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1.
The Lynch’s Crater peat deposit in NE-Australia is a sensitive environmental archive located in the tropical Southern Hemisphere. This unique deposit illustrates that local and regional changes had a profound effect on the local Australian ecosystem over the past 55 kyr. To obtain a proxy of past climate changes, trace and major element geochemistry analyses were applied to a 13 m peat core from the crater. Principle component analysis (PCA) was used to identify the main factors that control elemental distribution in the peat and to add interpretative strength to the geochemical behavior of selected major and trace elements. For example, Sc, Al, Cu, and Pb were found to be related to increased erosion of the basin soils, and from this, several periods of significant flux from atmospheric input and/or terrigenous run-off were identified. Geochemically mobile elements during rock weathering and pedogenesis, such as Mg, Ca, and Sr helped to identify the peat ombrotrophic-minerotrophic boundary at ∼1.5 m depth and offered important information about fluxes of these nutrients to the mire and their dynamics within the deposit. Arsenic and V comparisons between the peat record (high concentrations in some peat sections) and in local basin rocks (very low concentrations), suggested the presence of a long range, atmospheric dust source early in the formation of the mire. The Lynch’s Crater peat record presents a continuous record of environmental change in tropical Australia and contributes new understanding to geochemical processes in peatlands.  相似文献   

2.
Lead (Pb) isotopic compositions and concentrations, and barium (Ba) and indium (In) concentrations have been determined at monthly resolution in five Law Dome (coastal Eastern Antarctica) ice core sections dated from ∼1757 AD to ∼1898 AD. ‘Natural’ background Pb concentrations in ∼1757 AD average ∼0.2 pg g−1 and can be attributed to mineral dust and volcanic emissions, with 206Pb/207Pb ratios reaching up to 1.266 ± 0.002. From ∼1887 AD to ∼1898 AD, Pb concentrations reached ∼5 pg g−1 and 206Pb/207Pb ratios decreased to 1.058 ± 0.001 as a result of additional inputs of Pb from anthropogenic sources. Seasonal variability in the late 1880s has been investigated by decoupling volcanic Pb from the total measured Pb concentrations, revealing spring and autumn maxima, and consistent winter minima, in anthropogenic Pb and mineral dust (Ba) concentrations. We link this variability to the annual cycle in the position and strength of the Antarctic Circumpolar Trough and, the Southern Ocean westerly winds to the north of the trough region. During the autumn and spring seasons, these systems increase in strength, transporting more impurity laden air from the Southern Hemisphere continental regions to Eastern Antarctica and Law Dome. As this Pb is isotopically identical to that emitted from south-eastern Australia (Broken Hill, Port Pirie) this implies a relatively direct air trajectory pathway from southern Australia to Law Dome (Eastern Antarctica).  相似文献   

3.
Climate change especially moisture condition in the northeastern Qinghai-Tibetan in China are mainly controlled by the strength and variability of Asian winter and summer monsoon. In this paper, we presented the climate record and related winter and summer monsoonal history in Gonghe Basin, northeastern Qinghai-Tibetan Plateau, based on the geochemical indicators (geochemical elements content, i.e., Fe2O3, CaO, Zr and Sr content, and geochemical parameters, i.e., the chemical index of alteration (CIA), Zr/Rb, Rb/Sr, CaO/MgO, SiO2/TiO2 and SiO2/(Al2O3 + Fe2O3) ratio) of the peat deposits and 14C and OSL technologies. The regional temperature and humidity gradually increased in 10.0–8.5 cal ka BP, accompanied by enhanced summer monsoonal strength and decreased winter monsoonal strength. But climate became cold and dry between 8.5 cal ka BP and 7.6 cal ka BP owing to the stronger winter monsoon. During the 7.6–3.8 cal ka BP, stronger summer monsoon and weaker winter monsoon led to an optimal warm and humid condition, although it had several cold phases. From 3.8 cal ka BP to 0.5 cal ka BP, the regional climate tended to be cold and dry, with increasing winter monsoonal strength and decreasing summer monsoonal strength. Thereafter, the relatively warm and humid climate appeared again, due to the stronger summer monsoon. That is to say, the regional climate conditions are mainly related to the winter and summer monsoonal changes. These changes are consistent with palaeoclimatic records (monsoonal model) from the region influenced by the Asian monsoon in eastern China. In addition, nine cold events were recorded: 8.5–7.8 cal ka BP, 6.1–5.6 cal ka BP, 5.2–4.8 cal ka BP, 4.7–4.3 cal ka BP, 4.1–4.0 cal ka BP, 3.8–3.4 cal ka BP, 3.0–2.3 cal ka BP, 1.4–1.3 cal ka BP, and 1.0–0.5 cal ka BP, which are coincident with cold fluctuations in the high and low latitudes of the Northern Hemisphere on a millennial scale, as recorded by lakes, peat sediments, and ice cores in the Qinghai-Tibetan Plateau. In conclusion, Holocene millennial-scale climatic changes in Gonghe Basin were controlled by the dual function of Asian monsoonal changes and global cold fluctuations.  相似文献   

