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1.
The in situ redox potential (Eh) in anoxic groundwater with high methane and iron contents (approximately 12.3 and 28.4 mg/L, respectively) was potentiometrically measured to identify the processes that control Eh. The measured Eh ranged from −213 to −187 mV; it had an inverse correlation with the concentration of methane and no correlation with that of iron. The saturation indices indicate that goethite and amorphous FeS were nearly at solubility equilibrium. A comparison of the measured Eh with those calculated for the particular redox pairs indicates that either Fe2+/FeOOH or CH4/CO2, but not sulfur redox pairs, controlled the measured Eh. The inverse relationship between measured Eh and methane concentration suggests possible control of the redox conditions by the CH4/CO2 redox pair. Furthermore, the equilibrium solubility state of goethite, which has higher crystallinity and lower solubility than Fe(OH)3 indicates that the iron reaction was electrochemically irreversible. This further supports the contribution of the CH4/CO2 pair to controlling the measured Eh of groundwater.  相似文献   

2.
The geochemical and isotopic composition of surface waters and groundwater in the Velenje Basin, Slovenia, was investigated seasonally to determine the relationship between major aquifers and surface waters, water–rock reactions, relative ages of groundwater, and biogeochemical processes. Groundwater in the Triassic aquifer is dominated by HCO3 –, Ca2+, Mg2+ and δ13CDIC indicating degradation of soil organic matter and dissolution of carbonate minerals, similar to surface waters. In addition, groundwater in the Triassic aquifer has δ18O and δD values that plot near surface waters on the local and global meteoric water lines, and detectable tritium, likely reflecting recent (<50 years) recharge. In contrast, groundwater in the Pliocene aquifers is enriched in Mg2+, Na+, Ca2+, K+, and Si, and has high alkalinity and δ13CDIC values, with low SO4 2– and NO3 – concentrations. These waters have likely been influenced by sulfate reduction and microbial methanogenesis associated with coal seams and dissolution of feldspars and Mg-rich clay minerals. Pliocene aquifer waters are also depleted in 18O and 2H, and have 3H concentrations near the detection limit, suggesting these waters are older, had a different recharge source, and have not mixed extensively with groundwater in the Triassic aquifer.  相似文献   

3.
《Applied Geochemistry》2004,19(2):201-214
Detailed hydrochemical measurements, δ34SSO4 and 3H analyses were performed on 37 groundwater samples collected during February 1999, January and March 2000 from 6 locations in eastern and southeastern Bangladesh to examine redox processes that lead to As mobilization in groundwater. The study sites were chosen based on available nation-wide As surveys to span the entire spectrum of As concentrations in Bangladesh groundwater, and to represent 3 of 5 major geological units of the Ganges-Brahmaputra Delta: uplifted Pleistocene terrace, fluvial flood plain and delta plain. Arsenic was found to be mobilized under Fe-reducing conditions in shallow aquifers (<35 m depth), presumably of Holocene age. It remained mobile under SO4-reducing conditions, suggesting that authigenic sulfide precipitation does not constitute a significant sink for As in these groundwaters. The redox state of the water was characterized by a variety of parameters including dissolved O2, NO3−, Mn2+, Fe2+ concentrations, and SO42−/Cl− ratios. High dissolved [As] (> 50 μg/l; or > 0.7 μM ) were always accompanied by high dissolved [HCO3−] (> 4 mM), and were close to saturation with respect to calcite. Groundwater enriched in As (200–800 μg/l; or 2.7–10.7 μM) and phosphate (30–100 μM) but relatively low in dissolved Fe (5–40 μM) probably resulted from re-oxidation of reducing, As and Fe enriched water. This history was deduced from isotopic signatures of δ34SSO4 and 3H2O (3H) to delineate the nature of redox changes for some of the reducing groundwaters. In contrast, As is not mobilized in presumed Pleistocene aquifers, both shallow (30–60 m) and deep (150–270 m), because conditions were not reducing enough due to lack of sufficient O2 demand.  相似文献   

4.
Hydraulic fracturing of shale deposits has greatly increased the productivity of the natural gas industry by allowing it to exploit previously inaccessible reservoirs. Previous research has demonstrated that this practice has the potential to contaminate shallow aquifers with methane (CH4) from deeper formations. This study compares concentrations and isotopic compositions of CH4 sampled from domestic groundwater wells in Letcher County, Eastern Kentucky in order to characterize its occurrence and origins in relation to both neighboring hydraulically fractured natural gas wells and surface coal mines. The studied groundwater showed concentrations of CH4 ranging from 0.05 mg/L to 10 mg/L, thus, no immediate remediation is required. The δ13C values of CH4 ranged from −66‰ to −16‰, and δ2H values ranged from −286‰ to −86‰, suggesting an immature thermogenic and mixed biogenic/thermogenic origin. The occurrence of CH4 was not correlated with proximity to hydraulically fractured natural gas wells. Generally, CH4 occurrence corresponded with groundwater abundant in Na+, Cl−, and HCO3−, and with low concentrations of SO42−. The CH4 and SO42−concentrations were best predicted by the oxidation/reduction potential of the studied groundwater. CH4 was abundant in more reducing waters, and SO42− was abundant in more oxidizing waters. Additionally, groundwater in greater proximity to surface mining was more likely to be oxidized. This, in turn, might have increased the likelihood of CH4 oxidation in shallow groundwater.  相似文献   

