High-resolution sedimentary record of lead in the coastal mud of the East China Sea in the past one hundred and fifty years

In the East China Sea （ECS）, there are some mud areas, including the south coastal mud area, the north coastal mud area, and the mud area to the southwest of Cheju Island. X-ray fluorescence （XRF） techniques and Thermal Ionization Mass Spectrometry （TIMS） were used to study the high-resolution sedimentary record of Pb concentrations and Pb stable isotopic compositions in the past one hundred and fifty years in the coastal mud of the ECS. Pb concentrations of a ^210Pb dating S5 core in the study area have increased rapidly since 1980, and reached the maximal value with 65.08 μg/g in 2000, corresponding to the fast economic development of China since the implementation of the ＂Reform and Open Policy＂ in 1978; ^206Pb/^207Pb ratios generally had stabilized at 1.195 from 1860 to 1966, and decreased gradually from 1966 to 2000, indicating that the anthropogenic source Pb contribution to the ECS has increased gradually since 1966, especially since 1980. Pb concentrations decreased distinctly from 2000 to 2003 and ^206Pb/^207Pb ratios increased from 2001 to 2003, corresponding closely to the ban of lead gasoline from 2000 in China. From 1950 to 2003, there occurred four distinct decrease events of ^206Pb/^207Pb, possibly responding to the Changjiang River （Yangtze River） catastrophic floods in 1998, 1991, 1981 and 1954; from 1860 to 1966, there were two decrease periods of ^206Pb/^207Pb, which may respond to the catastrophic floods of Changjiang River in 1931 and 1935, and 1870. As a result of the erosion and drowning by the catastrophic floods, the anthropogenic lead accumulated in soil and water environments over a long period of time was brought into the Changjiang River, then part of them was finally transported into the ECS, which leads to changes in Pb stable isotopic composition.     

Study on the Sr,Nd,Pb and O Isotopes of Basic Dyke Swarms in the Wudang Block and Basic Volcanics of the Yaolinghe Group

The Sr,Nd and Pb isotopic characteristics of the Wudang basic dyke swarms and basic volcanics of the Yaolinghe Group show that they were derived from the same multi-component mixing source in the mantle.The Wudang basic dyke swarms have(^87Sr/^86Sr)i=0.6905-0.7061,εNd(t)=-1.9-5.0,△^208Pb/^204Pb=35.49-190.26,△^207Pb/^204Pb=Th/Ta and a wide range of La/Yb ratios;and the basic volcanics of the Yaolinghe Group have(^87Sr/^86Sr)i=0.6487-0.7075,εNd(t)=0.11-3.94，△^208Pb/^204Pb=-81.58-219.95,△^207Pb/^204Pb=4.44-16.68and higher Th/Ta and La/Yb ratios,indicating that their source is a mixture of DM and EMⅡ,and the basic volcanics of the Yaolinghe Group were contaminated by crust materials en rout to the surface.Based on the geochemical features of continental tholeiitic basalts and being products of differen tacies derived from the same source,it can be concluded that an important rifting event in the South Qinling basement block occurred during Neoproterozoic,followed by a setting of oceanic basic in the Early Paleozoic.     

Subduction—Modified Subcontinental Mantle in South China：Trace Element and Isotope Evidence in Basalts from Hainan Island

