Isotopic composition of Zn and Pb atmospheric depositions in an urban/Periurban area of northeastern France

Epiphytic lichens, ambient PM-10, and bus air-filter aerosols collected in a city and the surrounding area were used to monitor urban atmospheric metal deposition in the Metz area, NE France. According to the measured Pb and Zn concentrations, high-enrichment factors (EF) were calculated for lichens collected in 2001 and 2003, suggesting an anthropogenic origin for those metals. Pb and Zn concentrations in lichens and other samples are correlated, probably indicative of the level of pollution recorded. However, different trends and scatters in the relationship suggest decoupling of Zn and Pb sources in this area. The lead isotopic composition of lichens varies largely from downtown, near traffic roads and highways, to suburbs but indicate an overall stability of sources between 2001 and 2003, although some minor variations were noted. Remobilization of Pb from leaded gasoline is still significant. The Zn isotopic composition measured in all lichens yielded fairly homogeneous delta66Zn ranging from -0.2% per hundred to 0.5% per hundred relative to ZnJMC solution. Most lichen samples are indistinguishable from urban aerosols (PM-10 and bus air filters, delta66Zn = 0.12 +/- 0.21% per hundred) and from flue gases from the city waste combustor (delta66Zn = 0.13 +/- 0.12% per hundred). No systematic variations of Zn EF and isotopic compositions were observed for and between 2001 and 2003 samples. Some lichens having unradiogenic 206Pb/207Pb ratios displayed high Zn and negative delta66Zn, indicative of a possible traffic source for Zn. A review from the literature on the Zn isotopic composition of terrestrial materials is reported but a few reservoirs seem to have specific compositions. According to the actual precision obtained, Zn isotopes for tracing pollution sources might not be straightforward but might be potentially useful for specific studies.     

Chronicling a century of lead pollution in Mexico: stable lead isotopic composition analyses of dated sediment cores

Analyses of lead isotopic compositions (204Pb, 206Pb, 207Pb, and 208Pb) of dated sediment cores from two coastal estuaries and two inland lakes chronicle the predominance of industrial lead emissions in Mexico over the past century. These isotopic ratios exhibit a shift in composition from the turn of the previous century (1900) that corresponds with measurable increases (from 2- to 10-fold) in lead concentrations in the cores above their baseline values (3-22 microg/g)--both changes are consistent with the development of Mexican lead production for export and the manufacture of tetraethyl lead additives for Mexican gasolines. While subsequent changes in lead concentrations in the cores correspond with calculated emissions from the combustion of leaded gasoline in Mexico, isotopic compositions of the cores remain relatively constant throughout most of the 1900s (e.g., 206Pb/207Pb = 1.200 +/- 0.003; 208Pb/207Pb = 2.463 +/- 0.004). That isotopic constancy is attributed to the widespread pollution from lead production in Mexico and the dispersion of some of that lead used as an additive in Mexican gasolines.     

Historical trends in the lead isotopic composition of archival Sphagnum mosses from Scotland (1838-2000)

The analysis of almost 200 Scottish Sphagnum moss samples collected over the past 170 years has revealed trends in the isotopic composition of lead similar to those previously established for dated Scottish lake sediments and peat bogs, lending credibility to these proxy records of atmospheric lead contamination and deposition. The effect of temporal variations in contributions from sources such as smelting of indigenous lead ores (206Pb/207Pb approximately 1.16-1.18), coal combustion (206Pb/207Pb approximately 1.17-1.19), and the use of imported Australian lead (206Pb/207Pb approximately 1.04) was clearly seen in the Scottish moss 206Pb/207Pb record. This showed some differences from the corresponding archival herbage record for the south of England, where the initial influence of Australian lead occurred earlier, at the end of the 19th century. A significant decline from a 206Pb/ 207Pb value of approximately 1.17 in the Scottish moss record began in the 1920s and continued until the 1980s (206Pb/207Pb approximately 1.12). The success of measures to reduce lead emissions to the atmosphere over the past 20 years in the U.K., in particular from petrol-engined vehicles using alkyl lead additives manufactured primarily from Australian lead, is evident in both the increasing 206Pb/207Pb ratio and falling lead concentration data for Scottish moss.     

