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1.
We have collected ∼500 stream waters and associated bed-load sediments over an ∼400 km2 region of Eastern Canada and analyzed these samples for Fe, Mn, and the rare earth elements (REE + Y). In addition to analyzing the stream sediments by total digestion (multi-acid dissolution with metaborate fusion), we also leached the sediments with 0.25 M hydroxylamine hydrochloride (in 0.05 M HCl), to determine the REE + Y associated with amorphous Fe- and Mn-oxyhydroxide phases. We are thus able to partition the REE into “dissolved” (<0.45 μm), labile (hydroxylamine) and detrital sediment fractions to investigate REE fractionation, and in particular, with respect to the development of Ce and Eu anomalies in oxygenated surface environments. Surface waters are typically LREE depleted ([La/Sm]NASC ranges from 0.16 to 5.84, average = 0.604, n = 410; where the REE are normalized to the North America Shale Composite), have strongly negative Ce anomalies ([Ce/Ce∗]NASC ranges from 0.02 to 1.25, average = 0.277, n = 354), and commonly have positive Eu anomalies ([Eu/Eu∗]NASC ranges from 0.295 to 1.77, average = 0.764, n = 84). In contrast, the total sediment have flatter REE + Y patterns relative to NASC ([La/Sm]NASC ranges from 0.352 to 1.12, average = 0.778, n = 451) and are slightly middle REE enriched ([Gd/Yb]NASC ranges from 0.55 to 3.75, average = 1.42). Most total sediments have negative Ce and Eu anomalies ([Ce/Ce∗]NASC ranges from 0.097 to 2.12, average = 0.799 and [Eu/Eu∗]NASC ranges from 0.39 to 1.43, average = 0.802). The partial extraction sediments are commonly less LREE depleted than the total sediments ([La/Sm]NASC ranges from 0.24 to 3.31, average = 0.901, n = 4537), more MREE enriched ([Gd/Yb]NASC ranges from 0.765 to 6.28, average = 1.97) and Ce and Eu anomalies (negative and positive) are more pronounced.The partial extraction recovered, on average ∼20% of the Fe in the total sediment, ∼80% of the Mn, and 21-29% of the REEs (Ce = 19% and Y = 32%). Comparison between REEs in water, partial extraction and total sediment analyses indicates that REEs + Y in the stream sediments have two primary sources, the host lithologies (i.e., mechanical dispersion) and hydromorphically transported (the labile fraction). Furthermore, Eu appears to be more mobile than the other REE, whereas Ce is preferentially removed from solution and accumulates in the stream sediments in a less labile form than the other REEs + Y. Despite poor statistical correlations between the REEs + Y and Mn in either the total sediment or partial extractions, based on apparent distribution coefficients and the pH of the stream waters, we suggest that either sediment organic matter and/or possibly δ-MnO2/FeOOH are likely the predominant sinks for Ce, and to a lesser extent the other REE, in the stream sediments.  相似文献   

2.
This paper presents new major and trace-element data and Lu-Hf and Sm-Nd isotopic compositions for representative suites of marine sediment samples from 14 drill sites outboard of the world’s major subduction zones. These suites and samples were chosen to represent the global range in lithology, Lu/Hf ratios, and sediment flux in subducting sediments worldwide. The data reported here represent the most comprehensive data set on subducting sediments and define the Hf-Nd isotopic variations that occur in oceanic sediments and constrain the processes that caused them.Using new marine sediment data presented here, in conjunction with published data, we derive a new Terrestrial Array given by the equation, εHf = 1.55 × εNd + 1.21. This array was calculated using >3400 present-day Hf and Nd isotope values. The steeper slope and smaller y-intercept of this array, compared to the original expression (εHf = 1.36 × εNd + 2.89; Vervoort et al., 1999) reflects the use of present day values and the unradiogenic Hf of old continental samples included in the array.In order to examine the Hf-Nd isotopic variations in marine sediments, we have classified our samples into 5 groups based on lithology and major and trace-element geochemical compositions: turbidites, terrigenous clays, and volcaniclastic, hydrothermal and hydrogenetic sediments. Compositions along the Terrestrial Array are largely controlled by terrigenous material derived from the continents and delivered to the ocean basins via turbidites, volcaniclastic sediments, and volcanic inputs from magmatic arcs. Compositions below the Terrestrial Array derive from unradiogenic Hf in zircon-rich turbidites. The anomalous compositions above the Terrestrial Array largely reflect the decoupled behavior of Hf and Nd during continental weathering and delivery to the ocean. Both terrigenous and hydrogenetic clays possess anomalously radiogenic Hf, reflecting terrestrial sedimentary and weathering processes on the one hand and marine inheritance on the other. This probably occurs during complementary processes involving preferential retention of unradiogenic Hf on the continents in the form of zircon and release of radiogenic Hf from the breakdown of easily weathered, high Lu-Hf phases such as apatite.  相似文献   