Cenozoic lavas from Hainan Island,South China,comprise quartz tholeiite,olivine tholeiite,alkali basalt,and basanite and form a continuous,tholeiite-dominated,compositional spectrum.Highly incompatible elements and their relationships with isotopes in these lavas are shown to be useful in evaluating mantle-source composition,whereas modeling suggests that ratios of elements with bulk partition coefficients significantly larger than those of Nb and Ta may be sensitive to partial melting.Th/Ta and La/Nb ratios of alkali basalts are lower than those of tholeiites,and they are all lower than those of the primitive mantle,These ratios correlate positively with ^207Pb/^204Pb and ^87Sr/^86Sr ratios.Such relationships can be explained by mixing of depleted and enriched source components.A depleted component is indicated by alkali basalt compositions and is similar to some depleted OIB (PREMA).The enriched component,similar to sediment compositions,is indicated by tholeiites with high LILE/HFSE,^207Pb/^204Pb,and ^87Sr/^86Sr ratios.In general,basalts from Hainan and the South China Basin(SCB)share common geochemical characters.e.g.high Rb/Sr,Th/Ta,^207Pb/^206Pb,and low Ba/Th ratios.Such a geochemical trend is comparable to that of EMII-type OIB and best explained as the result of subduction.Occurrence of these characteristics in both continental Hainan basalts and SCB seamout basalts indicates the presence of a South China geochemical domain that exists in the mantle region below the lithosphere.     

Heavy metal concentrations and Pb isotopic composition in urban and suburban aerosols of Hong Kong and Guangzhou, South China-Evidence of the long-range transport of air contaminants

Rapid urbanization and industrialization in South China has placed a great strain on the environment and human health. In the present study, the total suspended particulate matter （TSP） in the urban and suburban areas of Hong Kong and Guangzhou, the two largest urban centres in South China, was sampled from December 2003 to January 2005. The samples were analyzed for their concentrations of major elements （Al, Fe, Mg and Mn） and trace metals （Cd, Cr, Cu, Pb, V and Zn）, and for Pb isotopic composition. Elevated concentrations of metals, especially Cd, Pb, V and Zn, were observed in the urban and suburban areas of Guangzhou, showing significant atmospheric trace element pollution. Distinct seasonal patterns were observed in the heavy metal concentrations of aerosols in Hong Kong, with higher metal concentrations during the winter monsoon period, and lower concentrations during summer time. The seasonal variations in metal concentrations of the aerosols of Guangzhou were less distinct, suggesting the dominance of local sources of pollution around the city. The Pb isotopic composition in the aerosols of Hong Kong had higher ^206Pb/^207Pb and ^208Pb/^207Pb ratios in winter, showing the influence of Pb from the northern inland areas of China and the Pearl River Delta （PRD） region, and lower ^206Pb/^207Pb and ^208Pb/^207Pb ratios in summer, indicating the influence of Pb from the South Asian region and from marine sources.     

Geochemical Characteristics of Pb Isotope of High-Pressure Metamorphic Rocks and Foliated Granites from HP Unit of Tongbai-Dabie Orogenic Belt

Whole-rock Pb isotopic compositions of the high-pressure (HP) metamorphic rocks, consisting of two-mica albite gneisses and eclogites, and foliated granites from the HP metamorphic unit of the Tongbai-Dabie orogenic belt are firstly reported in this paper. The results show that the tip metamorphic rocks in different parts of this orogenic belt have similar Pb isotopic compositions. The twomica albite gneisses have ^206 pb/^204 Pb=17. 657 -18. 168, ^207pb/^204 Pb=15. 318-15. 573,^ 208Pb/^204ob=38.315-38. 990, and the eclogites have ^206Pb/^204 Pb=17. 599 -18. 310, ^207Pb/^204 Pb=15. 465 -15. 615,^208Pb/^204Pb=37. 968-39. 143. The HP metamorphic rocks are characterized by upper crustal Pb isotopic composition. Although the Pb isotopic composition of the HP metamorphic rocks partly overlaps that of the ultrahigh-pressure (UHP) metamorphic rocks, as a whole, the former is higher than the latter. The high radiogenic Pb isotopic composition for the HP metamorphic rocks confirms that the subducted Yangtze continental crust in the Tongbai-Dabie orogenic belt has the chemical structure of increasing radiogenic Pb isotopic composition from lower crust to upper crust. The foliated granites, intruded in the HP metamorphic rocks post the HP/UHP metamorphism, have ^206Pb/^204 Pb=17. 128- 17. 434,^207Pb/^204pb=15. 313-15. 422 and ^208Pb/^204Pb=37. 631-38. 122, which are obviously different from the Pb isotopic compositions of the HP metamorphic rocks but similar to those of the UHP metamorphic rocks and the foliated garnet-bearing granites in the UHP unit. This shows that the foliated granites from the HP and UHP units have common magma source. Combined with the foliated granites having the geochemical characteristics of A-type granites, it is suggested that the magma for the foliated granites in the UHP and HP unit would be derived from the partial melting of the retrometamorphosed UHP metamorphic rocks exhumed into middle to lower crust, and partial magmas were intruded into the HP unit.     

