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1.
As a consequence of deposition of atmospheric pollution, the lead concentration in the mor layer (the organic horizon) of remote boreal forest soils in Sweden is raised far above natural levels. How the mor will respond to decreased atmospheric pollution is not well known and is dependent on future deposition rates, downward migration losses and upward fluxes in the soil profile. Plants may contribute to the upward flux of lead by ‘pumping’ lead back to the mor surface through root uptake and subsequent litter fall. We use lead concentration and stable isotope (206Pb, 207Pb and 208Pb) measurements of forest vegetation to quantify plant uptake rates from the soil and direct from the atmosphere at two sites in northern Sweden; an undisturbed mature forest and a disturbed site with Scots pine (Pinus sylvestris) growing on a recently exposed mineral soil (C-horizon) containing a minimum of atmospherically derived pollution lead. Analyses of forest mosses from a herbarium collection (spanning the last ∼100 yr) and soil matrix samples suggest that the atmospheric lead deposited on plants and soil has an average 206Pb/207Pb ratio of 1.15, while lead derived from local soil minerals has an average ratio of ∼1.47. Since the biomass of trees and field layer shrubs has an average 206Pb/207Pb ratio of ∼1.25, this indicates that 70% ± 10% of the inventory of 1 ± 0.8 mg Pb m−2 stored in plants in the mature forest originates from pollution. Needles, bark and apical stemwood of the pine growing on the disturbed soil, show lower 206Pb/207Pb ratios (as low as 1.21) than the roots and basal stemwood (having ratios > 1.36), which indicate that plants are able to incorporate lead directly from the atmosphere (∼50% of the total tree uptake). By partitioning the total uptake of lead into uptake from the atmosphere and different soil layers using an isotopic mixing model, we estimate that ∼0.03 ± 0.01, 0.02 ± 0.01 and 0.05 ± 0.01 mg Pb m−2 yr−1 (mean ± SD), is taken up from the mor layer, the mineral soil and the atmosphere, respectively, by plants in the undisturbed mature forest. These small fluxes, which are at least a magnitude lower than reported downward migration losses, suggest that plant uptake will not strongly prolong the self-cleaning rate of the mor layer.  相似文献   

2.
Anthropogenic Pb affects the environment worldwide. To understand its effect on forest ecosystem, Pb isotope ratios were determined in precipitation, various components of vegetation, the forest floor, soil and parent material in a Japanese cedar (Cryptomeria japonica D. Don) forest stand. The average 206Pb/207Pb ratio in bulk precipitation was 1.14 ± 0.01 (mean ± SD), whereas that in the subsoil (20–130 cm) was 1.18 ± 0.01. Intermediate ratios ranging from 1.15 to 1.16 were observed in the vegetation, the forest floor, and the surface soil (0–10 cm). Using the 206Pb/207Pb ratios, the contribution of anthropogenic sources to Pb accumulated in the forest were estimated by the simple binary mixing model. Sixty-two percent of the Pb in the forest floor, 71% in the vegetation, and 55% in the surface soil (0–10 cm) originated from anthropogenic sources, but only 16% in the sub-surface soil (10–20 cm) was anthropogenic. These results suggest that internal Pb cycling occurs mainly between surface soil and vegetation in a Japanese cedar ecosystem, and that anthropogenic Pb strongly influences Pb cycling. Although the Japanese cedar ecosystem has a shallow forest floor, very little atmospherically derived Pb migrated downward over 10 cm in depth.  相似文献   

