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1.
Two cores collected in 2001 and 2004 from Flanders Moss ombrotrophic peat bog in central Scotland were dated (14C, 210Pb) and analysed (ICP-OES, ICP-MS) to derive and compare the historical atmospheric deposition records of Sb and Pb over the past 2500 years. After correction, via Sc, for contributions from soil dust, depositional fluxes of Sb and Pb peaked from ca. 1920-1960 A.D., with >95% of the anthropogenic inventories deposited post-1800 A.D. Over the past two centuries, trends in Sb and Pb deposition have been broadly similar, with fluctuations in the anthropogenic Sb/Pb ratio reflecting temporal variations in the relative input from emission sources such as the mining and smelting of Pb ores (in which Sb is commonly present, as at Leadhills/Wanlockhead in southern Scotland), combustion of coal (for which the Sb/Pb ratio is approximately an order of magnitude greater than in Pb ores) and exhaust emissions (Pb from leaded petrol) and abrasion products from the brake linings (Sb from heat-resistant Sb compounds) of automobiles. The influence of leaded petrol has been most noticeable in recent decades, firstly through the resultant minima in Sb/Pb and 206Pb/207Pb ratios (the latter arising from the use of less radiogenic Australian Pb in alkylPb additives) and then, during its phasing out and the adoption of unleaded petrol, complete by 2000 A.D., the subsequent increase in both Sb/Pb and 206Pb/207Pb ratios. The extent of the 20th century maximum anthropogenic enrichment of Sb and Pb, relative to the natural Sc-normalised levels of the Upper Continental Crust, was similar at approximately 50- to 100-fold. Prior to 1800 A.D., the influence of metallurgical activities on Sb and Pb concentrations in the peat cores during both the Mediaeval and Roman/pre-Roman periods was discernible, small Sb and Pb peaks during the latter appearing attributable, on the basis of Pb isotopic composition, to the mining/smelting of Pb ores indigenous to Britain.  相似文献   

2.
The isotopic composition of lead collected with grass samples taken over the period 1989-2001 from plots at two upland locations (Glensaugh in north east and Hartwood in central Scotland) has been determined using thermal ionisation mass spectrometry. Although marked reductions in lead concentrations in grass were observed at Glensaugh in the initial three years, subsequently concentrations have remained relatively constant (1-3 microg g(-1)) in all plots to the present day. The one exception was a roadside plot at Hartwood which showed a large reduction from 1.0 microg g(-1) in 1999 to 0.2 microg g(-1) in 2000 following the abolition of petrol lead in the UK at the beginning of 2000. The total concentrations at this plot were consistently lower than those found at plots away from road traffic but exposed to the prevailing wind direction. The 206Pb/207Pb ratio increased steadily at all the plots throughout the period of the study indicating the reducing influence of petrol lead but the changes were not as great as might be expected with the decrease in the use of leaded petrol. Assuming the collected lead had only two sources, petrol lead and a diffuse background "industrial" lead, the proportion of petrol lead was only in the range 17-69% for roadside samples and 0-39% in other samples. A substantial proportion of deposited lead, therefore, now has its origin other than in petrol. Mixing curves indicate that whereas the lead deposited at Glensaugh could be defined by only two end members, that at Hartwood needs more than two components in the mixture. The results also suggest that although petrol lead has been eliminated, traffic is still a source of lead and another source defined as "traffic lead" should be considered.  相似文献   

3.
Samples of tree bark, which accumulate airborne material, were collected from seven locations in the UK to provide an indication of the magnitude and source of lead pollution. Measurement of the Pb content and 206/207Pb stable isotope ratio by inductively coupled plasma mass spectrometry revealed significant differences between the sites. The concentration of Pb varied over almost four orders of magnitude from 7.2 to 9,600 micrograms g-1, the maximum values being found near a 'secondary' Pb smelter. The 206/207Pb isotope ratios varied from 1.108 +/- 0.002 to 1.169 +/- 0.001. The lowest Pb concentrations and highest isotope ratios were detected in bark samples from the Scilly Isles, reflecting the low-level of industry and road traffic. In contrast, samples obtained from a city centre (Sheffield) and near a motorway (M1) contained 25-46 micrograms g-1 Pb and recorded the lowest 206/207Pb ratios. Higher concentrations in the vicinity of a coal-fired power station recorded a 206/207Pb ratio of 1.14, suggesting a significant contribution from fly-ash. The relative contribution of lead from petrol (206/207Pb = 1.08) and other sources such as coal (206/207Pb = 1.18) were thus estimated using mass balance equations. Tree bark near the lead smelter recorded an intermediate 206/207Pb ratio of 1.13 reflecting the processing of material of mixed origin.  相似文献   

