杭州市土壤铅污染的铅同位素示踪研究

根据杭州市40个土壤全铅和38个可溶相铅的统计分析,土壤中全铅平均含量为49.6×10^-6,可溶相铅平均为21.4×10^-6,城区表土的全铅高达76.1×10^-6,显著高于全国土壤平均值。分析结果还显示,从农村→远郊→近郊→公路旁,土壤可溶相铅含量逐渐增加,且土壤的可溶相铅含量与深度具明显的负相关关系。表明杭州市土壤受到了不同程度的铅污染,污染程度由农村→远郊→近郊→公路旁→城区有明显的增高趋势。通过对茶园土壤中可溶相铅、残渣态铅及城区表土全铅的同位素组成对比分析发现,从土壤残渣态(代表土壤背景)→土壤可溶相→城区表层土壤全铅²⁰⁶Pb/²⁰⁷Pb比值有明显的降低。²⁰⁸Pb/(²⁰⁶Pb+²⁰⁷Pb)也有类似的变化趋势。将土壤与杭州市的汽车尾气、大气等环境样品进行对比发现,随着土壤受污染程度的增加,铅同位素组成逐渐向汽车尾气铅漂移,表明汽车尾气排放的铅为其主要污染源。     

Genesis of the South Zhuguang Uranium Ore Field,South China: Pb Isotopic Compositions and Mineralization Ages

U–Pb isotopic analyses indicate that ores from the South Zhuguang uranium ore field, south China, have high common (non‐radiogenic) Pb contents, with variable and relatively radiogenic initial Pb contents. The U–Pb isochron method was used to date these ores, with plots of ²⁰⁸Pb/²⁰⁴Pb and ²⁰⁷Pb/²⁰⁴Pb versus ²⁰⁶Pb/²⁰⁴Pb being used to identify sample suites with similar initial Pb isotopic ratios and to normalize variable initial Pb isotopic ratios. The resulting U–Pb isochrons indicate two substages of uranium mineralization at ~57 and 52 Ma, with a later hydrothermal reformation at ~49 Ma, which homogenized Pb isotopic compositions. Initial Pb isotopic systematics indicate that the ore‐forming fluid was characterized by high ²⁰⁶Pb/²⁰⁴Pb and ²⁰⁷Pb/²⁰⁴Pb ratios and low ²⁰⁸Pb/²⁰⁴Pb ratios, suggesting that the ore‐forming fluid was sourced from Cretaceous–Paleogene red‐bed basins, rather than from magma or the mantle, with consideration of mineralization ages.     

若尔盖高原土壤和近地表大气气溶胶铅同位素组成测试及示踪研究

若尔盖高原牧场处于中国偏远洁净高海拔地区,大气沉降是污染物主要来源途径之一。由于季风的影响,污染源的辨析较为困难。本文通过多点大气气溶胶不同季节同时采样方式,利用热电离固体同位素质谱仪可有效校正质谱分析中同位素分馏效应的优点,对若尔盖地区土壤和大气气溶胶的铅同位素比值进行精确分析,并结合季风特征对该地区污染物的来源进行解析。结果表明:土壤的208Pb/204Pb比值变化范围为38.79059±0.00194~38.94461±0.00135,206Pb/207Pb为1.18551±0.00002~1.19362±0.00002;大气气溶胶的208Pb/204Pb比值变化范围为37.49571±0.00117~38.48980±0.00105,206Pb/207Pb为1.12894±0.00001~1.16734±0.00001。该地区土壤铅同位素的特征是放射成因铅高,来自于自身天然存在的岩石矿物,与大气污染关系不大;大气气溶胶的铅同位素组成与土壤差异较大,显示为多元混合模式,受到了天然物质和人类活动来源的混合影响,机动车尾气及来自北部(兰州)和西北部(青海、新疆、哈萨克斯坦、俄罗斯)的大气远程运移是若尔盖大气气溶胶及污染物质的主要来源。     

Tracing diffuse anthropogenic Pb sources in rural soils by means of Pb isotope analysis

