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1.
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   

2.
Declining water levels in arid and semi-arid regions increase an aquifer’s vulnerability to natural and anthropogenic influences. A multi-isotope (δD, δ18O, 87Sr/86Sr, and δ11B) approach was used to resolve the geochemical evolution of groundwater in a declining aquifer in a semi-arid region of the southwestern USA as groundwater composition reacts to source-water mixing, cross-formational flow including saltwater intrusion, water–rock interaction, and likely agricultural recharge. Sub-aquifers or local flow systems are present in the Southern High Plains aquifer along the Western Caprock Escarpment in New Mexico, and the study site’s local flow system contains a Na–Cl, high dissolved-solids groundwater that flows from the escarpment until it mixes with a high quality regional aquifer or regional flow system. The local flow system contains water that is similar in composition to the underlying, upper Dockum Group aquifer. Saltwater found in the upper Dockum Group aquifer likely originates in the adjacent Pecos River Basin and crosses beneath or possibly through the hydrologic divide of the Western Caprock Escarpment. Strontium concentrations of 0.9–31 mg/L and a 87Sr/86Sr range of 0.70845–0.70906 were sufficient to estimate source-water fractions, mixing patterns, and contributions from chemical weathering through mass balance inverse calculations. Boron concentrations (59–1740 mg/L) and δ11B values (+6.0–+46.0‰) were used to confirm source-water mixing, further evaluate water–rock interaction, and examine the influence of possible agricultural recharge. Alteration of B concentrations and δ11B values in an area of likely agricultural recharge indicated the loss of B and decrease in δ11B values likely from plant uptake, adsorption, and weathering contributions in the soil/vadose zone prior to recharge. The effectiveness of 87Sr/86Sr and δ11B for resolving the geochemical influences in groundwater in the Southern High Plains along the Western Caprock Escarpment allowed for the reinterpretation of the isotopic composition of water that has been shown to be highly variable in the Southern High Plains. This study shows the utility of a multi-isotope approach for resolving the geochemical evolution of groundwater in an aquifer that has a complex relationship with underlying aquifers and the applicability of these isotopes as indicators of the alteration of source waters from natural or anthropogenic influences.  相似文献   

3.
Groundwater quality in karst regions is largely controlled by natural processes and anthropogenic activities. Over the past 10?years, dissolved Sr and its radiogenic isotope, 87Sr/86Sr, were widely used to trace the sources of solutes in groundwater. However, there is little research about hydrogeochemistry and Sr isotopic compositions of the karst groundwater in Chongqing karst area. In this paper, thirty-five representative karst groundwater samples were collected from different aquifers (limestone and dolomite) and various land use types. Hydrochemical types of karst groundwater in Chongqing were mainly of the Ca-HCO3 type or Ca(Mg)-HCO3 type. The dissolved Sr concentrations of the studied groundwater ranged from 0.57 to 15.06???mmol/L, and the 87Sr/86Sr varied from 0.70751 to 0.71627. The groundwater samples from different aquifers and land use types showed distinctive dissolved Sr concentrations and 87Sr/86Sr. The very positive relationship between Ca/Sr and Mg/Sr in dolomite and limestone aquifers suggests that Ca, Mg and Sr element come mainly from the release of carbonate rock under the groundwater?Crock?CCO2 gas interaction. According to the 87Sr/86Sr ratio, the Sr element in karst groundwater in Chongqing was controlled by the weathering of limestone, dolomite and silicate rock (allogenic water in a non-karst area). The relationship 87Sr/86Sr versus Sr2+/[K+?+?Na+] shows that the anthropogenic inputs also obviously contribute to the Sr contents. The research results show that the karst groundwater in Chongqing is facing serious crisis of water quality, and needs to be protected further.  相似文献   

