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1.
This paper discusses the selective depression of pyrite from chalcopyrite and arsenopyrite by biomodulation using Acidithiobacillus ferrooxidans under natural conditions of pH. The effect of bacteria–mineral interaction on the surface charge of mineral and bacterial cell was studied by microelectrophoresis. Adhesion experiments were conducted to establish the relationship between cell adhesion to specific minerals and the electrokinetic behaviour of the minerals subsequent to interaction with cells. Effect of bacterial interaction on the xanthate-induced flotation of all the minerals was assessed. Adhesion of A. ferrooxidans on pyrite was rapid and tenacious and subsequent to interaction with cells, pyrite remained hydrophilic even in presence of xanthate collector. The collector, on the other hand, was able to render good flotability to chalcopyrite even after interaction with bacterial cells. Copper activated arsenopyrite was able to retain its hydrophobicity in presence of cells due to poor attachment kinetics of cells to the mineral surface. Thus, by suitably conditioning with the cells and collector, it was possible to effectively depress pyrite from chalcopyrite and arsenopyrite.  相似文献   

2.
The role of pH and pulp redox potential (EH) to control the flotation and depression of arsenopyrite has been investigated through studies on microflotation of arsenopyrite crystals and batch flotation of an arsenopyritic ore using isopropyl xanthate as collector. The transition between flotation and depression of arsenopyrite is established by the reversible potential of the xanthate/dixanthogen couple. Adsorption of arsenate ions on ferric hydroxide has been studied through electrokinetics to delineate mechanisms involved in the depression of arsenopyrite using oxidants. Chemical binding between arsenate species and ferric hydroxide sites on arsenopyrite is suggested as the mechanism responsible for depression of arsenopyrite. EH conditions are given for the flotation and depression of arsenopyite at various pH values for the arsenopyritic ore.  相似文献   

3.
Arsenite sorption on troilite (FeS) and pyrite (FeS2)   总被引：4，自引：0，他引：4  
Arsenic is a toxic metalloid whose mobility and availability are largely controlled by sorption on sulfide minerals in anoxic environments. Accordingly, we investigated reactions of As(III) with iron sulfide (FeS) and pyrite (FeS2) as a function of total arsenic concentration, suspension density, sulfide concentration, pH, and ionic strength. Arsenite partitioned strongly on both FeS and FeS2 under a range of conditions and conformed to a Langmuir isotherm at low surface coverages; a calculated site density of near 2.6 and 3.7 sites/nm2 for FeS and FeS2, respectively, was obtained. Arsenite sorbed most strongly at elevated pH (>5 to 6). Although solution data suggested the formation of surface precipitates only at elevated solution concentrations, surface precipitates were identified using X-ray absorption spectroscopy (XAS) at all coverages. Sorbed As was coordinated to both sulfur [d(As-S) = 2.35 Å] and iron [d(As-Fe) = 2.40 Å], characteristic of As coordination in arsenopyrite (FeAsS). The absorption edge of sorbed As was also shifted relative to arsenite and orpiment (As2S3), revealing As(III) reduction and a complete change in As local structure. Arsenic reduction was accompanied by oxidation of both surface S and Fe(II); the FeAsS-like surface precipitate was also susceptible to oxidation, possibly influencing the stability of As sorbed to sulfide minerals in the environment. Sulfide additions inhibit sorption despite the formation of a sulfide phase, suggesting that precipitation of arsenic sulfide is not occurring. Surface precipitation of As on FeS and FeS2 supports the observed correlation of arsenic and pyrite and other iron sulfides in anoxic sediments.  相似文献   

4.
Arsenic(V), as the arsenate (AsO4 3?) ion and its conjugate acids, has a strong affinity on Fe, Mn, and Al (oxyhydr)oxides and clay minerals. Removal of arsenate from aqueous solution by poorly crystalline ferrihydrite (hydrous ferric oxide) via a combination of macroscopic (equilibria and kinetics of sorption) and X-ray absorption spectroscopic studies was investigated. The removal of arsenate significantly decreased with increasing pH and sorption maxima of approximately 1.994 mmol/g (0.192 molAs/molFe) were achieved at pH 2.0. The Langmuir isotherm is most appropriate for arsenate sorption over the wide range of pH, indicating that arsenate sorption preferentially takes place at relatively homogenous and monolayer sites rather than heterogeneous and multilayer surfaces. The kinetic study demonstrated that arsenate sorption onto 2-line ferrihydrite is considerably fast, and sorption equilibrium was achieved within the reaction time of 2 h. X-ray absorption near-edge structure spectroscopy indicates no change in oxidation state of arsenate following interaction with the ferrihydrite surfaces. Extended X-ray absorption fine structure spectroscopy supports the efficient removal of arsenate by the 2-line ferrihydrite through the formation of highly stable inner-sphere surface complexes, such as bidentate binuclear corner-sharing (2C) and bidentate mononuclear edge-sharing (2E) complexes.  相似文献   

