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1.
The leaching rate of 134Cs in cement has been studied. The solidification matrix by a standard Portland cement mixed with the spent ion-exchange resins was previously developed. The leaching rates from cement matrices were measured in function of pH, the immersion and curing times, the resin amounts, and 134Cs concentration. In all cases, the leaching rate was deduced from 134Cs cumulative activity measured by gamma spectrometry. The study showed that only 11.8% of total 134Cs has been leached. This fraction concentrated to the solid surface by silanols has been moved during 34 days through two mechanisms. The Langmuir and Freundlich isotherms attributed these two mechanisms at successive attacks, by water and multilayer and monolayer site formed at the interface package/water. The presence of the spent ion-exchange resins in the matrix, as waste, improves and increases 134Cs retention power in the cemented package. In fact, the fraction of 134Cs mobilized in the absence of resins (3.18 Bq/Kg) becomes negligible in the presence of 12% of resins.  相似文献   

2.
Microscopic distribution and speciation of Na, Mg, Ni and Cs in a simulated (inactive) nuclear waste glass were studied using micro X-ray fluorescence (μ-XRF) and micro X-ray absorption spectroscopy (μ-XAS), after aqueous leaching during 12 years at 90 °C. Na and Mg are major constituents of the glass that can be used to determine the progress of the glass corrosion process and the nature of secondary alteration phases. Ni and Cs represent dose determining long-lived radionuclides (59Ni, 135Cs) in vitrified nuclear waste.The Na-Mg μ-XRF maps revealed that the core regions of the glass fragments are apparently unaltered and compositionally homogeneous, whereas rims and interstitial spaces are enriched with Mg-rich smectite formed during the leaching process. The micro X-ray absorption near edge structure (μ-XANES) spectra collected at the Mg K-edge in the altered zones show three sharp resonances typical for crystalline Mg-silicates. These resonances are distinctive of Mg occupying undistorted octahedral positions. In contrast, the μ-XANES spectra collected in the core zones of the glass fragments lack this resonance pattern and are identical to the spectra measured on the pristine (unleached) MW glass.Micro extended X-ray absorption fine structure (μ-EXAFS) and μ-XANES analyses at the Ni K-edge revealed three distinct Ni(II) species: (a) Ni uniformly distributed in the glass matrix, (b) micro-inclusions with high Ni concentrations and (c) Ni associated to the Mg-clay. The comparison with reference spectra of unleached MW and other Ni-bearing silicate glasses indicated that species (a) represents the original coordinative environment of Ni in the glass. The μ-EXAFS analyses revealed that species (b) is structural Ni in trevorite (NiFe2O4), which probably formed through unmixing processes during the cooling of the glass melt. The μ-EXAFS of species (c) could be successfully modeled assuming specific adsorption or incorporation of Ni into the lattice of trioctahedral Mg-clay minerals. Alternative models assuming other elements (Ni, Al, Fe) in addition to Mg in the second shell could not be fitted successfully.Aqueous concentration data were used to calculate the speciation of the leaching solutions. Saturation index (SI) calculations indicate undersaturation with respect to NiCO3 and NiSO4·7H2O, but oversaturation with respect to β-Ni(OH)2. The latter result is probably due to the omission of Ni borate and Ni silicate complexes in the speciation calculations, for which formation constants are not available. With the help of estimation techniques, we could infer that such complexes would dominate the Ni speciation and consequently reduce the SI below the saturation of β-Ni(OH)2.The μ-XRF maps show that Cs is uniformly distributed in the MW glass, since no region with high Cs concentration could be detected. The Cs LIII-edge μ-XAS spectra were all very similar independently of the degree of alteration, indicating similar coordination environments of Cs in the core regions of the glass as well as in the secondary clays. These spectra largely differ from that measured for pollucite (a potential secondary Cs-phase in altered glasses) implying that the coordination environments of Cs in the MW glass and in pollucite are fundamentally different.The present study shows that μ-XRF and μ-XAS are essential tools in determining the fate and the retention mechanisms of radionuclides released from nuclear waste during aqueous alteration. Our spectroscopic analyses allowed us to exclude formation of specific Ni and Cs secondary solids (e.g. nepouite, β-Ni(OH)2, pollucite) during the aqueous alteration. Ni and Cs are instead distributed as trace elements in the alteration phases formed by major elements during the leaching process. Our results imply that solid solution and/or adsorption equilibria, rather than pure phase solubility equilibria, are the adequate chemical models to determine Ni and Cs aqueous concentrations in performance assessments for radioactive waste repositories.  相似文献   

