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1.
Vertical and temporal variations in the activities of234Th,210Po and210Pb have been measured, in both dissolved and paniculate phases, at several stations in the eastern Arabian Sea and north-central Bay of Bengal. A comparative study allows us to make inferences about the particle associated scavenging processes in these two seas having distinct biogeochemical properties. A common feature of the234Th profiles, in the Arabian Sea and Bay of Bengal, is that the dissolved as well as total (dissolved + particulate) activity of234Th is deficient in the surface 200 m with respect to its parent,238U. This gross deficiency is attributed to the preferential removal of234Th by adsorption onto settling particles which account for its net loss from the surface waters. The scavenging rates of dissolved234Th are comparable in these two basins. The temporal variations in the234Th-238U disequilibrium are significantly pronounced both in the Arabian Sea and Bay of Bengal indicating that the scavenging rates are more influenced by the increased abundance of particles rather than their chemical make-up. In the mixed layer (0–50 m), the scavenging residence time of234Th ranges from 30 to 100 days. The surface and deep waters of both the seas show an enhanced deficiency of dissolved210Po relative to210Pb and that of210Pb relative to226Ra. The deficiencies of both210Po and210Pb in the dissolved phases are not balanced by their abundance in the particulate form indicating a net loss of both these nuclides from the water column. The scavenging rates of210Po and210Pb are significantly enhanced in the Bay of Bengal compared to those in the Arabian Sea. The mean dissolved210Po/210Pb and210Pb/226Ra activity ratios in deep waters of the Bay of Bengal are ∼ 0.7 and 0.1, respectively, representing some of the most pronounced disequilibria observed to date in the deep sea. The Bay of Bengal and the Arabian Sea appear to be the regions of most intense particle moderated scavenging processes in the world oceans. This is evidenced by the gross disequilibria exhibited by the three isotope pairs used in this study.  相似文献   

2.
《Applied Geochemistry》2007,22(4):821-836
High-resolution sampling (every 3 h) of SPM was performed during a major flood event in a heterogeneous, medium scale watershed of the Garonne-Gironde fluvial-estuarine system (the Lot River; A = 10,700 km2; Q = 151 m3/s). Particulate metal and metalloid (Cd, Zn, Pb, Co, Cr, Ni, Mo, V, U, As, Sb, Th) concentrations were compared with monthly data of the same site (Temple site) obtained during 1999–2002. During the flood event, suspended particulate matter (SPM) concentrations closely followed river discharge with a maximum value (1530 mg/L) coinciding with the discharge peak (2970 m3/s). Trace metal/metalloid concentrations showed significant temporal variations and very contrasted responses. Particulate concentrations were similar to baseline values at the beginning of the flood and mostly increased during the event, showing anticlockwise and complex shape hystereses. Comparison of SPM yield (440,000 t) and particulate metal/metalloid fluxes during the flood with annual fluxes (1999–2002) highlights the great importance of major flood events in fluvial transport. Adequate sampling frequency during floods is necessary for reliable annual flux estimates and provides geochemical signals that may greatly improve our understanding of fluvial transport processes. The scenario of SPM and metal and metalloid transport during the flood are reconstructed by combining variations of Zn, Cd and Sb concentrations, concentration ratios (e.g. Zn/Cd, As/Th, Cd/Th) and hysteresis loops. Changes in SPM and metal/metalloid transport during distinct key stages of the flood were attributed to successive dominance of different water masses transporting material from different sources (e.g. industrial point source, bed sediment from reservoirs, plain erosion). Flood management (dam flushing) clearly enhanced the remobilization of up to 30-a old polluted sediment from reservoir lakes. Sediment remobilization accounted for ∼185,000 t of SPM (i.e. 42% of the total SPM fluxes during the flood) and strongly contributed to particulate metal/metalloid transport for Cd (90%), Zn (83%) and Pb (61%). Therefore, flood management needs to be taken into consideration in future models for erosion and pollutant transport.  相似文献   