5.
Bolar earths deposits from Mt Amiata (Central Italy) consist of nanosized pseudo-spherical goethite, with average crystal size of 10–15 nm (as determined by X-ray powder diffraction and transmission electron microscopy observations), possibly associated to amorphous silica and minor sheet silicates, quartz and feldspars. Chemical analyses revealed high As contents (up to 7.4 wt% As2O5), thus indicating the occurrence of a potentially dangerous contaminant. Arsenic doesn’t occur as a specific As phase, but it is strictly associated with goethite nanocrystals. Eh and pH measurements suggest that As occurs as arsenate anions (H2AsO4− and HAsO42−), which are easily and strongly adsorbed to goethite surfaces. The high specific surface area, resulting from goethite nanosize, and the absence of competitive anions explain the extremely efficient adsorption of arsenate and the anomalously high As content in bolar earths. Overall physical/chemical data suggest stable arsenate adsorption, with very limited risk for As release to the environment.  相似文献   

6.
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   

7.
An industrial area contaminated by As was studied to determine the source of this element and its speciation in As-bearing solids and in run-off waters. Mineral precipitates and water samples were collected and analyzed to assess processes controlling As mobility at this site. The integrated study of a contaminated industrial area allowed identification of the source of the As and of the nature of secondary As-bearing phases. The results obtained both on solid and water samples were used to model As behavior during waste leaching on carbonate rocks. At the upper end of a topographic transect across the site, run-off waters (pH=7.9) interact with surficial waste piles (containing arsenolite, arsenopyrite and pyrite), becoming acidic (pH=2.2) and concentrated in dissolved arsenate species (As5+) (ΣAs ranging from 0.961 to 3.149·10−3 mol/l). Those acidic waters interact with the limestone substratum, providing dissolved Ca which reacts with As to precipitate 1:1 Ca arsenates (weilite CaHAsO4, haidingerite CaHAsO4.H2O and pharmacolite CaHAsO4.2H2O) and, in minor amounts, Ca–Mg arsenates (picropharmacolite (Ca,Mg)3(AsO4)2 6H2O). The 1:1 Ca arsenates identified are known to precipitate at low pH (3–6) and seem to be stable in media with high dissolved CO2, in comparison with other types of Ca arsenates. However, due to their high solubilities, they are not strictly relevant candidates to immobilize As in contaminated surficial environments. Although reported solubilities decrease to values close to the French and US drinking standards in Ca-rich solutions, a thorough examination of the precipitation/dissolution kinetics of Ca arsenates should be undertaken to assess their long-term stability and their efficiency in rapidly immobilizing As in contaminated surficial environments.  相似文献   

