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1.
Arsenic sequestration by sorption processes in high-iron sediments   总被引：3，自引：0，他引：3  
High-iron sediments in North Haiwee Reservoir (Olancha, CA), resulting from water treatment for removal of elevated dissolved arsenic in the Los Angeles Aqueduct system, were studied to examine arsenic partitioning between solid phases and porewaters undergoing shallow burial. To reduce arsenic in drinking water supplies, ferric chloride and a cationic polymer coagulant are added to the aqueduct upstream of Haiwee Reservoir, forming an iron-rich floc that scavenges arsenic from the water. Analysis by synchrotron X-ray absorption spectroscopy (XAS) showed that the aqueduct precipitate is an amorphous hydrous ferric oxide (HFO) similar to ferrihydrite, and that arsenic is associated with the floc as adsorbed and/or coprecipitated As(V). Arsenic-rich floc and sediments are deposited along the inlet channel as aqueduct waters enter the reservoir. Sediment core samples were collected in two consecutive years from the edge of the reservoir along the inlet channel using 30- or 90-cm push cores. Cores were analyzed for total and extractable arsenic and iron concentrations. Arsenic and iron speciation and mineralogy in sediments were examined at selected depths by synchrotron XAS and X-ray diffraction (XRD). Sediment-porewater measurements were made adjacent to the core sample sites using polyacrylamide gel probe samplers. Results showed that sediment As(V) is reduced to As(III) in all cores at or near the sediment-water interface (0-4 cm), and only As(III) was observed in deeper sediments. Analyses of EXAFS spectra indicated that arsenic is present in the sediments mostly as a bidentate-binuclear, inner-sphere sorption complex with local atomic geometries similar to those found in laboratory studies. Below about 10 cm depth, XAS indicated that the HFO floc had been reduced to a mixed Fe(II, III) solid with a local structure similar to that of synthetic green rust (GR) but with a slightly contracted average interatomic Fe-Fe distance in the hydroxide layer. There was no evidence from XRD for the formation of a crystalline GR phase. The release of dissolved iron (presumably Fe2+) and arsenic to solution, as monitored by in situ gel probes, was variable but, in general, occurred at greater depths than arsenic reduction in the sediments by spectroscopic observations and appears to be near or below the depth at which sediment GR was identified. These data point to reductive dissolution of the sorbent iron phase as the primary mechanism of release of sorbed arsenic to solution.  相似文献   

2.
High arsenic (As) groundwater is widely distributed in northwestern Hetao Plain, an arid region with sluggish groundwater flow. Observed As concentration in groundwater from wells ranges from 76 to 1,093 μg/l. Most water samples have high total dissolved solids, with Cl and HCO3 as the dominant anions and Na as the dominant cation. The major hydrochemical types of most saline groundwaters are Na–Mg–Cl–HCO3 and Na–Mg–Cl. By contrast, fresh groundwaters generally belong to the Na–Mg–HCO3 type. High concentrations of arsenic in shallow aquifers are associated with strongly reducing conditions, as evidenced by high concentrations of dissolved organic carbon, ammonium, as well as dissolved sulfide and Fe, dominance of arsenite, relatively low concentrations of nitrate and sulfate, and occasionally high content of dissolved methane (CH4). High As groundwaters from different places at Hetao Plain experienced different redox processes. Fluoride is also present in high As groundwater, ranging between 0.40 and 3.36 mg/l. Although fluorosis poses an additional health problem in the region, it does not correlate well with As in spatial distribution. Geochemical analysis indicates that evapotranspiration is an important process controlling the enrichment of Na and Cl, as well as trace elements such as As, B, and Br in groundwater. Electronic supplementary material  The online version of this article (doi:) contains supplementary material, which is available to authorized users.  相似文献   