3.
《Applied Geochemistry》2006,21(3):515-527
Dissolved and particulate Hg fluxes in the Lot–Garonne–Gironde fluvial-estuarine system were obtained from observation of daily discharge and suspended particulate matter (SPM) concentrations. In addition to the measurements of the total dissolved (<0.45 μm) and particulate Hg (>0.45 μm), called HgTD and HgTP respectively, the dissolved inorganic Hg species (HgRD) were determined monthly. Geochemical background values for HgTP in sediments and SPM were similar to crustal values and to typical concentrations in SPM of non-contaminated river systems, respectively. The Riou Mort watershed already known as the origin of important historical polymetallic (e.g., Cd, Zn) pollution was identified as an important Hg point source. In the downstream Lot River, Hg concentrations were clearly higher than those in other moderately contaminated systems. The mean relative contribution of HgRD to HgTD in the Lot River and in the Garonne River was close to 25% and 50%, respectively, and showed no correlation with water discharge or SPM concentration. Depending on the origin and nature of SPM, HgTP concentrations were correlated or not with particulate organic C (POC). Maximum HgTP concentrations were measured in samples containing low POC concentrations and were attributed to sediment resuspension. In contrast, high POC concentrations (6–17%) during algal blooms were associated with low/moderate HgTP concentrations (<0.5 mg kg−1) at different sites, suggesting that Hg concentrations in fluvial phytoplankton may be limited by bioavailability of dissolved Hg and/or physiologically controlled Hg accumulation. Mercury was mostly (up to 98%) transported in the particulate phase with estimated annual Hg fluxes at the outlet of the Lot River system ranging from 35 to 530 kg a−1 for the past decade. The minimum anthropogenic component (58–84% of total Hg fluxes) could not be explained by present Riou Mort point source contributions, suggesting important Hg release from contaminated sediment as a major source and from downstream point sources (e.g., coal-fired power plants and/or metal processing industries). HgTP concentrations and fluxes were strongly related to hydrologic variations and were clearly increased by riverbed dredging during lock construction. Therefore, the estimated Hg stocks in the Lot River sediment (5–13 tons) represent an important potential Hg source for the downstream fluvial-estuarine system.  相似文献   

4.
《Applied Geochemistry》2006,21(11):1837-1854
Total dissolved and total particulate Hg mass balances were estimated during one hydrological period (July 2001–June 2002) in the Thur River basin, which is heavily polluted by chlor-alkali industrial activity. The seasonal variations of the Hg dynamics in the aquatic environment were assessed using total Hg concentrations in bottom sediment and suspended matter, and total and reactive dissolved Hg concentrations in the water. The impact of the chlor-alkali plant (CAP) remains the largest concern for Hg contamination of this river system. Upstream from the CAP, the Hg partitioning between dissolved and particulate phases was principally controlled by the dissolved fraction due to snow melting during spring high flow, while during low flow, Hg was primarily adsorbed onto particulates. Downstream from the CAP, the Hg partitioning is controlled by the concentration of dissolved organic and inorganic ligands and by the total suspended sediment (TSS) concentrations. Nevertheless, the particulate fluxes were five times higher than the dissolved ones. Most of the total annual flux of Hg supplied by the CAP to the river is transported to the outlet of the catchment (total Hg flux: 70 μg m−2 a−1). Downstream from the CAP, the bottom sediment, mainly composed of coarse sediment (>63 μm) and depleted in organic matter, has a weak capacity to trap Hg in the river channel and the stock of Hg is low (4 mg m−2) showing that the residence time of Hg in this river is short.  相似文献   

5.
The convergence of the Nazca and South American plates along the subduction margin of the central Andes results in large subduction earthquakes and tectonic activity along major fault systems. Despite its relevance, the paleoseismic record of this region is scarce, hampering our understanding about the relationship between the Andes building and earthquake occurrence. In this study, we used the U-series disequilibrium method to obtain absolute ages of paleoearthquake events associated with normal displacements along the active Mejillones and Salar del Carmen faults in the Coastal Range of the Atacama Desert of northern Chile. The 230Th–234U disequilibrium ages in co-seismic gypsum salts sampled along the fault traces together with marine evidences indicate that earthquakes occurred at ca. 29.7 ± 1.7 ka, 11 ± 4 ka and 2.4 ± 0.8 ka. When coupled with paleoseismic marine and radiocarbon (14C) records in the nearby Mejillones Bay evidencing large dislocations along the Mejillones Fault, the geochronological dataset presented here is consistent with the notion that gypsum salts formed during large earthquakes as a result of co-seismic dilatancy pumping of saline waters along the major faults. Based on maximum observed cumulative vertical offsets in the studied faults, this phenomena could have occurred episodically at a rate in the order of 1:40 to 1:50 with respect to the very large subduction earthquakes during the latest Pleistocene–Holocene period. The results presented here reveal that the U-series disequilibrium method can be successfully applied to date the gypsum salts deposited along faults during seismic events, and therefore directly constrain the age of large paleoearthquakes in hyperarid and seismically active zones.  相似文献   