4.
《Applied Geochemistry》2000,15(5):599-609
The effects of agriculture on the isotope geochemistry of Sr were investigated in two small watersheds in the Atlantic coastal plain of Maryland. Stratified shallow oxic groundwaters in both watersheds contained a retrievable record of increasing recharge rates of chemicals including NO3−, Cl, Mg, Ca and Sr that were correlated with increasing fertilizer use between about 1940 and 1990. The component of Sr associated with recent agricultural recharge was relatively radiogenic (87Sr/86Sr=0.715) and it was overwhelming with respect to Sr acquired naturally by water–rock interactions in the oxidized, non-calcareous portion of the saturated zone. Agricultural groundwaters that penetrated relatively unoxidized calcareous glauconitic sediments at depth acquired an additional component of Sr from dissolution of early Tertiary marine CaCO3 (87Sr/86Sr=0.708) while undergoing O2 reduction and denitrification. Ground-water discharge contained mixtures of waters of various ages and redox states. Two streams draining the area are considered to have higher 87Sr/86Sr ratios and NO3− concentrations than they would in the absence of agriculture; however, the streams have consistently different 87Sr/86Sr ratios and NO3− concentrations because the average depth to calcareous reducing (denitrifying) sediments in the local groundwater flow system was different in the two watersheds. The results of this study indicate that agriculture can alter significantly the isotope geochemistry of Sr in aquifers and streams and that the effects could vary depending on the types, sources and amounts of fertilizers added, the history of fertilizer use and groundwater residence times.  相似文献   

5.
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6.
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   

7.
To compare relative reaction rates of mineral dissolution in a mineralogically simple groundwater aquifer, we studied the controls on solute concentrations, Sr isotopes, and rare earth element and yttrium (REY) systematics in the Cape Cod aquifer. This aquifer comprises mostly carbonate-free Pleistocene sediments that are about 90% quartz with minor K-feldspar, plagioclase, glauconite, and Fe-oxides. Silica concentrations and pH in the groundwater increase systematically with increasing depth, while Sr isotopic ratios decrease. No clear relationship between 87Sr/86Sr and Sr concentration is observed. At all depths, the 87Sr/86Sr ratio of the groundwater is considerably lower than the Sr isotopic ratio of the bulk sediment or its K-feldspar component, but similar to that of a plagioclase-rich accessory separate obtained from the sediment. The Si-87Sr/86Sr-depth relationships are consistent with dissolution of accessory plagioclase. In addition, solutes such as Sr, Ca, and particularly K show concentration spikes superimposed on their respective general trends. The K-Sr-87Sr/86Sr systematics suggests that accessory glauconite is another major solute source to Cape Cod groundwater. Although the authigenic glauconite in the Cape Cod sediment is rich in Rb, it is low in in-grown radiogenic 87Sr because of its young Pleistocene age. The low 87Sr/86Sr ratios are consistent with equilibration of glauconite with seawater. The impact of glauconite is inferred to vary due to its variable abundance in the sediments. In the Cape Cod groundwater, the variation of REY concentrations with sampling depth resembles that of K and Rb, but differs from that of Ca and Sr. Shale-normalized REY patterns are light REY depleted, show negative Ce anomalies and super-chondritic Y/Ho ratios, but no Eu anomalies. REY input from feldspar, therefore, is insignificant compared to input from a K-Rb-bearing phase, inferred to be glauconite. These results emphasize that interpretation of groundwater chemistry, even in relatively simple aquifers, may be complicated by solute contributions from “exotic” accessory minerals such as glauconite. To detect such peculiarities, groundwater studies should combine the study of elemental concentration and isotopic composition of several solutes that show different geochemical behavior.  相似文献   

