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1.
The common serpentine–diopside matrix assemblage in volcaniclastic kimberlite (VK) at the Venetia Mine, South Africa is ascribed to a secondary origin, because of post‐emplacement serpentinization and associated hydrothermal metamorphism. Volcaniclastic deposits with 20–30% porosity infill kimberlite pipes in the waning stages of kimberlite eruptions. Olivine macrocrysts are typically rimmed by talc and are pseudomorphed by lizardite, with minor magnetite. The fine matrix consists of mixtures of lizardite, chlorite, smectite, brucite, calcite, titanite and andradite, an assemblage which either pseudomorphed microcrysts or in‐filled voids. Locally we recognize microcryst pseudomorphs rich in sub‐microscopic mixtures of lizardite with smectite, and other microcryst pseudomorphs and void‐filling matrix rich in chlorite and lizardite. Interstitial lizardite and associated phyllosilicates (brucite, smectite and chlorite) crystallized progressively from meteoric or hydrothermally derived pore waters, and Si4+ and Mg2+ released into the fluid phase during serpentinization of olivine macrocrysts. Radial‐fibrous fringes of diopside microlites around crystals display void‐filling textures because of unrestricted growth into pore spaces. Secondary diopside is attributed to Si4+, Mg2+ and Ca2+ cations released into the fluid phase by interaction with olivine, calcite and plagioclase in siliceous xenoliths. The paucity of primary, fine‐grained groundmass phases resistant to alteration, for example, perovskite and spinel, precludes an origin for the intergrain matrix as altered interstitial ash, glass or a late‐stage kimberlite melt. Isovolumetric replacement of olivine results in a volume increase of 60% so that pore spaces in the original deposit can be easily filled up with serpentine. The source of Al3+ to form chlorite and smectite is attributed to alteration of plagioclase in xenoliths which comprise 20–30 vol.% of the deposit. Titanite, hydro‐andradite and second‐generation diopside precipitate as hydrothermal minerals from calcium‐bearing serpentinizing fluids in replacement reactions and as void‐filling minerals. Consideration of mineral equilibria in the CaO‐MgO‐SiO2‐H2O‐CO2 system constrains the common matrix assemblage of lizardite and diopside in XCO2)–T space. At 300 bar, the assemblage is stable only at temperatures below 370 °C and XCO2 < 0.01. This upper limit on temperature is well below the plausible solidus of ultrabasic magmas. Furthermore, the requirement of trace CO2 in the fluid phase implies a post‐emplacement external source rather than ‘autometamorphism’ from kimberlite‐derived fluids, because of high PCO2 commonly inferred for kimberlite magmas.  相似文献   

2.
Understanding mechanisms and kinetics of mineral carbonation reactions relevant to sequestering carbon dioxide as a supercritical fluid (scCO2) in geologic formations is crucial to accurately predicting long-term storage risks. Most attention so far has been focused on reactions occurring between silicate minerals and rocks in the aqueous dominated CO2-bearing fluid. However, water-bearing scCO2 also comprises a reactive fluid, and in this situation mineral carbonation mechanisms are poorly understood. Using in situ high-pressure X-ray diffraction, the carbonation of brucite [Mg(OH)2] in wet scCO2 was examined at pressure (82 bar) as a function of water concentration and temperature (50 and 75 °C). Exposing brucite to anhydrous scCO2 at either temperature resulted in little or no detectable reaction over three days. However, addition of trace amounts of water resulted in partial carbonation of brucite into nesquehonite [MgCO3·3H2O] within a few hours at 50 °C. By increasing water content to well above the saturation level of the scCO2, complete conversion of brucite into nesquehonite was observed. Tests conducted at 75 °C resulted in the conversion of brucite into magnesite [MgCO3] instead, apparently through an intermediate nesquehonite step. Raman spectroscopy applied to brucite reacted with 18O-labeled water in scCO2 show it was incorporated into carbonate at a relatively high concentration. This supports a carbonation mechanism with at least one step involving a direct reaction between the mineral and water molecules without mediation by a condensed aqueous layer.  相似文献   

3.

