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1.
We have determined the extent of Se isotope fractionation induced by reduction of selenate by sulfate interlayered green rust (GRSO4), a Fe(II)-Fe(III) hydroxide-sulfate. This compound is known to reduce selenate to Se(0), and it is the only naturally relevant abiotic selenate reduction pathway documented to date. Se reduction reactions, when they occur in nature, greatly reduce Se mobility and bioavailability. Se stable isotope analysis shows promise as an indicator of Se reduction, and Se isotope fractionation by various Se reactions must be known in order to refine this tool. We measured the increase in the 80Se/76Se ratio of dissolved selenate as lighter isotopes were preferentially consumed during reduction by GRSO4. Six different experiments that used GRSO4 made by two methods, with varying solution compositions and pH, yielded identical isotopic fractionations. Regression of all the data yielded an instantaneous isotope fractionation of 7.36 ± 0.24‰. Selenate reduction by GRSO4 induces much greater isotopic fractionation than does bacterial selenate reduction. If selenate reduction by GRSO4 occurs in nature, it may be identifiable on the basis of its relatively large isotopic fractionation.  相似文献   

2.
The well-defined and intensively studied episode of Se contamination at Kesterson Reservoir (Merced County, California, U.S.A.) provided a unique opportunity to describe the distribution, speciation and geochemical transformations of Se in a variety of geochemical and ecological settings, ranging from permanent ponds to semi-arid grasslands and salt flats. Kesterson Reservoir comprises 500 ha of land contaminated with Se from agricultural drain water. In most places. Se was concentrated in surficial organic detritus and the surficial decimeter of mineral soil. At dry sites, selenate ion predominated below 20 cm depth. Elemental selenium (Se0) also was prominent. The amount of zero-valent Se increased slowly with time. Although selenate is thermodynamically stable in the vadose zone in the presence of oxygen, Se0 is an additional, metastable product of the mineralization of organic selenium. Thiols and inorganic sulfides dramatically increase the solubility of Se0. Decreasing pH inhibits the reaction, explaining the observed decrease in solubility and biological availability of Se in soil and aquatic systems at low pH. Adding thiols or methionine to soil increases the emission of volatile Se compounds several-fold, suggesting that thiols play a major role in the microbial cycling of Se in soil.  相似文献   

3.
The possible contamination of a groundwater system with industrial wastewater originating from a paper mill factory has been investigated in Piteå, N. Sweden. Six samples were collected from the wastewater in the waste dump and twelve samples from the adjacent groundwater were analyzed for chemistry and sulfur isotopes. The industrial wastewater is a saline water consisting mainly of Na–HCO3–SO4, having a high pH and showing δ34S values between 7‰ and 9‰ affected by bacterial sulfate reduction. The groundwaters are relatively dilute, dominated by Na+, Ca2+ and HCO3−, but with varying concentrations as exemplified by sulfate with concentrations varying between 3 and 69 mg L− 1 while the δ34S values range from − 0.5‰ to 14.3‰. The data suggest that the main S sources in the waters are the bedrock sulfides and/or atmospheric deposition, which, sometimes, are overlapped by bacterial sulfate reduction. Contamination from the waste dump does not occur.  相似文献   

