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1.
The solubility controls on vanadium (V) in groundwater were studied due to concerns over possible harmful health effects of ingesting V in drinking water. Vanadium concentrations in the northeastern San Joaquin Valley ranged from <3 μg/L to 70 μg/L with a median of 21 μg/L. Concentrations of V were highest in samples collected from oxic groundwater (49% > 25 μg/L) and lowest in samples collected from anoxic groundwater (70% < 0.8 μg/L). In oxic groundwater, speciation modeling (SM) using PHREEQC predicted that V exists primarily as the oxyanion H2VO4−. Adsorption/desorption reactions with mineral surfaces and associated oxide coatings were indicated as the primary solubility control of V5+ oxyanions in groundwater. Environmental data showed that V concentrations in oxic groundwater generally increased with increasing groundwater pH. However, data from adsorption isotherm experiments indicated that small variations in pH (7.4–8.2) were not likely as an important a factor as the inherent adsorption capacity of oxide assemblages coating the surface of mineral grains. In suboxic groundwater, accurate SM modeling was difficult since Eh measurements of source water were not measured in this study. Vanadium concentrations in suboxic groundwater decreased with increasing pH indicating that V may exist as an oxycationic species [e.g. V(OH)3+]. Vanadium may complex with dissolved inorganic and organic ligands under suboxic conditions, which could alter the adsorption behavior of V in groundwater. Speciation modeling did not predict the existence of V-inorganic ligand complexes and organic ligands were not collected as part of this study. More work is needed to determine processes governing V solubility under suboxic groundwater conditions. Under anoxic groundwater conditions, SM predicts that aqueous V exists as the uncharged V(OH)3 molecule. However, exceedingly low V concentrations show that V is sparingly soluble in anoxic conditions. Results indicated that V may be precipitating as V3+- or mixed V3+/Fe3+-oxides in anoxic groundwater, which is consistent with results of a previous study. The fact that V appears insoluble in anoxic (Fe reducing) redox conditions indicates that the behavior of V is different than arsenic (As) in aquifer systems where the reductive dissolution of Fe-oxides with As adsorbed to the surface is a well-documented mechanism for increasing As concentrations in groundwater. This hypothesis is supported by the relation of V to As concentrations in oxic versus anoxic redox conditions.Sequential extraction procedures (SEP) applied to aquifer material showed that the greatest amount of V was recovered by the nitric acid (HNO3) extract (37–71%), followed by the oxalate-ascorbic acid extract (19–60%) and the oxalate extract (3–14%). These results indicate that V was not associated with the solid phase as an easily exchangeable fraction. Although the total amount of V recovered was greatest for the HNO3 extract that targets V adsorbed to sorption sites of crystalline Al, Fe and Mn oxides, the greatest V saturation of sorption sites appeared to occur on the amorphous and poorly crystalline oxide solid phases targeted by the oxalate and oxalate-ascorbic acid extracts respectively. Adsorption isotherm experiments showed no correlation between V sorption and any of the fractions identified by the SEP. This lack of correlation indicates the application of an SEP alone is not adequate to estimate the sorption characteristics of V in an aquifer system.  相似文献   

2.
This study has evaluated the main hydrogeochemical characteristics that affect the quality of shallow groundwater in the coastal area at Kimje in South Korea. In this area, the chemical composition of groundwater is mostly classified into Na+?Cl? and Ca2++Mg2+?NO3-+Cl? types. These types are affected by three major factors: seawater intrusion, fertilizers and redox processes. The Na+?Cl? type, which is generally localized in the coastal area, shows typical characteristics of groundwater affected not only by modern seawater but also by old seawater residing in the reclaimed land. In contrast, the Ca2++Mg2+?NO3-+Cl? type, which is usually found inland, is very contaminated by fertilizers. As groundwater flows from the inland area to the coast, the redox condition changes from an oxic condition to a suboxic/anoxic condition. In addition, the reclamation has caused a large amount of underlying organic matter. These effects provide optimum conditions for the occurrence of redox processes in the coastal area.  相似文献   

