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1.
Three large-scale experimental waste rock piles (test piles) were constructed and instrumented at the Diavik Diamond Mine in the Northwest Territories, Canada, as part of an integrated field and laboratory study to measure and compare physical and geochemical characteristics of experimental, low sulfide waste rock piles at various scales. This paper describes the geochemical response during the first season from a test pile containing 0.053 wt.% S. Bulk drainage chemistry was measured at two sampling points for pH, Eh, alkalinity, dissolved cations and anions, and nutrients. The geochemical equilibrium model MINTEQA2 was used to interpret potential mineral solubility controls on water chemistry. The geochemical response characterizes the initial flushing response of blasting residues and oxidation products derived from sulfides in waste rock exposed to the atmosphere for less than 1 year. Sulfate concentrations reached 2000 mg L−1 when ambient temperatures were >10 °C, and decreased as ambient temperatures declined to <0 °C. The pH decreased to <5, concomitant with an alkalinity minimum of <1 mg L−1 (as total CaCO3), suggesting all available alkalinity is consumed by acid-neutralizing reactions. Concentrations of Al and Fe were <0.36 and <0.11 mg L−1, respectively. Trends of pH and alkalinity and the calculated saturation indices for Al and Fe (oxy)hydroxides suggest that dissolution of Al and Fe (oxy)hydroxide phases buffers the pH. The effluent water showed increased concentrations of dissolved Mn (<13 mg L−1), Ni (<7.0 mg L−1), Co (<1.5 mg L−1), Zn (<0.5 mg L−1), Cd (<0.008 mg L−1) and Cu (<0.05 mg L−1) as ambient temperatures increased. Manganese is released by aluminosilicate weathering, Ni and Co by pyrrhotite [Fe1−xS] oxidation, Zn and Cd by sphalerite oxidation, and Cu by chalcopyrite [CuFeS2] oxidation. No dissolved metals appear to have discrete secondary mineral controls. Changes in SO4, pH and metal concentrations indicate sulfide oxidation is occurring and effluent concentrations are influenced by ambient temperatures and, possibly, increasing flow path lengths that transport reaction products from previously unflushed waste rock. 相似文献
2.
Three large-scale instrumented waste rock piles were constructed at the Diavik Diamond Mine in the Northwest Territories, Canada. These experimental waste rock piles (test piles) are 15 m high and are part of an integrated field and laboratory research program to characterize and compare low-sulfide waste rock and drainage at various scales. During test pile construction, samples of the <50 mm fraction of waste rock were collected from two types of waste rock that are segregated during mining operations based on S content. The samples were analyzed for S content and particle size distribution. One test pile contained waste rock with an average of 0.035 wt.% S in the <50 mm fraction, within the operational S target of <0.04 wt.% S for the lower S waste rock type. The second test pile contained waste rock with an average of 0.053 wt.% S in the <50 mm fraction, lower than the operational S target of >0.08 wt.% S for the higher S waste rock type. The third test pile has a low permeability till layer and a low sulfide waste rock thermal layer covering a core of waste rock with average 0.082 wt.% S in the <50 mm fraction, which is within the operational S target of >0.08 wt.% S for the higher S waste rock. Particle size distributions for the lower and higher S waste rock are similar, but the higher S waste rock has a higher proportion of fine-grained particles. Sulfur determinations for discrete particle sizes of the <50 mm fraction illustrate higher S concentrations in smaller particles for both the lower S waste rock and the higher S waste rock. Similarly, S concentrations calculated for the >10 m scale, from composite blast hole cuttings, are lower than those calculated for the <50 mm scale. Acid–base accounting using standard methods and site-specific mineralogical information was used to calculate the ratio of neutralization potential to acid generating potential. A comparison of calculation approaches to pH and alkalinity data from humidity cell and test pile effluent suggest that ratios are very sensitive to the calculation method. The preferred calculation method was selected by comparing calculation results to pH and alkalinity data from humidity cell effluent collected over 95 weeks and test pile effluent collected over five field seasons. The preferred acid–base accounting values were obtained by calculating the average neutralization potential divided by the average acid potential of a sample set. This approach indicates that waste rock with >0.05 wt.% S is of uncertain acid-generating potential and effluent data indicate this waste rock generates acidic effluent; whereas lower S waste rock does not produce acidic effluent, consistent with the acid–base accounting predictions. 相似文献
3.