8.
Karavansalija ore zone is situated in the Serbian part of the Serbo‐Macedonian magmatic and metallogenic belt. The Cu–Au mineralization is hosted mainly by garnet–pyroxene–epidote skarns and shifts to lesser presence towards the nearby quartz–epidotized rocks and the overlying volcanic tuffs. Within the epidosites the sulfide mineralogy is represented by disseminated cobalt‐nickel sulfides from the gersdorfite‐krutovite mineral series and cobaltite, and pyrite–marcasite–chalcopyrite–base metal aggregates. The skarn sulfide mineralization is characterized by chalcopyrite, pyrite, pyrrhotite, bismuth‐phases (bismuthinite and cosalite), arsenopyrite, gersdorffite, and sphalerite. The sulfides can be observed in several types of massive aggregates, depending on the predominant sulfide phases: pyrrhotite‐chalcopyrite aggregates with lesser amount of arsenopyrite and traces of sphalerite, arsenopyrite–bismuthinite–cosalite aggregates with subordinate sphalerite and sphalerite veins with bismuthinite, pyrite and arsenopyrite. In the overlying volcanoclastics, the studied sulfide mineralization is represented mainly by arsenopyrite aggregates with subordinate amounts of pyrite and chalcopyrite. Gold is present rarely as visible aggregate of native gold and also as invisible element included in arsenopyrite. The fluid inclusion microthermometry data suggest homogenization temperature in the range of roughly 150–400°C. Salinities vary in the ranges of 0.5–8.5 wt% NaCl eq for two‐phase low density fluid inclusions and 15–41 wt% NaCl eq for two‐phase high‐salinity and three‐phase high‐salinity fluid inclusions. The broad range of salinity values and the different types of fluid inclusions co‐existing in the same crystals suggest that at least two fluids with different salinities contributed to the formation of the Cu–Au mineralization. Geothermometry, based on EPMA data of arsenopyrite co‐existing with pyrite and pyrrhotite, suggests a temperature range of 240–360°C for the formation of the arsenopyrite, which overlaps well with the data for the formation temperature obtained through fluid inclusion microthermometry. The sulfur isotope data on arsenopyrite, chalcopyrite, pyrite and marcasite from the different sulfide assemblages (ranging from 0.4‰ to +3.9‰ δ34SCDT with average of 2.29 δ34SCDT and standard deviation of 1.34 δ34SCDT) indicates a magmatic source of sulfur for all of the investigated phases. The narrow range of the data points to a common source for all of the investigated sulfides, regardless of the host rock and the paragenesis. The sulfur isotope data shows good overlap with that from nearby base‐metal deposits; therefore the Cu–Au mineralization and the emblematic base‐metal sulfide mineralization from this metallogenic belt likely share same fluid source.  相似文献   

9.
Natural ferrihydrites (Fh) often contain impurities such as aluminum, especially in acid mine drainage, and these impurities can potentially impact the chemical reactivity of Fh with respect to metal (loid) adsorption. In the present study, we have investigated the influence of aluminum on the sorption properties of ferrihydrite with respect to environmentally relevant aqueous arsenic species, arsenite and arsenate. We have conducted sorption experiments by reacting aqueous As(III) and As(V) with synthetic Al-free and Al-bearing ferrihydrite at pH 6.5. Our results reveal that, when increasing the Al:Fe molar ratio in Fh, the sorption density dramatically decreased for As(III), whereas it increased for As(V). Extended X-ray Absorption Fine Structure (EXAFS) spectroscopy analysis at the As K-edge indicated that the AsIIIO3 pyramid binds to FeO6 octahedra on both Al-free Fh and Al-bearing Fh, by forming bidentate mononuclear edge-sharing (2E) and bidentate binuclear corner-sharing (2C) surface complexes characterized by As–Fe distances of 2.9 Å and 3.4 Å, respectively. The decrease in As(III) sorption density with increasing Al:Fe ratio in Fh could thus be explained by a low affinity of the As(OH)3 molecule for Al surface sites compared to Fe ones. In contrast, on the basis of available literature on As(V) adsorption mechanisms, we suggest that, in addition to inner-sphere 2C arsenate surface complexes, outer-sphere arsenate surface complexes forming hydrogen bonds with both Al–OH and Fe–OH surface sites could explain the enhancement of As(V) sorption onto aluminous Fh relative to Al-free Fh, as observed in the present study. The presence of aluminum in Fh may thus enhance the mobility of arsenite with respect to arsenate in Acid Mine Drainage impacted systems, while mixed Al:Fe systems could present an alternative for arsenic removal from impacted waters, provided that As(III) would be oxidized to As(V).  相似文献   

