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1.
Four sediment cores collected in the Seine River basin and dated between 1916 and 2003 were analyzed for lead concentrations and isotopic composition. In all four cores, the measured Pb concentration (up to 460 mg kg−1) lies significantly above the natural background (27-40 mg kg−1), although a significant decrease (down to 75 mg kg−1) was observed during the second half of the 20th century which can be explained by the reduction of lead emissions. The 206Pb/207Pb ratio measured in these samples indicates that the main source of Pb used in the Paris conurbation is characterized by a “Rio Tinto” signature (defined as 206Pb/207Pb = 1.1634 ± 0.0001). A high contribution, up to 25%, from the leaded gasoline (characterized by 206Pb/207Pb = 1.08 ± 0.02) is revealed in the Seine River downstream Paris, indicating that lead from the leaded gasoline is preferentially released to the river.The dominating Pb signature in the Paris conurbation that is currently sampled through incinerators fumes (206Pb/207Pb = 1.1550 ± 0.0005) and waste water treatment plant (206Pb/207Pb = 1.154 ± 0.002), represents a mixture of highly recycled lead from the Rio Tinto mine and lead from leaded gasoline (imprinted by the low 206Pb/207Pb of the Broken Hill mine). This signature is called “urban” rather than “industrial”, because it is clearly distinct from the Pb that is found in areas contaminated by heavy industry, i.e. the heavy industries located on the Oise River which used lead from European ores characterized by high 206Pb/207Pb ratios (∼1.18-1.19) and possibly a minor amount of North American lead (206Pb/207Pb ratios > 1.20). The “urban” signature is also found in a rural area upstream of Paris in the 1970’s. At the Seine River mouth in 2003, Pb with an urban signature represents 70% of the total Pb sediment content, with the 30% remaining corresponding to natural Pb.  相似文献   

2.
Atmospheric lead (Pb) pollution during the last century in central Yunnan province, one of the largest non-ferrous metal production centers in China, was reconstructed using sediment cores collected from Fuxian and Qingshui Lakes. Lead concentrations and isotopic ratios (207Pb/206Pb and 208Pb/206Pb) were measured in sediment cores from both lakes. The operationally defined chemical fractions of Pb in sediment core from Fuxian Lake were determined by the optimized BCR procedure. The chronology of the cores was reconstructed using 210Pb and 137Cs dating methods. Similar three-phase variations in isotopic ratios and enrichment factors of Pb were observed in the sediment cores from both lakes. Before the 1950s, the sediment data showed low 207Pb/206Pb and 208Pb/206Pb ratios and enrichment factors (EFs?=?~1), indicating that the sedimentary Pb was predominantly of lithogenic origin. However, these indices were increased gradually between the 1950s and the mid-1980s, implying an atmospheric Pb deposition. The EFs and isotopic ratios of Pb reached their peak during recent years, indicating aggravating atmospheric Pb pollution. The average anthropogenic Pb fluxes since the mid-1980s were estimated to be 0.032 and 0.053 g m?2 year?1 recorded in Fuxian and Qingshui cores, respectively. The anthropogenic Pb was primarily concentrated in the reducible fraction. Combining the results of Pb isotopic compositions and chemical speciations in the sediment cores and in potential sources, we deduced that recent aggravating atmospheric Pb pollution in central Yunnan province should primarily be attributed to regional emissions from non-ferrous metal production industries.  相似文献   

3.
Total lead (Pb) concentration and Pb isotopic ratio (206Pb/207Pb) were determined in 140 samples from the Seine River basin (France), covering a period of time from 1945 to 2011 and including bed sediments (bulk and size fractionated samples), suspended particulate matter (SPM), sediment cores, and combined sewer overflow (CSO) particulate matter to constrain the spatial and temporal variability of the lead sources at the scale of the contaminated Seine River basin. A focus on the Orge River subcatchment, which exhibits a contrasted land-use pattern, allows documenting the relation between hydrodynamics, urbanization, and contamination sources. The study reveals that the Pb contamination due to leaded gasoline that peaked in the 1980s has a very limited impact in the river nowadays. In the upstream Seine River, the isotopic ratio analysis suggests a pervasive contamination which origin (coal combustion and/or gasoline lead) should be clarified. The current SPM contamination trend follows the urbanization/industrialization spatial trend. Downstream of Paris, the lead from historical use originating from the Rio Tinto mine, Spain (206Pb/207Pb?=?1.1634?±?0.0001) is the major Pb source. The analysis of the bed sediments (bulk and grain size fractionated) highlights the diversity of the anthropogenic lead sources in relation with the diversity of the human activities that occurred in this basin over the years. The “urban” source, defined by waste waters including the CSO samples (206Pb/207Pb?=?1.157?±?0.003), results of a thorough mixing of leaded gasoline with “historical” lead over the years. Finally, a contamination mixing scheme related to hydrodynamics is proposed.  相似文献   