4.
The Asian Monsoon forms an important part of the earth’s climate system, yet our understanding of the past interactions between its different sub-systems, the East Asian and Indian monsoons, and between monsoonal winds and other prevailing wind currents such as the Westerly jet, is limited, particularly in central Asia. This in turn affects our ability to develop climate models capable of accurately predicting future changes in atmospheric circulation patterns and monsoon intensities in Asia. Provenance studies of mineral dust deposited in terrestrial settings such as peat bogs can address this problem directly, by offering the possibility to examine past deposition rates and wind direction, and hence reconstruct past atmospheric circulation patterns. However, such studies are challenged by several issues, most importantly the identification of proxies that unambiguously distinguish between the different potential dust sources and that are independent of particle size. In addition, a single analytical method that is suitable for sample preparation of both dust source (i.e. desert sand, soil) and receptor (i.e. dust archive such as peat or soil profiles) material is desirable in order to minimize error propagation derived from the experimental and analytical work. Here, an improved geochemical framework of provenance tracers to study atmospheric circulation patterns and palaeomonsoon variability in central Asia is provided, by combining for the first time mineralogical as well as major and trace elemental (Sc, Y, Th and the rare earth elements) information on Chinese (central Chinese loess plateau, northern Qaidam basin and Taklamakan, Badain Juran and Tengger deserts), Indian (Thar desert) and Tibetan (eastern Qinghai-Tibetan Plateau) dust sources.Quartz, feldspars and clay minerals are the major constituents of all studied sources, with highly variable calcite contents reflected in the CaO concentrations. Chinese and Tibetan dust sources are enriched in middle REE relative to the upper continental crust and average shale but the Thar desert has a REE signature distinctly different from all other dust sources. There are significant differences in major, trace and REE compositions between the coarse and fine fractions of the surface sands, with the finest <4 μm fraction enriched in Al2O3, Fe2O3, MnO, MgO and K2O and the <32 μm fractions in Sc, Y, Th and the REE relative to the coarse fractions. The <4 μm fraction best represents the bulk REE geochemistry of the samples. The provenance tracers Y/∑REE, La/Er, La/Gd, Gd/Er, La/Yb, Y/Tb, Y/La, Y/Nd and to a certain extent the europium anomaly Eu/Eu (all REE normalized to post-Archean Australian shale, PAAS) are particle size-independent tracers, of which combinations of Y/∑REE, La/Yb, Y/Tb, Y/La and Eu/Eu can be used to distinguish the Thar desert, the Chinese deserts, the Chinese loess plateau and the Tibetan soils. Their independence upon grain size means that these tracers can be applied to the long-range provenance tracing of Asian dust even when only bulk samples are available in the source region. Combinations of La/Th, Y/Tb, Y/∑REE, Sc/La and Y/Er distinguish the Tibetan soils from the Chinese loess plateau and the Chinese deserts. La/Th and notably Th/∑REE isolate the signature of the Badain Juran desert and the combination of Sc/La and Y/Er that of the Taklamakan desert. The similarity in all trace and REE-based provenance tracers between the northern Qaidam basin and Tengger desert suggests that these two deposits may have a common aeolian source.  相似文献   

5.
Biogeochemical processes in a forested tropical peat deposit and its record of past atmospheric dust deposition were assessed using the vertical distribution of lithophilic and plant essential elements in a dated core profile from Borneo, SE Asia. Peat formation started ∼22,120 14C yr before present (BP), and Ca/Mg mass ratios of the solid peat and very low ash contents indicate a strongly ombrotrophic character throughout the deposit, implying that most of the inorganic fraction has been supplied exclusively by atmospheric inputs. Concentration profiles of Mn, Sr, and Ca suggest a very minor influence of chemical diagenesis in the underlying sediments. Silicon, Ca, Mg, P, S, and K show a strong and extended zone of enrichment in the top 200 cm of the profile, indicating that biological accumulation mechanisms are much more extensive than in temperate peat bogs.In the lower core sections, where the element distribution is dominated solely by past atmospheric deposition, average Al/Ti ratios are similar to the upper continental crust (UCC), whereas Fe is slightly enriched and Si is strongly depleted: this condition favors highly weathered tropical soil dust as the main inorganic mineral source. Significant correlation of Al, Fe, Si, S, Ca, and Ti with the lithophilic elements Y and Zr suggests that the distribution of these elements is controlled by sources of atmospheric mineral dust. The Ca/Mg, Ca/K, and Mg/K ratios of the collected rainwater samples are similar to the global average of continental rainwater and suggest a continental character for the site. This is supported by the similarity of the average concentration of Br, Mg, Ca, and S to that in temperate continental and maritime bogs in Switzerland and Scotland.The concentration profiles of Si, Fe, Al, and Ti show distinct peaks within the profile, implying enhanced dust deposition, reduced rates of peat accumulation, or possibly both owing to climatic changes during the Holocene. Enhanced dust deposition between ∼10,830 and 9060 14C yr BP is tentatively interpreted as a Younger Dryas-like event with dust fluxes of ∼10.8 mg/m2/yr. The variations in Al/Ti and Fe/Ti profiles suggest that mineral dust sources have been changing constantly during the Holocene, with local sources being dominant between ∼7820 and 9500 14C yr BP and long-range transport (derived most likely from China) being important during the late Pleistocene and early Holocene and from ∼7820 14C yr BP to the present.  相似文献   