10.
The stoichiometry and stability of arsenic gaseous complexes were determined in the system As-H2O ± NaCl ± HCl ± H2S at temperatures up to 500°C and pressures up to 600 bar, from both measurements of As(III) and As(V) vapor-liquid and vapor-solid partitioning, and X-ray absorption fine structure (XAFS) spectroscopic study of As(III)-bearing aqueous fluids. Vapor-aqueous solution partitioning for As(III) was measured from 250 to 450°C at the saturated vapor pressure of the system (Psat) with a special titanium reactor that allows in situ sampling of the vapor phase. The values of partition coefficients for arsenious acid (H3AsO3) between an aqueous solution (pure H2O) and its saturated vapor (K = mAsvapor /mAsliquid) were found to be independent of As(III) solution concentrations (up to ∼1 to 2 mol As/kg) and equal to 0.012 ± 0.003, 0.063 ± 0.023, and 0.145 ± 0.020 at 250, 300, and 350°C, respectively. These results are interpreted by the formation, in the vapor phase, of As(OH)3(gas), similar to the aqueous As hydroxide complex dominant in the liquid phase. Arsenic chloride or sulfide gaseous complexes were found to be negligible in the presence of HCl or H2S (up to ∼0.5 mol/kg of vapor). XAFS spectroscopic measurements carried out on As(III)-H2O (±NaCl) solutions up to 500°C demonstrate that the As(OH)3 complex dominates As speciation both in dense H2O-NaCl fluids and low-density supercritical vapor. Vapor-liquid partition coefficients for As(III) measured in the H2O-NaCl system up to 450°C are consistent with the As speciation derived from these spectroscopic measurements and can be described by a simple relationship as a function of the vapor-to-liquid density ratio and temperature. Arsenic(III) partitioning between vapor and As-concentrated solutions (>2 mol As/kg) or As2O3 solid is consistent with the formation, in the vapor phase, of both As4O6 and As(OH)3. Arsenic(V) (arsenic acid, H3AsO4) vapor-liquid partitioning at 350°C for dilute aqueous solution was interpreted by the formation of AsO(OH)3 in the vapor phase.The results obtained were combined with the corresponding properties for the aqueous As(III) hydroxide species to generate As(OH)3(gas) thermodynamic parameters. Equilibrium calculations carried out by using these data indicate that As(OH)3(gas) is by far the most dominant As complex in both volcanic gases and boiling hydrothermal systems. This species is likely to be responsible for the preferential partition of arsenic into the vapor phase as observed in fluid inclusions from high-temperature (400 to 700°C) Au-Cu (-Sn, -W) magmatic-hydrothermal ore deposits. The results of this study imply that hydrolysis and hydration could be also important for other metals and metalloids in the H2O-vapor phase. These processes should be taken into account to accurately model element fractionation and chemical equilibria during magma degassing and fluid boiling.  相似文献   

11.
Mineral assemblages and chemical compositions of ore minerals from the Boroo gold deposit in the North Khentei gold belt of Mongolia were studied to characterize the gold mineralization, and to clarify crystallization processes of the ore minerals. The gold deposit consists of low‐grade disseminated and stockwork ores in granite, metasedimentary rocks and diorite dikes. Moderate to high‐grade auriferous quartz vein ores are present in the above lithological units. The ore grades of the former range from about 1 to 3 g/t, and those of the latter from 5 to 10 g/t, or more than 10 g/t Au. The main sulfide minerals in the ores are pyrite and arsenopyrite, both of which are divisible into two different stages (pyrite‐I and pyrite‐II; arsenopyrite‐I and arsenopyrite‐II). Sphalerite, galena, chalcopyrite, and tetrahedrite are minor associated minerals, with trace amounts of bournonite, boulangerite, geerite, alloclasite, native gold, and electrum. The ore minerals in the both types of ores are variable in distribution, abundance and grain size. Four modes of gold occurrence are recognized: (i) “invisible” gold in pyrite and arsenopyrite in the disseminated and stockwork ores, and in auriferous quartz vein ores; (ii) microscopic native gold, 3 to 100 µm in diameter, that occurs as fine grains or as an interstitial phase in sulfides in the disseminated and stockwork ores, and in auriferous quartz vein ores; (iii) visible native gold, up to 1 cm in diameter, in the auriferous quartz vein ores; and (iv) electrum in the auriferous quartz vein ores. The gold mineralization of the disseminated and stockwork ores consists of four stages characterized by the mineral assemblages of: (i) pyrite‐I + arsenopyrite‐I; (ii) pyrite‐II + arsenopyrite‐II; (iii) sphalerite + galena + chalcopyrite + tetrahedrite + bournonite + boulangerite + alloclasite + native gold; and (iv) native gold. In the auriferous quartz vein ores, five mineralization stages are defined by the following mineral assemblages: (i) pyrite‐I; (ii) pyrite‐II + arsenopyrite; (iii) sphalerite + galena + chalcopyrite; (iv) Ag‐rich tetrahedrite‐tennantite + bournonite + geerite + native gold; and (v) electrum. The As–Au relations in pyrite‐II and arsenopyrite suggest that gold detected as invisible gold is mostly attributed to Au+1 in those minerals. By applying the arsenopyrite geothermometer to arsenopyrite‐II in the disseminated and stockwork ores, crystallization temperature and logfs2 are estimated to be 365 to 300 °C and –7.5 to –10.1, respectively.  相似文献   