3.
《Applied Geochemistry》2000,15(5):599-609
The effects of agriculture on the isotope geochemistry of Sr were investigated in two small watersheds in the Atlantic coastal plain of Maryland. Stratified shallow oxic groundwaters in both watersheds contained a retrievable record of increasing recharge rates of chemicals including NO3−, Cl, Mg, Ca and Sr that were correlated with increasing fertilizer use between about 1940 and 1990. The component of Sr associated with recent agricultural recharge was relatively radiogenic (87Sr/86Sr=0.715) and it was overwhelming with respect to Sr acquired naturally by water–rock interactions in the oxidized, non-calcareous portion of the saturated zone. Agricultural groundwaters that penetrated relatively unoxidized calcareous glauconitic sediments at depth acquired an additional component of Sr from dissolution of early Tertiary marine CaCO3 (87Sr/86Sr=0.708) while undergoing O2 reduction and denitrification. Ground-water discharge contained mixtures of waters of various ages and redox states. Two streams draining the area are considered to have higher 87Sr/86Sr ratios and NO3− concentrations than they would in the absence of agriculture; however, the streams have consistently different 87Sr/86Sr ratios and NO3− concentrations because the average depth to calcareous reducing (denitrifying) sediments in the local groundwater flow system was different in the two watersheds. The results of this study indicate that agriculture can alter significantly the isotope geochemistry of Sr in aquifers and streams and that the effects could vary depending on the types, sources and amounts of fertilizers added, the history of fertilizer use and groundwater residence times.  相似文献   

4.
The semi-arid Sahel regions of West Africa rely heavily on groundwater from shallow to moderately deep(100 m b.g.l.)crystalline bedrock aquifers for drinking water production.Groundwater quality may be affected by high geogenic arsenic(As)concentrations(10μg/L)stemming from the oxidation of sulphide minerals(pyrite,arsenopyrite)in mineralised zones.These aquifers are still little investigated,especially concerning groundwater residence times and the influence of the annual monsoon season on groundwater chemistry.To gain insights on the temporal aspects of As contamination,we have used isotope tracers(noble gases,~3H,stable water isotopes(~2 H,~(18)O))and performed hydrochemical analyses on groundwater abstracted from tube wells and dug wells in a small study area in southwestern Burkina Faso.Results revealed a great variability in groundwater properties(e.g.redox conditions,As concentrations,water level,residence time)over spatial scales of only a few hundred metres,characteristic of the highly heterogeneous fractured underground.Elevated As levels are found in oxic groundwater of circum-neutral pH and show little relation with any of the measured parameters.Arsenic concentrations are relatively stable over the course of the year,with little effect seen by the monsoon.Groundwater residence time does not seem to have an influence on As concentrations,as elevated As can be found both in groundwater with short(50 a)and long(10~3 a)residence times as indicated by ~3He/~4He ratios spanning three orders of magnitude.These results support the hypothesis that the proximity to mineralised zones is the most crucial factor controlling As concentrations in the observed redox/pH conditions.The existence of very old water portions with residence times10~3 years already at depths of50 m b.g.l.is a new finding for the shallow fractured bedrock aquifers of Burkina Faso,suggesting that overexploitation of these relatively low-yielding aquifers may be an issue in the future.  相似文献   

5.
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   

6.
Anthropogenic sources of carbon from landfill or waste leachate can promote reductive dissolution of in situ arsenic (As) and enhance the mobility of As in groundwater. Groundwater from residential-supply wells in a fractured crystalline-rock aquifer adjacent to a Superfund site in Raymond, New Hampshire, USA, showed evidence of locally enhanced As mobilization in relatively reducing (mixed oxic-anoxic to anoxic) conditions as determined by redox classification and other lines of evidence. Redox classification was determined from geochemical indicators based on threshold concentrations of dissolved oxygen (DO), nitrate (NO 3 – ), iron (Fe2+), manganese (Mn2+), and sulfate (SO 4 2– ). Redox conditions were evaluated also based on methane (CH4), excess nitrogen gas (N2) from denitrification, the oxidation state of dissolved As speciation (As(III) and As(V)), and several stable isotope ratios. Samples from the residential-supply wells primarily exhibit mixed redox conditions, as most have long open boreholes (typically 50–100?m) that receive water from multiple discrete fractures with contrasting groundwater chemistry and redox conditions. The methods employed in this study can be used at other sites to gauge redox conditions and the potential for As mobilization in complex fractured crystalline-rock aquifers where multiple lines of evidence are likely needed to understand As occurrence, mobility, and transport.  相似文献   