3.
This study reports on the mobility and retention of trace elements in cassiterite tailings at the inactive Jumna mill, tropical north Queensland. Since the 1980s, the uncapped tailings have developed laterally discontinuous Fe-rich hardpans, which are located in the higher parts of gently sloping tailings masses and at the top (<50 cm) of the tailings piles. Hardpan-cemented tailings comprise thin layers (typically ∼0.2–2 mm thick) of HFO (hydrous ferric oxides) and sulfate efflorescences cementing tailings grains. In comparison to the tailings, the hardpan-cemented tailings contain significantly higher median As, Ca, Cd, Co, Cu, Fe, In, Mn, Mo, Stotal, Th, U, Y and Zn values. Partial leaching studies of tailings and pond water analyses indicate that wetting and acidification of Fe-cemented tailings removes significant proportions of trace elements into pore and surface waters. Tin shows no mobility due to the presence of weathering-resistant cassiterite (SnO2) and, As and Pb display limited mobility possibly due to their coprecipitation with jarosite-type phases and HFO materials at the top of the tailings profile. By contrast, the trace elements Cd, Ce, Cu, La, Ni, Pb, U and Zn display the greatest mobility, possibly due to their incorporation in soluble sulfate efflorescences and sorption onto mineral and HFO surfaces. Hence, the Fe-rich hardpans do not protect the sulfidic tailings from further oxidation nor do they cause permanent sequestration of trace elements.  相似文献   

4.
The sediment from an acid mine drainage affected reservoir of Guizhou province of China has the iron and arsenic concentration of about 400 and 2.6 g/kg, respectively. Sediment cores were collected, and were used to study the arsenic behavior in the seriously acidified reservoir from the viewpoint of chemical thermodynamics. The limestone neutralization and ferric iron hydrolysis regulated the porewater pH from about 2.9–5.8. The reductive dissolution of As–Fe-rich (hydr)oxides under the mild acidic conditions was the main mechanism for the release of absorbed arsenic into porewater. The maximum concentrations of iron, sulfate and arsenic reached to about 2,800, 9,000 and 1 mg/l, respectively. Arsenic speciation transformation and hydrous ferric oxide (HFO) crystallization enhanced the arsenic mobility in sediment. In addition, the iron sulfide minerals diagenesis could play a role in removing the dissolved arsenic from porewater. The actual distribution of arsenic concentration in porewater was well simulated using the model of surface complexation of arsenic to HFO. Although arsenic concentration in porewater could be above 100 times higher than that of reservoir water, it was not easy to release into the reservoir water through diffusion, because the shallow sediment had relatively strong arsenic adsorption capacity, and new HFO could be generated continuously at the sediment water interface.  相似文献   

5.
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   

6.
 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   

7.
The study region covers 1,650 km2 of the Mid-Ganga Basin in Bihar, experiencing intensive groundwater draft. The area forms a part of the Gangetic alluvial plain where high incidence of arsenic groundwater contamination (>50 μg/l) has recently been detected. Seventy-seven groundwater samples have been collected and analysed for major ions, iron and arsenic. Arsenic contamination (max 620 μg/l) is confined in hand pump zones (15–35 m) within the newer alluvium deposited during Middle Holocene to Recent age. The older alluvial aquifers are arsenic-safe and recorded maximum concentration as 9 μg/l. Out of 12 hydrochemical facies identified, four have been found arsenic-affected: Ca–HCO3, Mg–HCO3, Ca–Mg–HCO3 and Mg–Ca–HCO3. The geochemical evolution of groundwater, as investigated by graphical interpretation and statistical techniques (correlation, principal component analysis) revealed that dissolution of detrital calcite, dolomite and infiltration of rainwater are the major processes shaping the groundwater chemistry in the newer alluvium. Arsenic and iron showed strong positive correlation. Rainfall infiltration, carrying organic matter from recently accumulated biomass from this flood-prone belt, plays a critical role in releasing arsenic and iron present in the sediments. Geochemical evolution of groundwater in older alluvium follows a different path, where cation-exchange has been identified as a significant process.  相似文献   

8.
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   

9.
Detailed hydrogeochemical and isotopic data of groundwaters from the Hammamet–Nabeul unconfined aquifer are used to provide a better understanding of the natural and anthropogenic processes that control the groundwater mineralization as well as the sources of different groundwater bodies. It has been demonstrated that groundwaters, which show Na–Cl and Ca–SO4–Cl water facies, are mainly influenced by the dissolution of evaporates, the dedolomitization and the cation-exchange process; and supplementary by anthropogenic process in relation with return flow of irrigation waters. The isotopic signatures permit to classify the studied groundwaters into two different groups. Non-evaporated groundwaters that are characterized by depleted δ 18O and δ 2H contents highlighting the importance of modern recharge at higher altitude. Evaporated groundwaters with enriched contents reflecting the significance infiltration of return flow irrigation waters. Tritium data in the studied groundwaters lend support to the existence of pre-1950 and post-1960 recharge. Carbon-14 activities in shallow wells that provide evidence to the large contamination by organic 14C corroborate the recent origin of the groundwaters in the study area.  相似文献   

