首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献，搜索用时 62 毫秒
1.
Arsenic is a prevalent contaminant at US Superfund sites where remediation by pump and treat systems is often complicated by slow desorption of As from Fe and Al (hydr)oxides in aquifer solids. Chemical amendments that either compete with As for sorption sites or dissolve Fe and Al (hydr)oxides can increase As mobility and improve pump and treat remediation efficiency. The goal of this work was to determine optimal amendments for improving pump and treat at As contaminated sites such as the Vineland Chemical Co. Superfund site in southern New Jersey. Extraction and column experiments were performed using As contaminated aquifer solids (81 ± 1 mg/kg), site groundwater, and either phosphate (NaH2PO4·H2O) or oxalic acid (C2H2O4·2H2O). In extraction experiments, phosphate mobilized between 11% and 94% of As from the aquifer solids depending on phosphate concentration and extraction time (1 mM–1 M; 1–24 h) and oxalic acid mobilized between 38% and 102% depending on oxalic acid concentration and extraction time (1–400 mM; 1–24 h). In column experiments, phosphate additions induced more As mobilization in the first few pore volumes but oxalic acid was more effective at mobilizing As overall and at lower amendment concentrations. At the end of the laboratory column experiments, 48% of As had been mobilized from the aquifer sediments with 100 mM phosphate and 88% had been mobilized with 10 mM oxalic acid compared with 5% with ambient groundwater alone. Furthermore, simple extrapolations based on pore volumes suggest that chemical treatments could lower the time necessary for clean up at the Vineland site from 600 a with ambient groundwater alone to potentially as little as 4 a with 10 mM oxalic acid.  相似文献   

2.
One of the reasons the processes resulting in As release to groundwater in southern Asia remain poorly understood is the high degree of spatial variability of physical and chemical properties in shallow aquifers. In an attempt to overcome this difficulty, a simple device that collects groundwater and sediment as a slurry from precisely the same interval was developed in Bangladesh. Recently published results from Bangladesh and India relying on the needle-sampler are augmented here with new data from 37 intervals of grey aquifer material of likely Holocene age in Vietnam and Nepal. A total of 145 samples of filtered groundwater ranging in depth from 3 to 36 m that were analyzed for As (1–1000 μg/L), Fe (0.01–40 mg/L), Mn (0.2–4 mg/L) and S (0.04–14 mg/L) are compared. The P-extractable (0.01–36 mg/kg) and HCl-extractable As (0.04–36 mg/kg) content of the particulate phase was determined in the same suite of samples, in addition to Fe(II)/Fe ratios (0.2–1.0) in the acid-leachable fraction of the particulate phase. Needle-sampler data from Bangladesh indicated a relationship between dissolved As in groundwater and P-extractable As in the particulate phase that was interpreted as an indication of adsorptive equilibrium, under sufficiently reducing conditions, across 3 orders of magnitude in concentrations according to a distribution coefficient of 4 mL/g. The more recent observations from India, Vietnam and Nepal show groundwater As concentrations that are often an order of magnitude lower at a given level of P-extractable As compared to Bangladesh, even if only the subset of particularly reducing intervals characterized by leachable Fe(II)/Fe >0.5 and dissolved Fe >0.2 mg/L are considered. Without attempting to explain why As appears to be particularly mobile in reducing aquifers of Bangladesh compared to the other regions, the consequences of increasing the distribution coefficient for As between the particulate and dissolved phase to 40 mL/g for the flushing of shallow aquifers of their initial As content are explored.  相似文献   

