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1.
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   

2.
The mobilization of arsenic (As) to the groundwater was studied in a shallow Holocene aquifer on the Red River flood plain near Hanoi, Vietnam. The groundwater chemistry was investigated in a transect of 100 piezometers. Results show an anoxic aquifer featuring organic carbon decomposition with redox zonation dominated by the reduction of Fe-oxides and methanogenesis. Enhanced PCO2 pressure causes carbonate dissolution to take place but mainly in the soil and unsaturated zone. The concentration of As increases over depth to a concentration of up to 550 μg/L. Most As is present as As(III) but some As(V) is always found. Arsenic correlates well with NH4, relating its release to organic matter decomposition and the source of As appears to be the Fe-oxides being reduced. Part of the produced Fe(II) is apparently reprecipitated as siderite containing less As. Results from sediment extraction indicate most As to be related to the Fe-oxide fractions. The measured amount of sorbed As is low. In agreement, speciation calculations for a Fe-oxide surface suggest As(III) to constitute only 3% of the surface sites while the remainder is occupied by carbonate and silica species. The evolution in water chemistry over depth is homogeneous and a reactive transport model was constructed to quantify the geochemical processes along the vertical groundwater flow component. A redox zonation model was constructed using the partial equilibrium approach with organic carbon degradation in the sediment as the only rate controlling parameter. Apart from the upper meter a constant degradation rate of 0.15 C mmol/L/yr could explain the redox zonation throughout the aquifer. Modeling also indicates that the Fe-oxide being reduced is of a stable type like goethite or hematite. Arsenic is contained in the Fe-oxides and is first released during their dissolution. Our model further suggests that part of the released As is adsorbed on the surface of the remaining Fe-oxides and in this way may be retarded.  相似文献   

3.
Groundwater As concentrations >WHO limit (10 μg/L) are frequently found in the Po Plain (N. Italy). Although several hypotheses on As mobilization exist (i.e., reductive dissolution driven by peat degradation), the mechanisms of As release and subsequent attenuation acting in the multilayer aquifer in the Po Plain were poorly understood.The present work aims at implementing a reactive transport modeling of the aquifer system in Cremona, affected by As <183 μg/L, in order to quantify and test the feasibility of As release by the reductive dissolution of Fe-oxides driven by the degradation of peat contained in leaky aquitards and As attenuation downstream by the co-precipitation in iron sulfides.The model, based on a partial equilibrium approach, revealed that the observed As, Fe and Mn chemistry could be mostly explained by the simultaneous equilibrium between Fe-oxide and sulfate reduction and FeS precipitation and by the equilibrium of rhodochrosite precipitation/dissolution. Model results, together with litholog analysis, supported the assumption of peat as the likely source of organic matter driving As release. The model fitted to measured data showed that the peak in the organic carbon degradation rate at 20–40 m below surface (average of 0.67 mM/y), corresponding to the shallow peaty aquitard and the upper portion of the underlying semiconfined aquifer, is associated with the peak of net release of As (average of 0.32 μM/y) that is followed just downstream by a net precipitation in iron sulfides at 40–60 m below surface (average of 0.30 μM/y). These results support the assumptions of peaty aquifers as drivers of As release and iron sulfides as As traps. The model also outlined the following aspects that could have a broad applicability in other alluvial As affected aquifers worldwide: (a) shallow peaty aquitards may have a greater role in driving the As release since they likely have young and more reactive organic matter; (b) the occurrence of Fe-oxide reduction and FeS precipitation, that represent the As source and sink, together with sulfate reduction occurring simultaneously close to equilibrium may restrict the As mobility limiting the extent of contamination just downstream the source of organic matter that drives its release.  相似文献   

4.
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   

5.
An integrated study has been carried out to elucidate the distribution and occurrence of arsenic in selected groundwater samples in the area of Sherajdikhan, Bangladesh. Arsenic and other parameters (T, pH, EC, Na+, K+, Ca2+, Mg2+, Cl−, NO3 −, SO4 2−, HCO3 −, PO4 3−, Fe, Mn and DOC) have been measured in groundwater samples collected from shallow/deep tube wells at different depths. Hydrogeochemical data suggest that the groundwaters are generally Ca–Mg–HCO3 and Mg–Ca–HCO3 types with bicarbonate (HCO3 −) as the dominant anion, though the other type of water has also been observed. Dissolved arsenic in groundwater ranged from 0.006 to 0.461 mg/l, with 69% groundwater samples exceeded the Bangladesh limit for safe drinking water (0.05 mg/l). Correlation and principal component analysis have been performed to find out possible relationships among the examined parameters in groundwater. Low concentrations of NO3 − and SO4 2−, and high concentrations of DOC, HCO3 − and PO4 3− indicate the reducing condition of subsurface aquifer where sediments are deposited with abundant organic matter. Distinct relationship of As with Fe and Mn, and strong correlation with DOC suggests that the biodegradation of organic matter along with reductive dissolution of Fe–Mn oxyhydroxides has being considered the dominant process to release As in the aquifers studied herein.  相似文献   

