B.J.H. van Os

Trace element concentrations and stable lead isotopes in soils as tracers of lead pollution in Graft-De Rijp, the Netherlands

Abstract Graft-De Rijp is a former village of whalers, situated twenty-five kilometres north of Amsterdam, the Netherlands. Since the foundation of De Rijp in 1612 a mixture of sludge, manure and town refuse (containing Pb-based household artefacts and Pb-based building materials) was used to raise and fertilise the land. Gasworks, coal storehouses, printing works and tanneries were started in the industrial area (after 1860). Surface soils in the “old” town centre of De Rijp are highly contaminated with Pb and, to a lesser extent, with Zn, Cu and As. Stable Pb isotopes combined with statistical analysis of the chemical dataset provided a tool whereby the sources of contaminant Pb, and related heavy metals were identified. Three major sources of Pb contamination could be distinguished: (1) remnants of the “old” town (building materials such as Pb sheets, glazed roof tiles and paint), (2) coal ashes and (3) alkyl-leaded petrol. In addition, high Zn, Cu and As are strongly related to Pb pollution, which is predominantly found in the topsoil (0–0.5 m) of the “old” town centre of Graft-De Rijp.

Lichens (Parmelia sulcata) time response model to environmental elemental availability

Parmelia sulcata transplants, collected in a non-polluted area, were exposed to new atmospheric conditions at six stations, of which five were located near power plants and one at an unpolluted area. Data were collected for a 1-year period, on rainfall, airborne particulates, elemental deposition and on lichen elemental composition. The study was carried out to quantify the relationships between elemental availability and elemental accumulation in lichens. A mathematical model was developed, involving a simple representation of the lichen, and a memory loss function which describes the time relations for the lichens progressive representation of its new ambient conditions. The collected data set was used to test the model. The results indicate that the environmental data on Na, Al and Pb could be reproduced and predicted by the model, including the variability patterns. Half-memory times were calculated for Na, Al and Pb as 200, 500 and 600 days, respectively, based on using all station data. However, further improvements are still needed, including the clarification of differences in model outcomes between stations. Copyright (C) 1998 Elsevier Science B.V.

The lead (Pb) isotope signature, behaviour and fate of traffic-related lead pollution in roadside soils in The Netherlands

In this study the origin, behaviour and fate of anthropogenic Pb in sandy roadside soils were assessed by measuring soil characteristics, Pb isotope composition and content. In 1991 and 2003 samples were taken at different depth intervals at approximately 8 and 75 m from two highways in The Netherlands. The Pb isotope composition of the litter layer ((206)Pb/(207)Pb=1.12-1.14) differs from the deeper soil samples ((206)Pb/(207)Pb=1.20-1.21). Based on a mixing model it is concluded that the samples contain two Pb sources: natural Pb and anthropogenic Pb, the latter mainly derived from gasoline. (206)Pb/(207)Pb ratios demonstrate that the roadside soils were polluted to a depth of ~15 cm. Within this depth interval, anthropogenic Pb content is associated with organic matter. Although Pb pollution only reached a depth of ~15 cm, this does not mean that the topsoils retain all anthropogenic Pb. Due to the low pH and negligible binding capacity of soils at depths >15 cm, anthropogenic Pb migrated towards groundwater after reaching depths of >15 cm. The Pb isotope composition of the groundwater ((206)Pb/(207)Pb=1.135-1.185) establishes that groundwater is polluted with anthropogenic Pb. The contribution of anthropogenic Pb to the groundwater varies between ~30 and 100%. Based on the difference in soil Pb content and Pb isotope compositions over a period of 12 years, downward Pb migration is calculated to vary from 72 ± 95 to 324 ± 279 mg m(-2)y(-1). Assuming that the downward Pb flux is constant over time, it is calculated that 35-90% of the atmospherically delivered Pb has migrated to the groundwater.

Volcanogenic pollution by acid water discharges along Ciwidey River, West Java (Indonesia)

Abstract Active and recently extinct volcanoes surrounding the catchment area of the upper Citarum River (West Java) are the source areas of surface waters with high concentrations of natural contaminants. Ciwidey River, one of its tributaries, originates on the flanks of Patuha, a Quaternary volcano which contains an acid (pH

Calibration of lichen transplants considering faint memory effects

Biomonitoring, among other purposes, can be used as a tool to study the dispersion of trace elements through the atmosphere and back to the earths surface again. In this sense it has been used for more than 20 years now. Yet, the calibration of biomonitors elemental contents against other atmospheric element dispersion variables like deposition or airborne concentration is still an open subject. The knowledge of a calibration nevertheless represents a qualitative improvement upon the use of biomonitors. Biomonitors elemental contents are usually assumed to depend in a linear way on the average values of atmospheric element dispersion variables, thus a linear regression is assumed to provide a good calibration. In this work: the element dispersion variables like deposition or airborne concentration will be referred in general as availability variables due to reasons that will be clarified; an uptake experiment using transplants of lichen Parmelia sulcata carried out in Portugal during a 2-year period (1994/1996) is described; and new concepts and calibration methods are presented. Lichen and aerosol samples were analysed by nuclear analytical techniques PIXE and INAA, and total deposition dry residue samples were analysed by ICP-MS. A database of roughly 70,000 values was thus created and biomonitor calibration carried out considering that biomonitors are not mechanical instruments but that they rather describe their exposure with a non-perfect memory. Data shows that surveying lichens four times within 1 year, with a period of 3 months in between sampling campaigns, allows the recovery of availability mean, maxima and standard deviation for many elements.