The Coupled Re—Os and Pt—Os Systematics：A Theoretical Consideration

The ^190Pt-^186Os system should be a unique tracer for mantle processes be-cause both Pt and Os are concentrated in the mantle.The ^190Pt-^186Os system will also be a good supplement to the ^187Re-^187Os system for dating and tracing mantle pro-cesses because the ^190Pt-^186Os system is not so easily contaminated by crustal materials as the ^187Re-^187Os system.In turn,the application of the ^187Re-^187Os system to Pt-enriched materials uncontaminated by crustal materials will indirectly refine the half life of ^190Pt.The ^190Pt is refined.In the coupled ^187Re-^187Os and ^190Pt-^186Os sys-tematics,an ^186Os*/^190Pt-^187Os*/^187Re Concordia diagram similar to the ^206Pb*/^238U-^208Pb*/^232Th Concordia can be constructed.In such a Concordia diagram,a date will be obtained so long as the ^190Pt-^186Os system remains closed even if the ^187Re-^187Os sys -tem is contaminated by crustal materials.In addition ,for the coupled ^190Pt-^186Os and ^187Re-^187Os systematics,the mantle processes and the interactions between the mantle and the crust will be described by two ratios:^186Os/^188Os and ^187Os/^188Os .The coupled ^187Re-^187Os and ^190Pt-^186Os systematics will be a powerful tool in the investigation of the geodynamic history of the Earth because the ^187Re-^187Os system is sensitive to the interactions between the mantle and the crust,while the ^190Pt-^186Os system is a good tracer for mantle processes.     

Lead Isotopic Composition and Lead Source in the Bainiuchang Ag-polymetallic Deposit, Yunnan Province, China

The Bainiuchang deposit in Yunnan Province, China, is located geographically between the Gejiu ore field and the Dulong ore field. In addition to the 〉7000 t Ag reserves, the deposit also boasts of large-scale Pb, Zn and Sn reserves with a lot of dispersed elements （In, Cd, Ge, Ga, etc.）. We have determined systematically the Pb isotope composition of the deposit. The Pb isotope ratios of the ores that are of sea-floor exhalative sedimentary origin in the northwest of the mining district, are 206pb/204pb = 17.758-18.537, 207pb/204pb = 15.175-15.862 and 206pb/204pb = 37.289-39.424, while those of ores that are of magmatic hydrothermal superimposition origin in the southeast of the mining district, are 206pb/204pb = 17.264-18.359, 207pb/204pb = 14.843-15.683 and 208pb/204pb = 36.481-38.838, respectively. In terms of the Pb isotope composition of feldspar in magmatic rocks or magmatic whole- rock samples from the mining district, we have determined the Pb isotope composition and acquired the Pb isotope ratios as： 206pb/204pb -- 18.224-18.700, 207pb/204pb -- 15.595-15.797 and 208pb/204pb -- 38.193-39.608. Then, in the light of the Pb isotope composition of metamorphic rock samples from the Proterozoic basement exposed in the Dulong ore field, we have determined the Pb isotope composition and obtained the isotope ratios as： 206pb/204pb -- 18.434-19.119, 207pb/204pb -- 15.644-15.693, and 208pb/204pb = 38.514-38.832. And the Pb isotope ratios of Cambrian sedimentary rocks, which are exposed in the Bainiuchang mining district, are 206pb/204pb = 18.307-19.206, 207pb/204pb = 15.622-15.809, and 208pb/204pb = 38.436-39.932. By comparing the two types of ores with respect to their Pb isotope compositions, it is indicated that lead in the Bainiuchang deposit was derived largely from the lower-crust granulite which is earlier than Neoproterozoic in age, but the Yanshanian magmatic hydrothermal fluids probably provided a part of ore-forming elements such as Sn for the ore blocks in the south of the mining district.     