Origin of lead in the United States diet

We report 208Pb/207Pb and 206Pb/207Pb ratios for 1001 duplicate diets collected from mothers and children, 1304 samples of house dust and hand wipes, and 64 samples of aerosols that were taken in Omaha, Nebraska, during the period from 1990 to 1997. A plot of 208Pb/207Pb versus 206Pb/ 207Pb for the dust and hand wipes indicates that they contain lead from ores mined in Idaho, Missouri, and Mexico. The absence of lead from Utah suggests that this mixture is not representative of the whole country. The lead in the aerosols has a narrower range of isotope ratios and resembles aerosols collected elsewhere in the United States. Most dietary collections contain a large component of house dust. Some, especially those from infants, are dominated by uranogenic lead with high 206Pb/207Pb ratios. Its source is taken to be calcium-supplemented food where the calcium is derived from limestone. Another source of lead is thorogenic and is ascribed to lead in tin coatings. Agricultural lead, whether from soil (estimated from recently published analyses of sedimentary materials), fertilizer, or agricultural lime, could not be unambiguously identified in the diets. Lead derived from aerosols, if present at all, is insignificant.     

Asian industrial lead inputs to the North Pacific evidenced by lead concentrations and isotopic compositions in surface waters and aerosols

Recent trends of atmospheric lead deposition to the North Pacific were investigated with analyses of lead in aerosols and surface waters collected on the fourth Intergovernmental Oceanographic Commission Contaminant Baseline Survey from May to June, 2002. Lead concentrations of the aerosols varied by 2 orders of magnitude (0.1-26.4 pmol/m(3)) due in part to variations in dust deposition during the cruise. The ranges in lead aerosol enrichment factors relative to iron (1-119) and aluminum (3-168) were similar, evidencing the transport of Asian industrial lead aerosols across the North Pacific. The oceanic deposition of some of those aerosols was substantiated by the gradient of lead concentrations of North Pacific waters, which varied 3-fold (32.7-103.5 pmol/kg), were highest along with the Asian margin of the basin, and decreased eastward. The hypothesized predominance of Asian industrial lead inputs to the North Pacific was further corroborated by the lead isotopic composition of ocean surface waters ((206)Pb/(207)Pb = 1.157-1.169; (208)Pb/(206)Pb = 2.093-2.118), which fell within the range of isotopic ratios reported in Asian aerosols that are primarily attributed to Chinese industrial lead emissions.     

Transboundary atmospheric lead pollution

A high-temporal resolution collection technique was applied to refine aerosol sampling in Jerusalem, Israel. Using stable lead isotopes, lead concentrations, synoptic data, and atmospheric modeling, we demonstrate that lead detected in the atmosphere of Jerusalem is not only anthropogenic lead of local origin but also lead emitted in other countries. Fifty-seven percent of the collected samples contained a nontrivial fraction of foreign atmospheric lead and had 206Pb/207Pb values which deviated from the local petrol-lead value (206Pb/207Pb = 1.113) by more than two standard deviations (0.016). Foreign 206Pb/207Pb values were recorded in Jerusalem on several occasions. The synoptic conditions on these dates and reported values of the isotopic composition of lead emitted in various countries around Israel suggest that the foreign lead was transported to Jerusalem from Egypt, Turkey, and East Europe. The average concentration of foreign atmospheric lead in Jerusalem was 23 +/- 17 ng/m3, similar to the average concentration of local atmospheric lead, 21 +/- 18 ng/ m3. Hence, the load of foreign atmospheric lead is similar to the load of local atmospheric lead in Jerusalem.     

Historical perspective of industrial lead emissions to the atmosphere from a Canadian smelter

Dated sediment cores from four remote Canadian Shield headwater lakes, where atmospheric deposition has been the only input of anthropogenic Pb, situated along a transect extending 300 km from a nonferrous metal smelter, were analyzed for both lead concentrations and isotopic composition; porewater samples collected at the same sites were analyzed for Pb and other geochemical variables. The depth distributions of stable Pb isotope ratios show the presence of several isotopically distinct Pb types since the preindustrial period. Lead from the smelter emissions had an isotopic signature (e.g., 206Pb/207Pb approximately 0.993) that was clearly distinct from those of Pb in aerosols collected at sites remotefrom point sources in Eastern Canada (e.g., 206Pb/207Pb usually approximately 1.15-1.20) and the United States (e.g., 206Pb/207Pb usually approximately 1.15-1.22), allowing the geographical area impacted by the smelter Pb emissions to be traced. On the basis of the sediment Pb isotopic composition, it is estimated that lead from the smelter accounts for 89%, 88%, and 5-34% of the total inventory of anthropogenic Pb deposited in the sediments of lakes located 10, 25, and 150 km from the smelter, respectively; but lead from this point source was not detected in sediments of a fourth lake that is 300 km from the smelter. We also estimate that the amount of smelter-derived Pb deposited within a distance of 150 km is equivalent to 5-10% of the amount released by leaded gasoline combustion in all of Canada. Sharp decreases in the recent Pb fluxes to lake sediments indicate that the measures taken to mitigate metal emissions from the smelter were effective.     

