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1.
《Applied Geochemistry》2004,19(2):231-243
In large parts of rural Argentina people depend on groundwater whose As content exceeds the Argentine drinking water standards (0.05 mg l−1). The most affected areas are located in the Chaco-Pampean Plain, where aquifers comprise Tertiary loess deposits (in the Pampean Plain) and Tertiary and Quaternary fluvial and aeolian sediments (in the Chaco Plain). Robles county is located in the alluvial cone of the Dulce River consisting of loess (aeolian), and gravel, silt, sand and clay (alluvial) deposits. In the shallow aquifers, more than 48% of the 63 studied wells show As at toxic levels (maximum 4.8 mg l−1), while in the deep groundwater the concentration is below 0.05 mg l−1. The pH of the shallow groundwaters range between 6.5 and 9 and generally have high electrical conductivity with mean values of 2072 and 1693 μS/cm−1 in the years 1998 and 1999, respectively. Arsenic concentrations are high in the alkaline Na–HCO3 type groundwaters, where As correlates positively with Na+ and HCO3−. Moreover, As correlates positively with Mo, U, and V, while a negative correlation was observed with Ca2+ and Mg2+. The potential sources of groundwater As are: (i) layers of volcanic ash with 90% of rhyolitic glass; (ii) volcanic glass dispersed in the sediments; and (iii) clastic sediments of metamorphic and igneous origin. Great lateral variability in the concentration of groundwater As is caused by several hydrogeological and hydrogeochemical factors.  相似文献   

2.
《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   

3.
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   

4.
《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   

5.
《Applied Geochemistry》2002,17(3):259-284
Groundwaters from Quaternary loess aquifers in northern La Pampa Province of central Argentina have significant quality problems due to high concentrations of potentially harmful elements such as As, F, NO3-N, B, Mo, Se and U and high salinity. The extent of the problems is not well-defined, but is believed to cover large parts of the Argentine Chaco-Pampean Plain, over an area of perhaps 106 km2. Groundwaters from La Pampa have a very large range of chemical compositions and spatial variability is considerable over distances of a few km. Dissolved As spans over 4 orders of magnitude (<4–5300 μg l−1) and concentrations of F have a range of 0.03–29 mg l−1, B of 0.5–14 mg l−l, V of 0.02–5.4 mg l−1, NO3–N of <0.2–140 mg l−1, Mo of 2.7–990 μg l−1 and U of 6.2–250 μg l−1. Of the groundwaters investigated, 95% exceed 10 μg As l−1 (the WHO guideline value) and 73% exceed 50 μg As l−1 (the Argentine national standard). In addition, 83% exceed the WHO guideline value for F (1.5 mg l−1), 99% for B (0.5 mg l−1), 47% for NO3-N (11.3 mg l−1), 39% for Mo (70 μg l−1), 32% for Se (10 μg l−1) and 100% for U (2 μg l−1). Total dissolved solids range between 730 and 11400 mg l−1, the high values resulting mainly from evaporation under ambient semi-arid climatic conditions. The groundwaters are universally oxidising with high dissolved-O2 concentrations. Groundwater pHs are neutral to alkaline (7.0–8.7). Arsenic is present in solution predominantly as As(V). Groundwater As correlates positively with pH, alkalinity (HCO3), F and V. Weaker correlations are also observed with B, Mo, U and Be. Desorption of these elements from metal oxides, especially Fe and Mn oxides under the high-pH conditions is considered an important control on their mobilisation. Mutual competition between these elements for sorption sites on oxide minerals may also have enhanced their mobility. Weathering of primary silicate minerals and accessory minerals such as apatite in the loess and incorporated volcanic ash may also have contributed a proportion of the dissolved As and other trace elements. Concentrations of As and other anions and oxyanions appear to be particularly high in groundwaters close to low-lying depressions which act as localised groundwater-discharge zones. Concentrations up to 7500 μg l−1 were found in saturated-zone porewaters extracted from a cored borehole adjacent to one such depression. Concentrations are also relatively high where groundwater is abstracted from close to the water table, presumably because this zone is a location of more active weathering reactions. The development of groundwaters with high pH and alkalinity results from silicate and carbonate reactions, facilitated by the arid climatic conditions. These factors, together with the young age of the loess sediments and slow groundwater flow have enabled the accumulation of the high concentrations of As and other elements in solution without significant opportunity for flushing of the aquifer to enable their removal.  相似文献   