3.
The radiation resistance of the phase (Gd,Cm)2Sn2O7 with a pyrochlore-type structure containing 3.0 wt % 244Cm was studied. It was established that amorphization occurs at a dose of 1019 α-decay/g (1.52 displacements per atom), which is 2–5 times higher than that needed for amorphization of titanate and titanate–zirconate pyrochlore phases with a similar structure. The heating of the amorphous ceramics restores the structure of the pyrochlore. The restoration process begins in the temperature interval of 600–700°C. This allows us to estimate the critical amorphization temperature as 650°C. On the 14th day, the rate of Cm leaching from the initial sample in water at 90°C is 10–1; Gd, 10–2; and Sn, 10–3 g/(m2 day). After amorphization the leaching rate increases by an order of magnitude (Cm) and two orders of magnitude (Gd), but it does not change for Sn. Compared to the zirconate and titanate–zirconate phases, stannate pyrochlore is markedly less resistant in water and cannot be regarded as a matrix for the immobilization of REE-actinide fraction wastes.  相似文献   

4.
《Applied Geochemistry》2002,17(12):1503-1513
The interaction of CO2 with municipal solid waste incinerator (MSWI) bottom ash was studied in order to investigate the resulting changes in pH and bottom ash mineralogy and the impact that these changes have on the mobility of Cu and Mo. Carefully controlled carbonation experiments were performed on bottom ash suspensions and on filtered bottom ash leachates. Changes in leachate composition were interpreted with the geochemical model MINTEQA2, and neoformed minerals were investigated by means of chemical and spectroscopic analysis. The leaching of Cu and Mo during artificial carbonation is compared to the leachability of Cu and Mo from a sample of naturally carbonated bottom ash from the same incinerator. During carbonation in the laboratory, a precipitate was formed that consisted mainly of Al-rich amorphous material, calcite, and possibly gibbsite. Carbonation to pH ≈8.3 resulted in a reduction of more than 50% in Cu leaching, and a reduction of less than 3% in Mo leaching. The reduction in Cu leaching is attributed to sorption to the neoformed amorphous Al-minerals. During natural weathering/carbonation of bottom ash, additional sorption sites are formed which further reduce the leaching of Cu and Mo on a time scale of months to years.  相似文献   

5.
Red mud (RM) was produced during alumina production from bauxite known as the Bayer process. Arsenic was detected in the solid phase of RM (RMsf) which was disposed in the disposal area. This study investigates the effectiveness of using Zero-valent iron (ZVI), ferrihydrite, ferrous sulfate (FeSO4), waste acid (WA) or CO2 for immobilization of arsenic in the RMsf. To test the effect of the amendments on the arsenic leachability, the RMsf samples were amended with the iron-based materials or acidifiers at various w/w (weight/weight) ratios (1–10 %) for 30 days. The leachability of arsenic in the RMsf was evaluated by a 4-step water elusion process. After 30-day treatment of the RMsf, the leachability of As decreased from an initial (12.7 %) to (7.0 %) with a w/w ratio of 5 % ZVI (0 %) with 5 % FeSO4·7H2O, (3.4 %) with 5 % ferryhydrite, (2.0 %) with 6 % WA and (11.8 %) with 6 % CO2. FeSO4·7H2O and WA showed more effectively than other amendments for immobilizing arsenic. Arsenic fractionation with a sequential extraction procedure was used to evaluate the arsenic migration potential in the RMsf. FeSO4 and WA were effective in increasing the hydrous oxide combined arsenic in the RMsf. The leachable Cl? and SO4 2? in the RMsf increased from 2.9 to 14.1 mg/g and 19.9–44.4 mg/g with 6 % WA and 5 % FeSO4·7H2O added, respectively. The estimated cost of the FeSO4 and WA treatment was 0.47 and 0.49 USD per ton, respectively.  相似文献   