4.
Ratios of 206Pb/207Pb in a Lochnagar sediment core slowly decline from c. 1.32 at 140 cm to c. 1.23 at 9 cm, and then rapidly decline to c. 1.15 at the surface. Ninety percent of the Pb in the surface sediments can be attributed to anthropogenic sources. The 206Pb/207Pb ratio data imply that catchment peat surface contains a higher fraction of anthropogenic Pb than the sediment surface. The 206Pb/207Pb ratios in the surface of the sediment core are consistent with ratios in trapped sediments collected annually between 1998 and 2003. However, there is no significant decline in these recent samples suggesting that the reduction in atmospheric Pb emissions has not yet been recorded by the sediments due to Pb inputs from the catchment. As catchment peats store about 840 kg previously deposited anthropogenic Pb since 1860, it is likely that catchment inputs will continue to affect future 206Pb/207Pb ratios.  相似文献   

5.
During Fall 1996, epiphytic lichens were collected along altitudinal sections in two areas of France (the Vosges mountains in the North-East, and the Alps, in Haute-Savoie) in order to verify any geographic distribution of atmospheric metals on a small scale. These lichens have various Pb isotopic compositions (206Pb/207Pb=1.126–1.147) which are correlated with the altitude of sampling. Lichens sampled near valleys display isotopic ratios significantly less radiogenic than those sampled at several hundred to thousand meters of altitude. In the Vosges sections, Pb concentrations and isotopic compositions of lichens may be used to define three zones: (1) valley: Pb-rich and non-radiogenic ratios, (2) transition: low-Pb and intermediate isotopic compositions, (3) mountain: heterogeneous Pb concentrations but more radiogenic and homogeneous Pb isotopic composition. Other metals (Zn, Cu, Cd, As), when normalised one to another, are not fractionated between these zones and display homogeneous relative abundance along the altitudinal sections of both sites. Variation of 206Pb/207Pb ratios with altitude is interpreted in terms of mixing of at least two pollution sources: one being the petrol (leaded and/or unleaded) combustion, and the other being of industrial origin. The latter is characterised by a more radiogenic isotopic composition. The Pb isotopic composition of flue gas residues from different municipal solid waste combustors in the Rhine valley and in other areas of France would suggest that these plants might be an important source of industrial Pb in the atmosphere. If the average industrial Pb in France has a 206Pb/207Pb close to 1.15, between 60 and 80% of the total Pb in lichens from the Rhine valley would come from gasoline combustion, whereas 85–90% of the Pb would have an industrial origin in lichens from higher altitude in the Vosges mountains. Although lichens from the Alps were collected at higher altitude, the percentage of industrial Pb for these lichens would be slightly lower (65%). Major winds and convection winds in the different valleys must then play an important role in term of distribution of atmospheric Pb in function of altitude.  相似文献   

6.
Ratios of stable lead isotopes (204Pb, 206Pb, 207Pb, 208Pb) are used to characterize both spatial and temporal variations in anthropogenic emissions of industrial lead aerosols to the atmosphere of northwestern France. Differences in isotopic compositions of aerosols collected from a rural area (Wimereux) in the Nord-Pas de Calais region along the English Channel in 1982–1983 (206Pb/207Pb=1.108±0.005) and 1994 (206Pb/207Pb=1.148±0.003) are paralleled by similar variations in urban aerosols within France during the same period (e.g., 206Pb/207Pb=1.115±0.008 from 1981–1989 and 1.143±0.006 from 1992–1995). These results correlate well with recent findings in the Mediterranean basin (Alleman, 1997) where this radiogenicity increase is clearly associated with industrial sources other than leaded gasoline that has remained relatively constant during its phasing out (206Pb/207Pb=1.08–1.11). Here we used archived data, air mass trajectories and aerosol diameters combined with isotopic signatures to confirm this trend at a regional scale. Indeed, the main industrial signatures from lead smelting (206Pb/207Pb=1.133±0.001) and steel metallurgy (206Pb/207Pb=1.196±0.015) in northwestern France appear more radiogenic than that of leaded gasoline. The shift in isotopic compositions also conform with the systematic change in the mean size (diameter) of aerosols at Wimereux, which ranged from 0.30 to 0.61 μm in 1982–1984 and from 0.70 to 0.89 μm in 1994.  相似文献   