6.
《Applied Geochemistry》2005,20(10):1941-1964
The pH, alkalinity, and acidity of mine drainage and associated waters can be misinterpreted because of the chemical instability of samples and possible misunderstandings of standard analytical method results. Synthetic and field samples of mine drainage having various initial pH values and concentrations of dissolved metals and alkalinity were titrated by several methods, and the results were compared to alkalinity and acidity calculated based on dissolved solutes. The pH, alkalinity, and acidity were compared between fresh, unoxidized and aged, oxidized samples.Data for Pennsylvania coal mine drainage indicates that the pH of fresh samples was predominantly acidic (pH 2.5–4) or near neutral (pH 6–7); ≈ 25% of the samples had pH values between 5 and 6. Following oxidation, no samples had pH values between 5 and 6.The Standard Method Alkalinity titration is constrained to yield values >0. Most calculated and measured alkalinities for samples with positive alkalinities were in close agreement. However, for low-pH samples, the calculated alkalinity can be negative due to negative contributions by dissolved metals that may oxidize and hydrolyze.The Standard Method hot peroxide treatment titration for acidity determination (Hot Acidity) accurately indicates the potential for pH to decrease to acidic values after complete degassing of CO2 and oxidation of Fe and Mn, and it indicates either the excess alkalinity or that required for neutralization of the sample. The Hot Acidity directly measures net acidity (= −net alkalinity). Samples that had near-neutral pH after oxidation had negative Hot Acidity; samples that had pH < 6.3 after oxidation had positive Hot Acidity. Samples with similar pH values before oxidation had dissimilar Hot Acidities due to variations in their alkalinities and dissolved Fe, Mn, and Al concentrations. Hot Acidity was approximately equal to net acidity calculated based on initial pH and dissolved concentrations of Fe, Mn, and Al minus the initial alkalinity. Acidity calculated from the pH and dissolved metals concentrations, assuming equivalents of 2 per mole of Fe and Mn and 3 per mole of Al, was equivalent to that calculated based on complete aqueous speciation of FeII/FeIII. Despite changes in the pH, alkalinity, and metals concentrations, the Hot Acidities were comparable for fresh and most aged samples.A meaningful “net” acidity can be determined from a measured Hot Acidity or by calculation from the pH, alkalinity, and dissolved metals concentrations. The use of net alkalinity = (Alkalinitymeasured − Hot Aciditymeasured) to design mine drainage treatment can lead to systems with insufficient Alkalinity to neutralize metal and H+ acidity and is not recommended. The use of net alkalinity = −Hot Acidity titration is recommended for the planning of mine drainage treatment. The use of net alkalinity = (Alkalinitymeasured − Aciditycalculated) is recommended with some cautions.  相似文献   

7.
The main limiting factor in obtaining precise and accurate uranium-series (U-series) ages of corals that lived during the last few hundred years is the ability to constrain and correct for initial thorium-230 (230Th0), which is proportionally much higher in younger samples. This is becoming particularly important in palaeoecological research where accurate chronologies, based on the 230Th chronometer, are required to pinpoint changes in coral community structure and the timing of mortality events in recent time (e.g. since European settlement of northern Australia in the 1850s). In this study, thermal ionisation mass spectrometry (TIMS) U-series dating of 43 samples of known ages collected from living Porites spp. from the far northern, central and southern inshore regions of the Great Barrier Reef (GBR) was performed to spatially constrain initial 230Th/232Th (230Th/232Th0) variability. In these living Porites corals, the majority of 230Th/232Th0 values fell within error of the conservative bulk Earth 230Th/232Th atomic value of 4.3 ± 4.3 × 10?6 (2σ) generally assumed for 230Th0 corrections where the primary source is terrestrially derived. However, the results of this study demonstrate that the accuracy of 230Th ages can be further improved by using locally determined 230Th/232Th0 values for correction, supporting the conclusion made by Shen et al. (2008) for the Western Pacific. Despite samples being taken from regions adjacent to contrasting levels of land modification, no significant differences were found in 230Th/232Th0 between regions exposed to varying levels of sediment during river runoff events. Overall, 39 of the total 43 230Th/232Th0 atomic values measured in samples from inshore reefs across the entire region show a normal distribution ranging from 3.5 ± 1.1 to 8.1 ± 1.1 × 10?6, with a weighted mean of 5.76 ± 0.34 × 10?6 (2σ, MSWD = 8.1). Considering the scatter of the data, the weighted mean value with a more conservative assigned error of 25% (i.e. 5.8 ± 1.4 × 10?6) that encompasses the full variation of the 39 230Th/232Th0 measurements is recommended as a more appropriate value for initial 230Th corrections for U-series dating of most Porites samples from inshore regions of the GBR. This will result in significant improvement in both the precision and accuracy of the corrected 230Th ages related to those based on the assumed bulk Earth 230Th/232Th0 value of 4.3 ± 4.3 × 10?6. However, several anomalously high 230Th/232Th0 values reaching up to 28.0 ± 1.6 × 10?6 occasionally found in some coral annual bands coinciding with El Niño years imply high 230Th/232Th0 sources and highlight the complexities of understanding 230Th/232Th0 variability. For U-series dating of young coral samples from such sites where anomalous 230Th/232Th0 values occur, we suggest replicate dating of multiple growth bands with known age difference to verify age accuracy.  相似文献   

