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1.
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   

2.
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   

3.
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   

4.
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   

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.
We have investigated the potential of hübnerite for U-Pb dating. Hübnerite forms typically at medium to low-temperatures in a wide range of pneumatolytic-hydrothermal mineral deposits, particularly porphyry molybdenum and Sn-specialized granites. Hübnerite from the Sweet Home Mine (Alma, Colorado) formed in a Pb-rich, U-poor environment, but still developed relatively radiogenic Pb isotopic compositions. The low Pbcommon contents in hübnerite (0.075 to 0.155 ppm) demonstrate that Pb is efficiently excluded from the crystal lattice. In contrast, U may substitute for Mn. The U-Pb data of hübnerite scatter. Most of the scatter originates from samples with 206Pb/204Pb values below 50, where Pbblank contributes up to 30% to Pbtotal. Using the least radiogenic galena Pb, samples with 206Pb/204Pb values above 70 have overlapping 206Pb∗/238U and 207Pb∗/235U values and yield a 206Pb/238U age of 25.7 ± 0.3 Ma (2σ). Late stage apatite from the Sweet Home Mine yields a 206Pb/204Pb-238U/204Pb isochron corresponding to an age of 24.8 ± 0.5 Ma (2σ). A comparison of the U-Pb hübnerite ages with literature 40Ar/39Ar ages on earlier sericite and the U-Pb age on later apatite suggests that (i) hübnerite yields accurate U-Pb ages and (ii) the evolution of the Sweet Home mineralization from greisen-type mineralization to medium-temperature hydrothermal vein mineralization took place in a few hundred thousand years at most. Aqueous low-N2-bearing and aqueous inclusions in the dated hübnerite have homogenization temperatures between 325 and 356 °C and moderate salinity (up to 6.7 wt% NaCl equiv.). Thus, hübnerite represents one of the rare examples of a mineral that can be dated accurately and carries petrological information.  相似文献   

7.
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   

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.
Base metal–Ag mineralisation at Dikulushi and in other deposits on the Kundelungu Plateau (Democratic Republic of Congo) developed during two episodes. Subeconomic Cu–Pb–Zn–Fe polysulphide ores were generated during the Lufilian Orogeny (c. 520 Ma ago) in a set of E–W- and NE–SW-oriented faults. Their lead has a relatively unradiogenic and internally inhomogeneous isotopic composition (206Pb/204Pb = 18.07–18.49), most likely generated by mixing of Pb from isotopically heterogeneous clastic sources. These sulphides were remobilised and enriched after the Lufilian Orogeny, along reactivated and newly formed NE–SW-oriented faults into a chalcocite-dominated Cu–Ag mineralisation of high economic interest. The chalcocite samples contain only trace amounts of lead and show mostly radiogenic Pb isotope signatures that fall along a linear trend in the 207Pb/204Pb vs. 206Pb/204Pb diagram (206Pb/204Pb = 18.66–23.65; 207Pb/204Pb = 15.72–16.02). These anomalous characteristics reflect a two-stage evolution involving admixture of both radiogenic lead and uranium during a young fluid event possibly c. 100 Ma ago. The Pb isotope systematics of local host rocks to mineralisation also indicate some comparable young disturbance of their U–Th–Pb systems, related to the same event. They could have provided Pb with sufficiently radiogenic compositions that was added to less radiogenic Pb remobilised from precursor Cu–Pb–Zn–Fe polysulphides, whereas the U most likely originated from external sources. Local metal sources are also suggested by the 208Pb/204Pb–206Pb/204Pb systematics of combined ore and rock lead, which indicate a pronounced and diversified lithological control of the immediate host rocks on the chalcocite-dominated Cu–Ag ores. The Pb isotope systematics of polysulphide mineralisation on the Kundelungu Plateau clearly record a diachronous evolution.  相似文献   

