Stable lead isotope ratios in arctic aerosols: evidence for the origin of arctic air pollution (original) (raw)
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Stable lead isotope ratios in Alaskan arctic aerosols
Atmospheric Environment. Part A. General Topics
Aerosol samples collected at Barrow, Alaska, during February and March 1990 were found to have uniform stable lead isotope compositions. The mean 2°Spb/2°Tpb ratio was 2.423 + 0.009 and the mean 2°rpb/2°~Pb ratio was 1.161 + 0.014. The latter ratio is essentially the same as that obtained from an earlier study of aerosols at two Canadian stations in the High Arctic and is typical of, but not unique to, Eurasian sources of atmospheric lead. Further discriminating power was available in this study through the inclusion of 2oa pb/2OTpb ratios, which provided additional evidence that the former Soviet Union and eastern Europe are major contributors to atmospheric particulate lead in the Alaskan Arctic, accounting for around twothirds of the particulate lead measured at Barrow. The remaining third of the lead is attributed to west European sources. There was no evidence for a substantial North American component, other than local contamination.
Atmospheric Environment (1967)
Observations of lead 206/207 ratios and trace element concentrations in atmospheric aerosols at a rural location in Ontario, Canada confirm results of a previous study of urban aerosols that showed there are significant differences in the isotopic composition of lead from Canadian autos, Canadian smelters and eastern American sources. Lead measurements in fall 1984 and spring 1986 were apportioned to the respective sources as follows: for 1984 (55, 2, 43%) and for 1986 (69, 7, 24%). Lead isotopic and meteorological information point to In as the best elemental tracer of emissions from selected northern Canadian smelters.
Rendiconti Lincei, 2016
Size-segregated (PM 10) aerosol samples have been systematically collected at Ny-Å lesund (Svalbard Islands, Norwegian Arctic) during the spring and summer 2010 and analysed for elemental composition (major and trace elements, rare earth elements) and stable lead isotope ratios (206 Pb/ 207 Pb, 208 Pb/ 207 Pb). The analysis of the obtained dataset provided valuable information on the sources and long-range transport processes of atmospheric particulate and associated contaminants reaching the Arctic. In particular, a seasonal pattern was evident for Ba, Cd, Mn, Mo, Pb (p value B0.05), showing a higher input of elements related to anthropogenic emissions in spring compared to summer. Pb isotope ratios clearly showed that the geographic source of the anthropogenic input is subjected to a seasonal shift with an increased contribution of air masses coming from the north Eurasia during spring, and air masses coming from North America during summer. This finding was further corroborated by backtrajectory analysis. Finally, the analysis of the rare earth elements revealed an uniform pattern, without significant differences between the two seasons.
Isotopic composition of lead in moss and soil of the European Arctic
Geochimica et Cosmochimica Acta, 2004
Moss, O and C horizons of podzols, mainly forming complementary sample triplets, as well as filter residues of molten snow from northern Norway, northern Finland and NW Russia have been analyzed by TIMS for their Pb isotopic composition in order to study the impacts of local geogenic/anthropogenic sources and long range atmospheric transport on the Pb balance in the European Arctic. Samples were taken along two N-S transects covering an area of ϳ188.000 km 2 , including both pristine environments in the W and certain regions towards the E severely contaminated by heavy metal emissions originating from large nickel smelters and processing plants in NW Russia. The lead in moss and O horizon samples clearly reflects atmospheric deposition, as it displays overall uniform isotope ratios and is decoupled from the geogenic background, i.e. the underlying mineral soils in the C horizon. Moss and O horizon samples from the eastern N-S transect are isotopically indistinguishable from those taken along the western transect but their Pb concentrations tend to be ϳ2 times higher. This points to considerable contamination originating from the nearby Russian industrial and urban centers. However, isotopic signals of emissions from individual industrial point sources cannot be unambiguously identified because they lack characteristic isotope signatures. Pb derived from gasoline additives is swamped by Pb from other sources and can also be excluded as a major contributor to the environmental Pb in the European Arctic. Overall, the Pb isotopic signatures of moss and O horizon overlap values recorded in atmospheric lead all over central and southern Europe, more than 2000 km south of the study area. This may be taken as indicating continent-wide mixing of Pb derived from similar sources in the atmosphere or as reflecting economic globalization, or both. O horizon samples, which accumulate lead over 20-30 yr, conform to a distinct Pb isotope reference line in 207 Pb/ 206 Pb vs. 208 Pb/ 206 Pb space ("European Standard Pollution," ESP) defined by atmospheric Pb considered to be representative for the technical civilization in Europe. Conversely, the Arctic moss samples with a lifetime of Ͻ3 yr display a deviating linear trend reflecting a recent change of atmospheric input towards significantly more radiogenic Pb derived from Mississippi Valley-type ores in the U.S., fully compatible with signatures found in epiphytic lichens from Canada, but also in Pb from urban waste incinerators in central Europe. Considering the elevated Pb concentrations in moss collected along the eastern N-S transect, this congruence indicates that the Pb in moss of the European Arctic most probably originates from the nearby Russian centers of urbanization and not from transatlantic transport. We therefore suspect imported industrial goods and their subsequent attrition to be a more plausible explanation for the appearance of MVT lead in Europe.