7.
Although high As groundwater has been observed in shallow groundwater of the Hetao basin, little is known about As distribution in deep groundwater. Quantitative investigations into relationships among chemical properties and among samples in different areas were carried out. Ninety groundwater samples were collected from deep aquifers of the northwest of the basin. Twenty-two physicochemical parameters were obtained for each sample. Statistical methods, including principal component analysis (PCA) and hierarchical cluster analysis (HCA), were used to analyze those data. Results show that As species were highly correlated with Fe species, NH4-N and pH. Furthermore, result of PCA indicates that high As groundwater was controlled by geological, reducing and oxic factors. The samples are classified into three clusters in HCA, which corresponded to the alluvial fans, the distal zone and the flat plain. Moreover, the combination of PCA with HCA shows the different dominant factors in different areas. In the alluvial fans, groundwater is influenced by oxic factors, and low As concentrations are observed. In the distal zone, groundwater is under suboxic conditions, which is dominated by reducing and geological factors. In the flat plain, groundwater is characterized by reducing conditions and high As concentrations, which is dominated by the reducing factor. This investigations indicate that deep groundwater in the alluvial fans mostly contains low As concentrations but high NO3 and U concentrations, and needs to be carefully checked prior to being used for drinking water sources.  相似文献   

8.
Naturally-occurring radionuclides (uranium, radium, and radon), major dissolved constituents, and trace elements were investigated in fresh groundwater in 117 wells in fractured crystalline rocks from the Piedmont region (North Carolina, USA). Chemical variations show a general transition between two water types: (1) slightly acidic (pH 5.0–6.0), oxic, low-total dissolved solids (TDS) waters, and (2) near neutral, oxic to anoxic, higher-TDS waters. The uranium, radium, and radon levels in groundwater associated with granite (Rolesville Granite) are systematically higher than other rock types (gneiss, metasedimentary, and metavolcanic rocks). Water chemistry plays a secondary role on radium and radon distributions as the 222Rn/226Ra activity ratio is correlated with redox-sensitive solutes such as dissolved oxygen and Mn concentrations, as well as overall dissolved solids content including major divalent cations and Ba. Since 224Ra/228Ra activity ratios in groundwater are close to 1, we suggest that mobilization of Ra and Rn is controlled by alpha recoil processes from parent nuclides on fracture surfaces, ruling out Ra sources from mineral dissolution or significant long-distance Ra transport. Alpha recoil is balanced by Ra adsorption that is influenced by redox conditions and/or ion concentrations, resulting in an approximately one order of magnitude decrease (~ 20,000 to ~ 2000) in the apparent Ra distribution coefficient between oxygen-saturated and anoxic conditions and also across the range of dissolved ion concentrations (up to ~ 7 mM). Thus, the U and Th content of rocks is the primary control on observed Ra and Rn activities in groundwater in fractured crystalline rocks, and in addition, linked dissolved solids concentrations and redox conditions impart a secondary control.  相似文献   

9.
 An unconfined aquifer system suggests an open system in the study area. Hydrochemical evolution is related to the flow path of groundwater. The groundwaters are divided into two hydrochemical facies in the study area, 1) Ca–Mg–HCO3 and 2) Ca–Mg–SO4HCO3. Facies 1 has shallow (young) waters which dominate in recharge areas during rapid flow conditions, whereas facies 2 may show shallow and mixed waters which dominate intermediate or discharge areas during low flow conditions. Ionic concentrations, TDS, EC and water quality are related to groundwater residence time and groundwater types. The groundwaters in the plain are chemically potable and suitable for both domestic and agricultural purposes. Received: 20 May 1996 · Accepted: 30 July 1996  相似文献   

10.
Differences in the degree of confinement, redox conditions, and dissolved organic carbon (DOC) are the main factors that control the persistence of nitrate and pesticides in the Upper Floridan aquifer (UFA) and overlying surficial aquifer beneath two agricultural areas in the southeastern US. Groundwater samples were collected multiple times from 66 wells during 1993–2007 in a study area in southwestern Georgia (ACFB) and from 48 wells in 1997–98 and 2007–08 in a study area in South Carolina (SANT) as part of the US Geological Survey National Water-Quality Assessment Program. In the ACFB study area, where karst features are prevalent, elevated nitrate-N concentrations in the oxic unconfined UFA (median 2.5 mg/L) were significantly (p = 0.03) higher than those in the overlying oxic surficial aquifer (median 1.5 mg/L). Concentrations of atrazine and deethylatrazine (DEA; the most frequently detected pesticide and degradate) were higher in more recent groundwater samples from the ACFB study area than in samples collected prior to 2000. Conversely, in the SANT study area, nitrate-N concentrations in the UFA were mostly <0.06 mg/L, resulting from anoxic conditions and elevated DOC concentrations that favored denitrification. Although most parts of the partially confined UFA in the SANT study area were anoxic or had mixed redox conditions, water from 28 % of the sampled wells was oxic and had low DOC concentrations. Based on the groundwater age information, nitrate concentrations reflect historic fertilizer N usage in both the study areas, but with a lag time of about 15–20 years. Simulated responses to future management scenarios of fertilizer N inputs indicated that elevated nitrate-N concentrations would likely persist in oxic parts of the surficial aquifer and UFA for decades even with substantial decreases in fertilizer N inputs over the next 40 years.  相似文献   

