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1.
To better understand the sources and mobilization processes responsible for arsenic enrichment in groundwater in the central part of Datong Basin where serious arsenic poisoning cases have been reported, hydrochemical characteristics of the groundwater and the geochemical and mineralogical features of the aquifer sediments were studied. The aqueous arsenic levels are strongly depth-dependent in the study area and the high arsenic concentrations are found at depths between 15 m and 60 m, with a maximum up to 1820 μg/L. The hydrochemical characteristics of high arsenic groundwater from the Datong Basin indicate that the mobilization of arsenic is related to reductive dissolution of Fe oxides/oxyhydroxides and/or desorption from the Fe oxides/oxyhydroxides at high pH (above 8.0). The bulk chemical results of sediments show the arsenic and iron are moderately correlated, suggesting that arsenic is associated with iron-bearing minerals. Results of sequential-extraction experiment show that solid-phase arsenic is similarly distributed among the different pools of reservoir in the aquifer sediments. Strongly adsorbed arsenic and co-precipitated arsenic are its dominant species in the solid-phase. Geochemical studies using chemical analysis, X-ray diffraction and scanning electron microscopy on magnetically separated fractions demonstrate that iron oxides/oxyhydroxides with residual magnetite and chlorite, illite, iron oxides/oxyhydroxides-coated quartz and feldspar, and ankerite are the dominant carriers of arsenic in the sediments. The major processes of arsenic mobilization are probably linked to desorption of As from Fe oxides/oxyhydroxides and reductive dissolution of Fe-rich phases in the aquifer sediments under reducing and alkaline conditions.  相似文献   

2.
Understanding the mechanism of arsenic mobilization from sediments to groundwater is important for water quality management in areas of endemic arsenic poisoning, such as the Hetao Basin in Inner Mongolia, northern China. Aquifer geochemistry was characterized at three field sites (SH, HF, TYS) in Hangjinhouqi County of northwestern Hetao Basin. The results of bulk geochemistry analysis of sediment samples indicated that total As concentrations have a range of 6.8–58.5 mg/kg, with a median of 14.4 mg/kg. The highest As concentrations were found at 15–25 m depth. In the meanwhile, the range of As concentration in the sediments from background borehole is 3–21.8 mg/kg, with a median value of 9 mg/kg. The As sediments concentrations with depth from the SH borehole were correlated with the contents of Fe, Sb, B, V, total C and total S. Generally, the abundance of elements varied with grain size, with higher concentrations in finer fractions of the sediments. Distinct lithology profile and different geochemical characteristics of aquifer sediments indicate the sediments are associated with different sources and diverse sedimentary environments. Up to one third of arsenic in the sediments could be extracted by ammonium oxalate, suggesting that Fe oxyhydroxides may be the major sink of As in the aquifer. Sequential extraction results indicate that arsenic occurs as strongly adsorbed on and/or co-precipitated with amorphous Fe oxyhydroxides in sediments accounting for 35 and 20%, respectively, of the total contents of arsenic. The release of As into groundwater may occur by desorption from the mineral surface driven by reductive dissolution of the Fe oxide minerals. Furthermore, small proportions of As associated with iron sulfides occur in the reductive sediments.  相似文献   

3.
Environmental geochemistry of high arsenic groundwater at Hetao plain was studied on the basis of geochemical survey of the groundwater and a core sediment. Arsenic concentration in groundwater samples varies from 76 to 1093 μg/L. The high arsenic groundwater mostly appears to be weakly alkaline. The concentrations of NO3− and SO42− are relatively low, while the concentrations of DOC, NH4+, dissolved Fe and sulfide are relatively great. Analysis of arsenic speciation in 21 samples shows that arsenic is present in the solution predominantly as As(III), while particulate arsenic constitutes about 10% of the total arsenic. Methane is detected in five samples with the greatest content being 5107 μg/L. The shallow aquifer in Hangjinhouqi of western Hetao plain is of strongly reducing condition. The arsenic content in 23 core sediment samples varies from 7.7 to 34.6 mg/kg, with great value in clay and mild clay layer. The obvious positive relationship in content between Fe2O3, Mn, Sb, B, V and As indicates that the distribution of arsenic in the sediments may be related to Fe and Mn oxides, and the mobilization of Sb, B and V may be affected by similar geochemical processes as that of As.  相似文献   