Knowledge of the cause and source of Pb pollution is important to abate environmental Pb pollution by taking source-related actions. Lead isotope analysis is a potentially powerful tool to identify anthropogenic Pb and its sources in the environment. Spatial information on the variation of anthropogenic Pb content and anthropogenic Pb sources in rural topsoils is remarkably limited. This study presents results of a survey of approximately 350 topsoil samples from rural locations covering the entire Netherlands, for which the bulk geochemical and Pb isotope compositions were determined. The specific aim of this study is to determine the anthropogenic Pb sources in the topsoils from rural areas in The Netherlands. The spatial distribution of anthropogenic Pb in soils in The Netherlands will be explained in terms of land use and pollution sources.Nearly all studied topsoils display Pb contents that exceed the amount expected based on the soil lithology. The range in Pb isotope ratios of the additional Pb fraction in rural Dutch topsoils is established at 1.056–1.199, 2.336–2.486 and 0.452–0.490 for ²⁰⁶Pb/²⁰⁷Pb, ²⁰⁷Pb/²⁰⁸Pb and ²⁰⁶Pb/²⁰⁸Pb, respectively. Five land use types are distinguished (forest, open nature, moor, arable land and grassland) with distinct isotopic compositions for added Pb. Additional Pb in soils of natural areas (forest, open nature and moor) has on average lower ²⁰⁶Pb/²⁰⁷Pb, ²⁰⁸Pb/²⁰⁷Pb and ²⁰⁶Pb/²⁰⁸Pb ratios than the agricultural soils (arable land and grassland). Additional Pb in both natural area soils and agricultural soils is interpreted to be of anthropogenic origin: most likely a mixture of coal/galena, incinerator ashes and gasoline Pb. The dominant sources of additional Pb in the topsoil of open nature areas are most likely incinerator ash and gasoline Pb. In contrast, the on average higher ²⁰⁶Pb/²⁰⁷Pb, ²⁰⁸Pb/²⁰⁷Pb and ²⁰⁶Pb/²⁰⁸Pb ratios of additional Pb in agricultural soils are most likely caused by the presence of animal manure and N–P fertilizers.Several areas are observed with notably high additional Pb contents (26–211 mg/kg on an organic matter-free basis) in the topsoil. The largest area is the Randstad area, which has the highest population and traffic density, and hosts a considerable fraction of the Dutch chemical industry. Two other areas with high additional Pb contents in the topsoil are located near the Dutch borders and are most likely influenced by German and Belgian chemical industries. The topsoils in the coastal dunes and southern, central and northern forests are characterized by relatively low additional Pb contents (<10 mg/kg on an organic matter-free basis). The population, traffic and chemical industry density is low in these areas and no fertilizers are applied.     

T-检验在杭州市不同环境介质中铅同位素组成及其来源判别中的应用

应用Microsoft Excel软件中"数据分析"工具之T-检验,对杭州地区不同环境介质的铅同位素组成(206Pb/207Pb比值)进行了均值相等假设检验。通过T-检验,揭示了杭州市哪些环境介质具有相似或不同的铅同位素组成。结果表明,汽车尾气铅具有独特的铅同位素组成而不同于其它环境介质;汽车尾气铅对环境的污染导致环境中铅同位素组成逐渐偏离原值,如城区表土污染最为严重,其206Pb/207Pb比值已与土壤的残渣显示有显著差异,西湖表层沉积淤泥也与深部沉积柱样品有明显的不同。大气和水与多个环境介质具有相似的铅同位素比值,说明大气与水在环境中能与多种环境介质进行同位素物质交换,对污染的扩散起了重要的作用;茶叶与大气有相似的铅同位素比值,说明大气(降尘)对茶叶铅有较大的贡献。而运河沉积物与城区表土铅同位素比值高度一致则说明运河沉积物可能就是来自城区流失的表土。通过实例,介绍了Excel中T-检验在地球化学研究中的应用。     