8.
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9.
《Applied Geochemistry》2000,15(3):311-325
Barium/Sr and Ca/Sr ratios have been used to model the relative importance of different sources of stream water. Major and trace element concentrations together with 87Sr/86Sr ratios were measured in precipitation, soil water, groundwater and stream water in a small (9.4 km2) catchment in northern Sweden. The study catchment is drained by a first order stream and mainly covered with podzolized Quaternary till of granitic composition. It is underlain by a 1.8 Ga granite. A model with mixing equations used in an iterative mode was developed in order to separate the stream water into 3 subsurface components: soil water, shallow groundwater, and deep groundwater. Contributions from precipitation are thus not included in the model. This source may be significant for the stream water generation, but it does not interfere with the calculations of the relative contributions from the subsurface components. The results show that the deep groundwater constitutes between 5 and 20% of the subsurface water discharge into the stream water. The highest values of the deep groundwater fraction occur during base flow. Soil water dominates during snowmelt seasons, whereas during base flow it is the least important fraction. Soil water accounts for 10–100% of the subsurface water discharge into the stream water. Shallow groundwater accounts for up to 80% of the subsurface water discharge with the lowest values at peak discharge during snowmelt seasons and the highest values during base flow. The validity of the model was tested by comparing the measured 87Sr/86Sr ratios in the stream water with the 87Sr/86Sr ratios predicted by the model. There was a systematic difference between the measured and modelled 87Sr/86Sr ratios which suggests that the fraction of soil water is overestimated by the model, especially during spring flood. As a consequence of this overestimation of soil water the amount of shallow groundwater is probably underestimated during this period. However, it is concluded that the differences between measured and predicted values are relatively small, and that element ratios are potentially effective tracers for different subsurface water flowpaths in catchments.  相似文献   

10.
Chemical and isotopic data for 23 geothermal water samples collected in New Zealand within the Taupo Volcanic Zone (TVZ) are reported. Major and trace elements including Li, B and Sr and their isotopic compositions (δ7Li, δ11B, 87Sr/86Sr) were determined in high temperature geothermal waters collected from deep boreholes in different geothermal fields (Ohaaki, Wairakei, Mokai, Kawerau and Rotokawa geothermal systems). Lithium concentrations are high (from 4.5 to 19.9 mg/L) and Li isotopic compositions (δ7Li) are homogeneous, ranging between −0.5‰ and +1.4‰. In particular, it is noteworthy that, except for the samples from the Kawerau geothermal field having slightly higher δ7Li values (+1.4%), the other geothermal waters have a near constant δ7Li signature around a mean value of 0‰ ± 0.6 (2σ, n = 21). Boron concentrations are also high and relatively homogeneous for the geothermal samples, falling between 17.5 and 82.1 mg/L. Boron isotopic compositions (δ11B) are all negative, and display a range between −6.7‰ and −1.9‰. These B isotope compositions are in agreement with those of the Ngawha geothermal field in New Zealand. Lithium and B isotope signatures are in a good agreement with a fluid signature mainly derived from water/rock interaction involving magmatic rocks with no evidence of seawater input. On the other hand, Sr concentrations are lower and more heterogeneous and fall between 2 and 165 μg/L. The 87Sr/86Sr ratios range from 0.70549 to 0.70961. These Sr isotope compositions overlap those of the Rotorua geothermal field in New Zealand, confirming that some geothermal waters (with more radiogenic Sr) have interacted with bedrocks from the metasedimentary basement. Each of these isotope systems on their own reveals important information about particular aspects of either water source or water/rock interaction processes, but, considered together, provide a more integrated understanding of the geothermal systems from the TVZ in New Zealand.  相似文献   

11.
《Applied Geochemistry》1999,14(7):939-951
Strontium isotope ratios are used to identify end-member ground-water compositions at Äspö in southeastern Sweden where the Hard Rock Laboratory (HRL) has been constructed to evaluate the suitability of crystalline rock for the geologic disposal of nuclear waste. The Hard Rock Laboratory is a decline (tunnel) constructed in 1.8 Ga-old granitic rock that forms islands in an archipelago along the Swedish coast. Ground-water samples were obtained for isotopic analyses from boreholes drilled from the surface and from side boreholes drilled within the HRL. Infiltration at Äspö occurs primarily through fractures zones in the granitic bedrock beneath thin soils throughout the area. Because of extremely low Sr concentrations, rain and snow are not important contributors to the Sr isotope budget of the ground-water system. At shallow levels, water percolating downward along fractures and fracture zones acquires a δ87Sr between +9.5 and +10.0‰ and maintains this value downward while Sr concentrations increase by two orders of magnitude. Ground-water samples from both boreholes and from in the HRL show the effects of mixing with saline waters containing as much as 59 mg/L Sr and δ87Sr values as large as +13.9‰. Baltic Sea water is a potential component of the groundwater system with δ87Sr values only slightly larger than modern marine values (+0.3‰) but with much lower concentrations (1.5 mg/L) than ocean water (8 mg/L). However, because of large Sr concentration differences between the saline groundwater (59 mg/L) and Baltic Sea water (1.5 mg/L), δ87Sr values are not particularly sensitive indicators of sea-water intrusion even though their δ87Sr values differ substantially.  相似文献   