10.
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   

11.
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12.
Early Proterozoic volcanic and sedimentary rocks of the Rappen district in northern Sweden were deposited at a destructive plate margin to the south of the Archaean craton of the western Baltic Shield. The volcano-sedimentary suite was intruded by two generations of early Proterozoic granites at ca. 1.89–1.85 Ga and ca.1.82–1.78 Ga, respectively, and metamorphosed at upper amphibolite facies conditions. Small stratabound iron, copper, and zinc deposits occur in felsic to mafic tuffs and arkosic sediments. Small deposits of molybdenum, tungsten, and uranium formed during the emplacement of the younger granites. The lead isotopic compositions of sulfide trace lead from the various deposits are highly heterogeneous. In the 206Pb/204Pb–207Pb/204Pb diagram they fall on mixing arrays between little evolved early Proterozoic lead and highly radiogenic Caledonian lead. The least radiogenic lead isotopic compositions from the various deposits have a wide range of 207Pb/204Pb ratios and thus indicate variable involvement of Archaean crustal lead in the Proterozoic deposits. Deposits hosted by siliciclastic rocks have higher 207Pb/204Pb ratios than deposits hosted in mafic to felsic tuffites. The lead isotopic heterogeneity suggests that the lead in the various deposits was locally derived and, furthermore, that the sedimentary rocks in part originated from the Archaean craton to the north. Lead mixing arrays in the 206Pb/204Pb–207Pb/204Pb diagram demonstrate that in Paleozoic time radiogenic lead was mobilized and transported in the basement. Source ages calculated from the mixing arrays (ca.1.9 Ga and ca.1.8 Ga) correspond to the age of the Early Proterozoic volcanism and metamorphism respectively. One group of deposits includes lead from at least three sources and illustrates that radiogenic lead was multiply mobilized and transported in the Proterozoic basement. It occurs in deposits that occur in zones that became permeable during the reactivations of the basement.  相似文献   

13.
Uranium-lead ratios (commonly represented as 238U/204Pb = μ) calculated for the sources of martian basalts preserve a record of petrogenetic processes that were active during early planetary differentiation and formation of martian geochemical reservoirs. To better define the range of μ values represented by the source regions of martian basalts, we completed U-Pb elemental and isotopic analyses on whole rock, mineral and leachate fractions from the martian meteorite Queen Alexandra Range 94201 (QUE 94201). The whole rock and silicate mineral fractions have unradiogenic Pb isotopic compositions that define a narrow range (206Pb/204Pb = 11.16-11.61). In contrast, the Pb isotopic compositions of weak HCl leachates are more variable and radiogenic. The intersection of the QUE 94201 data array with terrestrial Pb in 206Pb/204Pb-207Pb/204Pb-208Pb/204Pb compositional space is consistent with varying amounts of terrestrial contamination in these fractions. We calculate that only 1-7% contamination is present in the purified silicate mineral and whole rock fractions, whereas the HCl leachates contain up to 86% terrestrial Pb. This terrestrial Pb contamination generated a 206Pb-207Pb array in the QUE fractions that appears to represent an ancient age, which contrasts with a much younger crystallization age of 327 ± 10 Ma derived from Rb-Sr and Sm-Nd isochrons (Borg L. E., Nyquist L. E., Taylor L. A., Wiesmann H. and Shih C. -Y. (1997) Constraints on Martian differentiation processes from Rb-Sr and Sm-Nd isotopic analyses of the basaltic shergottite QUE 94201. Geochim. Cosmochim. Acta61, 4915-4931). Despite the contamination, and accepting 327 ± 10 Ma as the crystallization age, we use the U-Pb data to determine the initial 206Pb/204Pb of QUE 94201 to be 11.086 ± 0.008 and to calculate the μ value of its mantle source to be 1.82 ± 0.01. The μ value calculated for the QUE 94201 source is the lowest determined for any martian basalt source, and, when compared to the highest values determined for martian basalt sources, indicates that μ values in martian source reservoirs vary by at least a factor of two. Additionally, the range of source μ values indicates that the μ value of bulk silicate Mars is approximately three. The amount of variation in the μ values of the mantle sources (μ ∼ 2-4) is greater than can be explained by igneous processes involving silicate phases alone. We suggest the possibility that a small amount of sulfide crystallization may generate greater extents of U-Pb fractionation during formation of the mantle sources of martian basalts.  相似文献   