4.
Pb isotope compositions of biologically significant PM(10) atmospheric particulates from a busy roadside location in London UK were measured using solution- and laser ablation-mode MC-ICP-MS. The solution-mode data for PM(10) sampled between 1998-2001 document a dramatic shift to increasingly radiogenic compositions as leaded petrol was phased out. LA-MC-ICP-MS isotope analysis, piloted on a subset of the available samples, is shown to be a potential reconnaissance analytical technique. PM(10) particles trapped on quartz filters were liberated from the filter surface, without ablating the filter substrate, using a 266 nm UV laser and a dynamic, large diameter, low-fluence ablation protocol. The Pb isotope evolution noted in the London data set obtained by both analytical protocols is similar to that observed elsewhere in Western Europe following leaded petrol elimination. The data therefore provide important baseline isotope composition information useful for continued UK atmospheric monitoring through the early 21(st) century.  相似文献   

5.
Soil samples (0-25 cm) have been taken annually since 1991 from three protected plots set up at an upland location at Glensaugh in Aberdeenshire, Scotland. The soils were analysed using the original BCR sequential extraction procedure and the lead isotopic composition was determined in each of the fractions, as well as the unfractionated soil using thermal ionisation mass spectrometry (TIMS). The lead concentrations in all the soils, including those well away from the road, were much higher than typical background values indicating that the whole area has been subject to deposition of anthropogenic lead. The distribution of lead between the different fractions was similar for the two non-roadside soils with most lead present in the oxidizable fraction. Although most lead in the roadside soil was also present in the oxidizable fraction, a substantial proportion (about 10%) was in the easily soluble fraction suggesting that roadside lead could be more mobile than lead in the other soils. Good reproducibility was obtained for the isotope analyses in all the fractions. The ratios calculated for the bulk soil from the ratios in the individual fractions agreed very closely with those measured directly in the unfractionated soil thereby demonstrating both reproducibilty and accuracy. The lowest (206)Pb/(207)Pb ratios were found in the roadside soil consistent with the recent deposition of petrol lead. The (206)Pb/(207)Pb ratios in all fractions of the other soils fell into a narrow band and it was necessary to use (204)Pb ratios to differentiate between lead in the extractable fractions and lead in the residual component. It is probable that lead in the non-roadside soils was deposited a considerable time ago and is characterised by a relatively high (206)Pb/(207)Pb ratio. Use of the (204)Pb ratios showed that the residual components in each of the three soils were isotopically distinct.  相似文献   

6.
Bark included within the trunk of a 200-year-old Japanese cedar tree harvested in Yakushima Island, Japan, a World Natural Heritage Site located 150 km south of mainland Japan and 800 km east of Shanghai, China, was analysed for trace metals by ICP-MS providing a chronology of atmospheric pollution. The concentration of V, As and Pb in decadal sections of the bark pocket increased 30 to 50 fold from 1900-09 to 1960-69, indicating increased atmospheric deposition of these metals. The trend coincided with the establishment and expansion of heavy industries in Kyushu, Japan, resulting in locally high levels of air pollution. V, As and Pb subsequently declined, reflecting lower industrial emissions following air pollution control legislation from the late 1960's and decline in heavy industries. Ni, Cu and Zn showed a relatively small, 7 to 10 fold increase over time. Lead isotope ratios in the bark pockets shifted from about 0.84 to 0.86 for 207Pb/206Pb and from 2.04 to 2.10 for 208Pb/206Pb, showing that the origin of atmospheric lead changed over time from coal to more diverse sources.  相似文献   

