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1.
The watershed in the southern Jiangxi Province (Jiangxi Province is called simply Gan) (SGW) and the watershed in the central Guizhou Province (Guizhou Province is called simply Qian) (CQW) are two subtropical watersheds of the Yangtze River in China. Both watersheds have similar latitudes and climate, but distinct differences in basin lithology. These similarities and differences provide a good natural laboratory in which to investigate weathering processes and Sr end-members in river waters. This work aims to identify and contrast the sources, fluxes and controls on Sr isotopic composition in the river waters of these two areas. Results showed that the 87Sr/86Sr in the SGW waters ranged from 0.716501 to 0.724931, with dissolved Sr averaging 27 μg l− 1. Rhyolites and granites are two major sources for the dissolved Sr. The SGW waters receive 42% of their Sr from silicates weathering, 32% from carbonates and 3.2% from evaporites. 87Sr/86Sr in the CQW waters has a lesser variation from 0.707694 to 0.710039, but higher Sr contents (average of 208 μg l− 1). Dolomite, limestone and dolomitic limestone are major sources of Sr in the waters. The CQW waters receive 69% of their Sr from carbonates, 1.7% from silicates and 0.9% from evaporites. The chemical erosion rate and Sr flux in the CQW are 122 t km− 2 a− 1 and 0.079 t km− 2 a− 1, respectively, which are higher than those of the SGW (56 t km− 2 a− 1 and 0.021 t km− 2 a− 1, respectively). These data suggest that the intensive carbonates weathering occurred in the karstic area in the upper-reach of the Yangtze River exert great influence on the high Sr concentration and low Sr isotopic ratios in the River.  相似文献   

2.
The oxidation of sulfide-rich rocks, mostly leftover debris from Cu mining in the early 20th century, is contributing to metal contamination of local coastal environments in Prince William Sound, Alaska. Analyses of sulfide, water, sediment, precipitate and biological samples from the Beatson, Ellamar, and Threeman mine sites show that acidic surface waters generated from sulfide weathering are pathways for redistribution of environmentally important elements into and beyond the intertidal zone at each site. Volcanogenic massive sulfide deposits composed of pyrrhotite and (or) pyrite + chalcopyrite + sphalerite with subordinate galena, arsenopyrite, and cobaltite represent potent sources of Cu, Zn, Pb, As, Co, Cd, and Hg. The resistance to oxidation among the major sulfides increases in the order pyrrhotite ? sphalerite < chalcopyrite ? pyrite; thus, pyrrhotite-rich rocks are typically more oxidized than those dominated by pyrite. The pervasive alteration of pyrrhotite begins with rim replacement by marcasite followed by replacement of the core by sulfur, Fe sulfate, and Fe–Al sulfate. The oxi dation of chalcopyrite and pyrite involves an encroachment by colloform Fe oxyhydroxides at grain margins and along crosscutting cracks that gradually consumes the entire grain. The complete oxidation of sulfide-rich samples results in a porous aggregate of goethite, lepidocrocite and amorphous Fe-oxyhydroxide enclosing hydrothermal and sedimentary silicates. An inverse correlation between pH and metal concentrations is evident in water data from all three sites. Among all waters sampled, pore waters from Ellamar beach gravels have the lowest pH (∼3) and highest concentrations of base metals (to ∼25,000 μg/L), which result from oxidation of abundant sulfide-rich debris in the sediment. High levels of dissolved Hg (to 4100 ng/L) in the pore waters probably result from oxidation of sphalerite-rich rocks. The low-pH and high concentrations of dissolved Fe, Al, and SO4 are conducive to precipitation of interstitial jarosite in the intertidal gravels. Although pore waters from the intertidal zone at the Threeman mine site have circumneutral pH values, small amounts of dissolved Fe2+ in the pore waters are oxidized during mixing with seawater, resulting in precipitation of Fe-oxyhydroxide flocs along the beach–seawater interface. At the Beatson site, surface waters funneled through the underground mine workings and discharged across the waste dumps have near-neutral pH (6.7–7.3) and a relatively small base-metal load; however, these streams probably play a role in the physical transport of metalliferous particulates into intertidal and offshore areas during storm events. Somewhat more acidic fluids, to pH 5.3, occur in stagnant seeps and small streams emerging from the Beatson waste dumps. Amorphous Fe precipitates in stagnant waters at Beatson have high Cu (5.2 wt%) and Zn (2.3 wt%) concentrations that probably reflect adsorption onto the extremely high surface area of colloidal particles. Conversely, crystalline precipitates composed of ferrihydrite and schwertmannite that formed in the active flow of small streams have lower metal contents, which are attributed to their smaller surface area and, therefore, fewer reactive sorption sites. Seeps containing precipitates with high metal contents may contribute contaminants to the marine environment during storm-induced periods of high runoff. Preliminary chemical data for mussels (Mytilus edulis) collected from Beatson, Ellamar, and Threeman indicate that bioaccumulation of base metals is occurring in the marine environment at all three sites.  相似文献   

