Lead concentrations and isotope ratios in speleothems as proxies for atmospheric metal pollution since the industrial revolution (original) (raw)
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Chemical Geology, 2015
We studied an aragonitic section of ca. 6 cm length of stalagmite HBSH-1 from the Hüttenbläserschachthöhle, western Germany. 230 Th/U-dating revealed that this section grew between~210 and~190 ka, with a relatively uniform growth rate of 3.1 μm a −1 . For the first time, we determined Pb isotope ratios ( 207 Pb/ 206 Pb and 208 Pb/ 206 Pb) in a stalagmite by laser ablation (LA)-ICP-MS. In addition, we analyzed various trace element (Mg, Al, Si, P, Mn, Sr, Pb and Th) concentrations.
A synthesis of lead isotopes in two millennia of European air
Earth and Planetary Science Letters, 1999
Four airborne particulate records from ombrotrophic peat bogs in southern Norway, extending back 300 years, have been measured for chronology, lead concentration, and lead isotope composition. Since southern Norway receives an airborne lead signal that accumulates emissions from the European continent, the trend in the four bog records can be used to correlate previously reported measurements from France, Switzerland, England, and Greenland that cover different ranges of time. When these are compiled, the integrated European record that emerges spans the last 2300 years of human influence on lead in the air over Europe and suggests human control of lead in airborne particulates over the entire period. From 366 BC through the first half of the 20th century, lead isotopic compositions in European air have fallen within the range of compositions in European ore bodies. Since 1950, isotopic compositions have been beyond the range in those ore body compositions and have fallen within the array of lead isotope compositions typical of gasoline from western industrial nations (a mixing line between US and Australian lead in gasoline). The overlap between the European record and the range in modern European air suggests an average isotopic composition of 206 Pb= 207 Pb ca. 1.13 and of 208P b= 207 Pb ca. 2.41 in air over Europe during the last 20 years.
Environmental Science & Technology, 2003
Lead originating from coal burning, gasoline burning, and ore smelting was identified in 210 Pb-dated profiles through eight peat bogs distributed over an area of 60 000 km 2. The Sphagnum-dominated bogs were located mainly in mountainous regions of the Czech Republic bordering with Germany, Austria, and Poland. Basal peat 14 C-dated at 11 000 years BP had a relatively high 206 Pb/ 207 Pb ratio (1.193). Peat deposited around 1800 AD had a lower 206 Pb/ 207 Pb 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 206 Pb/ 207 Pb ratio (1.175) throughout the 19th century, resembling the "anthropogenic baseline" described in Northern Europe (1.17). At all sites, the 206 Pb/ 207 Pb ratio of peat decreased at least until 1980; at four sites, a reversal to more radiogenic values (higher 206 Pb/ 207 Pb), 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 206 Pb/ 207 Pb 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 206 Pb/ 207 Pb 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.
Atmospheric Environment, 2016
During three winter seasons (2009-2011), Pb concentrations were measured in precipitation at 10 high-elevation sites in the Czech Republic, close to the borders with Austria, Germany, Poland, and Slovakia. Soluble and insoluble Pb forms were quantified in snow (vertical deposition), and rime (horizontal deposition). The objective was to compare Pb input fluxes into ecosystems via vertical and horizontal deposition, and to identify the residual Pb pollution sources in an era of rapidly decreasing industrial pollution. Lead soluble in diluted HNO 3 made up 96 % of total Pb deposition, with the remaining 4 % Pb bound mainly in silicates. Three times higher concentrations of soluble Pb in rime than in snow, and 2.5 times higher concentrations of insoluble Pb in rime than in snow were associated with slightly different Pb isotope ratios. On average, the 206 Pb/ 207 Pb ratios in rime were higher than those in snow. Higher mean 206 Pb/ 207 Pb ratios of insoluble Pb (1.175) than in soluble Pb (1.165) may indicate an increasing role of geogenic Pb in recent atmospheric deposition. A distinct reversal to more radiogenic 206 Pb/ 207 Pb ratios in snow and rime in 2010, compared to literature data from rain-fed Sphagnum peatlands (1800-2000 A.D.), documented a recent decrease in anthropogenic Pb in the atmosphere of Central Europe. Since the early 1980s, Pb concentrations in snow decreased 18 times in the rural south of the Czech Republic, but only twice in the industrial north of the Czech Republic. Isotope signatures indicated that Pb in today's atmospheric deposition is mainly derived from Mesozoic ores mined/processed in Poland and coal combustion in the Czech Republic and Poland. 4 America in that Pb emissions resulting from coal burning exceeded those from traffic (Vile et al., 2000, Novak et al., 2003, Farmer et al., 2016). The former East Germany was the largest, and the Czech Republic the third largest, soft coal producer in the world. The use of alkyl-lead in petrol was banned at the end of 1996 in Germany, 2000 in the Czech Republic, and 2003 in Poland. We hypothesized that, with easing pollution, Pb is well mixed before being deposited in rural locations. This hypothesis can be tested by a comparison of Pb isotope signatures of individual pollution sources with isotope signatures of Pb deposited in the ecosystems. Knowledge of Pb isotope composition of bedrock is needed to distinguish between geogenic and anthropogenic
Two peat cores from two bogs were used to reconstruct high–resolution changes in atmospheric Pb accumulation rate (Pb AR) in Belgium during the Roman period. The two records were compared to assess the reliability of peat cores as archives of atmospheric Pb deposition and to established histories of atmospheric emissions from anthropogenic sources. To address these issues we analyze Pb concentration and isotopes, using ICP-MS, LA-ICP-MS and MC-ICP-MS in two peat sections, spanning 1000 yr each. Lead concentrations in the two cores range from 0.1 to 60 μg g−1, with the maxima between 15 and 60 μg g−1. The average natural background of Pb AR was 0.005± 0.002 mg m-2 yr-1 and the maximum ranges from 0.7 to 1.2 mg m-2 yr-1 between 50 BC and AD 215. The highest Pb AR exceed the pre-Roman period values by a factor of 25-30. Pb isotopic composition indicates that mining and metallurgical activities were the predominant sources of pollution during the Roman per...
Journal of Environmental Monitoring, 2004
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 (w3000 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 y 1.17-1.19; 206 Pb/ 204 Pb y 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 y 1.13-1.16; 206 Pb/ 204 Pb y 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 y35 to v20 mg cm 22 yr 21). In the late 1980s, environmental policies made the Lake Anterne flux drop to pre-1900 values (v10 mg cm 22 yr 21) while Lake Le Bourget is always submitted to an important flux (y25 mg cm 22 yr 21). The good match of our distant records, together and with a previously established series in an ice core from Mont Blanc, 1 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. 1 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.
Isotopic evidence of pollutant lead sources in Northwestern France
Atmospheric …, 1999
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.