6.
An integrated study has been carried out to elucidate the distribution and occurrence of arsenic in selected groundwater samples in the area of Sherajdikhan, Bangladesh. Arsenic and other parameters (T, pH, EC, Na+, K+, Ca2+, Mg2+, Cl−, NO3 −, SO4 2−, HCO3 −, PO4 3−, Fe, Mn and DOC) have been measured in groundwater samples collected from shallow/deep tube wells at different depths. Hydrogeochemical data suggest that the groundwaters are generally Ca–Mg–HCO3 and Mg–Ca–HCO3 types with bicarbonate (HCO3 −) as the dominant anion, though the other type of water has also been observed. Dissolved arsenic in groundwater ranged from 0.006 to 0.461 mg/l, with 69% groundwater samples exceeded the Bangladesh limit for safe drinking water (0.05 mg/l). Correlation and principal component analysis have been performed to find out possible relationships among the examined parameters in groundwater. Low concentrations of NO3 − and SO4 2−, and high concentrations of DOC, HCO3 − and PO4 3− indicate the reducing condition of subsurface aquifer where sediments are deposited with abundant organic matter. Distinct relationship of As with Fe and Mn, and strong correlation with DOC suggests that the biodegradation of organic matter along with reductive dissolution of Fe–Mn oxyhydroxides has being considered the dominant process to release As in the aquifers studied herein.  相似文献   

7.
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8.
《Applied Geochemistry》2005,20(5):989-1016
Groundwater from the Quaternary loess aquifer of La Pampa, central Argentina, has significant problems with high concentrations of As (up to 5300 μg L−1) as well as other potentially toxic trace elements such as F, B, Mo, U, Se and V. Total As concentrations in 45 loess samples collected from the aquifer have a range of 3–18 mg kg−1 with a mean of 8 mg kg−1. These values are comparable to world-average sediment As concentrations. Five samples of rhyolitic ash from the area have As concentrations of 7–12 mg kg−1. Chemical analysis included loess sediments and extracted porewaters from two specially cored boreholes. Results reveal a large range of porewater As concentrations, being generally higher in the horizons with highest sediment As concentrations. The displaced porewaters have As concentrations ranging up to 7500 μg L−1 as well as exceptionally high concentrations of some other oxyanion species, including V up to 12 mg L−1. The highest concentrations are found in a borehole located in a topographic depression, which is a zone of likely groundwater discharge and enhanced residence time. Comparison of sediment and porewater data does not reveal unequivocally the sources of the As, but selective extract data (acid-ammonium oxalate and hydroxylamine hydrochloride) suggest that much of the As (and V) is associated with Fe oxides. Primary oxides such as magnetite and ilmenite may be partial sources but given the weathered nature of many of the sediments, secondary oxide minerals are probably more important. Extract compositions also suggest that Mn oxide may be an As source. The groundwaters of the region are oxidising, with dissolved O2, NO3 and SO4 normally present and As(V) usually the dominant dissolved As species. Under such conditions, the solubility of Fe and Mn oxides is low and As mobilisation is strongly controlled by sorption–desorption reactions. Desorption may be facilitated by the relatively high-pH conditions of the groundwaters in the region (7.0–8.8) and high concentrations of potential competitors (e.g. V, P, HCO3). PHREEQC modelling suggests that the presence of V at the concentrations observed in the Pampean porewaters can suppress the sorption of As to hydrous Fe(III) oxide (HFO) by up to an order of magnitude. Bicarbonate had a comparatively small competitive effect. Oxalate extract concentrations have been used to provide an upper estimate of the amount of labile As in the sediments. A near-linear correlation between oxalate-extractable and porewater As in one of the cored boreholes investigated has been used to estimate an approximate Kd value for the sediments of 0.94 L kg−1. This low value indicates that the sediments have an unusually low affinity for As.  相似文献   