3.
This contribution describes primary basalt mineral saturation in surface- and up to 90°C ground waters in a tholeiite flood basalt region in northern Iceland. It is based on data on 253 water samples and the mineralogical composition of the associated basalts. Surface waters are significantly under-saturated with plagioclase and olivine of the compositions occurring in the study area, saturation index (SI) values ranging from −1 to −10 and −5 to −20, respectively. With few exceptions these waters are also significantly under-saturated with pigeonite and augite of all compositions (SI = −1 to −7) and with ilmenite (SI = −0.5 to −6). The surface waters are generally over-saturated with respect to the titano-magnetite of the compositions occurring in the basalts of the study area, the range in SI being from −2 to +10. For crystalline OH-apatite, SI values in surface waters range from strong under-saturation (−10) to strong over-saturation (+5) but for crystalline F-apatite they lie in the range 0 to 15. Systematic under-saturation is, on the other hand, observed for “amorphous apatite,” i.e. an apatite of the kind Clark (1955) prepared by mixing Ca(OH)2 and H3PO4 solutions. Like surface waters, ground waters are under-saturated with plagioclase and olivine, its degree increasing with increasing Ca content of the plagioclase and increasing Fe content of the olivine, the SI values being −2 to −7 and 0 to −4 for the Ca-richest and Ca-poorest plagioclase, respectively, and about −3 to −18 and 0 to −15 for forsterite and fayalite, respectively. Ground waters are generally close to saturation with pigeonite and augite of all compositions. However, some non-thermal ground waters in highland areas are strongly under-saturated. Above 25°C the ground waters are ilmenite under-saturated but generally over-saturated at lower temperatures. These waters are titano-magnetite over-saturated at temperatures below 70°C, the SI values decreasing with increasing temperature from about 6 to 8 at 10°C to 0 at 70°C. The ground waters are highly over-saturated with both crystalline OH- and F-apatite, or by approximately 10 to 15 SI units but close to saturation with “amorphous apatite” containing about equal amounts of F and OH. The results presented here for the pyroxenes carry an unknown error because available thermodynamic data do not permit but a simple solid solution model for the calculation of their solubility. Published values on the dissociation constants for ferrous iron hydroxide complexes are very variable and those for ferric iron are limited. This casts an error of an unknown magnitude on the calculated SI values for all iron bearing minerals. This error may not be large for waters with a pH of less than 9 but it is apparently high for waters with a higher pH. Improved experimental data on the stability of ferrous and ferric hydrolysis constants are needed to improve the accuracy by which Fe-mineral saturation can be calculated in natural waters.  相似文献   

