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1.
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   

2.
Knowledge of the cause and source of Pb pollution is important to abate environmental Pb pollution by taking source-related actions. Lead isotope analysis is a potentially powerful tool to identify anthropogenic Pb and its sources in the environment. Spatial information on the variation of anthropogenic Pb content and anthropogenic Pb sources in rural topsoils is remarkably limited. This study presents results of a survey of approximately 350 topsoil samples from rural locations covering the entire Netherlands, for which the bulk geochemical and Pb isotope compositions were determined. The specific aim of this study is to determine the anthropogenic Pb sources in the topsoils from rural areas in The Netherlands. The spatial distribution of anthropogenic Pb in soils in The Netherlands will be explained in terms of land use and pollution sources.Nearly all studied topsoils display Pb contents that exceed the amount expected based on the soil lithology. The range in Pb isotope ratios of the additional Pb fraction in rural Dutch topsoils is established at 1.056–1.199, 2.336–2.486 and 0.452–0.490 for 206Pb/207Pb, 207Pb/208Pb and 206Pb/208Pb, respectively. Five land use types are distinguished (forest, open nature, moor, arable land and grassland) with distinct isotopic compositions for added Pb. Additional Pb in soils of natural areas (forest, open nature and moor) has on average lower 206Pb/207Pb, 208Pb/207Pb and 206Pb/208Pb ratios than the agricultural soils (arable land and grassland). Additional Pb in both natural area soils and agricultural soils is interpreted to be of anthropogenic origin: most likely a mixture of coal/galena, incinerator ashes and gasoline Pb. The dominant sources of additional Pb in the topsoil of open nature areas are most likely incinerator ash and gasoline Pb. In contrast, the on average higher 206Pb/207Pb, 208Pb/207Pb and 206Pb/208Pb ratios of additional Pb in agricultural soils are most likely caused by the presence of animal manure and N–P fertilizers.Several areas are observed with notably high additional Pb contents (26–211 mg/kg on an organic matter-free basis) in the topsoil. The largest area is the Randstad area, which has the highest population and traffic density, and hosts a considerable fraction of the Dutch chemical industry. Two other areas with high additional Pb contents in the topsoil are located near the Dutch borders and are most likely influenced by German and Belgian chemical industries. The topsoils in the coastal dunes and southern, central and northern forests are characterized by relatively low additional Pb contents (<10 mg/kg on an organic matter-free basis). The population, traffic and chemical industry density is low in these areas and no fertilizers are applied.  相似文献   

3.
Lead concentrations and stable lead isotopes (204Pb, 206Pb, 207Pb, 208Pb) were measured in forest moss samples (Pleurozium schreberi or Scleropodium purum) collected at 273 sites across the Czech Republic during 2010. Continuously decreasing median Pb concentrations in moss were documented over the last two decades: 1995: 11 mg/kg, 2000: 5.66 mg/kg, 2005: 4.94 mg/kg and 2010: 2.85 mg/kg. Several local anomalies have decreased in scale, the overall regional distribution patterns remained, however, the same. The regional Pb isotope ratio distributions show that the ratios show little variation for a large central part of the country and provide the large-scale background isotope ratios for the Czech Republic of about 204Pb/206Pb = 0.0550, 206Pb/207Pb = 1.167, 206Pb/208Pb = 0.478 and 207Pb/208Pb = 0.409 for 2010. This background Pb isotope ratio signal in moss has been locally (900–7500 km2) modified by specific Pb isotopic ratio signals caused by deposition of Pb emissions from known local anthropogenic Pb emission sources, such as industrial combustion of local coal, and a variety of industrial enterprises (metallurgical, engineering and glass works). At some sites where mining of uranium and polymetallic ores took place the moss samples show also a locally specific Pb isotope signal. The in terms of area affected largest deviations in the Pb-isotope ratios, e.g., in the Bohemian Massif, may be due to the input of geogenic dust.  相似文献   