6.
Trace element and isotopic compositions of carbonate from ore bodies, country rock which hosts the ore bodies (H8 dolomite), a carbonatite dyke exposed in Dulahala near Bayan Obo, and rare earth element (REE)-rich dolomite in Bayan Obo have been determined to understand the genesis of the Bayan Obo Fe-Nb-REE ore deposit, the world’s largest resource of REE. The REE and trace element distribution patterns of samples from the REE-rich carbonatite dykes are identical to those of mineralized carbonate rocks, indicating a genetic linkage between the REE-rich carbonatite and mineralization in this region. By contrast, carbon and oxygen isotopes in the mineralized carbonate varied significantly, δ13C = −7.98‰ to −1.12‰, δ18O = 8.60-25.69‰, which are distinctively different from those in mantle-derived carbonatite. Abnormal isotopic fractionations between dolomite and calcite suggest that these two minerals are in disequilibrium in the carbonatite dyke, ore bodies, and H8 marble from Bayan Obo. This isotopic characteristic is also found in mineralized sedimentary marine micrite from Heinaobao, ∼25 km southeast of the Bayan Obo Fe-Nb-REE ore deposit. These facts imply that the carbonate minerals in the Bayan Obo deposit have resulted from sedimentary carbonate rocks being metasomatised by mantle-derived fluids, likely derived from a REE-enriched carbonatitic magma. The initial Nd isotope values of ore bodies and carbonatite dykes are identical, indicating that ore bodies, carbonatite dykes and veins may have a similar REE source.  相似文献   

7.
Lynch's Crater preserves a continuous, high‐resolution record of environmental changes in north Queensland. This record suggests a marked increase in burning that appears to be independent of any known major climatic boundaries. This increase is accompanied, or closely followed, by the virtually complete replacement of rainforest by sclerophyll vegetation. The absence of any major climatic shift associated with this increase in fire frequency therefore has been interpreted as a result of early human impact in the area. The age for this increase in burning, on the basis of conventional radiocarbon dating, was previously thought to be approximately 38 000 14C yr BP, supporting the traditional model for human arrival in Australia at 40 000 14C yr BP Here we have applied a more rigorous pre‐treatment and graphitisation procedure for radiocarbon dating samples from the Lynch's Crater sequence. These new dates suggest that the increase in fire frequency occurred at 45 000 14C yr BP, supporting the alternative view that human occupation of Australia occurred by at least 45 000–55 000 cal. yr BP. Copyright © 2001 John Wiley & Sons, Ltd.  相似文献   

8.
Southern Ocean aerosols were collected at the Cape Grim Baseline Air Pollution Station from onshore air under baseline conditions between February 1999 and April 2000. Thermal ionization techniques (TIMS) and isotope dilution mass spectrometry (IDMS) were used to measure the isotopic composition and concentration of lead in the air giving concentrations as low as 0.6 ± 0.1 pg · m−3. Air collected under baseline conditions for 12 months (May 1999-April 2000) yielded an overall lead concentration of 11.0 ± 0.2 pg · m−3 and isotopic composition of 206Pb/207Pb = 1.154, 208Pb/207Pb = 2.387 and 206Pb/204Pb = 17.93. The range in isotopic ratios was consistent with the mixing of lead from major population centers in the Southern Hemisphere in the mid to high latitudes, except for the presence of highly radiogenic lead in some samples. Contributions from radiogenic lead of up to ∼0.8% were observed. Three periods with the highest percentage contribution of radiogenic lead (>0.5%) were investigated in more detail, and 4-d back-trajectories and radon concentrations were used to help identify the sources. The sources are probably associated with the mining and processing of uranium rich ores in southern Africa and possibly South Australia.  相似文献   

