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1.
《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   

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.
《Applied Geochemistry》2006,21(1):83-97
Groundwater in the Gwelup groundwater management area in Perth, Western Australia has been enriched in As due to the exposure of pyritic sediments caused by reduced rainfall, increased groundwater abstraction for irrigation and water supply, and prolonged dewatering carried out during urban construction activities. Groundwater near the watertable in a 25–60 m thick unconfined sandy aquifer has become acidic and has affected shallow wells used for garden irrigation. Arsenic concentrations up to 7000 μg/L were measured in shallow groundwater, triggering concerns about possible health effects if residents were to use water from household wells as a drinking water source. Deep production wells used for public water supply are not affected by acidity, but trends of progressively increasing concentrations of Fe, SO4 and Ca over a 30-a period indicate that pyrite oxidation products extend to the base of the unconfined aquifer. Falling Eh values are triggering the release of As from the reduction of Fe(III) oxyhydroxide minerals near the base of the unconfined aquifer, increasing the risk that groundwater used as a drinking water source will also become contaminated with high concentrations of As.  相似文献   

4.
Patchy occurrences of elevated As are often encountered in groundwater from the shallow aquifers (<50 m) of the Bengal Delta Plain (BDP). A clear understanding of various biogeochemical processes, responsible for As mobilization, is very important to explain this patchy occurrence and thus to mitigate the problem. The present study deals with the periodical monitoring of groundwater quality of five nested piezometeric wells between December 2008 and July 2009 to investigate the temporal changes in groundwater chemistry vis-a-vis the prevalent redox processes in the aquifer. Geochemical modeling has been carried out to identify key phases present in groundwater. A correlation study among different aqueous redox parameters has also been performed to evaluate prevailing redox processes in the aquifer. The long term monitoring of hydrochemical parameters in the multilevel wells together with hydrogeochemical equilibrium modeling has shown more subtle differences in the geochemical environment of the aquifer, which control the occurrence of high dissolved As in BDP groundwater. The groundwater is generally of Ca-HCO3 type. The dissolved As concentration in groundwater exceeded both WHO and National drinking water standard (Bureau of Indian Standards; BIS, 10 μg L−1) throughout the sampling period. The speciation of As and Fe indicate persistent reducing conditions within the aquifer [As(III): 87-97% of AsT and Fe(II): 76-96% of FeT]. The concentration of major aqueous solutes is relatively high in the shallow aquifer (wells A and B) and gradually decreases with increasing depth in most cases. The calculation of SI indicates that groundwater in the shallow aquifer is also relatively more saturated with carbonate minerals. This suggests that carbonate mineral dissolution is possibly influencing the groundwater chemistry and thereby controlling the mobilization of As in the monitored shallow aquifer. Hydrogeochemical investigation further suggests that Fe and/or Mn oxyhydroxide reduction is the principal process of As release in groundwater from deeper screened piezometric wells. The positive correlations of U and V with As, Fe and Mn indicate redox processes responsible for mobilization of As in the deeper screened piezometric wells are possibly microbially mediated. Thus, the study advocates that mobilization of As is depth dependent and concentrations of As in groundwater depends on single/combined release mechanisms.  相似文献   

5.
The concentration of arsenic measured in groundwater from three aquifers in the study area located in the Eastern Tucuman province, Argentina, mostly depends on the lithology, but the spatial and temporal variations of concentrations seem to be also controlled by pH changes, climatic factors, and human perturbations. The highest concentrations of As (more than 1,000 μg L−1) were found in the shallow aquifer, made of As-rich loess, while the lowest concentrations were measured in the deep confined aquifer, consisting of alternating layers of alluvial sands/gravels and clays. Intermediate values were measured in the semiconfined aquifer made of the fluvial sediments deposited in the Salí River valley, that alternate in the upper part of the sedimentary sequence with layers of loess. Because most of As in the loess is considered to be adsorbed onto Fe-oxyhydroxide coatings, the increase of pH in the flow direction (west-east) leads to increasing arsenic concentrations towards the eastern border of the study area. The decomposition of organic wastes poured into the Salí River or associated with local and diffuse sources of contamination in the eastern part of the study area depletes dissolved oxygen, which leads to the reductive dissolution of Fe and Mn oxyhydroxides, and to the subsequent release of the adsorbed and co-precipitated As. This process mainly affects shallow groundwater and the upper part of the semiconfined aquifer. Geochemical and hydrological data also suggest that rising water table levels at the end of the wet season may also lead to reductive dissolution of As-rich Fe oxyhydroxides in the shallow aquifer.  相似文献   