11.
Large karstic springs in east-central Florida, USA were studied using multi-tracer and geochemical modeling techniques to better understand groundwater flow paths and mixing of shallow and deep groundwater. Spring water types included Ca–HCO3 (six), Na–Cl (four), and mixed (one). The evolution of water chemistry for Ca–HCO3 spring waters was modeled by reactions of rainwater with soil organic matter, calcite, and dolomite under oxic conditions. The Na–Cl and mixed-type springs were modeled by reactions of either rainwater or Upper Floridan aquifer water with soil organic matter, calcite, and dolomite under oxic conditions and mixed with varying proportions of saline Lower Floridan aquifer water, which represented 4–53% of the total spring discharge. Multiple-tracer data—chlorofluorocarbon CFC-113, tritium (3H), helium-3 (3Hetrit), sulfur hexafluoride (SF6)—for four Ca–HCO3 spring waters were consistent with binary mixing curves representing water recharged during 1980 or 1990 mixing with an older (recharged before 1940) tracer-free component. Young-water mixing fractions ranged from 0.3 to 0.7. Tracer concentration data for two Na–Cl spring waters appear to be consistent with binary mixtures of 1990 water with older water recharged in 1965 or 1975. Nitrate-N concentrations are inversely related to apparent ages of spring waters, which indicated that elevated nitrate-N concentrations were likely contributed from recent recharge.The online version of the original article can be found at  相似文献   

12.
Large karstic springs in east-central Florida, USA were studied using multi-tracer and geochemical modeling techniques to better understand groundwater flow paths and mixing of shallow and deep groundwater. Spring water types included Ca–HCO3 (six), Na–Cl (four), and mixed (one). The evolution of water chemistry for Ca–HCO3 spring waters was modeled by reactions of rainwater with soil organic matter, calcite, and dolomite under oxic conditions. The Na–Cl and mixed-type springs were modeled by reactions of either rainwater or Upper Floridan aquifer water with soil organic matter, calcite, and dolomite under oxic conditions and mixed with varying proportions of saline Lower Floridan aquifer water, which represented 4–53% of the total spring discharge. Multiple-tracer data—chlorofluorocarbon CFC-113, tritium (3H), helium-3 (3Hetrit), sulfur hexafluoride (SF6)—for four Ca–HCO3 spring waters were consistent with binary mixing curves representing water recharged during 1980 or 1990 mixing with an older (recharged before 1940) tracer-free component. Young-water mixing fractions ranged from 0.3 to 0.7. Tracer concentration data for two Na–Cl spring waters appear to be consistent with binary mixtures of 1990 water with older water recharged in 1965 or 1975. Nitrate-N concentrations are inversely related to apparent ages of spring waters, which indicated that elevated nitrate-N concentrations were likely contributed from recent recharge.An erratum to this article can be found at  相似文献   

13.
Degradation patterns of sedimentary algal lipids were tracked with time under variable redox treatments designed to mimic conditions in organic-rich, bioturbated deposits. Uniformly 13C-labeled algae were mixed with Long Island Sound surface muddy sediments and exposed to different redox regimes, including continuously oxic and anoxic, and oscillated oxic: anoxic conditions. Concentrations of several 13C-labeled algal fatty acids (16:1, 16:0 and 18:1), phytol and an alkene were measured serially. Results showed a large difference (∼10×) in first-order degradation rate constants of cell-associated lipids between continuously oxic and anoxic conditions. Exposure to oxic conditions increased the degradation of cell-associated lipids, and degradation rate constants were positive functions (linear or nonlinear) of the fraction of time sediments were oxic. Production of two new 13C-labeled compounds (iso-15:0 fatty acid and hexadecanol) further indicated that redox conditions and oxic: anoxic oscillations strongly affect microbial degradation of algal lipids and net synthesis of bacterial biomass. Production of 13C-labeled iso-15:0 fatty acid (a bacterial biomarker) was inversely proportional to the fraction of time sediments were oxic, rapidly decreasing after 10 days of incubation under oxic and frequently oscillated conditions. Turnover of bacterial biomass was faster under continuously or occasionally oxic conditions than under continuously anoxic conditions. 13C-labeled hexadecanol, an intermediate degradation product, accumulated under anoxic conditions but not under oxic or periodically oxic conditions. The frequency of oxic: anoxic oscillation clearly alters both the rate and pathways of lipid degradation in surficial sediments. Terminal degradation efficiency and lipid products from degradation of algal material depend on specific patterns of redox fluctuations.  相似文献   