4.
Variations in the carbon isotopic composition (δ13C) of pristane, phytane, n-heptadecane (n-C17), C29 ααα 20R sterane, and aryl isoprenoids provide evidence for a diverse community of algal and bacterial organisms in organic matter of the Upper Ordovician Maquoketa Group of the Illinois Basin. Carbon isotopic compositions of pristane and phytane from the Maquoketa are positively covariant (r = 0.964), suggesting that these compounds were derived from a common source inferred to be primary producers (algae) from the oxygenated photic zone. A variation of 3‰ in δ13C values (−31 to −34‰) for pristane and phytane indicates that primary producers utilized variable sources of inorganic carbon. Average isotopic compositions of n-C17 (−32‰) and C29 ααα 20R sterane (−31‰) are enriched in 13C relative to pristane and phytane (−33‰) suggesting that these compounds were derived from a subordinate group of primary producers, most likely eukaryotic algae. In addition, a substantial enrichment of 13C in aryl isoprenoids (−14 to −18‰) and the identification of tetramethylbenzene in pyrolytic products of Maquoketa kerogen indicate a contribution from photosynthetic green sulfur bacteria to the organic matter. The presence of anaerobic, photosynthetic green sulfur bacteria in organic matter of the Maquoketa indicates that anoxic conditions extended into the photic zone.The δ13C of n-alkanes and the identification of an unusual suite of straight-chain n-alkylarenes in the m/z 133 fragmentograms of Ordovician rocks rich in Gloeocapsomorpha prisca (G. prisca) indicate that G. prisca did not contribute to the organic matter of the Maquoketa Group.  相似文献   

5.
The oxygen (δ18Oc) and carbon (δ13Cc) isotope compositions of the structural carbonate group (CO3) in apatites from lateritic profiles were investigated. The weathering profiles, located in southern Brazil and in western Senegal, are developed on three different types of apatite-rich parent rock: carbonatite, metamorphosed marine phosphorite and sedimentary marine phosphorite. The parent rock apatites are of magmatic, hydrothermal, metamorphic and sedimentary origins. The in situ formation of apatite of weathering origin in the profiles is well documented petrographically and geochemically.The overall range of measured δ18Oc and δ13Cc values of apatites of weathering origin (22 to 27 SMOW for δ18Oc and −15 to −10 PDB for δ13Cc) is much smaller than the range of measured and/or published isotope compositions of parent rock apatites (4–35 for δ18Oc and −11 to +1 for δ13Cc). In any profile, the apatites of weathering origin can exhibit lower, similar or higher δ18Oc values than parent rock apatites. In contrast, their δ13Cc values are systematically and significantly lower than those of the parent rock apatites. Apatites formed as a result of weathering in laterites can therefore be readily distinguished from apatites of other origin on the basis of their isotope composition.Assuming that apatite CO3 fractionates O in a way similar to calcite CO3, the structural carbonate group of the apatites of weathering origin appears to form in approximate isotopic equilibrium with the weathering solutions. The very low δ13Cc values exhibited by these apatites indicate that the dominant sources of dissolved CO2 in the soil water are organic. The isotope composition of structural carbonate in apatite of weathering origin in lateritic profiles may provide useful information for paleoenvironmental studies.  相似文献   

6.
Origins of high nitrate in groundwater in Tanzania   总被引：3，自引：0，他引：3  
Dodoma is located in a semi-arid climate (mean annual rainfall 550 mm) in an area of crystalline basement rock. The groundwater contains high nitrate with NO3− concentrations averaging 150 mg l−1 and total mineralization between 1000–3000 mg l−1. Factor analysis has been used for the identification of factors that bring about the chemical character of groundwater. Three rotated factors, explaining 77.2% of the total data variance, were extracted. The first factor accounts for 51.0% of the variance and shows high positive correlation with Na+, K+, Mg2+, Ca2+, Cl−, SO42−, HCO3− and SEC and is attributed to the leaching of surface and soil salts together with mineral dissolution. The second factor accounts for 14.1% of the variance and is positively correlated with NO3− and negatively correlated with pH; this is explained by the nitrification process taking place on the sewage effluents. The third factor is highly positively correlated with 18O and 2H, accounting for 12.1% of the variance and is a consequence of evaporation processes. Nitrate concentrations greater than 100 mg l−1 are commonly found in both deep and shallow groundwaters. It is concluded that the high nitrate concentrations have originated from the sewage effluents that are advecting and dispersing through macropores under bypass flow mechanisms.  相似文献   