5.
High arsenic (As) groundwater is widely distributed in northwestern Hetao Plain, an arid region with sluggish groundwater flow. Observed As concentration in groundwater from wells ranges from 76 to 1,093 μg/l. Most water samples have high total dissolved solids, with Cl and HCO3 as the dominant anions and Na as the dominant cation. The major hydrochemical types of most saline groundwaters are Na–Mg–Cl–HCO3 and Na–Mg–Cl. By contrast, fresh groundwaters generally belong to the Na–Mg–HCO3 type. High concentrations of arsenic in shallow aquifers are associated with strongly reducing conditions, as evidenced by high concentrations of dissolved organic carbon, ammonium, as well as dissolved sulfide and Fe, dominance of arsenite, relatively low concentrations of nitrate and sulfate, and occasionally high content of dissolved methane (CH4). High As groundwaters from different places at Hetao Plain experienced different redox processes. Fluoride is also present in high As groundwater, ranging between 0.40 and 3.36 mg/l. Although fluorosis poses an additional health problem in the region, it does not correlate well with As in spatial distribution. Geochemical analysis indicates that evapotranspiration is an important process controlling the enrichment of Na and Cl, as well as trace elements such as As, B, and Br in groundwater. Electronic supplementary material  The online version of this article (doi:) contains supplementary material, which is available to authorized users.  相似文献   

6.
In the Pine Creek Geosyncline, fast moving, annually recharged, low-salinity ground waters dissolve uranium- and magnesium-enriched gangue minerals from mineralized aquifer rocks. The level of dissolved uranium depends on prevailing pH, Eh, salinity and degree of adsorption, which limits its effectiveness as an exploration indicator. Near each known deposit, leaching of magnesium-enriched gangue minerals produces ground waters with very similar major-element concentration plots, the shape of which constitutes a mineralized aquifer “signature”. Gangue minerals also supply high levels of Mg2+ (expressed as NMg = [Mg2+]/[Ca2+ + Mg2+ + Na+ + K+] in milliequivalents per litre) to contained ground waters, NMg > 0.8 being common in ground waters from mineralized aquifers at each Pine Creek Geosyncline deposit. Data from Ranger One No. 3 ore body illustrates how progressive mixing of waters from mineralized and unmineralized aquifers causes graded reductions in NMg, which, when plotted onto a ground plan, delineate a hydrogeochemical aureole.High NMg (> 0.8) coincides with high uranium concentration (> 20 μg/l of U) in ground waters near Nabarlek and Ranger. Because pH-Eh conditions in aquifers at Jabiluka depress uranium solution, < 10 μg/l of U is present, although NMg values are generally > 0.8. To date NMg has always been < 0.8 in nonmineralized aquifer waters, whereas uranium may be > 50 μg/l in ground waters from felsic igneous aquifers, which can be identified as uneconomic by low (< 0.4) NMg, and by a fixed relationship between uranium and co-leached species such as F- and soluble salts.Measurements of pH, Eh, salinity, Fe(II), Ca, Mg, Na, K, Cl, SO4, total carbonate, phosphate, F-, Cu, Pb, Zn and U in waters from 48 percussion holes in and near the Koongarra ore bodies have been related to mineralogy recorded in drill logs. The composition of waters from 20 holes near and along strike from known mineralization, fitted the mineralized aquifer “signature”, had NMg > 0.8 and uranium up to 4100 μ/l. These data confirm the use in this region of NMg as a hydrogeochemical indicator of uranium mineralization; they also indicate additional zones of possible mineralization.  相似文献   