6.
The Guadalupe Valley aquifer is the only water source for one of the most important wine industries in Mexico, and also the main public water supply for the nearby city of Ensenada. This groundwater is monitored for major ion, N-NO3, P-PO4, Fe, As, Se, Mo, Cd, Cu, Pb, Zn and Sb concentrations, as well as TDS, pH, dissolved oxygen and temperature. High concentrations of N-NO3 (26 mg l−1), Se (70 μg l−1), Mo (18 μg l−1) and Cu (4.3 μg l−1) suggest that groundwater is being polluted by the use of fertilizers only in the western section of the aquifer, known as El Porvenir graben. Unlike the sites located near the main recharge area to the East of the aquifer, the water in El Porvenir graben has low tritium concentrations (<1.9 TU), indicating a pre-modern age, and thus longer water residence time. No significant variations in water quality (generally <10%) were detected throughout 2001–2002 in the aquifer, suggesting that reduced rainfall and recharge during this dry period did not significantly affect water quality. However, the wells nearest to the main recharge area in the Eastern aquifer show a slight but constant increase in TDS with time, probably as a result of the high (∼200 L S−1) uninterrupted extraction of water at this specific recharge site. Relatively high As concentrations for the aquifer (10.5 μg l−1) are only found near the northern limit of the basin associated with a geological fault.  相似文献   

7.
This study reexamines the notion that extensive As mobilization in anoxic groundwater of Bangladesh is intimately linked to the dissolution of Fe oxyhydroxides on the basis of analyses performed on a suite of freshly collected samples of aquifer material. Detailed sediment profiles extending to 40 to 70 m depth below the surface were obtained at six sites where local groundwater As concentrations were known to span a wide range. The sediment properties that were measured include (1) the proportion of Fe(II) in the Fe fraction leached in hot 1.2 N HCl, (2) diffuse spectral reflectance, and (3) magnetic susceptibility.In parallel with local concentrations of dissolved As ranging from <5 to 600 μg/L, Fe(II)/Fe ratios in shallow (gray) Holocene sands tended to gradually increase with depth from values of 0.3 to 0.5 to up to 0.9. In deeper (orange) aquifers of presumed Pleistocene age that were separated from shallow sands by a clay layer and contained <5 μg/L dissolved As, leachable Fe(II)/Fe ratios averaged ∼0.2. There was no consistent relation between sediment Fe(II)/Fe and dissolved Fe concentrations in groundwater in nearby wells. The reflectance measurements indicate a systematic linear relation (R2 of 0.66; n = 151) between the first derivative transform of the reflectance at 520 nm and Fe(II)/Fe. The magnetic susceptibility of the shallow aquifer sands ranged from 200 to 3600 (x 10−9 m3/kg SI) and was linearly related (R2 of 0.75; n = 29) to the concentrations of minerals that could be magnetically separated (0.03 to 0.79% dry weight). No systematic depth trends in magnetic susceptibility were observed within the shallow sands, although the susceptibility of deeper low-As aquifers was low (up to ∼200 × 10−9 m3/kg SI).This set of observations, complemented by incubation results described in a companion paper by van Geen et al. (this volume), suggests that the release of As is linked to the transformation of predominantly Fe (III) oxyhydroxide coatings on sand particles to Fe(II) or mixed Fe(II/III) solid phases with a flatter reflectance spectrum such as siderite, vivianite, or magnetite, without necessarily resulting in the release of Fe to groundwater. The very low As/Fe ratio of magnetically separated minerals compared to the As/Fe of bulk acid leachate (2 vs. 40 10−6, respectively) suggests that such a transformation could be accompanied by a significant redistribution of As to a mobilizable phase on the surface of aquifer particles.  相似文献   