12.
The chemical and isotopic characterization of formation water from 18 oil production wells, extracted from 5200 to 6100 m b.s.l. at the Jujo–Tecominoacán carbonate reservoir in SE-Mexico, and interpretations of historical production records, were undertaken to determine the origin and hydraulic behavior of deep groundwater systems. The infiltration of surface water during Late Pleistocene to Early Holocene time is suggested by 14C-concentrations from 2.15 to 31.86 pmC, and by 87Sr/86Sr-ratios for high-salinity formation water (0.70923–0.70927) that are close to the composition of Holocene to modern seawater. Prior to infiltration, the super-evaporation of seawater reached maximum TDS concentrations of 385 g/L, with lowest δ18O values characterizing the most hypersaline samples. Minor deviations of formation water and dolomite host rocks from modern and Jurassic 87Sr/86Sr-seawater composition, respectively, suggest ongoing water–rock interaction, and partial isotopic equilibration between both phases. The abundance of 14C in all sampled formation water, 87Sr/86Sr-ratios for high-salinity water close to Holocene – present seawater composition, a water salinity distribution that is independent of historic water-cut, and a total water extraction volume of 2.037 MMm3 (1/83–4/07) excludes a connate, oil-leg origin for the produced water of the Jurassic–Cretaceous mudstone-dolomite sequence. Temporal fluctuations of water chemistry in production intervals, the accelerated migration of water fronts from the reservoir flanks, and isotopic mixing trends between sampled wells confirms the existence of free aquifer water below oil horizons. Vertical and lateral hydraulic mobility has probably been accelerated by petroleum extraction.  相似文献   

13.
Sequential extractions were performed on small amounts of particulate and sediment samples (6 to10 mg) from the Mississippi River mixing zone. The leachates were analyzed for Sr concentration and 87Sr/86Sr isotope ratio. Mn and Fe contents were also measured as their oxyhydroxides are potential carrier phases for Sr. The largest fraction of Sr in the solid phase (particulates and sediments) was found to be present in the residual, refractory fraction (>70% of total). By comparison with the corresponding sediment, particulates appear to have higher concentrations of nonresidual, labile Sr (30% vs. 15%). Carbonate components seem to play an important role as carriers for labile Sr in particulates and sediments. Changes in the composition and content of the solid phase may significantly modify both the 87Sr/86Sr isotope ratio of the total labile fractions and that of the bulk components. However, such modifications, under normal conditions, exert little measurable influence on the Sr isotope composition of the dissolved phase.  相似文献   