Arsenic (As) mobilization and contamination of groundwater affects millions of people worldwide. Progress in developing effective in-situ remediation schemes requires the incorporation of data from laboratory experiments and field samples into calibrated geochemical models.In an oxidizing aquifer where leaching of high pH industrial waste from unlined surface impoundments led to mobilization of naturally occurring As up to 2 mg L−1, sequential extractions of solid phase As as well as, batch sediment microcosm experiments were conducted to understand As partitioning and solid-phase sorptive and buffering capacity. These data were combined with field data to create a series of geochemical models of the system with modeling programs PHREEQC and FITEQL. Different surface complexation modeling approaches, including component additivity (CA), generalized composite (GC), and a hybrid method were developed, compared and fitted to data from batch acidification experiments to simulate potential remediation scenarios. Several parameters strongly influence the concentration of dissolved As including pH, presence of competing ions (particularly phosphate) and the number of available sorption sites on the aquifer solids. Lowering the pH of groundwater to 7 was found to have a variable, but limited impact (<63%) on decreasing the concentration of dissolved As. The models indicate that in addition to lowering pH, decreasing the concentration of dissolved phosphate and/or increasing the number of available sorption sites could significantly decrease the As solubility to levels below 10 μg L−1. The hybrid and GC modeling results fit the experimental data well (NRMSE<10%) with reasonable effort and can be implemented in further studies for validation. 相似文献
4.
Arsenate and antimonate are water-soluble toxic mining waste species which often occur together and can be sequestered with varying success by a hydrous ferric oxide known as ferrihydrite. The competitive adsorption of arsenate and antimonate to thin films of 6-line ferrihydrite has been investigated using primarily adsorption/desorption kinetics monitored by in situ attenuated total reflectance infrared (ATR-IR) spectroscopy on flowed solutions containing 10−3 and 10−5 mol L−1 of both species at pH 3, 5, and 7. ICP-MS analysis of arsenate and antimonate adsorbed to 6-line ferrihydrite from 10−3 mol L−1 mixtures in batch adsorption experiments at pH 3 and 7 was carried out to calibrate the relative surface concentrations giving rise to the IR spectral absorptions. The kinetic data from 10−3 and 10−5 mol L−1 mixtures showed that at pH 3 antimonate achieved a greater surface concentration than arsenate after 60 min adsorption on 6-line ferrihydrite. However, at pH 7, the adsorbed arsenate surface concentration remained relatively high while that of adsorbed antimonate was much reduced compared with pH 3 conditions. Both species desorbed slowly into pH 3 solution while at pH 7 most adsorbed arsenate showed little desorption and adsorbed antimonate concentration was too low to register its desorption behaviour. The nature of arsenate which is almost irreversibly adsorbed to 6-line ferrihydrite remains to be clarified. 相似文献
5.
Jens Søndergaard Bo Elberling Gert Asmund Claus Gudum Karl Martin Iversen 《Applied Geochemistry》2007
It is well known that oxidation of sulphide-containing coal mine waste has considerable environmental impacts due to generation of acid mine drainage (AMD) containing high dissolved metal concentrations. This study is the first to evaluate seasonal trends in the release of AMD from high arctic coal mine waste rock. Runoff from an abandoned coal mine waste pile in Svalbard (78°N) was studied during the entire 3–4 month period with running water in 2005. Temporal variation in concentrations and fluxes of dissolved elements were quantified based on daily water sampling and used to evaluate weathering processes and estimate element budgets on a daily, seasonal and annual basis. Apart from alkali- and alkaline earth metals; Fe, Al, Mn, Zn and Ni were found to be the most abundant metals in the runoff. Element concentrations were highly correlated and suggest that the processes of sulphide oxidation, ion exchange and silicate weathering occurring within the waste pile were linked throughout the measuring period. Observed pH values varied from 2.8 to 5.2 and SO4 concentrations from 21 to 1463 mg L−1. Manganese and Al concentrations were observed above phytotoxic levels (up to 4 and 23 mg L−1, respectively) and were considered the most critical elements in terms of environmental impact. Throughout the summer a total dissolved quantity of 58 kg Mn, 238 kg Al and 13,700 kg SO4 was released from the pile containing approximately 200,000 m3 of pyritic waste material (<1% FeS2). The highest concentrations of metals, lowest pH values and a very high daily release of H2SO4 (up to twice as high as the following month) were observed during the first week of thaw. This is considered a result of an accumulation of weathering products, generated within the waste pile during winter and released as a pollution-flush during early spring. Similar accumulation/flush sequences were observed later in the summer where rain events following relatively long dry periods caused high daily metal fluxes and on some occasions also elevated dissolved metal concentrations. Despite highly variable weather/climate conditions during the rest of the summer the investigated waste rock pile acted like a relative constant pollution-source during this period. Future investigations regarding the environmental impact of mine waste in the region should include measurements of bioavailable metals in order to provide further details on the seasonal trends in environmental impact. 相似文献
6.