3.
Geochemical methods (major elements and Sr, Nd isotopes) have been used to (1) characterize Lake Le Bourget sediments in the French Alps, (2) identify the current sources of the clastic sediments and estimate the source variability over the last 600 years. Major element results indicate that Lake Le Bourget sediments consist of 45% clastic component and 55% endogenic calcite. In addition, several individual flood levels have been identified during the Little Ice Age (LIA) on the basis of their higher clastic content (> 70%).Potential sources of Lake Le Bourget clastic sediments have been investigated from Sr and Nd isotope compositions. The sediments from the Sierroz River and Leysse River which are mainly derived from the Mesozoic Calcareous Massifs are characterised by lower 87Sr/86Sr ratios and slightly lower ?Nd(0) ratios than the Arve River sediments which are derived from the Palaeozoic Mont-Blanc External Crystalline Massifs. The Rhône River appears to have been the main source of clastic sediments into the lake for the last 600 years, as evidenced by a similar Sr and Nd isotopic compositions analyzed in core B16 sediments (87Sr/86Sr = 0.719, ?Nd(0) = − 10) and in the sediments of the Rhône River (87Sr/86Sr = 0.719, ?Nd(0) = − 9.6).The isotopic signatures of flood events and background samples from core B16 in Lake Le Bourget are also similar. This indicates that prior to ∼ 1800, the inputs into the lake have remained relatively homogeneous with the proportion of clastic component mainly being a function of the palaeohydrology of the Rhone River. Early human modification (deforestation and agriculture) of the lake catchment before the 1800s appears to have had little influence on the source of clastic sediments.  相似文献   

4.
We investigated anaerobic ammonium oxidation (anammox) in continental shelf and slope sediments of the Irish and Celtic Seas by using anammox specific ladderane biomarker lipids. We used the presence of an intact ladderane phospholipid as a direct indicator for living anammox bacteria, and compared it with the abundance of ladderane core lipids derived from both living and dead bacterial biomass. All investigated sediments contained ladderane core lipids as well as the intact ladderane phospholipid, in agreement with 15N-labeling experiments, which revealed anammox activity at all sites. Ladderane core lipid and intact ladderane phospholipid concentrations were significantly correlated (R2 = 0.957 and 0.464, respectively) with anammox activity over the transect of the continental shelf and slope sediments. In the Irish Sea (50-100 m water depth) highest abundances of the intact ladderane phospholipid were found in the upper 2 cm of the sediment, indicating a zone of active anammox. A sharp decline further down-core suggested a strong decrease in anammox biomass and rapid degradation of the intact lipids. In comparison, ladderane core lipids were 1-2 orders of magnitude higher in concentration than the intact ladderane phospholipid and accumulated as dead cell remnants with depth. In the slope sediments of the Celtic Sea both ladderane core lipids and the intact ladderane phospholipid were found in sediments at water depths ranging from 500 to 2000 m. Here, anammox seemed to be active at greater depths of the sediment (>2 cm). Mean abundances of both intact and core ladderane lipids in whole sediment cores increased downslope, indicating an increasing importance of anammox in deeper slope sediments.  相似文献   

5.
Concentrations of tungsten (W) and uranium (U), which represent two of the most highly incompatible elements during mantle melting, have been measured in a suite of Hawaiian picrites and primitive tholeiites from nine main-stage shield volcanoes. Tungsten abundances in the parental melts are estimated from correlations between sample W abundances and MgO contents, and/or by olivine correction calculations. From these parental melt determinations, along with independent estimates for the degree of partial melting at each volcanic center, we extrapolate the W content of the mantle sources for each shield volcano. The mantle sources of Hualalai, Mauna Loa, Kohala, Kilauea, Mauna Kea, Koolau and Loihi contain 9 ± 2 (2σ), 11 ± 5, 10 ± 4, 12 ± 4, 10 ± 5, 8 ± 7 and 11 ± 5 ng/g, respectively. When combined, the mean Hawaiian source has an average of 10 ± 3 ng/g W, which is three-times as enriched as the Depleted MORB Mantle (DMM; 3.0 ± 2.3 ng/g).The relatively high abundances of W in the mantle sources that contribute to Hawaiian lavas may be explained as a consequence of the recycling of W-rich oceanic crust and sediment into a depleted mantle source, such as the depleted MORB mantle (DMM). However, this scenario requires varying proportions of recycled materials with different mean ages to account for the diversity of radiogenic isotope compositions observed between Kea- and Loa-trend volcanoes. Alternatively, the modeled W enrichments may also reflect a primary source component that is less depleted in incompatible trace elements than the DMM. Such a source would not necessarily require the addition of recycled materials, although the presence of some recycled crust is permitted within our model parameters and likely accounts for some of the isotopic variations between volcanic centers.The physical admixture of ?0.5 wt.% outer core material with the Hawaiian source region would not be resolvable via W source abundances or W/U ratios; however, W isotopes may provide a more sensitive to this mixing process. Recent W isotopic studies show no indication of core-mantle interaction, indicating that either such a process does not occur, or that mechanisms other than physical mixing may operate at the core-mantle boundary.  相似文献   