9.
Primary massive sulfide gossans (MSG) in the Bathurst Mining Camp (BMC), New Brunswick, Canada, are characterized by relative enrichment of Au, Sb, and As, formation of jarosite group minerals (jarosite, plumbojarosite, and argentojarosite) and little or no fractionation in the rare earth elements (REE), including preservation of large positive Eu anomalies (average [Eu/Eu*]NASC = 4.14 in MSG; 6.61 in massive sulfide mineralization; 0.60 in host rocks). The chemical and mineralogical characteristics of MSG (e.g., Halfmile Lake deposit) imply low pH (<3) and relatively oxidizing conditions during gossan formation; oxidation of a volcanogenic massive sulfide body (comprising pyrite, pyrrhotite, sphalerite, galena, and chalcopyrite) with a falling water table. The lack of light REE or heavy REE fractionation and preservation of positive Eu anomalies characteristic of the original (465 Ma) hydrothermal fluid is consistent with relatively large water-rock ratios during massive sulfide mineralization oxidation, and removal of the REE predominantly as sulfate complexes (LnSO4+, Ln(SO4)2). Low pH groundwaters recovered from past producing mines in the BMC display REE patterns reflecting those inferred to have occurred during gossan formation. Gossan at the Restigouche deposit, in contrast to the Halfmile Lake deposit, displays mineralogical and chemical evidence for having been chemically reworked since primary gossan formation. Evidence for chemical reworking includes loss of primary massive sulfide mineralization textures, replacement of plumbojarosite with anglesite, almost complete removal of jarosite minerals, loss of Au, Sb, and As and apparent preferential removal of Eu, resulting in loss of positive Eu anomalies for most samples (average [Eu/Eu*]NASC = 1.21 in the gossan, with many displaying strong negative anomalies; 3.65 in massive sulfide mineralization; 0.54 in host rocks). Based on geochemical modeling, conditions inferred for the chemical reworking of the Restigouche deposit include near neutral conditions and either relatively oxidizing conditions with Eu2+ hosted in a preferentially weathered mineral host (possibly through substitution for Pb in plumbojarosite and beudantite) or cycling between reduced and oxidized conditions during gossan reworking.  相似文献   

10.
Peatland of the eastern Qinghai–Tibetan Plateau lies at the convergence of the East Asian and Indian monsoon systems in eastern Asia. To understand the evolution of this peatland and its potential to provide new insights into the Holocene evolution of the East Asian monsoon a 6 m peat core was collected from the undisturbed central part of a peat deposit near Hongyuan. The age-depth profile was determined using 16 14C-AMS age dates, the peat analysed for a range of environmental variables including carbon, nitrogen and hydrogen concentration, bulk density, δ13C and the associated spring water analysed for hydrogen and oxygen isotopes. The age-depth profile of the recovered peat sequence covers the period from 9.6 to 0.3 kyr BP and is linear indicating that the conditions governing productivity and decay varied little over the Holocene. Using changes in carbon density, organic carbon content and its δ13C, cold dry periods of permafrost characterised by low density and impeded surface drainage were identified. The low δ18O and δD values of the spring water emanating around the peat deposit, down to ?13.8 and ?102‰ (VSMOW), respectively, with an inverse relationship between electrical conductivity and isotopic composition indicate precipitation under colder and drier conditions relative to the present day. In view of the current annual mean air temperature of 1 °C this suggests conditions in the past have been conducive to permafrost. Inferred periods of permafrost correspond to independently recognised cold periods in other Holocene records from across China at 8.6, 8.2–7.8, 5.6–4.2, 3.1 and 1.8–1.5 kyr BP. The transition to a cold dry climate appears to be more rapid than the subsequent recovery and cold dry periods at Hongyuan are of longer duration than equivalent cold dry periods over central and eastern China. Light–dark banding peat on a scale of 15–30 years from 9.6 to 5.5 kyr BP may indicate a strong influence of decadal oscillations possibly the Pacific Decadal Oscillation and a potential link between near simultaneous climatic changes in the northwest Pacific, ENSO, movement of the Intertropical Convergence Zone and the East Asian Monsoon.  相似文献   