6.
Radioactive core samples containing elevated concentrations of Cr from a high level nuclear waste plume in the Hanford vadose zone were studied to asses the future mobility of Cr. Cr(VI) is an important subsurface contaminant at the Hanford Site. The plume originated in 1969 by leakage of self-boiling supernate from a tank containing REDOX process waste. The supernate contained high concentrations of alkali (NaOH ≈ 5.25 mol/L), salt (NaNO3/NaNO2 >10 mol/L), aluminate [Al(OH)4− = 3.36 mol/L], Cr(VI) (0.413 mol/L), and 137Cs+ (6.51 × 10−5 mol/L). Water and acid extraction of the oxidized subsurface sediments indicated that a significant portion of the total Cr was associated with the solid phase. Mineralogic analyses, Cr valence speciation measurements by X-ray adsorption near edge structure (XANES) spectroscopy, and small column leaching studies were performed to identify the chemical retardation mechanism and leachability of Cr. While X-ray diffraction detected little mineralogic change to the sediments from waste reaction, scanning electron microscopy (SEM) showed that mineral particles within 5 m of the point of tank failure were coated with secondary, sodium aluminosilicate precipitates. The density of these precipitates decreased with distance from the source (e.g., beyond 10 m). The XANES and column studies demonstrated the reduction of 29-75% of the total Cr to insoluble Cr(III), and the apparent precipitation of up to 43% of the Cr(VI) as an unidentified, non-leachable phase. Both Cr(VI) reduction and Cr(VI) precipitation were greater in sediments closer to the leak source where significant mineral alteration was noted by SEM. These and other observations imply that basic mineral hydrolysis driven by large concentrations of OH− in the waste stream liberated Fe(II) from the otherwise oxidizing sediments that served as a reductant for CrO42−. The coarse-textured Hanford sediments contain silt-sized mineral phases (biotite, clinochlore, magnetite, and ilmenite) that are sources of Fe(II). Other dissolution products (e.g., Ba2+) or Al(OH)4− present in the waste stream may have induced Cr(VI) precipitation as pH moderated through mineral reaction. The results demonstrate that a minimum of 42% of the total Cr inventory in all of the samples was immobilized as Cr(III) and Cr(VI) precipitates that are unlikely to dissolve and migrate to groundwater under the low recharge conditions of the Hanford vadose zone.  相似文献   

7.
This study was conducted to investigate the stabilization of arsenic sulfide slag (ASS) with CaO calcinations at moderate temperature, including the effects of calcination temperature and different As/Ca molar ratios on arsenic leaching concentration. In the process of calcination for arsenic-contained waste, 90.95–97.23% of arsenic was reserved and the original waste was transformed into a dense and liquation state, which could physically wrap arsenic and reduce its leaching concentration. Meanwhile, the decrease in the As/Ca molar ratios was conducive to the formation of Ca5(AsO4)3(OH). When As/Ca molar ratio was less than 1:8, there was excessive CaO and the ASS samples stopped reacting with CaO. The results showed that the leaching concentration of arsenic was 4.08 mg/L when As/Ca molar ratio was 1:8 and the ASS sample was calcined for 2 h at temperature of 550 °C. In the process, arsenic’s chemical reaction and physical wrapping resulted in a remarkable decrease in its leaching concentration.  相似文献   

8.
The sorption of cesium and iodide ions onto KENTEX-bentonite was investigated using batch test and in-diffusion test methods. The cesium ions were highly sorbed on the bentonite, and the experimental data fit the Freundlich isotherm well. The distribution coefficient, K d, of the cesium ions was variably affected by the chemical conditions of the solution (initial ion concentration, pH, salinity) and temperature. An increasing pH of solution increased the K d. However, there were different K d values that decrease with an increase in the initial ion concentration, salinity, and temperature. The iodide ions, on the contrary, were negligibly sorptive. The K d values obtained from the in-diffusion tests were quite lower than those from the batch tests, which could be explained by changes in the pore water chemistry and surface area available for sorption.  相似文献   