4.
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5.
Acidic, metal-rich waters produced by the oxidative weathering and resulting leaching of major and trace elements from pyritic rocks can adversely affect water quality in receiving streams and riparian ecosystems. Five study areas in the southern Rocky Mountains with naturally acidic waters associated with porphyry mineralization were studied to document variations in water chemistry and processes that control the chemical variations. Study areas include the Upper Animas River watershed, East Alpine Gulch, Mount Emmons, and Handcart Gulch in Colorado and the Red River in New Mexico. Although host-rock lithologies in all these areas range from Precambrian gneisses to Cretaceous sedimentary units to Tertiary volcanic complexes, the mineralization is Tertiary in age and associated with intermediate to felsic composition, porphyritic plutons. Pyrite is ubiquitous, ranging from ∼1 to >5 vol.%. Springs and headwater streams have pH values as low as 2.6, SO4 up to 3700 mg/L and high dissolved metal concentrations (for example: Fe up to 400 mg/L; Cu up to 3.5 mg/L; and Zn up to 14.4 mg/L). Intensity of hydrothermal alteration and presence of sulfides are the primary controls of water chemistry of these naturally acidic waters. Subbasins underlain by intensely hydrothermally altered lithologies are poorly vegetated and quite susceptible to storm-induced surface runoff. Within the Red River study area, results from a storm runoff study documented downstream changes in river chemistry: pH decreased from 7.80 to 4.83, alkalinity decreased from 49.4 to <1 mg/L, SO4 increased from 162 to 314 mg/L, dissolved Fe increased from to 0.011 to 0.596 mg/L, and dissolved Zn increased from 0.056 to 0.607 mg/L. Compared to mine drainage in the same study areas, the chemistry of naturally acidic waters tends to overlap but not reach the extreme concentrations of metals and acidity as some mine waters. The chemistry of waters draining these mineralized but unmined areas can be used to estimate premining conditions at sites with similar geologic and hydrologic conditions. For example, the US Geological Survey was asked to estimate premining ground-water chemistry at the Questa Mo mine, and the proximal analog approach was used because a mineralized but unmined area was located adjacent to the mine property. By comparing and contrasting water chemistry from different porphyry mineralized areas, this study not only documents the range in concentrations of constituents of interest but also provides insight into the primary controls of water chemistry.  相似文献   

6.
This paper presents the results of a study on the geochemistry of waters circulating in the mineralised area of the south-eastern sector of Mt. Peloritani (north-eastern Sicily, Italy), aimed at basic understanding of the geochemical processes influencing their chemical composition. Chemico-physical parameters and data on 26 major and minor chemical elements are reported for 103 water samples. Water chemistry is mainly dominated by dissolution of carbonates and hydrolysis of aluminosilicate minerals. Total dissolved salts (TDS) range from 80 to 1398 mg/L. All the waters exhibit EH characteristic of an oxygenated environment. Excluding two samples, which show very high H+ activity (pH = 3.0 and 2.7), all the waters have pH values in the range 6.2–8.6. Cluster analysis based on major ion contents defined three main chemical water types, reflecting different hydrochemical processes. The first, group I, has low salinity (average TDS = 118 ± 30 mg/L) and abundance orders (meq/L) Na > Ca ≈ Mg > K and Cl ≈ HCO3 > SO4. With increased water–rock interaction, waters in groups II and III become more saline, changing composition towards SO4–Cl-alkaline earth and HCO3-alkaline earth types. Weathering of carbonate minerals causes waters to become saturated with respect to calcite and dolomite, whereas the incongruent dissolution of aluminosilicate minerals causes the solution to reach equilibrium with kaolinite and to form smectites. Trace element geochemistry in the analysed waters reflects interactions between waters and existing mineralisation, with elemental concentrations showing highly variable values, and higher concentrations of As, Pb, Sb and Zn near known mineralisation. Lead–Zn and As–Sb statistical associations, probably distinguishing interactions with different mineralogical phase paragenesis, were revealed by factor analysis. The main aqueous chemical forms of trace elements predicted by chemical speciation calculations are also reported. As most of the analysed spring waters provide the main source of freshwater for domestic purposes, attention should be given to As and Sb, whose concentrations exceed the recommended limits.  相似文献   

7.
Hydrogeochemical processes that accompany seawater intrusion in coastal aquifers can alter the resulting water quality and are important ingredients in coastal aquifer management. The presence of dissolution–precipitation reactions and ion exchange in the mixing zone of the Biscayne aquifer (FL, USA) are suggested based on changes in major ion concentrations and mineral saturation indices (SI). Major ion concentrations from 11 groundwater samples are compared with theoretical mixing between freshwater and seawater. PHREEQC code was used to calculate saturation indices of the samples with respect to common phases in the Biscayne aquifer. High Ca2+ and HCO3 ? content of the samples is typical of waters in contact with carbonate aquifers. Water quality of the samples is mainly attributed to mixing and precipitation–dissolution reactions with calcite and dolomite. The samples were saturated with calcite (SI ~ 0) and undersaturated for dolomite (SI < 0), while a few samples showed dolomite saturation. Because gypsum and halite SI could be predicted by theoretical mixing, reactions with those minerals, if present, are thought to be insignificant. In the active intrusion areas, cation exchange also appears to modify water quality leading to excess Ca2+, but depleted Na+, Mg2+ and K+ concentrations. On the other hand, samples from previous intrusion areas plotted very close to the theoretical mixing line and approached equilibrium with the seawater.  相似文献   