《Applied Geochemistry》2005,20(3):639-659
The oxidation of sulfide minerals from mine wastes results in the release of oxidation products to groundwater and surface water. The abandoned high-sulfide Camp tailings impoundment at Sherridon, Manitoba, wherein the tailings have undergone oxidation for more than 70 a, was investigated by hydrogeological, geochemical, and mineralogical techniques. Mineralogical analysis indicates that the unoxidized tailings contain nearly equal proportions of pyrite and pyrrhotite, which make up to 60 wt% of the total tailings, and which are accompanied by minor amounts of chalcopyrite and sphalerite, and minute amounts of galena and arsenopyrite. Extensive oxidation in the upper 50 cm of the tailings has resulted in extremely high concentrations of dissolved SO4 and metals and As in the tailings pore water (pH < 1, 129,000 mg L−1 Fe, 280,000 mg L−1 SO4, 55,000 mg L−1 Zn, 7200 mg L−1 Al, 1600 mg L−1 Cu, 260 mg L−1 Mn, 110 mg L−1 Co, 97 mg L−1 Cd, 40 mg L−1 As, 15 mg L−1 Ni, 8 mg L−1 Pb, and 3 mg L−1 Cr). The acid released from sulfide oxidation has been extensive enough to deplete carbonate minerals to 6 m depth and to partly deplete Al-silicate minerals to a 1 m depth. Below 1 m, sulfide oxidation has resulted in the formation of a continuous hardpan layer that is >1 m thick. Geochemical modeling and mineralogical analysis indicate that the hardpan layer consists of secondary melanterite, rozenite, gypsum, jarosite, and goethite. The minerals indicated mainly control the dissolved concentrations of SO4, Fe, Ca and K. The highest concentrations of dissolved metals are observed directly above and within the massive hardpan layer. Near the water table at a depth of 4 m, most metals and SO4 sharply decline in concentration. Although dissolved concentrations of metals and SO4 decrease below the water table, these concentrations remain elevated throughout the tailings, with up to 60,600 mg L−1 Fe and 91,600 mg L−1 SO4 observed in the deeper groundwater. During precipitation events, surface seeps develop along the flanks of the impoundment and discharge pore water with a geochemical composition that is similar to the composition of water directly above the hardpan. These results suggest that shallow lateral flow of water from a transient perched water table is resulting in higher contaminant loadings than would be predicted if it were assumed that discharge is derived solely from the deeper primary water table. The abundance of residual sulfide minerals, the depletion of aluminosilicate minerals in the upper meter of the tailings and the presence of a significant mass of residual sulfide minerals in this zone after 70 a of oxidation suggest that sulfide oxidation will continue to release acid, metals, and SO4 to the environment for decades to centuries. 相似文献
7.
Temporal changes of As concentration in surface waters were observed in some areas of the Czech Republic. Mobilized As originates from past atmospheric deposition. To understand the factors influencing As aqueous concentration and mobility the chemistry and runoff generation of a number of brooks, springs and rivers in the central part of the Elbe River catchment, Czech Republic, were monitored. Seasonal variations of As (from 0.5 to 10.5 μg L−1), Fe (from 0.05 to 3.9 mg L−1) and DOC (dissolved organic C – from 1.2 to 17.5 mg L−1) were observed in monitored stream waters with maximum values of As and Fe in the summer months at pH values 7.6–7.8. The concentration of As in particles with a diameter < 60 μm correlates with the Fe concentration. There is no correlation between Fe and As in filtered samples (<0.45 μm). The As concentration in stream water colloids depends on an increase in DOC concentration and a decrease in ionic strength. The DOC stabilizes As in solution and reduces its re-adsorption on Fe colloids and consequently As concentration in the stream increases. 相似文献
8.