7.
Salts produced using brines of the Mamfe Basin were analysed by XRD for their mineral composition and ICP-MS for minor element composition. Halite (NaCl) and dolomite (CaMg (CO3)2) constitute the major minerals with minor impurities from Mo and Cd in the chlorides and Sc and Cu in the carbonates. The mineral composition is evidence of dissolution of evaporites with parent brine of marine origin. Other elements analysed are suggested to be adsorbed to these salts and result from water–rock interaction. The elements partitioned based on their correlation to other elements are suggested to derive from sulphates including barite for Ba, sulphides for Pb, Zn, silicates for Zr, Mn and oxides for V, Cr. The electrical conductance of the brines is related to the salt yield by the equation; M = 9 × 10− 4E− 3.27, and it can be used to estimate salt yield throughout the year. Over 1200 tons of salt consisting dominantly of grade I halite are lost annually as brines across the basin. Purification is required for some minor elements including Ba, Pb, Hg and Cd for use as a condiment. A genetic relation between the parent brine, sulphide minerals and organic matter-rich sediments is proposed.  相似文献   

8.
On the south-eastern edge of Russia, the chemical composition of rainwater is controlled by sea salts, terrestrial material, as well as volcanic (Kuril islands volcanic area) and anthropogenic emissions, mostly in the southern part of the area. The predominant major ions of the Primorye, Sakhalin and the Kuril Islands rainwaters were respectively HCO3−–SO42−, Ca–Na, and of Cl–Na. Concentration of trace elements changes within 1–2 orders of magnitude but some difference in the distribution of the elements between continental and island rainwater is found. The concentration of the chemical elements in the particulate fraction varies from < 10% to 90% of the total concentration (dissolved + particulate) with the following distribution: Tl, Na, Ca, Sr, Zn, Cd (< 10%)–Be, Th, Bi, Rb, U, K, Sc (10–20%)–Cu, Mn, Mg, Mo, Se, Ba, Ni, As, Ag, Cs, Co, Y, Ga, V (20–50%)–Sb, Pb, Ge, Cr, Fe, Al (50–90%).The concentration of elements of the particulate fraction of the rainwater usually is significantly different from concentrations in the crust, including both higher and lower concentrations. The terrestrial contribution to dissolved elements was evaluated and follows the decreasing order: Fe > K, Mg, Ca > Ba, Sr > Na (65–1%). Close order was found for total (dissolved and solid) concentrations. Sea salt contribution to dissolved element concentration in the rainwater decrease in the following order: Cl, Mg > K, SO4 > Ca > HCO3−, Ba, Fe (78–0.1%). Calculation of anthropogenic and volcanic inputs for two ions (Cl− and SO42−) shows that anthropogenic inputs for the Vladivostok and Yuzno-Sakhalinsk cities can be evaluated as 15–20% of Cl− and up to 80–90% of SO42−. Volcanic components in the Kuril Islands, where anthropogenic inputs are absent, can reach up to 76% of SO42− and 36% of Cl−.  相似文献   