铅同位素示踪在大气降尘重金属污染来源解析中的应用

为了分析大气降尘中铅的污染来源,解析各污染源对大气降尘铅的相对贡献值,在厦门市不同功能区采集了29个大气降尘样品。用热电质谱仪测定了大气降尘的总铅同位素组成,用ICP-MS测定样品酸可溶相铅同位素组成。结果表明,厦门市大气降尘铅同位素²⁰⁶Pb/²⁰⁷Pb值变化较大,为1.111 9~1.173 8;酸可溶相铅²⁰⁶Pb/²⁰⁷Pb值与福建土壤残渣相²⁰⁶Pb/²⁰⁷Pb值相差较大,表明厦门市大气降尘受人类活动来源铅的影响较大;酸可溶相铅²⁰⁶Pb/²⁰⁷Pb值明显小于总量铅²⁰⁶Pb/²⁰⁷Pb值。铅同位素示踪表明,厦门市大气降尘铅主要来源是燃煤,其次是自然来源和汽车尾气。三元混合模型分析表明,燃煤、自然来源、汽车尾气对厦门市大气降尘总量铅的贡献率分别为48.57%、20.29%、31.14%。     

Tectonic Subdivision of Dabie Orogenic Belt,Central China：Evidence from Pb Isotope Geochemistry of Late Mesozoic Basalts

It has long been debated that the Dabie orogenic belt belongs to the North China or Yangtze craton. In recent years, eastern China has been suggested, based on the Pb isotopic compositions of Phanerozoic ore and Mesozoic granitoid K-feldspar (revealing the crust Pb) in combination with Meso-Cenozoic basalts (revealing the mantle Pb), being divided into the North China and Yangtze Pb isotopic provinces, where the crust and mantle of the Yangtze craton are characterized by more radiogenic Pb. In this sense, previous researchers suggested that the pro-EW-trending Dabie crogenic belt with less radiogenic Pb in the crust was part of the North China craton. In this paper, however, the Late Cretaceous basalts in the central and southern parts of the Dabie orogenic belt are characterized by some more radiogenic Pb (²⁰⁶Pb/²⁰⁴Pb=17.936−18.349,²⁰⁷Pb/²⁰⁴Pb=15.500−15.688,²⁰⁸Pb/²⁰⁴Pb=38.399−38.775) and a unique U-Th-Pb trace element system similar to those of the Yangtze craton, showing that the Mesozoic mantle is of the Yangtze type. In addition, the decoupled Pb isotopic compositions between crust and mantle were considerably derived from their rheological inhomogeneity, implying a complicated evolution of the Dabie orogenic belt. The study was funded by the National Natural Science Foundation of China (No. 49794043) and the Open Laboratory of Constitution, Interaction and Dynamics of the Crust-Mantle System, China.     

The biogeochemistry of atmospherically derived Pb in the boreal forest of Sweden

The use of stable Pb isotopes for tracing Pb contamination within the environment has strongly increased our understanding of the fate of airborne Pb contaminants within the boreal forest. This paper presents new stable Pb isotope (²⁰⁶Pb/²⁰⁷Pb ratio) measurements of solid soil samples, stream water (from a mire outlet and a stream draining a forest dominated catchment) and components of Picea abies (roots, needles and stemwood), and synthesizes some of the authors’ recent findings regarding the biogeochemistry of Pb within the boreal forest. The data clearly indicate that the biogeochemical cycling of Pb in the present-day boreal forest ecosystem is dominated by pollution Pb from atmospheric deposition. The ²⁰⁶Pb/²⁰⁷Pb ratios of the mor layer (O-horizon), forest plants and stream water (mainly between 1.14 and 1.20) are similar to atmospheric Pb pollution (1.14–1.19), while the local geogenic Pb of the mineral soil (C-horizon) has high ratios (>1.30). Roots and basal stemwood of the analyzed forest trees have higher ²⁰⁶Pb/²⁰⁷Pb ratios (1.15–1.30) than needles and apical stemwood (1.14–1.18), which indicate that the latter components are more dominated by pollution derived Pb. The low ²⁰⁶Pb/²⁰⁷Pb ratios of the mor layer suggest that the upward transport of Pb as a result of plant uptake is small (<0.04 mg m⁻² a⁻¹) in comparison to atmospheric inputs (∼0.5 mg m⁻² a⁻¹) and annual losses with percolating soil-water (∼2 mg m⁻² a⁻¹); consequently, the Pb levels in the mor layer are now decreasing while the pool of Pb in the mineral soil is increasing. Streams draining mires appear more strongly affected by pollution Pb than streams from forested catchments, as indicated by Pb concentrations about three times higher and lower ²⁰⁶Pb/²⁰⁷Pb ratios (1.16 ± 0.01 in comparison to 1.18 ± 0.02). To what extent stream water Pb levels will respond to the build-up of Pb in deeper mineral soil layers remains uncertain.     