《Applied Geochemistry》2004,19(8):1255-1293
In order to investigate the mechanism of As release to anoxic ground water in alluvial aquifers, the authors sampled ground waters from 3 piezometer nests, 79 shallow (<45 m) wells, and 6 deep (>80 m) wells, in an area 750 m by 450 m, just north of Barasat, near Kolkata (Calcutta), in southern West Bengal. High concentrations of As (200–1180 μg L−1) are accompanied by high concentrations of Fe (3–13.7 mg L−1) and PO4 (1–6.5 mg L−1). Ground water that is rich in Mn (1–5.3 mg L−1) contains <50 μg L−1 of As. The composition of shallow ground water varies at the 100-m scale laterally and the metre-scale vertically, with vertical gradients in As concentration reaching 200 μg L−1 m−1. The As is supplied by reductive dissolution of FeOOH and release of the sorbed As to solution. The process is driven by natural organic matter in peaty strata both within the aquifer sands and in the overlying confining unit. In well waters, thermo-tolerant coliforms, a proxy for faecal contamination, are not present in high numbers (<10 cfu/100 ml in 85% of wells) showing that faecally-derived organic matter does not enter the aquifer, does not drive reduction of FeOOH, and so does not release As to ground water.Arsenic concentrations are high (≫50 μg L−1) where reduction of FeOOH is complete and its entire load of sorbed As is released to solution, at which point the aquifer sediments become grey in colour as FeOOH vanishes. Where reduction is incomplete, the sediments are brown in colour and resorption of As to residual FeOOH keeps As concentrations below 10 μg L−1 in the presence of dissolved Fe. Sorbed As released by reduction of Mn oxides does not increase As in ground water because the As resorbs to FeOOH. High concentrations of As are common in alluvial aquifers of the Bengal Basin arise because Himalayan erosion supplies immature sediments, with low surface-loadings of FeOOH on mineral grains, to a depositional environment that is rich in organic mater so that complete reduction of FeOOH is common. 相似文献
9.
《Applied Geochemistry》2000,15(9):1383-1397
Water pollution arising from base metal sulphide mines is problematic in many countries, yet the hydrogeology of the subsurface contaminant sources is rarely well-characterized. Drainage water pumped from an active F–Pb mine in northern England has unusual chemistry (alkaline with up to 40 mg.l−1 Zn) which profoundly impacts the ecology of the receiving watercourse. Detailed in-mine surveys of the quantity and quality of all ground water inflows to the mine were made. These revealed major, temporally persistent heterogeneities in ground water quality, with three broad types of water identified as being associated with distinct hydrostratigraphic units. Type I waters (associated with the Firestone Sill aquifer) are cool (<10°C), Ca–HCO3–SO4 waters, moderately mineralized (specific electrical conductance (SEC)≤410 μS.cm−1) with <4 mg.l−1 Zn. Type II waters (associated with the Great Limestone aquifer) are warmer (≈15°C), of Ca–SO4 facies, highly mineralized (SEC≤1500 μS.cm−1) with ≤40 mg.l−1 Zn. Type III waters (in the deepest workings) are tepid (>18°C), of Ca–HCO3–SO4 facies, intermediately mineralized (SEC≤900 μS.cm−1) with ≤13 mg.l−1 Zn, and with significant Fe (≤12 mg.l−1) and Pb (≤8 mg/l). Monotonic increases in temperature and Cl− concentration with depth contrast with peaks in total mineralization, SO4 and Zn at medium depth (in Type II waters). Sulphate, Pb and Zn are apparently sourced via oxidation of galena and sphalerite, which would release each metal in stoichiometric equality with SO4. However, molal SO4 concentrations typically exceed those of Pb and Zn by 2–3 orders of magnitude, which mineral equilibria suggest is due to precipitation of carbonate “sinks” for these metals. Contaminant loading budgets demonstrate that, although Type II waters amount to only 25% of the total ground water inflow to the mine, they account for almost 60% of the total Zn loading. This observation has important management implications for both the operational and post-abandonment phases of the mine life cycle. 相似文献
10.
