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1.
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   

2.
Three marine sediment cores from Osaka Bay were analyzed for 210Pb geochronology, heavy metal concentrations (Zn, Cu, and Pb) and stable lead isotope ratios (206Pb/207Pb) in order to reconstruct high-resolution heavy metal pollution history from 1900–2006. Anthropogenic metal accumulation in sediments peaked in 1970 in agreement with the high economic growth period in Japan. The comparison of temporal patterns of 206Pb/207Pb ratio with other areas of Japan suggested that the heavy metals, imported from several different countries during the periods of economic growth (1955 to 1973), are the main pollution source for the country. For the period 1970–2006, the sediment data reflect the result of stricter environmental regulations applied after the late 1960s. However, heavy metal concentrations in the surface sediments are still elevated to levels several times higher than the levels at the bottoms of the cores. Additionally, the lead isotope ratio does not show significant change after the 1980s. Secondary heavy metal pollution through the mixing of deeper polluted sediment appears to be the likely reason for the deterioration of present time submarine sediment environments. In conclusion, this study has demonstrated that it is difficult to recover over a period of several years the benthic quality of a bay, once it is heavily polluted.  相似文献   

3.
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   

4.
应用Microsoft Excel软件中"数据分析"工具之T-检验,对杭州地区不同环境介质的铅同位素组成(206Pb/207Pb比值)进行了均值相等假设检验。通过T-检验,揭示了杭州市哪些环境介质具有相似或不同的铅同位素组成。结果表明,汽车尾气铅具有独特的铅同位素组成而不同于其它环境介质;汽车尾气铅对环境的污染导致环境中铅同位素组成逐渐偏离原值,如城区表土污染最为严重,其206Pb/207Pb比值已与土壤的残渣显示有显著差异,西湖表层沉积淤泥也与深部沉积柱样品有明显的不同。大气和水与多个环境介质具有相似的铅同位素比值,说明大气与水在环境中能与多种环境介质进行同位素物质交换,对污染的扩散起了重要的作用;茶叶与大气有相似的铅同位素比值,说明大气(降尘)对茶叶铅有较大的贡献。而运河沉积物与城区表土铅同位素比值高度一致则说明运河沉积物可能就是来自城区流失的表土。通过实例,介绍了Excel中T-检验在地球化学研究中的应用。  相似文献   

5.
The use of stable Pb isotopes for tracing Pb contamination within the environment has strongly increased our understanding of the fate of airborne Pb contaminants within the boreal forest. This paper presents new stable Pb isotope (206Pb/207Pb ratio) measurements of solid soil samples, stream water (from a mire outlet and a stream draining a forest dominated catchment) and components of Picea abies (roots, needles and stemwood), and synthesizes some of the authors’ recent findings regarding the biogeochemistry of Pb within the boreal forest. The data clearly indicate that the biogeochemical cycling of Pb in the present-day boreal forest ecosystem is dominated by pollution Pb from atmospheric deposition. The 206Pb/207Pb ratios of the mor layer (O-horizon), forest plants and stream water (mainly between 1.14 and 1.20) are similar to atmospheric Pb pollution (1.14–1.19), while the local geogenic Pb of the mineral soil (C-horizon) has high ratios (>1.30). Roots and basal stemwood of the analyzed forest trees have higher 206Pb/207Pb ratios (1.15–1.30) than needles and apical stemwood (1.14–1.18), which indicate that the latter components are more dominated by pollution derived Pb. The low 206Pb/207Pb ratios of the mor layer suggest that the upward transport of Pb as a result of plant uptake is small (<0.04 mg m−2 a−1) in comparison to atmospheric inputs (∼0.5 mg m−2 a−1) and annual losses with percolating soil-water (∼2 mg m−2 a−1); consequently, the Pb levels in the mor layer are now decreasing while the pool of Pb in the mineral soil is increasing. Streams draining mires appear more strongly affected by pollution Pb than streams from forested catchments, as indicated by Pb concentrations about three times higher and lower 206Pb/207Pb ratios (1.16 ± 0.01 in comparison to 1.18 ± 0.02). To what extent stream water Pb levels will respond to the build-up of Pb in deeper mineral soil layers remains uncertain.  相似文献   