7.
Lead isotopic ratios (LIR) of eight common food items, street dust, coal, diesel, sediments, lead ore and rainwater from India have been reported for the first time in this paper. This study characterized the source and extent of lead pollution in the different foodstuff consumed in Kolkata, a major metropolis of eastern India. The atmospheric lead input to the food items, sold openly in busy roadside markets of the city, has been quantified. The mean 207/206 and 208/206 LIRs of the eight food items ranged from 0.8847 to 0.8924 and 2.145 to 2.167, respectively. Diesel had the highest mean 207/206 and 208/206 values of 0.9015 and 2.1869, respectively, apart from the lead ore. The food items had a mean lead concentration between 3.78 and 43.35 mg kg?1. The two ratio scatter plots of all the different environmental matrices were spread linearly between the uncontaminated Ichapur sediment and diesel. The 207/206 LIRs of the coal with a mean of 0.8777 did not fall in the linear trend, while the street dust and food samples overlapped strongly. The rainwater sample had a 207/206 LIR of 0.9007. Contaminated sediments in Dhapa, the repository of the city’s municipal garbage, had a mean 207/206 LIR of 0.8658. The corresponding value obtained from the sewage-fed vegetable grown there was 0.8058. The present study indicated that diesel was one of the main contributor to Pb pollution. The atmospheric lead contribution to the food items was in the range of 68.48–86.66 %.  相似文献   

8.
Historical changes of anthropogenic Pb pollution were reconstructed based on Pb concentrations and isotope ratios in lake and peat sediment profiles from Ny-?lesund of Arctic. The calculated excess Pb isotope ratios showed that Pb pollution largely came from west Europe and Russia. The peat profile clearly reflected the historical changes of atmospheric deposition of anthropogenic Pb into Ny-?lesund, and the result showed that anthropogenic Pb peaked at 1960s-1970s, and thereafter a significant recovery was observed by a rapid increase of (206)Pb/(207)Pb ratios and a remarkable decrease in anthropogenic Pb contents. In contrast to the peat record, the longer lake record showed relatively high anthropogenic Pb contents and a persistent decrease of (206)Pb/(207)Pb ratios within the uppermost samples, suggesting that climate-sensitive processes such as catchment erosion and meltwater runoff might have influenced the recent change of Pb pollution record in the High Arctic lake sediments.  相似文献   

9.
In order to characterize airborne lead in eastern and central Russian cities in terms of lead isotope ratios, aerosol samples were collected at six selected cities and Moscow, and their lead concentrations and isotope ratios were studied by comparing them to the data of ore lead used in Russia. All eastern Russian cities (Vladivostok, Khabarovsk and Yakutsk) were found to have isotope ratios similar to those of ore leads in Kazakhstan, the major lead producer for Russia. Samples collected in Moscow also showed isotope ratios similar to those of eastern Russian cities. The contribution from coal combustion to airborne lead was considered to be small even in winter, in these cities. This observation suggested that the origin of lead in these Russian atmosphere regions is closely related to the lead products (e.g. leaded gasoline). The lead isotope ratios in three eastern Russian cities were very close to the value for Russian air mass reported previously in Japan, which were also in good agreement with the same observation in Sweden. However, considerably different lead isotope ratios were observed in central Russian cities, Kemerovo and Nizhnevartovsk, indicating that specific lead emissions, such as industrial activities using Precambrian-age ores or unique leaded gasoline, might contribute to the atmospheric lead.  相似文献   