9.
The groundwaters from Zhongxiang City, Hubei Province of central China, have high fluoride concentration up to 3.67 mg/L, and cases of dental fluorosis have been found in this region. To delineate the nature and extent of high fluoride groundwaters and to assess the major geochemical factors controlling the fluoride enrichment in groundwater, 14 groundwater samples and 5 Quaternary sediment samples were collected and their chemistry were determined in this study. Some water samples from fissured hard rock aquifers and Quaternary aquifers have high fluoride concentrations, whereas all karst water samples contain fluoride less than 1.5 mg/L due to their high Ca/Na ratios. For the high fluoride groundwaters in the fissured hard rocks, high HCO3 − concentration and alkaline condition favor dissolution of fluorite and anion exchange between OH− in groundwater and exchangeable F− in some fluoride-bearing minerals. For fluoride enrichment in groundwaters of Quaternary aquifers, high contents of fluoride in the aquifer sediments and evapotranspiration are important controls.  相似文献   

10.
Although arsenic (As) contamination has been extensively investigated in the aquifers of the lower and middle Gangetic plains, less attention has been given to the distribution and fate of As in the groundwater of the upper Gangetic plain, India. In the current study, groundwater samples (n = 40) were collected from Moradabad district in the upper Gangetic plain and analyzed for several physicochemical parameters to characterize the groundwater chemistry and evaluate various geogenic and anthropogenic factors controlling the occurrence, mobilization, and fate of As in the plain. Arsenic concentrations in groundwater ranged from 0.17 μg/L to 139 μg/L, with the majority of high-As groundwater associated with high Fe, Mn, and HCO3− and low NO3−, SO42−, and negative Eh values, implying that As was released via reductive dissolution of Fe and Mn oxyhydroxides in reducing conditions under the influence of organic matter degradation. Interrelationships between various geochemical variables and the natural background level (NBL) quantification of As suggested the influence of anthropogenic processes on the mobility of As in groundwater. Piper and Gibbs diagrams and various bivariate plots revealed that the majority of groundwater was of the Ca2+ − Mg2+ − HCO3− type and that the major ions in groundwater were derived from carbonate and silicate weathering, cation exchange and reverse ion exchange processes, and anthropogenic activities. Moreover, the results of principal component analysis (PCA), and hierarchical cluster analysis (HCA) also suggested geogenic and anthropogenic sources for the ion concentration in groundwater. The health risk assessment showed a higher non-carcinogenic risk for children and a higher carcinogenic risk for adults, respectively, due to the daily intake of As contaminated groundwater. Overall, this study represents the first systematic investigation of the distribution, geochemical behavior, and release process of As in groundwater in the study area and provides a strong base for future research in the alluvial aquifers of the upper Gangetic plain.  相似文献   