3.
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   

4.
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   

5.
The magnitude and sources of lead (Pb) pollution in the Gulf of California Ecoregion (GCE) in northwest Mexico were evaluated using various samples collected from urban and rural areas around two typical subtropical coastal ecosystems. Lead concentrations and isotopic compositions (206Pb/207Pb, 208Pb/207Pb, 206Pb/204Pb and 208Pb/204Pb) were measured using high resolution inductively-coupled plasma mass spectrometry (HR-ICP-MS) and thermal ionization mass spectrometry (TIMS). Urban street dust (157 ± 10.1 μg g− 1) was heavily enriched with Pb, compared to the Pb enrichment of agricultural soils (29.0 ± 16.0 μg g− 1) and surface estuary sediments (35.6 ± 15.4 μg g− 1), all of which contained higher Pb concentrations than found in the natural bedrock (16.0 ± 5.0 μg g− 1). Pb concentrations in SPM (> 95% of total Pb) were significantly higher in sewage effluent (132 ± 49.9 μg g− 1) than in agricultural effluents (29.3 ± 5.9 μg g− 1), and river runoff (7.3 ± 4.2 μg g− 1). SPM in estuary water column averaged 68.3 ± 48.0 μg g−1. The isotopic composition of Pb (206Pb/207Pb, 208Pb/207Pb) in rural samples of aerosols (1.181 ± 0.001, 2.444 ± 0.003) and soil runoff (1.181 ± 0.003, 2.441 ± 0.004) was comparable to that of natural Pb-bearing bedrock (1.188 ± 0.005, 2.455 ± 0.008); while urban samples of aerosols, street dust, and sewage (1.190–1.207, 2.452–2.467) showed a significant contribution from automotive emissions from past leaded gasoline combustion (1.201 ± 0.006, 2.475 ± 0.005). The absence of lead from fertilizer (1.387 ± 0.008, 2.892 ± 0.005) suggests that this mixture is not representative of the GCE. A mixing model revealed that the Pb content in the environmental samples is predominantly derived from natural weathering and the past leaded gasoline combustion with the later influence of inputs from a more radiogenic source related with anthropogenic lead of North American origin (1.21 ± 0.02; 2.455 ± 0.02).  相似文献   

6.
Lead concentrations were determined in samples of soil B-horizon (N = 258), forest-floor humus (O-horizon, N = 259), grass (Avenella flexuosa, N = 251) and spruce (Picea abies, N = 253) needles (2nd year) collected at the same locations evenly spread over the territory of the Czech Republic at an average density of 1 site/300 km2. Median Pb concentrations differ widely in the four materials: soil B-horizon: 27 mg/kg (3.3-220 mg/kg), humus: 78 mg/kg (19-1863 mg/kg), grass: 0.37 mg/kg (0.08-8 mg/kg) and spruce needles: 0.23 mg/kg (0.07-3 mg/kg). In the Pb distribution maps for humus, grass and spruce a number of well-known Pb-contamination sources are indicated by unusually high concentrations (e.g., the Pb smelter at Pribram, the metallurgical industry in the NE of the Czech Republic and along the Polish border, as well as the metallurgical industry in Upper Silesia and Europe’s largest coal-fired power plant at Bogatynia, Poland). The ratio 206Pb/207Pb was determined in all four materials. The median value of the 206Pb/207Pb isotope ratio in the soil B-horizon is 1.184 (variation: 1.145-1.337). In both humus and grass the median value for the 206Pb/207Pb isotope ratio is 1.162 (variation: 1.130-1.182), in spruce needles the median ratio is 1.159 (variation: 1.116-1.186). In humus, grass and spruce needles the known contamination sources are all marked by higher 206Pb/207Pb isotope ratios in the maps. Furthermore, the soil B-horizon, humus, grass and spruce needles show distinctly different spatial distribution patterns of the 206Pb/207Pb isotope ratios. The B-horizon does not provide a viable background value for metal concentrations in the O-horizon or plant materials. None of the maps provides evidence for the importance of traffic-related emissions for the observed isotope ratios at the scale of the Czech Republic.  相似文献   

7.
This paper assesses the role of airborne pollution and natural geological sources for lead enrichment in lake sediments and in surface soils of boreal forests. This assessment is based on analyses of stable lead isotopes (206Pb and 207Pb) and lead concentrations in sediment cores (>30 lakes), ombrotrophic peat and soil samples in Sweden. The 206Pb/207Pb ratio and concentration profiles in the sediment cores change synchronously over the last 3,000 years in different lakes, temporal concentration changes in sediments and peat deposits are very consistent, and these temporal concentration changes coincide well with the history of lead production in Europe. The 206Pb/207Pb ratio is almost the same in all soil mor samples (1.152ǂ.009; n=94), and similar to values recorded in aerosols, despite very high and different 206Pb/207Pb ratio of the mineral soil in the C-horizon (1.3-1.7). This study provides evidence that lead enrichment in recent sediments and peat, and in the mor layer are caused by deposition of pollution lead and not natural processes.  相似文献   

