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1.
Strontium isotopes and other geochemical signatures are used to determine the relationships between CO2-rich thermal (Chaves: 76 °C) and mineral (Vilarelho da Raia, Vidago and Pedras Salgadas: 17 °C) waters discharging along one of the major NNE–SSW trending faults in the northern part of mainland Portugal. The regional geology consists of Hercynian granites (syn-tectonic-310 Ma and post-tectonic-290 Ma) intruding Silurian metasediments (quartzites, phyllites and carbonaceous slates). Thermal and mineral waters have 87Sr/86Sr isotopic ratios between 0.716713 and 0.728035. 87Sr/86Sr vs. 1/Sr define three end-members (Vilarelho da Raia/Chaves, Vidago and Pedras Salgadas thermal and mineral waters) trending from rainfall composition towards that of the CO2-rich thermal and mineral waters, indicating different underground flow paths. Local granitic rocks have 87Sr/86Sr ratios of 0.735697–0.789683. There is no indication that equilibrium was reached between the CO2-rich thermal and mineral waters and the granitic rocks. The mean 87Sr/86Sr ratio of the thermal and mineral waters (0.722419) is similar to the Sr isotopic ratios of the plagioclases of the granitic rocks (0.71261–0.72087). The spatial distribution of Sr isotope and geochemical signatures of waters and the host rocks suggests that the thermal and mineral waters circulate in similar but not the same hydrogeological system. Results from this study could be used to evaluate the applicability of this isotope approach in other hydrogeologic investigations.  相似文献   

2.
The Nandong Underground River System (NURS) is located in a typical karst area dominated by agriculture in SE Yunnan Province, China. Groundwater plays an important role in the social and economical development in the area. The effects of human activities (agriculture and sewage effluents) on the Sr isotope geochemistry were investigated in the NURS. Seventy-two representative groundwater samples, which were collected from different aquifers (calcite and dolomite), under varying land-use types, both in summer and winter, showed significant spatial differences and slight seasonal variations in Sr concentrations and 87Sr/86Sr ratios. Agricultural fertilizers and sewage effluents significantly modified the natural 87Sr/86Sr ratios signature of groundwater that was otherwise dominated by water-rock interaction. Three major sources of Sr could be distinguished by 87Sr/86Sr ratios and Sr concentrations in karst groundwater. Two sources of Sr are the Triassic calcite and dolomite aquifers, where waters have low Sr concentrations (0.1-0.2 mg/L) and low 87Sr/86Sr ratios (0.7075-0.7080 and 0.7080-0.7100, respectively); the third source is anthropogenic Sr from agricultural fertilizers and sewage effluents with waters affected having radiogenic 87Sr/86Sr ratios (0.7080-0.8352 for agricultural fertilizers and 0.7080-0.7200 for sewage effluents, respectively), with higher Sr concentrations (0.24-0.51 mg/L). Due to the overlapping 87Sr/86Sr ratios, it is difficult to distinguish the sources of Sr in groundwater samples contaminated by agricultural fertilizers or sewage effluents based only on their 87Sr/86Sr ratios. However, 87Sr/86Sr ratios do provide key information for natural and anthropogenic sources in karst groundwater.  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 present strontium (Sr) isotope ratios that, unlike traditional 87Sr/86Sr data, are not normalized to a fixed 88Sr/86Sr ratio of 8.375209 (defined as δ88/86Sr = 0 relative to NIST SRM 987). Instead, we correct for isotope fractionation during mass spectrometry with a 87Sr-84Sr double spike. This technique yields two independent ratios for 87Sr/86Sr and 88Sr/86Sr that are reported as (87Sr/86Sr∗) and (δ88/86Sr), respectively. The difference between the traditional radiogenic (87Sr/86Sr normalized to 88Sr/86Sr = 8.375209) and the new 87Sr/86Sr∗ values reflect natural mass-dependent isotope fractionation. In order to constrain glacial/interglacial changes in the marine Sr budget we compare the isotope composition of modern seawater ((87Sr/86Sr∗, δ88/86Sr)Seawater) and modern marine biogenic carbonates ((87Sr/86Sr∗, δ88/86Sr)Carbonates) with the corresponding values of river waters ((87Sr/86Sr∗, δ88/86Sr)River) and hydrothermal solutions ((87Sr/86Sr∗, δ88/86Sr)HydEnd) in a triple isotope plot. The measured (87Sr/86Sr∗, δ88/86Sr)River values of selected rivers that together account for ∼18% of the global Sr discharge yield a Sr flux-weighted mean of (0.7114(8), 0.315(8)‰). The average (87Sr/86Sr∗, δ88/86Sr)HydEnd values for hydrothermal solutions from the Atlantic Ocean are (0.7045(5), 0.27(3)‰). In contrast, the (87Sr/86Sr∗, δ88/86Sr)Carbonates values representing the marine Sr output are (0.70926(2), 0.21(2)‰). We estimate the modern Sr isotope composition of the sources at (0.7106(8), 0.310(8)‰). The difference between the estimated (87Sr/86Sr∗, δ88/86Sr)input and (87Sr/86Sr∗, δ88/86Sr)output values reflects isotope disequilibrium with respect to Sr inputs and outputs. In contrast to the modern ocean, isotope equilibrium between inputs and outputs during the last glacial maximum (10-30 ka before present) can be explained by invoking three times higher Sr inputs from a uniquely “glacial” source: weathering of shelf carbonates exposed at low sea levels. Our data are also consistent with the “weathering peak” hypothesis that invokes enhanced Sr inputs resulting from weathering of post-glacial exposure of abundant fine-grained material.  相似文献   