6.
《Applied Geochemistry》2000,15(4):403-413
In some areas of Bangladesh and West Bengal, concentrations of As in groundwater exceed guide concentrations, set internationally and nationally at 10 to 50 μg l−1 and may reach levels in the mg l−1 range. The As derives from reductive dissolution of Fe oxyhydroxide and release of its sorbed As. The Fe oxyhydroxide exists in the aquifer as dispersed phases, such as coatings on sedimentary grains. Recalculated to pure FeOOH, As concentrations in this phase reach 517 ppm. Reduction of the Fe is driven by microbial metabolism of sedimentary organic matter, which is present in concentrations as high as 6% C. Arsenic released by oxidation of pyrite, as water levels are drawn down and air enters the aquifer, contributes negligibly to the problem of As pollution. Identification of the mechanism of As release to groundwater helps to provide a framework to guide the placement of new water wells so that they will have acceptable concentrations of As.  相似文献   

7.
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   

8.
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   

9.
The Wilcox aquifer is a major groundwater resource in the northern Gulf Coastal Plain (lower Mississippi Valley) of the USA, yet the processes controlling water chemistry in this clastic aquifer have received relatively little attention. The current study combines analyses of solutes and stable isotopes in groundwater, petrography of core samples, and geochemical modeling to identify plausible reactions along a regional flow path ～300 km long. The hydrochemical facies evolves from Ca-HCO3 upgradient to Na-HCO3 downgradient, with a sequential zonation of terminal electron-accepting processes from Fe(III) reduction through SO4 2? reduction to methanogenesis. In particular, decreasing SO4 2? and increasing δ34S of SO4 2? along the flow path, as well as observations of authigenic pyrite in core samples, provide evidence of SO4 2? reduction. Values of δ13C in groundwater suggest that dissolved inorganic carbon is contributed both by oxidation of sedimentary organic matter and calcite dissolution. Inverse modeling identified multiple plausible sets of reactions between sampled wells, which typically involved cation exchange, pyrite precipitation, CH2O oxidation, and dissolution of amorphous Fe(OH)3, calcite, or siderite. These reactions are consistent with processes identified in previous studies of Atlantic Coastal Plain aquifers. Contrasts in groundwater chemistry between the Wilcox and the underlying McNairy and overlying Claiborne aquifers indicate that confining units are relatively effective in limiting cross-formational flow, but localized cross-formational mixing could occur via fault zones. Consequently, increased pumping in the vicinity of fault zones could facilitate upward movement of saline water into the Wilcox.  相似文献   

10.
Continuous core sediments (to a depth of 90.1 m) taken at a transitional area of Holocene and Pleistocene deposits in Sonargaon, Bangladesh were characterized for their mineralogy and chemistry. Among the sediments of the lower part of the Holocene aquifer (depth: 18–29 m), where most domestic wells are installed, As is mostly fixed in biotite and organic phases. A positive correlation of As concentration with those of Al and Fe but not that of total organic C clearly suggests that biotite is a primary source of As. Although microbial reduction–dissolution of As-containing Fe oxyhydroxides is thought to cause As-enriched groundwater in the Ganges–Brahmaputra–Meghna delta plain, the authors conclude that chemical weathering of biotite is the primary formation mechanism and prevailing reducing conditions contribute to the expansion of As-enriched groundwater in the study area.  相似文献   

11.
Although arsenic (As) contamination has been extensively investigated in the aquifers of the lower and middle Gangetic plains, less attention has been given to the distribution and fate of As in the groundwater of the upper Gangetic plain, India. In the current study, groundwater samples (n = 40) were collected from Moradabad district in the upper Gangetic plain and analyzed for several physicochemical parameters to characterize the groundwater chemistry and evaluate various geogenic and anthropogenic factors controlling the occurrence, mobilization, and fate of As in the plain. Arsenic concentrations in groundwater ranged from 0.17 μg/L to 139 μg/L, with the majority of high-As groundwater associated with high Fe, Mn, and HCO3− and low NO3−, SO42−, and negative Eh values, implying that As was released via reductive dissolution of Fe and Mn oxyhydroxides in reducing conditions under the influence of organic matter degradation. Interrelationships between various geochemical variables and the natural background level (NBL) quantification of As suggested the influence of anthropogenic processes on the mobility of As in groundwater. Piper and Gibbs diagrams and various bivariate plots revealed that the majority of groundwater was of the Ca2+ − Mg2+ − HCO3− type and that the major ions in groundwater were derived from carbonate and silicate weathering, cation exchange and reverse ion exchange processes, and anthropogenic activities. Moreover, the results of principal component analysis (PCA), and hierarchical cluster analysis (HCA) also suggested geogenic and anthropogenic sources for the ion concentration in groundwater. The health risk assessment showed a higher non-carcinogenic risk for children and a higher carcinogenic risk for adults, respectively, due to the daily intake of As contaminated groundwater. Overall, this study represents the first systematic investigation of the distribution, geochemical behavior, and release process of As in groundwater in the study area and provides a strong base for future research in the alluvial aquifers of the upper Gangetic plain.  相似文献   