Seven thousand years of records on the mining and utilization of metals from lake sediments in central China

A 268 cm section of sediment core from Liangzhi Lake in Hubei province in central China was used to assess the use and accumulation of metals in the lake in the past 7,000 years. The concentrations of trace metals, including Cu, Pb, Ni, and Zn, and major elements, Ca, Fe, and Mg, in a 14C- dated segment of sediment core were analyzed. Historical trends on the input of metals to Liangzhi Lake from around 5000 BC to the present were recorded in the sediments, representing about 7,000 years of history on the mining and utilization of metals in central China. The concentrations of Cu, Ni, Pb, and Zn increased gradually from about 3000 +/- 328 BC, indicating the start of the Bronze Age in ancient China. During the period 467 +/- 257 to 215 +/- 221 AD, there was a rapid increase in the concentrations of these metals in the sediments, indicating enormous inputs of these metals at that time. This era corresponded to China's Warring States Period (475- 221 BC) and the early Han Dynasty (206 BC-220 AD), during which copper and lead were extensively used in making bronze articles such as vessels, tools, and weapons. From 1880 +/- 35 AD to the early 1900s, there was also a significant increase in the concentrations of metals such as Cu, Ni, and Pb, which probably reflected the metal emissions and utilization during the early period of industrial development and weapon manufacture during the wars in China. The Pb isotopic analysis showed that the surface and subsurface sediments had lower 206Pb/207Pb and 208Pb/ 207Pb ratios than the deeper layers, reflecting the additional input of Pb from mining activities that took place during the Bronze Age era and in modern times. This study provides direct evidence of the environmental impact of the mining and utilization of metals in the last 7,000 years in one of the important regions of Chinese civilization.     

Tracing of industrial aerosol sources in an urban environment using Pb, Sr, and Nd isotopes

A comprehensive Pb-Sr-Nd isotope tracer study of atmospheric trace metal pollution has been performed in the urban environment of Strasbourg-Kehl. Filter dust of the principal pollutant sources (waste incinerators, thermal power plant and steel plant) and soot of car and ship exhausts have been analyzed. In addition tree barks (as biomonitors) and PM10 have been analyzed to trace and determine the distribution of the pollution in the environment. The industrial sources have highly variable epsilonNd values (-9.7 and -12.5 for incinerators and -17.5 for steel plant). Much higher epsilonNd values have been found for soot of car exhausts (-6 and -6.9). These high values make the Nd isotope system a powerful tool for the discrimination of traffic emissions but especially for the identification of diesel derived particles in the urban environment. The 206Pb/207Pb isotope ratios of gasoline are low (1.089) compared to diesel soot (1.159). The 26Pb/207Pb ratios of 1.151-1.152 for the steel plant and 1.152 for the solid waste incinerator are close to the Pb isotope ratio of diesel. The 87Sr/ 8Sr isotope ratios of the principal industrial sources vary significantly: 0.7095 for the domestic solid waste incinerator, 0.709 for the steel plant, and 0.7087 for car exhaust soot. PM10 aerosols collected in the urban center of Strasbourg show the influence of the pollutant sources at 3-7 km distance from the center. Most of the aerosols Pb isotopic compositions suggest Pb admixtures from at least three sources: a natural background and in function of the wind direction the domestic waste incinerator (S-wind) or the steel plant and the chemical waste incinerator (NE-wind). The traffic contribution can only be estimated with help of Nd isotopes. Therefore the clear identification of different pollutant sources in the urban environment is only possible by combining the three different isotope systems and is based on the fact that significant differences exist between the Pb, Sr, and Nd isotope ratios of the natural atmospheric background and pollutants containing Pb, Sr, and Nd of industrial origin with similar variable 206Pb/207Pb, 87Sr/ 86Sr, and 143Nd/144Nd.     