5.
Late Pleistocene glaciers around Darhad Basin advanced to near their maximum positions at least three times, twice during the Zyrianka glaciation (at ∼ 17-19 ka and ∼ 35-53 ka), and at least once earlier. The Zyrianka glaciers were smaller than their predecessors, but the equilibrium-line altitude (ELA) difference was < 75 m. End moraines of the Zyrianka glaciers were ∼ 1600 m asl; ELAs were 2100-2400 m asl. 14C and luminescence dating of lake sediments confirm the existence of paleolake highstands in Darhad Basin before ∼ 35 ka. Geologic evidence and 10Be cosmic-ray exposure dating of drift suggests that at ∼ 17-19 ka the basin was filled at least briefly by a glacier-dammed lake ∼ 140 m deep. However, lake sediments from that time have not yet been recognized in the region. A shallower paleolake briefly occupied the basin at ∼ 11 ka, but between ∼ 11 and 17 ka and after ∼ 10 ka the basin was probably largely dry. The timing of maximum glacier advances in Darhad appears to be approximately synchronous across northern Mongolia, but different from Siberia and western Central Asia, supporting the inference that paleoclimate in Central Asia differed among regions.  相似文献   

6.
The determination of accurate Sr isotope ratios in calcium phosphate matrices by laser ablation multi-collector ICP-MS is demonstrated as possible even with low Sr concentration archaeological material. Multiple on-line interference correction routines for doubly-charged REE, Ca dimers and Rb with additional calibration against TIMS-characterised materials are required to achieve this. The calibration strategy proposed uses both inorganic and biogenic apatite matrices to monitor and correct for a 40Ca-31P-16O polyatomic present at levels of 0.3-1% of the non-oxide peak, which interferes on 87Sr causing inaccuracies of 0.03-0.4% in the 87Sr/86Sr isotope ratio. The possibility also exists for synthetic materials to be used in this calibration. After correction for interferences total combined uncertainties of 0.04-0.15% (2SD) are achieved for analyses of 13-24 μg of archaeological tooth enamel with Sr concentrations of ca. 100-500 ppm using MC-ICP-MS. In particular, for samples containing >300 ppm Sr, total uncertainties of ∼0.05% are possible utilising 7-12 ng Sr. Data quality is monitored by determination of 84Sr/86Sr ratios.When applied to an archaeological cattle tooth this approach shows Sr-isotope variations along the length of the tooth in agreement with independent TIMS data. The 40Ca-31P-16O polyatomic interference is the root cause of the bias at mass 87 during laser ablation ICP-MS analysis of inorganic and biogenic calcium phosphate (apatite) matrices. This results in inaccurate 87Sr/86Sr ratios even after correction of Ca dimers and doubly charged rare earth elements. This interference is essentially constant at specific ablation conditions and therefore the effect on 87Sr/86Sr data varies in proportion to changes in the Sr concentration of the ablated material. Complete elimination of this interference is unlikely through normal analytical mechanisms and therefore represents a limitation on the achievable accuracy of LA-(MC-)ICP-MS 87Sr/86Sr data without rigorous calibration to known reference materials.  相似文献   