Signatures of the source for the Emeishan flood basalts in the Ertan area： Pb isotope evidence

The Emeishan flood basalts can be divided into high-Ti (HT) basalt (Ti/Y>500) and low-Ti (LT) basalt (Ti/Y<500). Sr, Nd isotopic characteristics of the lavas indicate that the LT- and the HT-type magmas originated from distinct mantle sources and parental magmas. The LT-type magma was derived from a shallower lithospheric mantle, whereas the HT-type magma was derived from a deeper mantle source that may be possibly a mantle plume. However, few studies on the Emeishan flood basalts involved their Pb isotopes, especially the Ertan basalts. In this paper, the authors investigated basalt samples from the Ertan area in terms of Pb isotopes, in order to constrain the source of the Emeishan flood basalts. The ratios of 206Pb/204Pb (18.31–18.41), 207Pb/204Pb (15.55–15.56) and 208Pb/204Pb (38.81–38.94) are significantly higher than those of the depleted mantle, just lying between EM I and EM II. This indicates that the Emeishan HT basalts (in the Ertan area) are the result of mixing of EMI end-member and EMII end-member.     

Lead Isotopic Composition and Lead Source of the Huogeqi Cu-Pb-Zn Deposit, Inner Mongolia, China

The Huogeqi orefield located on the northern side of Mt. Langshan, Inner Mongolia occurs in the Middle Proterozoic Langshan Group metamorphic rocks, and the orebodies arc stratiform. In the past twenty years, many Chinese geologists have conducted researches on the Huogeqi Cu-Pb-Zn deposit, but there has been still a controversy on its origin. Some advocate that the deposit is of sedimentary-metamorphic rcworking origin, some hold that it is of sea-floor SEDEX origin, and others have a preference for magmatic superimposition origin. The crux of the controversy is that there is no common understanding about the source of ore-forming materials. In this paper, the Pb isotopic compositions of regional Achaean-Early Proterozoic basement rocks, various types of sedimentary- metamorphic rocks and volcanic rocks in the mining district, Late Proterozoic and Hercynian magmatic rocks arc introduced and compared with the orc-lead composition, so as to constrain the source of the ore lead. The result indicates that （1） sulfides in the ores have homogeneous Pb isotopic compositions, showing a narrow variation range. Their ^206pb/^204pb ratios arc within a range of 17.027- 17.317; ^207Pb/^204pb ratios, 15.451-15.786 and ^208Pb/^204pb ratios, 36.747-37.669; （2） the Pb isotopic compositions of the regional Achaean-Early Proterozoic basement rocks arc characteristic of the old Pb isotopic composition at the early-stage evolution of the Earth, which varies over a wider range, reflecting significant differences in Pb isotopic compositions of the ores. All this indicates that the source of ore lead has no bearing on the basement rocks; （3） the sedimentary-metamorphic rocks in the mining district arc characterized by highly variable and more radiogenic Pb isotopic compositions and their Pb isotopic ratios arc obviously higher than those of ores, demonstrating that ore lead did not result from metamorphic rcworking of these rocks; （4） Pb isotopic compositions of Late Proterozoic diorite-gabbro and Hercynian granite are higher than those of ores. Meanwhile, the Pb isotopic compositions of sulfides in the small-sized strata-penetrating mineralized veinlets formed at later stages arc completely consistent with that of sulfides in stratiform-banded ores, suggesting that these veiniets arc the product of autochthonous rcworking of the stratiform-banded ores during the period of metamorphism and the late magmatic superimposition-mineralization can be excluded; （5） amphibolite, whose protolith is basic volcanic rocks, has the same Pb isotopic compositions as ores, implying that ore lead was derived probably from basic volcanism. So, the source of ore-forming materials for the Huogeqi deposit is like that of the volcanic massive sulfide （VMS） deposits. However, the orebodies do not occur directly within the volcanic rocks, and instead they overlie the volcanic rocks, showing some differences from those typical VMS-type deposits.     