12.
《Chemical Geology》2006,225(3-4):278-290
The thermodynamic mixing properties of As into pyrite and marcasite have been investigated using first-principles and Monte Carlo calculations in order to understand the incorporation of this important metalloid into solid solution. Using quantum-mechanical methods to account for spin and electron transfer processes typical of sulfide minerals, the total energies of different As–S configurations were calculated at the atomic scale, and the resulting As–S interactions were incorporated into Monte Carlo simulations. Enthalpies, configurational entropies and Gibbs free energies of mixing show that two-phase mixtures of FeS2 (pyrite or marcasite) and FeAsS (arsenopyrite) are energetically more favorable than the solid solution Fe(S,As)2 (arsenian pyrite or marcasite) for a wide range of geologically relevant temperatures. Although miscibility gaps dominate both solid solution series, the solubility of As is favored for XAs < 0.05 in iron disulfides. Consequently, pyrite and marcasite can host up to ∼6 wt.% of As in solid solution before unmixing into (pyrite or marcasite) + arsenopyrite. This finding is in agreement with previously published HRTEM observations of As-rich pyrites (> 6 wt.% As) that document the presence of randomly distributed domains of pyrite + arsenopyrite at the nanoscale. According to the calculations, stable and metastable varieties of arsenian pyrite and marcasite are predicted to occur at low (XAs < 0.05) and high (XAs > 0.05) As bulk compositions, respectively.  相似文献   

13.
This report describes a new form of arsenian pyrite, called As3+-pyrite, in which As substitutes for Fe [(Fe,As)S2], in contrast to the more common form of arsenian pyrite, As1−-pyrite, in which As1− substitutes for S [Fe(As,S)2]. As3+-pyrite has been observed as colloformic overgrowths on As-free pyrite in a hydrothermal gold deposit at Yanacocha, Peru. XPS analyses of the As3+-pyrite confirm that As is present largely as As3+. EMPA analyses show that As3+-pyrite incorporates up to 3.05 at % of As and 0.53 at. %, 0.1 at. %, 0.27 at. %, 0.22 at. %, 0.08 at. % and 0.04 at. % of Pb, Au, Cu, Zn, Ni, and Co, respectively. Incorporation of As3+ in the pyrite could be written like: As3++yAu++1-y(□)⇔2Fe2+; where Au+ and vacancy (□) help to maintain the excess charge. HRTEM observations reveal a sharp boundary between As-free pyrite and the first overgrowth of As3+-pyrite (20-40 nm thick) and co-linear lattice fringes indicating epitaxial growth of As3+-pyrite on As-free pyrite. Overgrowths of As3+-pyrite onto As-free pyrite can be divided into three groups on the basis of crystal size, 8-20 nm, 100-300 nm and 400-900 nm, and the smaller the crystal size the higher the concentration of toxic arsenic and trace metals. The Yanacocha deposit, in which As3+-pyrite was found, formed under relatively oxidizing conditions in which the dominant form of dissolved As in the stability field of pyrite is As3+; in contrast, reducing conditions are typical of most environments that host As1−-pyrite. As3+-pyrite will likely be found in other oxidizing hydrothermal and diagenetic environments, including high-sulfidation epithermal deposits and shallow groundwater systems, where probably kinetically controlled formation of nanoscale crystals such as observed here would be a major control on incorporation and release of As3+ and toxic heavy metals in oxidizing natural systems.  相似文献   