7.
柴达木察尔汗贝壳堤剖面Sr同位素及其环境意义   总被引:6,自引:0,他引:6  
根据对柴达木盆地察尔汗古湖贝壳堤剖面酸不溶组分和酸溶组分的提取及其87Sr/86Sr的测定,结合沉积物中Rb/Sr的变化,指出Sr同位素组成特征可有效指示源区化学风化和沉积区古环境变化;依据酸溶组分中盐度指标Sr/Ca, Sr/Ba值与Sr同位素组成曲线的对比分析,揭示酸溶组分Sr同位素可以较好的指示水体形成时的盐度。通过分析贝壳堤剖面化学风化和部分盐度变化过程,探讨了研究区晚更新世39.6~ 17.1 ka BP(未经校正的AMS 14C测年结果,全文同)湖泊高湖面的演化历史。  相似文献   

8.
The spatial and temporal changes in hydrology and pore water elemental and 87Sr/86Sr compositions are used to determine contemporary weathering rates in a 65- to 226-kyr-old soil chronosequence formed from granitic sediments deposited on marine terraces along coastal California. Soil moisture, tension and saturation exhibit large seasonal variations in shallow soils in response to a Mediterranean climate. These climate effects are dampened in underlying argillic horizons that progressively developed in older soils, and reached steady-state conditions in unsaturated horizons extending to depths in excess of 15 m. Hydraulic fluxes (qh), based on Cl mass balances, vary from 0.06 to 0.22 m yr−1, resulting in fluid residence times in the terraces of 10-24 yrs.As expected for a coastal environment, the order of cation abundances in soil pore waters is comparable to sea water, i.e., Na > Mg > Ca > K > Sr, while the anion sequence Cl > NO3 > HCO3 > SO4 reflects modifying effects of nutrient cycling in the grassland vegetation. Net Cl-corrected solute Na, K and Si increase with depth, denoting inputs from feldspar weathering. Solute 87Sr/86Sr ratios exhibit progressive mixing of sea water-dominated precipitation with inputs from less radiogenic plagioclase. While net Sr and Ca concentrations are anomalously high in shallow soils due to biological cycling, they decline with depth to low and/or negative net concentrations. Ca/Mg, Sr/Mg and 87Sr/86Sr solute and exchange ratios are similar in all the terraces, denoting active exchange equilibration with selectivities close to unity for both detrital smectite and secondary kaolinite. Large differences in the magnitudes of the pore waters and exchange reservoirs result in short-term buffering of the solute Ca, Sr, and Mg. Such buffering over geologic time scales can not be sustained due to declining inputs from residual plagioclase and smectite, implying periodic resetting of the exchange reservoir such as by past vegetational changes and/or climate.Pore waters approach thermodynamic saturation with respect to albite at depth in the younger terraces, indicating that weathering rates ultimately become transport-limited and dependent on hydrologic flux. Contemporary rates Rsolute are estimated from linear Na and Si pore weathering gradients bsolute such that
  相似文献   

9.
Forty-one metric tons of the mineral wollastonite (CaSiO3) was applied to an 11.8 hectare watershed at the Hubbard Brook Experimental Forest (HBEF; White Mountains, New Hampshire, USA) with the goal of restoring the Ca estimated to have been depleted from the soil exchange complex by acid deposition. This experiment provided an opportunity to gain qualitative information on whole watershed hydrologic flow paths by studying the response of stream water chemistry to the addition of Ca. Because the Ca/Sr and 87Sr/86Sr ratios of wollastonite strongly contrast that of other Ca sources in the watershed, the wollastonite-derived Ca can be identified and its amount estimated in various ecosystem components. Stream water chemistry at the HBEF varies seasonally due to shifts in the proportion of base flow and interflow. Prior to the wollastonite application, seasonal variations in 87Sr/86Sr ratios indicated that 87Sr/86Sr was higher during base flow than interflow, due largely to greater amounts of biotite weathering along deeper flow paths. After the application, Ca/Sr and 87Sr/86Sr changed markedly as the high Ca/Sr and low 87Sr/86Sr wollastonite dissolved and mixed with stream water. The Ca addition provided information on the response times of various flow paths and ion exchange processes to Ca addition in this small upland watershed. During the first year after the addition, wollastonite applied to the near stream zone dissolved and was partially immobilized by cation exchange sites in the hyporheic zone. In the second and third years after the addition we infer that much of this Ca and Sr was subsequently desorbed from the hyporheic zone and was exported from the watershed in stream flow. In the fourth through ninth years after the addition, Ca and Sr from wollastonite that had dissolved in upland soils was transported to the stream by interflow during wet periods when the ground water table was elevated. Between years three and nine the minimum annual Ca/Sr ratio (in late summer base flow) increased, providing evidence that Ca and Sr had increasingly infiltrated to the deepest flow paths. Strong seasonal variations in Ca/Sr and 87Sr/86Sr ratios of stream water resulted from the wollastonite addition to upland forest soils, and these ratios have become sensitive to changing flow paths during the annual cycle. Most notably, high flow events now produce large excursions in stream geochemistry toward the high Ca/Sr and low 87Sr/86Sr ratios of wollastonite. Nine years after the application we estimate that ∼360 kg of Ca from wollastonite has been exported from the watershed in stream flow. The rate of export of Ca from wollastonite dissolution has stabilized at about 11 kg of Ca per year, which accounts for ∼30% of the dissolved Ca in the stream water. Given that 19 metric tons of Ca were applied to the watershed, and assuming this current rate of loss, it should take over 1000 years for this added Ca to be transported from the watershed.  相似文献   