4.
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   

5.
Arsenic mobility in fluvial environment of the Ganga Plain,northern India   总被引：1，自引：1，他引：0  
In the northern part of the Indian sub-continent, the Gomati River (a tributary of the Ganga River) was selected to study the dynamics of Arsenic (As) mobilization in fluvial environment of the Ganga Plain. It is a 900-km-long, groundwater-fed, low-gradient, alluvial river characterized by monsoon-controlled peaked discharge. Thirty-six water samples were collected from the river and its tributaries at low discharge during winter and summer seasons and were analysed by ICP-MS. Dissolved As and Fe concentrations were found in the range of 1.29–9.62 and 47.84–431.92 μg/L, respectively. Arsenic concentration in the Gomati River water has been detected higher than in its tributaries water and characteristically increases in downstream, attributed to the downstream increasing of Fe2O3 content, sedimentary organic carbon and silt-clay content in the river sediments. Significant correlation of determination (r 2 = 0.68) was also observed between As and Fe concentrations in the river water. Arsenic concentrations in the river water are likely to follow the seasonal temperature variation and reach the level of World Health Organization’s permissible limit (10 μg/L) for drinking water in summer season. The Gomati River longitudinally develops reducing conditions after the monsoon season that mobilize As into the river water. First, dissolved As enters into pore-water of the river bed sediments by the reductive dissolution of Fe-oxides/hydroxides due to microbial degradation of sedimentary organic matter. Thereafter, it moves upward as well as down slope into the river water column. Anthropogenically induced biogeochemical processes and tropical climatic condition have been considered the responsible factors that favour the release of As in the fluvial environment of the Ganga Plain. The present study can be considered as an environmental alarm for future as groundwater resources of the Ganga–Brahmaputra Delta are seriously affecting the human–environment relationship at present.  相似文献   

6.
Two boreholes and ten piezometers in the Ganges flood plain were drilled and installed for collecting As-rich sediments and groundwater. Groundwater samples from the Ganges flood plain were collected for the analysis of cations (Ca2+, Mg2+, K+, Na+), anions (Cl−, NO3 −, SO4 2−), total organic carbon (TOC), and trace elements (As, Mn, Fe, Sr, Se, Ni, Co, Cu, Mo, Sb, Pb). X-ray powder diffraction was performed to characterize the major mineral contents of aquifer sediments and X-ray fluorescence (XRF) to analyze the major chemical composition of alluvial sediments. Results of XRF analysis clearly show that fine-grained sediments contain higher amounts of trace element because of their high surface area for adsorption. Relative fluorescence index (15–38 QSU) of humic substance in groundwater was measured using spectrofluorometer, the results revealed that groundwater in the Ganges flood plain contains less organic matter (OM). Arsenic concentration in water ranges from 2.8 to 170 μg/L (mean 50 μg/L) in the Ganges flood plain. Arsenic content in sediments ranges from 2.1 to 14 mg/kg (mean 4.58 mg/kg) in the flood plains. TOC ranges from 0.49 to 3.53 g/kg (mean 1.64 g/kg) in the Ganges flood plain. Arsenic is positively correlated with TOC (R 2 = 0.55) in sediments of this plain. Humic substances were extracted from the sediments from the Ganges flood plain. Fourier transform infrared analysis of the sediments revealed that the plain contains less humic substances. The source of organic carbon was assigned from δ13C values obtained using elemental analysis-isotope ratio mass spectrometry (EA-IRMS); the values (−10 to −29.44‰) strongly support the hypothesis that the OM of the Ganges flood plain is of terrestrial origin.  相似文献   

7.
The geochemical study of groundwaters and core sediments from the Old Brahmaputra plain of Bangladesh was conducted to investigate the distribution of arsenic and related trace elements. Groundwaters from tube wells are characterized by pH of 6.4–7.4, dissolved oxygen (DO) of 0.8–1.8 mg/l, Ca contents of 5–50 mg/l, and Fe contents of 0.2–12.9 mg/l. Arsenic concentrations ranged from 8 to 251 μg/l, with an average value of 63 μg/l. A strong positive correlation exists between As and Fe (r 2 = 0.802; p = 0.001) concentrations in groundwater. The stratigraphic sequences in the cores consist of yellowish silty clays at top, passing downward into grayish to yellowish clays and sands. The uppermost 3 m and lower parts (from 13 to 31 m) of the core sediments are oxidized (average oxidation reduction potential (ORP) +170 and +220 mV, respectively), and the ORP values gradually become negative from 3 to 13 m depths (−35 to −180 mV), indicating that anoxic conditions prevail in the shallow aquifers of the Brahmaputra plain. Age determinations suggest that clay horizons at ~10 m depth were deposited at around 2,000 and 5,000 years BP (14C ages) during the transgressive phase of sea-level change. Elevated concentrations of As, Pb, Zn, Cu, Ni, Cr, and V are present in the silts and clays, probably due to adsorption onto clay particles. Significant concentrations of As occur in black peat and peaty sediments at depths between 9 and 13 m. A strong positive correlation between As and Fe was found in the sediments, indicating As may be adsorbed onto Fe oxides in aquifer sediments.  相似文献   