10.
Excessive arsenic concentrations above the Argentinean and WHO guidelines for drinking water (10 μg L−1) affects shallow aquifers of the southern Pampean Plain (Argentina) hosted in the Pampean and the Post Pampean formations (loess and reworked loess; Plio-Pleistocene–Holocene). Health problems related to high As concentrations in drinking waters are known as Endemic Regional Chronic Hydroarsenicism. Hydrochemistry of shallow groundwaters and soil geochemistry were investigated aiming to (1) understand the partition of As in the solid phase and its relationship with unacceptable As concentrations in waters, (2) identify the provision source of As to groundwaters. Only 5% of the samples had As concentrations <10 μg L−1; in 27% As concentrations ranged from 10 to 50 μg L−1 and in 58% it reached 60–500 μg L−1. The coarse fraction (50–2,000 μm) hosts about 27% of the total As in the solid phase, being positively correlated to Ba (p < 0.01; r 2 = 0.93). About 70% is included in the <2 μm fraction and had positive correlations of As–Fe (p < 0.05; r 2 = 0.85) and As–Cr (p < 0.05; r 2 = 0.68). Soils and sediment sand fractions of vadose zones are the primary sources of As in shallow groundwater while adsorption–desorption processes, codisolution–coprecipitation, and evaporation during the dry seasons raise As concentrations in waters exceeding the guideline value for drinking water.  相似文献   

11.
The arsenic content of geothermal hot springs and their sediments in the north-central Andean region of Ecuador has been investigated. The area of study is located between parallels 1°11′N and 1°30′S and includes five provinces. The area is rich in geothermal surface manifestations that are mainly used for medicinal baths in recreational complexes. Unfortunately, water residuals without treatment are released from the recreational facilities to surrounding water bodies. The results indicate that total arsenic in geothermal waters in this region has a range of 2–969 μg As/L, and sediments contain arsenic ranging from 1.6 to 717.6 mg/kg. Chemical analyses of sediment samples show the presence of sulfur, iron, aluminum and calcium. A high concentration of natural organic matter was also found in some samples (20–29.5%); thus sorption and coprecipitation can be the main mechanisms of As immobilization on mineral phases and natural organic matter.  相似文献   

12.
Arsenic and Antimony in Groundwater Flow Systems: A Comparative Study   总被引：3，自引：0，他引：3  
Arsenic (As) and antimony (Sb) concentrations and speciation were determined along flow paths in three groundwater flow systems, the Carrizo Sand aquifer in southeastern Texas, the Upper Floridan aquifer in south-central Florida, and the Aquia aquifer of coastal Maryland, and subsequently compared and contrasted. Previously reported hydrogeochemical parameters for all three aquifer were used to demonstrate how changes in oxidation–reduction conditions and solution chemistry along the flow paths in each of the aquifers affected the concentrations of As and Sb. Total Sb concentrations (SbT) of groundwaters from the Carrizo Sand aquifer range from 16 to 198 pmol kg−1; in the Upper Floridan aquifer, SbT concentrations range from 8.1 to 1,462 pmol kg−1; and for the Aquia aquifer, SbT concentrations range between 23 and 512 pmol kg−1. In each aquifer, As and Sb (except for the Carrizo Sand aquifer) concentrations are highest in the regions where Fe(III) reduction predominates and lower where SO4 reduction buffers redox conditions. Groundwater data and sequential analysis of the aquifer sediments indicate that reductive dissolution of Fe(III) oxides/oxyhydroxides and subsequent release of sorbed As and Sb are the principal mechanism by which these metalloids are mobilized. Increases in pH along the flow path in the Carrizo Sand and Aquia aquifer also likely promote desorption of As and Sb from mineral surfaces, whereas pyrite oxidation mobilizes As and Sb within oxic groundwaters from the recharge zone of the Upper Floridan aquifer. Both metalloids are subsequently removed from solution by readsorption and/or coprecipitation onto Fe(III) oxides/oxyhydroxides and mixed Fe(II)/Fe(III) oxides, clay minerals, and pyrite. Speciation modeling using measured and computed Eh values predicts that Sb(III) predominate in Carrizo Sand and Upper Floridan aquifer groundwaters, occurring as the Sb(OH)30 species in solution. In oxic groundwaters from the recharge zones of these aquifers, the speciation model suggests that Sb(V) occurs as the negatively charged Sb(OH)6− species, whereas in sufidic groundwaters from both aquifers, the thioantimonite species, HSb2S4 − and Sb2S4 2−, are predicted to be important dissolved forms of Sb. The measured As and Sb speciation in the Aquia aquifer indicates that As(III) and Sb(III) predominate. Comparison of the speciation model results based on measured Eh values, and those computed with the Fe(II)/Fe(III), S(-II)/SO4, As(III)/As(V), and Sb(III)/Sb(V) couples, to the analytically determined As and Sb speciation suggests that the Fe(II)/Fe(III), S(-II)/SO4 couples exert more control on the in situ redox condition of these groundwaters than either metalloid redox couple.  相似文献   