Lead isotopes as tracers of anthropogenic pollution in urban topsoils of Mexico City

A survey was performed to trace the main source of anthropogenic Pb pollution in Mexico City through Pb isotopic signatures (²⁰⁸Pb/²⁰⁴Pb, ²⁰⁶Pb/²⁰⁴Pb, ²⁰⁶Pb/²⁰⁷Pb, and ²⁰⁸Pb/²⁰⁷Pb) from 103 urban topsoil (0–5 cm) samples. Those were collected in the metropolitan area of Mexico City and compared with isotopic compositions of leaded gasoline (LG), domestic Pb ores (DLO) and parent rock (PR). The isotope ratios (IRs) of Pb were determined by inductively coupled plasma quadrupole mass spectrometry (ICP-QMS) and total Pb concentration analyzed by wavelength dispersive X-ray fluorescence (WDXRF). The range of Pb concentrations levels in urban topsoil samples was 15–473 mg/kg. The IR values obtained for these samples were 37.965–39.718 (²⁰⁸Pb/²⁰⁴Pb), 18.375–19.204 (²⁰⁶Pb/²⁰⁴Pb), 1.177–1.218 (²⁰⁶Pb/²⁰⁷Pb) and 2.443–2.496 (²⁰⁸Pb/²⁰⁷Pb). Analyzed topsoil samples with low Pb content (<50 mg/kg) displayed high dispersion in ²⁰⁸Pb/²⁰⁴Pb values, which are determined by different natural sources. Samples with 51–200 mg/kg Pb content, shown low dispersion that revealed the mixing between the natural Pb and anthropogenic Pb. The assessment of the IR values shown that, as Pb concentration increases, a trend toward gasoline IR data has been observed. The results obtained by this research suggest that although the use of leaded petrol had been banned in Mexico since 1997, the Pb pollution in the urban topsoils due to the historical use of Pb in petrol is still significant.     

松树沟元古宙蛇绿岩Nd、Sr、Pb同位素地球化学特征

松树沟蛇绿岩中镁铁质岩的Sm-Nd全岩等时年龄为1030±46Ma,∈_Nd(t)=+5.7,模式年龄在1422-1271Ma之间,矿物的内部等时年龄为983±140Ma。全岩等时年龄为其形成上限,矿物内部等时年龄为其变质年龄,说明该蛇绿岩形成于中元古代中、晚期。镁铁质岩的∈_Nd(t)在+4.2-+6.9之间,是DMM与EMI两个地幔端元的混合产物;²⁰⁶Pb/²⁰⁴Pb在18.06-18.66之间,²⁰⁷Pb/²⁰⁴Pb和²⁰⁸Pb/²⁰⁴Pb值较高,分别在15.55-15.60和37.59-38.38之间,²⁰⁷Pb/²⁰⁴Pb和²⁰⁸Pb/²⁰⁴Pb对²⁰⁶Pb/²⁰⁴Pb的关系表明,岩浆源于具DUPAL异常的源区,(²⁰⁷Pb/²⁰⁴Pb)_i相对(²⁰⁸Pb/²⁰⁴Pb)_i更偏离NHRL可能是变质流体作用的反映。∈_Sr(t)值较高且变化大,可与蛇绿岩类比,⁸⁷Sr/⁸⁶Sr比值变化大,可能与海水蚀变作用有关。据此推测,松树沟蛇绿岩代表洋壳残片。     