8.
The fate and transport of As was examined at an industrial site where soil- and groundwater contamination are derived from the application of As2O3 as a herbicide. Application of arsenical herbicides was discontinued in the 1970s and soils in the source area were partially excavated in 2003. Arsenic contamination (up to 280 mg/kg) remains in the source area soils and a plume of As-contaminated groundwater persists in the surficial aquifer downgradient of the source area with maximum observed As concentrations of 1200 μg/L near the source area. The spatial extent of As contamination as defined by the 10 μg/L contour appears to have remained relatively stable over the period 1996–2006; the boundary of the 1000 μg/L contour has retreated over the same time period indicating a decrease in total As mass in the surficial groundwater.In column experiments conducted with source area soil, the As concentrations in the column effluent were comparable to those observed in groundwater near the source area. A substantial fraction of the As could be leached from the source area soil with ammonium sulfate and ammonium phosphate. Exhaustive extraction with background groundwater removed most of the total As. These results indicate that As in the source area soils is geochemically labile. Source area soils are low in extractable Fe, Mn and Al, and characterization by X-ray absorption spectroscopy and electron microscopy indicated that As is present primarily as arsenate sorbed to (alumino)silicate minerals. Batch sorption experiments showed much less sorption on surficial aquifer sediments than on sediments from the Jackson Bluff Formation (JBF), a presumed confining layer. This limited capacity of the surficial aquifer sediments for As sorption is consistent with the similar As contents observed for these sediments within and upgradient of the As plume. The apparent stability of the As plume cannot be explained by sequestration of As within the surficial aquifer. Sorption to JBF sediments may contribute to As sequestration, but As enrichment in JBF sediments within the plume (i.e., as compared with JBF sediments upgradient) was not observed. These results indicate that neither the persistence of As in the source area soils or the apparent stability of the plume of As-contaminated groundwater at this site can be explained by geochemical controls on As mobility. The absence of demonstrable geochemical bases for such observations suggests that possible hydrologic controls should be further investigated at this site.  相似文献   

9.
Arsenic and fluoride in a loess aquifer in the central area of Argentina   总被引：3，自引：0，他引：3  
The objective of this study is to analyze the geochemical conditions associated with the presence of arsenic (As) and fluoride (F) in the phreatic aquifer of Coronel Moldes, in the central sector of the Argentine Chacopampean plain. The studied aquifer is composed of silty sand sediments of aeolian origin, typically loess-like sediments. The geochemical composition of water varies from sodium bicarbonate to sodium sulfate-chloride water. As contents range from low concentrations, below detection level, to 250 μg/l. High values of F (up to 12 mg/l) were recorded. A high As–F correlation was found (R 2 = 0.84). The pH varied from 7.31 to 8.85 and the nitrates reached concentrations up to 200 mg/l, indicating an oxidant environment. The highest values of As and F agreed with sodium bicarbonate waters as well as with the highest values of pH recorded. There was a high correlation between As and F− as well as between As and the Na/Ca ratio. The composition and texture of loess, low permeability and hydraulic gradients together with the geochemical features of sodium bicarbonate waters are proper conditions for the mobilization of As and F in groundwater in the central area of Argentina.  相似文献   

10.
A comparative hydrogeochemical study evaluated arsenic release mechanism and differences in contamination levels in the shallow groundwater of two areas within the deltaic environment of West Bengal (i.e. Karimpur and Tehatta blocks of Nadia district) in India. Groundwaters from both the areas are Ca-Na(K)-Cl-HCO3 type with highly reducing character (−110.16 ± 16.85 to −60.77 ± 16.93 mV). Low correlations among As, Fe, and Mn and the higher association between As and DOC are indicative of microbial decomposition of organic matter enhancing the weathering of shallow aquifer materials. Arsenic contamination in groundwater is higher in Karimpur (95 ± 81.17 μg/L) than that in Tehatta (43.05 ± 41.06 μg/L). The release mechanism of arsenic into groundwater is very complex. Low Fe (0.27–4.78 mg/L and 0.81–4.13 mg/L), Mn (0.08–0.2 mg/L and 0.03–0.22 mg/L), and SO42− (3.82 ± 0.31 and 2.78 ± 0.40 mg/L) suggest that the mechanism of arsenic release is not a single mechanistic pathway. Clustering of redox-active parameters in the principal component planes indicate that the reductive dissolution, and/or weathering/co-precipitation of Fe/Mn-bearing minerals in the shallow aquifer sediments control the dominant mechanistic pathway of arsenic release.  相似文献   