The early Cambrian to late Neoproterozoic Kelvin kimberlite pipe is located in the southeast of the Archean Slave Craton in northern Canada, eight km northeast of the Gahcho Kué diamond mine. Kelvin was first discovered in 2000 by De Beers Canada. Subsequent exploration undertaken by Kennady Diamonds Inc. between 2012 and 2016 resulted in the discovery of significant thicknesses of volcaniclastic kimberlite that had not previously been observed. Through extensive delineation drilling Kelvin has been shown to present an atypical, steep-sided inclined L-shaped pipe-like morphology with an overall dip of 15 to 20°. With a surface expression of only 0.08 ha Kelvin dips towards the northwest before turning north. The body (which remains open at depth) has been constrained to a current overall strike length of 700 m with varying vertical thickness (70 to 200 m) and width (30 to 70 m). Detailed core logging, petrography and microdiamond analysis have shown that the pipe infill comprises several phases of sub-horizontally oriented kimberlite (KIMB1, KIMB2, KIMB3, KIMB4, KIMB7 and KIMB8) resulting from multiple emplacement events. The pipe infill is dominated by Kimberley-type pyroclastic kimberlite or “KPK”, historically referred to as tuffisitic kimberlite breccia or “TKB”, with less common hypabyssal kimberlite (HK) and minor units with textures transitional between these end-members. An extensive HK sheet complex surrounds the pipe. The emplacement of Kelvin is believed to have been initiated by intrusion of this early sheet system. The main pipe-forming event and formation of the dominant KPK pipe infill, KIMB3, was followed by late stage emplacement of additional minor KPK and a hypabyssal to transitional-textured phase along the upper contact of the pipe, cross-cutting the underlying KIMB3. Rb-Sr age dating of phlogopite from a late stage phase has established model ages of 531 ± 8 Ma and 546 ± 8 Ma. Texturally and mineralogically, the Kelvin kimberlite is similar to other KPK systems such as the Gahcho Kué kimberlites and many southern African kimberlites; however, the external morphology, specifically the sub-horizontal inclination of the pipe, is unique. The morphology of Kelvin and the other kimberlites in the Kelvin-Faraday cluster defines a new type of exploration target, one that is likely not unique to the Kennady North Project area. Extensive evaluation work by Kennady Diamonds Inc. has resulted in definition of a maiden Indicated Mineral Resource for Kelvin of 8.5 million tonnes (Mt) of kimberlite at an average grade of 1.6 carats per tonne (cpt) with an average diamond value of US$ 63 per carat (ct).

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4.
《Applied Geochemistry》2006,21(9):1522-1538
Factors controlling the chemical composition of water interacting with finely-crushed kimberlite have been investigated by sampling pore waters from processed kimberlite fines stored in a containment facility. Discharge water from the diamond recovery plant and surface water from the containment facility, which acts as plant intake water, were also sampled. All waters sampled are pH-neutral, enriched in SO4, Mg, Ca, and K, and low in Fe. Pore-water samples, representing the most concentrated waters, are characterized by the highest SO4 (up to 4080 mg l−1), Mg (up to 870 mg l−1), and Ca (up to 473 mg l−1). The water discharged from the processing plant has higher concentrations of all major dissolved constituents than the intake water. The dominant minerals present in the processed fines and the kimberlite ore are serpentine and olivine, with small amounts of Ca sulphate and Fe sulphide restricted to mud xenoclasts. Reaction and inverse modeling suggest that much of the water-rock interaction takes place within the plant and involves the dissolution of chrysotile and Ca sulphate, and precipitation of silica and Mg carbonate. Evapoconcentration also appears to be a significant process affecting pore water composition in the containment facility. The reaction proposed to be occurring during ore processing involves the dissolution of CO2(g) and may represent an opportunity to sequester atmospheric CO2 through mineral carbonation.  相似文献   

5.
Constraining the composition of primitive kimberlite magma is not trivial. This study reconstructs a kimberlite melt composition using vesicular, quenched kimberlite found at the contact of a thin hypabyssal dyke. We examined the 4 mm selvage of the dyke where the most elongate shapes of the smallest calcite laths suggest the strongest undercooling. The analyzed bulk compositions of several 0.09-1.1 mm2 areas of the kimberlite free from macrocrysts were considered to be representative of the melt. The bulk analyses conducted with a new “chemical point-counting” technique were supplemented by modal estimates, studies of mineral compositions, and FTIR analysis of olivine phenocrysts. The melt was estimated to contain 26-29.5 wt% SiO2, ∼7 wt% of FeOT, 25.7-28.7 wt% MgO, 11.3-15 wt% CaO, 8.3-11.3 wt% CO2, and 7.6-9.4 wt% H2O. Like many other estimates of primitive kimberlite magma, the melt is too magnesian (Mg# = 0.87) to be in equilibrium with the mantle and thus cannot be primary. The observed dyke contact and the chemistry of the melt implies it is highly fluid (η = 101-103 Pa s at 1100-1000 °C) and depolymerized (NBO/T = 2.3-3.2), but entrains with 40-50% of olivine crystals increasing its viscosity. The olivine phenocrysts contain 190-350 ppm of water suggesting crystallization from a low SiO2 magma (aSiO2 below the olivine-orthopyroxene equilibrium) at 30-50 kb. Crystallization continued until the final emplacement at depths of few hundred meters which led to progressively more Ca- and CO2-rich residual liquids. The melt crystallised phlogopite (6-10%), monticellite (replaced by serpentine, ∼10%), calcite rich in Sr, Mg and Fe (19-27%), serpentine (29-31%) and minor amounts of apatite, ulvöspinel-magnetite, picroilmenite and perovskite. The observed content of H2O can be fully dissolved in the primitive melt at pressures greater than 0.8-1.2 kbar, whereas the amount of primary CO2 in the kimberlite exceeds CO2 soluble in the primitive kimberlite melt. A mechanism for retaining CO2 in the melt may require a separate fluid phase accompanying kimberlite ascent and later dissolution in residual carbonatitic melt. Deep fragmentation of the melt as a result of volatile supersaturation is not inevitable if kimberlite magma has an opportunity to evolve.  相似文献   