6.
Economic reform in China since 1978 has accelerated economic development nationwide hugely, but has also brought about some environmental pollution. In order to identify the primary Pb source to the atmosphere in the central Guizhou region, Pb isotopic ratios in the acid soluble fraction of sediment from Hongfeng Lake were investigated. Lead isotopes in the lake sediments record the history of regional atmospheric Pb pollution. Before the economic reform in 1978, the 208Pb/206Pb and 206Pb/207Pb ratios in the leachates of lake sediments were constant, with a range of 2.0060 to 2.0117 and of 1.2314 to 1.2355, respectively. In the early period of economic reform (1978 to 1988), with the rapid industrial growth in Guizhou province, the acid soluble Pb isotope ratios in the lake sediments changed sharply: the 208Pb/206Pb ratios increased from 2.0212 to about 2.05, while the 206Pb/207Pb ratios decreased from 1.2251 to 1.2060. Emissions from Pb-ore-related industries are suggested to be the major pollution source of Pb in this period. Due to output from a local power plant since 1988, the isotope ratios of the acid soluble Pb in sediments in 1990s are characterized by a little higher radiogenic Pb (208Pb/206Pb = 2.0340–2.0400; 206Pb/207Pb = 1.2122–1.2158) than for the 1980s.  相似文献   

7.
Todos os Santos (all Saints) Bay area on Brazil’s east coast is known for one of the most significant cases of lead contamination in the country owing to the past activities of a Pb-smelter plant. This work was carried out to assess the concentration and sources of Pb based on Pb isotopes and enrichment factor of soil profiles surrounding Todos os Santos Bay in order to understand the expansion of contamination and to help the establishment of Pb regulatory standards for the region. Forty-four samples were collected from soil genetic horizons of six pedons that represent the range of dominant soil properties and geologic materials in the region. Concentrations of Pb and the isotopes 204Pb, 206Pb, 207Pb, and 208Pb were determined on an inductively coupled plasma (quadrupole) mass spectrometry. The soil enrichment factor was calculated using Al and Fe as conservative index elements. Average Pb concentration (15.87 mg kg?1) in uppermost horizons (from all six pedons) is slightly higher than soil background concentrations commonly reported in Brazil. Samples feature a wide range of Pb isotope ratios, ranging from 36.71 to 47.38 for 208Pb/204Pb, 15.00 to 15.65 for 207Pb/204Pb, 16.86 to 20.59 for 206Pb/204Pb, and 1.10 to 1.31 for 206Pb/207Pb. For the enrichment factor calculations, only Fe demonstrated a good agreement with Pb isotopic ratios. Both Pb isotopic composition and enrichment factor were useful tools to distinguishing natural and anthropogenic influence on the Pb soil concentrations.  相似文献   

8.
Mesozoic and Cenozoic ore deposits in the Chilean Andes between La Serena (~30°S) and Santiago (~34°S) include polymetallic vein, low- and high-sulfidation epithermal vein, skarn, porphyry copper-molybdenum and porphyry copper-gold. These deposits are associated with volcanic and plutonic complexes emplaced in eastward-migrating longitudinal arcs which formed during subduction along the continental margin of South America since the Middle Jurassic. Stratabound, but epigenetic, volcanic rock- and sedimentary rock-hosted manto deposits contain additional copper resources. Lead isotopic compositions in ore minerals from 29 deposits vary with age and geographic location, and hence with basement and host rocks. Lead in most ore deposits is derived from temporally related igneous rocks, except for the manto deposits whose lead is derived from host volcanic and sedimentary rock sequences. Lead in the ore deposits is dominated by two crustal sources. Low 207Pb/204Pb characterizes one source whereas high 207Pb/204Pb characterizes the second source. Lead isotopic compositions of Jurassic and Miocene ore minerals (206Pb/204Pb>18.50; 207Pb/204Pb>15.61) lie along the average crustal growth curve. By contrast, most Cretaceous deposits have ore minerals with lower 206Pb/204Pb (<18.39) and 207Pb/204Pb (<15.58) than Jurassic ore minerals. The shift in lead isotopic composition to lower lead isotopic values precludes derivation of lead from a source of similar composition to those in the Jurassic or Tertiary deposits. For Cretaceous deposits, polymetallic and low-sulfidation epithermal veins and a skarn have lower 206Pb/204Pb than a porphyry copper-gold system and peripheral gold veins at Andacollo (18.43-18.50). Late Cretaceous veins from the Bellavista deposit have the lowest 206Pb/204Pb (18.33) of all deposits. Ore minerals in Miocene and Pliocene porphyry copper-molybdenum deposits have higher 206Pb/204Pb (18.58-18.67) than Cretaceous deposits, consistent with their age being younger. The Miocene and Pliocene ore minerals also have higher 207Pb/204Pb (15.58-15.66) than Cretaceous ore minerals, thereby requiring an additional input from the high-207Pb/204Pb source into the younger deposits. Miocene auriferous deposits in the north have similar 206Pb/204Pb values as the Miocene and Pliocene porphyry copper-molybdenum deposits in the south, but they are distinguished by higher and variable 207Pb/204Pb (15.61-15.66) and 208Pb/204Pb (38.54-39.01), which are arrayed along steep mixing trends. These ore minerals have the largest input of high-207Pb/204Pb material in the deposits studied. By contrast, lead in the epigenetic manto deposits appears to be derived from the host volcanic or sedimentary rock-dominated sequences, and locally exhibits large-scale isotopic heterogeneity within a deposit. Overall, the lead isotopic compositions of ore minerals mimic the values and variations established in age-equivalent rock sequences. The low-207Pb/204Pb material in the deposits is derived from Cretaceous igneous rocks or their sources as they evolved with time; low 207Pb/204Pb characterizes these rocks. By contrast, high-207Pb/204Pb material is likely derived from Carboniferous to Triassic igneous rocks or their sources, as this lead isotopic characteristic dominates these rocks.  相似文献   