Reconstruction of historical atmospheric Pb using Dutch urban lake sediments: A Pb isotope study

Lake sediments provide a record of atmospheric Pb deposition and changes in Pb isotope composition. To our knowledge, such an approach has not previously been performed in The Netherlands or linked to national air monitoring data. Results are presented for Pb content and isotope composition of (137)Cs dated lake sediments from 2 Dutch urban lakes. Between 1942 and 2002A.D. anthropogenic atmospheric Pb deposition rates in the two lakes varied from 12±2 to 69±16μgcm(-2)year(-1). The rise and fall of leaded gasoline is clearly reflected in the reconstructed atmospheric Pb deposition rates. After the ban on leaded gasoline, late 1970s/early 1980s, atmospheric Pb deposition rates decreased rapidly in the two urban lakes and the relative contributions of other anthropogenic Pb sources - incinerator ash (industrial Pb) and coal/galena - increased sharply. Atmospheric Pb deposition rates inferred from the lake record a clear relationship with nearby measured annual mean air Pb concentrations. Based on this relationship it was estimated that air Pb concentrations between 1942 and 2002A.D. varied between 5 and 293ng/m(3).

Effectiveness of different pre-treatments in recovering pre-burial isotopic ratios of charred plants

RATIONALE Isotopic analysis of archaeological charred plant remains offers useful archaeological information. However, adequate sample pre-treatment protocols may be necessary to provide a contamination-free isotopic signal while limiting sample loss and achieving a high throughput. Under these constraints, research was undertaken to compare the performance of different pre-treatment protocols. METHODS Charred archaeological plant material was selected for isotopic analysis (δ13 C and δ15 N values) by isotope ratio mass spectrometry from a variety of plant species, time periods and soil conditions. Preservation conditions and the effectiveness of cleaning protocols were assessed through Fourier transform infrared spectroscopy and X-ray fluorescence (XRF) spectrometry. An acid-base-acid protocol, successfully employed in radiocarbon dating, was used to define a contamination-free isotopic reference. Acid-base-acid isotopic measurements were compared with those obtained from untreated material and an acid-only protocol. RESULTS The isotopic signals of untreated material and the acid-only protocol typically did not differ more than 1‰ from those of the acid-base-acid reference. There were no significant isotopic offsets between acid-base-acid and acid-only or untreated samples. Sample losses in the acid-base-acid protocol were on average 50 ± 17% (maximum = 98.4%). Elemental XRF measurements showed promising results in the detection of more contaminated samples albeit with a high rate of false positives. CONCLUSIONS For the large range of preservation conditions described in the study, untreated charred plant samples, water cleaned of sediments, provide reliable stable isotope ratios of carbon and nitrogen. The use of pre-treatments may be necessary under different preservation conditions or more conservative measurement uncertainties should be reported.

Production of 210Pb from a Slochteren Sandstone gas reservoir

Abstract Recently, precipitates of metallic Pb and galena in gas production facilities have been reported to contain 210 Pb. In the North Sea area, U-bearing Kupferschiefer or Carboniferous coal measures have been suggested as a possible source of 210 Pb. Through coproduction of formation water with natural gas, 210 Pb may enter production facilities together with non-radioactive Pb, and precipitate as metallic Pb or galena. In this study, bituminous sandstones with up to 2.8 wt% organic C from a 210 Pb producing Permian, Slochteren Formation gas reservoir have been found to contain up to 330 ppm U. The sandstones show a complex diagenetic history, during which migrating oil was trapped in secondary pores. Continuing enlargement of pore space and the wetting characteristics of the reservoir fluids lead to a preferred distribution of oil rims around quartz grains, creating fluid-filled voids between the grains. Syngenetic precipitation of finely grained U oxide occurred along the bitumen–fluid boundaries. U-Pb chemical age dating of U oxide grains provides an age of 246 Ma for the influx of the oil, and the close association of abundant anhydrite with the bitumen impregnations points to a Zechstein source for both bitumen and U. One of the bituminous sandstones shows a marked depletion of 210 Pb with respect to 238 U and 226 Ra, probably caused by the production of natural gas from the reservoir. Production started at the end of the 1960s and induced fluid flow throughout the reservoir. This enabled transport of 222 Rn and its decay product 210 Pb away from the U oxide grains. The observed U concentrations and permeabilities make the bituminous sandstones in this reservoir probably a more important source of 210 Pb than the overlying Kupferschiefer or underlying Carboniferous coal measures.