3.
To study the geological control on groundwater As concentrations in Red River delta, depth-specific groundwater sampling and geophysical logging in 11 monitoring wells was conducted along a 45 km transect across the southern and central part of the delta, and the literature on the Red River delta’s Quaternary geological development was reviewed. The water samples (n = 30) were analyzed for As, major ions, Fe2+, H2S, NH4, CH4, δ18O and δD, and the geophysical log suite included natural gamma-ray, formation and fluid electrical conductivity. The SW part of the transect intersects deposits of grey estuarine clays and deltaic sands in a 15–20 km wide and 50–60 m deep Holocene incised valley. The NE part of the transect consists of 60–120 m of Pleistocene yellowish alluvial deposits underneath 10–30 m of estuarine clay overlain by a 10–20 m veneer of Holocene sediments. The distribution of δ18O-values (range −12.2‰ to −6.3‰) and hydraulic head in the sample wells indicate that the estuarine clay units divide the flow system into an upper Holocene aquifer and a lower Pleistocene aquifer. The groundwater samples were all anoxic, and contained Fe2+ (0.03–2.0 mM), Mn (0.7–320 μM), SO4 (<2.1 μM–0.75 mM), H2S (<0.1–7.0 μM), NH4 (0.03–4.4 mM), and CH4 (0.08–14.5 mM). Generally, higher concentrations of NH4 and CH4 and low concentrations of SO4 were found in the SW part of the transect, dominated by Holocene deposits, while the opposite was the case for the NE part of the transect. The distribution of the groundwater As concentration (<0.013–11.7 μM; median 0.12 μM (9 μg/L)) is related to the distribution of NH4, CH4 and SO4. Low concentrations of As (?0.32 μM) were found in the Pleistocene aquifer, while the highest As concentrations were found in the Holocene aquifer. PHREEQC-2 speciation calculations indicated that Fe2+ and H2S concentrations are controlled by equilibrium for disordered mackinawite and precipitation of siderite. An elevated groundwater salinity (Cl range 0.19–65.1 mM) was observed in both aquifers, and dominated in the deep aquifer. A negative correlation between aqueous As and an estimate of reduced SO4 was observed, indicating that Fe sulphide precipitation poses a secondary control on the groundwater As concentration.  相似文献   

4.
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   

5.
The importance of accessing safe aquifers in areas with high As is being increasingly recognized. The present study aims to investigate the sorption and mobility of As at the sediment-groundwater interface to identify a likely safe aquifer in the Holocene deposit in southwestern Bangladesh. The upper, shallow aquifer at around 18 m depth, which is composed mainly of very fine, grey, reduced sand and contains 24.3 μg/g As, was found to produce highly enriched groundwater (190 μg/L As). In contrast, deeper sediments are composed of partly oxidized, brownish, medium sand with natural adsorbents like Fe- and Al-oxides; they contain 0.76 μg/g As and impart low As concentrations to the water (4 μg/L). These observations were supported by spectroscopic studies with SEM, TEM, XRD and XRF, and by adsorption, leaching, column tests and sequential extraction. A relatively high in-situ dissolution rate (Rr) of 1.42 × 10−16 mol/m2/s was derived for the shallower aquifer from the inverse mass-balance model. The high Rr may enhance As release processes in the upper sediment. The field-based reaction rate (Kr) was extrapolated to be roughly 1.23 × 10−13 s−1 and 6.24 × 10−14 s−1 for the shallower and deeper aquifer, respectively, from the laboratory-obtained adsorption/desorption data. This implies that As is more reactive in the shallower aquifer. The partition coefficient for the distribution of As at the sediment-water interface (Kd-As) was found to range from 5 to 235 L/kg based on in-situ, batch adsorption, and flow-through column techniques. Additionally, a parametric equation for Kd-As (R2 = 0.67) was obtained from the groundwater pH and the logarithm of the leachable Fe and Al concentrations in sediment. A one-dimensional finite-difference numerical model incorporating Kd and Kr showed that the shallow, leached As can be immobilized and prevented from reaching the deeper aquifer (∼150 m) after 100 year by a natural filter of oxidizing sand and adsorbent minerals like Fe and Al oxides; in this scenario, 99% of the As in groundwater is reduced. The deeper aquifer appears to be an adequate source of sustainable, safe water.  相似文献   