4.
The identification of metal provenance is often based on chemical and Pb isotope analyses of materials from the operating chain, mainly ores and metallic artefacts. Such analyses, however, have their limits. Some studies are unable to trace metallic artefacts or ingots to their ore sources, even in well-constrained archaeological contexts. Possible reasons for this difficulty are to be found among a variety of limiting factors: (i) problems of ore signatures, (ii) mixing of different ores (alloys), (iii) the use of additives during the metallurgical process, (iv) metal recycling and (v) possible Pb isotopic fractionation during metal production. This paper focuses on the issue of Pb isotope fractionation during smelting to address the issue of metal provenance. Through an experimental reconstruction of argentiferous Pb production in the medieval period, an attempt was made to better understand and interpret the Pb isotopic composition of ore smelting products. It is shown that the measured differences (outside the total external uncertainties of 0.005 (2*sd) for 206Pb/204Pb ratios) in Pb signatures measured between ores, slag and smoke are not due to Pb mass fractionation processes, but to (1) ore heterogeneity (Δ206Pb/204Pbslag-ores = 0.066) and (2) the use of additives during the metallurgical process (Δ206Pb/204Pbslag-ores = 0.083). Even if these differences are due to causes (1) and/or (2), smoke from the ore reduction appears to reflect the ore mining area without a significant disturbance of its Pb signature for all the isotopic ratios (Δ206Pb/204Pbsmokes-ores = 0.026). Thus, because the isotopic heterogeneity of the mining district and additives is averaged in slags, slag appears as the most relevant product to identify ancient metal provenance. Whereas aiming at identifying a given mine seems beyond the possibilities provided by the method, searching for the mining district through analysis of the smelting workshop materials should provide a more appropriate approach in cases where no archaeological evidence of ancient mining is available. Furthermore, smoke Pb isotopic composition does not seem to be significantly affected by the metallurgical process. Paleopollution recorded in peat deposits could help to detect ancient mining production and workshops. Integrated collaboration between mining archaeologists and geochemists appears crucial to achieve this goal.  相似文献   

5.
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   

6.
Analytical techniques have been developed for using a secondary ion mass spectrometer, the ion microprobe mass analyzer (IMMA), to determine, in situ, 207Pb206Pb and U/Pb ages on approximately 10-μm areas of individual mineral phases containing relatively abundant radiogenic Pb isotopes. Standard samples of known age and U, Th and Pb contents, together with the Andersen-Hinthorne local thermal equilibrium (LTE) model for predicting ionization parameters are used to establish a semi-empirical relationship for correcting observed U/Pb intensities to atom ratios. Measurements of isotope standards show that mass fractionation corrections are not required and that the accuracy and precision of analysis are generally limited by Poisson counting statistics.Many U-rich accessory minerals yield spectra which consist only of Pb at masses 204, 206, 207 and 208; thus the measurement of 207Pb206Pb ages is accomplished by simply measuring the intensities of these peaks and the background. An excellent correspondence of the ages determined using the IMMA with those from more conventional techniques is demonstrated for terrestrial, lunar and meteoritic phases. For example, the following 207Pb206Pb ages were obtained from polished thin sections of crystalline lunar samples: 10047, 3.75 ± 0.05 (2σ) Ga; 14310, 3.96 ± 0.03 Ga; and 15555, 3.36 ± 0.06 Ga. From small U-rich phases in CaAl-rich inclusions in the Allende carbonaceous chondrite, seven 207Pb206Pb ages were obtained, averaging 4.60 ± 0.09 (2σ) Ga.A method of correcting low-resolution Pb-isotope data for molecular ion interferences in zircon and baddeleyite is presented and shown to be practical through the analysis of terrestrial and lunar samples.  相似文献   

7.
This study is a search for a genetic relationship between Pb sulphide ore and igneous rocks in the region of Mount Isa, Queensland. The approach involves derivation of Pb isotope initial ratios by the whole-rock isochron method, and comparison of the initial ratios (Pb206/Pb204, Pb207/Pb204 and Pb208/Pb204) with the isotopic composition of the ore Pb. Data are reported for four igneous units; Kalkadoon granodiorite, Kalkadoon adamellite, Sybella granite and Eastern Creek volcanics. The results display considerable scatter for each of the units, and reveal the effects of recent surficial loss of U. The positioning of isochrons is aided by previous Rb-Sr geochronological data wherever possible. Comparison of initial ratios and ore Pb suggests that none of the igneous rock units is co-genetic with the ore deposit. Both phases of the Sybella Granite are more radiogenic and are apparently younger than the ore Pb. The Kalkadoon Granite is possibly related to the ore through some post-emplacement process of extraction and transport of Pb (e.g. by erosion or by anatectic magma generation) to the present site of the orebodies.  相似文献   