14.
Mineral assemblages, chemical compositions of ore minerals, wall rock alteration and fluid inclusions of the Gatsuurt gold deposit in the North Khentei gold belt of Mongolia were investigated to characterize the gold mineralization, and to clarify the genetic processes of the ore minerals. The gold mineralization of the deposit occurs in separate Central and Main zones, and is characterized by three ore types: (i) low‐grade disseminated and stockwork ores; (ii) moderate‐grade quartz vein ores; and (iii) high‐grade silicified ores, with average Au contents of approximately 1, 3 and 5 g t?1 Au, respectively. The Au‐rich quartz vein and silicified ore mineralization is surrounded by, or is included within, the disseminated and stockwork Au‐mineralization region. The main ore minerals are pyrite (pyrite‐I and pyrite‐II) and arsenopyrite (arsenopyrite‐I and arsenopyrite‐II). Moderate amounts of galena, tetrahedrite‐tennantite, sphalerite and chalcopyrite, and minor jamesonite, bournonite, boulangerite, geocronite, scheelite, geerite, native gold and zircon are associated. Abundances and grain sizes of the ore minerals are variable in ores with different host rocks. Small grains of native gold occur as fillings or at grain boundaries of pyrite, arsenopyrite, sphalerite, galena and tetrahedrite in the disseminated and stockwork ores and silicified ores, whereas visible native gold of variable size occurs in the quartz vein ores. The ore mineralization is associated with sericitic and siliceous alteration. The disseminated and stockwork mineralization is composed of four distinct stages characterized by crystallization of (i) pyrite‐I + arsenopyrite‐I, (ii) pyrite‐II + arsenopyrite‐II, (iii) galena + tetrahedrite + sphalerite + chalcopyrite + jamesonite + bournonite + scheelite, and iv) boulangerite + native gold, respectively. In the quartz vein ores, four crystallization stages are also recognized: (i) pyrite‐I, (ii) pyrite‐II + arsenopyrite + galena + Ag‐rich tetrahedrite‐tennantite + sphalerite + chalcopyrite + bournonite, (iii) geocronite + geerite + native gold, and (iv) native gold. Two mineralization stages in the silicified ores are characterized by (i) pyrite + arsenopyrite + tetrahedrite + chalcopyrite, and (ii) galena + sphalerite + native gold. Quartz in the disseminated and stockwork ores of the Main zone contains CO2‐rich, halite‐bearing aqueous fluid inclusions with homogenization temperatures ranging from 194 to 327°C, whereas quartz in the disseminated and stockwork ores of the Central zone contains CO2‐rich and aqueous fluid inclusions with homogenization temperatures ranging from 254 to 355°C. The textures of the ores, the mineral assemblages present, the mineralization sequences and the fluid inclusion data are consistent with orogenic classification for the Gatsuurt deposit.  相似文献   

15.
The enrichment of gold in arsenian pyrite is usually associated closely with the enrichment of arsenic in the mineral, generally known as As1−-pyrite [Fe(As, S)2]. Direct analyses of the valence state of Au in pyrite are, however, difficult due to generally low (∼ppm level) Au concentrations. By means of X-ray photoelectron spectroscopy (XPS), this study obtained reliable valence states of As in pyrite from the Yang-shan gold deposit, a giant “Carlin-type” Au deposit in the western Qinling orogen, central China. The arsenian pyrite specimens were sputtered with Ar+ beam in the vacuum chamber of an XPS to obtain pristine surfaces and to avoid As oxidation during sample preparation. Analyses before and after sputtering show that the As3+ peak are only present on surface that was once exposed to the air. In contrast, the peak of As−1 was essentially unchanged during continuous sputtering. The results indicated that As− is the predominant state on the pristine surface of arsenian pyrite; the peak of As3+ previously reported for Au-bearing arsenian pyrite was probably due to oxidation when exposed to air during sample preparation. It is unlikely that the coupled substitution of (Au+ + As3+) for 2Fe2+ takes place in the pyrite lattice. The so-called As3+-pyrite proposed by previous studies may occur in some special (oxidizing) geologic settings, but it is not observed in the Yang-shan gold deposit, and is unlikely to be important in typical orogenic or Carlin-type gold deposits, in which arsenian pyrite is a dominant Au carrier. Combining previous studies on Carlin-type Au deposits with our XPS experimental results, we suggest that the most likely state of Au in the Yang-shan Au deposit is lattice-bounded Au with or without nanoparticles (Au0).  相似文献   

16.
Hemimorphite is a refractory mineral in surface environments and occurs commonly in supergene non-sulfide Zn deposits and Zn mine tailings. Single-crystal electron paramagnetic resonance (EPR) spectra of gamma-ray-irradiated hemimorphite from Mapimi (Durango, Mexico) reveal two arsenic-associated oxyradicals: [AsO4]4− and [AsO4]2−. Inductively coupled plasma mass spectrometry analyses confirm this sample to contain 270 ppm As and that hemimorphite from other Zn deposits has appreciable amounts of arsenic as well. Spin Hamiltonian parameters, including matrices g, A (75As) and P(75As), show that the [AsO4]4− radical formed from electron trapping by a locally uncompensated [AsO4]3− ion substituting for [SiO4]4−. Matrices g, A(75As) and P(75As) of the [AsO4]2− radical show it to have the unpaired spin on the bridging oxygen of an [AsO4]3− ion at a Si site and linked to a monovalent impurity ion. This structural model for the [AsO4]2− radical is further supported by observed 29Si and 1H superhyperfine structures arising from interactions with a single Si atom (A/geβe = ∼1 mT at B//c) and two equivalent H atoms (A/geβe = ∼0.3 mT at B∧b = 10°), respectively. Hydrothermal experiments at 200 °C and ∼9.5 MPa show that hemimorphite contains up to ∼2.5 wt% As2O5 and suggest that both the arsenate concentration and the pH value in the solution affect the As content in hemimorphite. These results demonstrate that hemimorphite is capable of sequestering arsenate in its crystal lattice, hence is a natural sink for attenuating As in supergene non-sulfide Zn deposits and Zn mine tailings. Moreover, results from hemimorphite potentially have more far-reaching implications for major silicates such as zeolites in the immobilization and removal of arsenic in surface environments.  相似文献   