7.
The semi-arid Sahel regions of West Africa rely heavily on groundwater from shallow to moderately deep(100 m b.g.l.)crystalline bedrock aquifers for drinking water production.Groundwater quality may be affected by high geogenic arsenic(As)concentrations(10μg/L)stemming from the oxidation of sulphide minerals(pyrite,arsenopyrite)in mineralised zones.These aquifers are still little investigated,especially concerning groundwater residence times and the influence of the annual monsoon season on groundwater chemistry.To gain insights on the temporal aspects of As contamination,we have used isotope tracers(noble gases,~3H,stable water isotopes(~2 H,~(18)O))and performed hydrochemical analyses on groundwater abstracted from tube wells and dug wells in a small study area in southwestern Burkina Faso.Results revealed a great variability in groundwater properties(e.g.redox conditions,As concentrations,water level,residence time)over spatial scales of only a few hundred metres,characteristic of the highly heterogeneous fractured underground.Elevated As levels are found in oxic groundwater of circum-neutral pH and show little relation with any of the measured parameters.Arsenic concentrations are relatively stable over the course of the year,with little effect seen by the monsoon.Groundwater residence time does not seem to have an influence on As concentrations,as elevated As can be found both in groundwater with short(50 a)and long(10~3 a)residence times as indicated by ~3He/~4He ratios spanning three orders of magnitude.These results support the hypothesis that the proximity to mineralised zones is the most crucial factor controlling As concentrations in the observed redox/pH conditions.The existence of very old water portions with residence times10~3 years already at depths of50 m b.g.l.is a new finding for the shallow fractured bedrock aquifers of Burkina Faso,suggesting that overexploitation of these relatively low-yielding aquifers may be an issue in the future.  相似文献   

8.
Sediment and groundwater profiles were compared in two villages of Bangladesh to understand the geochemical and hydrogeological factors that regulate dissolved As concentrations in groundwater. In both villages, fine-grained sediment layers separate shallow aquifers (< 28 m) high in As from deeper aquifers (40-90 m) containing < 10 μg/L As. In one village (Dari), radiocarbon dating indicates deposition of the deeper aquifer sediments > 50 ka ago and a groundwater age of thousands of years. In the other village (Bay), the sediment is < 20 ka old down to 90 m and the deeper aquifer groundwater is younger, on the order of hundreds of years. The shallow aquifers in both villages that are high in As contain bomb-3H and bomb-14C, indicating recent recharge. The major and minor ion compositions of the shallow and deeper aquifers also differ significantly. Deeper aquifer water is of the Na+-HCO3- type, with relatively little dissolved NH4+ (76 ± 192 μmol/L), Fe (27 ± 43 μmol/L) and Mn (3 ± 2 μmol/L). In contrast, shallow aquifer water is of the Ca2+-Mg2+-HCO3- type, with elevated concentrations of dissolved NH4+ (306 ± 355 μmol/L), Fe (191 ± 73 μmol/L), and Mn (27 ± 43 μmol/L). In both villages, the quantity of As extractable from deeper aquifer sands with a 1 mol/L phosphate solution (0.2 ± 0.3 mg/kg, n = 12; 0.1 ± 0.1 mg/kg, n = 5) is 1 order of magnitude lower than P-extractable As from shallow deposits (1.7 ± 1.2 mg/kg, n = 9; 1.4 ± 2.0 mg/kg, n = 11). The differences suggest that the concentration of P-extractable As in the sediment is a factor controlling the concentration of As in groundwater. Low P-extractable As levels are observed in both deeper aquifers that are low in As, even though there is a large difference in the time of deposition of these aquifers in the two villages. The geochemical data and hydrographs presented in this study suggest that both Holocene and Pleistocene deeper aquifers that are low in As should be a viable source of drinking water as long as withdrawals do not exceed recharge rates of ∼1 cm/yr.  相似文献   

9.
High concentrations of U and226Ra, and elevated234U/238U activity ratios have been measured in groundwater samples collected from water supply wells and exploratory boreholes in the area surrounding the Underground Research Laboratory (URL) of Atomic Energy of Canada Limited, in southeastern Manitoba. All groundwaters come from the Lac du Bonnet granite batholith or sediments overlying the batholith.Uranium concentrations attain almost 1 mg/l in some shallow, low-salinity groundwaters, whereas226Ra tends to be high (up to 38 Bq/l) in deeper, saline waters. The U concentrations are some of the highest observed in global groundwaters, yet no significant ore body or mineralization is known in the area. Analyses of unaltered rock samples of the Lac du Bonnet granite show slight U enrichment over average Canadian Shield granites (6.5 μg/g vs 4 μg/g), and altered wall rock in fracture zones is enriched in U by up to an order of magnitude compared to adjacent bedrock. Low234U/238U activity ratios in this altered rock indicate active and recent leaching of U by groundwater.The key control on U concentration appears to be redox potential. Concentrations of U in rock, residence time and groundwater composition are of lesser importance. Geochemical modelling of the shallower, oxidized waters indicates that U speciation consists mainly of anionic carbonate complexes of the uranyl ion. This is supported by the remarkable efficiency of an anionic filter developed to remove high levels of U from drinking water in the area.In more reducing groundwaters, U concentrations are similar to those determined in recent experimental work on uraninite solubility in the pH range 7–8.5. Colloidal U is <10% of total U and organic complexation is unlikely to be significant because of low dissolved organic concentrations. The results emphasize the significance of redox potential in controlling U mobility in both oxidizing and reducing environments and indicate the usefulness of U concentration in estimating groundwater Eh.  相似文献   