8.
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   

9.
The Pb contents and 206Pb/207Pb and 208Pb/206Pb isotopic ratios were studied in the soils and wines (2004 harvest) of three vineyard areas of the Czech Republic. The areas differ in their geological basements and anthropogenic loading. The isotopic compositions of wine in areas with intensive industry (Most, North Bohemia 206Pb/207Pbwine = 1.178 ± 0.004) and the agricultural areas of Central Bohemia (Roudnice nad Labem 206Pb/207Pbwine = 1.176 ± 0.007) are similar to the Pb isotopic composition of airborne particulate material typical of polluted and industrial environments (206Pb/207Pb = 1.17–1.19). The isotopic composition of wine from Prague (206Pb/207Pbwine = 1.174 ± 0.003) is different from that of the soil, which was severely contaminated in the past by vehicular Pb (206Pb/207Pbsoil = 1.147–1.168). This fact shows that interception of airborne Pb by plants is greater than its uptake by the root system.  相似文献   

10.
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   

11.
The Yinchanggou Pb-Zn deposit, located in southwestern Sichuan Province, western Yangtze Block, is stratigraphically controlled by late Ediacaran Dengying Formation and contains >0.3 Mt of metal reserves with 11 wt% Pb + Zn. A principal feature is that this deposit is structurally controlled by normal faults, whereas other typical deposits nearby (e.g. Maozu) are controlled by reverse faults. The origin of the Yinchanggou deposit is still controversial. Ore genetic models, based on conventional whole-rock isotope tracers, favor either sedimentary basin brine, magmatic water or metamorphic fluid sources. Here we use in situ Pb and bulk Sr isotope features of sulfide minerals to constrain the origin and evolution of hydrothermal fluids. The Pb isotope compositions of galena determined by femtosecond LA-MC-ICPMS are as follows: 206Pb/204Pb = 18.17–18.24, 207Pb/204Pb = 15.69–15.71, 208Pb/204Pb = 38.51–38.63. These in situ Pb isotope data overlap with bulk-chemistry Pb isotope compositions of sulfide minerals (206Pb/204Pb = 18.11–18.40, 207Pb/204Pb = 15.66–15.76, 208Pb/204Pb = 38.25–38.88), and both sets of data plotting above the Pb evolution curve of average upper continental crust. Such Pb isotope signatures suggest an upper crustal source of Pb. In addition, the coarse-grained galena in massive ore collected from the deep part has higher 206Pb/204Pb ratios (18.18–18.24) than the fine-grained galena in stockwork ore sampled from the shallow part (206Pb/204Pb = 18.17–18.19), whereas the latter has higher 208Pb/204Pb ratios (38.59–38.63) than the former (208Pb/204Pb = 38.51–38.59). However, both types of galena have the same 207Pb/204Pb ratios (15.69–15.71). This implies two independent Pb sources, and the metal Pb derived from the basement metamorphic rocks was dominant during the early phase of ore formation in the deep part, whereas the ore-hosting sedimentary rocks supplied the majority of metal Pb at the late phase in the shallow part. In addition, sphalerite separated from different levels has initial 87Sr/86Sr ratios ranging from 0.7101 to 0.7130, which are higher than the ore formation age-corrected 87Sr/86Sr ratios of country sedimentary rocks (87Sr/86Sr200 Ma = 0.7083–0.7096), but are significantly lower than those of the ore formation age-corrected basement rocks (87Sr/86Sr200 Ma = 0.7243–0.7288). Again, such Sr isotope signatures suggest that the above two Pb sources were involved in ore formation. Hence, the gradually mixing process of mineralizing elements and associated fluids plays a key role in the precipitation of sulfide minerals at the Yinchanggou ore district. Integrating all the evidence, we interpret the Yinchanggou deposit as a strata-bound, normal fault-controlled epigenetic deposit that formed during the late Indosinian. We also propose that the massive ore is formed earlier than the stockwork ore, and the temporal-spatial variations of Pb and Sr isotopes suggest a certain potential of ore prospecting in the deep mining area.  相似文献   