9.
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10.
The aim of the study was to determine whether the application of phosphate compounds (phosphorite rock, phosphate fertilizer) to polyminerallic waste rocks can inhibit sulfide oxidation and metal mobility (Cu, Pb, Zn, Cd, Ni, Mn, Mg). Waste rocks comprised sulfidic carbonaceous shales and were sourced from the Century Pb-Zn mine, NW Queensland, Australia. The acid producing, Pb-Zn rich rocks consisted of major quartz, muscovite/illite, dolomite, siderite and kaolinite as well as smaller amounts of sulfide minerals (e.g. galena, sphalerite, pyrite). Laboratory leach experiments were conducted on finely granulated phosphate-treated waste rocks (>2 to <30 mm) over 13 weeks, whereas phosphate amendment of coarsely granulated waste rocks (sand to boulder size) was investigated using heap leach piles at the mine site over an 11 months period. Results of the laboratory experiments demonstrate that the treatment of finely granulated waste rocks with phosphorite rock produced leachates with near-neutral pH values due to calcite dissolution. This in turn did not allow the leaching of apatite, formation of secondary phosphate phases and phosphate stabilization to occur. Metal mobility in these amended wastes was restricted by the dissolution of calcite and the resultant near-neutral pH conditions. By contrast, the application of the water-soluble phosphate fertilizer MKP (KH2PO4) to polyminerallic sulfidic waste rocks during the short-term laboratory experiments led to the formation of phosphate coatings and precipitates and inhibited acid and metal release (Cd, Mn, Ni, Pb, Zn). At least in the short term, the application of phosphate fertilizers proved to be an effective method. However, results of the long-term field trials demonstrate that coarsely granulated waste rocks were not coated by secondary phosphate phases and that amendment by phosphorite rock or superphosphate fertilizer did not improve leachate quality compared to the unamended waste. Thus, phosphate stabilization appears ineffective in suppressing oxidation of sulfides in coarsely granulated mine wastes.  相似文献   

11.
Extraction of the actinide-REE fraction and its subsequent incorporation into sparingly soluble crystalline phases (confinement matrices) is assumed in processing of spent nuclear fuel from high-level radioactive wastes (HLW). The chemical stability in the process of interaction with subsurface water governs the capability of a matrix phase to keep radionuclides from getting into the biosphere. In static experiments at 90 and 150°C, the chemical stability of ferrite garnets was investigated for three compositions with Th4+, Ce4+ and Gd3+ + serving as simulator components of the actinide fraction of HLW. Experiments were carried out in distilled water (pH 6.5), 0.01 M HCl solution (pH 2), and 0.01 M NaOH solution (pH 12). The behavior of ferrigarnet matrices depends on the acidity of the solution. In neutral and alkaline media, Th, Ce, and Gd are virtually not transferred into the liquid phase. Acid leaching promotes intense dissolution of garnet matrices. In this case, the leaching rate of Gd and Th from ceramics into the liquid phase is two orders of magnitude lower than the leaching rate of Ce because the Ce-doped phases contain less stable (relative to garnet) Ce-rich perovskite. Amorphization of the ferrigarnet structure due to 244Cm isotope decay leads to an increase in the leaching rate of Cm by no more than five times. In terms of radiation and chemical stability, ferrite garnets are not inferior to zirconolites and titanate pyrochlores. The experimental results suggest that garnet matrices can reliably immobilize actinides in subsurface repositories.  相似文献   

12.
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13.
The ability to properly manage the oxidation of pyritic minerals and associated acid mine drainage is dependent upon understanding the chemistry of the disposal environment. One accepted disposal method is placing pyritic-containing materials in the groundwater environment. The objective of this study was to examine solubility relationships of Al and Fe minerals associated with pyritic waste disposed in a low leaching aerobic saturated environment. Two eastern oil shales were used in this oxidizing equilibration study, a New Albany Shale (unweathered, 4.6 percent pyrite), and a Chattanooga Shale (weathered, 1.5 percent pyrite). Oil shale samples were equilibrated with distilled-deionized water from 1 to 180 d with a 1∶1 solid-to-solution ratio. The suspensions were filtered and the clear filtrates were analyzed for total cations and anions. Ion activities were calculated from total concentrations. Below pH 6.0, depending upon SO 4 2− activity, Al3+ solubility was controlled by AlOHSO4 (solid phase) for both shales. Initially, Al3+ solubility for the New Albany Shale showed equilibrium with amorphous Al(OH)3. The pH decreased with time, and Al3+ solubility approached equilibrium with AlOHSO4(s). Below pH 6.0, Fe3+ solubility appeared to be regulated by a basic iron sulfate solid phase with the stoichiometric composition of FeOHSO4(s). The results of this study indicate that below pH 6.0, Al3+ solubilities, are limited by basic Al and Fe sulfate solid phases (AlOHSO4(s) and FeHSO4(s)). The results from this study further indicate that the acidity in oil shale waters is produced from the hydrolysis of Al3+ and Fe3+ activities in solution. These results indicate a fundamental change in the stoichiometric equations used to predict acidity from iron sulfide oxidation. The results of this study also indicate that water quality predictions associated with acid mine drainage can be based on fundamental thermodynamic relationships. As a result, waste management decisions can be based on waste-specific/site-specific test methods.  相似文献   