10.
We present Os and Sr isotopes and Mg, Os, and Sr concentrations for ridge-crest high-temperature and diffuse hydrothermal fluids, plume fluids and ridge-flank warm spring fluids from the Juan de Fuca Ridge. The data are used to evaluate the extent to which (1) the high- and low-temperature hydrothermal alteration of mid-ocean ridge basalts (MORBs) provides Os to the deep oceans, and (2) hydrothermal contributions of non-radiogenic Os and Sr to the oceans are coupled. The Os and Sr isotopic ratios of the high-temperature fluids (265-353 °C) are dominated by basalts (187Os/188Os = 0.2; 87Sr/86Sr = 0.704) but the concentrations of these elements are buffered approximately at their seawater values. The 187Os/188Os of the hydrothermal plume fluids collected ∼1 m above the orifice of Hulk vent is close to the seawater value (=1.05). The low-temperature diffuse fluids (10-40 °C) associated with ridge-crest high-temperature hydrothermal systems on average have [Os] = 31 fmol kg−1, 187Os/188Os = 0.9 and [Sr] = 86 μmol kg−1, 87Sr/86Sr = 0.709. They appear to result from mixing of a high-temperature fluid and a seawater component. The ridge-flank warm spring fluids (10-62 °C) on average yield [Os] = 22 fmol kg−1, 187Os/188Os = 0.8 and [Sr] = 115 μmol kg−1, 87Sr/86Sr = 0.708. The data are consistent with isotopic exchange of Os and Sr between basalt and circulating seawater during low-temperature hydrothermal alteration. The average Sr concentration in these fluids appears to be similar to seawater and consistent with previous studies. In comparison, the average Os concentration is less than seawater by more than a factor of two. If these data are representative they indicate that low-temperature alteration of MORB does not provide adequate non-radiogenic Os and that another source of mantle Os to the oceans must be investigated. At present, the magnitude of non-radiogenic Sr contribution via low-temperature seawater alteration is not well constrained. If non-radiogenic Sr to the oceans is predominantly from the alteration of MORB, our data suggest that there must be a different source of non-radiogenic Os and that the Os and Sr isotope systems in the oceans are decoupled.  相似文献   