8.
Active and abandoned mine activities constitute the sources of deterioration of water and soil quality in many parts of the world, particularly in the African Copperbelt regions. The accumulation in soils and the release of toxic substances into the aquatic ecosystem can lead to water resources pollution and may place aquatic organisms and human health at risk. In this study, the impact of past mining activity (i.e., abandoned mine) on aquatic ecosystems has been studied using ICP-MS analysis for trace metals and Rare Earth Elements (REE) in sediment samples from Lubumbashi River (RL) and Tshamilemba Canal (CT), Katanga, Democratic Republic of the Congo (DRC). Soil samples from surrounding CT were collected to evaluate trace metal and REE concentrations and their spatial distribution. The extent of trace metal contamination compared to the background area was assessed by Enrichment Factor (EF) and Geoaccumulation Index (Igeo). Additionally, the trace metal concentrations probable effect levels (PELs) for their potential environmental impact was achieved by comparing the trace metal concentrations in the sediment/soil samples with the Sediment Quality Guidelines (SQGs). Spearman's Rank-order correlation was used to identify the source and origin of contaminants. The results highlighted high concentrations of trace metals in surface sediments of CT reaching the values of 40152, 15586, 610, 10322, 60704 and 15152 mg kg−1 for Cu, Co, Zn, Pb, Fe and Mn, respectively. In the RL, the concentrations reached the values of 24093, 2046, 5463, 3340, 68290 and 769 mg kg−1 for Cu, Co, Zn, Pb, Fe and Mn, respectively. The ΣREE varied from 66 to 218 and 142–331 mg kg−1 for CT and RL, respectively. The soil samples are characterized by variable levels of trace metals. The EF analysis showed “extremely severe enrichment” for Cu and Co. However, no enrichment was observed for REE. Except for Mo, Th, U, Eu, Mo, Ho and Tm for which Igeo is classified as “moderately polluted and/or unpolluted”, all elements in different sites are classified in the class 6, “extremely polluted”. The trace metal concentrations in all sampling sites largely exceeded the SQGs and the PELs for the Protection of Aquatic Life recommendation. Cu and Co had positive correlation coefficient values (r = 0.741, P < 0.05, n = 14). This research presents useful tools for the evaluation of water contamination in abandoned and active mining areas.  相似文献   

9.
Based on the concepts (a) that the stable C and O isotopes combined with the Sr isotope ratios of fracture fills should reflect the source groundwater from which the solid phases precipitated and (b) that U-series disequilibria (USD) enable the calculation of residence time for the U by using Fe oxides as the best candidate, an “isotopic toolbox” was applied to fracture fill from the crystalline basement of the Vienne district. The fracture fills are formed mainly of carbonates, clays and Fe oxides. The isotope data indicate two main generations of carbonate that originated from hydrothermal circulation and equilibrium with present-day groundwaters but the Sr isotope ratios highlight another component with a higher 87Sr/86Sr ratio reflecting the complexity of the water–rock interactions.For the USD, the Fe-hydroxides located at 207 m depth yield an age of 102 ± 5 ka (St. Germain I interglacial stage), whereas those located at 277 m and 300 m yield respective ages of 173 ± 15 ka and 181 ± 10 ka. These corresponding to the transition between the penultimate glacial period (isotopic stage 6) and the end of the preceding interglacial stage (isotopic sub-stage 7a). Investigating water–rock interaction (87Sr/86Sr, 18O, 13C, USD) in the fracture-fill minerals from the crystalline basement has shown that such an approach is relevant to developing an understanding of how the groundwater system has changed over time.  相似文献   