14.
Here we present the first set of metal-silicate partitioning data for Cs, which we use to examine whether the primitive mantle depletion of Cs can be attributed to core segregation. Our experiments independently varied pressure from 5 to 15 GPa, temperature from 1900 to 2400 °C, metallic sulfur content from pure Fe to pure FeS, silicate melt polymerization, expressed as a ratio of non-bridging oxygens to tetrahedrally coordinated cations (nbo/t) from 1.26 to 3.1, and fO2 from two to four log units below the iron-wüstite buffer. The most important controls on the partitioning behavior of alkalis were the metallic sulfur content, expressed as XS, and the nbo/t of the silicate liquid. Normalization of XS to 0.5 yielded the following expressions for D-values as a function of nbo/t: log DNa = −2.0 + 0.44 × (nbo/t), log DK = −2.4 + 0.67 × ( nbo/t), and log DCs = −3.2 + 1.17 × (nbo/t). Normalization of nbo/t to 2.7 resulted in the following equations for D-values as a function of S content: log DNa = −4.1 + 6.4 × XS, log DK = −7.7 + 13.9 × XS, and log DCs = −12.1 + 23.3 × XS.There appears to be a negative pressure effect up to 15 GPa, but it should be noted that this trend was not present before normalization, and is based on only two measurements. There is a positive trend in cesium’s metal-silicate partition coefficient with increasing temperature. DCs exhibits the largest change and increased by a factor of three over 500 °C. The effect of oxygen fugacity has not been precisely determined but in general, lowering fO2 by two log units resulted in a rise in all D-values of approximately an order of magnitude. In general, the sensitivity of partition coefficients to changing parameters increased with atomic number.The highest D-value for Cs observed in this study is 0.345, which was obtained at nbo/t of 2.7 and a metal phase of pure FeS. This metallic composition has far more S than has been suggested for any credible core-forming metal. We therefore conclude that the depletion of Cs in Earth’s mantle is either caused by radically different behavior of Cs at pressures higher than 15 GPa or is not related to core formation. Even so, we have shown that a planet with a sufficient S inventory may incorporate significant amounts of alkali elements into its core.  相似文献   

15.
The radioactive fission product, 137Cs, has been observed to mobilize from bottom sediments of two South Carolina reservoirs during summer thermal stratification and hypolimnetic anoxia. Mobilization is attributed to ion-exchange displacement of 137Cs from sediments by cations such as NH+4, Fe+2 and Mn+2 released under anaerobic conditions.Three types of 137Cs binding sites to sediment clay minerals are identified: 1) surface and planar sites from which 137Cs is generally exchangeable by all cations studied (Na+, NH+4, H+, Cs+, Ca+2, Mg+2, Fe+2, and Mn+2); 2) wedge sites where 137Cs exchange is sterically limited to cations of similar size and charge (NH+4, Cs+, K+, and perhaps H3O+); 3) interlayer sites from which 137Cs is not readily exchanged. More than 15 years after final 137Cs inputs, the reservoir sediments we studied showed the following percentage distribution of sites: 2 to 9% surface sites, 6 to 13% wedge sites, and 78 to 85% interlayer sites. In contrast, lake and stream sediments near Oak Ridge, Tennessee receiving 137Cs inputs more than 20 years earlier had greater than 99% of their 137Cs associated with non-exchangeable interlayer sites. The difference is attributed to the paucity in the South Carolina sediments of weathered micaceous clay minerals with their abundant interlayer sites. Such interlayer deficient clays are dominant in the Atlantic and Gulf coastal plains of the United States and elsewhere. This suggests that 137Cs will be physically and chemically more mobile in such areas as well as more biologically available. Mobility will be enhanced in regimes where cation inputs favoring 137Cs exchange occur. Subsurface waste disposal sites where anaerobic conditions develop with NH+4 production and Fe+2 and Mn+2 release might be such a regime.  相似文献   