6.
Clay-rich mine tailings from phosphate mine operations in Florida are a major environmental and economic problem. Options for reclamation and restoration for these tailings are very limited and are fundamentally restricted by poor physical properties such as low mechanical strength, low hydraulic conductivity, and heavy metal content. The major control on these bulk physical properties is the mineralogy of the materials. Eight continuous push borings were obtained to investigate stratigraphy, mineralogy, aspects of geochemistry, and bulk properties of a deposit of clay-rich mine tailings from a phosphate mine near Bartow, Florida that ceased operations in the early 1970s. Stratigraphy is dominated by laminated clay-rich sediment with minor units of silt and sand. An intact kaolinite liner occurs near the impoundment walls and the impoundment floor has approximately 4 m of relief. Moisture content varies from 4.35 to 57.40 wt% and organic content varies from 0.41 to 9.53 wt%. Bulk XRF investigation indicates that the P2O5 concentrations vary from approximately 4 to 21 wt%. A very strong correlation (r 2 = 0.92) between CaO and P2O5 indicates that apatite is a major control on the phosphate. The strong correlation (r 2 = 0.77) of Al2O3 and TiO2 suggests that the source materials for this deposit are comparatively uniform. A number of heavy metal elements and trace elements occur. Cr, V, Ni, Cu are interpreted to be in phosphate minerals, largely apatite. Sr and Pb are interpreted to be in both phyllosilicates and phosphate minerals. Two populations of apatite were observed in the clay-sized fraction, one that was Fe and Si- bearing and another that was only Si-bearing. Fe-bearing apatite had Fe2O3 contents that varied from 0.38 to 5.32 wt% and SiO2 contents that varied from 0.90 to 3.32 wt%. The other apatite population had a wider range of SiO2 contents that varied from 0.77 to 8.80 wt%. TEM imaging shows that apatite grains are dominantly single crystals with lesser amounts of aggregates. Wavellite commonly occurs as individual or clusters of lath-like crystals and the chemical composition differs from the pure aluminium phosphate end member with average concentrations of components being that of CaO (1.57 wt%), Fe2O3 (1.98 wt%), SiO2 (5.94 wt%). In the clay-sized phosphate minerals investigated no fluorine was found above detection limit (approximately 0.15 wt%), nor was any uranium, radium, heavy metal, or REE element detected. The phyllosilicate mineralogy of the deposit is dominated by smectite (montmorillonite with lesser amounts of nontronite), palygorskite, illite and kaolinite. No systematic variation in the relative proportions of phyllosilicates was observed in the clay deposit. Energy dispersive spectroscopy EDS analysis indicates that chemical compositions of phyllosilicates are somewhat typical but overall are enriched with respect to Fe compared to theoretical end members. The relative enrichment of Fe is interpreted to be a primary sedimentary feature. Ca content in smectite minerals is high and may inhibit stabilization using lime or similar methods. The high percentages of montmorillonite and palygorskite explain the high bulk water contents observed. This investigation provides fundamentally new details regarding clay tailing deposits from closed phosphate mines in central Florida which can be used in restoration and reclamation efforts.  相似文献   