7.
If it is assumed that the Pb collected in grass samples is derived mainly from atmospheric deposition then grass samples can be used as a convenient and easily analysed monitor for Pb deposition, in particular to establish the isotopic composition of current deposition in remote locations. As some studies have demonstrated a strong correlation between soil and grass Pb concentrations, it was considered important to establish the proportion of soil Pb in the grasses used to monitor atmospheric deposition at upland locations in Scotland. Consideration of earlier studies provided evidence that very little, if any, Pb in grass was derived from soil. Lead isotope analysis, by thermal ionisation mass spectrometry, of grasses grown on soils spiked with enriched (207)Pb in the field situation allowed the relative contribution of atmospheric deposition and soil to the grass Pb to be calculated. In most cases, >80% of Pb in grass was derived from atmospheric deposition and in recent years this value was >90%. Recalculation of the (206)Pb/(207)Pb ratio in grass samples showed that there was very little error in the results, published previously, which were based on the assumption that all the Pb collected with grass was derived from the atmosphere. The trends established by measuring the (206)Pb/(207)Pb ratio in grasses were confirmed and remain valid.  相似文献   

8.
Lead concentrations and isotopic ratios were measured along two well-dated sediment cores from two distant lakes: Anterne (2100 m a.s.l.) and Le Bourget (270 m a.s.l.), submitted to low and high direct human impact and covering the last 250 and 600 years, respectively. The measurement of lead in old sediment samples (>3000 BP) permits, in using mixing-models, the determination of lead concentration, flux and isotopic composition of purely anthropogenic origin. We thus show that since ca. 1800 AD the regional increase in lead contamination was mostly driven by coal consumption ((206)Pb/(207)Pb approximately 1.17-1.19; (206)Pb/(204)Pb approximately 18.3-18.6), which peaks around 1915 AD. The increasing usage of leaded gasoline, introduced in the 1920s, was recorded in both lakes by increasing Pb concentrations and decreasing Pb isotope ratios. A peak around 1970 ((206)Pb/(207)Pb approximately 1.13-1.16; (206)Pb/(204)Pb approximately 17.6-18.0) corresponds to the worldwide recorded leaded gasoline maximum of consumption. The 1973 oil crisis is characterised by a drastic drop of lead fluxes in both lakes (from approximately 35 to <20 mg cm(-2) yr(-1)). In the late 1980s, environmental policies made the Lake Anterne flux drop to pre-1900 values (<10 mg cm(-2) yr(-1)) while Lake Le Bourget is always submitted to an important flux (approximately 25 mg cm(-2) yr(-1)). The good match of our distant records, together and with a previously established series in an ice core from Mont Blanc, provides confidence in the use of sediments as archives of lead contamination. The integration of the Mont Blanc ice core results from Rosman et al. with our data highlights, from 1990 onward, a decoupling in lead sources between the high elevation sites (Lake Anterne and Mont Blanc ice core), submitted to a mixture of long-distance and regional contamination and the low elevation site (Lake Le Bourget), where regional contamination is predominant.  相似文献   

9.
南极大气气溶胶中铅同位素比值的研究   总被引:2,自引:1,他引:1  
通过对电感耦合等离子体质谱(ICP-MS)的工作条件和参数进行优化,建立了ICP-MS测定铅同位素比值的精确方法,测量了2007—2009年南极中山站采集到的气溶胶样品中208Pb/206Pb、207Pb/206Pb和206Pb/207Pb的比值。结果表明,南极大气气溶胶中铅同位素比值在逐年缓慢地发生线性变化,线性相关系数为0.996 2;气溶胶铅同位素示踪揭示南极附近国家(除南非)释放的铅可能成为南极大气中铅的重要来源。  相似文献   

10.
Cores from four Scottish ombrotrophic peat bogs were used to reconstruct the historical record of atmospheric vanadium (V) deposition in Scotland over the last 150 years. The general similarity of V and Pb concentration profile trends in (210)Pb-dated cores from each of the sites strongly suggested that V, like Pb, is essentially immobile in ombrotrophic peat. After allowance via use of the conservative element Ti for the contribution of soil dust V, the deposition of anthropogenic V was found to be greatest (~ 1.3 to 2.0 mg m(-2) y(-1)) in the mid-20(th) century before decreasing to 0.1-0.3 mg m(-2) y(-1) in the early years of the 21(st) century. The latter values were in good agreement with directly measured atmospheric V fluxes at nearby sites, a finding also observed in the case of Pb. The decline in peat-core-derived fluxes for both V and Pb from 1970 to 2004, however, was not as large as the decline in official UK emission estimates for the two metals during this period. This, along with an order of magnitude discrepancy between the anthropogenic V/Pb ratios at the peat core surface and the higher values of the ratio for UK emissions in the early 2000s, suggests that the recently revised UK emissions data for V may perhaps still be overestimated and/or that some previously deposited Pb is being resuspended in the atmosphere.  相似文献   