11.
In this paper Sr isotope signatures are reported for 192 surface water (lakes/ponds and rivers/creeks) samples from within Denmark and an isotope distribution map is presented that may serve as a base for provenance applications, including archaeological migration studies, ground water - surface water - seawater interaction/contamination monitoring, and potentially for agricultural applications, including cases of authenticity proof for particular food products. The Sr isotopic compositions of surface waters range from 87Sr/86Sr = 0.7078 to 0.7125 (average 0.7096 ± 0.0016; 2σ). This average value lies above the range of 87Sr/86Sr values between 0.7078 and 0.7082 expected from Late Cretaceous to Early Tertiary (Oligocene) limestones which form the dominant bedrock type in a NW-SE trending belt in Denmark. The elevated 87Sr/86Sr signatures >∼0.7095 are explained by additions to the surface waters of radiogenic Sr predominantly derived from the near-surface weathering and wash-out of Quarternary glaciogenic tills and soils deposited and formed during and after the last two ice age stages (Saale and Weichsel). The Sr isotopic compositions and concentrations of the surface waters can, therefore, best be modeled by a two-component mixing involving carbonaceous bedrock and glaciogenic cover sediments as the two predominant Sr sources. A feasibility study for using Sr isotopic compositions of surface waters as a proxy for bio-available Sr signatures was conducted in a representative test area on Zealand (Land of Legends, Lejre) where there is no use and application of commercial fertilizers. It is demonstrated that the Sr isotopic signatures of lake waters from within this area are slightly higher (but statistically still indistinguishable) from the average value defined by snail shells and soil leachates considered to characterize the true bio-available Sr. In combination with results from other studies, this is interpreted to reflect the wash-out of Sr with a higher 87Sr/86Sr signature released by weathering in the topsoils into the saturated water tables, a component which is consequently not readily transferred into the shallow-rooting plants and into small herbivores feeding on them. Since drinking water is a likely important source of Sr uptake of humans and larger animals, the contention is that a surface water isotopic composition can potentially characterize the bio-available component relevant for human and carnivorous large animals. Spline functions and ordinary linear kriging were used for modeling the geographic distribution of bio-available Sr isotopes over territorial Denmark. As expected, based on the two-source mixing scenario, the water 87Sr/86Sr ratio contour maps (with some notable exceptions) neither mirror the pre-Quarternary bedrock geology nor a (Pleistocene) soil-type distribution map of Denmark.As a conservative suggestion, the use of the average 87Sr/86Sr ratio of 0.7096 ± 0.0015 (2σ) is recommended as an average for bio-available Sr from within Denmark (Bornholm excluded) for human and larger animals and as a confidence band for distinguishing “local” from “non-local” signatures in archaeological provenance studies. The study also reveals that the average 87Sr/86Sr ratio of ∼0.7088 defined from soil extracts and small herbivores lies approximately 0.15% lower than that defined by the surface waters. The authors recommend using this lower value as a “local”-“non-local” discriminator for food and plant authenticity control in agricultural applications.  相似文献   

12.
《Applied Geochemistry》2005,20(8):1571-1586
87Sr/86Sr ratio variations were analyzed in rainfall, shallow ground water and base flow collected from 4 Piedmont streams within the Middle Oconee River basin in northeastern Georgia during the period between March, 2003 and March, 2004. They Sr isotope ratio analyses were accompanied by measurements of stream discharge, rainfall, stable O isotope ratios and major ion and 3H concentrations. The average Sr ion concentration and 87Sr/86Sr ratio for the terminal stream basin (the Middle Oconee River) were 23.6 μg/L and 0.7172, respectively. The average 87Sr/86Sr ratios of the rainwater and shallow ground water were below 0.7125, indicating that most of the Sr in this stream water is input by weathering reactions in deeper ground water, rather than by ion exchange in shallow soil horizons. This is consistent with the higher alkalinity concentrations (∼23–47 mg/L) and specific conductance values (60–113 μS/cm) that characterize stream base flow. Piedmont streams are characterized by lower concentrations of Sr and higher 87Sr/86Sr ratios than average global stream flow.Base flow rates decreased by a factor of 2–3 during the summer months and this is accompanied by increased alkalinity concentrations. 87Sr/86Sr ratios, however, were temporally invariant for a given stream basin and were independent of season, antecedent rainfall, and discharge. 87Sr/86Sr ratios were unique for each of the 4 basins and a general trend toward higher ratios with increasing basin area was apparent. The inferred contribution from minerals with high Rb contents such as K feldspar and muscovite may have resulted from the greater integration of flow from mineralogically diverse pathways afforded by a larger basin area. The basin specificity and temporal or seasonal invariability make 87Sr/86Sr ratios an invaluable hydrological tracer that can be readily employed in mass balance studies of stream flow within the Piedmont Province.  相似文献   

13.
We used analyses of the strontium isotope (87Sr/86Sr) ratios of tooth enamel to reconstruct the migration patterns of fossil mammals collected along the Aucilla River in northern Florida. Specimens date to the late-glacial period and before the last glacial maximum (pre-LGM). Deer and tapir displayed low 87Sr/86Sr ratios that were similar to the ratios of Florida environments, which suggest that these taxa did not migrate long distance outside of the Florida region. Mastodons, mammoths, and equids all displayed a wide range of 87Sr/86Sr ratios. Some individuals in each taxon displayed low 87Sr/86Sr ratios that suggest they ranged locally, while other animals had high 87Sr/86Sr ratios that suggest they migrated long distances (> 150 km) outside of the Florida region. Mastodons were the only taxa from this region that provided enough well-dated specimens to compare changes in migration patterns over time. Pre-LGM mastodons displayed significantly lower 87Sr/86Sr ratios than late-glacial mastodons, which suggests that late-glacial mastodons from Florida migrated longer distances than their earlier counterparts. This change in movement patterns reflects temporal changes in regional vegetation patterns.  相似文献   