10.
Dissolved and particulate Zn and Ni concentrations were determined at 76 locations along the Yangtze River basin from the headwaters to the estuary during flood and dry seasons. Spatial and temporal variations of Zn and Ni were investigated and six major source zones were identified. The Three Gorges Dam (TGD) blocked most of the suspended loads and extremely low concentration of Zn and Ni were observed downstream of the dam. Dissolved (ranging from 0.062 to 8.0 μg L−1) and particulate (ranging from 12 to 110 mg kg−1) Ni showed similar levels of concentrations during flood and dry seasons, whereas dissolved (ranging from 0.43 to 49 μg L−1) and particulate (ranging from 54 to 1100 mg kg−1) Zn were slightly and much lower in the flood season than dry season, respectively. This was attributed to the increased water discharge during the flood season causing a dilution effect and sediment resuspension. In the flood season, average concentrations of Zn and Ni were higher in the main channel than in tributaries, due to soil erosion and mining activities providing the dominant inputs. The situation was opposite in the dry season, attributed to the contribution of municipal sewage, industrial activities, and waste disposal. During the flood season, dissolved Zn and Ni concentrations were negatively correlated with pH. Water and suspended particulate matter (SPM) from the upper reaches, middle reaches, and lower reaches of the Yangtze River were characterized by their Zn and Ni concentrations. The Panzhihua, Nanling and Tongling mining areas were considered as the most important source zones of particulate Zn and Ni. The Chongqing region, Wuhan region and the Yangtze River Delta provided most of the dissolved Zn and Ni inputs into the river. Annual net flux of Zn (10–72 × 105 kg a−1) and Ni (5.0–19 × 105 kg a−1) in each source zone were estimated according to their respective influent and effluent fluxes. Contributions of the source zones to Zn and Ni transport decreased from the upper reaches to the lower reaches.  相似文献   

11.
Ice sheets and deep ice cores have yielded a wealth of paleoclimate information based on continuous dating methods while independent radiometric ages of ice have remained elusive. Here we demonstrate the application of (234U/238U) measurements to dating the EPICA Dome C ice core based on the accumulation of 234U in the ice matrix from recoil during 238U decay out of dust bound within the ice. Measured (234U/238U) activity ratios within the ice generally increase with depth while the surface areas of the dust grains are relatively constant. Using a newly designed device for measuring surface area for small samples, we were able to estimate reliably the recoil efficiency of nuclides from dust to ice. The resulting calculated radiometric ages range between 80 ka and 870 ka. Measured samples in the upper 3100 m fall on the previously published age-depth profile. Samples in the 3200–3255 m section show a marked change from 723–870 ka to 85 ka indicating homogenization of the deep ice prior to resetting of the (234U/238U) age in the basal layers. The mechanism for homogenization is likely enhanced lateral ice flow due to high basal melting and geothermal heat flux.  相似文献   

12.
Perovskite, a common Th- and U-enriched accessory mineral crystallised from kimberlitic magmas, has long been thought to be an important geochronometer for dating the emplacement of kimberlite. However, it also contains variably high levels of common Pb, which makes it difficult to obtain a precise measurement of radiogenic Pb/U and Pb/Th isotopic compositions using microbeam techniques such as SIMS and LA-ICP-MS. We present calibration protocols for in situ U–Pb and Th–Pb age determination of kimberlitic perovskite using the large double-focusing Cameca IMS 1280. Linear relationships are found between ln(206Pb?+/U+) and ln(UO2+/U+), and between ln(208Pb?+/Th+) and ln(ThO+/Th+), based on which the inter-element fractionation in unknown samples during SIMS analyses can be precisely calibrated against a perovskite standard. The well-characterized Ice River perovskite is chosen as the U–Pb and Th–Pb age standard in this study. The 204Pb-correction method was used to estimate the fraction of common Pb, which is consistent with the results obtained using the 207Pb-based correction method for the dated perovskites of Phanerozoic age.A Tazheran perovskite with unusually high U but rather low Th yielded a Concordia U–Pb age of 462.8 ± 2.5 Ma and a Th–Pb age of 462 ± 4 Ma. Two perovskite samples from the Iron Mountain kimberlite have identical Concordia U–Pb ages of 410.8 ± 3.4 Ma and 411.0 ± 2.6 Ma, which are consistent within errors with their corresponding Th–Pb ages of 409.2 ± 7.2 Ma and 412.3 ± 3.3 Ma, respectively. Two perovskite samples from the Wesselton Mine of South Africa yielded indistinguishable 206Pb/238U ages of 91.5 ± 2.2 Ma and 90.3 ± 2.9 Ma, and Th–Pb ages of 90.5 ± 0.8 Ma and 88.4 ± 1.6 Ma, respectively. Accuracy and precision of 1–2% (95% confidence level) for these measurements have been demonstrated by the consistency of their U–Pb and Th–Pb ages with the recommended U–Pb ages of previous works.  相似文献   