12.
The study area is located in the southwestern part of Bangladesh. Twenty-six groundwater samples were collected from both shallow and deep tube wells ranging in depth from 20 to 60 m. Multivariate statistical analyses including factor analysis, cluster analysis and multidimensional scaling were applied to the hydrogeochemical data. The results show that a few factors adequately represent the traits that define water chemistry. The first factor of Fe and HCO3 is strongly influenced by bacterial Fe (III) reduction which would raise both Fe and HCO3 concentrations in water. Na, Cl, Ca, Mg and PO4 are grouped under the second factor representing the salinity sources of waters. The third factor, represented by As, Mn, SO4 and K is related to As mobilization processes. Cluster analysis has been applied for the interpretation of the groundwater quality data. Initially Piper methods have been employed to obtain a first idea on the water types in the study area. Hierarchical cluster analysis was carried out for further classification of water types in the study area. Twelve components, namely, pH, Fe, Mn, As, Ca, Mg, Na, K, HCO3, Cl, SO4 and NO3 have been used for this purpose. With hierarchical clustering analysis the water samples have been classified into 3 clusters. They are very high, high and moderately As-enriched groundwater as well as groundwater with elevated SO4.  相似文献   

13.
《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   

14.
《Applied Geochemistry》2004,19(2):215-230
Sources of As in the Ganges sediments and microbial mechanisms of its release in groundwater were examined in the present study, where the authors have systematically examined the pertinent mineral species present in the sediments using XRD, TEM-EDS and EPMA techniques. The results show several As-bearing minerals in the Ganges sediments, in western Bangladesh. Iron-sulfide minerals consist of near-amorphous and/or crystalline precursors of framboidal pyrite and pyrite both of which contain As. Several types of Fe oxyhydroxides (oxides), which contain variable amounts of As were also found in muddy sediments. The content of As increases from Fe-oxides to the precursors of framboidal pyrite and pyrite. Four different chemical forms of As from the core sediments were determined. The sequentially extracted chemical forms are as follows: (1) acid soluble form (As mainly fixed in carbonates), (2) reducible form (As fixed in Fe- and/or Mn-oxides), (3) organic form, (4) insoluble form (As fixed mainly in sulfide and rarely in silicate minerals). Arsenic is dominantly sorbed on to Fe- and/or Mn-oxides, organic forms and sulfide minerals in most samples, although their relative abundances differ in different samples. Geomicrobial culture experiments were carried out to test the hypothesis that microbial processes play a key role in the release of As in groundwater. Batch culture and circulating water system experiments were designed using the sediments from Bangladesh. In the batch experiments, As was released at low Eh values a few days after adding nutrients containing glucose, polypepton and yeast extract, urea and fertilizer under a dominantly N2 atmosphere. This contrasts with the control experiments without nutrients. Circulating water experiments with sand layer in a N2 atmosphere showed similar results. These results support the hypothesis that microbial processes mediate the release of As into groundwater under reducing conditions. Glucose and polypepton used in the experiments may correspond to C and N sources, respectively. Younger sediments contain abundant organic matter, which is easily used by bacteria. So, the enhanced bacterial activity may correspond to simulation of accelerated natural diagenetic process using organic matter, or some fertilizer/wastewater effects.  相似文献   

15.
Pollution of groundwater in the Bengal Basin (Bangladesh and West Bengal, India) by arsenic (As) puts at risk the health of more than 100 million consumers. Using 1,580 borehole lithological logs and published hydrochemistry on 2,387 wells, it was predicted that low-As (<10 μg/L) groundwater exists, in palaeo-interfluvial aquifers of brown sand capped by a protective palaeosol, beneath at least 45,000 km2 of the Bengal Basin. The aquifers were predicted to be at a depth of as little as 25 m below ground level (mbgl), and typically no more than 50 mbgl. The predictions were confirmed along an east–west traverse 115 km in length (i.e. across half of Bangladesh) by drilling 28 new boreholes to 91-m depth to reveal subsurface sedimentology, and by mapping As distribution in groundwater. The aquifers identified occur at typically <40 mbgl and so are accessible with local drilling methods. A protective palaeosol that caps the palaeo-interfluvial aquifers prevents downward movement into them of As-polluted groundwater present in shallower palaeo-channel aquifers and ensures that the palaeo-interfluvial aquifers will yield low-As groundwater for the foreseeable future. Their use, in place of the shallower As-polluted palaeo-channel aquifers, would rapidly mitigate the health risks from consumption of As-polluted groundwater.  相似文献   