8.
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9.
Recent studies of chemical weathering of andesitic-dacitic material on high-standing islands (HSIs) have shown these terrains have some of the highest observed rates of chemical weathering and associated CO2 consumption yet reported. However, the paucity of stream gauge data in many of these terrains has limited determination of chemical weathering product fluxes. In July 2006 and March 2008, stream water samples were collected and manual stream gauging was performed in watersheds throughout the volcanic island of Dominica in the Lesser Antilles. Distinct wet and dry season solute concentrations reveal the importance of seasonal variations on the weathering signal. A cluster analysis of the stream geochemical data shows the importance of parent material age on the overall delivery of solutes. Observed Ca:Na, HCO3:Na and Mg:Na ratios suggest crystallinity of the parent material may also play an important role in determining weathering fluxes. From total dissolved solids concentrations and mean annual discharge calculations we calculate chemical weathering yields of (6-106 t km−2 a−1), which are similar to those previously determined for basalt terrains. Silicate fluxes (3.1-55.4 t km−2 a−1) and associated CO2 consumption (190-1575 × 103 mol km−2 a−1) determined from our study are among the highest determined to date. The calculated chemical fluxes from our study confirm the weathering potential of andesitic-dacitic terrains and that additional studies of these terrains are warranted.  相似文献   

10.
Sediment fluxes from high standing oceanic islands (HSIs) such as New Zealand are some of the highest known [Milliman J. D. and Syvitski J. P. M. (1992) Geomorphic/tectonic control of sediment discharge to the ocean: the importance of small mountainous rivers. J. Geol.100, 525-544]. Recent geochemical work has suggested that along with their extremely high physical weathering yields, many New Zealand watersheds also have very high chemical weathering yields. In New Zealand, the magnitude of both the physical and chemical weathering yields is related to the lithology of the watershed. Most of the previous work on this topic has been undertaken in Southern Alps watersheds of schist and greywacke and in East Cape watersheds of semi-consolidated marine sediments and greywacke. We recently sampled North Island watersheds in the Taranaki and Manawatu-Wanganui regions which have been subjected to volcanism since the Miocene. We sampled watersheds that contain both volcanic and sedimentary rocks. A series of water and sediment samples was collected and analyzed for major, minor and trace elements. This was done to quantify the weathering intensities in the watersheds and to establish the relationship between physical and chemical weathering yields in volcanic lithologies. Our results reveal distinct chemical signatures for the different regions. Waters draining the Taranaki region volcanics are significantly enriched in K+, and depleted in Ca2+ and Sr2+ compared to waters draining the Manawatu-Wanganui region volcanics, which also traverse expanses of sedimentary siltstones and mudstones. The Ca2+ and Sr2+ depletions may reflect the relative absence of CaCO3 in the Taranaki region watersheds. In addition, sediment samples from the Taranaki region show significant enrichment in Ti, Al, Ca, Fe, Mn, Mg, Ca, and P and depletion in Si and Rb compared to those of the Manawatu-Wanganui region. From total dissolved solids concentrations and mean annual water discharge, we calculate chemical weathering yields of 60-240 tons km−2 a−1. These weathering yields fall within the middle to upper range of those previously documented for the Southern Alps (93-480 tons km−2 a−1) and East Cape (62-400 tons km−2 a−1). Calculated silicate weathering yields of 12-33.6 tons km−2 a−1 and CO2 consumption of 852-2390 × 103 mol km−2 a−1 for the rivers draining the Taranaki volcanic region are higher than those previously reported for watersheds hosted in sedimentary and metamorphosed rock terrains on HSIs. CO2 consumption is found to be within the range previously measured for the basaltic terrains of the Deccan Traps (580-2450 × 103 mol km−2 a−1) and Réunion Island(1300-4400 × 103 mol km−2 a−1). Our calculated chemical weathering yields demonstrate the importance of HSIs, particularly those with volcanic terrains, when considering global geochemical fluxes.  相似文献   