14.
Thermal water samples and related young and fossil mineralization from a geothermal system at the northern margin of the Upper Rhine Graben have been investigated by combining hydrochemistry with stable and Sr isotope geochemistry. Actively discharging thermal springs and mineralization are present in a structural zone that extends over at least 60 km along strike, with two of the main centers of hydrothermal activity being Wiesbaden and Bad Nauheim. This setting provides the rare opportunity to link the chemistry and isotopic signatures of modern thermal waters directly with fossil mineralization dating back to at least 500–800 ka. The fossil thermal spring mineralization can be classified into two major types: barite-(pyrite) fracture filling associated with laterally-extensive silicification; and barite, goethite and silica impregnation mineralization in Tertiary sediments. Additionally, carbonatic sinters occur around active springs. Strontium isotope and trace element data suggest that mixing of a hot (>100 °C), deep-sourced thermal water with cooler groundwater from shallow aquifers is responsible for present-day thermal spring discharge and fossil mineralization. The correlation between both Sr and S isotope ratios and the elevation of the barite mineralization relative to the present-day water table in Wiesbaden is explained by mixing of deep-sourced thermal water having high 87Sr/86Sr and low δ34S with shallow groundwater of lower 87Sr/86Sr and higher δ34S. The Sr isotope data demonstrate that the hot thermal waters originate from an aquifer in the Variscan crystalline basement at depths of 3–5 km. The S isotope data show that impregnation-type mineralization is strongly influenced by mixing with SO4 that has high δ34S values. The fracture style mineralization formed by cooling of the thermal waters, whereas impregnation-type mineralization precipitated by mixing with SO4-rich groundwater percolating through the sediments.  相似文献   

15.
U-series disequilibria measured in waters and rocks from a chalk aquifer in France have been used as an analog for long-term radionuclide migration. Drill core samples from a range of depths in the vadose zone and in the saturated zone, as well as groundwater samples were analyzed for 238U, 234U, 232Th and 230Th to determine transport mechanisms at the water/rock interface and to quantify parameters controlling the migration of radionuclides. Isotope measurements in rocks were done by TIMS, whereas (234U/238U) and (230Th/232Th) activity ratios in water samples were measured by multi-collector-ICP-MS. Both depletion and enrichment in 234U relative to 238U were observed in carbonate rock samples resulting from chemical weathering in the unsaturated zone and calcite precipitation in the zone of water-table oscillation, respectively. The correlation between (230Th/232Th) activity ratios and 87Sr/86Sr ratios found in the chalk samples indicates that thorium is mainly contained in a minor silicate phase whose abundance is variable in chalk samples. Water samples are all characterized by (234U/238U) > 1 resulting from α-recoil effect of 234Th. Groundwaters are characterized by a more radiogenic signature in 87Sr/86Sr than the rocks. Moreover, (230Th/232Th) activity ratios in the waters are lower than in the rocks, and increase with distance from the water divide, which suggests that Th transport is controlled by colloids formed during water infiltration in the soil. A 1-D transport model has been developed in order to constrain the U-series nuclide transport considering a transient behavior of radionuclides in the aquifer and a time-dependent composition for the solid phase. This model permits a prediction of the time scale of equilibration of the system, and an estimation of parameters such as weathering rate, distribution coefficients and α-recoil fractions. Retardation factors of 10-35 and from 1 × 104 to 2 × 105 were predicted for U and Th, respectively, and can be used to predict the migration of radionuclides released as contaminants in the environment. At the scale of our watershed (∼32 km2), a characteristic migration time from recharge to riverine discharge of 200-600 yr for U and 0.2-3.7 Myr for Th was obtained.  相似文献   