13.
A combined study of petrography, whole-rock major and trace elements as well as Rb?Sr and Sm?Nd isotopes, and mineral oxygen isotopes was carried out for two groups of low-T/UHP granitic gneiss in the Dabie orogen. The results demonstrate that metamorphic dehydration and partial melting occurred during exhumation of deeply subducted continent. Zircon δ18O values of ? 2.8 to + 4.7‰ for the gneiss are all lower than normal mantle values of 5.3 ± 0.3‰, consistent with 18O depletion of protolith due to high-T meteoric-hydrothermal alteration at mid-Neoproterozoic. Most samples have extremely low 87Sr/86Sr ratios at t1 = 780 Ma, but very high 87Sr/86Sr ratios at t2 = 230 Ma. This suggests intensive fluid disturbance due to the hydrothermal alteration of protoliths during Neoproterozoic magma emplacement and the metamorphic dehydration during Triassic continental collision. Rb–Sr isotopes, Th/Ta vs. La/Ta and Th/Hf vs. La/Nb relationships suggest that Group I gneiss experienced lower degrees of hydrothermal alteration, but higher degrees of dehydration, than Group II gneiss. The two groups of gneiss have similar patterns of REE and trace element partition. Group I gneiss displays good correlations between Nb and LREEs but no correlations between Nb and LILEs (Rb, Ba, Pb, Th and U), indicating differential mobilities of LILEs during the dehydration. Thus the correlation between Nb and LREEs is inherited from protolith rather than caused by metamorphic modification. Relative to Group I gneiss, Group II gneiss has stronger negative Eu anomaly, lower contents of Sr and Ba but higher contents of Rb, Th and U. In particular, Nb correlates with LILEs (e.g., Rb, Sr, Ba, Th and U), but not with LREEs (La and Ce). This may indicate decoupling between the dehydration and LILEs transport during continental collision. Furthermore, dehydration melting may have occurred due to breakdown of muscovite during “hot” exhumation. Group II gneiss has extremely low contents of FeO + MgO + TiO2 (1.04 to 2.08 wt.%), high SiO2 contents of 75.33 to 78.23 wt%, and high total alkali (Na2O + K2O) contents (7.52 to 8.92 wt.%), comparable with compositions predicted from partial melting of felsic rocks by experimental studies. Almost no UHP metamorphic minerals survived; felsic veins of fine-grain minerals occurs locally between coarse-grain minerals, resulting in a kind of metatexite migmatites due to dehydration melting without considerable escape of felsic melts from the host gneiss. In contrast, Group I gneiss only shows metamorphic dehydration. Therefore, the two groups of gneiss show contrasting behaviors of fluid–rock interaction during the continental collision.  相似文献   

14.
《Applied Geochemistry》2006,21(10):1733-1749
The Tinto and Odiel rivers are heavily affected by acid mine drainage (AMD). However, the exact quantities of contaminants transported into the Huelva estuary and the Gulf of Cadiz are unknown. The existing previous investigations are, in general, based on studies with few data or incorrect methodology, and are therefore unreliable. This study aims to present a reliable estimation of the dissolved contaminant load transported by both rivers for the periods 1995/96 to 2002/03. The methodology used is based principally on the correlation between contaminant concentration and flow rate. The results show that both rivers transport enormous quantities of dissolved contaminants: 7900 t a−1 of Fe, 5800 t a−1 Al, 3500 t a−1 Zn, 1700 t a−1 Cu, 1600 t yr−1 Mn and minor quantities of other metals. These values represent 60% of the global gross flux of dissolved Zn transported by rivers in to the ocean, and 17% of the global gross flux of dissolved Cu.  相似文献   