6.
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   

7.
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   

8.
  相似文献   

9.
To advance understanding of hydrological influences on As concentrations within groundwaters of Southeast Asia, the flow system of an As-rich aquifer on the Mekong Delta in Cambodia where flow patterns have not been disturbed by irrigation well pumping was examined. Monitoring of water levels in a network of installed wells, extending over a 50 km2 area, indicates that groundwater flow is dominated by seasonally-variable gradients developed between the river and the inland wetland basins. While the gradient inverts annually, net groundwater flow is from the wetlands to the river. Hydraulic parameters of the aquifer (K ≈ 10−4 ms−1) and overlying clay aquitard (K ≈ 10−8 ms−1) were determined using grain size, permeameter and slug test analyses; when coupled with observed gradients, they indicate a net groundwater flow velocity of 0.04–0.4 ma−1 downward through the clay and 1–13 ma−1 horizontally within the sand aquifer, producing aquifer residence times on the order 100–1000 a. The results of numerical modeling support this conceptual model of the flow system and, when integrated with observed spatial trends in dissolved As concentrations, reveal that the shallow sediments (upper 2–10 m of fine-grained material) are an important source of As to the underlying aquifer.  相似文献   

10.
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   

11.
Sediments from the Red River and from an adjacent floodplain aquifer were investigated with respect to the speciation of Fe and As in the solid phase, to trace the diagenetic changes in the river sediment upon burial into young aquifers, and the related mechanisms of arsenic release to the groundwater. Goethite with subordinate amounts of hematite were, using Mössbauer spectroscopy, identified as the iron oxide minerals present in both types of sediment. The release kinetics of Fe, As, Mn and PO4 from the sediment were investigated in leaching experiments with HCl and 10 mM ascorbic acid, both at pH 3. From the river sediments, most of the Fe and As was mobilized by reductive dissolution with ascorbic acid while HCl released very little Fe and As. This suggests As to be associated with an Fe-oxide phase. For oxidized aquifer sediment most Fe was mobilized by ascorbic acid but here not much As was released. However, the reduced aquifer sediments contained a large pool of Fe(II) and As that is readily leached by HCl, probably derived from an unidentified authigenic Fe(II)-containing mineral which incorporates As as well. Extraction with ascorbic acid indicates that the river sediments contain both As(V) and As(III), while the reduced aquifer sediment almost exclusively releases As(III). The difference in the amount of Fe(II) leached from river and oxidized aquifer sediments by ascorbic acid and HCl, was attributed to reductive dissolution of Fe(III). The reactivity of this pool of Fe(III) was quantified by a rate law and compared to that of synthetic iron oxides. In the river mud, Fe(III) had a reactivity close to that of ferrihydrite, while the river sand and oxidized aquifer sediment exhibited a reactivity ranging from lepidocrocite or poorly crystalline goethite to hematite. Mineralogy by itself appears to be a poor predictor of the iron oxide reactivity in natural samples using the reactivity of synthetic Fe-oxides as a reference. Sediments were incubated, both unamended and with acetate added, and monitored for up to 2 months. The river mud showed the fastest release of both Fe and As, while the effect of acetate addition was minor. This suggests that the presence of reactive organic carbon is not rate limiting. In the case of the river and aquifer sediments, the release of Fe and As was always stimulated by acetate addition and here reactive organic carbon was clearly the rate limiting factor. The reduced aquifer sediment apparently can sustain slower but prolonged microbially-driven release of As. The highly reactive pools of Fe(III) and As in the river mud could be due to reoxidation of As and Fe contained in the reducing groundwater from the floodplain aquifers that are discharging into the river. Deposition of the suspended mud on the floodplain during high river stages is proposed to be a major flux of As onto the floodplain and into the underlying aquifers.  相似文献   