8.
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   

9.
Extreme U and Pb isotope variations produced by disequilibrium in decay chains of 238U and 232Th are found in calcite, opal/chalcedony, and Mn-oxides occurring as secondary mineral coatings in the unsaturated zone at Yucca Mountain, Nevada. These very slowly growing minerals (mm my−1) contain excess 206Pb and 208Pb formed from excesses of intermediate daughter isotopes and cannot be used as reliable 206Pb/238U geochronometers. The presence of excess intermediate daughter isotopes does not appreciably affect 207Pb/235U ages of U-enriched opal/chalcedony, which are interpreted as mineral formation ages.Opal and calcite from outer (younger) portions of coatings have 230Th/U ages from 94.6 ± 3.7 to 361.3 ± 9.8 ka and initial 234U/238U activity ratios (AR) from 4.351 ± 0.070 to 7.02 ± 0.12, which indicate 234U enrichment from percolating water. Present-day 234U/238U AR is ∼1 in opal/chalcedony from older portions of the coatings. The 207Pb/235U ages of opal/chalcedony samples range from 0.1329 ± 0.0080 to 9.10 ± 0.21 Ma, increase with microstratigraphic depth, and define slow long-term average growth rates of about 1.2-2.0 mm my−1, in good agreement with previous results. Measured 234U/238U AR in Mn-oxides, which pre-date the oldest calcite and opal/chalcedony, range from 0.939 ± 0.006 to 2.091 ± 0.006 and are >1 in most samples. The range of 87Sr/86Sr ratios (0.71156-0.71280) in Mn-oxides overlaps that in the late calcite. These data indicate that Mn-oxides exchange U and Sr with percolating water and cannot be used as a reliable dating tool.In the U-poor calcite samples, measured 206Pb/207Pb ratios have a wide range, do not correlate with Ba concentration as would be expected if excess Ra was present, and reach a value of about 1400, the highest ever reported for natural Pb. Calcite intergrown with opal contains excesses of both 206Pb and 207Pb derived from Rn diffusion and from direct α-recoil from U-rich opal. Calcite from coatings devoid of opal/chalcedony contains 206Pb and 208Pb excesses, but no appreciable 207Pb excesses. Observed Pb isotope anomalies in calcite are explained by Rn-produced excess Pb. The Rn emanation may strongly affect 206Pb-238U ages of slow-growing U-poor calcite, but should be negligible for dating fast-growing U-enriched speleothem calcite.  相似文献   

10.
At a watershed scale, sediments and soil weathering exerts a control on solid and dissolved transport of trace elements in surface waters and it can be considered as a source of pollution. The studied subwatershed (1.5 km2) was located on an As-geochemical anomaly. The studied soil profile showed a significant decrease of As content from 1500 mg kg−1 in the 135–165 cm deepest soil layer to 385 mg kg−1 in the upper 0–5 cm soil layer. Directly in the stream, suspended matter and the <63 μm fraction of bed sediments had As concentrations greater than 400 mg kg−1. In all these solid fractions, the main representative As-bearing phases were determined at two different observation scales: bulk analyses using X-ray absorption structure spectroscopy (XAS) and microanalyses using scanning electron microscope (SEM) and associated electron probe microanalyses (EPMA), as well as micro-Raman spectroscopy and synchrotron-based micro-scanning X-ray diffraction (μSXRD) characterization. Three main As-bearing phases were identified: (i) arsenates (mostly pharmacosiderite), the most concentrated phases As in both the coherent weathered bedrock and the 135–165 cm soil layer but not observed in the river solid fraction, (ii) Fe-oxyhydroxides with in situ As content up to 15.4 wt.% in the deepest soil layer, and (iii) aluminosilicates, the least concentrated As carriers. The mineralogical evolution of As-bearing phases in the soil profile, coupled with the decrease of bulk As content, may be related to pedogenesis processes, suggesting an evolution of arsenates into As-rich Fe-oxyhydroxides. Therefore, weathering and mineralogical evolution of these As-rich phases may release As to surface waters.  相似文献   