15.
《Chemical Geology》2007,236(1-2):134-166
The ∼ 5000 km3 Fish Canyon Tuff (FCT) is an important unit for the geochronological community because its sanidine, zircon and apatite are widely used as standards for the 40Ar/39Ar and fission track dating techniques. The recognition, more than 10 years ago [Oberli, F., Fischer, H. and Meier, M., 1990. High-resolution 238U–206Pb zircon dating of Tertiary bentonites and Fish Canyon Tuff; a test for age “concordance” by single-crystal analysis. Seventh International Conference on Geochronology, Cosmochronology and Isotope Geology. Geological Society of Australia Special Publication Canberra, 27:74], of a ≥ 0.4 Ma age difference between the U–Pb zircon ages and 40Ar/39Ar sanidine ages has, therefore, motivated efforts to resolve the origin of this discrepancy. To address this controversial issue, we initially performed 37 U–Pb analyses on mainly air-abraded zircons at ETH Zurich and nearly 200 40Ar/39Ar measurements on hornblende, biotite, plagioclase and sanidine obtained at the University of Geneva, using samples keyed to a refined eruptive stratigraphy of the FCT magmatic system.Disequilibrium-corrected 206Pb/238U ages obtained for 29 single-crystal and three multi-grain analyses span an interval of ∼ 28.67–28.03 Ma and yield a weighted mean age of 28.37 ± 0.05 Ma (95% confidence level), with MSWD = 8.4. The individual dates resolve a range of ages in excess of analytical precision, covering ∼ 600 ka. In order to independently confirm the observed spread in zircon ages, 12 additional analyses were carried out at the Berkeley Geochronology Center (BGC) on individual zircons from a single lithological unit, part of them pre-treated by the “chemical abrasion” (CA) technique [Mattinson, J.M., 2005. Zircon U–Pb chemical abrasion (“CA-TIMS”) method: Combined annealing and multi-step partial dissolution analysis for improved precision and accuracy of zircon ages. Chemical Geology, 220(1–2): 47–66]. Whereas the bulk of the BGC results displays a spread overlapping that obtained at ETH, the group of CA treated zircons yield a considerably narrower range with a mean age of 28.61 ± 0.08 Ma (MSWD = 1.0). Both mean zircon ages determined at ETH and BGC are older than the ∼ 28.0 Ma 40Ar/39Ar eruption age of FCT – even when considering the possibility that the latter may be low by as much as ∼ 1% due to a miscalibration of the 40K decay constants – and is thus indicative of a substantial time gap between magma crystallization and extrusion. The CA technique further reveals that younger FCT zircon ages are likely to be associated with chemically unstable U-enriched domains, which may be linked to crystallization during extended magma residence or may have been affected by pre-eruptive and/or post-eruptive secondary loss of radiogenic lead. Due to their complex crystallization history and/or age bias due to Pb loss, the FCT zircon ages are deemed unsuitable for an accurate age calibration of FCT sandine as a fluence monitor for the 40Ar/39Ar method.Even though data statistics preclude unambiguous conclusions, 40Ar/39Ar dating of sanidine, plagioclase, biotite, and hornblende from the same sample of vitrophyric Fish Canyon Tuff supports the idea of a protracted crystallization history. Sanidine, thought to be the mineral with the lowest closure temperature, yielded the youngest age (28.04 ± 0.18 Ma at 95% c.l., using Taylor Creek Rhyolite [Renne, P.R. et al., 1998. Intercalibration of standards, absolute ages and uncertainties in 40Ar/39Ar dating. Chemical Geology, 145: 117–152.] as the fluence monitor), whereas more retentive biotite, hornblende and plagioclase gave slightly older nominal ages (by 0.2–0.3 Ma). In addition, a laser step-heating experiment on a 2-cm diameter feldspar megacryst produced a “staircase” argon release spectrum (older ages at higher laser power), suggestive of traces of inherited argon in the system. Thermal and water budgets for the Fish Canyon magma indicate that the body remained above its solidus (∼ 700 °C) for an extended period of time (> 105 years). At these temperatures, argon volume diffusion is thought to be fast enough to prevent accumulation of radiogenic Ar. If this statement were true, an existing isotopic record should have been completely reset within a few hundred years, regardless of the phase and initial age of the phenocryst. As these minerals are unlikely to be xenocrysts that were incorporated within such a short time span prior to eruption, we suggest that a fraction of radiogenic Ar can be retained > 105 years, even at T ∼ 700 °C.  相似文献   

16.
During the past 60 years, more than 1800 metric tonnes of Pu, and substantial quantities of the “minor” actinides, such as Np, Am and Cm, have been generated in nuclear reactors. Some of these transuranium elements can be a source of energy in fission reactions (e.g., 239Pu), a source of fissile material for nuclear weapons (e.g., 239Pu and 237Np), and of environmental concern because of their long-half lives and radiotoxicity (e.g., 239Pu and 237Np). There are two basic strategies for the disposition of these heavy elements: (1) to “burn” or transmute the actinides using nuclear reactors or accelerators; (2) to “sequester” the actinides in chemically durable, radiation-resistant materials that are suitable for geologic disposal. There has been substantial interest in the use of actinide-bearing minerals, especially isometric pyrochlore, A2B2O7 (A = rare earths; B = Ti, Zr, Sn, Hf), for the immobilization of actinides, particularly plutonium, both as inert matrix fuels and nuclear waste forms. Systematic studies of rare-earth pyrochlores have led to the discovery that certain compositions (B = Zr, Hf) are stable to very high doses of alpha-decay event damage. Recent developments in our understanding of the properties of heavy element solids have opened up new possibilities for the design of advanced nuclear fuels and waste forms.  相似文献   