14.
Shear faults in Upper Cretaceous limestones of the central Negev desert adjacent to the Dead Sea Transform (DST) feature extensive ferruginous mineralization and dolomitization. This has been related to topographically driven flow of metalliferous groundwaters through an underlying clastic (Nubian Sandstone) aquifer and rise of the fluids up the fault zones. The present study combines Pb and Sr isotope measurements with detailed sampling and petrography at the eastern end of the Paran fault (Menuha Ridge) in order to identify the types of groundwater and the sources of enriched elements in this regional-scale sedimentary mineralization. Ferroan and non-ferroan dolomitization along the Paran fault caused significant enrichment of several elements (Mg, Cu, Mn, Ni, V, Zn, Pb, and U) and 87Sr/86Sr values that are significantly higher than the Upper Cretaceous limestone country rock. The non-ferroan dolomite and the ferroan dolomite sampled at three sites along the Menuha Ridge have similar 87Sr/86Sr values 0.7076-0.7089, and 0.7077-0.7086, respectively. Additionally, there is a positive correlation between Mg-content of the dolomites and their 87Sr/86Sr values. The isotopic composition of Sr and Pb of dolomite corresponds to the mineralogical type identified in the mineralized rock (non-ferroan dolomite, simple-zoned ferroan dolomite, and complex-zoned ferroan dolomite). The 207Pb/204Pb and 206Pb/204Pb ratios of Fe oxides and dolomites from the three sites plot on a straight line, where the simple-zoned ferroan dolomite values are at the non-radiogenic end of the line and the complex-zoned ferroan dolomites at the radiogenic end. Both 206Pb/204Pb and 207Pb/204Pb ratios in dolomites and to a lesser degree in Fe-oxides suggest that a mixing between two end-members controls the behavior of Pb in the mineralization products along the Paran fault. Rather than a single fluid source, the study indicates that two types of metalliferous groundwaters were involved in the dolomitization and mineralization along the Paran fault. The first, and hitherto undocumented, fluid source is the Mg-rich Dead Sea Rift brine, migrating in the sub-surface before dolomitizing the carbonate bedrock. Migration of the brines took a deep path to the site of mineralization, with temperatures reaching 75 °C. Based on the geological history of the region, this probably took place in the Late Miocene-Early Pliocene interval. The second type of groundwater acquired its high solute concentrations from leaching igneous rocks and clastic sediments in the sub-surface, and infiltrated along the Paran fault, precipitating Fe-rich minerals and caused the first stage of dolomitization. This groundwater flowed at shallower depth than the DSR brines, and at lower temperatures (T ? 50 °C). The study shows that sedimentary mineralization in faults adjacent to active transform fault zones may arise from the combination of several different fluid flow regimes.  相似文献   

15.
A 4-yr study of spatial and temporal variability in the geochemistry of vadose groundwaters from caves within the Edwards aquifer region of central Texas offers new insights into controls on vadose groundwater evolution, the relationship between vadose and phreatic groundwaters, and the fundamental influence of soil composition on groundwater geochemistry. Variations in Sr isotopes and trace elements (Mg/Ca and Sr/Ca ratios) of dripwaters and soils from different caves, as well as phreatic groundwaters, provide the potential to distinguish between local variability and regional processes controlling fluid geochemistry, and a framework for understanding the links between climatic and hydrologic processes.The Sr isotope compositions of vadose cave dripwaters (mean 87Sr/86Sr = 0.7087) and phreatic groundwaters (mean 87Sr/86Sr = 0.7079) generally fall between values for host carbonates (mean 87Sr/86Sr = 0.7076) and exchangeable Sr in overlying soils (mean 87Sr/86Sr = 0.7088). Dripwaters have lower Mg/Ca and Sr/Ca ratios, and higher 87Sr/86Sr values than phreatic groundwaters. Dripwater 87Sr/86Sr values also inversely correlate with both Mg/Ca and Sr/Ca ratios. Mass-balance modeling combined with these geochemical relationships suggest that variations in fluid compositions are predominantly controlled by groundwater residence times, and water-rock interaction with overlying soils and host aquifer carbonate rocks. Consistent differences in dripwater geochemistry (i.e., 87Sr/86Sr, Mg/Ca, and Sr/Ca) between individual caves are similar to compositional differences in soils above the caves. While these differences appear to exert significant control on local fluid evolution, geochemical and isotopic variations suggest that the controlling processes are regionally extensive. Temporal variations in 87Sr/86Sr values and Mg/Ca ratios of dripwaters from some sites over the 4-yr interval correspond with changes in both aquifer and climatic parameters. These results have important implications for the interpretation of trace element and isotopic variations in speleothems as paleoclimate records, as well as the understanding of controls on water chemistry for both present-day and ancient carbonate aquifers.  相似文献   