9.
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   

10.
杭州市土壤铅污染的铅同位素示踪研究   总被引:27,自引:0,他引:27       下载免费PDF全文
根据杭州市40个土壤全铅和38个可溶相铅的统计分析,土壤中全铅平均含量为49.6×10-6,可溶相铅平均为21.4×10-6,城区表土的全铅高达76.1×10-6,显著高于全国土壤平均值。分析结果还显示,从农村→远郊→近郊→公路旁,土壤可溶相铅含量逐渐增加,且土壤的可溶相铅含量与深度具明显的负相关关系。表明杭州市土壤受到了不同程度的铅污染,污染程度由农村→远郊→近郊→公路旁→城区有明显的增高趋势。通过对茶园土壤中可溶相铅、残渣态铅及城区表土全铅的同位素组成对比分析发现,从土壤残渣态(代表土壤背景)→土壤可溶相→城区表层土壤全铅206Pb/207Pb比值有明显的降低。208Pb/(206Pb+207Pb)也有类似的变化趋势。将土壤与杭州市的汽车尾气、大气等环境样品进行对比发现,随着土壤受污染程度的增加,铅同位素组成逐渐向汽车尾气铅漂移,表明汽车尾气排放的铅为其主要污染源。  相似文献   

11.
A high-resolution record of Pb deposition in Rhode Island over the past 250 yr was constructed using a sediment core from the anoxic Pettaquamscutt River basin. The sedimentary Pb concentration record shows the well-described maximum associated with leaded gasoline usage in the United States. Diminished Pb variability during recorded periods of local industrial activity (1735 to 1847) supports the greater importance of regional atmospheric lead transport vs. local inputs. The Pb isotopic composition at this site shows a clear maximum in anthropogenic 206Pb/207Pb in the mid-1800s. Similar peaks have also been observed in sediments from Chesapeake Bay and the Great Lakes, suggesting a common source. Possible causes for this event include mining and smelting of Pb ores in the Upper Mississippi Valley district, which accounted for almost all Pb production in the United States in that period. The timing of this event can provide an important stratigraphic marker for sediments deposited in the past 200 yr in the Northeastern United States. The downcore profile of anthropogenic 206Pb/207Pb provides a classic example of how changes in the mixture of ores for production of tetraethyl lead caused a regional-scale shift in the sedimentary record, and suggests that coal could have played a secondary role in Pb emissions after 1920.  相似文献   

12.
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   

13.
Annual growth rings of a common hardwood species, Picea abies L., were investigated as a potential archive of past atmospheric Pb pollution. Wide distribution of trees in terrestrial settings and straightforward chronology are two advantages of this potential geochemical archive, but several processes described in the literature may obscure the trends in past Pb deposition. These confounding factors include, e.g., radial post-depositional mobility of Pb in xylem, and ecosystem acidification leading to higher bioavailability of Pb. One- to five-year annual wood increments were analyzed for Pb concentrations and 206Pb/207Pb ratios at Jezeri (JEZ), Uhlirska (UHL) and Na Lizu (LIZ), three sites in the Czech Republic, differing in atmospheric Pb loads. Three to four trees per site were included in the study. Distinct Pb concentration maxima between 1960 and 1990 at the two heavily polluted sites (JEZ and UHL) coincided with historical Pb emissions known from inventories of industrial production. No Pb concentration maxima were found at one site, LIZ, situated in a national park 150 km from major pollution sources. Spruce tree rings from JEZ, located just 5 km from coal-burning power stations, contained a large proportion of coal-derived Pb (a high-206Pb/207Pb ratio of 1.19). A coal-related maximum in 206Pb/207Pb in JEZ tree rings was found using two different analytical techniques, laser-ablation multi-collector ICP MS, and single-collector sector-field ICP MS. In a three-isotope graph (206Pb/207Pb vs. 208Pb/207Pb), tree-ring data plotted into the field of ombrotrophic (i.e., rain-fed) peat bogs, suggesting negligible contribution of bedrock-derived Pb in the xylem. We concluded that none of the potential confounding factors played a major role at our sites. Annual growth rings of P. abies in Central Europe faithfully recorded historical changes in atmospheric Pb depositions.  相似文献   