10.
内蒙古河套平原典型高砷区地下水中砷的演化规律   总被引：1，自引：1，他引：0       下载免费PDF全文
通过对高砷地下水典型区完整地质单元不同深度含水层地下水进行监测,分析了与砷释放、迁移和富集有关的敏感因素（水位、Eh、总铁、亚铁等）的时间和空间变化规律,探讨了高砷地下水的形成机理。结果发现,地下水灌溉区和黄河水灌溉区,地下水水位均受人为灌溉活动的影响。地下水砷含量在空间和时间尺度上发生有规律的变化。在空间尺度上,地下水中砷含量随着深度的增加而升高,井深小于10 m的地下水砷含量在1.88～2.58 μg/L;井深在10~15 m之间的地下水中砷含量在18.2～217 μg/L;井深在15~25 m之间的地下水中砷含量在38.3～226 μg/L。受人为灌溉影响,地下水中砷的含量会随着地下水位的抬升而升高。地下水砷含量随时间变化的原因是水位抬升使水位变化造成氧化还原环境改变。地下水系统中含砷铁氧化物矿物的还原性溶解、脱硫酸作用等是控制地下水砷含量的主要水文地球化学过程。  相似文献   

11.
Water wells were sampled near North Madison, Ohio, following a gas well blow out that injected large amounts of CH4 into near-surface groundwater Chemical analyses showed elevated levels of Fe+2, Mn+2, Ca+2, sulfide, alkalinity, and pH, and low levels of dissolved oxygen, SO4 −2, and NO3 − in CH4-affected wells compared to unaffected wells. Sulfate reduction is quantitatively the most important vehicle for CH4 oxidation Equilibrium thermodynamic computer models were used to simulate groundwaters from the North Madison area Model results showed that CH4 is oxidized to HCO3 −, SO4 −2 is reduced, iron and manganese oxides are reduced and dissolved, and pH increases These simulations are in excellent agreement with trends observed in the field data A laboratory experiment was designed to simulate CH4 − perturbed groundwater in the methane-perturbed system, sulfide increased significantly, providing direct evidence for methane oxidation by sulfate reduction Although suitable anaerobic methane-oxidizing bacteria have not been isolated from groundwater aquifers, the combination of field data, laboratory experiment, and computer simulation form a convincing argument that CH4 perturbation of aquifers can and does affect groundwater chemistry  相似文献   

12.
Arsenic and Antimony in Groundwater Flow Systems: A Comparative Study   总被引：3，自引：0，他引：3  
Arsenic (As) and antimony (Sb) concentrations and speciation were determined along flow paths in three groundwater flow systems, the Carrizo Sand aquifer in southeastern Texas, the Upper Floridan aquifer in south-central Florida, and the Aquia aquifer of coastal Maryland, and subsequently compared and contrasted. Previously reported hydrogeochemical parameters for all three aquifer were used to demonstrate how changes in oxidation–reduction conditions and solution chemistry along the flow paths in each of the aquifers affected the concentrations of As and Sb. Total Sb concentrations (SbT) of groundwaters from the Carrizo Sand aquifer range from 16 to 198 pmol kg−1; in the Upper Floridan aquifer, SbT concentrations range from 8.1 to 1,462 pmol kg−1; and for the Aquia aquifer, SbT concentrations range between 23 and 512 pmol kg−1. In each aquifer, As and Sb (except for the Carrizo Sand aquifer) concentrations are highest in the regions where Fe(III) reduction predominates and lower where SO4 reduction buffers redox conditions. Groundwater data and sequential analysis of the aquifer sediments indicate that reductive dissolution of Fe(III) oxides/oxyhydroxides and subsequent release of sorbed As and Sb are the principal mechanism by which these metalloids are mobilized. Increases in pH along the flow path in the Carrizo Sand and Aquia aquifer also likely promote desorption of As and Sb from mineral surfaces, whereas pyrite oxidation mobilizes As and Sb within oxic groundwaters from the recharge zone of the Upper Floridan aquifer. Both metalloids are subsequently removed from solution by readsorption and/or coprecipitation onto Fe(III) oxides/oxyhydroxides and mixed Fe(II)/Fe(III) oxides, clay minerals, and pyrite. Speciation modeling using measured and computed Eh values predicts that Sb(III) predominate in Carrizo Sand and Upper Floridan aquifer groundwaters, occurring as the Sb(OH)30 species in solution. In oxic groundwaters from the recharge zones of these aquifers, the speciation model suggests that Sb(V) occurs as the negatively charged Sb(OH)6− species, whereas in sufidic groundwaters from both aquifers, the thioantimonite species, HSb2S4 − and Sb2S4 2−, are predicted to be important dissolved forms of Sb. The measured As and Sb speciation in the Aquia aquifer indicates that As(III) and Sb(III) predominate. Comparison of the speciation model results based on measured Eh values, and those computed with the Fe(II)/Fe(III), S(-II)/SO4, As(III)/As(V), and Sb(III)/Sb(V) couples, to the analytically determined As and Sb speciation suggests that the Fe(II)/Fe(III), S(-II)/SO4 couples exert more control on the in situ redox condition of these groundwaters than either metalloid redox couple.  相似文献   