12.
Field experiments and laboratory studies were performed to investigate migration processes of plutonium isotopes from a near-surface radioactive waste trench to the underlying sandy aquifer at the Red Forest waste dump in the Chernobyl zone. The objectives of these experiments were to characterize the spatial distribution and possible migration mechanisms of plutonium in the aquifer. During 2002–2007 experimental investigations were carried out and spatial distributions of plutonium isotopes (239,240Pu, 238Pu), 90Sr and major ions in the aquifer in the direction of the groundwater flow were obtained. Specific activities of radionuclides in groundwater depended on the location of the piezometer and varied in the range of 1–360 mBq kg−1 for 239,240Pu, 0.5–180 mBq kg−1 for 238Pu and n–n·104 Bq kg−1 for 90Sr. It was found that the spatial features of the distributions of plutonium and strontium specific activities in the upper eolian aquifer were similar, i.e. there was a correlation between the positions of the activity maxima of the radionuclides. The Pu isotopes plume in the aquifer spreads about 15 m downstream of the radionuclides source. Characterization of the initial radionuclide composition of the waste showed that all plutonium in the aquifer originated from the trench. The ratio of plutonium isotopes (239,240Pu/238Pu) at the sampling time was the same in waste material and in groundwater samples. In situ ultrafiltration of several groundwater samples was carried out. The size fractionation data obtained suggest that a significant part of plutonium (50–98%) in the groundwater sampled close to the source from the upper part of the aquifer is associated with a very low molecular weight fraction (<1 kDa).  相似文献   

13.
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   

14.
Mineral assemblages (heavy and light fractions) and sedimentological characteristics of the Quaternary alluvial aquifers were examined in the central Bengal Basin where As concentrations in groundwater are highly variable in space but generally decrease downward. Chemical compositions of sediment samples from two vertical core profiles (2-150 m below ground level, bgl) were analyzed along with groundwater in moderately As-enriched aquifers in central Bangladesh (Manikganj district), and the As mobilization process in the alluvial aquifer is described. Heavy minerals such as biotite, magnetite, amphibole, apatite and authigenic goethite are abundant at shallow (<100 m below ground level (mbgl)) depths but less abundant at greater depths. It is interpreted that principal As-bearing minerals were derived from multiple sources, primarily from ophiolitic belts in the Indus-Tsangpo suture in the northeastern Himalayan and Indo-Burman Mountain ranges. Authigenic and amorphous Fe-(oxy)hydroxide minerals that are generally formed in river channels in the aerobic environment are the major secondary As-carriers in alluvial sediments. Reductive dissolution (mediated by Fe-reducing bacteria) of Fe-(oxy)hydroxide minerals under anoxic chemical conditions is the primary mechanism responsible for releasing As into groundwater. Authigenic siderite that precipitates under reducing environment at greater depths decreases Fe and possibly As concentrations in groundwater. Presence of Fe(III) minerals in aquifers shows that reduction of these minerals is incomplete and this can release more As if further Fe-reduction takes place with increased supplies of organic matter (reactive C). Absence of authigenic pyrite suggests that SO4 reduction (mediated by SO4-reducing bacteria) in Manikganj groundwater is limited in contrast to the southeastern Bengal Basin where precipitation of arsenian pyrite is thought to sequester As from groundwater.  相似文献   

15.
Seasonal (Spring and Summer 2002) concentrations of dissolved (<0.22 μm) trace metals (Ag, Al, Co, Cu, Mn, Ni, Pb), inorganic nutrients (NO3, PO4, Si), and DOC were determined in groundwater samples from 5 wells aligned along a 30 m shore-normal transect in West Neck Bay, Long Island, NY. Results show that significant, systematic changes in groundwater trace metal and nutrient composition occur along the flowpath from land to sea. While conservative mixing between West Neck Bay water and the groundwaters explains the behavior of Si and DOC, non-conservative inputs for Co and Ni were observed (concentration increases of 10- and 2-fold, respectively) and removal of PO4 and NO3 (decreases to about half) along the transport pathway. Groundwater-associated chemical fluxes from the aquifer to the embayment calculated for constituents not exhibiting conservative behavior can vary by orders of magnitude depending on sampling location and season (e.g. Co, 3.4 × 102– 8.2 × 103 μmol d−1). Using measured values from different wells as being representative of the true groundwater endmember chemical composition also results in calculation of very different fluxes (e.g., Cu, 6.3 × 103 μmol d−1 (inland, freshwater well) vs. 2.1 × 105 μmol d−1(seaward well, S = 17 ppt)). This study suggests that seasonal variability and chemical changes occurring within the subterranean estuary must be taken into account when determining the groundwater flux of dissolved trace metals and nutrients to the coastal ocean.  相似文献   