16.
Dansgaard–Oeschger (D–O) cycles had far-reaching effects on Northern Hemisphere and tropical climate systems during the last glacial period, yet the climatic response to D–O cycles in western North America is controversial, especially prior to 55 ka. We document changes in precipitation along the western slope of the central Sierra Nevada during early Marine Oxygen Isotope Stages (MIS) 3 and 4 (55–67 ka) from a U-series dated speleothem record from McLean's Cave. The timing of our multi-proxy geochemical dataset is coeval with D–O interstadials (15–18) and stadials, including Heinrich Event 6. The McLean's Cave stalagmite indicates warmer and drier conditions during Greenland interstadials (GISs 15–18), signified by elevated δ18O, δ13C, reflectance, and trace element concentrations, and less radiogenic 87Sr/86Sr. Our record extends evidence of a strong linkage between high-latitude warming and reduced precipitation in western North America to early MIS 3 and MIS 4. This record shows that the linkage persists in diverse global climate states, and documents the nature of the climatic response in central California to Heinrich Event 6.  相似文献   

17.
Jin, Z. D., Bickle, M. J., Chapman, H. J., Yu, J., An, Z., Wang, S. & Greaves, M. J. 2010: Ostracod Mg/Sr/Ca and 87Sr/86Sr geochemistry from Tibetan lake sediments: Implications for early to mid‐Pleistocene Indian monsoon and catchment weathering. Boreas, 10.1111/j.1502‐3885.2010.00184.x. ISSN 0300‐9483 Lacustrine sediment serves as a valuable archive for tracing catchment weathering processes associated with past climatic and/or tectonic changes. High‐resolution records of fossil ostracod Mg/Ca, Sr/Ca and 87Sr/86Sr ratios from a lake sediment core from the central Tibetan Plateau reveal a temporal link between lake‐water chemistry and catchment weathering and distinct monsoonal oscillations over the early to mid‐Pleistocene. Between 2.01 and 0.95 Ma, lake‐water chemistry was dominated by a high proportion of carbonate weathering related to variations in the Indian monsoon, resulting in relatively low and constant ostracod 87Sr/86Sr but obvious fluctuations in Mg/Ca, Sr/Ca and δ18O. Across the mid‐Pleistocene transition (MPT), a significant increase in 87Sr/86Sr and frequently fluctuating ratios of ostracod Mg/Ca, Sr/Ca and δ18O are coincident with increases in both Chinese loess grain size and Arabian Sea lithogenic flux. This correlation indicates an increased glaciation and a strong monsoon seasonal contrast over the plateau. The increase in lake‐water 87Sr/86Sr across the MPT highlights a change in catchment weathering patterns, rather than one in climate‐enhanced weathering intensity, with an increased weathering of 87Sr‐rich minerals potentially induced by marked extensive glaciation and strong seasonality in the central plateau.  相似文献   

18.
《Chemical Geology》2007,236(3-4):281-290
Ostracods preserved in late Quaternary sediments of Wallywash Great Pond, a fresh coastal lake in SW Jamaica, record temporal variations in the strontium-isotope composition of lake water. Oxygen-isotope and Sr/Ca ratios in ostracods reveal temporal variations in the lake's hydrology, related to effective precipitation, and in its salinity related to varying marine-saline groundwater input from changes in relative sea level. Evaluation of isotopic and trace-element data indicates that the stratigraphic variations in 87Sr/86Sr ratios during the late Quaternary are best explained by climatically-controlled hydrological changes. During wetter periods, the lake's Sr budget was dominated by springwater input with relatively low 87Sr/86Sr ratio, whereas during drier times reduced springflow, possibly coupled with input of more-radiogenic Sr from other sources, such as sea-spray aerosols and perhaps Saharan dust, led to an increase in the Sr-isotope ratio of the lake water. Despite proximity of the lake to the sea and evidence for slight intrusion of marine saline groundwater in the past, however, the extent of marine input appears to have had limited influence on the lake's Sr-isotope ratios. Whereas the 87Sr/86Sr ratios cannot be used as a palaeosalinity proxy in this particular lake, they do provide valuable information about the mechanisms underlying hydrological change.  相似文献   