9.
High groundwater As concentrations in oxidizing systems are generally associated with As adsorption onto hydrous metal (Al, Fe or Mn) oxides and mobilization with increased pH. The objective of this study was to evaluate the distribution, sources and mobilization mechanisms of As in the Southern High Plains (SHP) aquifer, Texas, relative to those in other semiarid, oxidizing systems. Elevated groundwater As levels are widespread in the southern part of the SHP (SHP-S) aquifer, with 47% of wells exceeding the current EPA maximum contaminant level (MCL) of 10 μg/L (range 0.3–164 μg/L), whereas As levels are much lower in the north (SHP-N: 9%  As MCL of 10 μg/L; range 0.2–43 μg/L). The sharp contrast in As levels between the north and south coincides with a change in total dissolved solids (TDS) from 395 mg/L (median north) to 885 mg/L (median south). Arsenic is present as arsenate (As V) in this oxidizing system and is correlated with groundwater TDS (Spearman’s ρ = 0.57). The most likely current source of As is sorbed As onto hydrous metal oxides based on correlations between As and other oxyanion-forming elements (V, ρ = 0.88; Se, ρ = 0.54; B, ρ = 0.51 and Mo, ρ = 0.46). This source is similar to that in other oxidizing systems and constitutes a secondary source; the most likely primary source being volcanic ashes in the SHP aquifer or original source rocks in the Rockies, based on co-occurrence of As and F (ρ = 0.56), oxyanion-forming elements and SiO2 (ρ = 0.41), which are found in volcanic ashes. High groundwater As concentrations in some semiarid oxidizing systems are related to high evaporation. Although correlation of As with TDS in the SHP aquifer may suggest evaporative concentration, unenriched stable isotopes (δ2H: −65 to −27; δ18O: −9.1 to −4.2) in the SHP aquifer do not support evaporation. High TDS in the SHP aquifer is most likely related to upward movement of saline water from the underlying Triassic Dockum aquifer. Mobilization of As in other semiarid oxidizing systems is caused by increased pH; however, pH in the SHP aquifer is near neutral (10–90 percentiles, 7.0–7.6). Although many processes, such as competitive desorption with SiO2, VO4, or PO4, could be responsible for local mobilization of As in the SHP aquifer, the most plausible explanation for the regional As distribution and correlation with TDS is the counterion effect caused by a change from Ca- to Na-rich, water as shown by the high correlation between As and Na/(Ca)0.5 ratios (ρ = 0.57). This change in chemistry is related to mixing with saline water that moves upward from the underlying Dockum aquifer. This counterion effect may mobilize other anions and oxyanion-forming elements that are correlated with As (F, V, Se, B, Mo and SiO2). Competition among the oxyanions for sorption sites may enhance As mobilization. The SHP case study has similar As sources to those of other semiarid, oxidizing systems (original volcanic ash source followed by sorption onto hydrous metal oxides) but contrasts with these systems by showing lack of evaporative concentration and pH mobilization of As but counterion mobilization of As instead in the SHP-S aquifer.  相似文献   

10.
Sulfur and carbon contents and isotope ratios are reported for five Archean iron-formations, Helen, Nakina and Finlayson, Lumby and Bending Lake areas, distributed across 850 km of the Canadian shield all 2.7 Ga-old.A δ34S profile through a complete stratigraphic column (oxide facies excluded) of the Helen iron-formation shows a δ34S range of 30.2‰, mean δ34S value of 2.5‰ and a standard deviation (δi) of 7.3‰ In sharp contrast to the sulfide and siderite facies, the oxide facies in the column shows a uniform δ34S value close to zero. The δ34S values obtained for the other four iron-formations are again wide ranging, highly variable in the sulfide and pyrite—siderite facies, but uniform and close to zero for the oxide facies.The carbon in the oxide, siderite, chert facies has δ13C values of +2.3 to −1.1‰ in the range of Phanerozoic marine carbonates. However, the carbonates in the graphite rich sulfide facies have δ13C values as low as −7.6‰. The mixing of reduced carbon with marine carbonate is suggested to explain the light carbonate values. The reduced carbon associated with the light carbonate is also relatively light at up to δ13Corg = 33.5‰, but is in the range of other Precambrian values. Distal, high temperature, abiogenic sulfate reduction as a source of highly fractionated sulfides in the Archean iron-formations is ruled out on the basis of both isotopic and geologic evidence. It is concluded that only the bacterial reduction of sulfate at low temperatures could produce the wide ranging, highly variable δ34S values exhibited by these sulfides over large areas.  相似文献   