16.
鹿帅  苏小四  冯晓语  孙超 《地学前缘》2022,29(4):455-467
沈阳黄家水源地是我国北方地区典型的傍河地下水水源地,近岸带地下水中铁(Fe)、锰(Mn)、砷(As)含量严重超标。为查明地下水中As的来源与影响因素,对研究区河水、地下水以及土壤样品进行采集与测试,分析了水样常规指标与碳硫稳定同位素、土样中典型矿物、砷的含量及赋存形态。结果表明,研究区河水中As含量很低,而地下水中As含量普遍超标。河水入渗初期,氧化性河水使部分含As矿物发生氧化而释放As;随着河水入渗,地下水向还原环境转变,含As的Fe/Mn矿物发生还原性溶解,地下水中As含量逐渐升高。研究区典型矿物有黄铁矿、菱铁矿、软锰矿、赤铁矿、针铁矿、菱锰矿等,通过可交换态砷解吸、有机质结合态砷氧化、铁锰氧化物结合态砷还原性溶解等,介质中的As释放至地下水中。地下水中As含量与酸碱度(pH)、氧化还原电位(Eh)呈一定负相关,与溶解有机碳(DOC)、 HCO 3 -、Fe、Mn含量呈正相关。  相似文献   

17.
《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   

18.
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   

19.
The shallow alluvial aquifers of the delta plains and flood plains of Bangladesh, comprises about 70% of total land area are mostly affected by elevated concentrations of arsenic (As) in groundwater exposing a population of more than 35 million to As toxicity. Geochemical studies of shallow alluvial aquifer in the Meghna flood plain show that the uppermost yellowish grey sediment is low in As (1.03 mg/kg) compared to the lower dark grey to black sediment (5.24 mg/kg) rich in mica and organic matter. Sequential extraction data show that solid phase As bound to poorly crystalline and amorphous metal (Fe, Mn, Al)-oxyhydroxides is dominant in the grey to dark grey sediment and reaches its maximum level (3.05 mg/kg) in the mica rich layers. Amount of As bound to sulphides and organic matter also peaks in the dark grey to black sediment. Vertical distributions of major elements determined by X-ray fluorescence (XRF) show that iron (Fe2O3), aluminum (Al2O3) and manganese (MnO) follow the general trend of distribution of As in the sediments. Concentrations of As, Mn, Fe, HCO3 −, SO4 2− and NO3 − in groundwater reflect the redox status of the aquifer and are consistent with solid phase geochemistry. Mineralogical analysis by X-ray diffraction (XRD) and scanning electron microscopy (SEM) fitted with energy dispersive X-ray spectrometer (EDS) revealed dominance of crystalline iron oxides and hydroxides like magnetite, hematite and goethite in the oxidised yellowish grey sediment. Amorphous Fe-oxyhydroxides identified as grain coating in the mica and organic matter rich sediment suggests weathering of biotite is playing a critical role as the source of Fe(III)-oxyhydroxides which in turn act as sink for As. Presence of authigenic pyrite in the dark grey sediment indicates active reduction in the aquifer.  相似文献   

20.
《Applied Geochemistry》2006,21(6):949-963
In the central part of the Pannonian Basin, factors controlling the distribution of As in sediments and groundwater of the upper 500 m were studied. In core samples, the amounts of As, Fe and Mn extractable with hydroxylamine hydrochloride (NH2OH · HCl) in 25% acetic acid, the proportion of the <0.063 mm size fraction, and the sediment organic C (Corg) contents were measured. In the groundwaters concentrations of As, humic substances, and selected major chemical components were determined. In most core samples extractable Fe, as FeOOH, and Corg are correlated, but some samples have excess Fe, or organic matter. In cases where either excess Fe or excess organic matter is found, the amount of As is also elevated. The spatial distribution of As in the groundwater and the lack of a consistent correlation of As with a single component indicate that there is no single factor controlling the concentration of dissolved As over the entire study area. The only consistent feature is enrichment of As relative to Fe in the groundwater, compared to the sediments. This suggests that the dissolution of Fe minerals, which primarily adsorb As, is not congruent. In reducing conditions Fe(III) oxyhydroxides together with adsorbed As dissolve, and siderite with little or no As precipitates. When sub-regions are separated and studied individually, it can be shown that hydrogeological features of the sediments, the proportions of Fe minerals and sedimentary organic matter, and the concentration of dissolved humic materials, all influence the accumulation and mobilization of As. The significance of the different mobilizing processes, however, and the mean concentration of As, is different in the recharge, through-flow and discharge areas.  相似文献   

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