13.
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   

14.
Arsenic (As) concentrations and speciation were determined in groundwaters along a flow-path in the Upper Floridan aquifer (UFA) to investigate the biogeochemical “evolution“ of As in this relatively pristine aquifer. Dissolved inorganic As species were separated in the field using anion-exchange chromatography and subsequently analyzed by inductively coupled plasma mass spectrometry. Total As concentrations are higher in the recharge area groundwaters compared to down-gradient portions of UFA. Redox conditions vary from relatively oxic to anoxic along the flow-path. Mobilization of As species in UFA groundwaters is influenced by ferric iron reduction and subsequent dissolution, sulfate reduction, and probable pyrite precipitation that are inferred from the data to occur along distinct regions of the flow-path. In general, the distribution of As species are consistent with equilibrium thermodynamics, such that arsenate dominates in more oxidizing waters near the recharge area, and arsenite predominates in the progressively reducing groundwaters beyond the recharge area.  相似文献   

15.
The need for more agricultural or residential land has encouraged reclamation at the coastal areas of Korea since 1200 ad (approximately). The groundwaters of these reclaimed areas could be expected to reveal hydrogeochemical properties different from those of areas directly affected by seawater intrusion. The purpose of this study, therefore, was to examine the salinization of shallow groundwater in a coastal reclaimed area and to identify the effect of land reclamation on groundwater quality. Major cations and anions, iodide, total organic carbon, δD, δ 18O and δ 13C were measured to assist the hydrogeochemical analysis. Chloride, δD and δ 18O data clearly show that the Na–Cl type water results from mixing of groundwater with seawater. In particular, the δD and δ 18O of Ca+Mg–Cl+NO3 type groundwaters are close to the meteoric water line, but Na–Cl type waters enriched in chloride are 18O-enriched with respect to the meteoric water line. Meanwhile, carbon isotopic data and I/Cl ratios strongly suggest that there are various sources of salinity. The δ 13C values of Na–Cl type groundwaters are generally similar to those of Ca+Mg–Cl+NO3 type waters, which are depleted in 13C with respect to seawater. I/Cl ratios of Na–Cl type groundwater are 10–100 times higher than that of seawater. Because the reclamation has incorporated a large amount of organic matter, it provides optimum conditions for the occurrence of redox processes in the groundwater system. Therefore, the salinization of groundwater in the study area seems to be controlled not only by saltwater intrusion but also by other effects, such as those caused by residual salts and organic matter in the reclaimed sediments.  相似文献   

16.
High levels of arsenic in groundwater and drinking water are a major health problem. Although the processes controlling the release of As are still not well known, the reductive dissolution of As-rich Fe oxyhydroxides has so far been a favorite hypothesis. Decoupling between arsenic and iron redox transformations has been experimentally demonstrated, but not quantitatively interpreted. Here, we report on incubation batch experiments run with As(V) sorbed on, or co-precipitated with, 2-line ferrihydrite. The biotic and abiotic processes of As release were investigated by using wet chemistry, X-ray diffraction, X-ray absorption and genomic techniques. The incubation experiments were carried out with a phosphate-rich growth medium and a community of Fe(III)-reducing bacteria under strict anoxic conditions for two months. During the first month, the release of Fe(II) in the aqueous phase amounted to only 3% to 10% of the total initial solid Fe concentration, whilst the total aqueous As remained almost constant after an initial exchange with phosphate ions. During the second month, the aqueous Fe(II) concentration remained constant, or even decreased, whereas the total quantity of As released to the solution accounted for 14% to 45% of the total initial solid As concentration. At the end of the incubation, the aqueous-phase arsenic was present predominately as As(III) whilst X-ray absorption spectroscopy indicated that more than 70% of the solid-phase arsenic was present as As(V). X-ray diffraction revealed vivianite Fe(II)3(PO4)2.8H2O in some of the experiments. A biogeochemical model was then developed to simulate these aqueous- and solid-phase results. The two main conclusions drawn from the model are that (1) As(V) is not reduced during the first incubation month with high Eh values, but rather re-adsorbed onto the ferrihydrite surface, and this state remains until arsenic reduction is energetically more favorable than iron reduction, and (2) the release of As during the second month is due to its reduction to the more weakly adsorbed As(III) which cannot compete against carbonate ions for sorption onto ferrihydrite. The model was also successfully applied to recent experimental results on the release of arsenic from Bengal delta sediments.  相似文献   