11.
As a consequence of the accumulation of anthropogenic Pb in upland catchments, there has been much recent concern about the potential mobilisation and transport of Pb from the soils to receiving waters and also the possible harmful effects that this might have on aquatic biota. This paper presents the findings of a two-year study of Pb behaviour in an organic-rich upland catchment at Glensaugh in NE Scotland. Pb inputs to the catchment were characterised by direct measurements of Pb concentration and (206)Pb/(207)Pb ratios in rain water and interception. Pb outputs from the catchment were calculated from measurements on stream water samples taken from the two main streams, the Cairn Burn and Birnie Burn. The relative contribution of Pb from groundwater and throughflow, under different flow conditions (base flow and high flow), to stream waters was investigated via analysis of springs sourced from groundwater and of waters flowing through the various soil horizons (S (surface), A, B, C, and D), respectively. The outcome of intensive sampling and analysis over the two-year time period was that, even with marked reduction in Pb inputs over the past two decades, the catchment was still acting as a net sink for the current atmospheric deposition. Although the Pb isotopic signature for stream water is very similar to that for the contemporaneous rain water ((206)Pb/(207)Pb approximately 1.15-1.16), only a small portion of the rain water is transferred directly to stream water. Instead, the Pb input is transferred to the stream waters mainly via groundwater and it was also confirmed that the latter had a similar Pb isotopic signature. From the Pb isotopic measurements on throughflow waters, however, Pb being removed via the streams contained some previously deposited Pb, i.e. mobilisation of a small portion of soil-derived anthropogenic Pb was occurring. These findings are important not only with respect to the source/sink status of the catchment but also for calculation of the extent of retention of the current atmospheric Pb inputs, which must take account of the release of previously deposited Pb from the catchment soils, a process occurring mainly under high flow conditions.  相似文献   

12.
Examination of car fleet records in Accra demonstrates an increasing proportion of catalytic converter-equipped cars in the relatively old car fleet (average age 13 years) due to their import from developed countries. However, only leaded petrol is sold in Ghana. Lead anti-knocking additives, which are known to affect catalyst activity and promote thermal sintering and mechanical abrasion, may increase Pt emissions. This possible synergism prompted the concomitant determination of Pb and Pt levels in road dust and roadside soils in Ghana. Both metals followed traffic density with higher concentrations in urban areas compared to remote sites. In urban areas, the range for Pb (365 +/- 93 microg g(-1) for dust and 291 +/- 76 microg g(-1) for soil) reflects precatalyst levels in Europe and the US, while the range for Pt (39 +/- 24 ng g(-1) for dust and 15 +/- 5.3 ng g(-1) for soil) is typical for the same countries. The elevated Pt concentrations were unexpected due to recent introduction of catalysts to Ghana compared to the prolonged use of catalysts in Europe and the US.  相似文献   

13.
This study is a continuation of our preceding research identifying suitable environmental samples for the tracing of atmospheric pollution in industrial areas. Three additional types of environmental samples were used to characterise contamination sources in the industrial area of Ostrava city, Czech Republic. The region is known for its extensive metallurgical and mining activities. Fingerprinting of stable Pb isotopes was applied to distinguish individual sources of anthropogenic Pb. A wide range of 206Pb/207Pb ratios was observed in the investigated samples: 206Pb/207Pb = 1.168–1.198 in mosses; 206Pb/207Pb = 1.167–1.215 in soils and 206Pb/207Pb = 1.158–1.184 in tree cores. Black and brown coal combustion, as well as metallurgical activities, is the two main sources of pollution in the area. Fossil fuel burning in industry and households seems to be a stronger source of Pb emissions than from the metallurgical industry. Concentration analyses of tree rings showed that a significant increase in As concentrations occurred between 1999 and 2016 (from 0.38 mg kg?1 to 13.8 mg kg?1). This shift corresponds to the use of brown coal from Bílina, Czech Republic, with an increased As concentration. The burning of low-quality fuels in households remains a problem in the area, as small ground sources have a greater influence on the air quality than do industrial sources.  相似文献   