8.
《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   

9.
Riverbank sediment cores and pore waters, shallow well waters, seepage waters and river waters were collected along the Meghna Riverbank in Gazaria Upazila, Bangladesh in Jan. 2006 and Oct.–Nov. 2007 to investigate hydrogeochemical processes controlling the fate of groundwater As during discharge. Redox transition zones from suboxic (0–2 m depth) to reducing (2–5 m depth) then suboxic conditions (5–7 m depth) exist at sites with sandy surficial deposits, as evidenced by depth profiles of pore water (n = 7) and sediment (n = 11; diffuse reflectance, Fe(III)/Fe ratios and Fe(III) concentrations). The sediment As enrichment zone (up to ∼700 mg kg−1) is associated with the suboxic zones mostly between 0 and 2 m depth and less frequently between 5 and 7 m depth. The As enriched zones consist of several 5–10 cm-thick dispersed layers and span a length of ∼5–15 m horizontally from the river shore. Depth profiles of riverbank pore water deployed along a 32 m transect perpendicular to the river shore show elevated levels of dissolved Fe (11.6 ± 11.7 mg L−1) and As (118 ± 91 μg L−1, mostly as arsenite) between 2 and 5 m depth, but lower concentrations between 0 and 2 m depth (0.13 ± 0.19 mg L−1 Fe, 1 ± 1 μg L−1 As) and between 5 and 6 m depth (1.14 ± 0.45 mg L−1 Fe, 28 ± 17 μg L−1 As). Because it would take more than a few hundred years of steady groundwater discharge (∼10 m yr−1) to accumulate hundreds of mg kg−1 of As in the riverbank sediment, it is concluded that groundwater As must have been naturally elevated prior to anthropogenic pumping of the aquifer since the 1970s. Not only does this lend unequivocal support to the argument that As occurrence in the Ganges-Brahmaputra-Meghna Delta groundwater is of geogenic origin, it also calls attention to the fate of this As enriched sediment as it may recycle As into the aquifer.  相似文献   

10.
《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   

11.
Enriched As in drinking water wells in south and Southeast Asia has increased the risk of cancer for nearly 100 million people. This enrichment is generally attributed to the reductive dissolution of Fe oxides; however, the complex expression of As enrichment in these areas is not yet well understood. Here, the coupled sedimentological and geochemical factors that contribute to the extent and spatial distribution of groundwater As concentrations in the Mekong River delta, Cambodia in an avulsed scroll bar sequence are examined. X-Ray absorption spectroscopy (XAS) was used to determine Fe and As speciation in redox preserved sediment collected from drilled cores. Dissolved As, Fe and S solution concentrations in existing and newly drilled wells (cores) differed considerably depending on their source sedimentology. The rapid burial of organic matter in the scroll bar sequence facilitated the development of extensive Fe-reducing conditions, and As release into the aquifer. In older features organic C levels are high enough to sustain extensive Fe reduction and provide ample SO4 which is reduced to sulfide. This S reduction impacts As levels; As is sequestered in sulfide minerals outside of the scrollbar sequence, decreasing pore water concentrations. In contrast, As is depleted in sediments from the scroll sequence, and associated with elevated pore water aqueous concentrations. The concentration and form of organic C in the scrollbar sequence is related to depositional environment, and can facilitate Fe and S mineral transformations, distinct sedimentary environments explain a portion of the inherent heterogeneity of aquifer As concentrations.  相似文献   

12.
《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   

13.
《Applied Geochemistry》2005,20(1):55-68
In 49 samples of groundwater, sampled in Muzaffargarh District of south-western Punjab, central Pakistan, concentrations of As exceeded the World Health Organisation provisional guideline value, and United States Environmental Protection Agency (USEPA) Maximum Contaminant Level (MCL), of 10 μg L−1 in 58% of samples and reached up to 906 μg L−1. In this semi-arid region canal irrigation has lead to widespread water-logging, and evaporative concentration of salts has the potential to raise As concentrations in shallow groundwater well above 10 μg L−1. In fact, in rural areas, concentrations stay below 25 μg L−1 because As in the oxic shallow groundwater, and in recharging water, is sorbed to aquifer sediments. In some urban areas, however, shallow groundwater is found to contain elevated levels of As. The spatial distribution of As-rich shallow groundwater indicates either direct contamination with industrial or agricultural chemicals, or some other anthropogenic influence. Geochemical evidence suggests that pollutant organics from unconfined sewage and other sources drives reduction of hydrous ferric oxide (HFO) releasing sorbed As to shallow groundwater. The situation is slightly less clear for seven wells sampled which tap deeper groundwater, all of which were found with >50 μg L−1 As. Here As concentrations seem to increase with depth and differing geochemical signatures are seen, suggesting that As concentrations in older groundwater may be governed by different processes. Other data on parameters of potential concern in drinking water are discussed briefly at the end of the paper.  相似文献   