7.
A MgO-based binder developed to simultaneously solidify/stabilize contaminated sediment and store CO2 has been described previously. The objectives of the study presented here were to investigate the kinetics of the carbonation reactions of the binder and the extent to which carbonation occurred and to identify the optimal conditions for using the binder. The carbonation reaction was clearly faster and the degree of carbonation higher at CO2 concentrations of 50 and 100% than in the ambient atmosphere (which contains 0.04% CO2). A modified unreactive core model adequately described the kinetics. The rate constants were 0.0217–0.319 h?1 and were proportional to the degree of carbonation. A high degree of carbonation, 93.8%, was achieved at a CO2 concentration of 100%. The water to sediment ratio strongly affected carbonation, the optimal ratio being around 0.7. The relative humidity did not strongly affect the carbonation performance. The carbonation products were magnesite (MgCO3) and nesquehonite (MgCO3·3H2O). X-ray diffraction analysis showed that brucite (Mg(OH)2) was not present, suggesting that brucite was very quickly transformed into magnesium carbonates, the presence of which was confirmed by thermal gravimetric analysis. The results indicated that, in 7 d, 1 kg of binder could sequester up to 0.507 kg of CO2 in a 100% CO2 atmosphere. The results indicate that the MgO-based binder has great potential to be used to sequester CO2 under accelerated carbonation conditions.  相似文献   

8.
The Cambrian Gahcho Kué kimberlite cluster includes four main pipes that have been emplaced into the Archaean basement granitoids of the Slave Craton. Each of the steep-sided pipes were formed by the intrusion of several distinct phases of kimberlite in which the textures vary from hypabyssal kimberlite (HK) to diatreme-facies tuffisitic kimberlite breccia (TKB). The TKB displays many diagnostic features including abundant unaltered country rock xenoliths, pelletal lapilli, serpentinised olivines and a matrix composed of microlitic phlogopite and serpentine without carbonate. The HK contains common fresh olivine set in a groundmass composed of monticellite, phlogopite, perovskite, serpentine and carbonate. A number of separate phases of kimberlite display a magmatic textural gradation from TKB to HK, which is characterised by a decrease in the proportion of pelletal lapilli and country rock xenoliths and an increase in groundmass crystallinity, proportion of fresh olivine and the degree of xenolith digestion.

The pipe shapes and infills of the Gahcho Kué kimberlites are similar to those of the classic South African pipes, particularly those of the Kimberley area. Similar intrusive magmatic emplacement processes are proposed in which the diatreme-zone results from the degassing, after breakthrough, of the intruding magma column. The transition zones represent ‘frozen’ degassing fronts. The style of emplacement of the Gahcho Kué kimberlites is very different from that of many other pipes in Canada such as at Lac de Gras, Fort à la Corne or Attawapiskat.  相似文献   


9.
The oxidation and subsequent dissolution of sulfide minerals within mine tailings impoundments releases H+, Fe(II), SO4 and trace elements to the tailings pore water. Subsequent pH-buffering and hydrolysis reactions result in the precipitation of secondary phases such as gypsum, goethite and jarosite. In areas of intense precipitation, cemented layers or “hardpans” often form within the shallow tailings. Three cemented layers within pyrrhotite-bearing mine tailings at the Fault Lake, Nickel Rim and East Mine impoundments located near Sudbury, Canada, were examined. The location of the three cemented layers within the tailings stratigraphy varies as does their location relative to the water table. The morphology, mineralogy and chemical composition of the cemented layers also vary between sites. The bulk density within the three cemented layers all showed an increase relative to the surrounding uncemented tailings ranging from 9% to 29%. The porosity of each cemented layer decreased relative to the surrounding uncemented tailings ranging from an 8% to 18% decrease. The cemented layers also showed relative enrichment of total sulfur, carbon and trace elements relative to the surrounding uncemented tailings. Arsenic concentrations showed an enrichment in the cemented layers of up to 132%, Cd up to 99%, Co up to 84%, Cu up to 144%, Ni up to 693% and Zn up to 145% relative to the surrounding uncemented tailings. All the cemented layers studied show an evolution of the secondary phases with time from a gypsum–jarosite-based cement to a goethite-rich cement. The formation of these layers could potentially have a significant effect on the environmental impacts of sulfide-bearing mine waste.  相似文献   