16.
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   

17.
Exploration of unconventional natural gas reservoirs such as impermeable shale basins through the use of horizontal drilling and hydraulic fracturing has changed the energy landscape in the USA providing a vast new energy source. The accelerated production of natural gas has triggered a debate concerning the safety and possible environmental impacts of these operations. This study investigates one of the critical aspects of the environmental effects; the possible degradation of water quality in shallow aquifers overlying producing shale formations. The geochemistry of domestic groundwater wells was investigated in aquifers overlying the Fayetteville Shale in north-central Arkansas, where approximately 4000 wells have been drilled since 2004 to extract unconventional natural gas. Monitoring was performed on 127 drinking water wells and the geochemistry of major ions, trace metals, CH4 gas content and its C isotopes (δ13CCH4), and select isotope tracers (δ11B, 87Sr/86Sr, δ2H, δ18O, δ13CDIC) compared to the composition of flowback-water samples directly from Fayetteville Shale gas wells. Dissolved CH4 was detected in 63% of the drinking-water wells (32 of 51 samples), but only six wells exceeded concentrations of 0.5 mg CH4/L. The δ13CCH4 of dissolved CH4 ranged from −42.3‰ to −74.7‰, with the most negative values characteristic of a biogenic source also associated with the highest observed CH4 concentrations, with a possible minor contribution of trace amounts of thermogenic CH4. The majority of these values are distinct from the reported thermogenic composition of the Fayetteville Shale gas (δ13CCH4 = −35.4‰ to −41.9‰). Based on major element chemistry, four shallow groundwater types were identified: (1) low (<100 mg/L) total dissolved solids (TDS), (2) TDS > 100 mg/L and Ca–HCO3 dominated, (3) TDS > 100 mg/L and Na–HCO3 dominated, and (4) slightly saline groundwater with TDS > 100 mg/L and Cl > 20 mg/L with elevated Br/Cl ratios (>0.001). The Sr (87Sr/86Sr = 0.7097–0.7166), C (δ13CDIC = −21.3‰ to −4.7‰), and B (δ11B = 3.9–32.9‰) isotopes clearly reflect water–rock interactions within the aquifer rocks, while the stable O and H isotopic composition mimics the local meteoric water composition. Overall, there was a geochemical gradient from low-mineralized recharge water to more evolved Ca–HCO3, and higher-mineralized Na–HCO3 composition generated by a combination of carbonate dissolution, silicate weathering, and reverse base-exchange reactions. The chemical and isotopic compositions of the bulk shallow groundwater samples were distinct from the Na–Cl type Fayetteville flowback/produced waters (TDS ∼10,000–20,000 mg/L). Yet, the high Br/Cl variations in a small subset of saline shallow groundwater suggest that they were derived from dilution of saline water similar to the brine in the Fayetteville Shale. Nonetheless, no spatial relationship was found between CH4 and salinity occurrences in shallow drinking water wells with proximity to shale-gas drilling sites. The integration of multiple geochemical and isotopic proxies shows no direct evidence of contamination in shallow drinking-water aquifers associated with natural gas extraction from the Fayetteville Shale.  相似文献   

18.
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   

19.
《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   

20.
Hydrogeochemistry and environmental tracers (2H, 18O, 87Sr/86Sr) in precipitation, river and reservoir water, and groundwater have been used to determine groundwater recharge sources, and to identify mixing characteristics and mineralization processes in the Manas River Basin (MRB), which is a typical mountain–oasis–desert ecosystem in arid northwest China. The oasis component is artificial (irrigation). Groundwater with enriched stable isotope content originates from local precipitation and surface-water leakage in the piedmont alluvial–oasis plain. Groundwater with more depleted isotopes in the north oasis plain and desert is recharged by lateral flow from the adjacent mountains, for which recharge is associated with high altitude and/or paleo-water infiltrating during a period of much colder climate. Little evaporation and isotope exchange between groundwater and rock and soil minerals occurred in the mountain, piedmont and oasis plain. Groundwater δ2H and δ18O values show more homogeneous values along the groundwater flow direction and with well depths, indicating inter-aquifer mixing processes. A regional contrast of groundwater allows the 87Sr/86Sr ratios and δ18O values to be useful in a combination with Cl, Na, Mg, Ca and Sr concentrations to distinguish the groundwater mixing characteristics. Two main processes are identified: groundwater lateral-flow mixing and river leakage in the piedmont alluvial–oasis plain, and vertical mixing in the north oasis plain and the desert. The 87Sr/86Sr ratios and selected ion ratios reveal that carbonate dissolution and mixing with silicate from the southern mountain area are primarily controlling the strontium isotope hydrogeochemistry.  相似文献   

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