Lead isotopic signatures of wine and vineyard soils—tracers of lead origin

The Pb contents and ²⁰⁶Pb/²⁰⁷Pb and ²⁰⁸Pb/²⁰⁶Pb isotopic ratios were studied in the soils and wines (2004 harvest) of three vineyard areas of the Czech Republic. The areas differ in their geological basements and anthropogenic loading. The isotopic compositions of wine in areas with intensive industry (Most, North Bohemia ²⁰⁶Pb/²⁰⁷Pb_wine = 1.178 ± 0.004) and the agricultural areas of Central Bohemia (Roudnice nad Labem ²⁰⁶Pb/²⁰⁷Pb_wine = 1.176 ± 0.007) are similar to the Pb isotopic composition of airborne particulate material typical of polluted and industrial environments (²⁰⁶Pb/²⁰⁷Pb = 1.17–1.19). The isotopic composition of wine from Prague (²⁰⁶Pb/²⁰⁷Pb_wine = 1.174 ± 0.003) is different from that of the soil, which was severely contaminated in the past by vehicular Pb (²⁰⁶Pb/²⁰⁷Pb_soil = 1.147–1.168). This fact shows that interception of airborne Pb by plants is greater than its uptake by the root system.     

西湖茶园茶叶铅污染铅同位素示踪

通过对西湖茶园的植物和土壤样品进行一系列的调查,以着力寻找茶叶的铅污染源。利用铅同位素技术对西湖茶园的土壤、茶叶和城区的燃煤、大气气溶胶、汽车尾气进行铅同位素示踪研究。研究表明,茶园土壤铅物质的可溶相具同源性和残查态偏于多源性。清洗后的茶叶铅含量显著降低,但其同位素组成不发生明显改变,显示出茶叶中的铅与叶面空气沉降物中的铅同源。不同介质铅同位素对比值平均值呈现表土、大气(气溶胶)、煤的w(²⁰⁶Pb)/w(²⁰⁷Pb)与茶叶趋于相近,汽油低之;表土、大气(气溶胶)、汽油的w(²⁰⁸Pb)/〔w(²⁰⁶Pb)+w(²⁰⁷Pb)〕与茶叶趋于相近,煤略高之。不同区域茶叶铅物质具同源性,与种植的农业地质背景无关。在煤燃烧、气化过程中,Pb进入大气,通过大气沉降或被茶树吸收或附着在茶叶叶面;汽车尾气的排放是茶树铅污染的重要原因之一。     

湘东南铜山岭铅锌多金属矿床成矿时代与成矿物质来源——Sm-Nd等时线年龄和Pb同位素证据

铜山岭铅锌多金属矿床位于扬子地块湘南-桂东北坳陷与华夏地块粤北坳陷的拼贴部位,是中国南岭多金属成矿区代表性矿床之一。为确定矿床成矿时代,挑选铜山岭铅锌多金属矿床中含矿矽卡岩的石榴子石进行Sm-Nd同位素定年,获得的等时线年龄为173±3Ma,指示成矿作用发生于燕山早期。对金属硫化物矿物进行了Pb同位素分析,其~(206)Pb/~(204)Pb、~(207)Pb/~(204)Pb、~(208)Pb/~(204)Pb平均值分别为18.602、15.701、38.729,表明成矿物质来源于相对富集铀铅、略微亏损钍铅的上地壳源区。从(~(207)Pb/~(204)Pb)i-(~(206)Pb/~(204)Pb)i铅同位素演化模式图可知,寄主花岗闪长岩是铜山岭铅锌多金属矿床的重要物质来源,且成矿物质中可能含有寄存在花岗闪长岩中的地幔组分。     

Albany K-Feldspar: A New Pb Isotope Reference Material

Lead isotopes are a powerful and versatile tool to elucidate fundamental geological problems related to the formation and evolution of continental crust. K-feldspar is a popular target for Pb isotope measurement as it is prevalent in many rock types and tends to capture the initial Pb isotope composition of its parental magma. We present data for a new Pb isotope reference material: Albany K-feldspar; as well as updated data for Shap K-feldspar. Results of Pb double-spike TIMS for Albany K-feldspar are ²⁰⁶Pb/²⁰⁴Pb = 16.7872 ± 0.0062, ²⁰⁷Pb/²⁰⁴Pb = 15.5640 ± 0.0056, and ²⁰⁸Pb/²⁰⁴Pb = 36.6600 ± 0.0168 (2s). TIMS measurement results for Shap K-feldspar indicate two isotopically distinct Pb populations. LA-MC-ICP-MS, with a spatial resolution as high as 15 μm, indicates a homogeneous Pb isotopic composition in Albany K-feldspar. In accord with previous studies, our results show that scatter in the measured Pb isotope ratios, related to the low natural isotopic abundance of ²⁰⁴Pb, along with the effect of isobaric ²⁰⁴Hg-²⁰⁴Pb interference, increases at lower count rates. However, the mean Pb isotope ratios measured via LA-MC-ICP-MS using a range of spot sizes are in excellent agreement with TIMS results thus highlighting the feasibility of Pb isotope determination via LA-MC-ICP-MS to access geological information preserved in small crystals, including mineral inclusions.     