11.
Bottled waters are an increasingly significant product in the human diet. In this work, we present a dataset of stable isotope ratios for bottled waters sampled in Greece. A total of 25 domestic brands of bottled still waters, collected on the Greek market in 2009, were analysed for δ18O and δ2H. The measured stable isotope ratios range from − 9.9‰ to − 6.9‰ for δ18O and from − 67.50‰ to − 46.5‰ for δ2H. Comparison of bottled water isotope ratios with natural spring water isotope ratios demonstrates that on average the isotopic composition of bottled water tends to be similar to the composition of naturally available local water sources, showing that bottled water isotope ratios preserve information about the water sources from which they were derived and suggesting that in many cases bottled water should not be considered as an isotopically distinct component of the human diet. This investigation also helped to determine the natural origin of bottled water, and to indicate differences between the natural and production processes. The production process may influence the isotopic composition of waters. No such modification was observed for sampled waters in this study. The isotopic methods applied can be used for the authentication of bottled waters and for use in the regulatory monitoring of water products.  相似文献   

12.
This work, which was done within the Swedish nuclear waste management program, was carried out in order to increase the understanding of the mobility and fate of rare earth elements (REEs) in natural boreal waters in granitoidic terrain. Two areas were studied, Forsmark and Simpevarp, one of which will be selected as a site for spent nuclear fuel. The highest REE concentrations were found in the overburden groundwaters, in Simpevarp in particular (median ∑REE 52 μg/L), but also in Forsmark (median ∑REE 6.7 μg/L). The fractionation patterns in these waters were characterised by light REE (LREE) enrichment and negative Ce and Eu anomalies. In contrast, the surface waters had relatively low REE concentrations. They were characterised either by an increase in relative concentrations throughout the lanthanide series (Forsmark which has a carbonate-rich till) or flat patterns (Simpevarp with carbonate-poor till), and had negative Ce and Eu anomalies. In the bedrock groundwaters, the concentrations and fractionation patterns of REEs were entirely different from those in the overburden groundwaters. The median La concentrations were low (just above 0.1 μg/L in both areas), only in a few samples were the concentrations of several REEs (and in a couple of rare cases all REEs) above the detection limit, and there was an increase in the relative concentrations throughout the lanthanide series. In contrast to these large spatial variations, the temporal trends were characterised by small (or non existent) variations in REE-fractionation patterns but rather large variations in concentrations. The Visual MINTEQ speciation calculations predicted that all REEs in all waters were closely associated with dissolved organic matter, and not with carbonate. In the hydrochemical data for the overburden groundwater in particular, there was however a strong indication of association with inorganic colloids, which were not included in the speciation model. Overall the results showed that within a typical boreal granitoidic setting, overburden groundwaters are enriched in REEs, organic complexes are much more important than carbonate complexes, there is little evidence of significant mixing of REEs between different water types (surface, overburden, bedrock) and spatial variations are more extensive than temporal ones.  相似文献   

13.
Twenty-eight tube well water samples were collected in February, 2006, from households in the Cambodian provinces of Prey Veng and Kandal. Concentrations of total As in both provinces ranged from not detectable (ND) up to about 900 μg/L, with about 54% of all the samples collected exceeding the WHO drinking water guide value of 10 μg/L. In addition, about 32% of all samples contained concentrations of Mn exceeding the WHO drinking water guide value of 400 μg/L. It is interesting to note that more than half (about 56%) of tube wells with Mn over 400 μg/L had the non-detectable As. Barium, Sr and Fe were also detected in most of tube well samples, which were typically circum-neutral and reducing. Arsenic speciation was dominated (80%) by dissolved inorganic As(III). The occurrence and composition of the well waters is consistent with the As being mobilized from aquifer sediments by natural processes in a highly reducing environment. The highest estimated cumulative As intake for individuals using the sampled well waters as drinking water is estimated to be around 400 mg As/a – this is comparable to intakes that have resulted elsewhere in the world in serious As-related illnesses and highlights the possibility that such adverse health impacts may arise in Cambodia unless appropriate remedial measures are taken.  相似文献   