10.
周志强 《地质与勘探》2021,57(5):981-993
青海茫崖石棉矿区超基性岩体是由原岩以纯橄岩、辉橄岩和橄辉岩为主体组成的富镁质超基性岩体,经历自变质和后期多期热液的叠加变质蚀变作用,经蛇纹石化后形成蚀变完全的蛇纹岩岩体,其中部分蛇纹岩又进一步发生滑石化及碳酸盐化蚀变为滑石菱镁片岩、菱镁滑石片岩、滑石片岩和菱镁岩等。本文在野外地质调查基础上,在室内通过镜下岩矿综合鉴定、全岩化学成分分析以及电子探针成分分析等手段进行了岩石化学特征、矿物学特征及其蚀变演化过程研究。结果表明,该变质超基性岩体蛇纹岩主要特征组合矿物为蛇纹石(利蛇纹石、叶蛇纹石、纤蛇纹石)、磁铁矿、菱镁矿、滑石、水镁石、铬铁矿,变余矿物有斜方辉石、单斜辉石和铬铁矿,滑石菱镁片岩类主要组成矿物为菱镁矿、滑石、蛇纹石及磁铁矿,局部可见石英脉。该地区变质超基性岩体较完整地记录了橄榄岩水化、滑石化及碳酸盐化作用过程的各个阶段,超基性岩蚀变演化过程主要有两个作用阶段:(Ⅰ)橄榄石、辉石类矿物的蛇纹石化作用及蛇纹石绿泥石化作用;(Ⅱ)富Ca、CO2流体交代蛇纹石、滑石及水镁石的碳酸盐化作用。蛇纹石化等变质蚀变作用促进了Si、Mg及Fe元素化学活动性,使元素发生富集与迁移,对于次生矿物的形成与演化起到了一定的催化作用。多期不同组成流体热液的交代作用过程,清晰地展示了利蛇纹石、纤蛇纹石和叶蛇纹石的演化序列,以及滑石、水镁石、铬铁矿和磁铁矿的形成过程及标形特征。  相似文献   

11.
Metamorphic assemblages within Karoo basalt xenoliths, found within volcaniclastic kimberlite of the B/K9 pipe, Damtshaa, Botswana, constrain conditions of kimberlite alteration. Bultfonteinite and chlorite partially replace the original augite-plagioclase assemblage, driven by the serpentinisation of the kimberlite creating strong chemical potential gradients for Si and Mg. Hydrogarnet and serpentine replace these earlier metamorphic assemblages as the deposits cool. The bultfonteinite (ideally Ca2SiO2[OH,F]4) and hydrogarnet assemblages require a water-rich fluid containing F, and imply hydrothermal alteration dominated by external fluids rather than autometamorphism from deuteric fluids. Bultfonteinite and hydrogarnet are estimated to form at temperatures of ca. 350–250°C, which are similar to those for serpentinisation. Alteration within the B/K9 kimberlite predominantly occurs between 250 and 400°C. We attribute these conditions to increased efficiency of mass transfer and chemical reactions below the critical point of water and a consequence of volume-increasing serpentinisation and metasomatic reactions that take place over this temperature range. A comparison of the B/K9 kimberlite with kimberlites from Venetia, South Africa suggests that the composition and mineralogy of included xenoliths affects the alteration assemblages within kimberlite deposits.  相似文献   

12.
Speciation and colloid transport of arsenic from mine tailings   总被引:2,自引:0,他引:2  
In addition to affecting biogeochemical transformations, the speciation of As also influences its transport from tailings at inoperative mines. The speciation of As in tailings from the Sulfur Bank Mercury Mine site in Clear Lake, California (USA) (a hot-spring Hg deposit) and particles mobilized from these tailings have been examined during laboratory-column experiments. Solutions containing two common, plant-derived organic acids (oxalic and citric acid) were pumped at 13 pore volumes d−1 through 25 by 500 mm columns of calcined Hg ore, analogous to the pedogenesis of tailings. Chemical analysis of column effluent indicated that all of the As mobilized was particulate (1.5 mg, or 6% of the total As in the column through 255 pore volumes of leaching). Arsenic speciation was evaluated using X-ray absorption spectroscopy (XAS), indicating the dominance of arsenate [As(V)] sorbed to poorly crystalline Fe(III)-(hydr)oxides and coprecipitated with jarosite [KFe3(SO4, AsO4)2(OH)6] with no detectable primary or secondary minerals in the tailings and mobilized particles. Sequential chemical extractions (SCE) of <45 μm mine tailings fractions also suggest that As occurs adsorbed to Fe (hydr)oxides (35%) and coprecipitated within poorly crystalline phases (45%). In addition, SCEs suggest that As is associated with 1 N acid-soluble phases such as carbonate minerals (20%) and within crystalline Fe-(hydr)oxides (10%). The finding that As is transported from these mine tailings dominantly as As(V) adsorbed to Fe (hydr)oxides or coprecipitated within hydroxysulfates such as jarosite suggests that As release from soils and sediments contaminated with tailings will be controlled by either organic acid-promoted dissolution or reductive dissolution of host phases.  相似文献   