11.
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   

12.
土著微生物作用下含水层沉积物砷的释放与转化   总被引：4，自引：0，他引：4  
在原位采集内蒙古河套平原高砷含水层中沉积物和土著微生物的基础上,进行了室内微生物淋滤实验研究。实验过程中,使用了3种水溶液(包括去离子水和2种人工配水)和2种营养条件(包括添加2%葡萄糖和未添加葡萄糖)。结果表明,葡萄糖可强化土著微生物的活性,使得悬浮液pH值明显降低,并增加悬浮液中As质量浓度。配水成分影响悬浮物中As质量浓度。在第9 d之后,添加葡萄糖的样品中存在一定强度的硫酸根还原作用,且这种脱硫酸作用受配水成分的影响较小。研究表明,土著微生物影响下砷的释放和转化过程包括沉积物中As(V)的释放、溶液中As(V)的还原以及沉积物中As(Ⅲ)的释放等。与溶液As(V)相比,As(Ⅲ)更有利于沉积物As的释放。在As释放的过程中,溶液中Fe/Mn含量同时增加,且呈很好的线性相关关系。这意味着土著微生物作用下Fe/Mn氧化物矿物的还原性溶解是导致沉积物As释放的主要原因之一。  相似文献   

13.
The chemical and microbiological characteristics of groundwater from two provinces of central Spain were studied. In some zones of this area, the concentrations of As in groundwater exceed the guideline concentrations, set internationally between 10 g/l and 50 g/l, reaching levels over 100 g/l. A narrow correlation between the contents of arsenic and HCO3– was observed. These data suggest a possible mechanism of the As mobilization from aquifer sediments to groundwater: the bicarbonate ions could displace HAsO42– adsorbed on aquifer oxyhydroxides. Sediments containing relatively high contents of adsorbed arsenic are deposited in surface water environments with low carbonate concentrations. Subsequently, the sediments become exposed to groundwater with highly dissolved carbonate content, and arsenic can be mobilized by displacement from mineral surfaces. In addition, the presence of Pseudomonas genera bacteria, which secrete siderophores (Fe chelating agents) could mobilize As adsorbed on Fe oxides through their dissolution. These combined microbiological and chemical processes might have increased the natural mobility of As.  相似文献   

14.
微生物参与铁氧化物矿物的还原性溶解是高砷地下水形成的关键过程,其中具有砷还原功能的微生物如何参与含水层砷释放的生物地球化学过程亟待研究.利用从江汉平原典型高砷含水层中厌氧条件下分离出的四株细菌(Citrobacter sp.JH-1、Clostridium sp.JH-6、Exiguobacterium sp.JH-13、Paenibacillus sp.JH-33),通过室内厌氧模拟培养实验,查明其砷、铁还原能力,并通过分别与铁氧化物矿物及原位沉积物共同培养,探究原位含水层微生物参与的砷释放机理.结果表明:四株细菌均具有厌氧条件下砷、铁还原功能,Citrobacter sp.JH-1砷还原能力最强,96 h内还原的As(Ⅴ)浓度为2.22 μmol/L.其中Citrobacter sp.JH-1不仅可在厌氧和有氧条件下还原溶液中的As(Ⅴ),还可在厌氧条件下还原溶液中的Fe(Ⅲ)和无定型的水铁矿,在与含水层沉积物共培养12 d后,沉积物中铁与砷的释放量分别为510 mg/kg及1 150 μg/kg.江汉平原含水层中的原位微生物兼具砷/铁还原功能,在厌氧条件下可还原沉积物中的铁氧化物矿物并促进砷的释放,为深入揭示高砷地下水成因机理与地下水砷污染的防控提供重要科学依据.   相似文献   