14.
Coalbed natural gas (CBNG) production from coal bed aquifers requires large volumes of produced water to be pumped from the subsurface. The produced water ranges from high quality that meets state and federal drinking water standards to low quality due to increased salinity and/or sodicity. The Powder River Basin of northeastern Wyoming is a major coalbed natural gas producing region, where water quality generally decreases moving from the southeastern portion of the basin towards the center. Most produced water in Wyoming is disposed into impoundments and other surface drainages, where it may infiltrate into shallow groundwater. Groundwater degradation caused by infiltration of CBNG produced water holding impoundments into arid, soluble salt-rich soils is an issue of immense importance because groundwater is a major source for stock water, irrigation, and drinking water for many small communities in these areas. This study examines the potential of using stable C isotope signatures of dissolved inorganic C (δ13CDIC) to track the fate of CBNG produced water after it is discharged into the impoundments. Other geochemical proxies like the major cations and major anions were used in conjunction with field water quality measurements to understand the geochemical differences between CBNG produced waters and ambient waters in the study area. Samples were collected from the CBNG discharge outfalls, produced water holding impoundments, and monitoring wells from different parts of the Powder River Basin and analyzed for δ13CDIC. The CBNG produced waters from outfalls and impoundments have positive δ13CDIC values that fall within the range of +12‰ to +22‰, distinct from the ambient regional surface and groundwaters with δ13CDIC values ranging from −10‰ to −14‰. The results from the study demonstrate that these contrasting δ13CDIC signatures can be used to trace seepage out of CBNG produced water impoundments into shallow groundwaters.  相似文献   

15.
This study examined the removal of U, Mo, and Re from seawater by sedimentary processes at a shallow-water site with near-saturation bottom water O2 levels (240-380 μmol O2/L), very high organic matter oxidation rates (annually averaged rate is 880 μmol C/cm2/y), and shallow oxygen penetration depths (4 mm or less throughout the year). Under these conditions, U, Mo, and Re were removed rapidly to asymptotic pore water concentrations of 2.2-3.3 nmol/kg (U), 7-13 nmol/kg (Mo), and 11-14 pmol/kg (Re). The depth order in which the three metals were removed, determined by fitting a diffusion-reaction model to measured profiles, was Re < U < Mo. Model fits also suggest that the Mo profiles clearly showed the presence of a near-interface layer in which Mo was added to pore waters by remineralization of a solid phase. The importance of this solid phase source of pore water Mo increased from January to October as the organic matter oxidation rate increased, bottom water O2 decreased, and the O2 penetration depth decreased. Experiments with in situ benthic flux chambers generally showed fluxes of U and Mo into the sediments. However, when the overlying water O2 concentration in the chambers was allowed to drop to very low levels, Mn and Fe were released to the overlying water along with the simultaneous release of Mo and U. These experiments suggest that remineralization of Mn and/or Fe oxides may be a source of Mo and perhaps U to pore waters, and may complicate the accumulation of U and Mo in bioturbated sediments with high organic matter oxidation rates and shallow O2 penetration depths.Benthic chamber experiments including the nonreactive solute tracer, Br−, indicated that sediment irrigation was very important to solute exchange at the study site. The enhancement of sediment-seawater exchange due to irrigation was determined for the nonreactive tracer (Br−), TCO2, , U and Mo. The comparisons between these solutes showed that reactions within and around the burrows were very important for modulating the Mo flux, but less important for U. The effect of these reactions on Mo exchange was highly variable, enhancing Mo (and, to a lesser extent, U) uptake at times of relatively modest irrigation, but inhibiting exchange when irrigation rates were faster. These results reinforce the observation that Mo can be released to and removed from pore waters via sedimentary reactions.The removal rate of U and Mo from seawater by sedimentary reactions was found to agree with the rate of accumulation of authigenic U and Mo in the solid phase. The fluxes of U and Mo determined by in situ benthic flux chamber measurements were the largest that have been measured to date. These results confirm that removal of redox-sensitive metals from continental margin sediments underlying oxic bottom water is important, and suggest that continental margin sediments play a key role in the marine budgets of these metals.  相似文献   