6.
SHRIMP zircon U-Pb dates, combined with in-situ Hf isotopic data, provide new constraints on the petrogenesis and protolith of peralkaline, metaluminous and peraluminous intrusions and rhyolitic tuffs in the Emeishan large igneous province, with significant bearing on crustal melting associated with mantle plumes. Syenite and A-type granitic intrusions from Huili, Miyi and Taihe in the center of this large igneous province yield U-Pb dates at ∼260 Ma, consistent with the ages obtained for mafic layered intrusions in the same province. Zircon from these rocks exhibits a wide range of initial Hf isotope ratios (εHf(t) = −1.4 to +13.4), with corresponding TDM1 of 400-900 Ma. The highest εHf(t) value is only marginally lower than that of depleted mantle reservoir at 260 Ma, suggesting that their source is primarily juvenile crust added during Emeishan volcanism, with incorporation of variable amounts of Neoproterozoic crust. The trigger of crustal melting is most likely related to advective heating associated with magmatic underplating. In contrast, the 255-251 Ma peraluminous granites from Ailanghe and 238 Ma rhyolitic tuff from Binchuan, have negative initial εHf values of −1.3 to −4.4, and of −7.7 to −14, respectively. Hf isotopic model ages and presence of inherited zircons indicate their derivation from Mesoproterozoic and Paleoproterozoic crust, respectively. Given the time lag relative to the plume impact (∼260 Ma) and insignificant mantle contribution to 255-238 Ma magmatism, conductive heating is suggested as the trigger of crustal melting that resulted in formation of delayed felsic magmas. The involvement of older crust in younger felsic magmas is consistent with upward heat transfer to the lithosphere during plume impregnation, if the age of crust is inversely stratified, i.e., changes from Paleoproterozoic to Mesoproterozoic to Neoproterozoic to Permian with increasing depth. Such crust may have resulted from episodic, downward crustal growth during the evolution of the western Yangtze Craton.  相似文献   

7.
We present the first comprehensive major, trace element and Hf, Nd and Sr isotope investigation of clinopyroxene and garnet mineral separates from a set of garnet clinopyroxenite xenoliths from the Salt Lake Crater, Oahu, Hawaii. These xenoliths occur in the posterosional Honolulu Volcanics Series lavas and represent some of the deepest samples from the oceanic mantle lithosphere. Our study shows that the Salt Lake Crater pyroxenites represent high pressure (>20 kb) accumulates from melts similar (but not identical) to the erupted Honolulu Volcanics, and unlike MORB or E-MORB-type melts. All clinopyroxene-garnet mineral pairs in these xenoliths show, within error, zero-age Lu-Hf and Sm-Nd isotope systematics. These pyroxenites have relatively radiogenic Hf isotope compositions (for a given Nd) and define a distinct steep slope (3.3) in εHf-εNd isotope space, similar to the Honolulu Volcanics but unlike other ocean island basalts (OIB). These compositions require an end-member component that falls above the OIB array in Nd-Hf space. This component is different than present-day MORB-mantle and it is best explained by an old depleted oceanic lithosphere. We suggest that this depleted component most likely represents a recycled depleted lithosphere that is intrinsic to the Hawaiian plume. In this respect, the Hawaiian plume is sampling both the enriched portion of a subducted oceanic crust (basalt and sediments) as well as the depleted lithospheric portion of it. This suggests that, at least for Hawaii, the whole subducted oceanic slab package has retained its integrity during subduction and subsequent mixing and storage in the mantle, probably in the order of a billion years, and that the plume is sampling the full range of these compositions.  相似文献   