15.
Incubation studies were carried out using 5 freshly collected sediments from shallow aquifers of the Hetao Basin, Inner Mongolia. The aquifer sediments covering a range of redox conditions, as indicated by their deep grey to yellow color were mixed with degassed artificial As solution or degassed deionized water at a ratio of solid to water of about 1:10 (wt./wt.). Suspensions which were either amended with glucose or autoclaved, were incubated in parallel with unamended suspensions. Five microcosm cultures of unamended sediments gradually release the equivalent of 0.03–0.30 μg/g As to the dissolved phase. The addition of glucose as a potential electron donor results in a marked stimulation in the mobilization of As (0.71–3.81 μg/g) in the amended incubations for all sediments. The quantity of As released accounts for 60–70% of As bound to Fe/Mn oxides in the original sediments. The microbially mediated mobilization of As with the organic nutrient as an electron donor is strongly associated with the As bound to Fe/Mn oxides, as well as the exchangeable As. During the incubations amended with glucose, 2–4% of the sediment Fe is released. The results suggest that the introduction of labile dissolved organic C into the yellowish sediment aquifers with As-free groundwater would reduce a significant proportion of the Fe(III) oxyhydroxides mediated by anaerobic bacteria respiration and increase groundwater As concentrations.  相似文献   

16.
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   

17.
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   

18.
Aquifer geochemistry was characterized at a field site in the Munshiganj district of Bangladesh where the groundwater is severely contaminated by As. Vertical profiles of aqueous and solid phase parameters were measured in a sandy deep aquifer (depth >150 m) below a thick confining clay (119 to 150 m), a sandy upper aquifer (3.5 to 119 m) above this confining layer, and a surficial clay layer (<3.5 m). In the deep aquifer and near the top of the upper aquifer, aqueous As levels are low (<10 μg/L), but aqueous As approaches a maximum of 640 μg/L at a depth of 30 to 40 m and falls to 58 μg/L near the base (107 m) of the upper aquifer. In contrast, solid phase As concentrations are uniformly low, rarely exceeding 2 μg/g in the two sandy aquifers and never exceeding 10 μg/g in the clay layers. Solid phase As is also similarly distributed among a variety of reservoirs in the deep and upper aquifer, including adsorbed As, As coprecipitated in solids leachable by mild acids and reductants, and As incorporated in silicates and other more recalcitrant phases. One notable difference among depths is that sorbed As loads, considered with respect to solid phase Fe extractable with 1 N HCl, 0.2 M oxalic acid, and a 0.5 M Ti(III)-citrate-EDTA solution, appear to be at capacity at depths where aqueous As is highest; this suggests that sorption limitations may, in part, explain the aqueous As depth profile at this site. Competition for sorption sites by silicate, phosphate, and carbonate oxyanions appear to sustain elevated aqueous As levels in the upper aquifer. Furthermore, geochemical profiles are consistent with the hypothesis that past or ongoing reductive dissolution of Fe(III) oxyhydroxides acts synergistically with competitive sorption to maintain elevated dissolved As levels in the upper aquifer. Microprobe data indicate substantial spatial comapping between As and Fe in both the upper and deep aquifer sediments, and microscopic observations reveal ubiquitous Fe coatings on most solid phases, including quartz, feldspars, and aluminosilicates. Extraction results and XRD analysis of density/magnetic separates suggest that these coatings may comprise predominantly Fe(II) and mixed valence Fe solids, although the presence of Fe(III) oxyhydroxides can not be ruled out. These data suggest As release may continue to be linked to dissolution processes targeting Fe, or Fe-rich, phases in these aquifers.  相似文献   

19.
Core sediments from two boreholes and groundwater from fifty four As-contaminated well waters were collected in the Chapai-Nawabganj area of northwestern Bangladesh for geochemical analysis. Groundwater arsenic concentrations in the uppermost aquifer (10 to 40 m of depth) range from 2.76?C315.15 mg/l (average 48.81 mg/l). Arsenic concentration in sediments ranges from 3.26?C10 mg/kg. Vertical distribution of arsenic in both groundwater and sediments shows that maximum As concentration (462 mg/l in groundwater and 10 mg/kg in sediments) occurs at a depth of 24 m. In January 2008, 2009 and 2010, maximum As concentration occurs at the same depth. Environmental scanning electron microscope (ESEM) with EDAX was used to investigate the presence of major and trace elements in the sediments. The dominant groundwater type is Ca-HCO3 with high concentrations of As and Fe, but with low levels of NO3 ? and SO3 ?2. Statistical analysis clearly shows that As is closely associated with Fe (R2 = 0.64) and Mn (R2 = 0.91) in sediments while As is not correlated with Fe and Mn in groundwater samples. Comparatively low Fe and Mn concentrations in some groundwater, suggest that probably siderite and/or rhodochrosite precipitated as secondary mineral on the surface of the sediment particles. The correlations along with results of sequential leaching experiments suggest that reductive dissolution of FeOOH and MnOOH mediated by anaerobic bacteria represents mechanism for releasing arsenic into the groundwater.  相似文献   

20.
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   

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