16.
Many geochemical reactions that control the composition of natural waters, contaminant fate and transport, and biogeochemical element cycling take place at the interface between minerals and aqueous solutions. A fundamental understanding of these important processes requires knowledge of the structure of mineral-water interfaces. High-resolution specular X-ray reflectivity was used to determine the structure of the hematite (0 1 2)-water interface. Relaxation of the surface was observed to be minor, and water was found to order near the hematite surface. Two sites of adsorbed water are inferred to be ordered laterally, one bridging between triply coordinated functional groups and the other bridging between the singly coordinated functional groups on the surface, as steric constraints limit the possible arrangements of water molecules occurring at the observed heights above the hematite surface. Relaxations of the hematite and corundum (0 1 2) surfaces, which are isostructural, are similar and limited primarily to the top most layer of the structures. No significant changes to the interfacial stoichiometry (i.e., partial occupancy of surface species) are observed in either case. The structure of interfacial water is similar on the hematite and corundum (0 1 2) surfaces as well, although water appeared to be less well ordered on the hematite surface. This may be due to expected differences in the oxygen exchange rates from surface functional groups or the apparent better matching of the corundum oxygen lattice to the natural structural ordering in water, and suggests that the dielectric constant gradients of interfacial water may differ on the two surfaces. Similar charging behavior is expected for these surfaces as similar types of surface functional groups are exposed. Although generally similar, subtle differences in the reactivity of hematite and corundum (0 1 2) surfaces to arsenate adsorption, and possibly the adsorption of other species, may be related to the difference in ordering of interfacial water observed in this study.  相似文献   

17.
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   

18.
We report lithium (Li) isotopic measurements in seawater-derived waters that were discharged from geothermal wells, thermal springs, and sub-marine springs located in volcanic island arc areas in Guadeloupe (the Bouillante geothermal field) and Martinique (Lamentin plain and the Diamant areas). While Li isotopic signatures of the geothermal fluids collected from deep reservoirs were found to be homogeneous for a given site, the δ7Li signatures for each of these reservoirs were significantly different. The first low temperature (25-250 °C) experiments of Li isotope exchange during seawater/basalt interaction confirmed that Li isotopic exchange is strongly temperature dependent, as previously inferred from natural studies. Li isotopic fractionation ranged from +19.4‰ (Δsolution-solid) at 25 °C to +6.7‰ at 250 °C. These experiments demonstrated the importance of Li isotopic fractionation during the formation of Li-bearing secondary minerals and allowed us to determine the following empirical relationship between isotopic fractionation and temperature: Δsolution-solid = 7847/T − 8.093. Application of experimental results and literature data to the Bouillante area suggested that geothermal water was in equilibrium at 250-260 °C. It likely has a deep and large reservoir located in the upper sheeted dike complex of the oceanic crust, just below the transition zone between andesite volcanic flows and the basaltic dikes. The upper dike section, from which Li is extracted by hydrothermal fluids, was characterized by light Li isotopic values in the rocks, indicating retention of 6Li by the altered rocks. For the Lamentin and Diamant areas, the geothermal fluids appeared to be in equilibrium with reservoir volcano-sedimentary rocks at 90-120 °C and 180 °C, respectively. Further evidence for this argument is provided by the fact that only the Na/Li thermometric relationship determined for sedimentary basins yielded temperature values in agreement with those measured or estimated for the reservoir fluids. This suggests the importance of a sedimentary signature in these reservoir rocks. Altogether, this study highlights that the use of Li isotopic systematics is a powerful tool for characterizing the origin of geothermal waters as well as the nature of their reservoir rocks.  相似文献   