11.
Located in semi-arid regions of northwestern China, Datong basin is a Quaternary sedimentary basin, where groundwater is the most important source for water supply. It is very important to study groundwater characteristics and hydrogeochemical processes for better management of the groundwater resource. We have identified five geochemical zones of shallow groundwater (between 5 and 80 m) at Datong: A. Leaching Zone (Zone I); B. Converging Zone (Zone II); C. Enriching Zone (Zone III); D. Reducing Zone (Zone IV); E. Oxidizing Zone (Zone V). In Zones I, II, and V and some parts of Zones III and IV, hydrolysis of albite/K-feldspar/chalcedony system and/or albite/K-feldspar/quartz system enhanced concentrations of Na+, K+, HCO3− and silicate. In Zone I, dissolution of carbonate and hydrolysis of feldspar generally controlled the groundwater chemistry. Infiltration of meteoric water promoted the formation of HCO3− in the water. In Zone II, the main geochemical processes influencing the groundwater chemistry were dissolutions of calcite and dolomite, ion exchange and evaporation. In Zones III and IV, in addition to ion exchange, evaporation and precipitation of calcite and dolomite, leaching of NaHCO3 in saline–alkaline soils dominated the water quality. Zone IV was under anoxic condition, and reduction reactions led to the decrease of SO42−, NO3− and occurrence of H2S, with the highest arsenic content (mean value of 366 μg/L), far exceeding Maximum Contaminant Level (MCL). Abnormal arsenic in the groundwater resulted in endemic disease of waterborne arsenic poisoning among local people. Zone V overlapped Zone I was intensively affected by coal mining activities. Sulfide minerals, such as pyrite, would have been oxidized when exposed to air due to coal mining, which directly added sulfate to groundwater and thus increased SO42− concentration. Oxidization of sulfide minerals also decreased pH and promoted dissolutions of calcite and dolomite.  相似文献   

12.
A reversal of the conventional carbon isotope relationship, “terrestrial-lighter-than-marine” organic matter, has been documented for two Pennsylvanian (Desmoinesian) cyclothemic sequence cores from the Midcontinent craton of the central United States. “Deep” water organic-rich phosphatic black shales contain a significant proportion of algal-derived marine organic matter (as indicated by organic petrography, Rock-Eval hydrogen index and ratios) and display the lightest δ13C-values (max −27.80‰ for kerogen) while shallower water, more oxic facies (e.g. fossiliferous shales and limestones) contain dominantly terrestrial organic matter and have heavier δ13Ckerogen-values (to −22.87‰ for a stratigraphically adjacent coal). δ13C-values for extract fractions were relatively homogeneous for the organic-rich black shales with the lightest fraction (often the aromatics) being only 1‰, or less, more negative than the kerogen. Differences between extract fractions and kerogens were much greater for oxic facies and coals (e.g. saturates nearly 5‰ lighter than the kerogen).A proposed depositional model for the black shales calls upon a large influx of nutrients and humic detritus to the marine environment from the laterally adjacent, extremely widespread Pennsylvanian (peat) swamps which were rapidly submerged by transgression of the epicontinental seas. In this setting marine organisms drew upon a CO2-reservoir which was in a state of disequilibrium with the atmosphere, being affected by isotopically light “recycled-CO2” derived from the decomposition of peaty material in the water column and possibly from the anoxic diagenesis of organic matter in the sediments.  相似文献   

13.
Yongliang Xiong   《Ore Geology Reviews》2003,23(3-4):259-276
In this study, an attempt has been made to assess aqueous speciation of selenium and solubility product constants of common selenides at elevated temperatures (up to 300 °C) by using various extrapolation methods. This study predicts that reduced selenium species are dominant species in many geological processes even under relatively oxidized conditions such as those dictated by the magnetite–hematite buffer. On the basis of extrapolated equilibrium constants and solubility product constants for common Se-bearing mineral phases, critical ∑Se/∑S ratios (molal ratios) in mineralizing fluids are proposed for independent selenium mineralization. The minimum ∑Se/∑S ratios in mineralizing fluids for independent selenium mineralization should be at least 10−6, 10−5 and 10−4 at 100, 200 and 300 °C, respectively. For giant independent selenium deposits such as the La'erma and Qiongmo Au–Se deposits in the western Qingling mountains, and Yutangba Se deposits in Hubei Province, China, the mineralizing fluids have reached much higher ∑Se/∑S ratios ranging from 10−1 to 10−3 at 200 °C. This study also suggests that the equilibrium assemblage of pyrite–ferroselite among the common ore minerals requires the highest ∑Se/∑S ratios in mineralizing fluids, followed in decreasing order by the assemblages of stibnite–antimonselite, galena–clausthalite, cinnabar–tiemannite, and acanthite/argentite–naumannite. The assemblage of pyrite–ferroselite can also be formed under relatively oxidizing conditions where [∑H2Se]/[∑H2S] ratios can be high enough for the formation of independent ferroselite.  相似文献   