14.
Lead is a purely toxic heavy metal which induces a wide variety of adverse physiologic effects. Nevertheless, it has been mined and used for more than 8,000 years. Among the different contemporary sources of lead pollution, traffic-induced emissions from the combustion of leaded gasoline is of particular concern, as it can constitute more than 90 percent of total lead emissions into the atmosphere in congested urban areas where no phase-out activities have been adopted. Gasoline lead content and traffic volume are strongly correlated with concentrations of lead in various environmental media. In the absence of policies to reduce the use of lead in gasoline or to favor the use of unleaded gasoline, leaded gasoline remains the predominant grade in many countries. This paper assesses the status of lead pollution from the combustion of leaded gasoline in Beirut based on field measurements of lead in air and roadside dust of urban and rural/suburban areas and recent data on soil and blood lead levels. Average atmospheric lead concentrations was about 1.86 microg m(-3) at urban locations and 0.147 microg m(-3) at suburban locations. The analysis of roadside dust revealed an average lead level of 353 microg g(-1) along urban streets and 125 microg g(-1) along rural/suburban roads. Blood lead levels were also relatively high in comparison to countries where leaded gasoline has been phased-out.  相似文献   

15.
In order to understand relationships between sources and receptors of atmospheric deposition, computer models must be used. This paper describes a Lagrangian acid deposition model that represents emissions of trace species across Northern Europe. The chemistry of sulphur dioxide, dimethyl sulphide and hydrogen sulphide is represented and the model tested against estimates of UK wet and dry deposition. Mean UK wet and dry deposition for the period 1992–1994 was 206 and 145 ktonne S yr-1, respectively. The model predicted wet and dry deposition of 222 and 166 ktonne S yr-1, in good agreement with measurements. The model has been used to examine the sources of deposited S to the UK. For a base year of 1992, 86% of the UK's SO2 emissions are exported. The S deposition attributable from mainland European sources was 36% of the UK total S deposition, in good agreement with other UK models but this differs substantially from the calculations of the EMEP model. Natural sources of S deposition from planktonic emissions of dimethyl sulphide, biological emissions of hydrogen sulphide and non-eruptive volcanic emissions of sulphur dioxide contributed approximately 1% of the modelled UK S deposition, of which 95% originated from dimethyl sulphide. The explicit chemical scheme for dimethyl sulphide incorporated into the model showed that 24% of the resultant deposited S was methane sulphonic acid. Boundary conditions of the model were tested and it was found that initialisation of sulphur dioxide and sulphate concentrations to representative ambient conditions had a very small effect. The modelled contribution of UK and European sources to UK S deposition was approximately 40 and 60%, respectively, showing the dramatic change arising from projected UK SO2 emissions in 2010. This revised version was published online in July 2006 with corrections to the Cover Date.  相似文献   

16.
Pakistan is one of the few countries in Asia thatcontinues to use only leaded-petrol as vehicular fuel. Theconcentration of Pb in its petrol reported in 1991 was thehighest (1.5 – 2.0 g Pb L-1) of all produced by the various Asiancountries and far exceeded the WHOs guideline of 0.15 g Pb L-1. We have undertaken a study to trace and quantify this toxicelement in the environs of Karachi, Pakistans major metropolis,having more than 30% of the nations total number of vehicles.In this article we report the Pb contents of petrol and dieselcurrently manufactured and marketed in the city. Samples of`Regular petrol collected in 1999 was found to contain 0.363 gPb L-1 (range: 0.335 – 0.390 g Pb L-1), a factor of 5 lower than thatmarketed prior to 1991. Its concentration in diesel fuel was muchlower (0.017 g Pb L-1). Based on the available statistical data onthe type and volume of vehicular traffic, we assessed that thecurrent lead emission from vehicular traffic into the atmosphereis 391 metric tons a year, which is a factor of 2.7 lower thanthat estimated for 1989.  相似文献   