Application of Pb isotopic tracing technique to constraining the source of Pb in the West Lake Longjing tea

This paper dealt with the Pb contents and Pb isotopic composition of the West Lake Longjing tea. The results showed that in the tea leaves, from young leaf →old leaf →tea limb, the Pb contents tend to increase gradu-ally from 1.63 →4.84 →6.07×10-6, wich revealed that the Pb was accumulated gradually in the tea. After cleaned, the Pb contents of tea leaves were significantly reduced. This indicated that the deposits on the surface of tea leaves made a great contributuion to Pb contents. The survey results for soils in the relevant tea gardens showed that soil from the Longjing tea garden has higher Pb contents, with an average level of 49.6×10-6, two times those of common soils (24×10-6) in China. Results of the systematic analysis for tea, tea garden soil and the samples with the relevant background of the Pb isotopic composition displayed that the Pb isotopic ratio of tea is 206Pb/207Pb=1.164±0.005 (2σ). The ratio of 206Pb/207Pb for the soil gradually decreased from residue phase, soil dilute acid extract phase, and then to urban topsoil, i.e., 1.175 →1.171 →1.170. The 208Pb/(206Pb+207Pb) ratios also show a similar variation trend. 206Pb/207Pb ratios in the samples with the relevant background were: vehicle exhaust, 1.124; coal-combustion, 1.156; atmosphere, 1.168; and water, 1.166. Comparative studies have shown that Pb pollution is popular in the environ-mental media (soil, atmosphere, water) in Hangzhou. With the aggravation of Pb pollution, the Pb isotopic composi-tion gradually changed from the natural background (soil residues) to the direction of automobile exhaust. This phe-nomenon could illustrate that the pollution source was the vehicle exhaust, while the coal-combustion contributed little to environmental pollution in Hangzhou. The Pb of the Longjing tea came mostly from soluble phase Pb in the polluted soil. Moreover, secondary pollution was caused by vehicle exhaust.     

Measurement of SIMS Instrumental Mass Fractionation of Pb Isotopes During Zircon Dating

An igneous zircon reference material (OG1) was characterised for U-Pb isotopes by ID-TIMS, and utilised to evaluate SIMS (SHRIMP) instrumental mass fractionation (IMF) of radiogenic Pb isotopes (²⁰⁷Pb*/²⁰⁶Pb*). The TIMS ²⁰⁷Pb*/²⁰⁶Pb* reference value for OG1 was 0.29907 ± 0.00011 (95% confidence limit), 3465.4 ± 0.6 Ma. The high ²⁰⁷Pb* (∼ 30 μg g⁻¹), negligible common Pb, and isotopic homogeneity permitted precise (± 1–2‰) ²⁰⁷Pb*/²⁰⁶Pb* measurements within the analytical sessions. External reproducibility of mean ²⁰⁷Pb*/²⁰⁶Pb* ratios between sessions was demonstrated for one instrument, yielding a mean IMF of +0.87 ± 0.49‰. The mean ²⁰⁷Pb*/²⁰⁶Pb* ratios between instruments were dispersed beyond uncertainties, with session IMF values from +3.6 ± 1.7‰ to −2.4 ± 1.3‰, and a grand mean IMF value (twenty-six sessions) of +0.70 ± 0.52‰, indicating a tendency towards elevated ²⁰⁷Pb*/²⁰⁶Pb*. The specific causes of variability in IMF are unclear, but generally reflect subtle differences in analytical conditions. The common practice in SIMS of assuming that IMF for Pb⁺ is insignificant could result in systematic age biases and underestimated uncertainties, of critical importance for precise correlation of Precambrian events. Nevertheless, a zircon RM such as OG1 can be readily incorporated into routine dating to improve ²⁰⁷Pb*/²⁰⁶Pb* accuracy and external reproducibility.     