14.
Heterogeneous shallow Plio-Quaternary formations of the Souss Plain represent the most important aquifer in southern High Atlas Mountains in Morocco. The present work was conducted in the Souss Upstream Basin to identify the chemical characteristics and the origin of groundwater in an aquifer under semi-arid climate. Isotopic and hydrochemical compositions combined with geological and hydrogeological data were used for this purpose. The total dissolved solids vary from 239 to 997 mg l−1, and the following groundwater types are recognized: Ca2+–Mg2+–HCO3−, Ca2+–Mg2+–SO42− and Ca2+–Mg2+–Cl−. The groundwater is saturated and slightly supersaturated with respect to carbonate minerals and undersaturated with respect to evaporite minerals, which means that the groundwater composition is largely controlled by the dissolution of carbonate rocks known in the basin. The isotopic contents of groundwaters ranged from −8‰ to −5.2‰ for δ18O, from −52‰ to −34‰ for δD, and from 0 to 5.5 TU for tritium. The hydrogen (δD) and oxygen (δ18O) isotope signatures reveal a significant infiltration before evaporation takes place, indicating a major recharge directly from fractures in the crystalline and limestone formations of Atlas Mountains (above 800 m a.s.l.) and infiltration of surface water in the alluvial cones at the border of the Atlas basins. The very low tritium values suggest that the groundwater recharge follows a long flow path and a mixing between old and modern water is shown. However, a slight evaporation effect is noted in the southern part of the basin close to the Anti-Atlas Mountains.  相似文献   

15.
The Mapocho river, which crosses downtown Santiago, is one of the most important rivers in contact with a population of about six million inhabitants. Anthropogenic activities, industrialization, farming activities, transport, urbanization, animal and human excretions, domestic wastes and copper mining have affected the river, contaminating it and its sediments with heavy metals. Concentration and distribution of Cu, Zn, Pb and Cd were studied with the purpose of determining their bioavailability and their relation with the characteristics of the sediments. Freshly deposited seasonal sediments were collected from 0–8 cm depths from 6 locations (S1 to S6) along the 30-km long channel length, in the four seasons of year on the following dates: May 2001 (D1, autumn); August 2001 (D2, winter); October 2001 (D3, spring) and January 2002 (D4, summer). The dried samples were sifted to obtain the < 63-μm sediment fraction, since it has been shown that large amounts of heavy metals are bound in the fine-grained fraction of the sediment. Cu and Zn were analyzed by atomic absorption spectrophotometry and Pb and Cd by square wave anodic stripping voltammetry. The highest concentrations of Cu (2850 μg g− 1) were found in the northern part of the river (S1, average D1–D4), near the mountains and a copper mine, and then decreased downstream to 209 μg g− 1 (S6). Total Zn showed an irregular variation, with higher values at S1 (1290 μg g− 1) and high values in some winter sampling (1384 μg g− 1 S4, S5–D2). Pb showed different trends, increasing from S1 to S6 (17 to 61 μg g− 1), with the highest values in the summer samples (83 μg g− 1, S4–S6, D4), and total Cd increased slightly from mean values of 0.2 and 0.5 μg g− 1. Partition into five fractions was made using Tessier's analytical sequential extraction technique; the residue was treated with aqua regia for recovery studies, although this step is not part of the Tessier procedure. The results show that Cu, Zn and Pb in the sediments were dependent on the sampling places along the river, and variation in two years was low (D1–D4). The highest values of total organic matter, carbonate and conductivity were found in S6, which has the smallest size particles, while at S1 the sediments were predominantly sand and contain larger amounts of silica. Cu associated with carbonate decreased gradually from 58% (1771 μg g− 1, S1) to 16% (32 μg g− 1, S6); Cu bonded to reducible fraction was almost constant (33% to 37%), and Cu associated with oxidizable fraction increased from 7% (S1) to 34% (S6), but copper content was lower (214 to 68 μg g− 1). Zn had a similar fractionation profile. However, Pb bound to oxidizable fraction did not show significant percent variation along the river (20% to 19%), but the amount bounded was 4 to 12 μg g− 1. The residual fraction increased from 24% to 41% (5 to 25 μg g− 1, S1 to S6). The distribution of Cd in the sediment was almost independent of the sampling stations and was bound to carbonate, reducible and residual fraction in similar proportion. Cu and Zn at S1 were mainly bound to carbonates and reducible phases with 91% and 73% (2779 and 965 μg g− 1, respectively), and with a change in the pH and/or the redox potential of the sediment–water system, these contaminants could easily enter the food chain. In S6 the amount of Cu and Zn in these phases was 50% and 53% (100 to 313 μg g− 1, respectively).  相似文献   