19.
Strontium concentrations of 253 natural water samples from Skagafjördur, a Tertiary tholeiitic flood basalt region in northern Iceland range between 0.10 and 28 ppb. Surface environments (rivers, lakes, and peat soil waters) include the whole range of observed Sr concentrations whereas the Sr concentrations of ground waters are, in most cases, <3.5 ppb. Concentrations of Sr derived from basalt dissolution (i.e., rock-derived Sr) in waters of rivers and lakes exhibit a near linear correlation with the concentration of rock-derived Ca with a median molar Ca/Sr ratio of 1350. This systematic correlation suggests that Ca and Sr concentrations are controlled by weathering processes, i.e., the extent of dissolution of the basalt. The relative mobility of Sr during weathering in Skagafjördur is approximately half that of Ca, which is consistent with observed relative mobilities of these elements elsewhere in Iceland and in other basaltic regions. Peat soil waters commonly have lower concentrations of Sr and higher Ca concentrations than rivers and lakes, and molar ratios of rock-derived Ca to Sr in peat soil waters exhibit no systematic pattern. In several cases calculated concentrations of rock-derived Sr in peat soil waters yield negative values, suggesting a mineralogic sink for Sr in these waters.The low Sr concentrations in cold and thermal ground waters (<3.5 ppb) suggest mineralogic control over Sr in the ground water systems. Precipitation of secondary Sr minerals such as strontianite and celestite is ruled out as the ground waters are understaturated with respect to these minerals. Ground waters are characterized by high Ca/Sr molar ratios (∼5000 compared to bedrock Ca/Sr ratio of 730) suggesting that Sr is being preferentially incorporated (relative to Ca) into secondary minerals. The secondary minerals present in the bedrock in Skagafjördur that can preferentially incorporate Sr include zeolites, such as heulandite, chabazite, and thomsonite, and smectite. Ion-exchange calculations demonstrate that activities of Sr2+ and Ca2+ in ground water solutions in Skagafjördur are consistent with ion-exchange equilibria between these waters and heulandite from other Tertiary basalts in Iceland suggesting that this mineral may play an important role in controlling the concentration of Sr in the Skagafjördur ground waters. Incorporation of Sr into calcite cannot explain the observed high Ca/Sr ratios of the Skagafjördur ground waters because calcite, when precipitating, only admits limited amounts of Sr. Aragonite is not considered a likely candidate either because it has only very slight preference for Sr over Ca and ground waters above 40 °C are undersaturated with respect to this phase. However, predicted Sr content of calcite in equilibrium with the Skagafjördur ground waters (0.5-83 ppm Sr) is in good agreement with measured Sr content of this mineral in Tertiary basalts elsewhere in Iceland (<0.1-63 ppm), suggesting that the Skagafjördur ground waters can be used as analogues for Tertiary crustal solutions involved in the zeolite facies metamorphism of the Icelandic crust.  相似文献   

20.
The solubilities of the assemblages albite + paragonite + quartz and jadeite + paragonite + quartz in H2O were determined at 500 and 600 °C, 1.0-2.25 GPa, using hydrothermal piston-cylinder methods. The three minerals are isobarically and isothermally invariant in the presence of H2O, so fluid composition is uniquely determined at each pressure and temperature. A phase-bracketing approach was used to achieve accurate solubility determinations. Albite + quartz and jadeite + quartz dissolve incongruently in H2O, yielding residual paragonite which could not be retrieved and weighed. Solution composition fixed by the three-mineral assemblage at a given pressure and temperature was therefore bracketed by adding NaSi3O6.5 glass in successive experiments, until no paragonite was observed in run products. Solubilities derived from experiments bounding the appearance of paragonite thus constrain the equilibrium fluid composition. Results indicate that, at a given pressure, Na, Al, and Si concentrations are higher at 600 °C than at 500 °C. At both 500 and 600 °C, solubilities of all three elements increase with pressure in the albite stability field, to a maximum at the jadeite-albite-quartz equilibrium. In the jadeite stability field, element concentrations decline with continued pressure increase. At the solubility maximum, Na, Al, and Si concentrations are, respectively, 0.16, 0.05, and 0.48 molal at 500 °C, and 0.45, 0.27, and 1.56 molal at 600 °C. Bulk solubilities are 3.3 and 10.3 wt% oxides, respectively. Observed element concentrations are everywhere greater than those predicted from extrapolated thermodynamic data for simple ions, monomers, ion pairs, and the silica dimer. The measurements therefore require the presence of additional, polymerized Na-Al-Si-bearing species in the solutions. The excess solubility is >50% at all conditions, indicating that polymeric structures are the predominant solutes in the P-T region studied. The solubility patterns likely arise from combination of the large solid volume change associated with the albite-jadeite-quartz equilibrium and the rise in Na-Al-Si polymerization with approach to the hydrothermal melting curves of albite + quartz and jadeite + quartz. Our results indicate that polymerization of Na-Al-Si solutes is a fundamental aspect of fluid-rock interaction at high pressure. In addition, the data suggest that high-pressure metamorphic isograds can impose unexpected controls on metasomatic mass transfer, that significant metasomatic mass transfer prior to melting should be considered in migmatitic terranes, and that polymeric complexes may be an important transport agent in subduction zones.  相似文献   

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