U–Pb zircon geochronology of ferrodiorites and quartz diorites from the Turkel Anorthosite Complex: a Neoarchaean convergent margin in eastern India

The Turkel anorthosite Complex (TAC) in the Eastern Ghats Belt in India is composed of anorthosites and leuconorites at the centre and ferrodiorites and quartz diorites at the periphery. Here we report whole‐rock geochemistry, and zircon U–Pb data and REE geochemistry from a co‐spatial ferrodiorite and two quartz diorites from the TAC. The diorites have low abundance of High Field Strength Elements (HFSE) and REE, exhibit a flat chondrite‐normalized pattern with slight LREE enrichment and negligible or no Eu anomaly. Our results show weighted mean ²⁰⁷Pb/²⁰⁶Pb ages of 2433 ± 33 Ma for the ferrodiorite. Two quartz diorite samples from Turkel yield mean²⁰⁷Pb/²⁰⁶Pb ages of 2419 ± 32 Ma and 2505 ± 31 Ma. The zircons from all the analysed samples show high REE contents, prominent HREE enrichment and a conspicuous positive Eu anomaly, suggesting a common magmatic source. The prominent Neoarchaean to early Palaeoproterozoic magmatic ages from the anorthosite complex deviate from the late Neoproterozoic ages reported from other anorthosite suites in the Eastern Ghats Belt, and suggest an active convergent margin along SE India during Archaean–Proterozoic transition. Copyright © 2014 John Wiley & Sons, Ltd.     

RMJG Rutile: A New Natural Reference Material for Microbeam U‐Pb Dating and Hf Isotopic Analysis

Matrix‐matched reference materials are necessary for accurate microbeam U‐Pb dating and Hf isotopic determination. This study introduces the RMJG rutile as a new potential reference material, which was separated from Palaeoproterozoic pelitic granulites collected in Hebei Province, China. LA‐ICP‐MS measurements indicate the RMJG rutile has extremely low Th (< 0.003 ± 0.01 µg g^?1) and common Pb contents, but high Hf (102 ± 34 µg g^?1), U (61 ± 11 µg g^?1), and radiogenic Pb (~ 20 µg g^?1) contents. Moreover, the rutile yields relatively constant U‐Pb ages and Hf isotopic data. The LA‐ICP‐MS analyses suggest that this rutile has a concordant U‐Pb age with a statistical mean ²⁰⁶Pb/²³⁸U and ²⁰⁷Pb/²³⁵U ages of 1749.9 ± 32.1 Ma and 1750.0 ± 26.4 Ma, respectively (2s), which are statistically indistinguishable from its ID‐TIMS ages (1750.6 ± 8.4 and 1750.1 ± 4.7 Ma). Precise determination of the ¹⁷⁶Hf/¹⁷⁷Hf ratio by MC‐ICP‐MS in solution mode (0.281652 ± 0.000006) is in good agreement with the statistical mean of the LA‐MC‐ICP‐MS measurements (0.28166 ± 0.00018). Therefore, the limited variations of RMJG U‐Pb age and Hf isotopic composition together with its extremely low common Pb and high Hf, U and Pb contents make it an ideal calibration and monitor reference material for LA‐ICP‐MS measurements.     

A Correction Approach to the Common Pb Contribution to ^207Pb／^206Pb Ratios Obtained by the Zircon Evaporation Technique

An approach is recommended for the correction of common Pb contribution to ^207Pb/^206Pb ages obtained by the zircon evaporation technique.A comparison with that by Cocherie et al.(1992)shows that two approaches yield similar results in the ^207Pb*/^206Pb* ratios.But when using the new approach,only two errors of the measured ^204Pb/^206Pb and ^207Pb/^207Pb ratios are introduced to the calculated ^207Pb^*/^206Pb^* ratios.     