16.
《Applied Geochemistry》2003,18(9):1361-1371
The study of inactive As-bearing tailings impoundments at the Khovu-Aksy mine-site (Russia) revealed high concentrations of As in the porewater of tailings solids and in their aqueous extracts, as well as in adjacent soils. In these investigations, experimental leaching of As-containing tailings was performed in the laboratory. The three types of solutions which were used in the leach experiments to model natural waters and waters of anthropogenic origin were H2O, HNO3 and NH4HCO3, and during leaching with these solutions As concentrations were maintained at 10±2, 16±1 and ∼20 mg/l. No low-pH waters were observed at the end of the leach experiments, where pH varied between 8.3 and 9.1. These alkaline pH conditions are attributed to the effect of acid consuming carbonate mineral dissolution reactions, which are also indicated by increased concentrations of Mg and Ca. Also, the solution of certain heavy metals (Co, Ni, Fe) was negligible compared to that of As, and these metals were assumed to have been conserved in the solid phase. Analysis of the leach solutions, and modeling of the results showed that As could be removed from the surface of different particles where it had been adsorbed, and also its concentration could increase with time from the breakdown of Ca(Mg)- and Ni(Co)-arsenate phases. In the absence of an effective remediation program, As release will continue to be an environmental problem.  相似文献   

17.
In situ X-ray diffraction study on KAlSi3O8 has been performed using the cubic type high pressure apparatus, MAX90, combined with synchrotron radiation. We determined the phase relations of sanidine, the wadeite-type K2Si4O9+kyanite (Al2SiO5)+coesite (SiO2) assemblage, and hollandite-type KAlSi3O8, including melting temperatures of potassic phases, up to 11 GPa. Our data on subsolidus phase boundaries are close to the recent data of Yagi and Akaogi (1991). Melting relations of sanidine are consistent with the low pressure data of Lindsley (1966). The breakdown of sanidine into three phases reduces melting temperature, and wadeite-type K2Si4O9 melts first around 1500° C in three phase coexisting region. Melting point of hollandite-type KAlSi3O8 is between 1700° C and 1800° C at 11 GPa. If these potassic phases host potassium in the earth's mantle, the true mantle solidus temperature will be much lower than the reported dry solidus temperature of peridotite.  相似文献   

18.
In this study, changes in surface area, morphology and leachability of antimony from mechanically activated berthierite—FeSb2S4, boulangerite—Pb5Sb4S11 and franckeite—FePb5Sn3Sb2S14 by a high-energy planetary mill were investigated. It appears that a selective extraction of antimony from these complex sulphosalts in alkaline solution of sodium sulphide is positively affected by mechanical activation. The influence of milling on mineral particle size and shape was studied by scanning electron microscopy. The temperature dependencies of berthierite alkaline leaching were investigated in an interval of 323–363 K. Resulting experimental activation energies E a were 0.11 and 6.78 kJ mol−1 for mechanically activated berthierite due to a break of Arrhenius plot. The values E a are characteristic for a process controlled by diffusion as the rate-controlling step of leaching reaction.  相似文献   

19.
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   

20.
The leaching behaviour of electrostatic precipitator dust from the Mufulira Cu smelter (Copperbelt, Zambia) was studied using a 48-h pH-static leaching experiment (CEN/TS 14997). The release of metals (Cd, Co, Cu, Ni, Pb and Zn) and changes in mineralogical composition using X-ray diffraction and PHREEQC-2 modelling were investigated in the pH range of 3–7. The highest concentrations of metals were released at pH 3–4.5, which encompasses the natural pH of the dust suspension (～4.3). About 40% of the total Cu was leached at pH 3, yielding 107 g/kg. Chalcanthite (CuSO4·5H2O), magnetite (Fe3O4) and delafossite (CuFeO2) represented the principal phases of the studied dust. In contact with water, chalcanthite was dissolved and hydrated Cu sulphates precipitated at pH 4–7. Gypsum (CaSO4·2H2O) and secondary Fe or Al phases were observed in the leached residues. Serious environmental impact due to leaching may occur in dust-contaminated soil systems in the vicinity of the smelting plants.  相似文献   

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