11.
Hydrogeochemical characteristics and elemental features of groundwater and core sediments have been studied to better understand the sources and mobilization process responsible for As-enrichment in part of the Gangetic plain (Barasat, West Bengal, India). Analysis of water samples from shallow tubewells (depth 24.3–48.5 m) and piezometer wells (depth 12.2–79.2 m) demonstrate that the groundwater is mostly the Ca-HCO3 type and anoxic in nature (mean EhSHE = 34 mV). Arsenic concentrations ranged from <10–538 μg/L, with high concentrations only present in the shallow to medium depth (30–50 m) of the aquifer along with high Fe (0.07–9.8 mg/L) and relatively low Mn (0.15–3.38 mg/L) as also evidenced in core sediments. Most groundwater samples contained both As(III) and As(V) species in which the concentration of As(III) was generally higher than that of As(V), exhibiting the reducing condition. Results show lower concentrations of NO3, SO4 and NO2 along with higher values of DOC and HCO3, indicating the reducing nature of the aquifer with abundant organic matter that can promote the release of As from sediments into groundwater. Positive correlations of As with Fe and DOC were also observed. The presence of DOC may actively drive the redox processes. This study revealed that reduction processes of FeOOH was the dominant mechanism for the release of As into the groundwater in this part of the Ganges Delta plain.  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》2003,18(9):1283-1296
This paper discusses the abundance, speciation and mobility of As in groundwater systems from active volcanic areas in Italy. Using literature data and new additional determinations, the main geochemical processes controlling the fate of As during gas–water–rock interaction in these systems are examined. Arsenic concentrations in the fluids range from 0.1 to 6940 μg/l, with wide differences observed among the different volcanoes and within each area. The dependence of As content on water temperature, pH, redox potential and major ions is investigated. Results demonstrate that As concentrations are highest where active hydrothermal circulation takes place at shallow levels, i.e. at Vulcano Island and the Phlegrean Fields. In both areas the dissolution of As-bearing sulphides is likely to be the main source of As. Mature Cl-rich groundwaters, representative of the discharge from the deep thermal reservoirs, are typically enriched in As with respect to SO4-rich “steam heated groundwaters”. In the HCO3− groundwaters recovered at Vesuvius and Etna, aqueous As cycling is limited by the absence of high-temperature interactions and by high-Fe content of the host rocks, resulting in oxidative As adsorption. Thermodynamic modelling suggests that reducing H2S-rich groundwaters are in equilibrium with realgar, whereas in oxidising environments over-saturation with respect to Fe oxy-hydroxides is indicated. Under these oxidising conditions, As solubility decreases controlled by As co-precipitation with, or adsorption on, Fe oxy-hydroxides. Consistent with thermodynamic considerations, As mobility in the studied areas is enhanced in intermediate redox environments, where both sulphides and Fe hydroxides are unstable.  相似文献   

14.
《Applied Geochemistry》2003,18(9):1417-1434
The mechanism of As release and source(s) of As has been investigated in a small part of a watershed in the Murshidabad district of West Bengal. Analyses include major ion and trace element concentrations, as well as O, H and S isotope ratios of groundwater, surface water and a thermal spring. The results indicate that all water samples belong to the Ca–HCO3 type, except for the thermal spring which is of the Na–HCO3 type. Shallow and deeper groundwaters have distinct hydrochemical features. High As contents were registered only in the deeper groundwater horizon. Factor analysis and the distribution pattern of major and trace elements indicate that As is present in the aquifer as a scavenged phase by Fe(III) and to a lesser extent by Mn(IV) phases. The release of As into the groundwater occurs gradually in successive stages, corresponding to the actual redox state in the aquifer. The main stage of As release is related to the bacterial reduction of Fe(III) to Fe(II) (i.e. to the simultaneous dissolution of Fe oxyhydroxides). Low redox conditions in highly polluted areas are indicated by low SO4 concentration and high δ34S values. During bacterial SO4 reduction, residual SO4 in groundwater is depleted in the lighter S isotope (32S). However, the cause of the gradual decrease of the redox state in the groundwater is still not well understood.  相似文献   

15.
《Applied Geochemistry》2000,15(6):819-832
In this paper the groundwater in-situ generation of dissolved organic carbon (DOC) is discussed based on the origin of groundwaters, their physico-chemical and isotopic properties, chemical composition and the dissolved inorganic carbon (DIC) concentration and its 13C content. Three aquifer systems are investigated. Two of these have relatively well defined hydrological and geochemical conditions (Fuhrberg and Munich) and are used as reference systems. The third aquifer (Gorleben) is a complex system containing DOC concentrations up to 200 mg C/L in deep groundwaters. From this aquifer system 19 groundwaters from different hydrogeochemical conditions are analyzed. The in-situ generation of DOC is found to occur in conjunction with the microbiologically mediated mineralization of sedimentary organic carbon (SOC). Thereby, SO4 is reduced and phosphate is released into the groundwater. Where SO4 is depleted, the mineralization of SOC occurs via fermentation, resulting in CH4 generation.  相似文献   