11.
Stable Pb-isotope ratios are widely used as tracers for Pb-sources in the environment. Recently, a few publications have challenged the predominating view of environmental applications of Pb-isotopes. Present applications of Pb-isotopic tracers in soils largely represent the northern hemisphere. This study focuses on tropical soils from Paraíba, north-eastern Brazil. Lead concentrations and Pb-isotopic signatures (both 7N HNO3) were determined at 30 sites along a 327 km E–W-transect, from the Atlantic coast at João Pessoa to some kilometers west of Patos, to identify possible processes for the observed (and anticipated) distribution pattern. Thirty samples each of litter (ORG) and top mineral soil (TOP) were taken on pasture land at suitable distance from roads or other potential contamination sources. Lead-content was determined by inductively-coupled plasma atomic emission spectrometry (ICP-AES) and the ratios of 206Pb/207Pb, 206Pb/208Pb, and 208Pb/207Pb by ICP-sector field mass spectrometry (ICP-SFMS). Both sample materials show similarly low Pb-concentrations with a lower median in the ORG samples (ORG 3.4 mg kg−1 versus TOP 6.9 mg kg−1). The 206Pb/207Pb ratios revealed a large spread along the transect with median 206Pb/207Pb ratios of 1.160 (ORG) and 1.175 (TOP). The 206Pb/207Pb ratios differ noticeably between sample sites located in the Atlantic Forest biome along the coast and sample sites in the inland Caatinga biome. The “forest” sites were characterised by a significant lower median and a lower spread in the 206Pb/207Pb and 206Pb/208Pb ratios compared to the Caatinga sites. Results indicate a very restricted influence of anthropogenic activities (individual sites only). The main process influencing the spatial variability of Pb-isotope ratios is supposed to be precipitation-dependent bioproductivity and weathering.  相似文献   

12.
Distribution of Tl, Zn, Cd, Pb, K, Ca, Mg and Mn and Pb isotopic composition in tree rings of Scots pine (Pinus sylvestris L.) from an area affected by primary Zn smelting (Olkusz, southern Poland) were investigated. Elevated concentrations of Tl (up to 0.8 mg kg−1) in pine trees imply that conifers tend to accumulate this metal to some extent. A generally positive relationship between soil and tree-ring Tl levels was identified. The Tl patterns in stem wood did not correspond to changes in Tl deposition; the lateral translocation of Tl in the sapwood and its accumulation at the sapwood-heartwood boundary (i.e., in the inner sapwood) is suggested. It is probable that the specific behavior of Tl in trees results from its biogeochemical analogy with K. In contrast, tree-ring patterns of Zn and Cd significantly correlated with their deposition; nevertheless, a partial shift of these metals towards the stem center cannot be excluded. The isotopic composition of Pb (206Pb/207Pb ~ 1.172–1.184) in trees and underlying soils revealed the predominant influence of smelter emissions (206Pb/207Pb ~ 1.17) on Pb contamination. Analysis of main nutrients (Ca, Mg and Mn) in wood reflected environmental changes related to acid deposition.  相似文献   

13.
The Pb sorption capacity of apatite ore mine tailings and its potential to act as a remediation agent in a Pb polluted areas were investigated. The tailings, originating from the Siilinjärvi carbonatite complex in Finland, consist mainly of phlogopite and calcite accompanied by apatite residues. The ability of the tailings to retain Pb from an aqueous solution was investigated using an isotherm technique. Furthermore, in a 3-month incubation experiment, uncontaminated mineral soil was amended with untreated tailings and with tailings artificially weathered with acid to increase the quantity of Al and Fe (hydr)oxides. Tailings of two particle-sizes (∅ > 0.2 mm and ∅ < 0.2 mm) somewhat differing in their mineralogical composition were investigated as separate amendments. All tailings materials were added to the soil in two dosages (5 g and 10 g of tailings per 125 g of soil). Following incubation, tailings-induced changes in the Pb sorption capacity of the soil were investigated with the isotherm technique. Finally, to investigate the distribution of sorbed Pb among various chemical pools, the soil samples amended with tailings were contaminated with Pb and then subjected to sequential fractionation analysis. The results revealed efficient removal of Pb from an aqueous solution by the tailings, presumably through precipitation and surface complexation mechanisms. Amending the soil with the tailings increased the mass-based maximum Pb sorption capacity from 10.8 mg kg−1 of the control soil to 14–20.5 mg kg−1 for the untreated tailings and to 32.1–72.1 mg kg−1 for the acid-treated material. The tailings transferred Pb from the exchangeable pool to the non-extracted one and thereby substantially decreased its bioavailability. The material with a particle diameter of less than 0.2 mm had a higher mass-based Pb sorption capacity than the large-sized material. The results suggest that the tailings may potentially serve as an immobilizing agent in polluted areas.  相似文献   