19.
Magnesium and strontium isotope signatures were determined during different seasons for the main rivers of the Moselle basin, northeastern France. This small basin is remarkable for its well-constrained and varied lithology on a small distance scale, and this is reflected in river water Sr isotope compositions. Upstream, where the Moselle River drains silicate rocks of the Vosges mountains, waters are characterized by relatively high 87Sr/86Sr ratios (0.7128-0.7174). In contrast, downstream of the city of Epinal where the Moselle River flows through carbonates and evaporites of the Lorraine plateau, 87Sr/86Sr ratios are lower, down to 0.70824.Magnesium in river waters draining silicates is systematically depleted in heavy isotopes (δ26Mg values range from −1.2 to −0.7‰) relative to the value presently estimated for the continental crust and a local diorite (−0.5‰). In comparison, δ26Mg values measured in soil samples are higher (∼0.0‰). This suggests that Mg isotope fractionation occurs during mineral leaching and/or formation of secondary clay minerals. On the Lorraine plateau, tributaries draining marls, carbonates and evaporites are characterized by low Ca/Mg (1.5-3.2) and low Ca/Sr (80-400) when compared to local carbonate rocks (Ca/Mg = 29-59; Ca/Sr = 370-2200), similar to other rivers draining carbonates. The most likely cause of the Mg and Sr excesses in these rivers is early thermodynamic saturation of groundwater with calcite relative to magnesite and strontianite as groundwater chemistry progressively evolves in the aquifer. δ26Mg of the dissolved phases of tributaries draining mainly carbonates and evaporites are relatively low and constant throughout the year (from −1.4‰ to −1.6‰ and from −1.2‰ to −1.4‰, respectively), within the range defined for the underlying rocks. Downstream of Epinal, the compositions of the Moselle River samples in a δ26Mg vs. 87Sr/86Sr diagram can be explained by mixing curves between silicate, carbonate and evaporite waters, with a significant contribution from the Vosgian silicate lithologies (>70%). Temporal co-variation between δ26Mg and 87Sr/86Sr for the Moselle River throughout year is also observed, and is consistent with a higher contribution from the Vosges mountains in winter, in terms of runoff and dissolved element flux. Overall, this study shows that Mg isotopes measured in waters, rocks and soils, coupled with other tracers such as Sr isotopes, could be used to better constrain riverine Mg sources, particularly if analytical uncertainties in Mg isotope measurements can be improved in order to perform more precise quantifications.  相似文献   

20.
Changes in 87Sr/86Sr and major element geochemistry, from two sediment cores (9509 and 9501) in the Eastern Mediterranean (EM), were used to resolve changes in sediment provenance and, hence, determine climate changes in the Nile catchment and Eastern Sahara desert over the past 25 ka. The sediment was described by a three end-member system comprising Blue Nile (BN; 87Sr/86Sr = 0.7506; Sr = 210 ppm), White Nile (WN; 87Sr/86Sr = 0.7094; Sr = 72.5 ppm) and Saharan dust (SD; 87Sr/86Sr = 0.7183; Sr = 99 ppm). The sedimentary record of these cores represents the suspended load carried down the Nile river and discharged into the S.E. Levantine basin and thus records palaeoclimatically controlled changes in erosion and transport in the catchment. During arid periods (0–5 ka BP) and prior to 11 ka BP, fluxes of BN sediment at 9509 (~6 g/cm2/yr & 10–12 g/cm2/yr, respectively) were greater than during the peak of the African Humid Period (AHP) from 5 to 11 ka BP (<2 g/cm2/yr); this latter period witnessed the deposition of the youngest organic-rich sediment, termed sapropel (S-1), in the EM basin. By contrast the flux of WN increased during the AHP from ~5 g/cm2/yr at ~13 ka BP to >15 g/cm2/yr. In the Ethiopian Highlands (BN catchment) increases in the amount and duration of the monsoon during the AHP caused more vegetation to grow resulting in less soil erosion. In the WN catchment increased rainfall caused more catchment erosion and higher sediment flux through the Sudd marshes. The sedimentation rate in core 9509 increased during the AHP because of the greater importance of the WN sediment flux relative to the BN sediment flux. Saharan dust flux also decreased during the AHP reaching a minimum at ~6 ka BP (core 9509) due to ‘greening’ of the Sahara desert. At the onset of S-1, the changes in Nile flow as determined by 87Sr/86Sr and climatic changes in the EM basin determined by δ18O of planktonic foraminifera were simultaneous, confirming that such isotopic tracers cannot be used directly to determine the cause of the circulation changes in the EM at this time. The increase in the proportion of BN sediment at 9509 with a somewhat higher grain size during the H-1 period (15–17 ka BP) was caused by erosion and redistribution of sediment from the Nile delta and/or the Israeli coast as sea-level rose.  相似文献   

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