8.
We report 15N/14N ratios of porewater nitrate in sediments from the Bering Sea basin, where microbial nitrate reduction has been identified as a significant sink for fixed nitrogen (N). Strong 15N enrichment in porewater nitrate is observed as one goes deeper in the sediments and nitrate concentration decreases (δ15N generally reaches 25-35‰). Analysis of profiles with a one-dimensional diffusion-reaction model yields organism-scale isotope effects for dissimilatory nitrate reduction (εcell) of 11‰ to 30‰, in the same range as measured in previous studies of cultures and the marine and lacustrine water column. Estimates of εcell, while uncertain, show a negative correlation with bottom water [O2]; we propose that this relates to the at the depth of denitrification. The N isotope effect at the scale of nitrate sediment-water exchange (εapp) is ∼0‰ in two unreactive deep sites and is typically <3‰ at more reactive sites at various depths. εapp is much lower than εcell because nitrate consumption is nearly complete at the sediment depth of denitrification, minimizing the escape of 15N-enriched nitrate from the sediments. In reactive sediments, this is due to rapid denitrification, while in less reactive sediments, it is due to greater diffusive distances for nitrate to the depth of denitrification. The data suggest that low bottom water [O2] tends to yield more complete expression of εcell at the sediment-water scale, due to higher at the depth of denitrification. While porewater ammonium-N isotopes were not measured, our porewater model suggests that, in sediments with high organic matter supply and/or low-[O2] bottom waters, the efflux and subsequent oxidation of ammonium enriched in 15N by incomplete nitrification can significantly enhance the total net isotope effect of sedimentary N loss (εsed, equivalent to εapp but including ammonium fluxes). Model analysis of representative sedimentary environments suggests a global mean εsed of ∼4‰ (∼2‰ if restricted to seafloor below 1 km depth).  相似文献   

9.
Estimates of glacial sediment delivery to the oceans have been derived from fluxes of meltwater runoff and iceberg calving, and their sediment loads. The combined total (2900 Tg yr−1) of the suspended sediment load in meltwaters (1400 Tg yr−1) and the sediment delivered by icebergs (1500 Tg yr−1) are within the range of earlier estimates. High-resolution microscopic observations show that suspended sediments from glacial meltwaters, supraglacial, and proglacial sediments, and sediments in basal ice, from Arctic, Alpine, and Antarctic locations all contain iron (oxyhydr)oxide nanoparticles, which are poorly crystalline, typically ∼5 nm in diameter, and which occur as single grains or aggregates that may be isolated or attached to sediment grains. Nanoparticles with these characteristics are potentially bioavailable. A global model comparing the sources and sinks of iron present as (oxyhydr)oxides indicates that sediment delivered by icebergs is a significant source of iron to the open oceans, beyond the continental shelf. Iceberg delivery of sediment containing iron as (oxyhydr)oxides during the Last Glacial Maximum may have been sufficient to fertilise the increase in oceanic productivity required to drawdown atmospheric CO2 to the levels observed in ice cores.  相似文献   

10.
Chromium(VI) concentrations in groundwater sampled from three contaminant plumes in aquifers in the Mojave Desert near Hinkley, Topock and El Mirage, California, USA, were as high as 2600, 5800 and 330 μg/L, respectively. δ53/52Cr compositions from more than 50 samples collected within these plumes ranged from near 0‰ to almost 4‰ near the plume margins. Assuming only reductive fractionation of Cr(VI) to Cr(III) within the plume, apparent fractionation factors for δ53/52Cr isotopes ranged from εapp = 0.3 to 0.4 within the Hinkley and Topock plumes, respectively, and only the El Mirage plume had a fractionation factor similar to the laboratory derived value of ε = 3.5. One possible explanation for the difference between field and laboratory fractionation factors at the Hinkley and Topock sites is localized reductive fractionation of Cr(VI) to Cr(III), with subsequent advective mixing of native and contaminated water near the plume margin. Chromium(VI) concentrations and δ53/52Cr isotopic compositions did not uniquely define the source of Cr near the plume margin, or the extent of reductive fractionation within the plume. However, Cr(VI) and δ53/52Cr data contribute to understanding of the interaction between reductive and mixing processes that occur within and near the margins of Cr contamination plumes. Reductive fractionation of Cr(VI) predominates in plumes having higher εapp, these plumes may be suitable for monitored natural attenuation. In contrast, advective mixing predominates in plumes having lower εapp, the highly dispersed margins of these plumes may be difficult to define and manage.  相似文献   

11.
The isotopic compositions of Sm and Gd in lunar regolith samples from the Apollo 16 and 17 deep drill stems showed clear isotopic shifts in 150Sm /149Sm (ε = +124 to +191 for A-16, and +37 to +111 for A-17) and 158Gd/157Gd (ε = +107 to +169 for A-16, and +31 to +84 for A-17) corresponding to neutron fluences of (5.68-9.03) × 1016 n cm−2 for A-16 and (1.85-5.04) × 1016 n cm−2 for A-17. The depth profiles of neutron fluences suggest that the regoliths at both sites were due to incomplete mixing of three different slabs which experienced individual two-stage irradiation before and after deposition of the upper slabs. The variations in REE compositions provide chemical evidence for incompletely vertical mixing of regoliths especially at upper layers of the two sites. The thermal neutron energy index estimated from the combination of Sm and Gd isotopic shifts, defined as εSm/εGd, shows a small variation (0.61-0.64) in the A-16 core except for the surface layer. On the other hand, a large variation in εSm/εGd = 0.67 to 0.83 in the A-17 core may result from complicated history such as two-stage irradiation and incomplete mixing during the gardening processes. Isotopic enrichments of 152Gd and 154Gd correlated with Eu/Gd elemental abundances and neutron fluences were also observed in almost all of 15 samples, showing evidence of neutron-capture from 151Eu and 153Eu, respectively.  相似文献   