13.
《Applied Geochemistry》2004,19(6):937-946
Analysis of stable isotopes and major ions in groundwater and surface waters in Belize, Central America was carried out to identify processes that may affect drinking water quality. Belize has a subtropical rainforest/savannah climate with a varied landscape composed predominantly of carbonate rocks and clastic sediments. Stable oxygen (δ18O) and hydrogen (δD) isotope ratios for surface and groundwater have a similar range and show high d-excess (10–40.8‰). The high d-excess in water samples suggest secondary continental vapor flux mixing with incoming vapor from the Caribbean Sea. Model calculations indicate that moisture derived from continental evaporation contributes 13% to overhead vapor load. In surface and groundwater, concentrations of dissolved inorganic carbon (DIC) ranged from 5.4 to 112.9 mg C/l and δ13CDIC ranged from −7.4 to −17.4‰. SO42, Ca2+ and Mg2+ in the water samples ranged from 2–163, 2–6593 and 2–90 mg/l, respectively. The DIC and δ13CDIC indicate both open and closed system carbonate evolution. Combined δ13CDIC and Ca2+, Mg2+, and SO42− suggest additional groundwater evolution by gypsum dissolution and calcite precipitation. The high SO42−content of some water samples indicates regional geologic control on water quality. Similarity in the range of δ18O, δD and δ13CDIC for surface waters and groundwater used for drinking water supply is probably due to high hydraulic conductivities of the karstic aquifers. The results of this study indicate rapid recharge of groundwater aquifers, groundwater influence on surface water chemistry and the potential of surface water to impact groundwater quality and vise versa.  相似文献   

14.
Natural gas reservoirs in organic-rich shales in the Appalachian and Michigan basins in the United States are currently being produced via hydraulic fracturing. Stratigraphically-equivalent shales occur in the Canadian portion of the basins in southwestern Ontario with anecdotal evidence of gas shows, yet there has been no commercial shale gas production to date. To provide baseline data in the case of future environmental issues related to hydraulic fracturing and shale gas production, such as leakage of natural gas, saline water, and/or hydraulic fracturing fluids, and to evaluate hydrogeochemical controls on natural gas accumulations in shallow groundwater in general, this study investigates the origin and distribution of natural gas and brine in shallow aquifers across southwestern Ontario. An extensive geochemical database of major ion and trace metal chemistry and methane concentrations of 1010 groundwater samples from shallow, domestic wells in bedrock and overburden aquifers throughout southwestern Ontario was utilized. In addition, select wells (n = 36) were resampled for detailed dissolved gas composition, δ13C of CH4, C2, C3, and CO2, and δD of CH4. Dissolved gases in groundwater from bedrock and overburden wells were composed primarily of CH4 (29.7–98.6 mol% of total gas volume), N2 (0.8–66.2 mol%), Ar + O2 (0.2–3.4 mol%), and CO2 (0–1.2 mol%). Ethane was detected, but only in low concentrations (<0.041 mol%), and no other higher chain hydrocarbons were present, except for one well in overburden overlying the Dundee Formation, which contained 0.81 mol% ethane and 0.21 mol% propane. The highest methane concentrations (30 to >100 in situ % saturation) were found in bedrock wells completed in the Upper Devonian Kettle Point Formation, Middle Devonian Hamilton Group and Dundee Formation, and in surficial aquifers overlying these organic-rich shale-bearing formations, indicating that bedrock geology is the primary control on methane occurrences. A few (n = 40) samples showed Na–Cl–Br evidence of brine mixing with dilute groundwater, however only one of these samples contained high (>60 in situ % saturation) CH4. The relatively low δ13C values of CH4 (−89.9‰ to −57.3‰), covariance of δD values of CH4 and H2O, positive correlation between δ13C values of CH4 and CO2, and lack of higher chain hydrocarbons (C3+) in all but one dissolved gas sample indicates that the methane in groundwater throughout the study area is primarily microbial in origin. The presence or absence of alternative electron acceptors (e.g. dissolved oxygen, Fe, NO3, SO4), in addition to organic substrates, controls the occurrence of microbial CH4 in shallow aquifers. Microbial methane has likely been accumulating in the study area, since at least the Late Pleistocene to the present, as indicated by the co-variance and range of δD values of CH4 (−314‰ to −263‰) and associated groundwater (−19‰ to −6‰ δD-H2O).  相似文献   