16.
Here new data from field bioremediation experiments and geochemical modeling are reported to illustrate the principal geochemical behavior of As in anaerobic groundwaters. In the field bioremediation experiments, groundwater in Holocene alluvial aquifers in Bangladesh was amended with labile water-soluble organic C (molasses) and MgSO4 to stimulate metabolism of indigenous SO4-reducing bacteria (SRB). In the USA, the groundwater was contaminated by Zn, Cd and SO4, and contained <10 μg/L As under oxidized conditions, and a mixture of sucrose and methanol were injected to stimulate SRB metabolism. In Bangladesh, groundwater was under moderately reducing conditions and contained ∼10 mg/L Fe and ∼100 μg/L As. In the USA experiment, groundwater rapidly became anaerobic, and dissolved Fe and As increased dramatically (As > 1000 μg/L) under geochemical conditions consistent with bacterial Fe-reducing conditions. With time, groundwater became more reducing and biogenic SO4 reduction began, and Cd and Zn were virtually completely removed due to precipitation of sphalerite (ZnS) and other metal sulfide mineral(s). Following precipitation of chalcophile elements Zn and Cd, the concentrations of Fe and As both began to decrease in groundwater, presumably due to formation of As-bearing FeS/FeS2. By the end of the six-month experiment, dissolved As had returned to below background levels. In the initial Bangladesh experiment, As decreased to virtually zero once biogenic SO4 reduction commenced but increased to pre-experiment level once SO4 reduction ended. In the ongoing experiment, both SO4 and Fe(II) were amended to groundwater to evaluate if FeS/FeS2 formation causes longer-lived As removal. Because As-bearing pyrite is the common product of SRB metabolism in Holocene alluvial aquifers in both the USA and Southeast Asia, it was endeavored to derive thermodynamic data for arsenian pyrite to better predict geochemical processes in naturally reducing groundwaters. Including the new data for arsenian pyrite into Geochemist’s Workbench, its stability field completely dominates in reducing Eh–pH space and “displaces” other As-sulfides (orpiment, realgar) that have been implied to be important in previous modeling exercises and reported in rare field conditions.  相似文献   

17.
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18.
High concentrations of geogenic As in the groundwaters of south and SE Asia, which are used as drinking waters, are causing severe health impacts to the exposed human populations. It is widely accepted that As mobilisation from sediments into these shallow reducing groundwaters requires active metal-reducing microbes and electron donors such as organic matter (OM). Although OM in such Holocene aquifers has been characterised, there is a dearth of data on Pleistocene aquifers from the same areas. Reported here are preliminary studies of OM and microbial communities present in two aquifers, one of Pleistocene and one of Holocene age, with contrasting concentrations of As (viz. Pleistocene: low As <10 μg/L; Holocene: high As up to 600 μg/L) from Van Phuc village in the Red River Delta, Vietnam. Results revealed OM inputs from multiple sources, including potential contributions from naturally occurring petroleum seeping into the shallow aquifer sediments from deeper thermally mature source rocks. Although concentrations vary, no noticeable systematic differences in biomarker distribution patterns within the OM were observed between the two sites. Microbial analyses did not show a presence of microbial communities previously associated with As mobilisation. All clone libraries were dominated by α-, β-, and γ-Proteobacteria not known to be able to reduce Fe(III) or sorbed As(V). Furthermore, representatives of the Fe(III)-reducing genus Geobacter could only be detected at very low abundance by PCR, using highly selective 16S rRNA gene primers, supporting the hypothesis that metal reduction is not a dominant in situ process in these sediments. No correlation between As concentration in groundwater and OM composition nor microbial community in the host sediments was found. This suggests that either (i) As is not being significantly mobilised in situ in these sediments, instead As appears to be mobilised elsewhere and transported by groundwater flow to the sites or (ii) sorption/desorption processes, as implicated by geochemical data from the cores, play a critical role in controlling As concentrations at these sites.  相似文献   