12.
Ion-microprobe was used to measure Li abundances and isotopic compositions in pyroxenes from three Martian meteorites belonging to the nakhlite family. The profiles performed across augite crystals from Northwest Africa 817 show a large isotopic zoning from crystal cores (δ7Li ∼ 0‰) to rims (δ7Li ∼ +20‰) while Li abundances are almost constant (∼9.2 μg/g). Unlike NWA 817, the pyroxene studied in the Miller Range 03346 nakhlite shows a zoning in Li abundance, with concentrations increasing from ∼2.5 μg/g in the core to ∼9 μg/g in the rim. The augite rim (δ7Li = +7‰) is slightly enriched in 7Li with regard to the core (δ7Li = +4‰), but most of the isotopic variations observed occur at an intermediate position along the profile, where δ7Li falls down to ∼−11‰. In the case of Nakhla, Li concentrations in augite increase from cores (∼3.5 μg/g) to rims (∼6.5 μg/g), while the δ7Li variation is restricted (i.e., between δ7Li = +6.0 and +12.6‰). For the three meteorites the Li abundances were also measured in the groundmass, which was found to be enriched in lithium (∼10 μg/g). Conventional magmatic and post-magmatic processes such as alteration and fractional crystallization, fail to explain the dataset obtained on nakhlites. Degassing processes, which were previously proposed to explain the Li distribution in shergottite crystals, cannot result in the strong decoupling between Li abundances and isotopic composition observed in nakhlites. We suggest that the original magmatic Li distributions (concentrations and isotopic compositions) in nakhlites have been modified by diffusion of Li from the Li-rich groundmass towards the pyroxene crystals during sub-solidus cooling. Diffusion appears to have been efficient for NWA 817 and MIL 03346 but, apparently, did not produce a significant migration of Li in Nakhla, possibly because of the lower abundance of groundmass in the latter. Diffusion induced Li redistributions may also affect terrestrial porphyric rocks but very specific cooling rates are required to quench the diffusion profiles as observed in two of the present nakhlites.  相似文献   

13.
We report new chemical and isotopic data from 26 volcanic and geothermal gases, vapor condensates, and thermal water samples, collected along the Nicaraguan volcanic front. The samples were analyzed for chemical abundances and stable isotope compositions, with a focus on nitrogen abundances and isotope ratios. These data are used to evaluate samples for volatile contributions from magma, air, air-saturated water, and the crust. Samples devoid of crustal contamination (based upon He isotope composition) but slightly contaminated by air or air-saturated water are corrected using N2/Ar ratios in order to obtain primary magmatic values, composed of contributions from upper mantle and subducted hemipelagic sediment on the down-going plate. Using a mantle endmember with δ15N = −5‰ and N2/He = 100 and a subducted sediment component with δ15N = +7‰ and N2/He = 10,500, the average sediment contribution to Nicaraguan volcanic and geothermal gases was determined to be 71%. Most of the gases were dominated by sediment-derived nitrogen, but gas from Volcán Mombacho, the southernmost sampling location, had a mantle signature (46% from subducted sediment, or 54% from the mantle) and an affinity with mantle-dominated gases discharging from Costa Rica localities to the south. High CO2/N2 exc. ratios (N2 exc. is the N2 abundance corrected for contributions from air) in the south are similar to those in Costa Rica, and reflect the predominant mantle wedge input, whereas low ratios in the north indicate contribution by altered oceanic crust and/or preferential release of nitrogen over carbon from the subducting slab. Sediment-derived nitrogen fluxes at the Nicaraguan volcanic front, estimated by three methods, are 7.8 × 108 mol N/a from 3He flux, 6.9 × 108 mol/a from SO2 flux, and 2.1 × 108 and 1.3 × 109 mol/a from CO2 fluxes calculated from 3He and SO2, respectively. These flux results are higher than previous estimates for Central America, reflecting the high sediment-derived volatile contribution and the high nitrogen content of geothermal and volcanic gases in Nicaragua. The fluxes are also similar to but higher than estimated hemipelagic nitrogen inputs at the trench, suggesting addition of N from altered oceanic basement is needed to satisfy these flux estimates. The similarity of the calculated input of N via the trench to our calculated outputs suggests that little or none of the subducted nitrogen is being recycled into the deeper mantle, and that it is, instead, returned to the surface via arc volcanism.  相似文献   