11.
Analysis of a well-dated peat core from Blue Cypress Marsh (BCM) provides a detailed record of natural and anthropogenic factors that controlled the geochemical cycles of a number of trace elements in Florida over the last five centuries. The trace elements were divided into “natural” and “anthropogenic” groups using concentration trends from the bottom to the top of the core. The “natural” group includes Li, Sc, Cr, Co, Ga, Ge, Zr, Nb, Cs, Ba, Hf, Y, Ta, Th, and REE (Rare Earth Elements). These elements show similar concentrations throughout the core, indicating that changes in human activities after European arrival in the “New World” did not affect their geochemical cycles. The “anthropogenic” group includes Pb, Cu, Zn, V, Sb, Sn, Bi, and Cd. Upcore enrichment of these elements indicates enhancement by anthropogenic activities. From the early 1500s to present, fluxes of the “anthropogenic” metals to the marsh increased significantly, with modern accumulation rates several-fold (e.g., V) to hundreds of times (e.g., Zn) greater than pre-colonial rates. The dominant input mechanism for trace elements from both groups to the marsh has been atmospheric deposition. Atmospheric input of a number of the elements, including the anthropogenic metals, was dominated by local sources during the last century. For several elements, long-distant transport may be important. For instance, REE and Nd isotopes provide evidence for long-range atmospheric transport dominated by Saharan dust.The greatest increase in flux of the “anthropogenic” metals occurred during the 20th century and was caused by changes in the chemical composition of atmospheric deposition entering the marsh. Increased atmospheric inputs were a consequence of several anthropogenic activities, including fossil fuel combustion (coal and oil), agricultural activities, and quarrying and mining operations. Pb and V exhibit similar trends, with peak accumulation rates in 1970. The principal anthropogenic source of V is oil combustion. The decline in V accumulation after 1970 in the BCM peat corresponds to the introduction of low-sulfur fuels and the change from heavy to distilled oils since the 1970s. After the 1920s, Pb distribution in the peat follows closely the history of alkyl lead consumption in the US, which peaked in the 1970s. Pb isotopes support this inference and furthermore, record changes in the ore sources used to produce leaded gasoline. Idaho ores dominated the peat Pb isotope record until the 1960s, followed by Pb from Mississippi Valley Type deposits from the 1960s to the 1980s. Enhanced fluxes of Cu, Zn, Cd, Sn, Sb, Bi, and to some extent Ni during the last century are likely also related to fossil fuel combustion. Local agricultural activities may also have influenced the geochemical cycles of Cu and Zn. The peat record shows enhanced U accumulation during the last century, possibly related to phosphate mining in western Florida. Sr isotopes in the peat core also reflect anthropogenic influence. The 87Sr/86Sr ratio decreases from natural background values in the basal part of the core to lower values in the upper part of the core. The Sr isotope shift is probably related to quarrying operations in Florida, and marks the first time an anthropogenic signal has been detected using the Sr isotope record in a peat core.  相似文献   

12.
Annual growth rings of a common hardwood species, Picea abies L., were investigated as a potential archive of past atmospheric Pb pollution. Wide distribution of trees in terrestrial settings and straightforward chronology are two advantages of this potential geochemical archive, but several processes described in the literature may obscure the trends in past Pb deposition. These confounding factors include, e.g., radial post-depositional mobility of Pb in xylem, and ecosystem acidification leading to higher bioavailability of Pb. One- to five-year annual wood increments were analyzed for Pb concentrations and 206Pb/207Pb ratios at Jezeri (JEZ), Uhlirska (UHL) and Na Lizu (LIZ), three sites in the Czech Republic, differing in atmospheric Pb loads. Three to four trees per site were included in the study. Distinct Pb concentration maxima between 1960 and 1990 at the two heavily polluted sites (JEZ and UHL) coincided with historical Pb emissions known from inventories of industrial production. No Pb concentration maxima were found at one site, LIZ, situated in a national park 150 km from major pollution sources. Spruce tree rings from JEZ, located just 5 km from coal-burning power stations, contained a large proportion of coal-derived Pb (a high-206Pb/207Pb ratio of 1.19). A coal-related maximum in 206Pb/207Pb in JEZ tree rings was found using two different analytical techniques, laser-ablation multi-collector ICP MS, and single-collector sector-field ICP MS. In a three-isotope graph (206Pb/207Pb vs. 208Pb/207Pb), tree-ring data plotted into the field of ombrotrophic (i.e., rain-fed) peat bogs, suggesting negligible contribution of bedrock-derived Pb in the xylem. We concluded that none of the potential confounding factors played a major role at our sites. Annual growth rings of P. abies in Central Europe faithfully recorded historical changes in atmospheric Pb depositions.  相似文献   