Dating of Columbite-tantalite and Monazite from Pegmatites of the Kawadgaon–Challanpara Area,Bastar Craton,Central India

The results of geochronological studies on columbite-tantalite and monazite from the rare metal pegmatites of the Kawadgaon–Challanpara area in Bastar craton, central India are presented. Columbite-tantalite yielded U-Pb concordia upper intercept age of 1978±16 Ma (MSWD = 0.18). Radiogenic ²⁰⁷Pb*/²⁰⁶Pb* (T_7/6) ages on 4 out of 5 columbite-tantalite vary in a narrow range of 1903 to 2077 Ma and are similar to U-Pb age, whereas, one sample shows younger ²⁰⁷Pb*/²⁰⁶Pb*(T_7/6) age of 1728 Ma. Younger Pb-Pb age of 1744 ± 250 Ma (MSWD = 150) has also been indicated by these columbite-tantalite samples. Four out of five monazite samples define Pb-Pb errorchron age of 2050±370 Ma (MSWD = 165) and radiogenic ²⁰⁷Pb*/²⁰⁶Pb* (T_7/6) ages on 3 out of 5 monazites show a narrow range of 1983 to 2083 Ma. Other two samples show younger ²⁰⁷Pb*/²⁰⁶Pb*(T_7/6) ages as 1254 Ma and 1592Ma. Both monazite and columbite-tantalite indicate disturbance in Pb and U isotopic systematics as revealed by high MSWD. However, selected samples from both monazite and columbite-tantalite indicate age of their formation as c. 2000 Ma. Younger ages, i.e., 1254 to 1744 Ma are indicative of later geological disturbances. Reported age of c. 2000 Ma is comparable to Rb-Sr date of pegmatitic muscovite (1850-2330 Ma) from this area and is younger to intrusive granites of c. 2500 Ma. By analogy, therefore, it may be inferred that the age of the rare element mineralization may be ~2000 Ma old, and linked with younger granitic activity that spanned over the period from 2300 to 2100 Ma in the Bastar craton.     

Precise geochronology of phoscorites and carbonatites:: The critical role of U-series disequilibrium in age interpretations