17.
Seawater temperatures throughout Earth's history have been suggested to illustrate a long-term cooling trend from nearly 70 °C at ～3500 Ma to around 20 °C at ～800 Ma. The terminal Neoproterozoic prior to the “Cambrian Explosion” is a key interval in evolutionary history, as complex multicellularity appeared with the advent of the Ediacara fauna. These organisms were likely the first that required higher levels of atmospheric and dissolved marine oxygen for their sustainability. It is known that most modern macroinvertebrates are intolerant of temperatures in excess of 45 °C. Perhaps more importantly, these high seawater temperatures limit the potential of dissolved oxygen, and therefore become an integral part of this evolutionary story. Previously, our understanding of seawater temperature during the terminal Neoproterozoic comes only from 18O/16O and 30Si/28Si ratios ascertained from a limited number of cherts. Isotopic ratio methods for assessing seawater temperatures are inherently indirect and have a wide range of oscillation. However, maximum homogenization temperatures (Thmax) of primary fluid inclusions in halite provide a direct means of assessing brine temperature, and have been shown to correlate well with average maximum air temperatures. The oldest halites date to the Neoproterozoic–lower Paleozoic (～700–500 Ma), and Ediacaran representatives can be found in Sichuan Province, China, which do preserve primary fluid inclusions for analysis via cooling nucleation methods. We utilized halite samples from the Changning-2 well, correlative to the Dengying Formation (551–542 Ma), to provide a direct assessment of terminal Neoproterozoic seawater temperature. Our measurements indicate that seawater temperatures where these halites formed are highly similar to tropical Phanerozoic seawater temperature estimates. From compiled paleotemperature data, the decline in seawater temperatures over the course of the Proterozoic, accompanied by the reduction of seawater salinity with the sequestration of salt in massive halite deposits in the Neoproterozoic, allowed the ocean system to accumulate more dissolved oxygen, and potentially paved the way for the evolutionary innovation of complex multicellularity.  相似文献   

18.
Radiocarbon dates from known age, pre-bomb eastern oyster (Crassostrea virginica) shells provide local marine reservoir corrections (?R) for Chesapeake Bay and the Middle Atlantic coastal area of eastern North America. These data suggest subregional variability in ?R, ranging from 148 ± 46 14C yr on the Potomac River to ? 109 ± 38 14C yr at Swan Point, Maryland. The ?R weighted mean for the Chesapeake's Western Shore (129 ± 22 14C yr) is substantially higher than the Eastern Shore (? 88 ± 23 14C yr), with outer Atlantic Coast samples falling between these values (106 ± 46 and 2 ± 46 14C yr). These differences may result from a combination of factors, including 14C-depleted freshwater that enters the bay from some if its drainages, 14C-depleted seawater that enters the bay at its mouth, and/or biological carbon recycling. We advocate using different subregional ?R corrections when calibrating 14C dates on aquatic specimens from the Chesapeake Bay and coastal Middle Atlantic region of North America.  相似文献   

19.
Granulite grade marble layers interlayered with metapelitic granulites from Lützow Holm Bay, East Antarctica, provide insight into fluid–rock interactions during burial to and exhumation from lower crustal levels. Sub-millimeter scale strontium, oxygen and carbon isotope variations along with LA-ICPMS trace element geochemistry and mineral chemistry of texturally characterized carbonates and associated minerals helped to reconstruct the multistage metamorphic fluid history.Fluid–rock interaction dating back to prograde metamorphism are still preserved in consistently low oxygen and high strontium isotope compositions (δ18O = 12‰; 87Sr/86Sr(550Ma) = 0.7248) within a massif dolomitic marble layer that escaped significant later metasomatism. In most marbles, total re-crystallization and isotopic resetting occurred in the presence of “externally derived” hyper-saline fluids that circulated along the carbonate layers during the early stages of prograde metamorphism. This leads to a trend of increased radiogenic Sr in marbles towards the value of associated metapelitic rocks that have 87Sr/86Sr(550Ma) of 0.764.LA-ICPMS studies on trace elements in carbonate and associated silicate minerals at different textural settings, distinguished using cathodoluminescence microscopy, revealed multiple metasomatic events during retrograde metamorphism. Trace element contents of Ba, Sr, Pb and U gave compelling evidence for metasomatic alteration that postdate the exsolution of carbonate at ~ 600 ºC, which can be correlated with the fluids released from the crystallization of anatectic melts and pegmatites. Subsequently, meteoric fluid infiltration occurred at a shallower level of the crust and caused extreme oxygen isotopic heterogeneity (δ18O = 14.7 ~ ? 4.9‰) and imprinted high concentration of fluid mobile elements. Taken together our results emphasize the importance of integrating textural and chemical heterogeneities to reveal the multiple episodes of fluid–rock interaction processes in a dynamic continental crust, which has major implications on migration of fluids and material and help in formulating models on the geodynamic evolution of crust.  相似文献   

20.
《Applied Geochemistry》2005,20(5):919-931
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