13.
The capacity of mine waste to trap CO2 is, in some cases, much larger than the greenhouse gas production of a mining operation. In mine tailings, the presence of secondary carbonate minerals that trap CO2 can therefore represent substantial fixation of this greenhouse gas. The abilities of three methods of quantitative phase analysis to measure trace nesquehonite (MgCO3·3H2O) in samples of processed kimberlite have been assessed: the method of reference intensity ratios (RIR), the internal standard method, and the Rietveld method with X-ray powder diffraction data. Tests on synthetic mixtures made to resemble processed kimberlite indicate that both the RIR and Rietveld methods can be used accurately to quantify nesquehonite to a lower limit of approximately 0.5 wt.% for conditions used in the laboratory. Below this value, estimates can be made to a limit of approximately 0.1 wt.% using a calibration curve according to the internal standard method. The RIR method becomes increasingly unreliable with decreasing abundance of nesquehonite, primarily as a result of an unpredictable decline in preferred orientation of crystallites. For Rietveld refinements, structureless pattern fitting was used to account for planar disorder in lizardite by considering it as an amorphous phase. Rietveld refinement of data collected from specimens that were serrated to minimize preferred orientation of crystallites gives rise to systematic overestimates of refined abundances for lizardite and underestimates for other phases. The resulting pattern of misestimates may be mistaken for the effect of amorphous and/or nanocrystalline material in samples. This effect is mitigated by collecting data from non-serrated specimens, which typically give relative errors on refined abundances for major and minor phases in the range of 5–20%. However, relative error can increase rapidly for abundances less than 5 wt.%. Nonetheless, absolute errors are sufficiently small that estimates can be made for the amount of CO2 stored in secondary nesquehonite using the RIR method or the Rietveld method for abundances ?0.5 wt.% and a calibration curve for abundances <0.5 wt.%. The extent to which C is being mineralized in an active mine setting at the Diavik Diamond Mine, Northwest Territories, Canada, has been investigated. Rietveld refinement results and calibrated abundances for trace nesquehonite are used to estimate the amount of CO2 trapped in Diavik tailings. Results of quantitative phase analysis are also used to calculate neutralization potentials for the kimberlite mine tailings and to estimate the contribution made by secondary nesquehonite.  相似文献   

14.
Anthropogenic greenhouse gas emissions may be offset by sequestering carbon dioxide (CO2) through the carbonation of magnesium silicate minerals to form magnesium carbonate minerals. The hydromagnesite [Mg5(CO3)4(OH)2·4H2O] playas of Atlin, British Columbia, Canada provide a natural model to examine mineral carbonation on a watershed scale. At near surface conditions, CO2 is biogeochemically sequestered by microorganisms that are involved in weathering of bedrock and precipitation of carbonate minerals. The purpose of this study was to characterize the weathering regime in a groundwater recharge zone and the depositional environments in the playas in the context of a biogeochemical model for CO2 sequestration with emphasis on microbial processes that accelerate mineral carbonation.Regions with ultramafic bedrock, such as Atlin, represent the best potential sources of feedstocks for mineral carbonation. Elemental compositions of a soil profile show significant depletion of MgO and enrichment of SiO2 in comparison to underlying ultramafic parent material. Polished serpentinite cubes were placed in the organic horizon of a coniferous forest soil in a groundwater recharge zone for three years. Upon retrieval, the cube surfaces, as seen using scanning electron microscopy, had been colonized by bacteria that were associated with surface pitting. Degradation of organic matter in the soil produced chelating agents and acids that contributed to the chemical weathering of the serpentinite and would be expected to have a similar effect on the magnesium-rich bedrock at Atlin. Stable carbon isotopes of groundwater from a well, situated near a wetland in the southeastern playa, indicate that  12% of the dissolved inorganic carbon has a modern origin from soil CO2.The mineralogy and isotope geochemistry of the hydromagnesite playas suggest that there are three distinct depositional environments: (1) the wetland, characterized by biologically-aided precipitation of carbonate minerals from waters concentrated by evaporation, (2) isolated wetland sections that lead to the formation of consolidated aragonite sediments, and (3) the emerged grassland environment where evaporation produces mounds of hydromagnesite. Examination of sediments within the southeastern playa–wetland suggests that cyanobacteria, sulphate reducing bacteria, and diatoms aid in producing favourable geochemical conditions for precipitation of carbonate minerals.The Atlin site, as a biogeochemical model, has implications for creating carbon sinks that utilize passive microbial, geochemical and physical processes that aid in mineral carbonation of magnesium silicates. These processes could be exploited for the purposes of CO2 sequestration by creating conditions similar to those of the Atlin site in environments, artificial or natural, where the precipitation of magnesium carbonates would be suitable. Given the vast quantities of Mg-rich bedrock that exist throughout the world, this study has significant implications for reducing atmospheric CO2 concentrations and combating global climate change.  相似文献   