16.
Mineralogy and geochemistry of modern shallow sediments (up to 5 m thick) within the zone of water table fluctuations were studied to determine the likely sources and processes responsible for releasing As into groundwater. Samples were collected from different geological settings with varying groundwater As concentrations during dry (December 2005) and wet (September 2006) seasons at Sonargaon, Bangladesh. Stratigraphic sequences of the studied sediments showed three distinct lithofacies, viz. clayey-silt, silty-clay, and silty-very fine sand, corresponding to fine-grained overbank associations. Total As concentrations of shallow sediments ranged from <1 to 16 mg/kg without a significant difference in the range of As concentrations between the seasons. Sequential chemical extraction analysis of As revealed that >80% of the As was fixed in insoluble and organic phases, while the amount of As in reducible and acid-soluble phases was very low (<20%) and varied inversely with total As content. Total As concentration varied with mica content (muscovite and biotite) and its related elements (Al, Mg and Fe), but not with total organic C, suggesting that biotite is the major host phase of As. Arsenic appears to be liberated from biotite and/or other As-bearing minerals via chemical weathering (i.e., hydration-decomposition), either from the near-surface sediments which are subject to seasonal cycling of the redox conditions, or from within the aquifer sediments. Once released, progressive diagenesis to form As-bearing organic matter may be responsible for controlling As distribution in the sediments and coexisting groundwater of the study area.  相似文献   

17.
The shallow aquifer beneath the Western Snake River Plain (Idaho, USA) exhibits widespread elevated arsenic concentrations (up to 120 μg L−1). While semi-arid, crop irrigation has increased annual recharge to the aquifer from approximately 1 cm prior to a current rate of >50 cm year−1. The highest aqueous arsenic concentrations are found in proximity to the water table (all values >50 μg L−1 within 50 m) and concentrations decline with depth. Despite strong vertical redox stratification within the aquifer, spatial distribution of aqueous species indicates that redox processes are not primary drivers of arsenic mobilization. Arsenic release and transport occur under oxidizing conditions; groundwater wells containing dissolved arsenic at >50 μg L−1 exhibit elevated concentrations of O2 (average 4 mg L−1) and NO3 (average 8 mg L−1) and low concentrations of dissolved Fe (<20 μg L−1). Sequential extractions and spectroscopic analysis of surficial soils and sediments indicate solid phase arsenic is primarily arsenate and is present at elevated concentrations (4–45 mg kg−1, average: 17 mg kg−1) relative to global sedimentary abundances. The highest concentrations of easily mobilized arsenic (up to 7 mg kg−1) are associated with surficial soils and sediments visibly stained with iron oxides. Batch leaching experiments on these materials using irrigation waters produce pore water arsenic concentrations approximating those observed in the shallow aquifer (up to 152 μg L−1). While As:Cl aqueous phase relationships suggest minor evaporative enrichment, this appears to be a relic of the pre-irrigation environment. Collectively, these data indicate that infiltrating irrigation waters leach arsenic from surficial sediments to the underlying aquifer.  相似文献   