14.
A survey was performed to trace the main source of anthropogenic Pb pollution in Mexico City through Pb isotopic signatures (208Pb/204Pb, 206Pb/204Pb, 206Pb/207Pb, and 208Pb/207Pb) from 103 urban topsoil (0–5 cm) samples. Those were collected in the metropolitan area of Mexico City and compared with isotopic compositions of leaded gasoline (LG), domestic Pb ores (DLO) and parent rock (PR). The isotope ratios (IRs) of Pb were determined by inductively coupled plasma quadrupole mass spectrometry (ICP-QMS) and total Pb concentration analyzed by wavelength dispersive X-ray fluorescence (WDXRF). The range of Pb concentrations levels in urban topsoil samples was 15–473 mg/kg. The IR values obtained for these samples were 37.965–39.718 (208Pb/204Pb), 18.375–19.204 (206Pb/204Pb), 1.177–1.218 (206Pb/207Pb) and 2.443–2.496 (208Pb/207Pb). Analyzed topsoil samples with low Pb content (<50 mg/kg) displayed high dispersion in 208Pb/204Pb values, which are determined by different natural sources. Samples with 51–200 mg/kg Pb content, shown low dispersion that revealed the mixing between the natural Pb and anthropogenic Pb. The assessment of the IR values shown that, as Pb concentration increases, a trend toward gasoline IR data has been observed. The results obtained by this research suggest that although the use of leaded petrol had been banned in Mexico since 1997, the Pb pollution in the urban topsoils due to the historical use of Pb in petrol is still significant.  相似文献   

15.
Lead concentrations and isotopic composition of sediment samples collected from three sites within the Lebanese coastal zones were measured: at Akkar, Dora and Selaata. Akkar is located far from any direct source of contamination, while Dora and Selaata receive urban and industrial wastes, respectively. Low Pb concentrations (6–16 μg g−1) were detected in the Akkar sediments, and high concentrations of Pb (70–101 μg g−1) were detected in the Dora sediments. Measuring stable isotope ratios of Pb makes it possible to identify the principal sources of Pb in the Akkar sediments as Pb emitted from gasoline combustion and Pb originating from natural sources. On the other hand, Pb stable isotopic ratios in Dora sediments indicate that they are more highly influenced by anthropogenic sources. Isotopic Pb ratios in the Selaata deposits, where Pb concentrations range between 5 and 35 μg g−1, have an exceptional radiogenic signature for marine sediments 1.25 < 206Pb/207Pb < 1.6 and 0.5 < 206Pb/208Pb < 0.67, which shows the impact of the phosphogypsum discharged by Selaata’s chemical plant. Isotopic Pb analysis applied to EDTA extracts, to test the mobility of Pb, shows that that this mobility is high (>60%) after 24 h of extraction, and that the extracted Pb is less radiogenic than the residual Pb.  相似文献   

16.
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   

17.
Despite reduced anthropogenic deposition during the last decades, deposition sulphate may still play an important role in the biogeochemical cycles of S and many catchments may act as net sources of S that may remain for several decades. The aim of this study is to elucidate the temporal and spatial dynamics of both SO42− and δ34SSO4 in stream water from catchments with varying percentage of wetland and forest coverage and to determine their relative importance for catchment losses of S. Stream water samples were collected from 15 subcatchments ranging in size from 3 to 6780 ha, in a boreal stream network, northern Sweden. In forested catchments (<2% wetland cover) S-SO42− concentrations in stream water averaged 1.7 mg L−1 whereas in wetland dominated catchments (>30% wetland cover) the concentrations averaged 0.3 mg L−1. A significant negative relationship was observed between S-SO42− and percentage wetland coverage (r2 = 0.77, p < 0.001) and the annual export of stream water SO42− and wetland coverage (r2 = 0.76, p < 0.001). The percentage forest coverage was on the other hand positively related to stream water SO42− concentrations and the annual export of stream water SO42− (r2 = 0.77 and r2 = 0.79, respectively). The annual average δ34SSO4 value in wetland dominated streams was +7.6‰ and in streams of forested catchments +6.7‰. At spring flood the δ34SSO4 values decreased in all streams by 1‰ to 5‰. The δ34SSO4 values in all streams were higher than the δ34SSO4 value of +4.7‰ in precipitation (snow). The export of S ranged from 0.5 kg S ha−1 yr−1 (wetland headwater stream) to 3.8 kg S ha−1 yr−1 (forested headwater stream). With an average S deposition in open field of 1.3 kg S ha−1 yr−1 (2002-2006) the mass balance results in a net export of S from all catchments, except in catchments with >30% wetland. The high temporal and spatial resolution of this study demonstrates that the reducing environments of wetlands play a key role for the biogeochemistry of S in boreal landscapes and are net sinks of S. Forested areas, on the other hand were net sources of S.  相似文献   