15.
A detailed study of low-pressure gas-solid carbonation of chrysotile in dry and humid environments has been carried out. The evolving structure of chrysotile and its reactivity as a function of temperature (300-1200 °C), humidity (0-10 mol %) and CO2 partial pressure (20-67 mol %), thermal preconditioning, and alkali metal doping (Li, Na, K, Cs) have been monitored through in-situ X-ray photoelectron spectroscopy, isothermal thermogravimetry/mass spectrometry, ex-situ X-ray powder diffraction, and water and nitrogen adsorption/desorption. Based on chrysotile crystalline structure and its nanofibrilar orderliness, a multistep carbonation mechanism was elaborated to explain the role of water during chrysotile partial amorphisation, formation of periclase, brucite, and hydromagnesite crystalline phases, and surface passivation thereof, during humid carbonation. The weak carbonation reactivity was rationalized in terms of incongruent CO2 van der Waals molecular diameters with the octahedral-tetrahedral lattice constants of chrysotile. This lack of reactivity appeared to be relatively indifferent to the facilitated water crisscrossing during chrysotile core dehydroxylation/pseudo-amorphisation and surface hydroxylation induced product stabilization during humid carbonation. Thermodynamic stability domains of the species observed at low pressure have been thoroughly discussed on the basis of X-ray powder diffraction patterns and X-ray photoelectron spectroscopy evidence. The highest carbon dioxide uptake occurred at 375 °C in moist atmospheres. On the basis of chrysotile fresh N2 BET area, nearly 15 atoms out of 100 of the surface chrysotile brucitic Mg moiety have been carbonated at this temperature which was tantamount to the carbonation of about 2.5 at. % of the total brucitic Mg moiety in chrysotile. The carbonation of brucite (Mg(OH)2) impurities coexisting in chrysotile was minor and estimated to contribute by less than 17.6 at. % of the total converted magnesium. The presence of cesium traces (3 Cs atoms per 100 Mg atoms) was found to boost chrysotile carbonation capacity by a factor 2.7.  相似文献   

16.
Mineral aerosols play a significant role in gas–solid interfacial and atmospheric chemistry. Carbonation of olivine aerosol, which takes place in a multiphase reaction processes, can be an effective means to reduce the concentration of atmospheric carbon dioxide. Due to the presence of a huge reserve of silicate minerals in nature, olivine aerosol could be an ideal potential raw material for mineral carbonation for its higher reactivity with H2O and CO2. However, quantitative information about the carbonation process on the surface of natural olivine aerosol is not available. In this paper, calculations on the carbonation reaction processes with and without a H2O molecule using a periodic olivine model has been carried out via the density functional theory. The pathways and their corresponding energies and structures in the carbonation reactions have been established, and the effect of water as means to reduce the energy barriers and stabilize the carbonated structures by forming hydrogen bonds has been confirmed.  相似文献   

17.
Mineral processing operation at the Sarcheshmeh porphyry copper mine has produced huge quantities of tailings materials containing sulphide minerals in particular pyrite. These tailings materials were geochemically and mineralogically characterised to assess pyrite and chalcopyrite oxidation, acid mine drainage generation, and trace element mobility to lead development of a proper remediation plan. Five vertical trenches up to 4.2 m deep were excavated from the tailings surface, and 70 solid samples were taken in 0.3 m intervals. The samples were first mineralogically analysed. Pyrite was the main sulphide mineral found in the tailings. The gangue minerals include quartz ± muscovite–illite ± chlorite ± albite ± orthoclase ± halite. The samples were geochemically analysed for total concentrations of 62 elements, paste pH, SO4 2?, CO3 2?, and HCO3 ?. The maximum concentrations of SO4 2? (1,300, 1,170, 1,852, 1,960 and 837 mg/L) were observed at a depth of 0.9 m in profiles A, B, C, D and E, respectively. The tailings have a high acid-producing potential and low acid-neutralising potential (pyrite 4–6 wt %, calcite 1 wt %). Fe2(SO4)3, CuSO4, MgSO4 and MnSO4 were the dominant secondary sulphate minerals in the tailings. The lowest pH values (2.9, 3 and 3) were measured at a depth of 0.3 m in the profiles A, B and C, 3.9 at a depth of 0.6 m in the profile D and 3 at a depth of 0.9 m in the profile E. The upper portions of the profiles C (1.8 m) and D (2.1 m) were moderately oxidised, while oxidation in the profiles A, B and E did not extend more than 1.2, 1.2 and 1.5 m beneath the tailings surface. Zn, Pb, Rb, U, Hf, Nd, Zr and Ga show almost a constant trend with depth. Cd, Sr, Th, La and Ce increased with increasing depth of the tailings materials while, Co, V, Ti, Cr, Cu, As, Mn, Ag, Mo and Ni exhibit initially a decreasing trend from tailings surface to the depths that vary between 0.9 and 1.2. They then remained constant with the depth. The results show pyrite and chalcopyrite oxidation at surface layers of the tailings and subsequent leaching of the oxidation products and trace elements by infiltrated atmospheric precipitation.  相似文献   