The physicochemical processes that affect acid mine drainage (AMD) in unsaturated waste rock piles and the capabilities of small-scale laboratory experiments to predict AMD from waste rock are not well understood. An integrated laboratory and field study to measure and compare low sulfide waste rock and drainage characteristics at various scales has been initiated. This paper describes the design, construction and instrumentation of three field-scale experimental waste rock piles (test piles), and six active zone lysimeters at the Diavik diamond mine in the Northwest Territories, Canada. The test piles are comprised of granitic and sulfide-bearing metasedimentary waste rock excavated during open pit mining operations. One test pile contains waste rock with a target S content of <0.04 wt.% S; the second test pile contains waste rock with a target S content of >0.08 wt.% S; and the third test pile contains the higher sulfide waste rock (>0.08 wt.% S) and was re-sloped and capped with a low permeability till layer and a low sulfide waste rock cover. The first two test piles are approximately 15 m high with bases of 50 m by 60 m, and the re-sloped test pile has a larger base of 80 m by 125 m. Instrumentation was selected to measure matrix flow, geochemistry of pore water and drainage, gas-phase O2 concentration, temperature evolution, microbiological populations, waste rock permeability to air, and thermal conductivity, as well as to resolve mass and flow balances. Instrument locations were selected to characterize coupled physicochemical processes at multiple scales and the evolution of those processes over time. Instruments were installed at a density such that the number of instruments that survived construction (40% to >80% by instrument type) was sufficient to allow adequate characterization of the physicochemical processes occurring at various scales in the test piles. 相似文献
11.
Continuous monitoring of a 15 m high heavily instrumented experimental waste rock pile (0.053 wt.% S) since 2006 at the Diavik diamond mine in northern Canada provided a unique opportunity to study the evolution of fresh run-of-mine waste rock as it evolved over annual freeze–thaw cycles. Samples were collected from soil water solution samplers to measure pore water properties, from twelve 4 to 16 m2 basal collection lysimeters to measure basal leachate properties in the region underlying the crest of the pile (the core), and from basal drains to measure aggregate total pile leachate properties. By 2012, monitoring of pore water geochemistry within the core structure of the test pile revealed an apparent steady state with respect to weathering geochemistry, represented by (i) a flush of pre-existing blasting residuals and applied tracers, (ii) declining pH, (iii) a stepwise progression and subsequent equilibrium with acid-neutralizing phases (depletion of available carbonates; equilibrium with respect to aluminum hydroxide phases and subsequent iron (III) hydroxide phases), and (iv) concordant release of SO4, major cations (Ca, Mg, K, Na, Si), and trace metals (Al, Fe, Ni, Co, Cu, Zn). Distinct, high concentration ‘spring flushes’, characteristic of drainage in northern environments and primarily explained by a combination of fluid residence time and the build-up of oxidation products over the winter, were released from core drainage each season. Following the initial flush, the concentration of all dissolved constituents steadily declined, with distinct minimums prior to freeze-up. The opposite trend was observed in the cumulative pile drainage, in which early season leachate dominated by snowmelt and batter flow had low concentrations and late season leachate dominated by contributions from the core of the pile (indicated by season end merging of core and cumulative drainage geochemistry) had higher concentrations. Northern waste rock pile drainage geochemistry is strongly influenced by freeze–thaw cycling and varying core and batter subsystem contributions to total drainage. A comprehensive understanding of thermal cycling in waste rock piles is an important component of temporal predictions of drainage water composition based on up-scaling or reactive transport modeling. 相似文献
12.