10.
The rapid economic development in the Yangtze River Delta (YRD), China in the last three decades has had a significant impact on the environment of the East China Sea (ECS). Lead isotopic compositions of a 210Pb dated sediment core collected from the coastal ECS adjacent to the Yangtze River Estuary were analyzed to track the Pb pollution in the region. The baseline Pb concentration in the coastal ECS sediments before the industrialization in China was 32 μg g−1, and the corresponding 206Pb/207Pb ratio was 1.195. The high-resolution profiles of Pb flux and 206Pb/207Pb ratios had close relationships with the economic development and the history of the use of leaded gasoline in China, and they were clearly different from those of most European countries and United States.  相似文献   

11.
Urban soil Pb contamination is a great human health risk. Lead distribution and source in topsoils from 14 parks in Shanghai, China were investigated along an urban-rural gradient. Topsoils were contaminated averagely with 65 mg Pb kg−1, 2.5 times higher than local soil background concentrations. HCl-extracts contained more anthropogenic Pb signatures than total sample digests as revealed by the higher 207/206Pb and 208/206Pb ratios in extracts (0.8613 ± 0.0094 and 2.1085 ± 0.0121 versus total digests 0.8575 ± 0.0098 and 2.0959 ± 0.0116). This suggests a higher sensitivity of HCl-extraction than total digestion in identifying anthropogenic Pb sources. Coal combustion emission was identified as the major anthropogenic Pb source (averagely 47%) while leaded gasoline emission contributed 12% overall. Urbanization effects were observed by total Pb content and anthropogenic Pb contribution. This study suggests that to reduce Pb contamination, Shanghai might have to change its energy composition to clean energy.  相似文献   

12.
Lead concentrations and Pb isotope ratios were measured in the forest floor, mineral soil and vegetation at a white pine and a sugar maple stand in a woodland in south central Ontario. Lead concentrations decreased and 206Pb/207Pb ratios increased with mineral soil depth reflecting the mixing of pollution and natural Pb sources. Lead concentrations and 206Pb/207Pb ratios at 20-30 cm depth were approximately 6-7 mg/kg and 1.31-1.32, respectively. Assuming an integrated 206Pb/207Pb ratio in deposition over time of 1.18, estimated from lichen measurements and published data for the region, approximately 65% of Pb in the surface (0-1 cm) mineral soil is from anthropogenic sources. Approximately 90% of pollution Pb is found in the 0-10 cm soil layer (Ah) and less than 3% of the pollution Pb is present in the forest biomass and mull-type forest floor combined. Despite low Pb concentrations in vegetation (<2.5 mg/kg), we estimate that between 65 and 100% of the Pb in vegetation and approximately 75% of the Pb in the forest floor is from pollution sources. In total, the pollution Pb burdens at the pine and maple stands are estimated to be 860 and 750 mg/m2, respectively.  相似文献   

13.
Soil samples from the vicinity of a non-ferrous metal smelter near Plovdiv, Bulgaria contained very high concentrations of cadmium, lead and zinc (up to 140, 4900 and 5900 mg kg(-1), respectively). A roadside soil in a relatively uncontaminated area also contained high concentrations of the same metals (24, 1550 and 1870 mg kg(-1), respectively) indicating that the transport of ores could be a source of contamination. Even though the lead isotope ratios in all the samples fell within a very narrow range (for example, 1.186-1.195 for (206)Pb/(207)Pb), the samples could be differentiated into three distinct groups: ores ((206)Pb/(207)Pb and (208)Pb/(207)Pb ratios of 1.1874-1.1884 and 2.4755-2.4807, respectively), current deposition (1.1864 and 2.4704-2.4711, respectively) and local background (1.1927-1.1951 and 2.4772-2.4809, respectively). Although most of the current deposition has its origin in the ores used at the smelter, up to 12% could be from other sources such as petrol lead.  相似文献   