17.
The mobility of subsurface arsenic is controlled by sorption, precipitation, and dissolution processes that are tied directly to coupled redox reactions with more abundant, but spatially and temporally variable, iron and sulfur species. Adjacent to the site of a former pesticide manufacturing facility near San Francisco Bay (California, USA), soil and groundwater arsenic concentrations are elevated in sediments near the prior source, but decrease to background levels downgradient where shallow groundwater mixes with infiltrating tidal waters at the plume periphery, which has not migrated appreciably in over two decades of monitoring. We used synchrotron X-ray absorption spectroscopy, together with supporting characterizations and sequential chemical extractions, to directly determine the oxidation state of arsenic and iron as a function of depth in sediments from cores recovered from the unsaturated and saturated zones of a shallow aquifer (to 3.5 m below the surface). Arsenic oxidation state and local bonding in sediments, as As-sulfide, As(III)-oxide, or As(V)-oxide, were related to lithologic redox horizons and depth to groundwater. Based on arsenic and iron speciation, three subsurface zones were identified: (i) a shallow reduced zone in which sulfide phases were found in either the arsenic spectra (realgar-like or orpiment-like local structure), the iron spectra (presence of pyrite), or both, with and without As(III) or As(V) coordinated by oxygen; (ii) a middle transitional zone with mixed arsenic oxidation states (As(III)–O and As(V)–O) but no evidence for sulfide phases in either the arsenic or iron spectra; and (iii) a lower oxidized zone in the saturated freshwater aquifer in which sediments contained only oxidized As(V) and Fe(III) in labile (non-detrital) phases. The zone of transition between the presence and absence of sulfide phases corresponded to the approximate seasonal fluctuation in water level associated with shallow groundwater in the sand-dominated, lower oxic zone. Total sediment arsenic concentrations showed a minimum in the transition zone and an increase in the oxic zone, particularly in core samples nearest the former source. Equilibrium and reaction progress modeling of aqueous-sediment reactions in response to decreasing oxidation potential were used to illustrate the dynamics of arsenic uptake and release in the shallow subsurface. Arsenic attenuation was controlled by two mechanisms, precipitation as sulfide phases under sulfate-reducing conditions in the unsaturated zone, and adsorption of oxidized arsenic to iron hydroxide phases under oxidizing conditions in saturated groundwaters. This study demonstrates that both realgar-type and orpiment-type phases can form in sulfate-reducing sediments at ambient temperatures, with realgar predicted as the thermodynamically stable phase in the presence of pyrite and As(III) under more reduced conditions than orpiment. Field and modeling results indicate that the potential for release of arsenite to solution is maximized in the transition between sulfate-reduced and iron-oxidized conditions when concentrations of labile iron are low relative to arsenic, pH-controlled arsenic sorption is the primary attenuation mechanism, and mixed Fe(II,III)-oxide phases do not form and generate new sorption sites.  相似文献   