Isotopic tracing of landfill leachates and pollutant lead mobility in soil and groundwater

Here we provide evidence of the capability of stable lead isotopes to trace landfill leachate in a shallow groundwater. The municipal landfill we have investigated is located in southeastern France. It has no bottom liner, and wastes are placed directly on the ground. Stable lead isotopes allow the characterization of this landfill leachate signature (206Pb/207Pb = 1.189 +/- 0.004) that is clearly different from that of the local atmosphere (206Pb/207Pb = 1.150 +/- 0.006) and crustal lead (206Pb/207Pb = 1.200 +/- 0.005). Piezometers located in the direct vicinity of the landfill generally display this contaminant imprint. The landfill plume is monitored up to 1000 m downgradient of the landfill, in very good agreement with evaluation from chloride concentration. Meanwhile, 206Pb/207Pb ratios measured at a piezometer located 4600 m downgradient of the landfill suggest a contamination by the landfill plume. This result shows that the complexity of a pollutant plume dispersion in this shallow groundwater system requires several independent tracers to clearly resolve origin and transport pathways for contaminants. Furthermore, seasonal rainfall variation for this Mediterranean mixed Quaternary alluvion reservoir and the use of KCl fertilizers might favor an efficient remobilization of atmospheric lead in plowed soils and its transfer into groundwater as shown by lead isotope systematics.     

Identifying sources of Pb exposure in waterbirds and effects on porphyrin metabolism using noninvasive fecal sampling

Waterbird feces (mainly mallard Anas platyrhynchos and coot Fulica atra) were collected from four wetlands in Southern Spain in the field or during capture (n = 558 and n = 59, respectively) to study lead (Pb) shot ingestion. Lead and aluminum (Al) concentrations along with Pb isotope signatures were used to identify sources of Pb exposure. The profile and concentrations of porphyrins and biliverdin in feces were used as biomarkers of toxicological effects. Feces with Pb concentrations ≥ 34 μg/g d.w. showed higher Pb/Al ratios, together with lower (206)Pb/(207)Pb and (208)Pb/(207)Pb ratios, and higher (208)Pb/(206)Pb ratios, than feces with <34 μg/g d.w. Isotope signatures and Pb/Al ratios together indicated that Pb shot ingestion was the likely cause of the high Pb levels in some samples, whereas sediment ingestion was linked to lower/background levels. Coproporphyrin I and protoporphyrin IX were also higher in feces with Pb ≥ 34 μg/g d.w., indicating measurable disruption in heme synthesis. Noninvasive fecal sampling permits study of the degree and source of Pb exposure and physiological effects, with low-effort and minimal disturbance to waterbirds.     

New peat bog record of atmospheric lead pollution in Switzerland: Pb concentrations,enrichment factors,isotopic composition,and organolead species

A peat core collected at Etang de la Gruère, an ombrotrophic bog in the Jura Mountains of Switzerland, was analyzed for organolead species (DEL, TEL, DML, and TML) using GC-MIP AES, Pb isotopes using TIMS, and total Pb using XRF and age-dated using 210Pb. The earliest occurrence of quantifiable alkyllead is found at a depth of 24 cm, which is dated at AD 1946 +/- 3; this finding is consistent with the introduction of leaded gasoline in Switzerland in 1947. The maximum concentration of alkyllead (2.89 ng/g) is found at 5 cm, which is dated at AD 1988 +/- 2. This same sample yielded 206Pb/207Pb = 1.1254, which is the least radiogenic value in the entire 2K core and comparable to the isotopic composition of Pb in leaded gasoline. The highest concentrations of DML (906 ng/g) and DEL (1906 ng/g) also were found in this sample. Total alkyllead never accounts for more than 0.02% of total Pb in any given sample. The spatial and temporal variations in organolead species is matched by the changes in the isotopic composition of Pb over the same interval. Despite this, the decline in anthropogenic Pb pre-dates the maximum in total alkyllead and minimum 206Pb/207Pb, indicating that atmospheric Pb emissions had already begun their decline prior to the introduction of unleaded gasoline. In fact the decline in anthropogenic Pb was probably in response to the introduction of legislation, first in Germany and later in the European Union, establishing a maximum allowable concentration of Pb in gasoline.     