13.
Natural Pb-isotope variability in the oceans encodes information about the sources of continental material to the oceans, about ocean circulation, and about Pb removal. In order to use this information, we must understand the natural cycle of Pb in the oceans, which is overprinted by large anthropogenic input. In this study we use 210Pb, which has not been significantly anthropogenically perturbed, to investigate oceanic Pb. GEOSECS 226Ra and model-derived atmospheric fluxes of 210Pb are used to input 210Pb into an ocean general circulation model. Irreversible scavenging of this 210Pb onto settling biogenic particles and at the seafloor are tuned so that the model replicates the observed pattern of 210Pb in the oceans. The best-fit model run provides a map of the variability of residence time for Pb. The global average residence time of Pb in this model is 48 yr, but there is over an order of magnitude variation between areas of high and low productivity. This is expected to enhance provinciality of Pb isotope ratios in the oceans. Because stable Pb isotopes are expected to behave in seawater in a similar fashion to 210Pb, the pattern of removal of 210Pb derived by the model can be used to investigate the behavior of stable Pb isotopes. We use a simplified input of Pb consisting of five point sources representing major rivers and a disseminated dust input. Although this simplified input scheme does not allow precise reconstruction of Pb concentration and isotopes in the oceans, it allows us to answer some first-order questions about the behavior of Pb as an ocean tracer. With a total Pb input of 6.3 × 107 mol/yr (Chow T. J. and Patterson C. C., “The occurrence and significance of Pb isotopes in pelagic sediments,” Geochim. Cosmochim. Acta26, 263-308, 1962), the model predicts natural seawater Pb concentrations averaging 2.2 pmol/kg. Even in the absence of anthropogenic input, the model ocean exhibits a near-surface maximum in Pb concentration. And the model suggests natural Pb concentrations in the Northern Hemisphere an order of magnitude higher than in the Southern Hemisphere. A point source of Pb is suggested to dominate the seawater Pb inventory close to the source but is reduced to typically less than 10% of the inventory by the time that Pb is advected out of the originating ocean. This length scale of advection for Pb isotope signals confirms their potential as tracers of ocean circulation. Assuming an 8% dissolution of dust, their input to the open ocean are seen to be a significant portion of Pb inventory throughout the oceans and make up >50% of the Pb inventory in the model’s Southern Ocean. Finally, a preliminary investigation of the response of Pb-isotope distributions to changes in boundary conditions between glacial and interglacial times illustrates that significant variation in the Pb isotopes are expected in some regions, even for reasonably small changes in climate conditions.  相似文献   

14.
A peat core from an ombrotrophic bog documents the isotopic evolution of atmospheric Pb in central Ontario since AD 1804 ± 53 (210Pb dating). Despite the introduction of unleaded gasoline in the mid-1970’s, the ratio 206Pb/207Pb in atmospheric deposition has not increased as expected, but rather continues to decline. In fact, snowpack sampling (2005 and 2009) and rainwater samples (2008) show that the isotopic composition of atmospheric Pb today is often far less radiogenic than the gasoline lead that had been used in Canada in the past. The peat, snow, and rainwater data presented here are consistent with the Pb isotope data for aerosols collected in Dorset in 1984 and 1986 which were traced by Sturges and Barrie (1989) to emissions from the Noranda smelter in northern Quèbec, Canada’s largest single source of atmospheric Pb. Understanding atmospheric Pb deposition in central Ontario, therefore, requires not only consideration of natural sources and past contributions from leaded gasoline, but also emissions from metal smelting and refining.Lead in the streams which enter Kawagama Lake today (206Pb/207Pb = 1.16 − 1.19) represents a mixture between the natural values (1.191 − 1.201 estimated using pre-industrial lake sediments) and the values found in the humus layer of the surrounding forest soils (206Pb/207Pb = 1.15 − 1.19). In the lake itself, however, Pb is much less radiogenic (206Pb/207Pb as low as 1.09) than in the streams, with the dissolved fraction less radiogenic than particulate material. The evolution of Pb isotope ratios within the watershed apparently reflects preferential removal by sedimentation of comparatively dense, radiogenic, terrestrial particles (derived from the mineral fraction of soils) from the humus particles with lower ratios of 206Pb/207Pb (because of atmospheric Pb contamination). Despite the contemporary enrichments of Pb in rain and snow, concentrations of dissolved Pb in the lake are extremely low (sometimes below 10 ng/l), with Pb concentrations and Pb/Sc ratios approaching “natural” values because of efficient binding to particles, and their subsequent removal in the watershed.  相似文献   