14.
Lead (Pb), like many other pollutants, is carried into the Arctic by long-range atmospheric transport from industrial centers at lower latitudes. Unlike other pollutants, Pb can be used to assess emission source regions through the use of stable Pb isotope analyses. Using sediment cores from 17 lakes (three profiles and 14 top/bottom sample pairs) in the Søndre Strømfjord (Kangerlussuaq) region, West Greenland (67°N), this study assesses the extent and origin of Pb pollution along a 150 km transect between the Inland Ice and Davis Strait. Like ice core analyses from the interior of Greenland, the isotope analyses suggest pre-industrial contamination, although significant concentration changes in the lake sediments do not occur until the 18th/19th centuries, with the maximum concentrations occurring about 1970. Compared to the background, the Pb concentrations in recent sediments have increased about 2.5-fold, with slightly higher enrichments towards the coast, where annual precipitation is highest. For all of the lakes, there is a major decline in the 206Pb/207Pb ratio in the recent sediments (mean 1.218±0.030) as compared to deeper sediments (mean 1.365±0.084). Using a Pb isotope mixing model, we calculated an excess Pb isotope ratio, i.e. the isotope ratio necessary to produce the observed declines in recent sediments. While studies of atmospheric aerosols in the high Arctic (206Pb/207Pb ratio ∼1.16) have indicated that Russian emissions (206Pb/207Pb ratio ∼1.15–1.16) are a dominant source of arctic pollution, the excess Pb ratios of the lake sediments in the Søndre Strømfjord region (206Pb/207Pb ratio ∼1.14–1.15), in the low Arctic, suggest that W Europe (206Pb/207Pb ratio ∼1.14) is also a major emission source for this region.  相似文献   

15.
Cores covering the last 6000 years were recovered from two marshes from south-western France. They were studied in an attempt to build a reliable regional record of heavy metal pollution. The cores were dated using 14C and historical data. Both Pb concentrations and Pb isotopic composition (206Pb/207Pb and 208Pb/206Pb) were measured in bulk sediment samples using the inductively coupled plasma-mass spectrometer technique. The evolution of the 206Pb/207Pb ratio recorded in both marshes reveals a good correlation with the worldwide Pb production during the last 5000 years. The lead isotopic records reveal some general trends, along with a few typical events such as the imprints of the pre-anthropogenic background between 6000 and 2300 years BP, the mining activity during the Roman and Greek periods from 2300 to 1700 years BP, the fall of the Roman Empire and the mining activity in Central Europe since the 11th century AD. These results are also consistent with records obtained in other European environments. Consequently, the European atmospheric signal is recorded in these marshes, hiding expected local riverine contributions. Thus, such records may contribute to the construction of a chronological standard curve for continental environments. However, it will be necessary to study other records more accurately dated to obtain an adequate precision before such a reference curve can be set-up.  相似文献   

16.
Even after its being phased out in gasoline in the late 90s, lead (Pb) is still present at relatively high levels in the atmosphere of Beijing, China (0.10–0.18 μg m?3). Its origin is subject to debate as several distinct sources may contribute to the observed pollution levels. This study proposes to constrain the origin(s) of Pb and strontium (Sr) in aerosols, by coupling both Pb and Sr isotope systematics. The characterisation of the main pollution sources (road traffic, smelters, metal refining plants, coal combustion, cement factories, and soil erosion) shows that they can unambiguously be discriminated by the multi-isotope approach (206Pb/204Pb and 87Sr/86Sr). The study of total suspended particulates (TSP) and fine particles (PM2.5) from Beijing and its vicinity indicates that both size fractions are controlled by the same sources. Lead isotopes indicate that metal refining plants are the major source of atmospheric lead, followed by thermal power stations and other coal combustion processes. The role of this latter source is confirmed by the study of strontium isotopes. Occasionally, emissions from cement plants and/or input from soil alteration are isotopically detectable.  相似文献   