15.
《Applied Geochemistry》2002,17(5):517-568
The range of As concentrations found in natural waters is large, ranging from less than 0.5 μg l−1 to more than 5000 μg l−1. Typical concentrations in freshwater are less than 10 μg l−1 and frequently less than 1 μg l−1. Rarely, much higher concentrations are found, particularly in groundwater. In such areas, more than 10% of wells may be ‘affected’ (defined as those exceeding 50 μg l−1) and in the worst cases, this figure may exceed 90%. Well-known high-As groundwater areas have been found in Argentina, Chile, Mexico, China and Hungary, and more recently in West Bengal (India), Bangladesh and Vietnam. The scale of the problem in terms of population exposed to high As concentrations is greatest in the Bengal Basin with more than 40 million people drinking water containing ‘excessive’ As. These large-scale ‘natural’ As groundwater problem areas tend to be found in two types of environment: firstly, inland or closed basins in arid or semi-arid areas, and secondly, strongly reducing aquifers often derived from alluvium. Both environments tend to contain geologically young sediments and to be in flat, low-lying areas where groundwater flow is sluggish. Historically, these are poorly flushed aquifers and any As released from the sediments following burial has been able to accumulate in the groundwater. Arsenic-rich groundwaters are also found in geothermal areas and, on a more localised scale, in areas of mining activity and where oxidation of sulphide minerals has occurred. The As content of the aquifer materials in major problem aquifers does not appear to be exceptionally high, being normally in the range 1–20 mg kg−1. There appear to be two distinct ‘triggers’ that can lead to the release of As on a large scale. The first is the development of high pH (>8.5) conditions in semi-arid or arid environments usually as a result of the combined effects of mineral weathering and high evaporation rates. This pH change leads either to the desorption of adsorbed As (especially As(V) species) and a range of other anion-forming elements (V, B, F, Mo, Se and U) from mineral oxides, especially Fe oxides, or it prevents them from being adsorbed. The second trigger is the development of strongly reducing conditions at near-neutral pH values, leading to the desorption of As from mineral oxides and to the reductive dissolution of Fe and Mn oxides, also leading to As release. Iron (II) and As(III) are relatively abundant in these groundwaters and SO4 concentrations are small (typically 1 mg l−1 or less). Large concentrations of phosphate, bicarbonate, silicate and possibly organic matter can enhance the desorption of As because of competition for adsorption sites. A characteristic feature of high groundwater As areas is the large degree of spatial variability in As concentrations in the groundwaters. This means that it may be difficult, or impossible, to predict reliably the likely concentration of As in a particular well from the results of neighbouring wells and means that there is little alternative but to analyse each well. Arsenic-affected aquifers are restricted to certain environments and appear to be the exception rather than the rule. In most aquifers, the majority of wells are likely to be unaffected, even when, for example, they contain high concentrations of dissolved Fe.  相似文献   

16.
Twenty-two bottled mineral and spring waters from Norway, Sweden, Finland and Iceland have been analysed for 71 inorganic chemical parameters with low detection limits as a subset of a large European survey of bottled groundwater chemistry (N = 884). The Nordic bottled groundwaters comprise mainly Ca–Na–HCO3–Cl water types, but more distinct Ca–HCO3, Na HCO3 and Na–Cl water types are also offered. The distributions for most elements fall between groundwater from Fennoscandian Quaternary unconsolidated aquifers and groundwater from Norwegian crystalline bedrock boreholes. Treated tap waters have slightly lower median values for many parameters, but elements associated with plumbing have significantly higher concentrations in tap waters than in bottled waters. The small dataset is able to show that excessive fluoride and uranium contents are potential drinking water problems in Fennoscandia. Nitrate and arsenic displayed low to moderate concentrations, but the number of samples from Finland and Northern Sweden was too low to detect that elevated concentrations of arsenic occur in bedrock boreholes in some regions. The data shows clearly that water sold in plastic bottles is contaminated with antimony. Antimony is toxic and suspected to be carcinogenic, but the levels are well below the EU drinking water limit. The study does not provide any health-based arguments for buying bottled mineral and spring waters for those who are served with drinking water from public waterworks. Drinking water from crystalline bedrock aquifers should be analysed. In case of elevated concentrations of fluoride, uranium or arsenic, most bottled waters, but not all, will be better alternatives when treatment of the well water is not practicable.  相似文献   