Riverbank sediment cores and pore waters, shallow well waters, seepage waters and river waters were collected along the Meghna Riverbank in Gazaria Upazila, Bangladesh in Jan. 2006 and Oct.–Nov. 2007 to investigate hydrogeochemical processes controlling the fate of groundwater As during discharge. Redox transition zones from suboxic (0–2 m depth) to reducing (2–5 m depth) then suboxic conditions (5–7 m depth) exist at sites with sandy surficial deposits, as evidenced by depth profiles of pore water (n = 7) and sediment (n = 11; diffuse reflectance, Fe(III)/Fe ratios and Fe(III) concentrations). The sediment As enrichment zone (up to ∼700 mg kg−1) is associated with the suboxic zones mostly between 0 and 2 m depth and less frequently between 5 and 7 m depth. The As enriched zones consist of several 5–10 cm-thick dispersed layers and span a length of ∼5–15 m horizontally from the river shore. Depth profiles of riverbank pore water deployed along a 32 m transect perpendicular to the river shore show elevated levels of dissolved Fe (11.6 ± 11.7 mg L−1) and As (118 ± 91 μg L−1, mostly as arsenite) between 2 and 5 m depth, but lower concentrations between 0 and 2 m depth (0.13 ± 0.19 mg L−1 Fe, 1 ± 1 μg L−1 As) and between 5 and 6 m depth (1.14 ± 0.45 mg L−1 Fe, 28 ± 17 μg L−1 As). Because it would take more than a few hundred years of steady groundwater discharge (∼10 m yr−1) to accumulate hundreds of mg kg−1 of As in the riverbank sediment, it is concluded that groundwater As must have been naturally elevated prior to anthropogenic pumping of the aquifer since the 1970s. Not only does this lend unequivocal support to the argument that As occurrence in the Ganges-Brahmaputra-Meghna Delta groundwater is of geogenic origin, it also calls attention to the fate of this As enriched sediment as it may recycle As into the aquifer. 相似文献
13.
《Comptes Rendus Geoscience》2015,347(2):77-83
Bacterial activity in the near-field environment of radioactive waste disposal facilities in deep argillaceous rocks is currently under investigation. Bacterial development could be enhanced by the availability of low-molecular-weight organic acids (LMWOA) dissolved in the pore water of clayey rocks. This study firstly aimed at isolating and characterizing the LMWOA of the Toarcian argillite from the Tournemire Underground Research Laboratory (France, Aveyron). It also aimed at assessing the disturbing effects that could be induced by a disposal facility on the type and release of LMWOA (exposure to oxygen, alkaline pH, temperature increase). Under the experimental conditions investigated at 60 °C, the mean dissolved organic carbon (DOC) is about 15 mg L−1 with a LMWOA proportion of 35 %. The main LMWOA are composed of formate, fumarate, propionate, acetate, and lactate. DOC is mainly influenced by both temperature and pH increases, whereas the LMWOA type nature and release are more specifically affected by the exposure to oxygen. 相似文献
14.
《Applied Geochemistry》2006,21(8):1347-1361
The relationships between factors that control subsurface flow and the timing, duration, and intensity of acidity generation and leaching of metals from waste-rock dumps are investigated. A 12 m high waste-rock pile that had been constructed in 1994 at Key Lake, Saskatchewan, Canada was disassembled, sampled and characterized in 2000. Physical properties that control water flow were characterized by measuring soil–water suction, volumetric water content, and the grain-size distribution at 60 randomized sites within the pile. Grain-size distribution was also measured at an additional 20 grid locations within the pile. Paste pH, pore-water geochemistry, mineralogy, and water-soluble extractions were used to investigate geochemical processes and sulfide oxidation at each of the 20 grid locations. A field-based soil–water characteristic curve could not be developed from the spatially variable and hysteretic field data; consequently, the grain-size distribution was used as a relative measure of subsurface flow and of the tendency to contain water under unsaturated conditions. The geochemical characterization demonstrated that marcasite underwent preferential weathering relative to pyrite and chalcopyrite, that dolomite was the main buffering carbonate mineral, and that gypsum, jarosite, and Fe oxyhydroxides were the main secondary (supergene) minerals. The pore waters contained up to 78,000 mg L−1 SO4, 690 mg L−1 Ni and 1400 mg L−1 U (800, 11.7 and 6 mM, respectively), suggesting that significant weathering had occurred. The pore water chemistry varied considerably between sampling sites. However, neither a correlation of pore-water chemistry with grain-size distribution nor a spatial relationship within the sampled grid was discernible. 相似文献
15.