14.
The groundwater downstream of a former sewage irrigation farm in Berlin is contaminated with ammonium (NH4 +) and para-toluenesulfonamide (p-TSA), besides other anthropogenic pollutants. In the field, in situ removal of NH4 + by gaseous oxygen (O2) and air injection is currently being tested. A laboratory column experiment using aquifer material and groundwater from the site was performed to determine whether this remediation technology is also feasible to reduce high p-TSA concentrations in the anoxic groundwater. First, the column was operated under anoxic conditions. Later, compressed air was introduced into the system to simulate oxic conditions. Samples were collected from the column outlet before and after the addition of compressed air. The experiment revealed that whereas p-TSA was not removed under anoxic conditions, it was almost fully eliminated under oxic conditions. Results were modelled using a transient one-dimensional solute transport model. The degradation rate constants for p-TSA increased from 2.8E−06 to 7.5E−05 s–1 as a result of microbial adaption to the change of redox conditions. Results show that O2 injection into an anoxic aquifer is a successful strategy for p-TSA remediation.  相似文献   

15.
Analyses of groundwater samples collected from several locations in a small watershed of the Deccan Trap Hydrologic Province, indicated anomalously higher values of nitrate than the background. However, the NO3 concentrations in water from dug wells under pastureland where the subsurface material consisted of stony waste were minimum. The maximum values were reported for water from dug wells where the principal land use was agricultural. Lowering of NO3 values under shallow water-table conditions suggests denitrification. Higher concentrations of nitrate determined for samples collected from the wells with a deeper water-table indicate that denitrification process is inactive. The high values of nitrate coinciding with agricultural land use indicate fertilizers as the main source of nitrate pollution of ground-water. Decrease in Cl/NO3 ratio for agricultural land use confirms this inference.  相似文献   

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

17.
Groundwater residence time in the Kulnura–Mangrove Mountain aquifer was assessed during a multi-year sampling programme using general hydrogeochemistry and isotopic tracers (H2O stable isotopes, δ13CDIC, 3H, 14C and 87Sr/86Sr). The study included whole-rock analysis from samples recovered during well construction at four sites to better characterise water–rock interactions. Based on hydrogeochemistry, isotopic tracers and mineral phase distribution from whole-rock XRD analysis, two main groundwater zones were differentiated (shallow and deep). The shallow zone contains oxidising Na–Cl-type waters, low pH, low SC and containing 3H and 14C activities consistent with modern groundwater and bomb pulse signatures (up to 116.9 pMC). In this shallow zone, the original Hawkesbury Sandstone has been deeply weathered, enhancing its storage capacity down to ～50 m below ground surface in most areas and ～90 m in the Peats Ridge area. The deeper groundwater zone was also relatively oxidised with a tendency towards Ca–HCO3-type waters, although with higher pH and SC, and no 3H and low 14C activities consistent with corrected residence times ranging from 11.8 to 0.9 ka BP. The original sandstone was found to be less weathered with depth, favouring the dissolution of dispersed carbonates and the transition from a semi-porous groundwater media flow in the shallow zone to fracture flow at depth, with both chemical and physical processes impacting on groundwater mean residence times.

Detailed temporal and spatial sampling of groundwater revealed important inter-annual variations driven by groundwater extraction showing a progressive influx of modern groundwater found at >100 m in the Peats Ridge area. The progressive modernisation has exposed deeper parts of the aquifer to increased NO3? concentrations and evaporated irrigation waters. The change in chemistry of the groundwater, particularly the lowering of groundwater pH, has accelerated the dissolution of mineral phases that would generally be inactive within this sandstone aquifer triggering the mobilisation of elements such as aluminium in the aqueous phase.  相似文献   