14.
Sediments from the Aquia aquifer in coastal Maryland were collected as part of a larger study of As in the Aquia groundwater flow system where As concentration are reported to reach levels as high as 1072 nmol kg−1, (i.e., ∼80 μg/L). To test whether As release is microbially mediated by reductive dissolution of Fe(III) oxides/oxyhydroxides within the aquifer sediments, the Aquia aquifer sediment samples were employed in a series of microcosm experiments. The microcosm experiments consisted of sterilized serum bottles prepared with aquifer sediments and sterilized (i.e., autoclaved), artificial groundwater using four experimental conditions and one control condition. The four experimental conditions included the following scenarios: (1) aerobic; (2) anaerobic; (3) anaerobic + acetate; and (4) anaerobic + acetate + AQDS (anthraquinone-2,6-disulfonic acid). AQDS acts as an electron shuttle. The control condition contained sterilized aquifer sediments kept under anaerobic conditions with an addition of AQDS. Over the course of the 27 day microcosm experiments, dissolved As in the unamended (aerobic and anaerobic) microcosms remained constant at around ∼28 nmol kg−1 (2 μg/L). With the addition of acetate, the amount of As released to the solution approximately doubled reaching ∼51 nmol kg−1 (3.8 μg/L). For microcosm experiments amended with acetate and AQDS, the dissolved As concentrations exceeded 75 nmol kg−1 (5.6 μg/L). The As concentrations in the acetate and acetate + AQDS amended microcosms are of similar orders of magnitude to As concentrations in groundwaters from the aquifer sediment sampling site (127-170 nmol kg−1). Arsenic concentrations in the sterilized control experiments were generally less than 15 nmol kg−1 (1.1 μg/L), which is interpreted to be the amount of As released from Aquia aquifer sediments owing to abiotic, surface exchange processes. Iron concentrations released to solution in each of the microcosm experiments were higher and more variable than the As concentrations, but generally exhibited similar trends to the As concentrations. Specifically, the acetate and acetate + AQDS amended microcosm typically exhibited the highest Fe concentrations (up to 1725 and 6566 nmol kg−1, respectively). The increase in both As and Fe in the artificial groundwater solutions in these amended microcosm experiments strongly suggests that microbes within the Aquia aquifer sediments mobilize As from the sediment substrate to the groundwaters via Fe(III) reduction.  相似文献   

15.
《Applied Geochemistry》2000,15(6):791-805
This paper describes the geochemical evolution of groundwater in the Bathonian and Bajocian aquifer along its flowpath. Since this aquifer represents one of the main sources of fresh water supply in the Caen area and has been subjected to a Holocene marine intrusion, its management requires a sound knowledge of (1) the primary conditions and (2) the potential influence of either natural or anthropogenic pressures. Groundwater vertical sampling validity is discussed with the contribution of high resolution temperature logging. The main processes of geochemical evolution along a groundwater flow line and the sea-water intrusion characteristics are discussed using ionic concentrations (Br−, F− and major elements) and isotopes (water δ2H and δ18O, TDIC δ13C and A14C, sulphate δ18O and δ34S). As the 13C content of TDIC is used as a tracer of water-rock interaction, it shows evidence of specific chemical and isotopic evolutions of groundwater within the aquifer, both related to water-rock interaction and mineral equilibria in groundwater. All the above-mentioned tracers evolve downflow: cation concentrations are modified by exchange with clay minerals allowing a high F− concentration in groundwater, whereas Br− and SO2−4 concentrations appear to be redox condition dependant. Superimposed on these geochemical patterns, δ18O and δ2H compositions indicate that aquifer recharge has varied significantly through time. The chemical evolution of groundwater is locally affected by a salty water intrusion that is characterised by mixing between Flandrian fresh water and sea-water which has interacted with peat as evidenced by a high Br−/Cl− ratio and SO2−4 reduction.  相似文献   

16.
Arsenic release from aquifers can be a major issue for aquifer storage and recovery (ASR) schemes and understanding the processes that release and attenuate As during ASR is the first step towards managing this issue. This study utilised the first and fourth cycles of a full scale field trial to examine the fate of As within the injectant plume during all stages of the ASR cycle, and the resultant water quality. The average recovered As concentration was greater than the source concentration; by 0.19 μmol/L (14 μg As/L) in cycle 1 and by 0.34 μmol/L (25 μg As/L) in cycle 4, indicating that As was being released from the aquifer sediments during ASR and the extent of As mobilisation did not decline with subsequent cycles. In the injection phase, As mobilisation due to oxidation of reduced minerals was limited to an oxic zone in close proximity to the ASR well, while desorption from Fe oxyhydroxide or oxide surfaces by injected P occurred further in the near well zone (0–4 m from the ASR well). With further aquifer passage during injection and greater availability of sorption sites there was evidence of attenuation via adsorption to Fe oxyhydroxides which reduced concentrations on the outer fringes of the injectant plume. During the period of aquifer storage, microbial activity resulting from the injection of organic matter resulted in increased As mobility due to reductive Fe oxyhydroxide dissolution and the subsequent loss of sorption sites and partial reduction of As(V) to the more mobile As(III). A reduced zone directly around the ASR well produced the greatest As concentration and illustrated the importance of Fe oxyhydroxides for controlling As concentrations. Given the small spatial extent of this zone, this process had little effect on the overall recovered water quality.  相似文献   