17.
A peat core from Lindow bog near Manchester, England, was precisely cut into 2 cm slices to provide a high-resolution reconstruction of atmospheric Pb deposition. Radiocarbon and (210)Pb age dates show that the peat core represents the period ca. 2000 BC to AD 1800. Eleven radiocarbon age dates of bulk peat samples reveal a linear age-depth relationship with an average temporal resolution of 18.5 years per cm, or 37 years per sample. Using the Pb/Ti ratio to calculate the rates of anthropogenic, atmospheric Pb deposition, the profile reveals Pb contamination first appearing in peat samples dating from ca. 900 BC which clearly pre-date Roman mining activities. Using TIMS, MC-ICP-MS, and SF-ICP-MS to measure the isotopic composition of Pb, the (208)Pb/(206)Pb and (206)Pb/(207)Pb data indicate that English ores were the predominant sources during the pre-Roman, Roman, and Medieval Periods. The study shows that detailed studies of peat profiles from ombrotrophic bogs, using appropriate preparatory and analytical methods, can provide new insight into the timing, intensity, and predominant sources of atmospheric Pb contamination, even in samples dating from ancient times.  相似文献   

18.
Epiphytic lichens, collected from 119 sampling sites grown over “Roistonea Royal Palm” trees, were used to assess the spatial distribution pattern of lead (Pb) and identify possible pollution sources in Havana (Cuba). Lead concentrations in lichens and topsoils were determined by flame atomic absorption spectrophotometry and inductively coupled plasma (ICP) atomic emission spectrometry, respectively, while Pb in crude oils and gasoline samples were measured by ICP-time of flight mass spectrometry (ICP-ToF-MS). Lead isotopic ratios measurements for lichens, soils, and crude oils were obtained by ICP-ToF-MS. We found that enrichment factors (EF) reflected a moderate contamination for 71% of the samples (EF > 10). The 206Pb/207Pb ratio values for lichens ranged from 1.17 to 1.20 and were a mixture of natural radiogenic and industrial activities (e.g., crude oils and fire plants). The low concentration of Pb found in gasoline (<7.0 μg L?1) confirms the official statement that leaded gasoline is no longer used in Cuba.  相似文献   

19.
The leaves of roadside Rhododendron pulchrum Sweet were examined as a bioindicator of traffic-related heavy metal pollution in Okayama. Total contents of heavy metals in roadside soil and the R. pulchrum leaves were determined. Results of correlation analyses showed significant correlations among Pb, Ni, and Zn contents of roadside soil and leaf samples. These results suggest that R. pulchrum is a useful bioindicator of heavy metal pollution in traffic areas. To identify traffic-related heavy metal pollution sources, traffic-related materials such as tires, asphalt pavement, and road paint were collected and analyzed. The results of analyses of our data show that Zn is emitted mainly from the abrasion of tires; Cr is emitted mainly from wear of the asphalt pavement. Furthermore, the respective lead isotope ratios in R. pulchrum leaves, soil, roadside dust, and traffic-related materials were measured using inductively coupled plasma mass spectrometry. The isotopic compositions of lead in R. pulchrum leaves were 207Pb/206Pb = 0.861-0.871 and 208Pb/206Pb = 2.093-2.127, which agrees well with ratios in automobile wheel balance weights, suggesting that lead-containing products associated with automobiles, such as wheel balance weights, contribute to traffic-related lead pollution.  相似文献   

20.
Sediment cores from four boreal and remote lakes in a south to north transect in central Sweden were analysed for acid leachable silver, antimony, thallium and indium in the solid sediment phase and the corresponding porewater. Dating of the cores was made by their content of acid leachable lead and the (206)Pb/(207)Pb ratio, in one lake also by (210)Pb. The impact of diagenesis on element redistribution in the sediments was included and found to be minor except for thallium. The results show lowered concentrations towards the north and most intense accumulation after the Second World War, which is taken as evidence for atmospheric deposition being the primary source. Indium has declining concentrations in recent strata while silver and antimony increase. Thallium has lowered acid-leachable concentrations in recent strata. For all metals the impact of domestic industrialisation as well as the early industrialisation of central Europe is discernible. Only thallium appears to reach a geological background at depths that correspond to the late 18th century. For the other metals elevated levels are concluded.  相似文献   

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