15.
The organic horizon (the mor layer) of podzolized boreal forest soils has accumulated atmospheric fallout of mercury and lead over centuries, resulting in current concentrations close to levels where negative effects on soil biota are thought to occur. To what extent the pollution history is preserved in the stratigraphy of this horizon is not well known. In this study we asses whether the chronology of a large historic pulse of atmospheric pollution emitted from the Rönnskär smelter in northern Sweden, particularly between 1950 and 1980, is preserved within the stratigraphy of the mor layer, which is typically 5-cm thick. Vertical sub-sampling (?5 mm) of five mor profiles sampled along a 100-km pollution gradient away from the smelter are analyzed for mercury and lead concentrations, spheroidal carbonaceous particles from fossil fuel combustion (SCPs) and stable lead isotopes (206Pb/207Pb and 208Pb/207Pb). Their vertical distribution is compared with the temporal variations in atmospheric inputs reconstructed for the last ∼100 years from analyses of an ombrotrophic peat core and a varved lake sediment core sampled within a distance of 50 km of the smelter. The mor profiles situated ?12 km from the smelter record the pollution history of the smelter. There is a 20 to 40-times enrichment of Hg, Pb and SCP at the transition in the O-horizon from the F- to H-layer compared to the basal part and a distinct peak in the 206Pb/207Pb ratio (∼1.22) in the F-layer. The mor profiles situated outside the historical contamination range of the smelter (80 and 100 km away) record no obvious influence from the Rönnskär smelter, instead their vertical 206Pb/207Pb profiles follow the general regional pollution history in northern Sweden. We conclude that the mor layer preserves a record of atmospheric Hg, Pb and SCP inputs and due to low leaching rates this organic horizon serves as a semi-archive of atmospheric Hg and Pb pollution. We stress the need of including this property in the existing ‘black-box’ models predicting the fate of Hg and Pb within contaminated boreal forest soils.  相似文献   

16.
The transitional character of climatic conditions confers great relevance to paleoclimate studies in the semiarid region where glacial and Holocene geomorphologic records are scarce. Here we present the paraglacial and fluvial evolution of the Turbio valley (30°S) using both field observations and 14C AMS chronology. Two key sites at the uppermost Turbio valley show glacial margins which likely formed during the 17-12 ka Central Andean Pluvial Event and earlier 37-27 ka episodes associated with glacial advances reported elsewhere in the semiarid Andes. Likewise, two episodes of subsequent paraglacial response are identified: a first episode corresponds to early Holocene fine-grained deposits (~ 11,500-7800 cal yr BP) extending far downstream (> 40 km) from the glacial margins. These deposits and coeval debris cones (~ 11,000-5500 cal yr BP) are the result of arid conditions with occasional runoffs that were unable to export sediments along the trunk valley. The second episode corresponds to disconformably overlying fluvial gravels extending ~ 70 km downstream from the glacial margin, indicative of an increase in the fluvial transport capacity occurring not long after 5500 cal yr BP. Fluvial transport increase resulted from a late Holocene shift to wetter climate conditions, representing a forcing factor which enhanced the paraglacial response.  相似文献   

17.
Rare earth element (REE) distributions and Pb isotope compositions were explored in soils varying in age from ca. 0.4 to ?300 ka, developed on moraines in the Wind River Mountains, Wyoming. Soil extracts (0.6 M HCl) were used to examine the soil labile pool while the major element distribution in soil profiles was used to determine the extent of weathering at different soil depths. The results show that the chondrite-normalized REE patterns of the deepest bulk soil within each profile reflects the composition of the moraine till, except for the oldest soil. Up to ca. 12 ka, the soil extract fraction is enriched in light REE, indicating early release of light REE to the soil labile pool while that of the two oldest soils are relatively enriched in heavy REE. In the soil extracts the La/Sm ratio normalized to the deepest soil (LaD/SmD) decreases systematically with soil age. Similarly, the Eu-anomaly in the deepest soil from each profile (EuD/EuD*) decreases slightly with soil age in the three young soils; however, EuD/EuD* increases with soil age in the older soils. The systematic trends of these two ratios indicate the depletion of light REE in young soils and the enrichment of Eu and heavy REE in the older soils. Based on the Pb isotope ratios, the relative contribution of Pb to the soil labile pool via mineral weathering of U- or Th-rich phases was assessed for the different stages of weathering. The whole-soil profile 208Pb/204Pb ratio was found to decrease with soil age and with LaD/SmD, whereas it increased with the EuD/EuD* ratio. In each horizon, Pb isotope ratios (206Pb/204Pb, 207Pb/204Pb, and 208Pb/204Pb) ratio generally decrease with soil age. In order to overcome possible effects from parent material heterogeneity, the amount of radiogenic Pb as compared to the whole-soil composition was calculated and this was found to decrease systematically with soil age.  相似文献   

18.
The REE and Pb, Sr, Nd isotopes in three xenoliths from limburgite and scoria-breccias, including spinel-lherzolite, spinel-garnet-lherzolite and phlogopite-gamet-lherzolite, were analysed. The REE contents of the xenoliths are 1.3 to 3.3 times those of the chondrites with their REE patterns characterized by weak LREE depletion. The143Nd/144Nd values of whole rocks and minerals range from 0.51306 to 0.51345 with εNd=+ 8.2− +15.8,206Pb/204 Pb < 18.673, and207Pb/204Pb < 15.574. All this goes to show that the upper mantle in Mingxi at the depth of 67–82 km is a depleted mantle of MORB type, with87Sr/86 Sr ratios 0.70237–0.70390. In Nd-Sr diagram the data points of whole rocks are all out of the mantle array, implying that the xenoliths from Mingxi have more radiogenic Sr isotopes than those of the mantle array.  相似文献   