16.
Literature data on the thermodynamics of complexation of Zr with inorganic species, at 25°C, have been critically reviewed. The preponderance of published complexation constants deal with F− and OH− ions. Stability constants for the complexation reactions are relatively independent of ionic strength and thus recomended values for each ligand type are averages of the most reliable data. Complexation constants under elevated conditions (T 250°C andPv = PH2O) have been predicted for various Zr complexes (F−, Cl−, SO42− and OH−) using Helgeson's electrostatic approach. Predominance diagrams (calculated for simple systems with these constants) suggest that, over a wide range of pH conditions, Zr(OH)4(aq) will dominate the aqueous geochemistry of Zr except under very high activities of competing ligands (e.g., F−, SO42−).The solubilities of vlasovite [Na2ZrSi4O11] and weloganite [Sr3Na2Zr(CO3)6·3H2O have been measured in KCI solutions (0.5–1.0 M) at 50°C. Weloganite dissolution is complicated by the predictable precipitation of strontianite (SrCO3) whereas vlasovite dissolves incongruently. Solubility products for the dissolution of welonganite and vlasovite are determined to be −28.96±0.14 and −20.40±1.18, respectively. Concentrations of Zr up to 10−3 m were present in the experimental solutions; the presence of large amounts of Zr in aqueous solutions support the possibility of extensive remobilization of Zr during hydrothermal mineralization.  相似文献   

17.
The wetland constructed at the Big Five Tunnel in Idaho Springs, Colorado was designed to remove, passively, heavy metals from acid mine drainage. In optimizing the design of such a wetland, an improved understanding of the chemical processes operating there was required, particularly SO42− reduction and sulfide precipitation. For this purpose, field and laboratory data were collected to study the balance of S in the system. Field data collected included water analyses of the mine drainage and wetland effluents and measurements of H2S gas emissions from the wetland. The concentration of sulfide in the wetland effluent ranged from 10−4 to 10−3 mol/l. The average rates of H2S emission from the surface of the substrate were 150 nmol/cm2/d in the summer and 0.17 and 0.35 nmol/cm2/d in the winter. This maximum estimated loss of sulfide was not significant in reducing the amount of sulfide available for precipitation with metals. Sequential extraction experiments for S on wetland substrates showed that acid volatile sulfides (AVS) increased with time in the wetland substrate. A serum bottle experiment was conducted to study the S balance in the Big Five wetland by quantitatively measuring the amount of S in different phases as microbial SO42− reduction progressed. The increase in AVS reasonably balanced the decrease in SO42− concentration in the experiment, suggesting that the decrease in SO42− concentration represented the amount of SO42− reduced and that nearly all of the sulfide produced was precipitated as AVS. Sulfide precipitation was determined to be the primary metal removal process in the wetland system and amorphous FeS is the primary iron sulfide formed in the substrate.  相似文献   