Isotopic provenancing of Pb in Mitrovica,northern Kosovo: Source identification of chronic Pb enrichment in soils,house dust and scalp hair

Mitrovica, northern Kosovo, is the site of some of the highest Pb concentrations reported in human populations; exemplified by Pb concentrations in scalp hair of up to 130 μg g⁻¹ and widely-publicized of Pb-related ill-health and mortality amongst internally displaced populations. High human Pb burdens are accompanied by elevated concentrations of potentially harmful elements (PHEs) in soils and house dust within the city, which has a long history of mining and metallurgy. In this study enrichment-levels for PHEs in soils are quantified and compared to environmental quality guidelines and a statistically-derived estimation of background concentration. In addition, Pb isotopes (²⁰⁷Pb/²⁰⁶Pb, ²⁰⁸Pb/²⁰⁶Pb) are used to characterise the isotopic signatures of potential point sources of Pb and a mixing model employed to quantify the contribution of sources to Pb present in soils, house dust, and the scalp hair of children and young people. Pb isotopic evidence suggests that Pb in surface soils and house-dust is predominantly sourced from historical deposition of Pb-containing aerosols from metal smelting, with lower contributions from wind-blown dispersal of metalliferous waste. Pb present in scalp hair is interpreted as the result of non-occupational exposure and the ingestion and/or inhalation of Pb-enriched surface soil and house dust. This study represents one of the very few instances where this type of geochemical tracing technique has been successfully applied to definitively identify the source of Pb present within biological samples. The results of this study are of particular relevance to environmental management and highlight the human health risk posed by the legacy of now inactive mining and metallurgy in addition to the challenge posed in mitigating the risk posed by diffuse soil pollution.     

Lead Isotopic Composition in Biogenic Certified Reference Materials Determined by Different ICP‐based Mass Spectrometric Techniques

This work presents data for the radiogenic Pb isotopic ratios (²⁰⁶Pb/²⁰⁷Pb and ²⁰⁸Pb/²⁰⁶Pb) in nine biogenic certified reference materials (NIST SRM 1515, 1566b, 1570a, 1573a, 1575a; BCR 100, BCR 101, BCR 670 and IAEA 359), which are suitable for analytical quality control in environmental research. The results were obtained using three different types of ICP‐based mass spectrometer (quadrupole‐based/magnetic sector field single‐collector ICP‐MS instruments and a multi‐collector ICP‐MS) and applying different mass bias correction procedures (calibrator‐sample bracketing and external Tl normalisation) with and without Pb separation from the matrix using ion exchange chromatography. In the majority of the samples, the measurements from all three of the ICP‐MS instruments were in agreement within ± 0.1%, despite the lower analytical precision of the single‐collector ICP‐MS instruments. We demonstrate that the presence of the sample matrix did not significantly influence the Pb isotopic ratios measured by magnetic sector field ICP‐MS, whereas the use of the two different mass bias corrections resulted in a systematic difference of 0.09% for the ²⁰⁸Pb/²⁰⁶Pb ratio.     

The biosphere: A homogeniser of Pb-isotope signals

Rock, soil, and plant (terrestrial moss, European mountain ash leaves, mountain birch leaves, bark and wood, and spruce needles and wood) samples, collected at 3 km intervals along a 120 km long transect (40 sites) cutting the city of Oslo, Norway, were analysed for their Pb concentration and Pb-isotope ratios. A general decrease in ²⁰⁶Pb/²⁰⁷Pb, ²⁰⁸Pb/²⁰⁷Pb and ²⁰⁶Pb/²⁰⁸Pb ratios, with a characteristic low variability in all plant materials and the plant-derived O-horizon of soil profiles, compared to rocks and mineral soils, is observed along the transect. It is demonstrated that minerogenic and biogenic sample materials belong to two different spheres, the lithosphere and biosphere, and that geochemical processes determining their chemical and isotopic compositions differ widely. Background variation for both sample materials needs to be established and documented at the continental and global scale before the anthropogenic influence on the geochemistry of the earth’s surface can be reliably estimated.