17.
《Applied Geochemistry》2003,18(9):1453-1477
Observed As concentrations in groundwater from boreholes and wells in the Huhhot Basin of Inner Mongolia, northern China, range between <1 μg l−1 and 1480 μg l−1. The aquifers are composed of Quaternary (largely Holocene) lacustrine and fluvial sediments. High concentrations are found in groundwater from both shallow and deep boreholes as well as from some dug wells (well depths ranging between <10 m and 400 m). Populations from the affected areas experience a number of As-related health problems, the most notable of which are skin lesions (keratosis, melanosis, skin cancer) but with internal cancers (lung and bladder cancer) also having been reported. In both the shallow and deep aquifers, groundwaters evolve down the flow gradient from oxidising conditions along the basin margins to reducing conditions in the low-lying central part of the basin. High As concentrations occur in anaerobic groundwaters from this low-lying area and are associated with moderately high dissolved Fe as well as high Mn, NH4, dissolved organic C (DOC), HCO3 and P concentrations. Many of the deep groundwaters have particularly enriched DOC concentrations (up to 30 mg l−1) and are often brown as a result of the high concentrations of organic acid. In the reducing groundwaters, inorganic As(III) constitutes typically more than 60% of the total dissolved As. The highest As concentrations tend to be found in groundwater with low SO4 concentrations and indicate that As mobilisation occurs under strongly reducing conditions, where SO4 reduction has been an active process. High concentrations of Fe, Mn, NH4, HCO3 and P are a common feature of reducing high-As groundwater provinces (e.g. Bangladesh, West Bengal). High concentrations of organic acid (humic, fulvic acid) are not a universal feature of such aquifers, but have been found in groundwaters from Taiwan and Hungary for example. The observed range of total As concentrations in sediments is 3–29 mg kg−1 (n=12) and the concentrations correlate positively with total Fe. Up to 30% of the As is oxalate-extractable and taken to be associated largely with Fe oxides. The release of As into solution under the reducing conditions is believed to be by desorption coupled with reductive dissolution of the Fe oxide minerals. The association of dissolved As with constituents such as HCO3, DOC and P may be a coincidence related to the prevalent reducing conditions and slow groundwater flow, but they may also be directly involved because of their competition with As for binding sites on the Fe oxides. The Huhhot groundwaters also have some high concentrations of dissolved U (up to 53 μg l−1) and F− (up to 6.8 mg l−1). In contrast to As, U occurs predominantly under the more oxidising conditions along the basin margins. Fluoride occurs dominantly in the shallow groundwaters which have Na and HCO3 as the dominant ions. The combination of slow flow of groundwater and the young age of the aquifer sediments are also considered potentially important causes of the high dissolved As concentrations observed as the sediments are likely to contain newly-formed and reactive minerals and have not been well flushed since burial.  相似文献   

18.
In this study a typical coastal karst aquifer, developed in lower Cretaceous limestones, on the western Mediterranean seashore (La Clape massif, southern France) was investigated. A combination of geochemical and isotopic approaches was used to investigate the origin of salinity in the aquifer. Water samples were collected between 2009 and 2011. Three groundwater groups (A, B and C) were identified based on the hydrogeological setting and on the Cl− concentrations. Average and maximum Cl− concentrations in the recharge waters were calculated (ClRef. and ClRef.Max) to be 0.51 and 2.85 mmol/L, respectively). Group A includes spring waters with Cl− concentrations that are within the same order of magnitude as the ClRef concentration. Group B includes groundwater with Cl− concentrations that range between the ClRef and ClRef.Max concentrations. Group C includes brackish groundwater with Cl− concentrations that are significantly greater than the ClRef.Max concentration. Overall, the chemistry of the La Clape groundwater evolves from dominantly Ca–HCO3 to NaCl type. On binary diagrams of the major ions vs. Cl, most of the La Clape waters plot along mixing lines. The mixing end-members include spring waters and a saline component (current seawater or fossil saline water). Based on the Br/Clmolar ratio, the hypothesis of halite dissolution from Triassic evaporites is rejected to explain the origin of salinity in the brackish groundwater.Groundwaters display 87Sr/86Sr ratios intermediate between those of the limestone aquifer matrix and current Mediterranean seawater. On a Sr mixing diagram, most of the La Clape waters plot on a mixing line. The end-members include the La Clape spring waters and saline waters, which are similar to the deep geothermal waters that were identified at the nearby Balaruc site. The 36Cl/Cl ratios of a few groundwater samples from group C are in agreement with the mixing hypothesis of local recharge water with deep saline water at secular equilibrium within a carbonate matrix. Finally, PHREEQC modelling was run based on calcite dissolution in an open system prior to mixing with the Balaruc type saline waters. Modelled data are consistent with the observed data that were obtained from the group C groundwater. Based on several tracers (i.e. concentrations and isotopic compositions of Cl and Sr), calculated ratios of deep saline water in the mixture are coherent and range from 3% to 16% and 0% to 3% for groundwater of groups C and B, respectively.With regard to the La Clape karst aquifer, the extension of a lithospheric fault in the study area may favour the rise of deep saline water. Such rises occur at the nearby geothermal Balaruc site along another lithospheric fault. At the regional scale, several coastal karst aquifers are located along the Gulf of Lion and occur in Mezosoic limestones of similar ages. The 87Sr/86Sr ratios of these aquifers tend toward values of 0.708557, which suggests a general mixing process of shallow karst waters with deep saline fossil waters. The occurrence of these fossil saline waters may be related to the introduction of seawater during and after the Flandrian transgression, when the highly karstified massifs invaded by seawater, formed islands and peninsulas along the Mediterranean coast.  相似文献   