17.
Arsenic(V), as the arsenate (AsO4)3− ion and its conjugate acids, is strongly sorbed to iron(III) oxides (α-Fe2O3), oxide hydroxides (α-,γ-FeOOH) and poorly crystalline ferrihydrite (hydrous ferric oxide). The mechanism by which arsenate complexes with iron oxide hydroxide surfaces is not fully understood. There is clear evidence for inner sphere complexation but the nature of the surface complexes is controversial. Possible surface complexes between AsO4 tetrahedra and surface FeO6 polyhedra include bidentate corner-sharing (2C), bidentate edge-sharing (2E) and monodentate corner-sharing (1V). We predicted the relative energies and geometries of AsO4-FeOOH surface complexes using density functional theory calculations on analogue Fe2(OH)2(H2O)nAsO2(OH)23+ and Fe2(OH)2(H2O)nAsO4+ clusters. The bidentate corner-sharing complex is predicted to be substantially (55 kJ/mole) more favored energetically over the hypothetical edge-sharing bidentate complex. The monodentate corner-sharing (1V) complex is very unstable. We measured EXAFS spectra of 0.3 wt. % (AsO4)3− sorbed to hematite (α-Fe2O3), goethite(α-FeOOH), lepidocrocite(γ-FeOOH) and ferrihydrite and fit the EXAFS directly with multiple scattering. The phase-shift-corrected Fourier transforms of the EXAFS spectra show peaks near 2.85 and 3.26 Å that have been attributed by previous investigators to result from 2E and 2C complexes. However, we show that the peak near 2.85 Å appears to result from As-O-O-As multiple scattering and not from As-Fe backscatter. The observed 3.26 Å As-Fe distance agrees with that predicted for the bidentate corner-sharing surface (2C) complex. We find no evidence for monodentate (1V) complexes; this agrees with the predicted high energies of such complexes.  相似文献   

18.
Mine tailings at the former Delnite gold mine in northern Ontario were characterized to assess the impact of a biosolids cover on the stability of As species and evaluate options for long-term management of the tailings. Arsenic concentrations in the tailings range from 0.15 to 0.36 wt% distributed among goethite, pyrite and arsenopyrite. Pyrite and arsenopyrite occur as small and liberated particles that are enveloped by goethite in the uncovered tailings and the deeper portions of the biosolids-covered tailings. Sulfide particles in the shallower portions of the biosolids-covered tailings are free of goethite rims. Arsenic occurs predominantly as As5+ with minor amount of As1− in the uncovered tailings. Coinciding with the disappearence of goethite rims on sulfide particles, the biosolids-covered tailings have As3+ species gradually increasing in proportion towards the cover. Leaching tests indicated that the As concentrations in the leachate gradually increase from less than 0.085 to 13 mg/L and Fe from 28 to 179 mg/L towards the biosolids cover. These are in sheer contrast to the leachate concentrations of less than 0.085 mg/L As and 24–64 mg/L Fe obtained from the uncovered tailings confirming the role of biosolids-influenced reduction and mobilization of As in the form of As3+ species. The evidence suggests that reductive dissolution of goethite influenced by the biosolids-cover caused the mobilization of As as As3+ species.  相似文献   