We present the results of a comparative study of several geochronometer minerals (baddeleyite, zircon, apatite, phlogopite and tetraferriphlogopite) and isotopic systems (U-Pb, Th-Pb and Rb-Sr) from phoscorites (magnetite-forsterite-apatite-calcite rocks) and carbonatites of the Kovdor ultramafic-alkaline-carbonatite massif, Kola Peninsula, Russia. Uranium, thorium and their decay products are extremely fractionated by minerals that crystallise from carbonatite and phoscorite magma. We obtain high-precision ages from different chronometers, compare their accuracy, and evaluate the role of geochronological pitfalls of initial radioactive disequilibrium, differential migration of radiogenic isotopes, and inaccurate decay constants.Apatite yielded concordant U-Th-Pb ages between 376 and 380 Ma. The accuracy of the apatite ²³⁸U-²⁰⁶Pb ages is, however, compromised by uncertainty in the amount of radiogenic ²⁰⁶Pb produced from initial excess ²³⁰Th. The ²³⁵U-²⁰⁷Pb ages are relatively imprecise due to large common Pb correction and the uncertainty in the initial Pb isotopic composition. The Th-Pb system yields a more precise age of 376.4 ± 0.6 Ma.Zircon from two carbonatite samples is characterised by moderate to low U contents, high Th contents, and very high Th/U ratios up to 9000. The ²⁰⁶Pb*/²³⁸U systems in the zircon are strongly affected by the presence of excess ²⁰⁶Pb*, produced by decay of initial ²³⁰Th. The ²⁰⁸Pb*/²³²Th ages of zircon from both carbonatite samples are uniform and yield a weighted average of 377.52 ± 0.94 Ma.Baddeleyite U-Pb analyses are 3 to 6% normally discordant and have variable ²⁰⁷Pb*/²⁰⁶Pb* apparent ages. Eleven alteration-free baddeleyite fractions from three samples with no evidence for Pb loss yield uniform ²⁰⁶Pb*/²³⁸U ages with a weighted average of 378.54±0.23 Ma (378.64 Ma after correction for initial ²³⁰Th deficiency), which we consider the best estimate for age of the phoscorite-carbonatite body of the Kovdor massif. The ²⁰⁶Pb*/²³⁸U ages of baddeleyite fractions from five other samples spread between 378.5 and 373 Ma, indicating a variable lead loss up to 1.5%. The anomalously old ²⁰⁷Pb/²³⁵U and ²⁰⁷Pb/²⁰⁶Pb ages are consistent with the presence of excess radiogenic ²⁰⁷Pb* in the baddeleyite. We interpret this as a result of preferential partitioning of ²³¹Pa to baddeleyite.Fifteen phlogopite and tetraferriphlogopite fractions from five carbonatite and phoscorite samples yielded precise Rb-Sr isochron age of 372.2 ± 1.5 Ma, which is 5 to 7 m.y. younger than our best estimate based on U-Th-Pb age values. This difference is unlikely to be a result of the disturbance or late closure of Rb-Sr system in phlogopite, but rather suggests that the accepted decay constant of ⁸⁷Rb is too high.Comparative study of multiple geochronometer minerals from the Kovdor massif has revealed an exceptional complexity of isotopic systems. Reliable ages can be understood through systematic analysis of possible sources of distortion. No single geochronometer is sufficiently reliable in these rocks. Th-Pb and Rb-Sr can be a very useful supplement to U-Pb geochronometry, but the routine use of these geochronometers together will require more precise and accurate determination of decay constants for ²³²Th and ⁸⁷Rb.     

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.     

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.     

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.     

Sources and chronology of atmospheric lead deposition to a Canadian Shield lake: Inferences from Pb isotopes and PAH profiles

The depth-distribution of lead and its stable isotope ratios were determined in a dated sediment core from a Canadian Shield lake receiving anthropogenic Pb inputs exclusively from atmospheric deposition. The results demonstrate that anthropogenic Pb deposited to the sediments of this lake since the preindustrial period can be modeled successfully using as little as two isotopically distinct Pb types. The first, whose flux was not detectable before 1850, reached a maximum value around 1950, and then decreased significantly thereafter; it was characterized by ²⁰⁶Pb/²⁰⁷Pb and ²⁰⁶Pb/²⁰⁸Pb ratios of 1.222 and 0.495, respectively, and was derived mainly from coal combustion. The second, whose flux was not detectable before 1880, increased sharply to exceed that of the Pb type derived from coal combustion around 1930, and reached a maximum in the mid 1970s; it is characterized by ²⁰⁶Pb/²⁰⁷Pb and ²⁰⁶Pb/²⁰⁸Pb ratios of 1.179 and 0.482, respectively, and was derived mainly from leaded gasoline combustion and industrial sources. The chronology of deposition of these two anthropogenic lead types agrees well with the historical records of fossil fuel uses in Canada and the USA, and also with the history of sediment-deposited polycyclic aromatic hydrocarbons (PAHs) originating from coal combustion. The inventory of Pb derived from coal combustion (0.09 μmol cm⁻²) is ∼30% of that derived mainly, but not exclusively, from leaded gasoline (0.31 μmol cm⁻²). Apportionment among source regions of lead deposited to the sediments during the period when leaded gasoline dominated Pb atmospheric emissions indicates that ∼50% of this lead originated in the USA.     