Pyrogenic remobilization of historic industrial lead depositions

Relatively high levels (4.3 to 51 μg/g) of labile lead (Pb) in ash from the 2009 Jesusita Fire in Santa Barbara County, California attest to the pyrogenic remobilization of historic industrial lead depositions in this relatively pristine area in Southern California, USA. The primarily industrial origin of that lead was evidenced by its poor correlations (simple linear regressions) with lithogenic aluminum (r = 0.18, p = 0.354, n = 30) and iron (r = 0.21, p = 0.270, n = 30) concentrations and by its associated enrichment factors (EFs): EF using aluminum as conservative element (f-Al) vs lead concentration [Pb] (r = 0.79, p < 0.001, n = 30), and EF using iron as conservative element (f-Fe) vs [Pb] (r = 0.83, p < 0.001, n = 30). The industrial origins of much of that lead were corroborated by its isotopic compositions ((206)Pb/(207)Pb and (208)Pb/(207)Pb), which fell between those of natural lead in the Santa Barbara Basin and previous leaded gasoline emissions in Southern California. This apparent pyrogenic remobilization of legacy lead pollution indicates that it-and other persistent pollutants-will increase with the projected increase in the frequency and intensity of forest fires in the Southwest U.S. and elsewhere as a consequence of climate change.     

Lead concentrations and isotopic ratios in the sediments of the Sea of Galilee

The isotopic composition and concentrations of Pb in the sediments of the Sea of Galilee (Lake Kinneret) were measured. The studied sediments have been deposited in the lake since the early 1900s (ca. 1920), hence Pb data record the transition from a period when the lake vicinity was sparsely populated to the present (approximately 100,000 people living in the area around the lake). In general, there is either a constant or a relatively slow increase in Pb concentrations from 40 cm depth (3.5-4.4 microg/g; ca. 1920) to 17 +/- 2 cm below the sediment-water interface (3.7-7.2 microg/g;), which was deposited in the mid-1960s. From 17 +/- 2 cm below the surface, there is a much faster increase up to 7 +/- 2 cm below the surface (from 6.5 to 11.5 microg/g; 1982-1983), and from 7 +/- 2 cm there is a gradual decrease in Pb concentrations toward the sediment-water interface. At station G, near the outlet of the Jordan River, Pb concentrations drop between 29 and 25 cm below the surface, probably reflecting changes in the particulate load of the Jordan River due to the drying out of the Hula Swamp in the early 1950s. 206Pb/207Pb values in all the stations record most of the shifts displayed by Pb concentrations in the sediment. The estimated value of total Pb deposited annually in the lake sediment in the early 1990s is very close to the value obtained from measurements of Pb fluxes to the lake from eolian and fluvial sources. On the basis of the linear relationship between 206Pb/207Pb (or 208Pb/207Pb) and 1/[Pb], we argue that two end-members contribute most of the Pb to the lake sediments. Sources of Pb to the lake include (i) the weathering of basalt from the eastern Galilee and the Golan Heights contributing 2.6 +/- 0.5 microg/g Pb to the sediment and (ii) anthropogenic Pb that is affecting both surface and deep (from 30 to 40 cm) lake sediments. At station S, a third source, Pb released from soils developed on carbonates, should be considered as well.     

Flux rates of atmospheric lead pollution within soils of a small catchment in northern Sweden and their implications for future stream water quality

It is not well-known how the accumulated pool of atmospheric lead pollution in the boreal forest soil will affect the groundwater and surface water chemistry in the future as this lead migrates through the soil profile. This study uses stable lead isotopes (206Pb/207Pb and 208Pb/ 207Pb ratios) to trace the transport of atmospheric lead pollution within the soil of a small catchment and predict future lead level changes in a stream draining the catchment. Low 206Pb/207Pb and 208Pb/207Pb ratios for the lead in the soil water (1.16 +/- 0.02; 2.43 +/- 0.03) and streamwater (1.18 +/- 0.03; 2.42 +/- 0.03) in comparison to that of the mineral soil (>1.4; >2.5) suggest that atmospheric pollution contributes by about 90% (65-100%) to the lead pool found in these matrixes. Calculated transport rates of atmospheric lead along a soil transect indicate that the mean residence time of lead in organic and mineral soil layers is at a centennial to millennial time scale. A maximum release of the present pool of lead pollution in the soil to the stream is predicted to occur within 200-800 years. Even though the uncertainty of the prediction is large, it emphasizes the magnitude of the time lag between the accumulation of atmospheric lead pollution in soils and the subsequent response in streamwater quality.     