14.
Analyses of co-existing silicate melt and fluid inclusions, entrapped in quartz crystals in volatile saturated magmatic systems, allowed direct quantitative determination of fluid/melt partition coefficients. Investigations of various granitic systems (peralkaline to peraluminous in composition, log fO2 = NNO−1.7 to NNO+4.5) exsolving fluids with various chlorinities (1-14 mol/kg) allowed us to assess the effect of these variables on the fluid/melt partition coefficients (D). Partition coefficients for Pb, Zn, Ag and Fe show a nearly linear increase with the chlorinity of these fluid (DPb ∼ 6 ∗ mCl, DZn ∼ 8 ∗ mCl, DAg ∼ 4 ∗ mCl, DFe ∼ 1.4 ∗ mCl, where mCl is the molinity of Cl). This suggests that these metals are dissolved primarily as Cl-complexes and neither oxygen fugacity nor the composition of the melt affects significantly their fluid/melt partitioning. By contrast, partition coefficients for Mo, B, As, Sb and Bi are highest in low salinity (1-2 mol/kg Cl) fluids with maximum values of DMo ∼ 20, DB ∼ 15, DAs ∼ 13, DSb ∼ 8, DBi ∼ 15 indicating dissolution as non-chloride (e.g., hydroxy) complexes. Fluid/melt partition coefficients of copper are highly variable, but highest between vapor like fluids and silicate melt (DCu ? 2700), indicating an important role for ligands other than Cl. Partition coefficients for W generally increase with increasing chlorinity, but are exceptionally low in some of the studied brines which may indicate an effect of other parameters. Fluid/melt partition coefficients of Sn show a high variability but likely increase with the chlorinity of the fluid (DSn = 0.3-42, DW = 0.8-60), and decrease with decreasing oxygen fugacity or melt peraluminosity.  相似文献   

15.
Strontium-90 is a beta emitting radionuclide produced during nuclear fission, and is a problem contaminant at many nuclear facilities. Transport of 90Sr in groundwaters is primarily controlled by sorption reactions with aquifer sediments. The extent of sorption is controlled by the geochemistry of the groundwater and sediment mineralogy. Here, batch sorption experiments were used to examine the sorption behaviour of 90Sr in sediment–water systems representative of the UK Sellafield nuclear site based on groundwater and contaminant fluid compositions. In experiments with low ionic strength groundwaters (<0.01 mol L−1), pH variation is the main control on sorption. The sorption edge for 90Sr was observed between pH 4 and 6 with maximum sorption occurring (Kd ∼ 103 L kg−1) at pH 6–8. At ionic strengths above 10 mmol L−1, and at pH values between 6 and 8, cation exchange processes reduced 90Sr uptake to the sediment. This exchange process explains the lower 90Sr sorption (Kd ∼ 40 L kg−1) in the presence of artificial Magnox tank liquor (IS = 29 mmol L−1). Strontium K-edge EXAFS spectra collected from sediments incubated with Sr2+ in either HCO3-buffered groundwater or artificial Magnox tank liquor, revealed a coordination environment of ∼9 O atoms at 2.58–2.61 Å after 10 days. This is equivalent to the Sr2+ hydration sphere for the aqueous ion and indicates that Sr occurs primarily in outer sphere sorption complexes. No change was observed in the Sr sorption environment with EXAFS analysis after 365 days incubation. Sequential extractions performed on sediments after 365 days also found that ∼80% of solid associated 90Sr was exchangeable with 1 M MgCl2 in all experiments. These results suggest that over long periods, 90Sr in contaminated sediments will remain primarily in weakly bound surface complexes. Therefore, if groundwater ionic strength increases (e.g. by saline intrusion related to sea level rise or by design during site remediation) then substantial remobilisation of 90Sr is to be expected.  相似文献   