18.
The injection and recovery of oxic water into deep anoxic aquifers may help to alleviate short- and long-term imbalance between freshwater supply and demand. The extent and structure of physical and geochemical heterogeneity of the aquifer will impact the water quality evolution during injection, storage and recovery. Water–sediment interactions within the most permeable parts of the aquifer, where the bulk of the injectant will penetrate, may dominate, however, water quality may also be impacted by interactions within the finer-grained, less permeable but potentially highly reactive media. In this study, the heterogeneity of the reductive capacity of an aquifer selected for water reuse projects was characterised, the amount, type and reactivity of the sedimentary reductants present determined, and the relationship between reductive capacity and sedimentary lithologies quantified. The average potential reductive capacities (PRCTOT), based on total organic C and pyrite concentrations of the sediment, were quantified for sands (382 μmol O2 g−1), clays (1522 μmol O2 g−1), and silts (1957 μmol O2 g−1). Twenty-seven samples, spanning the three different lithologies, were then incubated for 50 days and the measured reductive capacities (MRC) determined for the sands (29.2 μmol O2 g−1), silts (136 μmol O2 g−1), and clays (143 μmol O2 g−1). On average, the MRC were 10% of the PRCTOT. The main consumers of O2 were pyrite (20–100%), sedimentary organic matter (SOM; 3–56%), siderite (3–28%) and Fe(II)-aluminosilicates (8–55%). The incubation data plus hydrogeochemical modelling, indicated that pH-buffering was controlled firstly by dissolution of trace level carbonates, followed by dissolution of feldspars. Zinc, Co, Ni, Cd and Pb were readily mobilized during incubation.  相似文献   

19.
Currently, the most widely accepted hypothesis to explain high As concentrations in Bangladesh groundwaters is that dissolved organic C (DOC) reduces solid Fe (hydr)oxides and mobilizes sorbed arsenate. The nature of the DOC and its release mechanism are still controversial. Based on weekly to biweekly sampling over the course of one monsoon cycle at six monitoring wells of different depths, it is proposed that storativity changes drive natural DOC release from clay–peat layers to the adjacent aquifers. With a decrease in hydraulic heads during the dry season, total mineralization and DOC concentrations increased. With the onset of the rainy season and an increase in hydraulic heads, release of clay–peat derived components stopped and vertical water displacement due to groundwater recharge from rainwater occurred, causing aquifer flushing and a decrease in total mineralization and DOC concentrations. Total As and DOC concentrations correlated over depth. However, at the depth of maximum concentrations, the As peak was observed during the rainy season. At present, the reason for this inverse seasonal trend between As and DOC is unclear. Higher mineralization or DOC concentrations could lead to increased As sorption or the increased arsenite release is a time-lag abiotic or microbial response to the DOC peak. The vulnerability of the Pleistocene aquifer towards increased As concentrations was found to be much higher than previously assumed. Though sorption capacities were determined to be higher than in the Holocene aquifer, probably due to intact Fe (hydr)oxides, long-term continuous As input from overlying clay and peat layers by the proposed seasonal storativity changes has led to increased aqueous As concentrations of 85 μg/L, considerably higher than drinking water standards. Until now, aquifer and especially aquitard and aquiclude hydraulics have not been considered sufficiently when attempting to explain As mobilization in Bangladesh.  相似文献   

20.
The Northern Basque Country (Southwestern France) is subject to a constant need of increasing water due to a rising population. The fissured aquifer of the Ursuya Mount is one of the main water supplies able to meet these needs. Unfortunately, there is a lack of knowledge on the residence time of groundwater and flow pattern in this strategic resource. Geochemical monitoring of groundwater was carried out from 2009 to 2011 in conjunction with CFC–SF6 measurement and with a detailed geological field characterization. It appears that groundwater flows and water geochemistry are conditioned by the development of a weathered layer overlying the fissured aquifer. When the weathered layer is absent, groundwater flows take place in unconfined conditions along fractures and fissures. The rapid circulation (mean residence time between 11 and 15 a) and the low solubility of the matrix generates low mineralization (mean about 61 μS cm−1). When a weathered layer is present, the flow depends on the degree of weathering, with groundwater circulating in the deep fissured zone in the case of a high degree of weathering. The apparent age is then between 10 and 42 a and the mineralization tends to increase concomitantly with the residence time, and particularly terrigenic element concentrations. In the case of a lesser degree of weathering, mixing between recent water from the shallow weathered layer and the oldest water (25 to >50 a) from the underlying fissured aquifer is observed. These results allow the definition of a conceptual model of flow characteristics in the study area which is also applicable to other weathered–fractured systems worldwide.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号