Ammunition is the principal source of lead accumulated by California condors re-introduced to the wild

The endangered California Condor (Gymnogyps californianus) was reduced to a total population of 22 birds by the end of 1982. Their captive-bred descendants are now being released back into the wild in California, Arizona, and Baja California, where monitoring indicates they may accumulate lead to toxic levels. Fragments of ammunition in the carcasses of game animals such as deer, elk, and feral pigs not retrieved by hunters or in gut piles left in the field have been considered a plausible source of the lead, though little direct evidence is available to support this hypothesis. Here, we measured lead concentrations and isotope ratios in blood from 18 condors living in the wild in central California, in 8 pre-release birds, and in diet and ammunition samples to determine the importance of ammunition as a source of exposure. Blood lead levels in pre-release condors were low (average 27.7 ng/mL, SD 4.9 ng/ mL) and isotopically similar to dietary and background environmental lead in California. In contrast, blood lead levels in free-flying condors were substantially higher (average 246 ng/mL, SD 229 ng/mL) with lead isotopic compositions that approached or matched those of the lead ammunition. A two-endmember mixing model defined by the background 207Pb/206Pb ratio of representative condor diet samples (0.8346) and the upper 207Pb/206Pb ratio of the ammunition samples (0.8184) was able to account for the blood lead isotopic compositions in 20 out of the 26 live condors sampled in this study (i.e., 77%). Finally, lead in tissues and in a serially sampled growing feather recovered postmortem from a lead-poisoned condor in Arizona evidence acute exposure from an isotopically distinct lead source. Together, these data indicate that incidental ingestion of ammunition in carcasses of animals killed by hunters is the principal source of elevated lead exposure that threatens the recovery in the wild of this endangered species.     

Pyrogenic inputs of anthropogenic Pb and Hg to sediments of the Hood Canal, Washington, in the 20th century: source evidence from stable Pb isotopes and PAH signatures

Combustion-derived PAHs and stable Pb isotopic signatures ((206)Pb/(207)Pb) in sedimentary records assisted in reconstructing the sources of atmospheric inputs of anthropogenic Pb and Hg to the Hood Canal, Washington. The sediment-focusing corrected peak fluxes of total Pb and Hg (1960-70s) demonstrate that the watershed of Hood Canal has received greater atmospheric inputs of these metals than its mostly rural land use would predict. The tight relationships between the Pb, Hg, and organic markers in the cores indicate that these metals are derived from industrial combustion emissions. Multiple lines of evidence point to the Asarco smelter, located in the Main Basin of Puget Sound, as the major emission source of these metals to the watershed of the Hood Canal. The evidence includes (1) similar PAH isomer ratios in sediment cores from the two basins, (2) the correlations between Pb, Hg, and Cu in sediments and previously studied environmental samples including particulate matter emitted from the Asarco smelter's main stack at the peak of production, and (3) Pb isotope ratios. The natural rate of recovery in Hood Canal since the 1970s, back to preindustrial metal concentrations, was linear and contrasts with recovery rates reported for the Main Basin which slowed post late 1980s.     

Using stable and radioactive isotopes to trace atmospherically deposited Pb in montane forest soils