19.
《Applied Geochemistry》2004,19(8):1255-1293
In order to investigate the mechanism of As release to anoxic ground water in alluvial aquifers, the authors sampled ground waters from 3 piezometer nests, 79 shallow (<45 m) wells, and 6 deep (>80 m) wells, in an area 750 m by 450 m, just north of Barasat, near Kolkata (Calcutta), in southern West Bengal. High concentrations of As (200–1180 μg L−1) are accompanied by high concentrations of Fe (3–13.7 mg L−1) and PO4 (1–6.5 mg L−1). Ground water that is rich in Mn (1–5.3 mg L−1) contains <50 μg L−1 of As. The composition of shallow ground water varies at the 100-m scale laterally and the metre-scale vertically, with vertical gradients in As concentration reaching 200 μg L−1 m−1. The As is supplied by reductive dissolution of FeOOH and release of the sorbed As to solution. The process is driven by natural organic matter in peaty strata both within the aquifer sands and in the overlying confining unit. In well waters, thermo-tolerant coliforms, a proxy for faecal contamination, are not present in high numbers (<10 cfu/100 ml in 85% of wells) showing that faecally-derived organic matter does not enter the aquifer, does not drive reduction of FeOOH, and so does not release As to ground water.Arsenic concentrations are high (≫50 μg L−1) where reduction of FeOOH is complete and its entire load of sorbed As is released to solution, at which point the aquifer sediments become grey in colour as FeOOH vanishes. Where reduction is incomplete, the sediments are brown in colour and resorption of As to residual FeOOH keeps As concentrations below 10 μg L−1 in the presence of dissolved Fe. Sorbed As released by reduction of Mn oxides does not increase As in ground water because the As resorbs to FeOOH. High concentrations of As are common in alluvial aquifers of the Bengal Basin arise because Himalayan erosion supplies immature sediments, with low surface-loadings of FeOOH on mineral grains, to a depositional environment that is rich in organic mater so that complete reduction of FeOOH is common.  相似文献   

20.
《Applied Geochemistry》2004,19(7):1137-1155
Within the Lower Peninsula of Michigan, groundwaters from the Marshall Formation (Mississippian) contain As derived from As-rich pyrites, often exceeding the World Heath Organization drinking water limit of 10 μg/L. Many Michigan watersheds, established on top of Pleistocene glacial drift derived from erosion of the underlying Marshall Formation, also have waters with elevated As. The Huron River watershed in southeastern Lower Michigan is a well characterized hydrogeochemical system of glacial drift deposits, proximate to the Marshall Fm. subcrop, which hosts carbonate-rich groundwaters, streams, and wetlands (fens), and well-developed soil profiles. Aqueous and solid phase geochemistry was determined for soils, soil waters, surface waters (streams and fens) and groundwaters from glacial drift aquifers to better understand the hydrogeologic and chemical controls on As mobility. Soil profiles established on the glacial drift exhibit enrichment in both Fe and As in the oxyhydroxide-rich zone of accumulation. The amounts of Fe and As present as oxyhydroxides are comparable to those reported from bulk Marshall Fm. core samples by previous workers. However, the As host in core samples is largely unaltered pyrite and arsenopyrite. This suggests that the transformation of Fe sulfides to Fe oxyhydroxides largely retains As and Fe at the oxidative weathering site. Groundwaters have the highest As values of all the waters sampled, and many were at or above the World Health limit. Most groundwaters are anaerobic, within the zones of Fe3+ and As(V) reduction. Although reduction of Fe(III) oxyhydroxides is the probable source of As, there is no correlation between As and Fe concentrations. The As/Fe mole ratios in drift groundwaters are about an order of magnitude greater than those in soil profiles, suggesting that As is more mobile than Fe. This is consistent with the dominance of As(III) in these groundwaters and with the partitioning of Fe2+ into carbonate cements. Soil waters have very low As and Fe contents, consistent with the stability of oxyhydroxides under oxidizing vadose conditions. When CO2 charged groundwaters discharge in streams and fens, dissolved As is effectively removed by adsorption onto Fe-oxides or carbonate marls. Although Fe does not display conservative behavior with As in groundwaters, a strong positive correlation exists between As and Sr concentrations. As water–rock interactions proceed, the As/Fe and Sr/Ca ratios would be expected to increase because both As and Sr behave as incompatible elements. Comparisons with groundwater chemistries from other drift-hosted aquifers proximate to the Marshall sandstone are consistent with these relations. Thus, the Sr content of carbonate-rich groundwaters may provide useful constraints on the occurrence, origin and evolution of dissolved As in such systems.  相似文献   

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