《Applied Geochemistry》2000,15(4):425-438
The dissolution of silica and diffusion of reactive dissolved Si in the porewaters of river sediments are investigated using sediments of different physical and chemical properties. Three sediments are considered: (a) from sectioned cores taken from a river-bed, (b) fine organic-rich surface sediment (<5 cm depth) installed in a fluvarium channel and, (c) coarse river sediment of low organic matter content also installed in a fluvarium channel. Dissolution rates of silica are measured at 10°C using batches of suspended material. The derived dissolution rate constants show large differences between the sediments. The river bed-sediment cores had vertical concentration profiles of dissolved Si that are consistent with the diffusion and dissolution of biogenic silica. Experiments in a fluvarium channel enabled Si fluxes to be calculated from a mass-balance of the overlying solution. The results are consistent with the attainment of a steady-state concentration profile of dissolved Si in the sediment. There are no discernible effects of water velocity over the sediment between 5 and 11 cm s−1. However, at 20 cm s−1, the flux increases as a result of either entrainment of fine particles at the surface or advective effects in the surface sediment. A fluvarium experiment with the fine sediment (<125 μm) over 61 days, produced a concentration profile with the highest concentration of 1025 μmol dm−3 at a depth of 4–5 cm in the sediment. A FORTRAN program is used to model the results of the increase in dissolved Si in the overlying water and development of a concentration profile in the porewater. This leads to a sediment diffusion coefficient of 1.21×10−9 m2 s−1 at 8.8°C at the beginning of the experiment and rate constant k=13.1×10−7 s−1 at pH=7.82 and average temperature of 7.6°C for the entire experiment. Fluxes measured at the sediment–surface interface and calculated assuming steady-state profiles had developed are typically 0.01–0.04 μmol m−2 (of river bed) s−1. The approach enables the efflux of dissolved Si from bottom-sediments to be estimated from dissolution rates measured using suspensions of bed-sediment. 相似文献
16.
Dissolved and particulate Zn and Ni concentrations were determined at 76 locations along the Yangtze River basin from the headwaters to the estuary during flood and dry seasons. Spatial and temporal variations of Zn and Ni were investigated and six major source zones were identified. The Three Gorges Dam (TGD) blocked most of the suspended loads and extremely low concentration of Zn and Ni were observed downstream of the dam. Dissolved (ranging from 0.062 to 8.0 μg L−1) and particulate (ranging from 12 to 110 mg kg−1) Ni showed similar levels of concentrations during flood and dry seasons, whereas dissolved (ranging from 0.43 to 49 μg L−1) and particulate (ranging from 54 to 1100 mg kg−1) Zn were slightly and much lower in the flood season than dry season, respectively. This was attributed to the increased water discharge during the flood season causing a dilution effect and sediment resuspension. In the flood season, average concentrations of Zn and Ni were higher in the main channel than in tributaries, due to soil erosion and mining activities providing the dominant inputs. The situation was opposite in the dry season, attributed to the contribution of municipal sewage, industrial activities, and waste disposal. During the flood season, dissolved Zn and Ni concentrations were negatively correlated with pH. Water and suspended particulate matter (SPM) from the upper reaches, middle reaches, and lower reaches of the Yangtze River were characterized by their Zn and Ni concentrations. The Panzhihua, Nanling and Tongling mining areas were considered as the most important source zones of particulate Zn and Ni. The Chongqing region, Wuhan region and the Yangtze River Delta provided most of the dissolved Zn and Ni inputs into the river. Annual net flux of Zn (10–72 × 105 kg a−1) and Ni (5.0–19 × 105 kg a−1) in each source zone were estimated according to their respective influent and effluent fluxes. Contributions of the source zones to Zn and Ni transport decreased from the upper reaches to the lower reaches. 相似文献
17.