12.
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   

13.
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   

14.
The internal precision of Pb isotope analyses using single-zircon evaporation in a double-filament solid source mass spectrometer (Kober 1986) can be improved combining the evaporation of Pb directly from the single grain with a suitable Pb+ emitter-bedding technique. This is most easily done by step-wise evaporating the investigated grain at temperatures of 1700–1800 K generating on the ‘cold’ ionization filament a deposit of radiogenic Pb together with further elements and compounds derived directly from the crystal. The heating of the deposit on the ionization filament to 1400–1500 K results in long-lived and stable Pb+ ion beams. The ‘activating reagents’ in the deposit are HfO2 and SiO2. Their release from the zircon grain together with the radiogenic Pb, which presumably is sited in the crystalline zircon domains as Pb4+, is probably due to disintegration reactions of trace-element silicates hosted in the grain. In the bedding deposited on the ionization filament thermally stable Pb/Hf/SiO2 compounds are formed (PbHfSiO5(?)). They retain the Pb isotopes on the (Re) filament up to 1400 K–1500 K and are highly efficient Pb+ ion emitters similar to the ‘Si-gel’-method (Cameron et al. 1969). The combined evaporation/emitter-bedding technique has been applied to natural zircons of different genesis and to isotope standards. Routinely, a Pb+ ion yield of 2*10?4-1*10?3 and a relative standard deviation of the 207Pb/206Pb ratio in the order of 1% have been obtained for sub-ng- to ng-amounts of Pb from standards and samples. The method rapidly can yield Pb isotope information on the ‘concordant’ zircon phases with a standard deviation of ±15–20 Ma of the derived ages also in the case of Paleozoic zircon populations.  相似文献   

15.
This study reports metal abundances and Pb isotope ratios of emissions from the Horne copper smelter, and ambient (ground level) atmosphere at Rouyn, Québec retrieved during 2-week field studies in the winter and summer seasons of 2000. Plume aerosols were sampled during horizontal and vertical passes using a DHC-6 Twin Otter aircraft, which typically tracked the plume up to 30 km from the stack. Samples of the ‘background’ atmospheric conditions were taken simultaneously from a ground site meteorological station located 2.5 km in the predominant upwind direction from the stack.Overall, metal concentrations (ng/m3 of As, Cd, Cu, Pb, Se, Zn) for the in-plume samples are elevated by one or more orders of magnitude over those measured in the ground site samples. The Pb isotope compositions for the in-plume samples are extremely variable (206Pb/207Pb range from ∼1.120 to ∼1.170) but define well-constrained linear arrays in conventional Pb-Pb isotope plots. Correlations between metal concentrations (e.g. As/Pb, Cu/Pb, Zn/Pb) and the Pb isotope data are indicative of binary mixing between two anthropogenic end members; most probably imported industrial Pb found in recycled materials, and nonradiogenic Pb derived from Archean sulfide ore deposits. Pb isotope data from the winter ground site (‘background’) samples indicate that the ground level atmosphere at Rouyn contains a mixture of Pb emitted from the Horne smelter and long-range anthropogenic Pb transported from Eurasian pollution sources. Compared to the Pb isotope composition of epiphytic lichens, snowpack, and precipitations collected in 1990 to 1999 from adjacent geographic regions, the Pb isotope results obtained here suggest that aerosols emitted from the Horne smelter are dispersed into northeastern North America. However, future studies dealing with point source apportionment for this region of the globe will be rendered difficult due to the processing at the Horne smelter of recycled material containing industrial Pb from various sources.  相似文献   