Atmospheric deposition of lead (Pb) throughout the 1900s resulted in elevated amounts of this toxic metal even in remote forest soils of the northeastern United States. Soils can act as a net sink for metals and thus minimize groundwater and surface water contamination. Recent studies utilizing forest floor temporal data and models of total Pb in precipitation, surface soils, and streams have estimated the time scale of Pb release from soils. However, due to the limited availability and spatial variability of forest floor survey data, other methods for quantifying anthropogenic Pb movement are needed. This study uses the isotopic composition (206Pb/207Pb) of soil Pb and measurements of 210Pb and 226Ra to directly trace the transit of atmospherically deposited Pb in the soil profile. We also report on the recovery of an enriched 207Pb dose applied in 1984 to the surface of a soil plot in the coniferous forest at Camels Hump in Vermont. The isotopic composition of soil Pb in low elevation deciduous forests suggests that approximately 65% of the original atmospheric Pb load has migrated from the forest floor to the upper 10 cm of the mineral soil. Higher elevation sites with coniferous vegetation have thicker forest floors, which have prevented significant amounts of Pb from entering the mineral soil. After 17 years, the soil organic horizon in the coniferous zone prevented any penetration of the applied Pb into the mineral soil. Using 210Pb budgets in different soil compartments, we determine forest floor response times for atmospherically delivered Pb to be approximately 60 years in the low elevation deciduous forest zone and 150 years for the high elevation spruce-fir forest zone at Camels Hump. According to its distribution in the soil profile, we conclude that a dispersed release of anthropogenic Pb to groundwater and surface water is possible this century. Our results also offer independent confirmation of Pb deposition models previously generated for the region.     

Natural fluctuations of mercury and lead in Greenland lake sediments

Given the current scenario of increasing global temperatures, it is valuable to assess the potential influence of changing climate on pollution distribution and deposition. In this study we use long-term sediment records from three lakes (spanning ca. 1000, 4800, and 8000 years, respectively) from the Greenland west coast to assess recent and long-term variations in mercury (Hg) and lead (Pb), including stable Pb isotopes (206Pb and 207Pb), in terms of pollution and climate influences. The temporal trends in sediment deposited from about the mid-19th century and forward are in general agreement with the history of industrial emissions at lower latitudes. Therefore, in recent sediment a possible influence from changing climate is difficult to assess. However, by using deeper sediment layers we show that changes in Greenland climate caused changes in the lake influx of material from regional aeolian activity, which resulted in large fluctuations in Hg and Pb concentrations and 206Pb/207Pb ratios. The aeolian material is primarily derived from glacio-fluvial material with low Hg and Pb concentrations and a different isotopic composition. For one of the lakes, the fluctuations in Hg concentrations (10 to 70 ng g(-1)) prior to the 19th century are equal to the anthropogenic increase in the uppermost layers, suggesting that when studying recent concentrations and time trends of pollution in relatively low-contaminated areas such as the Arctic, the early natural fluctuations must be considered.     

Origin of lead in eight Central European peat bogs determined from isotope ratios,strengths, and operation times of regional pollution sources

Lead originating from coal burning, gasoline burning, and ore smelting was identified in 210Pb-dated profiles through eight peat bogs distributed over an area of 60,000 km2. The Sphagnum-dominated bogs were located mainly in mountainous regions of the Czech Republic bordering with Germany, Austria, and Poland. Basal peat 14C-dated at 11,000 years BP had a relatively high 206Pb/207Pb ratio (1.193). Peat deposited around 1800 AD had a lower 206Pb/207Pb ratio of 1.168-1.178, indicating that environmental lead in Central Europe had been largely affected by human activity (smelting) even before the beginning of the Industrial Revolution. Five of the sites exhibited a nearly constant 206Pb/207Pb ratio (1.175) throughout the 19th century, resembling the "anthropogenic baseline" described in Northern Europe (1.17). At all sites, the 206Pb/207Pb ratio of peat decreased at least until 1980; at four sites, a reversal to more radiogenic values (higher 206Pb/207Pb), typical of easing pollution, was observed in the following decade (1980-1990). A time series of annual outputs for 14 different mining districts dispersing lead into the environment has been constructed for the past 200 years. The production of Ag-Pb, coal, and leaded gasoline peaked in 1900, 1980, and 1980, respectively. In contrast to other European countries, no peak in annual Pb accumulation rates was found in 1900, the year of maximum ore smelting. The highest annual Pb accumulation rates in peat were consistent with the highest Pb emission rates from coal-fired power plants and traffic (1980). Although maximum coal and gasoline production coincided in time, their isotope ratios were unique. The mean measured 206Pb/207Pb ratios of local coal, ores, and gasoline were 1.19, 1.16, and 1.11, respectively. A considerable proportion of coal emissions, relative to gasoline emisions, was responsible for the higher 206Pb/207Pb ratios in the recent atmosphere (1.15) compared to Western Europe (1.10). As in West European countries, the gasoline sold in the Czech Republic during the Communist era (1948-1989) contained an admixture of low-radiogenic Precambrian lead from Australia.