18.
High nitrate concentrations, above the WHO guideline of 50 mg l−1, were observed in samples of shallow wells reaching the Yeumbeul suburb (Senegal) area groundwater. This groundwater is exploited by 7000 houses and therefore there are health implications. Correlations between parameters such as nitrate content (NO3−) in the groundwater and soil water, the distance between shallow wells and family latrines, and soil water chloride (Cl−) and colon bacillus content led to two possible sources of groundwater pollution: first, contamination by non impervious and shallow latrines; and second, the leaching of soil NO3− from waste organic matter carried in groundwater.  相似文献   

19.
Interplay of S and As in Mekong Delta sediments during redox oscillations   总被引：1，自引：1，他引：0  
The cumulative effects of periodic redox cycling on the mobility of As,Fe,and S from alluvial sediment to groundwater were investigated in bioreactor experiments.Two particular sediments from the alluvial floodplain of the Mekong Delta River were investigated:Matrix A(14 m deep)had a higher pyrite concentration than matrix B(7 m deep)sediments.Gypsum was present in matrix B but absent in matrix A.In the reactors,the sediment suspensions were supplemented with As(Ⅲ)and SO_4~(2-),and were subjected to three full-redox cycles entailing phases of nitrogen/CO_2,compressed air sparging,and cellobiose addition.Major differences in As concentration and speciation were observed upon redox cycling.Evidences support the fact that initial sediment composition is the main factor controlling arsenic release and its speciation during the redox cycles.Indeed,a high pyrite content associated with a low SO_4~(2-)content resulted in an increase in dissolved As concentrations,mainly in the form of As(Ⅲ),after anoxic half-cycles;whereas a decrease in As concentrations mainly in the form of As(Ⅴ),was instead observed after oxic half-cycles.In addition,oxic conditions were found to be responsible for pyrite and arsenian pyrite oxidation,increasing the As pool available for mobilization.The same processes seem to occur in sediment with the presence of gypsum,but,in this case,dissolved As were sequestered by biotic or abiotic redox reactions occurring in the Fe—S system,and by specific physico-chemical condition(e.g.pH).The contrasting results obtained for two sediments sampled from the same core show that many complexes and entangled factors are at work,and further refinement is needed to explain the spatial and temporal variability of As release to groundwater of the Mekong River Delta(Vietnam).  相似文献   

20.
The Silurian bedrock aquifer constitutes a major aquifer system for groundwater supply across the Ontario province in Canada. The application of natural and industrial fertilizers near urban centers has led to groundwater NO3−-N concentrations that sometimes have exceeded the drinking water limit, posing a threat to the usage of groundwater for the human consumption. Therefore, there is a growing interest and concern about how nitrate is being leached, transported and potentially attenuated in bedrock aquifers. This study assesses the local distribution of groundwater NO3− in the up-gradient area of two historically impacted municipal wells, called Carter Wells, in the City of Guelph, Canada, in order to evaluate the potential nitrate attenuation mechanisms, using both groundwater geochemical and isotopic analysis (3H, δ15N-NO3, δ18O-NO3, δ18O-SO4, δ34S-SO4) and a detailed vertical hydrogeological and geochemical bedrock characterization. The results indicate that probably the main source of nitrate to the Carter Wells is the up-gradient Arkell Research Station (ARS), an agricultural research facility where manure has been historically applied. The overburden and bedrock groundwater with high NO3 concentrations at the ARS exhibits a manure-related δ15N and δ18O signature, isotopically similar to the high nitrate in the down-gradient groundwater from domestic wells and from the Carter Wells. The nitrate spatial distribution appears to be influenced and controlled by the geology, in which more permeable rock is found in the Guelph Formation which in turn is related to most of the high NO3− groundwater. The presence of an underlying low permeability Eramosa Formation favors the development of oxygen-depleted conditions, a key factor for the occurrence of denitrification. Groundwater with low NO3−-N concentrations associated with more oxygen-limited conditions and coincident with high SO42− concentrations are related to more enriched δ15N and δ18O values in NO3− and to more depleted δ34S and δ18O values in SO42−, suggesting that denitrification coupled with pyrite oxidation is taking place. The presence of macro crystalized and disseminated pyrite especially in the Eramosa Formation, can support the occurrence of this attenuation process. Moreover, based on tritium analysis, some denitrification can occur in shallow bedrock and within relatively short residence times, associated with less permeable conditions in depth which facilitates oxygen consumption through sulfide oxidation. The role of denitrification mediated by organic carbon cannot be discarded at the study site. This study suggests that the geological configuration and particularly the presence of low permeability Eramosa Formation can play an important role on nitrate natural attenuation, which may serve as a decision factor on defining the bedrock water supply system for both domestic and municipal purposes.  相似文献   

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