14.
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   

15.
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   

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.
We evaluate initial (26Al/27Al)I, (53Mn/55Mn)I, and (182Hf/180Hf)I ratios, together with 207Pb/206Pb ages for igneous differentiated meteorites and chondrules from ordinary chondrites for consistency with radioactive decay of the parent nuclides within a common, closed isotopic system, i.e., the early solar nebula. The relative initial isotopic abundances of 26Al, 53Mn, and 182Hf in differentiated meteorites and chondrules are consistent with decay from common solar system initial values, here denoted by I(Al)SS, I(Mn)SS, and I(Hf)SS, respectively. I(Mn)SS and I(Hf)SS = 9.1 ± 1.7 × 10−6 and 1.07 ± 0.08 × 10−4, respectively, correspond to “canonical” I(Al)SS = 5.1 × 10−5. I(Hf)SS so determined is consistent with I(Hf)SS = 9.72 ± 0.44 × 10−5 directly determined from an internal Hf-W isochron for CAI minerals. I(Mn)SS is within error of the lowest value directly measured for CAIs. We suggest that erratically higher values measured for CAIs in carbonaceous chondrites may reflect proton irradiation of unaccreted CAIs by the early Sun after other asteroids destined for melting by 26Al decay had already accreted. The 53Mn incorporated within such asteroids would have been shielded from further “local” spallogenic contributions from within the solar system. The relative initial isotopic abundances of the short-lived nuclides are less consistent with the 207Pb/206Pb ages of the corresponding materials than with one another. The best consistency of short- and long-lived chronometers is obtained for (182Hf/180Hf)I and the 207Pb/206Pb ages of angrites. (182Hf/180Hf)I decreases with decreasing 207Pb/206Pb ages at the rate expected from the 8.90 ± 0.09 Ma half-life of 182Hf. The model solar system age thus determined is TSS,Hf-W = 4568.3 ± 0.7 Ma. (26Al/27Al)I and (53Mn/55Mn)I are less consistent with 207Pb/206Pb ages of the corresponding meteorites, but yield TSS,Mn-Cr = 4568.2 ± 0.5 Ma relative to I(Al)SS = 5.1 × 10−5 and a 207Pb/206Pb age of 4558.55 ± 0.15 Ma for the LEW86010 angrite. The Mn-Cr method with I(Mn)SS = 9.1 ± 1.7 × 10−6 is useful for dating accretion (if identified with chondrule formation), primary igneous events, and secondary mineralization on asteroid parent bodies. All of these events appear to have occurred approximately contemporaneously on different asteroid parent bodies. For I(Mn)SS = 9.1 ± 1.7 × 10−6, parent body differentiation is found to extend at least to ∼5 Ma post-TSS, i.e., until differentiation of the angrite parent body ∼4563.5 Ma ago, or ∼4564.5 Ma ago using the directly measured 207Pb/206Pb ages of the D’Orbigny-clan angrites. The ∼1 Ma difference is characteristic of a remaining inconsistency for the D’Orbigny-clan between the Al-Mg and Mn-Cr chronometers on one hand, and the 207Pb/206Pb chronometer on the other. Differentiation of the IIIAB iron meteorite and ureilite parent bodies probably occurred slightly later than for the angrite parent body, and at nearly the same time as one another as shown by the Mn-Cr ages of IIIAB irons and ureilites, respectively. The latest recorded episodes of secondary mineralization are for carbonates on the CI carbonaceous chondrite parent body and fayalites on the CV carbonaceous chondrite parent body, both extending to ∼10 Ma post-TSS.  相似文献   