16.
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   

17.
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   

18.
《Gondwana Research》2009,15(4):587-596
We developed a 238U–206Pb⁎ and 207Pb⁎–206Pb⁎ zircon dating method using a Cameca NanoSIMS NS50 ion microprobe. A 7-to 9-nA O− primary beam was used to sputter a 15-μm crater, and secondary positive ions were extracted for mass analysis using the Mattauch–Herzog geometry. The multicollector system was modified to detect 90Zr+, 204Pb+, 206Pb+, 238U16O+, and 238U16O2+ ions simultaneously. A mass resolution of about 4000 at 10% peak height and with a flat peak top was attained, and the sensitivity of Pb was about 4 cps·nA− 1·ppm− 1. A multicrystal zircon standard (QGNG) from South Australia with a U–Pb age of 1842 Ma was used as a reference for Pb+/UO+–UO2+/UO+ calibration, and on the basis of the positive correlation between these ratios, we determined the sample 206Pb/238U ratios. 207Pb/206Pb ratios were measured by magnetic scanning in single-collector mode. The standard zircons 91500, from Canada, and SL13, from Sri Lanka, were analyzed against QGNG. Observed 238U–206Pb⁎ and 207Pb⁎–206Pb⁎ ages agreed well with published ages within experimental error. Then, 16 zircon grains in a metamorphic rock from Nagasaki, Japan, were analyzed. Observed ages were compatible with SHRIMP ages, suggesting that the NanoSIMS with a 15-μm probe diameter is suitable for ion microprobe U–Pb zircon dating.  相似文献   

19.
《Applied Geochemistry》2001,16(2):207-229
The environment surrounding Palmerton, Pennsylvania is contaminated with Pb arising from primary Zn smelting and a process involving Zn recovery from electric arc steel furnace dusts. Lead isotope systematics have been used to distinguish primary Zn smelting Pb (206Pb/204Pb∼18.4–18.5) from electric arc furnace dust lead (206Pb/204Pb∼19.0–19.1). Primary Zn smelting is the dominant source of Pb in O2 horizon soils from undisturbed near-Palmerton locations, which contain up to 3570 ppm Pb and 782 ppm Cd. Soils from undeveloped near-Palmerton locations also exhibit unusually elevated concentrations of other sphalerite-derived chalcophilic elements (Se, Ag, In, Sb, Te, Au, Hg, Tl and Bi); indium concentrations of up to 17.0 ppm are observed therein. Residential soils and dusts from Palmerton contain Pb which is largely explainable via mixing of Pb from primary Zn smelting and electric arc furnace dusts. Approximately 80% of the Pb in airborne particulate matter sampled at Palmerton in 1991 is derived from electric arc furnace dusts, and atmospheric enrichment factors for Cu, Sb, Pb, and Bi are observed which confirm this major source contribution. Residential samples from a control location contain Pb which is less radiogenic than is found in Palmerton, and exhibit no unusual elevation in sphalerite elements. Lead source discrimination in the Palmerton environment via Pb isotopic and elemental constituents approaches result in parallel conclusions.  相似文献   

20.
The results of our combined U-Pb, Rb-Sr, and Sm-Nd isotope study of mare basalt 10017 contribute to the understanding of the petrogenetic processes involved in the origin of geochemical diversity in lunar mare basalt sources, as well as the U-Pb isotope systematics of the Moon. The Rb-Sr, Sm-Nd, and 238U-206Pb isotope systems yield concordant crystallization ages of 3.633 ± 0.057 Ga, 3.678 ± 0.069 Ga, and 3.616 ± 0.098 Ga, respectively. The 235U-207Pb isochron yields an older, though still concordant, age of 3.80 ± 0.12 Ga. Neither the 206Pb-207Pb system nor U-Pb concordia system yields an age for 10017 that is concordant with the age determined from the Sm-Nd, Rb-Sr, and 238U-206Pb systems. The initial 87Sr/86Sr of 10017 is 0.69941 ± 7 and the initial εNd is +3.2 ± 0.4. Initial Pb isotopic compositions, determined from the U-Pb isochrons, are 206Pb/204Pbi = 31 ± 11 and 207Pb/204Pbi = 34 ± 15. Together, these initial Pb compositions constrain the μ value of the 10017 source to be 70 ± 30, assuming a single-stage Pb growth model. This is considerably lower than μ values typically estimated for mare basalt sources (∼100-600). Regardless, the μ values calculated for the sources of mare basalts, as well as other lunar samples, show a range that is larger than can be explained by fractionation of U from Pb solely by crystallization of silicate phases and ilmenite during magma ocean solidification and formation of lunar mantle sources. The U-Pb isotope systematics may reflect late-stage formation of a sulfide phase, which strongly fractionates Pb from U but has minimal effect on Rb/Sr or Sm/Nd compositions, during crystallization of the lunar magma ocean.  相似文献   

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