19.
We have carried out a Pb double-spike and Lu-Hf isotope study of clinopyroxenes from spinel-facies mantle xenoliths entrained in Cenozoic intraplate continental volcanism of the French Massif Central (FMC). U-Th-Pb and Lu-Hf isotope systematics verify the existence of different lithospheric domains beneath the northern and southern FMC. Northern FMC clinopyroxenes have extreme Lu/Hf ratios and ultra-radiogenic Hf (εHf = +39.6 to +2586) that reflect ∼15-25% partial melting in Variscan times (depleted mantle model ages ∼360 Ma). Zr, Hf and Th abundances in these clinopyroxenes are low and unaffected by hydrous/carbonatitic metasomatism that overprinted LILE and light REE abundances and caused decoupling of Lu/Hf-Sm/Nd ratios and Nd-Hf isotopes (εNd = +2.1 to +91.2). Pb isotopes of northern FMC clinopyroxenes are radiogenic (206Pb/204Pb > 19), and typically more so than the host intraplate volcanic rocks. 238U/204Pb ratios range from 17 to 68, and most samples have distinctively low 232Th/238U (<1) and 232Th/204Pb (3-22). Clinopyroxenes from southern FMC lherzolites are generally marked by overall incompatible trace element enrichment including Zr, Hf and Th abundances, and have Pb isotopes that are similar to or less radiogenic than the host volcanic rocks. Hf isotope ratios are less radiogenic (εHf = +5.4 to +41.5) than northern FMC mantle and have been overprinted by silicate-melt-dominated metasomatism that affected this part of FMC mantle. Major element and Lu concentrations of clinopyroxenes from southern FMC harzburgites are broadly similar to northern FMC clinopyroxenes and suggest they experienced similar degrees of melt extraction as northern FMC mantle. 238U/204Pb (53-111) and 232Th/204Pb ratios (157-355) of enriched clinopyroxenes from the southern FMC are extreme and significantly higher than the intraplate volcanic rocks. In summary, mantle peridotites from different parts of the FMC record depletion at ∼360 Ma during Variscan subduction, followed by differing styles of enrichment. Northern FMC mantle was overprinted by a fluid/carbonatitic metasomatic agent that carried elements like U, Pb, Sr and light REE. In contrast, much of the southern FMC mantle was metasomatised by a small-degree partial silicate melt resulting in enrichment of all incompatible trace elements. The extreme mantle 238U/204Pb (northern and southern FMC), 232Th/238U (northern FMC) and 232Th/204Pb ratios (southern FMC), coupled with unremarkable present-day Pb isotope ratios, constrain the timing of enrichment. Mantle metasomatism is a young feature related to melting of the upwelling mantle responsible for Cenozoic FMC volcanism, rather than subduction-related metasomatism intimately associated with mantle depletion during the Variscan orogeny. The varying metasomatic styles relate to pre-existing variations in the thickness of the continental lithospheric lid, which controlled the extent to which upwelling mantle could ascend and melt. In the northern FMC, a thicker and more refractory lithospheric lid (?80 km) only allowed incipient degrees of melting resulting in fluid/carbonatitic metasomatism of the overlying sub-continental lithospheric mantle. The thinner lithospheric lid of the southern FMC (?70 km) allowed larger degrees of melting and resulted in silicate-melt-dominated metasomatism, and also focused the location of the volcanic fields of the FMC above this region.  相似文献   

20.
A long dust history established using geological archives from dust provenance areas is necessary to understand the role of atmospheric dust in the global climate system better. Core sediments from a closed-basin groundwater-recharged lake in arid Central Asia were investigated using a multi-proxy approach (e.g. 14C AMS dating, pollen, and grain size) to trace the dust history since ~ 15 cal ka BP. Pollen analysis showed that before 7.9 cal ka BP, the vegetation was of desert type. After 7.9 cal ka BP, vegetation density increased, probably due to slightly increased moisture. The Chenopodiaceae-dominated desert expanded rapidly at 4.2–3.8 cal ka BP. Grain-size analysis was conducted for samples of lake deposits, modern aeolian dust, and dust trapped in snow, and the data showed that there was strong aeolian dust deposition at 11.8–11.1, 10.6–8, 6.1–4.9, and after 3.3 cal ka BP. This timing corresponds well with periods of increased terrestrial dust fluxes recorded by Greenland ice cores. Our study may document changes in the location and intensity of the Siberia High. These changes may play a more important role in the history of dust emission in arid Central Asia than previously thought.  相似文献   

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