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
Size-segregated (PM 10) aerosol samples have been systematically collected at Ny-A ˚ lesund (Svalbard Islands, Norwegian Arctic) during the spring and summer 2010 and analysed for elemental composition (major and trace elements, rare earth elements) and stable lead isotope ratios (206 Pb/ 207 Pb, 208 Pb/ 207 Pb). The analysis of the obtained dataset provided valuable information on the sources and long-range transport processes of atmospheric particulate and associated contaminants reaching the Arc-tic. In particular, a seasonal pattern was evident for Ba, Cd, Mn, Mo, Pb (p value B0.05), showing a higher input of elements related to anthropogenic emissions in spring compared to summer. Pb isotope ratios clearly showed that the geographic source of the anthropogenic input is subjected to a seasonal shift with an increased contribution of air masses coming from the north Eurasia during spring, and air masses coming from North America during summer. This finding was further corroborated by back-trajectory analysis. Finally, the analysis of the rare earth elements revealed an uniform pattern, without significant differences between the two seasons.
The Science of the Total …, 2002
To investigate the capability of the lead isotope signature technique to support a source apportionment study at a Continental scale, atmospheric particulate matter was collected at Cap Gris-Nez (Eastern Channel, northern France), over one year (1995–1996). Four days retrospective trajectories of air masses were available during each sampling experiment. Twenty-eight samples, for which the origin of aerosols was unambiguously determined, were selected for isotopic measurements. Considering the Enrichment Factors, EFCrust of lead and its size distribution, we show that lead is mostly from anthropogenic origin and mainly associated with [0.4<diameter<0.9 μm] particles. The extent to which various Continental sources influence the lead abundance in aerosols is exhibited by considering both the lead concentration and the origin of air masses. Lead concentration is higher by a factor of approximately seven, when air masses are derived from Continental Europe, by comparison with marine air masses. Taking into account these concentrations and the vertical movements of air masses, we compare the different isotopic compositions using a statistical non-parametric test (Kolmogorov–Smirnov). We produce evidence that, for most of the cases, air masses originating from Continental Europe exhibit a more radiogenic composition (1.134<206Pb/207Pb<1.172) than air masses coming from the United Kingdom (1.106<206Pb/207Pb<1.124). Generally, lead isotopic compositions in aerosols are clearly distinct from the gasoline signatures in European countries, strongly suggesting that automotive lead is no longer the major component of this metal in the air. Gasoline and industrial isotopic signatures could explain the origin of lead in our aerosol samples. A source apportionment based upon 206Pb/207Pb ratios, suggests that the difference between British (206Pb/207Pb=1.122±0.038) and Continental (206Pb/207Pb=1.155±0.022) signatures may be largely explained by differences in the petrol lead content of aerosols (23–62% in Great Britain vs. 10–36% in Continental Europe).
Potential Source Areas for Atmospheric Lead Reaching Ny-Ålesund from 2010 to 2018
Atmosphere, 2021
Lead content, enrichment factors, and isotopic composition (208Pb/206Pb and 207Pb/206Pb) measured in atmospheric particulate matter (PM10) samples collected for nine years at Ny-Alesund (Svalbard islands, Norwegian Arctic) during spring and summer are presented and discussed. The possible source areas (PSA) for particulate inferred from Pb isotope ratio values were compared to cluster analysis of back-trajectories. Results show that anthropogenic Pb dominates over natural crustal Pb, with a recurring higher influence in spring, compared to summer. Crustal Pb accounted for 5–16% of the measured Pb concentration. Anthropogenic Pb was affected by (i) a Central Asian PSA with Pb isotope signature compatible with ores smelted in the Rudny Altai region, at the Russian and Kazakhstan border, which accounted for 85% of the anthropogenic Pb concentration, and (ii) a weaker North American PSA, contributing for the remaining 15%. Central Asian PSA exerted an influence on 71–86% of spring sampl...