18.
Thiosulphate is present in hot springs, streams and thermal pools of the Taupo Volcanic Zone and Ngawha, New Zealand, at concentrations of 1.2 (±1.3) × 10−5 M to 7.05 (±0.12) × 10−4M. Formed as a metastable product of sulphide oxidation, thiosulphate is buffered in the presence of elemental S according to, . Unless all sulphide present has been bacterially oxidised to sulphate, a steady state concentration of thiosulphate is maintained. As a soft base thiosulphate is capable of complexing several transition metals. The thermodynamically predicted speciation of Ag in Champagne Pool, for example, indicates a Ag(S2O3)2−3 activity similar to that of AgCl2− though less than that of Ag(HS)2−.  相似文献   

19.
This study deals with the experimental determination of the rate of weathering and As release from Au-bearing sulfide ores of the Mokrsko-West deposit (Czech Republic). The elevated As contents in the ore and the possible As mobilisation must be taken into account due to the close proximity of the deposit to the Vltava River, a source of drinking water for Prague. Crushed and homogenized ore material was divided into four grain-size fractions showing uniform chemical and mineralogical composition and subjected to batch and column leaching experiments. The most important reactions controlling metal leaching include (i) oxidation of sulfides, (ii) carbonate equilibrium and (iii) precipitation of hydrated ferric oxides (HFO). Hydrated ferric oxides were found to be important sorbents of mobilized As. The highest concentration of As in the leachates was obtained from the 64–1000 μm fraction. The oxidation rate in the agitated batch experiment calculated on the basis of sulfate concentrations is an order of magnitude higher (3.8×10−9 to 4.4×10−8 mol SO42− h−1 g−1) than in the static column experiment (9.6×10−10 to 7.4×10−9 mol SO42− h−1 g−1). The higher oxidation rate of batch experiments is explained by abrasion of oxidation products (mainly HFO) and by further exposition of reaction surfaces of the sulfide grains.  相似文献   

20.
Several methods were evaluated and compared for the estimation of pyrite oxidation rates (POR) in waste rock at Mine Doyon, Quebec, Canada. Methods based on data collected in situ, such as the interpretation of temperature and oxygen concentration profiles (TOP) measured in the waste rock pile and pyrite mass balance (PMB) on solid phase samples were compared with the oxygen consumption measurements (OCM) in closed chamber in the laboratory. A 1-D analytical solution to a gas and heat transport equation used temperature and oxygen profiles (TOP) measured in the pile for the preliminary POR estimates at a site close to the slope of the pile (Site 6) and in the core of the pile (Site 7). Resulting POR values were 1.1 × 10− 9 mol(O2) kg− 1 s− 1 and 1.0 × 10− 10 mol(O2) kg− 1 s− 1 for the slope site and the core site, respectively. Oxidation rates based on pyrite mass balance (PMB) calculations for solid samples were 2.21 × 10− 9 mol(O2) kg− 1 s− 1 and 2.03 × 10− 9 mol(O2) kg− 1 s− 1, respectively, for the same slope and core sites, but the difference between sites was within the error margin. The OCM measurements in the laboratory on fresh waste rock samples yielded higher POR values than field methods, with average oxidation rate of 6.7 × 10− 8 mol(O2) kg− 1 s− 1. However, the OCM results on weathered and decomposed material from the rock stockpile (average oxidation rate 3.4 × 10− 9 mol(O2) kg− 1 s− 1) were consistent with results from the field-based estimates. When POR values based on fresh material are excluded, the remaining POR values for all methods range from 1.0 × 10− 10 to 3.4 × 10− 9 mol(O2) kg− 1 s− 1. The lowest estimated value (1.0 × 10− 10 mol(O2) kg− 1 s− 1) was based on TOP estimates in the interior of the pile where oxygen transport was limited by diffusion from the surface. These results suggest that small-scale OCM laboratory experiments may provide relatively representative values of POR in the zones of waste rock piles in which oxygen transport is not dominated by diffusion.  相似文献   

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