18.
Tailings generated during processing of sulfide ores represent a substantial risk to water resources. The oxidation of sulfide minerals within tailings deposits can generate low-quality water containing elevated concentrations of SO4, Fe, and associated metal(loid)s. Acid generated during the oxidation of pyrite [FeS2], pyrrhotite [Fe(1−x)S] and other sulfide minerals is neutralized to varying degrees by the dissolution of carbonate, (oxy)hydroxide, and silicate minerals. The extent of acid neutralization and, therefore, pore-water pH is a principal control on the mobility of sulfide-oxidation products within tailings deposits. Metals including Fe(III), Cu, Zn, and Ni often occur at high concentrations and exhibit greater mobility at low pH characteristic of acid mine drainage (AMD). In contrast, (hydr)oxyanion-forming elements including As, Sb, Se, and Mo commonly exhibit greater mobility at circumneutral pH associated with neutral mine drainage (NMD). These differences in mobility largely result from the pH-dependence of mineral precipitation–dissolution and sorption–desorption reactions. Cemented layers of secondary (oxy)hydroxide and (hydroxy)sulfate minerals, referred to as hardpans, may promote attenuation of sulfide-mineral oxidation products within and below the oxidation zone. Hardpans may also limit oxygen ingress and pore-water migration within sulfide tailings deposits. Reduction–oxidation (redox) processes are another important control on metal(loid) mobility within sulfide tailings deposits. Reductive dissolution or transformation of secondary (oxy)hydroxide phases can enhance Fe, Mn, and As mobility within sulfide tailings. Production of H2S via microbial sulfate reduction may promote attenuation of sulfide-oxidation products, including Fe, Zn, Ni, and Tl, via metal-sulfide precipitation. Understanding the dynamics of these interrelated geochemical and mineralogical processes is critical for anticipating and managing water quality associated with sulfide mine tailings.  相似文献   

19.
《Applied Geochemistry》2003,18(11):1733-1750
The Rabbit Lake U mine in-pit tailings management facility (TMF) (425 m long×300 m wide×91 m deep) is located in northern Saskatchewan, Canada. The objectives of this study were to quantify the distribution of As phases in the tailings and evaluate the present-day geochemical controls on dissolved As. These objectives were met by analyzing pore fluid samples collected from the tailings body for dissolved constituents, measuring Eh, pH, and temperature of tailings core and pore fluid samples, conducting sequential extractions on solid samples, conducting geochemical modeling of pore fluid chemistry using available thermodynamic data, and by reviewing historical chemical mill process records. Dissolved As concentrations in 5 monitoring wells installed within the tailings body ranged from 9.6 to 71 mg/l. Pore fluid in the wells had a pH between 9.3 and 10.3 and Eh between +58 and +213 mV. Sequential extraction analyses of tailings samples showed that the composition of the solid phase As changed at a depth of 34 m. The As above 34 m was primarily associated with amorphous Fe and metal hydroxides while the As below 34 m was associated with Ca, likely as amorphous poorly ordered calcium arsenate precipitates. The change in the dominant As solid phases at this depth was attributed to the differences in the molar ratio of Fe to As in the mill tailings. Below 34 m it was <2 whereas above 34 m it was >4. The high Ca/As ratio during tailings neutralization would likely precipitate Ca4(OH)2(AsO4)2:4H2O type Ca arsenate minerals. Geochemical modeling suggested that if the pore fluids were brought to equilibrium with this Ca-arsenate, the long-term dissolved As concentrations would range between 13 and 126 mg/l.  相似文献   

20.
When nickeliferous peridot is submitted to a serpentinisation reaction with formation of brucite, the peridotic nickel is partitioned between the two minerals (serpentine and brucite) with a distribution coefficient K=[(Ni/Mg) brucite]/[(Ni/Mg)] serpentine=1,63 (at 350°C and 1 kbar), in favour of brucite.  相似文献   

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