16.
A synthetic composition representing the Yamato 980459 martian basalt (shergottite) has been used to carry out phase relation, and rare earth element (REE) olivine and pyroxene partitioning experiments. Yamato 980459 is a sample of primitive basalt derived from a reduced end-member among martian mantle sources. Experiments carried out between 1-2 GPa and 1350-1650 °C simulate the estimated pressure-temperature conditions of basaltic melt generation in the martian mantle. Olivine-melt and orthopyroxene-melt partition coefficients for La, Nd, Sm, Eu, Gd and Yb (DREE values) were determined by LA-ICPMS, and are similar to the published values for terrestrial basaltic systems. We have not detected significant variation in D-values with pressure over the range investigated, and by comparison with previous studies carried out at lower pressure.We apply the experimentally obtained olivine-melt and orthopyroxene-melt DREE values to fractional crystallization and partial melting models to develop a three-stage geochemical model for the evolution of martian meteorites. In our model we propose two ancient (∼4.535 Ga) sources: the Nakhlite Source, located in the shallow mantle, and the Deep Mantle Source, located close to the martian core-mantle boundary. These two sources evolved distinctly on the ε143Nd evolution curve due to their different Sm/Nd ratios. By partially melting the Nakhlite Source at ∼1.3 Ga, we are able to produce a slightly depleted residue (Nakhlite Residue). The Nakhlite Residue is left undisturbed until ∼500 Ma, at which point the depleted Deep Mantle Source is brought up by a plume mechanism carrying with it high heat flow, melts and isotopic signatures of the deep mantle (e.g., ε182W, ε142Nd, etc.). The plume-derived Deep Mantle Source combines with the Nakhlite Residue producing a mixture that becomes a mantle source (herein referred to as “the Y98 source”) for Yamato 980459 and the other depleted shergottites with the characteristic range of Sm/Nd ratios of these meteorites. The same hot plume provides a heat source for the formation of enriched and intermediate shergottites. Our model reproduces the REE patterns of nakhlites and depleted shergottites and can explain high ε143Nd in depleted shergottites. Furthermore, the model results can be used to interpret whole rock Rb-Sr and Sm-Nd ages of shergottites.  相似文献   

17.
Contaminated fluvial sediments represent both temporary sinks for river-borne pollutants and potential sources in case of natural and/or anthropogenic resuspension. Reservoir lakes play a very important role in sediment dynamics of watersheds and may offer great opportunities to study historical records of river-borne particles and associated elements transported in the past. The fate and potential environmental impact of Hg depends on its abundance, its carrier phases and its chemical speciation. Historical Hg records and solid state Hg speciation were compared in sediments from two contrasting reservoirs of the Lot River (France) upstream and downstream from a major polymetallic pollution (e.g. Cd, Zn) source. Natural (geochemical background) and anthropogenic Hg concentrations and their relationships with predominant carrier phases were determined. The results reveal important historical Hg contamination (up to 35 mg kg−1) of the downstream sediment, reflecting the historical evolution of industrial activity at the point source, i.e. former coal mining, Zn ore treatment and post-industrial remediation work. Single chemical extractions (ascorbate, H2O2, KOH) suggest that at both sites most (∼75%) of the Hg is bound to organic and/or reactive sulphide phases. Organo-chelated (KOH-extracted) Hg, representing an important fraction in the uncontaminated sediment, shows similar concentrations (∼0.02 mg kg−1) at both sites and may be mainly attributed to natural inputs and/or processes. Although, total Hg concentrations in recent surface sediments at both sites are still very different, similar mono-methylmercury concentrations (up to 4 μg kg−1) and vertical distributions were observed, suggesting comparable methylation-demethylation processes. High mono-methylmercury concentrations (4–15 μg kg−1) in 10–40 a-old, sulphide-rich, contaminated sediment suggest long-term persistence of mono-methylmercury. Beyond historical records of total concentrations, the studied reservoir sediments provided new insights in solid state speciation and carrier phases of natural and anthropogenic Hg. In case of sediment resuspension, the major part of the Hg historically stored in the Lot River sediments will be accessible to biogeochemical recycling in the downstream fluvial-estuarine environment.  相似文献   

18.
Superliquidus metal-silicate partitioning was investigated for a number of moderately siderophile (Mo, As, Ge, W, P, Ni, Co), slightly siderophile (Zn, Ga, Mn, V, Cr) and refractory lithophile (Nb, Ta) elements. To provide independent constrains on the effects of temperature, oxygen fugacity and silicate melt composition, isobaric (3 GPa) experiments were conducted in piston cylinder apparatus at temperature between 1600 and 2600 °C, relative oxygen fugacities of IW−1.5 to IW−3.5, and for silicate melt compositions ranging from basalt to peridotite. The effect of pressure was investigated through a combination of piston cylinder and multi-anvil isothermal experiments between 0.5 and 18 GPa at 1900 °C. Oxidation states of siderophile elements in the silicate melt as well as effect of carbon saturation on partitioning are also derived from these results. For some elements (e.g. Ga, Ge, W, V, Zn) the observed temperature dependence does not define trends parallel to those modeled using metal-metal oxide free energy data. We correct partitioning data for solute interactions in the metallic liquid and provide a parameterization utilized in extrapolating these results to the P-T-X conditions proposed by various core formation models. A single-stage core formation model reproduces the mantle abundances of several siderophile elements (Ni, Co, Cr, Mn, Mo, W, Zn) for core-mantle equilibration at pressures from 32 to 42 GPa along the solidus of a deep peridotitic magma ocean (∼3000 K for this pressure range) and oxygen fugacities relevant to the FeO content of the present-day mantle. However, these P-T-fO2 conditions cannot produce the observed concentrations of Ga, Ge, V, Nb, As and P. For more reducing conditions, the P-T solution domain for single stage core formation occurs at subsolidus conditions and still cannot account for the abundances of Ge, Nb and P. Continuous core formation at the base of a magma ocean at P-T conditions constrained by the peridotite liquidus and fixed fO2 yields concentrations matching observed values for Ni, Co, Cr, Zn, Mn and W but underestimates the core/mantle partitioning observed for other elements, notably V, which can be reconciled if accretion began under reducing conditions with progressive oxidation to fO2 conditions consistent with the current concentration of FeO in the mantle as proposed by Wade and Wood (2005). However, neither oxygen fugacity path is capable of accounting for the depletions of Ga and Ge in the Earth’s mantle. To better understand core formation, we need further tests integrating the currently poorly-known effects of light elements and more complex conditions of accretion and differentiation such as giant impacts and incomplete equilibration.  相似文献   