18.
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   

19.
Angrite Sahara 99555 (hereafter SAH), precisely dated by Baker et al. (Baker J., Bizzarro M., Wittig N., Connelly J. and Haack H. (2005) Early planetesimal melting from an age of 4.5662 Gyr for differentiated meteorites. Nature436, 1127-1131), has been proposed as a new reference point for the early Solar System timescale and for calculation of the revised minimum age of our Solar System. The Pb-Pb age of SAH of 4566.18 ± 0.14 Ma, reported by Baker et al., differs from the Pb-Pb age of D’Orbigny, another basaltic angrite, of 4564.42 ± 0.12 Ma (Amelin Y. (2008) U-Pb ages of angrites. Geochim. Cosmochim. Acta72, 221-232), despite the fact that the relative 53Mn-53Cr and 182Hf-182W ages of these meteorites are identical. Here I report U-Pb data for 21 whole rock and pyroxene fractions from SAH, analyzed using the same approach as D’Orbigny (Amelin, 2008). These fractions contain between 1.3 and 8.9 pg of total common Pb, slightly more than analytical blank. Measured 206Pb/204Pb ratios are between 625 and 2817 for D’Orbigny, blank-corrected 206Pb/204Pb ratios are between 1173 and 6675. Eight acid-washed whole rock fractions yielded an isochron age of 4564.86 ± 0.38 Ma, MSWD = 1.5. Data for pyroxene fractions plot mostly above the whole rock isochron, and do not form a linear array in 207Pb/206Pb vs. 204Pb/206Pb isochron coordinates. The 207Pb∗/206Pb∗ model dates of the pyroxene fractions vary from 4563.8 ± 0.3 to 4567.1 ± 0.5 Ma. The difference between whole rock and pyroxene U-Pb systematics may be a result of re-distribution of radiogenic Pb at a mineral grain scale several million years after crystallization. Complexities of Sm-Nd, Lu-Hf, and possibly 26Al-26Mg mineral systematics of SAH, described previously, may be related to the same process that caused the re-distribution of radiogenic Pb. Disturbance of isotopic chronometers renders SAH an imperfect anchor for the early Solar System timescale. The problems with age determination revealed by the studies of SAH call for greater attention in Pb-isotopic dating of angrites and other achondrites.  相似文献   

20.
An investigation of the Pb isotopic compositions of plagioclase and sulfide in a stratigraphic interval including the UG2 chromitite of the eastern Bushveld Complex has been conducted to determine the Pb isotopic composition(s) of the magma(s) that crystallized to form this part of the intrusion, gain a better understanding of why coexisting plagioclase and sulfide commonly exhibit widely different Pb isotopic compositions, and explore the use of Pb isotopes in deducing post-accumulation history. Analyses were obtained in situ with a NuPlasma multicollector ICP-MS coupled with 193 nm Excimer or 213 nm lasers.Most plagioclase compositions fall on the 207Pb/204Pb vs 206Pb/204Pb geochron of 2.06 Ga, which is the solidification age of the intrusion. The measured ratios have not been affected by radiogenic ingrowth, and plagioclase generally remained closed to Pb exchange after initial cooling. The array of plagioclase compositions on the geochron is significantly larger than that defined by analytical error. This indicates that in terms of Pb at least two different magma compositions were present. The composition of the least radiogenic magma was approximated by that of the contemporaneous BSE with μ (238U/204Pb) and ω (232Th/204Pb) values of ≈9.0 and 35, respectively, suggesting a mantle derivation with little or no involvement of the continental crust, while the second magma possessed a Pb isotopic composition similar to the upper crust with μ ≈ 9.6.Compared to plagioclase, sulfides generally possess slightly higher 206Pb/204Pb ratios for equivalent 207Pb/204Pb ratios such that their compositions fall between the 2.06 and 1.86 Ga geochrons. The latter age is much younger than the cooling age. The data are interpreted to mean that the Bushveld Complex remained buried in the crust at temperatures of several hundred °C for about 200 Ma after solidification, and that any sulfides accessible to fluid continued to re-equilibrated during this time with more radiogenic Pb. The sulfide Pb may have been transported into the Bushveld Complex by fluids from an external reservoir when the rocks were still partially molten and thus permeable. Alternatively, the sulfide Pb may have originated mainly from radiogenic decay of U and Th present in minerals other than the sulfides in the immediately surrounding Bushveld rocks, followed by local redistribution of Pb by whatever fluid was present. Indeed, some sulfides are characterized by 208Pb/204Pb ratios sufficiently high that an external source is unlikely. This observation and the fact that the sulfides display small-scale heterogeneity suggest that most, if not all, of the radiogenic sulfide Pb was locally derived. It also implies that during the post-solidification, re-equilibration period there was no large-scale fluid-flow through the microfracture network because otherwise the isotopic heterogeneities would not have been preserved. The minerals in 2 of the 19 samples studied contain young Pb, presumably introduced by meteoric waters that permeated the macrofracture network.  相似文献   

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