18.
Rock, soil, and plant (terrestrial moss, European mountain ash leaves, mountain birch leaves, bark and wood, and spruce needles and wood) samples, collected at 3 km intervals along a 120 km long transect (40 sites) cutting the city of Oslo, Norway, were analysed for their Pb concentration and Pb-isotope ratios. A general decrease in 206Pb/207Pb, 208Pb/207Pb and 206Pb/208Pb ratios, with a characteristic low variability in all plant materials and the plant-derived O-horizon of soil profiles, compared to rocks and mineral soils, is observed along the transect. It is demonstrated that minerogenic and biogenic sample materials belong to two different spheres, the lithosphere and biosphere, and that geochemical processes determining their chemical and isotopic compositions differ widely. Background variation for both sample materials needs to be established and documented at the continental and global scale before the anthropogenic influence on the geochemistry of the earth’s surface can be reliably estimated.  相似文献   

19.
The occurrence of mining areas in the vicinities of salt marshes may affect their ecological functions and facilitate the transfer of pollutants into the food chain. The mobilisation of metals in salt marsh soils is controlled by abiotic (pH, redox potential) and biotic (influence of rhizosphere) factors. The effect of the rhizosphere of two plant species (Sarcocornia fruticosa and Phragmites australis) and different flooding regimes on potentially harmful metals and As mobilisation from salt marsh soil polluted by mining activities were investigated (total concentrations: 536 mg kg−1 As, 37 mg kg−1 Cd, 6746 mg kg−1 Pb, 15,320 mg kg−1 Zn). The results show that the changes in redox conditions (from 300 mV to −100 mV) and pH after flooding and rewetting periods may mobilise the contaminant elements into soil solution (e.g., 100 μg L−1 Cd, 30 μg L−1 Pb, 7 mg L−1 Zn), where they are available for plants or may be leached from the soil. Drying periods generated peaks of concentrations in the soil solution (up to 120 μg L−1 Cd and 50 μg L−1 Pb). The risk assessment of As and metal-polluted salt marshes should take into account flood dynamics in order to prevent metal(loid) mobilisation.  相似文献   

20.
Southern Ocean aerosols were collected at the Cape Grim Baseline Air Pollution Station from onshore air under baseline conditions between February 1999 and April 2000. Thermal ionization techniques (TIMS) and isotope dilution mass spectrometry (IDMS) were used to measure the isotopic composition and concentration of lead in the air giving concentrations as low as 0.6 ± 0.1 pg · m−3. Air collected under baseline conditions for 12 months (May 1999-April 2000) yielded an overall lead concentration of 11.0 ± 0.2 pg · m−3 and isotopic composition of 206Pb/207Pb = 1.154, 208Pb/207Pb = 2.387 and 206Pb/204Pb = 17.93. The range in isotopic ratios was consistent with the mixing of lead from major population centers in the Southern Hemisphere in the mid to high latitudes, except for the presence of highly radiogenic lead in some samples. Contributions from radiogenic lead of up to ∼0.8% were observed. Three periods with the highest percentage contribution of radiogenic lead (>0.5%) were investigated in more detail, and 4-d back-trajectories and radon concentrations were used to help identify the sources. The sources are probably associated with the mining and processing of uranium rich ores in southern Africa and possibly South Australia.  相似文献   

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