14.
This paper dealt with the Pb contents and Pb isotopic composition of the West Lake Longjing tea. The results showed that in the tea leaves, from young leaf →old leaf →tea limb, the Pb contents tend to increase gradu-ally from 1.63 →4.84 →6.07×10-6, wich revealed that the Pb was accumulated gradually in the tea. After cleaned, the Pb contents of tea leaves were significantly reduced. This indicated that the deposits on the surface of tea leaves made a great contributuion to Pb contents. The survey results for soils in the relevant tea gardens showed that soil from the Longjing tea garden has higher Pb contents, with an average level of 49.6×10-6, two times those of common soils (24×10-6) in China. Results of the systematic analysis for tea, tea garden soil and the samples with the relevant background of the Pb isotopic composition displayed that the Pb isotopic ratio of tea is 206Pb/207Pb=1.164±0.005 (2σ). The ratio of 206Pb/207Pb for the soil gradually decreased from residue phase, soil dilute acid extract phase, and then to urban topsoil, i.e., 1.175 →1.171 →1.170. The 208Pb/(206Pb+207Pb) ratios also show a similar variation trend. 206Pb/207Pb ratios in the samples with the relevant background were: vehicle exhaust, 1.124; coal-combustion, 1.156; atmosphere, 1.168; and water, 1.166. Comparative studies have shown that Pb pollution is popular in the environ-mental media (soil, atmosphere, water) in Hangzhou. With the aggravation of Pb pollution, the Pb isotopic composi-tion gradually changed from the natural background (soil residues) to the direction of automobile exhaust. This phe-nomenon could illustrate that the pollution source was the vehicle exhaust, while the coal-combustion contributed little to environmental pollution in Hangzhou. The Pb of the Longjing tea came mostly from soluble phase Pb in the polluted soil. Moreover, secondary pollution was caused by vehicle exhaust.  相似文献   

15.
Petrogenetic models for the origin of lamproites are evaluatedusing new major element, trace element, and Sr, Nd, and Pb isotopedata for Holocene lamproites from the Gaussberg volcano in theEast Antarctic Shield. Gaussberg lamproites exhibit very unusualPb isotope compositions (206Pb/204Pb = 17·44–17·55and 207Pb/204Pb = 15·56–15·63), which incommon Pb isotope space plot above mantle evolution lines andto the left of the meteorite isochron. Combined with very unradiogenicNd, such compositions are shown to be inconsistent with an originby melting of sub-continental lithospheric mantle. Instead,a model is proposed in which late Archaean continent-derivedsediment is subducted as K-hollandite and other ultra-high-pressurephases and sequestered in the Transition Zone (or lower mantle)where it is effectively isolated for 2–3 Gyr. The high207Pb/204Pb ratio is thus inherited from ancient continent-derivedsediment, and the relatively low 206Pb/204Pb ratio is the resultof a single stage of U/Pb fractionation by subduction-relatedU loss during slab dehydration. Sr and Nd isotope ratios, andtrace element characteristics (e.g. Nb/Ta ratios) are consistentwith sediment subduction and dehydration-related fractionation.Similar models that use variable time of isolation of subductedsediment can be derived for all lamproites. Our interpretationof lamproite sources has important implications for ocean islandbasalt petrogenesis as well as the preservation of geochemicallyanomalous reservoirs in the mantle. KEY WORDS: lamproites; Pb isotopes; mantle Transition Zone; subducted sediment; anomalous mantle reservoirs  相似文献   