《Applied Geochemistry》2006,21(10):1760-1780
Sulfide-rich mine tailings in Adak that are exposed to weathering cause acid mine drainage characterized by low pH (2–4) and high SO4 (up to 800 mg L−1). Surface water, sediment and soil samples collected in this study contain higher concentrations of As, Cu, Fe and Zn, compared to the target and/or intervention limits set by international regulatory agencies. In particular, high As concentrations in water (up to 2900 μg L−1) and sediment (up to 900 mg kg−1) are of concern. There is large variability in trace element concentrations, implying that both physical (grain size) and chemical factors (pH, secondary phases as sulfides, Al-oxides or clay minerals) play an important role in their distribution. The low pH keeps the trace elements dissolved, and they are transported farther downstream. Trace element partition coefficients are low (log Kd = 0.3–4.3), and saturation indices calculated with PHREEQC are <0 for common oxide and sulfidic minerals. The sediment and soil samples indicate an enhanced pollution index (up to 17), and high enrichment factors for trace elements (As up to 38,300; Zn up to 800). Finally, leaves collected from different plant types indicate bioaccumulation of several elements (As, Al, Cu, Fe and Zn). However, some of the plants growing in this area (e.g., Salix, Equisétum) are generally resistant to metal toxicity, and hence, liming and phytoremediation could be considered as potential on-site remediation methods. 相似文献
18.
19.
《Journal of Geochemical Exploration》2005,85(3):119-137
This study reports on the seepage of metals, metalloids and radionuclides from the Mary Kathleen uranium mill tailings repository. Since rehabilitation in the 1980s, the capped tailings have developed a stratified hydrochemistry, with acid (pH 3.7), saline, metal-rich (Fe, Mn, Ni, U ± As, Pb, Zn), oxygenated (1.05 mg L−1 DO), radioactive waters in the upper tailings pile and near-neutral pH (pH 7.57), metal-poor, reduced (0.08 mg L−1 DO) waters at depth. Seepage (∼0.5 L s−1) of acid (pH 5.5), metal-rich (Fe, Mn ± Ni, U, Zn), radioactive (U-235, U-238, Ra-226, Ra-228, Ac-227) waters occurs from the base of the tailings dam retaining wall into the former evaporation pond and local drainage system. Oxygenation of the seepage waters causes the precipitation of Fe and coprecipitation and adsorption of other metals (U, Y), metalloids (As), rare earth elements (Ce, La) and radionuclides (U-235, U-238). By contrast, alkalis and alkaline–earth elements (Ca, K, Mg, Na, Sr), Mn, sulfate and to some degree metals (U, Zn, Ni), rare earth elements (Ce, La) and radionuclides (U-235, U-238, Ra-226, Ra-228) remain in solution until pH neutralisation and evaporation lead to their precipitation in efflorescences and sulfate-rich evaporative sediments. While the release of contaminant loads from the waste repository through seepage is insignificant (e.g. ∼5 kg of U per year), surface waters downstream of the tailings impoundment possess TDS, U and SO4 concentrations that exceed Australian water quality guideline values in livestock drinking water. Thus, in areas with a semi-arid climate, even insignificant load releases of contaminants from capped tailings repositories can still cause the deterioration of water quality in ephemeral creek systems. 相似文献
20.
In a high-level radioactive waste (HLW) repository, pH has an impact on the solubility, migration, and adsorption of radionuclides. Thus, understanding the effects of pH on the diffusion of radionuclides is essential for long-term disposal of HLW. In this work, the diffusion behaviors of Re(VII) and Se(IV) in compacted Gaomiaozi (GMZ) bentonite at different pH have been investigated by a through-diffusion method. The effective diffusion coefficient, i.e., De values of Re(VII) and Se(IV) were in the range of (1.0–2.4) × 10−11 m2/s at pH 3.0–10.0 and (0.38–2.3) × 10−11 m2/s at pH 3.0–9.0. In the case of Re(VII), the De values remained almost unchanged probably because ReO4− was the dominant species in the pH range of 3.0–10.0. In the case of Se(IV), whose predominant species were HSeO3− at pH < 9.0 and SeO32− at pH ≥ 9.0, the De values decreased by a factor of 3–6 at pH 9.0, i.e., De (pH < 9.0)/De (pH 9.0) ≈ 3–6, implying that the species with a higher valence state had a stronger anion exclusion effect. The decrease in De values can be explained by the diffusion species of Se(IV). Additionally, the rock capacity factor α decreased with the increase of pH. HSeO3− was absorbed on GMZ bentonite with distribution coefficient Kd values in the range of (1.0–2.5) × 10−4 m3/kg at pH ≤ 8.0, whereas SeO32− was negligibly sorbed at pH > 8.0. 相似文献