18.
The knowledge of mineralogy and molecular structure of As is needed to better understand the stability of As in wastes resulting from processing of gold ores. In this study, optical microscopy, scanning electron microscopy, electron microprobe, X-ray diffraction and X-ray absorption fine structure (XAFS) spectroscopy (including both XANES and EXAFS regimes) were employed to determine the mineralogical composition and local coordination environment of As in gold ores and process tailings from bench-scale tests designed to mimic a common plant practice. Arsenic-bearing minerals identified in the ores and tailings include iron (III) oxyhydroxides, scorodite (FeAsO4·2H2O), ferric arsenates, arseniosiderite (Ca2Fe3(AsO4)3O2·3H2O), Ca-Fe arsenates, pharmacosiderite (KFe4(AsO4)3(OH)4·6-7H2O), jarosite (K2Fe6(SO4)4(OH)12) and arsenopyrite (FeAsS). Iron (III) oxyhydroxides contain variable levels of As from trace to about 22 wt% and Ca up to approximately 9 wt%.Finely ground ore and tailings samples were examined by bulk XAFS and selected mineral grains were analyzed by microfocused XAFS (micro-EXAFS) spectroscopy to reconcile the ambiguities of multiple As sources in the complex bulk EXAFS spectra. XANES spectra indicated that As occurs as As5+in all the samples. Micro-EXAFS spectra of individual iron (III) oxyhydroxide grains with varying As concentrations point to inner-sphere bidentate-binuclear arsenate complexes as the predominant form of As. There are indications for the presence of a second Fe shell corresponding to bidentate-mononuclear arrangement. Iron (III) oxyhydroxides with high As concentrations corresponding to maximum adsorption densities probably occur as nanoparticles. The discovery of Ca atoms around As in iron (III) oxyhydroxides at interatomic distances of 4.14-4.17 Å and the coordination numbers suggest the formation of arseniosiderite-like nanoclusters by coprecipitation rather than simple adsorption of Ca onto iron (III) oxyhydroxides. Correlation of Ca with As in iron (III) oxyhydroxides as determined by electron microprobe analysis supports the coprecipitate origin for the presence of Ca in iron (III) oxyhydroxides.The samples containing higher abundances of ferric arsenates released higher As concentrations during the cyanidation tests. The presence of highly soluble ferric arsenates and Ca-Fe arsenates, and relatively unstable iron (III) oxyhydroxides with Fe/As molar ratios of less than 4 in the ore and process tailings suggests that not only the tailings in the impoundment will continue to release As, but also there is the potential for mobilization of As from the natural sources such as the unmined ore.  相似文献   

19.
Unplanned exploitation of groundwater constitutes emerging water-related threats to MayoTsanaga River Basin. Shallow groundwater from crystalline and detrital sediment aquifers, together with rain, dams, springs, and rivers were chemically and isotopically investigated to appraise its evolution, recharge source and mechanisms, flow direction, and age which were used to evaluate the groundwater susceptibility to contamination and the basin’s stage of salinization. The groundwater which is Ca–Na–HCO3 type is a chemically evolved equivalent of surface waters and rain water with Ca–Mg–Cl–SO4 chemistry. The monsoon rain recharged the groundwater preferentially at an average rate of 74 mm/year, while surface waters recharge upon evaporation. Altitude effect of rain and springs show a similar variation of −0.4‰ for δ18O/100 m, but the springs which were recharged at 452, 679, and 773 m asl show enrichment of δ18O through evaporation by 0.8‰ corresponding to 3% of water loss during recharge. The groundwater which shows both local and regional flow regimes gets older towards the basins` margin with coeval enrichment in F− and depletion in NO3 −. Incidentally, younger groundwaters are susceptible to anthropogenic contamination and older groundwaters are sinks of lithologenic fluoride. The basins salinization is still at an early stage.  相似文献   

20.
Shallow marine sediments of the Buyat-Ratototok district of North Sulawesi, Indonesia, are affected by submarine disposal of industrial gold mine tailings and small-scale gold mining using mercury amalgamation. Industrial mine tailings contained 590–660 ppm arsenic, 490–580 ppm antimony, and 0.8–5.8 ppm mercury. Electron microprobe survey found both colloidal iron–arsenic-phases without sulphur and arsenian pyrite in tailings and sites to which tailings had dispersed, but only arsenopyrite in sediments affected by artisanal mining. Antimony in tailings was present as antimony oxides, colloidal iron–antimony phases, colloidal iron–antimony phases, and stibnite in sediments affected by both types of mining. A sequential extraction found that 2% of arsenic held in tailings and tailings-contaminated sediments was exchangeable, 20–30% was labile, including weakly adsorbed, carbonate- and arsenate bound, 20–30% was metastable, probably incorporated into iron or manganese oxyhydroxides, or strongly adsorbed to silicate minerals, and 40–48% was relatively insoluble, probably incorporated into sulphides or silicates. Arsenic in sediments affected by artisanal gold mining was 75–95% relatively insoluble. Antimony in all sediments was >90% relatively insoluble. Relative solubility patterns of most other metals did not differ between industrial tailings-affected, artisanal-mining affected areas, and fluvial sediments. Results suggest that submarine tailings disposal is not suitable for refractory Carlin-like gold deposits because ore processing converts arsenic to forms unstable in anoxic marine sediments. Electronic supplementary material Supplementary material is available in the online version of this article at and is accessible for authorized users.  相似文献   

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