16.
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   

17.
Geochemical data are reported for samples from the flanks and floor of the southern Kenya Rift Valley in the Lake Magadi area, and from two central volcanoes located within the rift valley. Rift lavas include samples of Singaraini and Ol Tepesi basalts on the eastern flank, Kirikiti basalts from the western flank, and plateau trachytes from the rift valley floor. Central volcano samples are from Ol Esayeiti and Lenderut located on the eastern flank. The rift basalts are mildly ne-normative, moderately evolved (Mg#=0.39-0.62) alkali basalts and show an overall range in differentiation. Incompatible trace element abundances are moderately elevated (Nb=17-51; Zr=93-274; La=17-55 ppm) and show strongly coherent variations and constant inter-element ratios (e.g. Zr/Nb=4.2-5.5; Nb/Ta=17.5ǂ.4; (La/Sm)n=7.3ǃ.1); isotope ratios are restricted in range (87Sr/86Sr=0.70393-0.70436; 143Nd/144Nd=0.51272-0.51280; 206Pb/204Pb=19.87-19.92; 207Pb/204Pb=15.68-15.70; 208Pb/204Pb=39.56-39.71). Central volcano lavas are more alkaline in character and include basanite (Ol Esayeiti; Mg# >60) and hawaiite to benmoreite (Lenderut; Mg#=0.48-0.38). Incompatible element ratio are similar to those of the rift basalts, although the chondrite normalised REE patterns are steeper (La/Sm)n=17.4ǃ.2). 87Sr/86Sr (0.70358, 0.70391), 143Nd/144Nd (0.51280, 0.51267), 206Pb/204Pb (19.96,20.17), 207Pb/204Pb (15.66,15.76) and 208Pb/204Pb (39.80,40.00) ratios of Ol Esayeiti basanites are similar to the rift basalts, whereas the Lenderut lavas have unusually low143Nd/144Nd (0.512388-0.512453) ratios for their 87Sr/86Sr (0.70370-0.70481) ratios, and distinctly less radiogenic and variable Pb isotope compositions (206Pb/204Pb=17.93-19.01; 207Pb/204Pb=15.43-15.58; 208Pb/204Pb=37.91-39.14). An integrated model is developed in which the geochemical signature of the lavas is attributed to variable degrees of melting to depths within the garnet stability field, and in the presence of residual amphibole. The stability fields of these phases in P-T space indicates that the lavas must have formed within the sub-continental lithosphere rather than within the underlying ambient asthenosphere or a rising mantle plume. The subcontinental lithospheric mantle must therefore extend to a depth of at least 75 km beneath the Lake Magadi area, which contrasts with recent gravity models for the area, which infer that lithospheric mantle is absent beneath this section of the southern Kenya Rift.  相似文献   

18.
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   

19.
Isotopic evidence for the source of lead in the North Pacific abyssal water   总被引:1,自引:0,他引:1  
The absence of accurate measurements of lead (Pb) isotopic composition in the North Pacific abyssal water has made it difficult to assess the relative importance of what are believed to be the two major Pb sources: the natural Pb introduced during preindustrial time and recent anthropogenic Pb resulting from leaded gasoline combustion and high temperature industrial activities. Here we report a vertical profile of seawater 206Pb/207Pb ratio and a meridional section of Pb concentration in the North Pacific Ocean. We observe 2-3-fold increases in Pb concentration along the deep-water flow path and a deep-water 206Pb/207Pb ratio (∼1.188) substantially lower than the pre-industrial value (∼1.210). These data suggest that anthropogenic Pb has invaded the North Pacific abyssal water and become the predominant Pb source there. A simple model calculation based on these data indicates that the anthropogenic Pb is transported to the deep ocean by sinking particles and that this Pb vertical flux has a 206Pb/207Pb ratio that decreased during the past two centuries.  相似文献   

20.
The depth-distribution of lead and its stable isotope ratios were determined in a dated sediment core from a Canadian Shield lake receiving anthropogenic Pb inputs exclusively from atmospheric deposition. The results demonstrate that anthropogenic Pb deposited to the sediments of this lake since the preindustrial period can be modeled successfully using as little as two isotopically distinct Pb types. The first, whose flux was not detectable before 1850, reached a maximum value around 1950, and then decreased significantly thereafter; it was characterized by 206Pb/207Pb and 206Pb/208Pb ratios of 1.222 and 0.495, respectively, and was derived mainly from coal combustion. The second, whose flux was not detectable before 1880, increased sharply to exceed that of the Pb type derived from coal combustion around 1930, and reached a maximum in the mid 1970s; it is characterized by 206Pb/207Pb and 206Pb/208Pb ratios of 1.179 and 0.482, respectively, and was derived mainly from leaded gasoline combustion and industrial sources. The chronology of deposition of these two anthropogenic lead types agrees well with the historical records of fossil fuel uses in Canada and the USA, and also with the history of sediment-deposited polycyclic aromatic hydrocarbons (PAHs) originating from coal combustion. The inventory of Pb derived from coal combustion (0.09 μmol cm−2) is ∼30% of that derived mainly, but not exclusively, from leaded gasoline (0.31 μmol cm−2). Apportionment among source regions of lead deposited to the sediments during the period when leaded gasoline dominated Pb atmospheric emissions indicates that ∼50% of this lead originated in the USA.  相似文献   

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