19.
Lavas from the island of São Miguel, Azores Archipelago have long been known to display large radiogenic isotopic variability, that ranges from “depleted” isotopic signatures (e.g. high εNd ∼ +5) in the west, typical of many ocean island basalts, to more “enriched” compositions (e.g. low εNd ∼ +1) in the east. Here, we further characterise the geochemistry of lavas from this remarkable locality, focussing on the nature and origin of the enriched source. Our new isotope data define a striking, linear array in Nd and Hf isotope space that points towards an unusual, enriched composition below the mantle array. This distinctive Hf-Nd isotope signature is associated with elevated values of all three radiogenic Pb isotope ratios. Although the enriched component has certain geochemical similarities to both terrigenous sediments and some samples of the continental mantle lithosphere, such comparisons do not stand closer examination. In the absence of a clear, modern analogue we explore the isotope evolution of some simple, model melt compositions to investigate plausible means of producing an appropriate enriched component. Nd-Hf isotope characteristics provide the tightest constraints and can be reproduced by an ancient (∼3 Ga), modest-degree melt (∼2%) from a garnet peridotite source. Currently, modest-degree melts from garnet-bearing sources are found forming some major oceanic islands. Subduction, isolation and later mixing of small amounts (<5%) of such basaltic material with more ubiquitous ambient mantle can account for the isotopic characteristics of the enriched São Miguel source. Yet the incompatible element ratios of the enriched São Miguel lavas do not show “recycled” signatures of near-surface alteration nor subduction zone dehydration. Thus, we infer that the enriched component was originally under-plated basalt, intruded into oceanic mantle lithosphere rather than forming the island edifice itself. Since the extreme isotope compositions of São Miguel reflect unextraordinary, albeit ancient, magmatic fractionation, the general rarity of such signatures indicates the efficiency of mantle processes in homogenising or hiding similar sources.  相似文献   

20.
The distribution of neodymium isotopes in Arctic Ocean basins   总被引：1，自引：0，他引：1  
Nd concentration and isotope data have been obtained for the Canada, Amundsen, and Makarov Basins of the Arctic Ocean. A pattern of high Nd concentrations (up to 58 pM) at shallow depths is seen throughout the Arctic, and is distinct from that generally seen in other oceans where surface waters are relatively depleted. A range of isotopic variations across the Arctic and within individual depth profiles reflects the different sources of waters. The dominant source of water, and so Nd, is the Atlantic Ocean, with lesser contributions from the Pacific and Arctic Rivers. Radiogenic isotope Nd signatures (up to εNd = −6.5) can be traced in Pacific water flowing into the Canada Basin. Waters from rivers draining older terrains provide very unradiogenic Nd (down to εNd = −14.2) that can be traced in surface waters across much of the Eurasian Basin. A distinct feature of the Arctic is the general influence of the shelves on the Nd concentrations of waters flowing into the basins, either from the Pacific across the Chukchi Sea, or from across the extensive Siberian shelves. Water-shelf interaction results in an increase in Nd concentration without significant changes in salinity in essentially all waters in the Arctic, through processes that are not yet well understood. In estuarine regions other processes modify the Nd signal of freshwater components supplied into the Arctic Basin, and possibly also contribute to sedimentary Nd that may be subsequently involved in sediment-water interactions. Mixing relationships indicate that in estuaries, Nd is removed from major river waters to different degrees. Deep waters in the Arctic are higher in Nd than the inflowing Atlantic waters, apparently through enrichments of waters on the shelves that are involved in ventilating the deep basins. These enrichments generally have not resulted in major shifts in the isotopic compositions of the deep waters in the Makarov Basin (εNd ∼ −10.5), but have created distinctive Nd isotope signatures that were found near the margin of the Canada Basin (with εNd ∼ −9.0). The deep waters of the Amundsen Basin are also distinct from the Atlantic waters (with εNd = −12.3), indicating that there has been limited inflow from the adjacent Makarov Basin through the Lomonosov Ridge.  相似文献   

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