in sediments, water and freshwater mussels (Velesunio angasi) from two catchments in the Alligator Rivers Region, Australia. Sediment U and Pb concentrations were higher in Magela Creek downstream than upstream of the Ranger U mine due to the mineralised nature of the catchment and potential local input of sediment from the mine site. Water metal concentrations were highest in Georgetown Creek, which is a tributary of Magela Creek and part drains the Ranger mine site, but there was little difference in concentrations between the Magela Creek upstream and downstream sites. Metal concentrations in mussels collected immediately upstream and downstream of the mine site also showed little difference, whereas Pb isotope ratios displayed a very distinct pattern. The 206Pb/207Pb and 208Pb/207Pb isotope ratios were more uranogenic downstream than upstream of the site and also more uranogenic than ratios measured in Sandy Billabong, a reference billabong in a catchment not influenced by U mineralisation. Isotope ratios were also more uranogenic in younger mussels, potentially due to the increasing footprint of the mine site over the past decade. The most uranogenic ratios were found in mussels from Georgetown Creek and at a site approximately 2 km downstream. At Mudginberri Billabong, approximately 12 km downstream of the Ranger mine, the relative contribution of uranogenic Pb to the total Pb concentration in mussels was small and overwhelmed by the input of industrial Pb with a Broken Hill type Pb signature. Whereas metal uptake by and thus concentrations in mussel flesh are influenced by water chemistry, mussel condition and metabolic rates, Pb isotope ratios are independent of these factors and provide a powerful means of source apportionment of contaminants in mussels and waterways, in particular in an U mining environment.  相似文献   

18.
The Pb, Sr and Nd isotopic compositions of biomonitors (lichen, moss, bark) and soil litter from different regions in the Rhine valley, as well as of <0.45 μm particles separated out of ice of the Rhône and Oberaar glaciers and lichens from the Swiss Central Alps, have been determined in order to deduce the natural baseline of the atmospheric isotopic compositions of these regions, which are suggested to be close to the isotopic compositions of the corresponding basement rocks or soils at the same sites. 206Pb/207Pb and 87Sr/86Sr isotope ratios are positively correlated. Most polluted samples from traffic-rich urban environments have the least radiogenic Pb and Sr isotopic compositions with 206Pb/207Pb and 87Sr/86Sr ratios of 1.11 and 0.7094, respectively. These ratios are very different from those of the atmospheric baseline for the Vosges mountains and the Rhine valley (206Pb/207Pb: 1.158–1.167; 87Sr/86Sr: 0.719–0.725; εNd: −7.5 to −10.1). However, this study indicates that the baseline of the atmospheric natural Pb and Sr isotopic compositions is affected by anthropogenic (traffic, industrial and urban) emissions even in remote areas. Lichen samples from below the Rhône and Oberaar glaciers reflect the baseline composition close to the Grimsel pass in the Central Swiss Alps (87Sr/86Sr: 0.714 − 0.716; εNd: −3.6 to −8.1). The 143Nd/144Nd isotope ratios are highly variable (8ε units) and it is suggested that the variation of the 143Nd/144Nd is controlled by wet deposition and aerosols originating from the regional natural and industrial urban environments and from more distant regions like the Sahara in North Africa. The least anthropogenetically affected samples collected in remote areas have isotopic compositions closest to those of the corresponding granitoid basement rocks.  相似文献   

19.
Sediments of the Lagoa Vermelha (Red Lake), situated in the Ribeira Valley, southeastern Brazil, are made of a homogeneous, organic-rich, black clay with no visible sedimentary structures. The inorganic geochemical record (Al, As, Ba, Br, Co,Cs, Cr, Fe, Mn, Ni, Rb, Sc, Sb, V, Zn, Hg and Pb) of the lake sediments was analyzed in a core spanning 2430 years. The largest temporal changes in trace metal contents occurred approximately within the last 180 years. Recent sediments were found to be enriched in Pb, Zn, Hg, Ni, Mn, Br and Sb (more than 2-fold increase with respect to the “natural background level”). The enhanced accumulation of Br, Sb, and Mn was attributed to biogeochemical processes and diagenesis. On the other hand, the anomalous concentrations of Pb, Zn, Hg and Ni were attributed to pollution. As Lagoa Vermelha is located in a relatively pristine area, far removed from direct contamination sources, the increased metal contents of surface sediments most likely resulted from atmospheric fallout. Stable Pb isotopes provided additional evidence for anthropogenic contamination. The shift of 206Pb/207Pb ratios toward decreasing values in the increasingly younger sediments is consistent with an increasing contribution of airborne anthropogenic lead. In the uppermost sediments (0-10 cm), the lowest values of the 206Pb/207Pb ratios may reflect the influence of the less radiogenic Pb from the Ribeira Valley District ores (206Pb/207Pb between 1.04 and 1.10), emitted during the last 50 years.  相似文献   

20.
Zinc isotope ratios were measured in the top sections of dated ombrotrophic peat cores in Finland to investigate their potential as proxies for atmospheric sources and to constrain post depositional processes affecting the geochemical record. The peat deposits were located in Hietajärvi, a background site well away from any point pollution source and representing ‘background’ conditions, in Outokumpu, next to a mining site, and in Harjavalta, next to a smelter. Measured total concentrations, calculated excess concentrations and mass balance considerations suggest that zinc is subjected to important biogeochemical cycling within the peat. Significant isotopic variability was found in all three peat bogs, with heavier zinc in the deeper and lighter zinc in the upper sections. Isotope ratios and concentrations correlated in the two peats located next to dominant point sources, i.e. the smelting and mining site, suggesting that zinc isotopes trace pollution sources. Concentration and isotope peaks were offset from the period of mining and smelting activity, supporting migration of zinc down the profile. The δ66ZnJMC (where δ66Zn = [(66Zn/64Zn)sample/(66Zn/64Zn)JMC-standard − 1] × 103) of the top section sample at the remote Hietajärvi site was 0.9‰ and we suggest this represents the regional background isotope signature of atmospheric zinc. The deeper sections of the peat cores show isotopically heavier zinc than any potential atmospheric source, indicating that post depositional processes affected the isotopic records. The large variations encountered (up to 1.05‰ for δ66Zn) and Rayleigh modelling imply that multiple fractionation of zinc during diagenetic alterations occurs and nutrient recycling alone cannot explain the fractionation pattern.We propose that zinc isotopes are amenable to identify different atmospheric zinc sources, including zinc derived from anthropogenic activities such as mining and smelting, but multiple biogeochemical processes seriously affect the record and they need to be evaluated and assessed carefully if zinc isotopes are used in terrestrial paleorecords.  相似文献   

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