17.
The principle of subsurface iron removal for drinking water supply is that aerated water is periodically injected into the aquifer through a tube well. On its way into the aquifer, the injected O2-rich water oxidizes adsorbed Fe2+, creating a subsurface oxidation zone. When groundwater abstraction is resumed, the soluble Fe2+ is adsorbed and water with reduced Fe concentrations is abstracted for multiple volumes of the injection water. In this article, Fe accumulation deposits in the aquifer near subsurface treatment wells were identified and characterized to assess the sustainability of subsurface iron removal regarding clogging of the aquifer and the potential co-accumulation of other groundwater constituents, such as As. Chemical extraction of soil samples, with Acid-Oxalate and HNO3, showed that Fe had accumulated at specific depths near subsurface iron removal wells after 12 years of operation. Whether it was due to preferred flow paths or geochemical mineralogy conditions; subsurface iron removal clearly favoured certain soil layers. The total Fe content increased between 11.5 and 390.8 mmol/kg ds in the affected soil layers, and the accumulated Fe was found to be 56-100% crystalline. These results suggest that precipitated amorphous Fe hydroxides have transformed to Fe hydroxides of higher crystallinity. These crystalline, compact Fe hydroxides have not noticeably clogged the investigated well and/or aquifer between 1996 and 2008. The subsurface iron removal wells even need less frequent rehabilitation, as drawdown increases more slowly than in normal production wells. Other groundwater constituents, such as Mn, As and Sr were found to co-accumulate with Fe. Acid extraction and ESEM-EDX showed that Ca occurred together with Fe and by X-ray Powder Diffraction it was identified as calcite.  相似文献   

18.
《Applied Geochemistry》2004,19(6):863-886
Large scale redox processes were investigated in a river recharged aquifer in the Oderbruch polder alongside the river Oder in north-eastern Germany. Major hydraulic and hydrochemical processes were identified qualitatively. As a result of intensive drainage activities in the past 250 a, the groundwater level within the polder is situated below the river water level and a levee prevents flooding of the lowland. As a consequence, river water permanently infiltrates into the shallow confined aquifer. A sequence of redox reactions, driven by organic matter degradation, can be observed during infiltration of oxic river water into the groundwater. Up to 3 km from the river, reduction processes from O2 respiration to SO2−4 reduction dominate the groundwater chemistry. While reduction of Fe- and Mn(hydr)oxides is the source of the high amounts of dissolved Fe2+ and Mn2+, carbonate dissolution/precipitation reactions control the actual groundwater concentration of Mn2+. The first order rate constant for SO2−4 reduction was found to be −0.0169 a−1. Fe2+ is released into the groundwater at a rate of 0.0033 mmol l−1 a−1. The groundwater chemistry is strongly linked to the hydraulic conditions. Near the river, the groundwater is confined and recharged by bank-filtration only. In contrast, in the central polder the groundwater is unconfined and percolation of rainwater through the dried loam is possible because of texture changes such as shrinkage fissures. Geogenic pyrite present within the alluvial loam is oxidised and large amounts of SO2−4 are released into the groundwater.  相似文献   

19.
《Applied Geochemistry》2001,16(6):583-596
Nitrate concentrations monitored for 2.5 a in the stream water and groundwater of a small catchment, 86.5% of which is devoted to intensive agriculture, show temporal variations with a maximum during winter (as much as 200 mg l−1 in groundwater and 100 mg l−1 in stream water) and a minimum at the end of summer/beginning of autumn. Variations were also observed in the stream water and shallow groundwater after rainfall. The processes involved to explain these variations, determined mainly from NO3− Cl−, SO42−, piezometric and streamflow data, are: (a) variability of the relative contributions to stream water and shallow groundwater by upward fluxes of deeper groundwater which, as demonstrated previously, is denitrified mainly as a result of reaction with pyrite. (b) Denitrification of shallow groundwater during summer with organic matter acting as the electron donor. (c) Dilution by rain water. Nitrate concentrations in both stream water and shallow groundwater depend on the amount of precipitation, with an increased contribution from deep denitrified groundwater during dry periods. The temporal variations in NO3− concentration observed several metres below the water table are related to the preferential and rapid movement of NO3−-polluted water through fractures and large fissures, which has been estimated at 1 m day−1. Nitrate pollution in the catchment, because of the interaction with pyrite, also increases the net chemical weathering rate to values exceeding the world average.  相似文献   

20.
《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   

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