Determination of the extent of anthropogenic Pb migration through fractured sandstone using Pb isotope tracing

The extent of vertical migration of anthropogenic Pb beneath a medieval smelting site in Derbyshire, U.K. has been estimated using the determination of total Pb concentrations and ²⁰⁶Pb/²⁰⁷Pb isotope ratio from samples taken down 6 m of drill core. Preliminary studies of total Pb concentrations established that the surface slag derived from the smelting contained up to 16% Pb and that the normal background levels in uncontaminated sandstone were 10±2 ppm. Sample analyses beneath the site revealed elevated Pb concentrations in fracture infill clays (270 ppm Pb) and sandstone (76–83 ppm Pb). Both are well above the background Pb concentration.Lead isotope analysis of the slag wastes, the underlying contaminated sandstone and fracture infill has shown that all 3 contain very similar isotope ratios for ²⁰⁶Pb/²⁰⁷Pb (1.1802–1.1820). However, matched control sandstone samples show that the background ²⁰⁶Pb/²⁰⁷Pb isotope ratio (1.1670 ± 0.003) is distinctly different. This would indicate that both the sandstone and fracture infill underlying the historical smelting site contain a substantial proportion of Pb that has been derived from the overlying contamination.The application of total Pb concentrations along the core and isotope analysis suggest that anthropogenically derived Pb from the smelting site (that was operated between 665 and 445 a BP) has migrated to a depth of 4.50 m. Assuming a uniform migration rate and a mean time of migration of 555 a, then the mean migration rate is estimated to be 8 ± 2 mm/a.The proportion of natural versus anthropogenic Pb in the samples has been estimated from small variations in the ²⁰⁶Pb/²⁰⁷Pb isotope ratio. If the slag is considered to contain 100% anthropogenic Pb and the uncontaminated sandstone considered to contain 100% natural Pb, the linear interpolation can be applied between the 2 end members of the isotope ratio. The use of this approach to the ²⁰⁶Pb/²⁰⁷Pb ratio measurements has shown that 88% of the Pb in the contaminated sandstone (i.e. 69 ppm from a mean total Pb concentration of 78.5 ppm) has been derived from the anthropogenic Pb at the surface. For the fracture infill sample taken at a depth of 4.50 m, and with a total Pb concentration of 270 ppm, the % of Pb that has been derived from the slag wastes is approximately 98% (equivalent to 265 ppm Pb). The remaining Pb in both these samples (9.4 and 5 ppm, respectively) is deduced to have originated from the natural background concentration of Pb in the sandstone.The closeness of these estimates to the measured background concentration, suggests that a simple two-source model of Pb contamination is valid for this site.     

Lead isotopic systematics of major river sediments: a new estimate of the Pb isotopic composition of the Upper Continental Crust

The lead isotopic composition of river sediments is reported in the present work for the Earth's major river basins, from old cratonic to young orogenic areas and from subarctic to tropical climates. Sediment samples from these large river basins provide a useful tool to calculate the average upper crustal composition because they are large-scale integrated samples of the weathering products of the present-day Upper Continental Crust (UCC). Two different and complementary calculations were done to estimate the average lead isotopic composition of the UCC. The first, based on the flux weighted average of particulate lead delivered by the rivers, gave values of 19.07, 15.74 and 39.35 for ²⁰⁶Pb/²⁰⁴Pb, ²⁰⁷Pb/²⁰⁴Pb and ²⁰⁸Pb/²⁰⁴Pb ratios, respectively. To avoid over-estimating the contribution of orogenic areas, which produces a bias (because the flux of particulate lead depends strongly on the physical erosion rate), a second calculation was done by averaging with drainage areas of each river basin. This gave values of 18.93, 15.71 and 39.03 for ²⁰⁶Pb/²⁰⁴Pb, ²⁰⁷Pb/²⁰⁴Pb and ²⁰⁸Pb/²⁰⁴Pb ratios, respectively. These direct calculations of the lead isotopic composition of the UCC are similar and are in agreement with previous estimates made using an indirect approach.