19.
Over 60 minerals, including native elements, intermetallic compounds, haloids, sulfides, sulfates, arsenides, oxides and hydroxides, silicates, borosilicates, wolframates, phosphates and REE phosphates, were established in Triassic siliceous rocks of Sikhote Alin. Allothigenic and authigenic minerals in the carbonaceous silicites were formed over a long period through several stages. Judging from morphology, chemical composition, and structural position, K-feldspar (K-Fsp), illite, kaolinite, metahalloysite, monazite, xenotime, zircon, rutile, or its polymorphs are the disintegration products of sialic rocks of continental crust. Authigenic sulfides are dominated by diagenetic pyrite (fine-crystalline, microglobular, framboidal, as well as those developed after biogenic siliceous and carbonate fragments), which has been formed prior to precipitation of siliceous cement and lithification of siliceous rocks. Most of other sulfides (sphalerite, galena, chalcopyrite, pyrrhotite, argentite, pentlandite, antimonite, ulmanite, and bravoite), arsenides and sulfoarsenides (arsenopyrite, nickeline, skutterudite, cobaltite, glaucodot, and gersdorffite), wolframates (scheelite and wolframite), intermetallides (Cu2Zn, Cu3Zn2, Cu3Zn, Cu4Zn, CuSn, Cu4Sn, Cu8Sn, Cu4Zn2Ni, Ni2Cu2Zn, Ni4Cd), and native elements (Au, Pd, Ag, Cu, Fe, W, Ni, Se) were crystallized later (during catagenesis after the lithification and brecciation of siliceous beds) from metals involved in the easily mobile fractions of bitumens. Supergene mineral formation was mainly expressed in the sulfide oxidation and replacement of diagenetic pyrite by jarosite and iron hydroxides.  相似文献   

20.
Six epizonal gold deposits in the 30-km-long Yangshan gold belt, Gansu Province are estimated to contain more than 300 t of gold at an average grade of 4.76 g/t and thus define one of China's largest gold resources. Detailed paragenetic studies have recognized five stages of sulfide mineral precipitation in the deposits of the belt. Syngenetic/diagenetic pyrite (Py0) has a framboidal or colloform texture and is disseminated in the metasedimentary host rocks. Early hydrothermal pyrite (Py1) in quartz veins is disseminated in metasedimentary rocks and dikes and also occurs as semi-massive pyrite aggregates or bedding-parallel pyrite bands in phyllite. The main ore stage pyrite (Py2) commonly overgrows Py1 and is typically associated with main ore stage arsenopyrite (Apy2). Late ore stage pyrite (Py3), arsenopyrite (Apy3), and stibnite occur in quartz ± calcite veins or are disseminated in country rocks. Post-ore stage pyrite (Py4) occurs in quartz ± calcite veins that cut all earlier formed mineralization. Electron probe microanalyses and laser ablation-inductively coupled plasma mass spectrometry analyses reveal that different generations of sulfides have characteristic of major and trace element patterns, which can be used as a proxy for the distinct hydrothermal events. Syngenetic/diagenetic pyrite has high concentrations of As, Au, Bi, Co, Cu, Mn, Ni, Pb, Sb, and Zn. The Py0 also retains a sedimentary Co/Ni ratio, which is distinct from hydrothermal ore-related pyrite. Early hydrothermal Py1 has high contents of Ag, As, Au, Bi, Cu, Fe, Sb, and V, and it reflects elevated levels of these elements in the earliest mineralizing metamorphic fluids. The main ore stage Py2 has a very high content of As (median value of 2.96 wt%) and Au (median value of 47.5 ppm) and slightly elevated Cu, but relatively low values for other trace elements. Arsenic in the main ore stage Py2 occurs in solid solution. Late ore stage Py3, formed coevally with stibnite, contains relatively high As (median value of 1.44 wt%), Au, Fe, Mn, Mo, Sb, and Zn and low Bi, Co, Ni, and Pb. The main ore stage Apy2, compared to late ore stage arsenopyrite, is relatively enriched in As, whereas the later Apy3 has high concentrations of S, Fe, and Sb, which is consistent with element patterns in associated main and late ore stage pyrite generations. Compared with pyrite from other stages, the post-ore stage Py4 has relatively low concentrations of Fe and S, whereas As remains elevated (2.05～3.20 wt%), which could be interpreted by the substitution of As? for S in the pyrite structure. These results suggest that syngenetic/diagenetic pyrite is the main metal source for the Yangshan gold deposits where such pyrite was metamorphosed at depth below presently exposed levels. The ore-forming elements were concentrated into the hydrothermal fluids during metamorphic devolatilization, and subsequently, during extensive fluid–rock interaction at shallower levels, these elements were precipitated via widespread sulfidation during the main ore stage.  相似文献   

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