19.
《Applied Geochemistry》2005,20(2):423-441
An investigation of a childhood leukemia cluster by US Centers for Disease Control and Prevention revealed that residents of the Carson Desert, Nevada, are exposed to high levels of W and this prompted an investigation of W in aquifers used as drinking water sources. Tungsten concentrations in 100 ground water samples from all aquifers used as drinking water sources in the area ranged from 0.27 to 742 μg/l. Ground water in which W concentrations exceed 50 μg/l principally occurs SE of Fallon in a geothermal area. The principal sources of W in ground water are natural and include erosion of W-bearing mineral deposits in the Carson River watershed upstream of Fallon, and, possibly, upwelling geothermal waters. Ground water in the Fallon area is strongly reducing and reductive dissolution of Fe and Mn oxyhydroxides may be releasing W; however, direct evidence that the metal oxides contain W is not available.Although W and Cl concentrations in the Carson River, a lake, and water from many wells, appear to be controlled by evaporative concentration, evaporation alone cannot explain the elevated W concentrations found in water from some of the wells. Concentrations of W exceeding 50 μg/l are exclusively associated with Na–HCO3 and Na–Cl water types and pH > 8.0; in these waters, geochemical modeling indicates that W exhibits <10% adsorption. Tungsten concentrations are strongly and positively correlated with As, B, F, and P, indicating either common sources or common processes controlling their concentrations. Geochemical modeling indicates W concentrations are consistent with pH-controlled adsorption of W.The geochemical model PHREEQC was used to calculate IAP values, which were compared with published Ksp values for primary W minerals. FeWO4, MnWO4, Na2WO4, and MgWO4 were undersaturated and CaWO4 and SrWO4 were approaching saturation. These conclusions are tentative because of uncertainty in the thermodynamic data.The similar behavior of As and W observed in this study suggests ground water in areas where elevated As concentrations are present also may contain elevated W concentrations, particularly if there is a mineral or geothermal source of W and reducing conditions develop in the aquifer.  相似文献   

20.
Twenty-nine wells were selected for groundwater sampling in the town of Shahai, in the Hetao basin, Inner Mongolia. Four multilevel samplers were installed for monitoring groundwater chemistry at depths of 2.5–20 m. Results show that groundwater As exhibits a large spatial variation, ranging between 0.96 and 720 μg/L, with 71% of samples exceeding the WHO drinking water guideline value (10 μg/L). Fluoride concentrations range between 0.30 and 2.57 mg/L. There is no significant correlation between As and F− concentrations. Greater As concentrations were found with increasing well depth. However, F− concentrations do not show a consistent trend with depth. Groundwater with relatively low Eh has high As concentrations, indicating that the reducing environment is the major factor controlling As mobilization. Low As concentrations (<10 μg/L) are found in groundwater at depths less than 10 m. High groundwater As concentration is associated with aquifers that have thick overlying clay layers. The clay layers, mainly occurring at depths <10 m, have low permeability and high organic C content. These strata restrict diffusion of atmospheric O2 into the aquifers, and lead to reducing conditions that favor As release. Sediment composition is an additional factor in determining dissolved As concentrations. In aquifers composed of yellowish-brown fine sands at depths around 10 m, groundwater generally has low As concentrations which is attributed to the high As adsorption capacity of the yellow–brown Fe oxyhydroxide coatings. Fluoride concentration is positively correlated with pH and negatively correlated with Ca2+ concentration. All groundwater samples are over-saturated with respect to calcite and under-saturated with respect to fluorite. Dissolution and precipitation of Ca minerals (such as fluorite and calcite), and F− adsorption–desorption are likely controlling the concentration of F− in groundwater.  相似文献   

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