17.
Rapid urbanization and industrialization in South China has placed great strain on the environment and on human health. In the present study, the total suspended particulate matter (TSP) in the urban and suburban areas of Hong Kong and Guangzhou, the two largest urban centres in South China, was sampled from December 2003 to January 2005. The samples were analysed for the concentrations of major elements (Al, Fe, Mg and Mn) and trace metals (Cd, Cr, Cu, Pb, V and Zn), and for Pb isotopic composition. Elevated concentrations of metals, especially Cd, Pb, V and Zn, were observed in the urban and suburban areas of Guangzhou, showing significant atmospheric trace element pollution. Distinct seasonal patterns were observed in the heavy metal concentrations of aerosols in Hong Kong, with higher metal concentrations during the winter monsoon period, and lower concentrations during summertime. The seasonal variations in the metal concentrations of the aerosols in Guangzhou were less distinct, suggesting the dominance of local sources of pollution around the city. The Pb isotopic composition in the aerosols of Hong Kong had higher 206Pb/207Pb and 208Pb/207Pb ratios in winter, showing the influence of Pb from the northern inland areas of China and the Pearl River Delta (PRD) region, and lower 206Pb/207Pb and 208Pb/207Pb ratios in summer, indicating the influence of Pb from the South Asian region and from marine sources. The back trajectory analysis showed that the enrichment of heavy metals in Hong Kong and Guangzhou was closely associated with the air mass from the north and northeast that originated from northern China, reflecting the long-range transport of heavy metal contaminants from the northern inland areas of China to the South China coast.  相似文献   

18.
Li HB  Yu S  Li GL  Deng H 《Chemosphere》2012,88(10):1161-1169
Lead contamination becomes of importance to urban resident health worldwide, especially for child health and growth. Undisturbed lake sediment cores are increasingly employed as a useful tool to backdate environmental contamination history. Five intact sediment cores collected from lakes in five urban parks were dated using (210)Pb and analyzed for total Pb content and isotope ratio to reconstruct the Pb contamination history over the last century in Shanghai, China. Total Pb content in the sediment cores increased by about 2- to 3-fold since 1900s. The profile of Pb flux in each sediment core revealed a remarkable increase of Pb contamination in Shanghai over the past century, especially in the latest three decades when China was experiencing a rapid economic and industrial development. Significant correlations were found between Pb fluxes in sediment cores and Pb emission from coal combustion in Shanghai. Coal combustion emission dominated anthropogenic Pb sources during the past century contributing from 52% to 69% of total Pb in cores, estimated by a three-end member model of Pb isotope ratios. Leaded gasoline emission generally contributed <30% of total Pb, which was banned by 1997 in the Shanghai region. Our results implicate that coal combustion-based energy consumption should be replaced, or at least partially replaced, to reduce health risks of Pb contamination in Shanghai.  相似文献   

19.
An approximately 59-year (1955–2014) sedimentary record of metal elements (Cu, Pb, Zn, Ni, Co, Mn, and Fe) in a sediment core, collected from the Huaihe River, Huainan City, Anhui Province, China, was reconstructed by using 210Pb geochronology. Copper, Zn, Ni, Co, and Mn evaluated by enrichment factor (EF) indicated minor contamination due to water pollution accidents of the Huaihe River that occurred in 1990s and 2004. Lead presented the most severe pollution among the metals studied, especially during 1957–1974. The use of leaded petrol and atmospheric deposition of coal combustion flue gases could have contributed to Pb contamination. In spite of the general good quality (mean sediment pollution index (SPI) 35.69) of the sediment core evaluated by SPI based on the principal component analysis, worse sediment qualities in the upper section (<6 cm, 2004) were still observed, suggesting intensive human activities causing the increasing concentrations of metals in recent decades.  相似文献   

20.
In the context of intense emissions causing atmospheric pollution, tree growth reductions could be related to soil chemistry modifications or direct foliar injuries. To verify these hypotheses, mineral soils were sampled in an area (Murdochville, Canada) where previous studies had demonstrated that tree growth was impacted by smelter emissions and that forest floor lead concentrations could be used as a proxy for atmospheric pollutant depositions. Samples were analysed for Al, Pb (concentrations and isotope ratios), basic cations (Ca, K, P, and Mg) and Zr. Mass balance calculations were performed on soil profiles to assess vertical migration of elements. Pb concentrations in litter diminished gradually with distance from the smelter. The Pb isotope ratios in these organic soil layers were close to those measured in the Murdochville ores. These patterns were not encountered in mineral soil layers. Pb isotope ratios in these layers were close to those measured in uncontaminated geological materials, and Pb concentrations and basic cation depletions were not related to the proximity of the smelter. Growth reduction was closely associated with litter Pb concentrations, which were used as a proxy for atmospheric deposition, but was not correlated with any elemental concentration or cation depletion measured in mineral soil layers. Our overall results suggest that trees responded mainly to direct atmospheric emissions, which caused foliar damage, rather than to soil chemistry modifications.  相似文献   

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